Modulating the potent oxidative nature of Pt sites is the central strategy for optimizing the selective catalytic oxidation of NH3(NH3-SCO).The primary challenge is to suppress byproduct formation(N2O,NOx)...Modulating the potent oxidative nature of Pt sites is the central strategy for optimizing the selective catalytic oxidation of NH3(NH3-SCO).The primary challenge is to suppress byproduct formation(N2O,NOx)while preserving the intrinsic activity for N2 production,a balance governed by the metal-support interaction.Herein,a facile physical-mixing strategy is demonstrated to engineer a Pt/Cu-SSZ-13 catalyst that simultaneously establishes a moderate Pt-Cu interaction while preserving the integrity of isolated Z2Cu sites.This catalyst demonstrates superior performance,achieving 98% NH3 conversion at 180℃ and over 90% N2 selectivity(280-300℃),outperforming its coun-terpart prepared by intensive grinding.It also exhibits exceptional hydrothermal stability(750℃,10 h).Electronic structure and in-situ spectroscopy results reveal that the Pt-Cu electronic interaction tunes the reactivity of Pt sites to selectively catalyze the formation of *NOx intermediates.Concurrently,the preserved Z2Cu sites act as distinct active centers for NH3 adsorption,which then readily reduce these intermediates to N2.展开更多
The devastating neurodegenerative disorder of Alzheimer's disease hallmarks the presence of protein aggregates known as amyloid-β plaques and neurofibrillary tangles,composed of amyloid-β peptides and aberrantly...The devastating neurodegenerative disorder of Alzheimer's disease hallmarks the presence of protein aggregates known as amyloid-β plaques and neurofibrillary tangles,composed of amyloid-β peptides and aberrantly phosphorylated Tau protein,respectively.The accumulation of these inclusions leads to significant alterations in neuronal homeostasis and overall brain function,resulting in a progressive and rapid cognitive decline.Autophagy,the molecular mechanism of cellular waste removal through the lysosomal pathway,accounts for the degradation of both amyloid-β plaques and neurofibrillary tangles in the brain,conferring therefore protection against the pathology.In addition to general autophagy,several lines of evidence have reported the implication of selective autophagy receptors,including sequestosome 1/p62,the neighbor of BRCA1 gene,the nuclear-dot protein 52,and optineurin,in mediating the autophagic clearance of amyloid-β,phosphorylated Tau,or both.Herein,we have highlighted autophagy and selective autophagy as pivotal mechanisms in Alzheimer's disease,underlining selective autophagy receptors as a potential target for treatments in the future.展开更多
With the rapid global expansion of nuclear energy,the safe and efficient management of radioactive waste has emerged as a critical bottleneck restricting the sustainable development of the nuclear industry.Adsorption-...With the rapid global expansion of nuclear energy,the safe and efficient management of radioactive waste has emerged as a critical bottleneck restricting the sustainable development of the nuclear industry.Adsorption-based separation has garnered widespread attention for its high efficiency,facile operation,and inherent selectivity,among which zeolites stand out as promising radionuclide sequestration adsorbents,owing to their tailorable microporous framework,tunable surface chemistry,and exceptional chemicaladiation stability.This review takes adsorption selectivity as the overarching core perspective to systematically consolidate and critically assess the state-of-the-art advances in zeolite-mediated radionuclide adsorption over the past decade.It elaborates the selective adsorption mechanisms of zeolites towards key radionuclides(fission products:Cs,Sr,I;actinides:U,Th),critically analyzes the core factors modulating selectivity(framework topology,framework charge,surface functionalization,solution chemistry),and discusses the practical applications of zeolites in complex scenarios including radionuclide mining wastewater,nuclear power plant effluents,and contaminated soils.This review differs from conventional reviews that mainly focus on adsorption capacity in ideal single-nuclide systems.In contrast,this review systematically addresses selective adsorption mechanisms,performance modulation,and practical applications in complex matrices,aims to establish a theoretical foundation for the rational design of high-selectivity zeolite adsorbents,and provides forward-looking insights into the targeted separation,efficient enrichment,and safe disposal of radionuclides.展开更多
Catalytically powered micro-anomotors have become a compelling alternative to conventional catalysts for active and efficient removal of environmental pollutants in water remediation.We developed a novel biocatalytic ...Catalytically powered micro-anomotors have become a compelling alternative to conventional catalysts for active and efficient removal of environmental pollutants in water remediation.We developed a novel biocatalytic nanomotor system by encapsulating catalase and peroxidase enzymes into metal-organic frameworks(MOFs),demonstrating exceptional speed and facilitated motion-induced convection and mass transfer.Leveraging a synergistic structural etching and surface engineering strategy using tannic acid(TA),we create a tailored microenvironment of the MOF’s framework with charge-selective and nanoconfinement properties.Both experimental and simulation results indicate that microenvironment modulation of MOF matrix could act in synergy with the encapsulated enzymes and significantly improve efficiency and selectivity in removing charged pollutants.Surface engineering of TA selectively preconcentrates target contaminants by modulating the MOF shell’s surface charge,while etching-induced voids facilitate rapid mass transfer to the enzyme active sites.Finally,we also validated the applicability of these nanomotors in the transformative removal of pollutants from the aqueous phase into polymeric products via an enzyme-mediated polymerization pathway.This biocatalytic nanomotor system provides a promising water remediation paradigm for reducing carbon emissions and recycling chemical energy from emerging contaminants.展开更多
Since sulfur oxides in the engine exhaust usually lead to the catalyst deactivation,so SO2 resistance under low-temperature conditions serves as a critical performance criterion to the catalysts.A series of ZrVO_(x...Since sulfur oxides in the engine exhaust usually lead to the catalyst deactivation,so SO2 resistance under low-temperature conditions serves as a critical performance criterion to the catalysts.A series of ZrVOx@CeO2 catalysts with excellent catalytic activity and SO2 tolerance was synthesized using the combination of hydrothermal and precipitation methods for the ammonia selective catalytic reduction(NH3-SCR)reaction.In the range of 160-380℃,the NO conversion is consistently over 90%.Notably,with the addition of 200 ppm SO2,the NO conversion stabilizes at 90%within 10 h at 230℃.The CeO2 species are deposited as fine particles on the catalyst surface,forming irregular spherical protrusions.This morphology significantly increases the specific surface area,which in turn enhances the activation and adsorption of reactant.The incorporation of CeO2 modifies the electronic structure of the O 1s orbital,and generates a higher density of oxygen vacancies to maintain electrostatic equilibrium.In situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTs)shows that SO2 has little effect on the adsorption and activation of NO and NH3.Therefore,the ZrVOx@CeO2 catalysts exhibit excellent reducibility,effectively enhancing the catalytic performance.Overall,the main mechanism on the ZrVOx@CeO2 catalyst is the Langmuir-Hinshelwood mechanism.展开更多
Although lithium metal has been regarded as an ideal anode material for high-energy-density batteries,its practical applications remain hindered by many serious challenges.Three-dimensional(3D)porous Cu current collec...Although lithium metal has been regarded as an ideal anode material for high-energy-density batteries,its practical applications remain hindered by many serious challenges.Three-dimensional(3D)porous Cu current collectors demonstrate potential in ensuring uniform Li deposition.However,notable drawbacks of 3D Cu collectors—such as poor lithophilic properties,unordered interface microstructure,and insufficient surface area—still hamper their effectiveness.Herein,a 3D porous Cu skeleton with lithiophilic Cu0.64Zn0.36 alloy“skins”and curvature boundaries(CuZn@Cu)is developed.In CuZn@Cu,the Cu0.64Zn0.36 alloy layer endows the collector with good lithium affinity and low surface reaction activation energy,thereby promoting uniform lithium deposition.In addition,the abundant curvature boundaries in CuZn@Cu regulate the distributions of the electric field and lithium ion flux,guiding the selective nucleation and growth of lithium.Consequently,compact and dendrite-free lithium deposition is achieved on CuZn@Cu,and the CuZn@Cu collector enables a high average Coulombic efficiency of 98.15%in 1000 cycles.The lithium symmetric cells with the CuZn@Cu exhibit a long cycle life of more than 1400 h at1 m A cm-2.展开更多
Powder paving is an intermediate process of selective laser sintering(SLS).The dimensional accuracy and mechanical properties of sintered components are directly affected by the quality of the powder paving process,wh...Powder paving is an intermediate process of selective laser sintering(SLS).The dimensional accuracy and mechanical properties of sintered components are directly affected by the quality of the powder paving process,which is closely related to the flow characteristics of the powder and the process parameters of powder paving.This study investigated the simulation and optimization of the nylon powder paving in SLS by combining a discrete-element-method numerical simulation with a process test.A dynamic model was established to describe the flow and paving process of nylon powder at a preheating temperature considering mesoscopic van der Waals and electrostatic forces.The effects of the physical parameters and ambient temperature on the flow characteristics of nylon powder were analyzed,and the intrinsic relationship between the physical parameters of nylon powder,the process parameters of powder paving,and the quality of the powder paving were explored.A multi-objective regression model of the quality of powder paving was established using the response surface methodology,and a genetic algorithm was adopted to optimize the quality of the powder paving.A scientific and intelligent database of the nylon powder paving process in SLS was constructed by matching the process parameters of powder paving and physical parameters of the nylon powder,and the level of the SLS process was improved.展开更多
The selective hydrogenation of furfural(FAL)to furfuryl alcohol(FOL)over Ni catalysts offers a sustainable route for biomass valorization.However,the conventional Ni catalysts suffer from poor selectivity in FAL hydro...The selective hydrogenation of furfural(FAL)to furfuryl alcohol(FOL)over Ni catalysts offers a sustainable route for biomass valorization.However,the conventional Ni catalysts suffer from poor selectivity in FAL hydrogenation.Herein,we report that the moderate Fe doping in Ni/TiO2 significantly enhances selectivity without compromising catalytic activity for the selective hydrogenation of FAL to FOL.Notably,Ni/Fe-TiO2 catalyst with Fe content≥4.9 wt% maintained>90%selectivity toward FOL at nearly 100% conversion,whereas Ni/TiO2 achieved only 38% under the identical condition.Combined experimental and theoretical studies revealed that the enhanced catalytic performance of Ni/Fe-TiO2 originates from the dilution of contiguous Ni sites by Fe,which suppresses the further hydrogenation of FOL.Moreover,Fe sites exhibited a stronger affinity for carbonyl groups compared to Ni(0),indicating complementary role where Ni(0)primarily facilitates H2 dissociation,while Fe sites play a critical role in carbonyl activation.These findings underscore the superior synergistic effect of bimetallic systems in promoting selective functional group transformation.展开更多
With the dramatic accumulation of the end-of-life lithium-ion batteries,their recycling is attracting extensive attention worldwide.To address the problem of low lithium recovery in the current typical hydrometallurgy...With the dramatic accumulation of the end-of-life lithium-ion batteries,their recycling is attracting extensive attention worldwide.To address the problem of low lithium recovery in the current typical hydrometallurgy recovery process,this research uses sodium bisulfate as an auxiliary roasting reagent to extract lithium from spent lithium-ion batteries through sulphation roasting,which can enhance the lithium recovery rate significantly.A systematic study of the sulphation roasting process and the mechanisms was carried out with experiments,thermodynamic calculations,and characterization of the roasted sample phases.The results showed that at a roasting temperature of 600℃,NaHSO4·H2O/spent LiNixCoyMnzO2 cathode powders(S-NCM)mass ratio of 1.2,and roasting time of 60 min,95% selective dissolution of lithium was acquired,while the leaching rates of Ni,Co,and Mn were confined under 1%.During roasting,the NCM layered structure collapses and the lithium is transformed into the LiNaSO4 phase,while the transition metals transform into Ni6MnO8 and MnCo2O4 phases.The removal of impurity ions from the lithium-rich leaching solution and the generation of Li2CO3 were achieved by a combination of thermodynamic calculations and experiments.展开更多
Precisely controlling acid center position in zeolites is still challenging.Pentene monomolecular cracking offers an ideal route to maximize ethylene and propylene yields simultaneously.To reveal the relationship betw...Precisely controlling acid center position in zeolites is still challenging.Pentene monomolecular cracking offers an ideal route to maximize ethylene and propylene yields simultaneously.To reveal the relationship between acid site distribution in FER-zeolite and pentene monomolecular cracking activity,this study proposes a novel strategy integrating pyridine pre-adsorption with K+ exchange modification to selectively shield acid sites within FER cages,while phosphorus modification is employed to selectively passivate acid sites in 10-MR channels and on the external surface.Adsorption infrared(IR)spectroscopy(CD3CN-IR,Py-IR,and 2,6-DMPy-IR),and OH-IR characterization verified the selectivity and efficiency of these modification process.FER zeolites with distinct acid site distributions exhibit typical monomolecular cracking characteristics in pentene cracking,where the pentene cracking activity is linearly related to the acid density in the 10-MR channel and independent of the FER cage acidity.This result identifies 10-MR channel as primary pentene monomolecular cracking reaction position for the first time,providing a theoretical basis for designing zeolite catalysts that maximize ethylene and propylene production.The synergistic application of the pre-adsorption-K+exchange modiϐication strategy using different size basic molecules and phosphorus modification will provide an effective approach for precise control of acid site locations in zeolites with diverse pore/cavities architectures.展开更多
Selective extraction of precious metals from urban mines plays a crucial role in mitigating the risk of depletion of precious metal resources and reducing waste pollution.However,a major obstacle in precious metal ext...Selective extraction of precious metals from urban mines plays a crucial role in mitigating the risk of depletion of precious metal resources and reducing waste pollution.However,a major obstacle in precious metal extraction lies in the difficulty of distinguishing the subtle differences in the physicochemical characteristics between them,especially gold and palladium.Herein,a proton-driven separation system was presented for cascade recovery of gold and palladium from waste-printed circuit boards(W-PCBs)leachate using poly(amidoxime)(PAO)hydrogel.This exhibits an ultra-high capacity,extra-fast rate,and excellent selectivity for the extraction of Au(Ⅲ)and Pd(Ⅱ).Notably,the separation of Au(Ⅲ)and Pd(Ⅱ)can be achieved with high selectivity at pH=0,resulting in a remarkable separation factor of kAu(Ⅲ/Pd(Ⅱ))=36.5.This was demonstrated to originate from the differential mechanism of PAO hydrogel for the capture of Au(Ⅲ)and Pd(Ⅱ)under proton-mediated conditions.Drawing inspiration from the mechanism,the proton-driven cascade recovery system demonstrates remarkable efficiency in sequentially recovering 99.92%of gold and 99.05%of palladium from W-PCBs acid leachate.This research opens up a strategy to precisely separate and recover precious metals from e-waste of urban mines.展开更多
The oxygen evolution reaction suffers from sluggish kinetics and poor structural stability,necessitating the development of nonprecious metal electrocatalysts with efficient electronic regulation and intrinsic structu...The oxygen evolution reaction suffers from sluggish kinetics and poor structural stability,necessitating the development of nonprecious metal electrocatalysts with efficient electronic regulation and intrinsic structural robustness.Herein,we construct a composite precatalyst of LaFe species modified cobalt carbonate hydroxide supported on nickel foam(LaFe–CoCH/NF)through a three-step process involving electrodeposition,hydrothermal growth,and co-deposition.This strategy enables the formation of a Ni–Co–Fe tri-level electron regulation pathway coupled with a spatially selective LaFe coating layer,achieving dual enhancement in both electronic modulation and structural stabilization.The hierarchical electron pathway effectively activates Ni sites within the nickel foam substrate,promotes the generation of high-valence Ni and Co species,and simultaneously suppresses the overoxidation of Fe.Meanwhile,the La-induced local electric field and buffering effect alleviate the detachment of the active phase during electrochemical reconstruction.As a result,the optimized LaFe–CoCH/NF catalyst exhibits outstanding oxygen evolution reaction performance,with a low Tafel slope of 33.75 mV dec-1 and exceptional durability,maintaining over 1500 h of stable operation at 10 mA cm-2,continuous operation for 1200 h at 50 and 100 mA cm-2,and more than 200 h of durability even at an ultrahigh current density of 500 mA cm-2.Mechanistic investigations reveal that the tri-metallic electron regulation strategy significantly improves interfacial charge transfer efficiency and structural integrity,offering theoretical guidance and a viable design route for advanced multi-metallic oxygen evolution reaction precatalysts.展开更多
The rational design of high-performance CO2adsorbents remains a critical challenge in addressing global carbon emissions,with metal-organic frameworks(MOFs)emerging as promising candidates due to their tunable pore...The rational design of high-performance CO2adsorbents remains a critical challenge in addressing global carbon emissions,with metal-organic frameworks(MOFs)emerging as promising candidates due to their tunable pore environments.However,the lack of systematic guidelines for functional group selection has hindered their practical implementation in carbon capture applications.Here,this gap was addressed by developing a comprehensive design framework through high-throughput computational screening.Through construction of a topology-directed database of 4797,integrating 10 metal centers with 144 functionalized ligands(18 ligands modified by–NH2,–NO2,–CH3,–CF3,–SH2,–SO2,–OH,and–OLi)across 36 topologies,the fundamental structure–property relationships governing CO2capture performance was established.Multi-metric evaluation reveals that–NO2,–SO2,and–OLi dramatically enhance CO2selectivity over CH_4/N2via selectivity(Sads),working capacity(ΔN),adsorbent performance score(APS),sorbent selection parameter(Ssp),and renewability R.Specially,ΔN rises from 2.34(pristine)to 5.91–7.94 mmol g-1and Sadssurges from 24.94/40.36 to 121.11/176.87(–NO2),149.94/215.54(–SO2),and 58.64/267.44(–OLi).Besides,the critical trade-off between adsorption strength and renewability demonstrates that enhanced performance comes at the cost of reduced renewability,where stronger CO2affinity(isosteric heat of-29.15,-29.96,and-30.09 for–NO2,–SO2,and–OLi)compromises renewability(R reduced by -50%).To resolve this trade-off,a novel energy efficiency(η)metric was introduced,which holistically evaluates both adsorption performance(Sads,ΔN,APS,Ssp,and R)and energy inputs(desorption heat,pressure-swing energy,net loss).This leads to the identification of–SO2as the optimal functional group that balances exceptional CO2capture(η=6.17/12.78 for CO2over CH_4/N2),surpassing the second higher of 4.74/8.80 in–CF3and 0.99/2.18 in non-functionalized counterparts.Adopting high-throughput computational screening methods,this work provides both fundamental insights into host–guest interactions in functionalized MOFs and a practical framework for designing next-generation adsorbents,bridging the gap between materials discovery and process engineering considerations in carbon capture technologies.展开更多
In this work,a Cu-based carbon catalyst(H-Cu/C)with an octahedral morphology was synthesized by pyrolyzing the metal-organic framework(MOF)precursor HKUST-1,where Cu(0)nanoparticles were uniformly dispersed in the car...In this work,a Cu-based carbon catalyst(H-Cu/C)with an octahedral morphology was synthesized by pyrolyzing the metal-organic framework(MOF)precursor HKUST-1,where Cu(0)nanoparticles were uniformly dispersed in the carbon matrix,alongside the formation of island-like Cu2O structures as the active sites.Multiple characterization techniques,including XPS,XRD,SEM and HRTEM,reveal the critical role of carbon matrix in stabilizing the metal nanoparticles.In combination with TEMPO and using molecular oxygen as a green oxidant,the H-Cu/C catalyst is highly efficient in the selective oxidation of aromatic alcohols to the corresponding aldehydes under alkali-free conditions.Using benzyl alcohol as a model substrate,an alcohol conversion of 99.2%and a benzaldehyde yield of 94.1%were achieved under mild reaction conditions(100℃,0.5 MPa O2,1 h).The catalytic system displays excellent universality for various mono-and ortho/para-disubstituted aromatic alcohols,affording an alcohol conversion of over 99%and a yield of corresponding aromatic aldehydes of above 95%.In addition,the H-Cu/C catalyst can be regenerated via H2 reduction and reused without significant loss of activity.This work provides a new strategy for designing green and efficient non-noble metal catalytic systems for the oxidation reactions.展开更多
Selective depression of pyrite remains a major bottleneck in copper flotation,particularly when high-pyrite ores are processed and saline water is used.In such environments,conventional approaches using lime and inert...Selective depression of pyrite remains a major bottleneck in copper flotation,particularly when high-pyrite ores are processed and saline water is used.In such environments,conventional approaches using lime and inert grinding media often fail to discriminate ef-fectively between pyrite and valuable copper minerals due to strong copper activation on pyrite surfaces.This study introduced a novel approach using inorganic radicals generated from peroxymonosulfate(PMS)to selectively oxidize and depress pyrite.Flotation tests with synthetic high-pyrite ore blends showed that PMS significantly reduced pyrite recovery while maintaining or improving chalcopyrite flot-ation.Ethylenediaminetetraacetic acid(EDTA)extraction confirmed selective oxidation of pyrite,and electron paramagnetic resonance(EPR)spectroscopy identified hydroxyl(·OH)and sulfate(SO4·-)radicals as the dominant reactive species.Iron ions from grinding me-dia and mineral surfaces were identified as key activators of PMS.A major insight was pyrite’s dual role,acting both as a radical scav-enger and an activator,which made it highly reactive and susceptible to radical-induced oxidation.This process converted surface copper-sulfur species into copper hydroxides,effectively suppressing pyrite flotation.While previous studies have applied EPR to detect radicals in simplified activator/precursor systems,this study provides the first direct mechanistic evidence of radical-driven selectivity in flotation by detecting inorganic radicals in a complex flotation slurry,thereby demonstrating their persistence under industrially relevant conditions and establishing a foundation for more effective and targeted flotation strategies.展开更多
Cu electrocatalysts have been demonstrated to have unique ability to reduce CO2to various high value-added C2 products like ethylene and alcohols.However,realizing high selectivity of C2 products are still a ...Cu electrocatalysts have been demonstrated to have unique ability to reduce CO2to various high value-added C2 products like ethylene and alcohols.However,realizing high selectivity of C2 products are still a main challenge due to complex CO2electroreduction pathways and small opportunity of C-C coupling reactions.Here,we found the origin of enhanced CO2electroreduction reaction activity and product selectivity towards C2 products and C-C coupling mechanism at halogen atoms-adsorbed Cu/H2O interfaces,the corresponding CO2electroreduction evolution mechanisms at the halogen atoms-modified Cu/H2O interfaces are systematically studied via theoretical modeling and calculations.The calculated results indicate that halide anions modifications are beneficial to CO dimerization into OCCO dimer,especially Cl--adsorbed Cu(111)/H2O interface has the optimum activity and selectivity towards OCCO dimer,subsequent Cl-adsorbed Cu(111)/H2O interface can selectively reduce CO2into C2H4 product.The function relationship between adsorption free energy of Cl atom and electrode potential explain why the adsorption of Cl-can enhance selectivity of C2H4 product.The determinations of onset potentials indicate that electroreduction pathways of CO2towards C2H4 product are facile to take place and further explain the origin of the significantly enhanced CO production activity and C2H4 product selectivity.This work on selective realization of CO2electroreduction towards C2H4 product via Cl--modified Cu(111)/H2O interface provide a theoretical guideline for how to selectively realize other high value-added C2 products.展开更多
The selective oxidation of methane to formaldehyde presents a formidable challenge due to the inherent stability of methane and the tendency for overoxidation.Herein,we report core-shell structured 1%Cu/m-SiO2@TiO_...The selective oxidation of methane to formaldehyde presents a formidable challenge due to the inherent stability of methane and the tendency for overoxidation.Herein,we report core-shell structured 1%Cu/m-SiO2@TiO2-x catalysts designed to enhance catalytic performance for the selective oxidation of methane.The incorporation of a TiO2coating was found to play a critical role in modulating the dispersion of copper species and the surface chemical microenvironment.Characterization techniques revealed that the TiO2layer modulates the surface chemical environment,promoting the formation of Si-O-Ti interfaces and influencing the electronic interaction among Cu,Ti,and Si.The Si-O-Ti interface was identified as crucial for anchoring highly dispersed CuOxclusters,optimizing oxygen vacancy generation,and regulating reactive oxygen species.Consequently,this tailored interface suppressed the overoxidation of formaldehyde,leading to improved formaldehyde selectivity while maintaining comparable methane conversion.The optimized catalyst(1%Cu/m-SiO2@TiO2-1)achieved a formaldehyde yield of 1.3%at 700℃,with significantly improved selectivity compared with its unmodified counterpart(1%Cu/m-SiO2).This work highlights the importance of interface engineering in catalyst design and provides a viable strategy for developing efficient catalysts for the direct conversion of methane to formaldehyde.展开更多
Background:Selective laser trabeculoplasty(SLT)is a first-line treatment for open-angle glaucoma(OAG)or ocular hypertension(OHT).However,the optimal SLT protocol remains unsettled.Randomized controlled trials(RCTs)com...Background:Selective laser trabeculoplasty(SLT)is a first-line treatment for open-angle glaucoma(OAG)or ocular hypertension(OHT).However,the optimal SLT protocol remains unsettled.Randomized controlled trials(RCTs)comparing 180°and 360°SLT have yielded conflicting outcomes.This systematic review and meta-analysis aimed to determine which approach provides superior efficacy and safety.Methods:We searched PubMed,Embase,Cochrane,and Web of Science through November 8,2025 for RCTs comparing 180°with 360°SLT in OAG or OHT.We excluded conference abstracts.The primary outcome was intraocular pressure(IOP).Secondary outcomes included treatment success,visual acuity,and adverse events.We assessed the risk of bias with the Cochrane risk-of-bias tool for randomized trials,and estimated mean differences(MDs)and risk ratios(RRs)with 95%confidence intervals(CIs)using a randomeffects model.Trial sequential analysis(TSA)evaluated the robustness of evidence.Results:We included six studies comprising 892 eyes.180°SLT was associated with higher IOP at 1 month(MD 1.17 mmHg;95%CI:0.52–1.81;P<0.01;I2=36%),3 months(MD 0.96 mmHg;95%CI:0.45–1.47;P<0.01;I2=0%),6 months(MD 1.03 mmHg;95%CI:0.14–1.92;P=0.02;I2=58%),and 12 months(MD 1.63 mmHg;95%CI:0.66–2.60;P<0.01;I2=0%).Treatment success(RR 0.72;95%CI:0.58–0.90;P<0.01;I2=50%)and pain or discomfort rates(RR 0.63;95%CI:0.50–0.81;P<0.01;I2=0%)were lower with 180°SLT.There was no difference between groups in visual acuity(MD−0.002 logMAR;95%CI:−0.029 to 0.026 logMAR;P=0.90;I2=41%)and adverse events risk(RR 1.08;95%CI:0.69–1.68;P=0.75;I2=0%).TSA showed robust evidence for the superiority of 360°vs.180°SLT on IOP.Conclusions:180°SLT was inferior to 360°SLT for IOP control and treatment success in OAG or OHT,yet it was associated with a lower risk of pain or discomfort.These findings support 360°SLT as the preferred protocol,though evidence is limited by the number of trials,heterogeneity,and follow-up.Highquality,long-term RCTs are required to validate these findings.展开更多
Cyclohexene is an important raw material for nylon production,and the selective hydrogenation of benzene is a key route for preparing cyclohexene.To promote data sharing and reuse in this field,we collected and standa...Cyclohexene is an important raw material for nylon production,and the selective hydrogenation of benzene is a key route for preparing cyclohexene.To promote data sharing and reuse in this field,we collected and standardized experimental data on the hydrogenation of benzene to cyclohexene from publicly available literature and constructed a comprehensive dataset containing catalyst composition,reaction conditions,and reaction results(conversion,selectivity and yield).This data descriptor details the source,field definitions,generation and processing workflow,quality control,sharing approach and usage recommendations of the dataset,with the aim of providing a reusable data foundation for subsequent statistical analysis,machine learning modeling,experimental design,and catalyst screening.展开更多
Carbon-chain rubbers have been widely used in many fields including transportation,medicine,construction,and everyday life,owing to their excellent flexibility.Now,waste rubbers have caused serious environmental pollu...Carbon-chain rubbers have been widely used in many fields including transportation,medicine,construction,and everyday life,owing to their excellent flexibility.Now,waste rubbers have caused serious environmental pollution and resource waste.Chemical recovery is expected to provide a solution to solve these problems fundamentally.Here,the recent progress in selective chain scissions of the waste sulfur-vulcanized carbon-chain rubbers for reuse was reviewed.Based on the different devulcanization approaches,the polysulfide crosslinking chains or carbon chains were broken and the linear or branched degraded products could be obtained as structural prepolymers for new rubber products.After a comprehensive literature review on the effect of the molecular composition and topology of the devulcanized and degraded products on the new rubbers,the future perspectives were proposed.展开更多
摘要Modulating the potent oxidative nature of Pt sites is the central strategy for optimizing the selective catalytic oxidation of NH3(NH3-SCO).The primary challenge is to suppress byproduct formation(N2O,NOx)while preserving the intrinsic activity for N2 production,a balance governed by the metal-support interaction.Herein,a facile physical-mixing strategy is demonstrated to engineer a Pt/Cu-SSZ-13 catalyst that simultaneously establishes a moderate Pt-Cu interaction while preserving the integrity of isolated Z2Cu sites.This catalyst demonstrates superior performance,achieving 98% NH3 conversion at 180℃ and over 90% N2 selectivity(280-300℃),outperforming its coun-terpart prepared by intensive grinding.It also exhibits exceptional hydrothermal stability(750℃,10 h).Electronic structure and in-situ spectroscopy results reveal that the Pt-Cu electronic interaction tunes the reactivity of Pt sites to selectively catalyze the formation of *NOx intermediates.Concurrently,the preserved Z2Cu sites act as distinct active centers for NH3 adsorption,which then readily reduce these intermediates to N2.
基金supported by AIRC Foundation(Grant IG MFAG-202024467)Fondation Alzheimer and Ligue contre le Cancer to FS。
摘要The devastating neurodegenerative disorder of Alzheimer's disease hallmarks the presence of protein aggregates known as amyloid-β plaques and neurofibrillary tangles,composed of amyloid-β peptides and aberrantly phosphorylated Tau protein,respectively.The accumulation of these inclusions leads to significant alterations in neuronal homeostasis and overall brain function,resulting in a progressive and rapid cognitive decline.Autophagy,the molecular mechanism of cellular waste removal through the lysosomal pathway,accounts for the degradation of both amyloid-β plaques and neurofibrillary tangles in the brain,conferring therefore protection against the pathology.In addition to general autophagy,several lines of evidence have reported the implication of selective autophagy receptors,including sequestosome 1/p62,the neighbor of BRCA1 gene,the nuclear-dot protein 52,and optineurin,in mediating the autophagic clearance of amyloid-β,phosphorylated Tau,or both.Herein,we have highlighted autophagy and selective autophagy as pivotal mechanisms in Alzheimer's disease,underlining selective autophagy receptors as a potential target for treatments in the future.
基金supported by the National Natural Science Foundation of China(22472152)the Natural Science Foundation of Zhejiang Province(LY22B030006)the Fundamental Research Funds of Zhejiang Sci-Tech University(26262135-Y)。
摘要With the rapid global expansion of nuclear energy,the safe and efficient management of radioactive waste has emerged as a critical bottleneck restricting the sustainable development of the nuclear industry.Adsorption-based separation has garnered widespread attention for its high efficiency,facile operation,and inherent selectivity,among which zeolites stand out as promising radionuclide sequestration adsorbents,owing to their tailorable microporous framework,tunable surface chemistry,and exceptional chemicaladiation stability.This review takes adsorption selectivity as the overarching core perspective to systematically consolidate and critically assess the state-of-the-art advances in zeolite-mediated radionuclide adsorption over the past decade.It elaborates the selective adsorption mechanisms of zeolites towards key radionuclides(fission products:Cs,Sr,I;actinides:U,Th),critically analyzes the core factors modulating selectivity(framework topology,framework charge,surface functionalization,solution chemistry),and discusses the practical applications of zeolites in complex scenarios including radionuclide mining wastewater,nuclear power plant effluents,and contaminated soils.This review differs from conventional reviews that mainly focus on adsorption capacity in ideal single-nuclide systems.In contrast,this review systematically addresses selective adsorption mechanisms,performance modulation,and practical applications in complex matrices,aims to establish a theoretical foundation for the rational design of high-selectivity zeolite adsorbents,and provides forward-looking insights into the targeted separation,efficient enrichment,and safe disposal of radionuclides.
基金supported by the National Natural Science Foundation of China(Grant No.52300017)the Australian Research Council(ARC,DP250101401,FT220100479)S.Xu would like to acknowledge financial support from the China Scholarship Council(Grant No.201906120387).
摘要Catalytically powered micro-anomotors have become a compelling alternative to conventional catalysts for active and efficient removal of environmental pollutants in water remediation.We developed a novel biocatalytic nanomotor system by encapsulating catalase and peroxidase enzymes into metal-organic frameworks(MOFs),demonstrating exceptional speed and facilitated motion-induced convection and mass transfer.Leveraging a synergistic structural etching and surface engineering strategy using tannic acid(TA),we create a tailored microenvironment of the MOF’s framework with charge-selective and nanoconfinement properties.Both experimental and simulation results indicate that microenvironment modulation of MOF matrix could act in synergy with the encapsulated enzymes and significantly improve efficiency and selectivity in removing charged pollutants.Surface engineering of TA selectively preconcentrates target contaminants by modulating the MOF shell’s surface charge,while etching-induced voids facilitate rapid mass transfer to the enzyme active sites.Finally,we also validated the applicability of these nanomotors in the transformative removal of pollutants from the aqueous phase into polymeric products via an enzyme-mediated polymerization pathway.This biocatalytic nanomotor system provides a promising water remediation paradigm for reducing carbon emissions and recycling chemical energy from emerging contaminants.
基金Project supported by the National Key R&D Program of China(2023YFC3707300,2023YFC3707304,2024YFC3712300)the National Natural Science Foundation of China(52200128)+1 种基金the Natural Science Foundation of Tianjin,China(23JCQNJC00500)the National Nonprofit Institute Research Grants of Tianjin Research Institute of Water Transport Engineering,China(TKS20240302,TKS20230303,TKS20230304)。
摘要Since sulfur oxides in the engine exhaust usually lead to the catalyst deactivation,so SO2 resistance under low-temperature conditions serves as a critical performance criterion to the catalysts.A series of ZrVOx@CeO2 catalysts with excellent catalytic activity and SO2 tolerance was synthesized using the combination of hydrothermal and precipitation methods for the ammonia selective catalytic reduction(NH3-SCR)reaction.In the range of 160-380℃,the NO conversion is consistently over 90%.Notably,with the addition of 200 ppm SO2,the NO conversion stabilizes at 90%within 10 h at 230℃.The CeO2 species are deposited as fine particles on the catalyst surface,forming irregular spherical protrusions.This morphology significantly increases the specific surface area,which in turn enhances the activation and adsorption of reactant.The incorporation of CeO2 modifies the electronic structure of the O 1s orbital,and generates a higher density of oxygen vacancies to maintain electrostatic equilibrium.In situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTs)shows that SO2 has little effect on the adsorption and activation of NO and NH3.Therefore,the ZrVOx@CeO2 catalysts exhibit excellent reducibility,effectively enhancing the catalytic performance.Overall,the main mechanism on the ZrVOx@CeO2 catalyst is the Langmuir-Hinshelwood mechanism.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.52001066 and 21805039)the Natural Science Foundation of Fujian Province(Grant Nos.2023J01500 and2021J01157)Fuzhou Science and Technology Project(Grant No.2024-Y-001)。
摘要Although lithium metal has been regarded as an ideal anode material for high-energy-density batteries,its practical applications remain hindered by many serious challenges.Three-dimensional(3D)porous Cu current collectors demonstrate potential in ensuring uniform Li deposition.However,notable drawbacks of 3D Cu collectors—such as poor lithophilic properties,unordered interface microstructure,and insufficient surface area—still hamper their effectiveness.Herein,a 3D porous Cu skeleton with lithiophilic Cu0.64Zn0.36 alloy“skins”and curvature boundaries(CuZn@Cu)is developed.In CuZn@Cu,the Cu0.64Zn0.36 alloy layer endows the collector with good lithium affinity and low surface reaction activation energy,thereby promoting uniform lithium deposition.In addition,the abundant curvature boundaries in CuZn@Cu regulate the distributions of the electric field and lithium ion flux,guiding the selective nucleation and growth of lithium.Consequently,compact and dendrite-free lithium deposition is achieved on CuZn@Cu,and the CuZn@Cu collector enables a high average Coulombic efficiency of 98.15%in 1000 cycles.The lithium symmetric cells with the CuZn@Cu exhibit a long cycle life of more than 1400 h at1 m A cm-2.
基金Supported by National Natural Science Foundation of China(Grant Nos.52375466,51975504)Guangdong Provincial Basic and Applied Basic Research Foundation(Grant No.2022A1515110862)+1 种基金Jiangsu Provincial Key Laboratory of Precision and Micro-Manufacturing Technology(Grant No.JSKL2223K06)Hunan Provincial Excellent Youth Project of Education Department(Grant No.22B0109).
摘要Powder paving is an intermediate process of selective laser sintering(SLS).The dimensional accuracy and mechanical properties of sintered components are directly affected by the quality of the powder paving process,which is closely related to the flow characteristics of the powder and the process parameters of powder paving.This study investigated the simulation and optimization of the nylon powder paving in SLS by combining a discrete-element-method numerical simulation with a process test.A dynamic model was established to describe the flow and paving process of nylon powder at a preheating temperature considering mesoscopic van der Waals and electrostatic forces.The effects of the physical parameters and ambient temperature on the flow characteristics of nylon powder were analyzed,and the intrinsic relationship between the physical parameters of nylon powder,the process parameters of powder paving,and the quality of the powder paving were explored.A multi-objective regression model of the quality of powder paving was established using the response surface methodology,and a genetic algorithm was adopted to optimize the quality of the powder paving.A scientific and intelligent database of the nylon powder paving process in SLS was constructed by matching the process parameters of powder paving and physical parameters of the nylon powder,and the level of the SLS process was improved.
摘要The selective hydrogenation of furfural(FAL)to furfuryl alcohol(FOL)over Ni catalysts offers a sustainable route for biomass valorization.However,the conventional Ni catalysts suffer from poor selectivity in FAL hydrogenation.Herein,we report that the moderate Fe doping in Ni/TiO2 significantly enhances selectivity without compromising catalytic activity for the selective hydrogenation of FAL to FOL.Notably,Ni/Fe-TiO2 catalyst with Fe content≥4.9 wt% maintained>90%selectivity toward FOL at nearly 100% conversion,whereas Ni/TiO2 achieved only 38% under the identical condition.Combined experimental and theoretical studies revealed that the enhanced catalytic performance of Ni/Fe-TiO2 originates from the dilution of contiguous Ni sites by Fe,which suppresses the further hydrogenation of FOL.Moreover,Fe sites exhibited a stronger affinity for carbonyl groups compared to Ni(0),indicating complementary role where Ni(0)primarily facilitates H2 dissociation,while Fe sites play a critical role in carbonyl activation.These findings underscore the superior synergistic effect of bimetallic systems in promoting selective functional group transformation.
基金Project(2024BAA012)supported by the Hubei Provincial Major Science and Technology Program,China。
摘要With the dramatic accumulation of the end-of-life lithium-ion batteries,their recycling is attracting extensive attention worldwide.To address the problem of low lithium recovery in the current typical hydrometallurgy recovery process,this research uses sodium bisulfate as an auxiliary roasting reagent to extract lithium from spent lithium-ion batteries through sulphation roasting,which can enhance the lithium recovery rate significantly.A systematic study of the sulphation roasting process and the mechanisms was carried out with experiments,thermodynamic calculations,and characterization of the roasted sample phases.The results showed that at a roasting temperature of 600℃,NaHSO4·H2O/spent LiNixCoyMnzO2 cathode powders(S-NCM)mass ratio of 1.2,and roasting time of 60 min,95% selective dissolution of lithium was acquired,while the leaching rates of Ni,Co,and Mn were confined under 1%.During roasting,the NCM layered structure collapses and the lithium is transformed into the LiNaSO4 phase,while the transition metals transform into Ni6MnO8 and MnCo2O4 phases.The removal of impurity ions from the lithium-rich leaching solution and the generation of Li2CO3 were achieved by a combination of thermodynamic calculations and experiments.
摘要Precisely controlling acid center position in zeolites is still challenging.Pentene monomolecular cracking offers an ideal route to maximize ethylene and propylene yields simultaneously.To reveal the relationship between acid site distribution in FER-zeolite and pentene monomolecular cracking activity,this study proposes a novel strategy integrating pyridine pre-adsorption with K+ exchange modification to selectively shield acid sites within FER cages,while phosphorus modification is employed to selectively passivate acid sites in 10-MR channels and on the external surface.Adsorption infrared(IR)spectroscopy(CD3CN-IR,Py-IR,and 2,6-DMPy-IR),and OH-IR characterization verified the selectivity and efficiency of these modification process.FER zeolites with distinct acid site distributions exhibit typical monomolecular cracking characteristics in pentene cracking,where the pentene cracking activity is linearly related to the acid density in the 10-MR channel and independent of the FER cage acidity.This result identifies 10-MR channel as primary pentene monomolecular cracking reaction position for the first time,providing a theoretical basis for designing zeolite catalysts that maximize ethylene and propylene production.The synergistic application of the pre-adsorption-K+exchange modiϐication strategy using different size basic molecules and phosphorus modification will provide an effective approach for precise control of acid site locations in zeolites with diverse pore/cavities architectures.
基金supported by the National Natural Science Foundation of China grant nos.52470149(P.H.Shao)and 52125002(X.B.Luo)the National Key Research and Development Program of China grant no.2023YFC3905903(P.H.Shao)Nanchang Hangkong University Doctoral Start-up Fund grant no.EA202502100(Y.Y.Zhou).
摘要Selective extraction of precious metals from urban mines plays a crucial role in mitigating the risk of depletion of precious metal resources and reducing waste pollution.However,a major obstacle in precious metal extraction lies in the difficulty of distinguishing the subtle differences in the physicochemical characteristics between them,especially gold and palladium.Herein,a proton-driven separation system was presented for cascade recovery of gold and palladium from waste-printed circuit boards(W-PCBs)leachate using poly(amidoxime)(PAO)hydrogel.This exhibits an ultra-high capacity,extra-fast rate,and excellent selectivity for the extraction of Au(Ⅲ)and Pd(Ⅱ).Notably,the separation of Au(Ⅲ)and Pd(Ⅱ)can be achieved with high selectivity at pH=0,resulting in a remarkable separation factor of kAu(Ⅲ/Pd(Ⅱ))=36.5.This was demonstrated to originate from the differential mechanism of PAO hydrogel for the capture of Au(Ⅲ)and Pd(Ⅱ)under proton-mediated conditions.Drawing inspiration from the mechanism,the proton-driven cascade recovery system demonstrates remarkable efficiency in sequentially recovering 99.92%of gold and 99.05%of palladium from W-PCBs acid leachate.This research opens up a strategy to precisely separate and recover precious metals from e-waste of urban mines.
摘要The oxygen evolution reaction suffers from sluggish kinetics and poor structural stability,necessitating the development of nonprecious metal electrocatalysts with efficient electronic regulation and intrinsic structural robustness.Herein,we construct a composite precatalyst of LaFe species modified cobalt carbonate hydroxide supported on nickel foam(LaFe–CoCH/NF)through a three-step process involving electrodeposition,hydrothermal growth,and co-deposition.This strategy enables the formation of a Ni–Co–Fe tri-level electron regulation pathway coupled with a spatially selective LaFe coating layer,achieving dual enhancement in both electronic modulation and structural stabilization.The hierarchical electron pathway effectively activates Ni sites within the nickel foam substrate,promotes the generation of high-valence Ni and Co species,and simultaneously suppresses the overoxidation of Fe.Meanwhile,the La-induced local electric field and buffering effect alleviate the detachment of the active phase during electrochemical reconstruction.As a result,the optimized LaFe–CoCH/NF catalyst exhibits outstanding oxygen evolution reaction performance,with a low Tafel slope of 33.75 mV dec-1 and exceptional durability,maintaining over 1500 h of stable operation at 10 mA cm-2,continuous operation for 1200 h at 50 and 100 mA cm-2,and more than 200 h of durability even at an ultrahigh current density of 500 mA cm-2.Mechanistic investigations reveal that the tri-metallic electron regulation strategy significantly improves interfacial charge transfer efficiency and structural integrity,offering theoretical guidance and a viable design route for advanced multi-metallic oxygen evolution reaction precatalysts.
基金supported by The National Natural Science Foundation of China(22471289 and 22478430)Shandong Natural Science Foundation(ZR2022ME105 and ZR2023ME004)+4 种基金Qingdao Natural Science Foundation(23-2-1-232-zyyd-jch)Geological body description and key technologies of reservoir engineering of CCUS oil displacement(2021ZZ01-03)Science and Technology Major Project on New Oil and Gas Exploration and Development:Research on Comprehensive Control Technology for CO2-Enhanced Miscible and Immiscible Displacement(2024ZD1406601)State Key Laboratory of Enhanced Oil Recovery of Open Fund Funded Project(2024-KFKT-19)the Fundamental Research Funds for the Central Universities(24CX06042A and 24CX06070A)。
摘要The rational design of high-performance CO2adsorbents remains a critical challenge in addressing global carbon emissions,with metal-organic frameworks(MOFs)emerging as promising candidates due to their tunable pore environments.However,the lack of systematic guidelines for functional group selection has hindered their practical implementation in carbon capture applications.Here,this gap was addressed by developing a comprehensive design framework through high-throughput computational screening.Through construction of a topology-directed database of 4797,integrating 10 metal centers with 144 functionalized ligands(18 ligands modified by–NH2,–NO2,–CH3,–CF3,–SH2,–SO2,–OH,and–OLi)across 36 topologies,the fundamental structure–property relationships governing CO2capture performance was established.Multi-metric evaluation reveals that–NO2,–SO2,and–OLi dramatically enhance CO2selectivity over CH_4/N2via selectivity(Sads),working capacity(ΔN),adsorbent performance score(APS),sorbent selection parameter(Ssp),and renewability R.Specially,ΔN rises from 2.34(pristine)to 5.91–7.94 mmol g-1and Sadssurges from 24.94/40.36 to 121.11/176.87(–NO2),149.94/215.54(–SO2),and 58.64/267.44(–OLi).Besides,the critical trade-off between adsorption strength and renewability demonstrates that enhanced performance comes at the cost of reduced renewability,where stronger CO2affinity(isosteric heat of-29.15,-29.96,and-30.09 for–NO2,–SO2,and–OLi)compromises renewability(R reduced by -50%).To resolve this trade-off,a novel energy efficiency(η)metric was introduced,which holistically evaluates both adsorption performance(Sads,ΔN,APS,Ssp,and R)and energy inputs(desorption heat,pressure-swing energy,net loss).This leads to the identification of–SO2as the optimal functional group that balances exceptional CO2capture(η=6.17/12.78 for CO2over CH_4/N2),surpassing the second higher of 4.74/8.80 in–CF3and 0.99/2.18 in non-functionalized counterparts.Adopting high-throughput computational screening methods,this work provides both fundamental insights into host–guest interactions in functionalized MOFs and a practical framework for designing next-generation adsorbents,bridging the gap between materials discovery and process engineering considerations in carbon capture technologies.
基金Supported by National Natural Science Foundation of China(22272172)Dalian High-Level Talent Innovation Support Program(2023RQ060)+1 种基金the fund of the State Key Laboratory of Catalysis in DICP(N-23-04)Guangzhou Municipal Science and Technology Bureau(2024A04J4679)。
摘要In this work,a Cu-based carbon catalyst(H-Cu/C)with an octahedral morphology was synthesized by pyrolyzing the metal-organic framework(MOF)precursor HKUST-1,where Cu(0)nanoparticles were uniformly dispersed in the carbon matrix,alongside the formation of island-like Cu2O structures as the active sites.Multiple characterization techniques,including XPS,XRD,SEM and HRTEM,reveal the critical role of carbon matrix in stabilizing the metal nanoparticles.In combination with TEMPO and using molecular oxygen as a green oxidant,the H-Cu/C catalyst is highly efficient in the selective oxidation of aromatic alcohols to the corresponding aldehydes under alkali-free conditions.Using benzyl alcohol as a model substrate,an alcohol conversion of 99.2%and a benzaldehyde yield of 94.1%were achieved under mild reaction conditions(100℃,0.5 MPa O2,1 h).The catalytic system displays excellent universality for various mono-and ortho/para-disubstituted aromatic alcohols,affording an alcohol conversion of over 99%and a yield of corresponding aromatic aldehydes of above 95%.In addition,the H-Cu/C catalyst can be regenerated via H2 reduction and reused without significant loss of activity.This work provides a new strategy for designing green and efficient non-noble metal catalytic systems for the oxidation reactions.
基金support from the Australian Research Council(ARC)Linkage Project(No.LP230100166).
摘要Selective depression of pyrite remains a major bottleneck in copper flotation,particularly when high-pyrite ores are processed and saline water is used.In such environments,conventional approaches using lime and inert grinding media often fail to discriminate ef-fectively between pyrite and valuable copper minerals due to strong copper activation on pyrite surfaces.This study introduced a novel approach using inorganic radicals generated from peroxymonosulfate(PMS)to selectively oxidize and depress pyrite.Flotation tests with synthetic high-pyrite ore blends showed that PMS significantly reduced pyrite recovery while maintaining or improving chalcopyrite flot-ation.Ethylenediaminetetraacetic acid(EDTA)extraction confirmed selective oxidation of pyrite,and electron paramagnetic resonance(EPR)spectroscopy identified hydroxyl(·OH)and sulfate(SO4·-)radicals as the dominant reactive species.Iron ions from grinding me-dia and mineral surfaces were identified as key activators of PMS.A major insight was pyrite’s dual role,acting both as a radical scav-enger and an activator,which made it highly reactive and susceptible to radical-induced oxidation.This process converted surface copper-sulfur species into copper hydroxides,effectively suppressing pyrite flotation.While previous studies have applied EPR to detect radicals in simplified activator/precursor systems,this study provides the first direct mechanistic evidence of radical-driven selectivity in flotation by detecting inorganic radicals in a complex flotation slurry,thereby demonstrating their persistence under industrially relevant conditions and establishing a foundation for more effective and targeted flotation strategies.
基金supported by the Natural Science Foundation of Hunan Province(No.2025JJ50059)Key Program of Hunan University of Arts and Science(No.23ZZ03)Aid Program for Science and Technology Innovative Research Team in Higher Educational Institutions of Hunan Province and National Natural Science Foundation of China(No.21303048).
摘要Cu electrocatalysts have been demonstrated to have unique ability to reduce CO2to various high value-added C2 products like ethylene and alcohols.However,realizing high selectivity of C2 products are still a main challenge due to complex CO2electroreduction pathways and small opportunity of C-C coupling reactions.Here,we found the origin of enhanced CO2electroreduction reaction activity and product selectivity towards C2 products and C-C coupling mechanism at halogen atoms-adsorbed Cu/H2O interfaces,the corresponding CO2electroreduction evolution mechanisms at the halogen atoms-modified Cu/H2O interfaces are systematically studied via theoretical modeling and calculations.The calculated results indicate that halide anions modifications are beneficial to CO dimerization into OCCO dimer,especially Cl--adsorbed Cu(111)/H2O interface has the optimum activity and selectivity towards OCCO dimer,subsequent Cl-adsorbed Cu(111)/H2O interface can selectively reduce CO2into C2H4 product.The function relationship between adsorption free energy of Cl atom and electrode potential explain why the adsorption of Cl-can enhance selectivity of C2H4 product.The determinations of onset potentials indicate that electroreduction pathways of CO2towards C2H4 product are facile to take place and further explain the origin of the significantly enhanced CO production activity and C2H4 product selectivity.This work on selective realization of CO2electroreduction towards C2H4 product via Cl--modified Cu(111)/H2O interface provide a theoretical guideline for how to selectively realize other high value-added C2 products.
基金financial support from the National Natural Science Foundation of China(Grant Nos.22472107 and 92145301)the Liaoning Science and Technology Plan Project(Grant Nos.2025-MSLH-620 and 2025-BS-0790)+1 种基金the scholarship for the subject development of Shenyang Normal University(Grant No.099-52501002)the Fundamental Research Funds for the Liaoning Universities(Grant Nos.LJ232410166032 and LJ202410166037).
摘要The selective oxidation of methane to formaldehyde presents a formidable challenge due to the inherent stability of methane and the tendency for overoxidation.Herein,we report core-shell structured 1%Cu/m-SiO2@TiO2-x catalysts designed to enhance catalytic performance for the selective oxidation of methane.The incorporation of a TiO2coating was found to play a critical role in modulating the dispersion of copper species and the surface chemical microenvironment.Characterization techniques revealed that the TiO2layer modulates the surface chemical environment,promoting the formation of Si-O-Ti interfaces and influencing the electronic interaction among Cu,Ti,and Si.The Si-O-Ti interface was identified as crucial for anchoring highly dispersed CuOxclusters,optimizing oxygen vacancy generation,and regulating reactive oxygen species.Consequently,this tailored interface suppressed the overoxidation of formaldehyde,leading to improved formaldehyde selectivity while maintaining comparable methane conversion.The optimized catalyst(1%Cu/m-SiO2@TiO2-1)achieved a formaldehyde yield of 1.3%at 700℃,with significantly improved selectivity compared with its unmodified counterpart(1%Cu/m-SiO2).This work highlights the importance of interface engineering in catalyst design and provides a viable strategy for developing efficient catalysts for the direct conversion of methane to formaldehyde.
摘要Background:Selective laser trabeculoplasty(SLT)is a first-line treatment for open-angle glaucoma(OAG)or ocular hypertension(OHT).However,the optimal SLT protocol remains unsettled.Randomized controlled trials(RCTs)comparing 180°and 360°SLT have yielded conflicting outcomes.This systematic review and meta-analysis aimed to determine which approach provides superior efficacy and safety.Methods:We searched PubMed,Embase,Cochrane,and Web of Science through November 8,2025 for RCTs comparing 180°with 360°SLT in OAG or OHT.We excluded conference abstracts.The primary outcome was intraocular pressure(IOP).Secondary outcomes included treatment success,visual acuity,and adverse events.We assessed the risk of bias with the Cochrane risk-of-bias tool for randomized trials,and estimated mean differences(MDs)and risk ratios(RRs)with 95%confidence intervals(CIs)using a randomeffects model.Trial sequential analysis(TSA)evaluated the robustness of evidence.Results:We included six studies comprising 892 eyes.180°SLT was associated with higher IOP at 1 month(MD 1.17 mmHg;95%CI:0.52–1.81;P<0.01;I2=36%),3 months(MD 0.96 mmHg;95%CI:0.45–1.47;P<0.01;I2=0%),6 months(MD 1.03 mmHg;95%CI:0.14–1.92;P=0.02;I2=58%),and 12 months(MD 1.63 mmHg;95%CI:0.66–2.60;P<0.01;I2=0%).Treatment success(RR 0.72;95%CI:0.58–0.90;P<0.01;I2=50%)and pain or discomfort rates(RR 0.63;95%CI:0.50–0.81;P<0.01;I2=0%)were lower with 180°SLT.There was no difference between groups in visual acuity(MD−0.002 logMAR;95%CI:−0.029 to 0.026 logMAR;P=0.90;I2=41%)and adverse events risk(RR 1.08;95%CI:0.69–1.68;P=0.75;I2=0%).TSA showed robust evidence for the superiority of 360°vs.180°SLT on IOP.Conclusions:180°SLT was inferior to 360°SLT for IOP control and treatment success in OAG or OHT,yet it was associated with a lower risk of pain or discomfort.These findings support 360°SLT as the preferred protocol,though evidence is limited by the number of trials,heterogeneity,and follow-up.Highquality,long-term RCTs are required to validate these findings.
基金Supported by Strategic Priority Research Program of the Chinese Academy of Sciences(XDB 1190000)the General Program of the National Natural Science Foundation of China(22572209)。
摘要Cyclohexene is an important raw material for nylon production,and the selective hydrogenation of benzene is a key route for preparing cyclohexene.To promote data sharing and reuse in this field,we collected and standardized experimental data on the hydrogenation of benzene to cyclohexene from publicly available literature and constructed a comprehensive dataset containing catalyst composition,reaction conditions,and reaction results(conversion,selectivity and yield).This data descriptor details the source,field definitions,generation and processing workflow,quality control,sharing approach and usage recommendations of the dataset,with the aim of providing a reusable data foundation for subsequent statistical analysis,machine learning modeling,experimental design,and catalyst screening.
基金financially supported by the Natural Science Foundation of Gansu Province,China(No.21JR7RA478).
摘要Carbon-chain rubbers have been widely used in many fields including transportation,medicine,construction,and everyday life,owing to their excellent flexibility.Now,waste rubbers have caused serious environmental pollution and resource waste.Chemical recovery is expected to provide a solution to solve these problems fundamentally.Here,the recent progress in selective chain scissions of the waste sulfur-vulcanized carbon-chain rubbers for reuse was reviewed.Based on the different devulcanization approaches,the polysulfide crosslinking chains or carbon chains were broken and the linear or branched degraded products could be obtained as structural prepolymers for new rubber products.After a comprehensive literature review on the effect of the molecular composition and topology of the devulcanized and degraded products on the new rubbers,the future perspectives were proposed.