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Dynamic evolution of copper-based catalysts during CO2 electroreduction 认领 引用 被引量：2
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作者 Zhizheng Wu Pengpeng Yang Minrui Gao 《Nano Materials Science》 EI CAS CSCD 2026年第3期687-702,共16页
The CO2 electroreduction reaction(CO2RR)is a promising approach of using renewable electricity to synthesize fuels and value-added chemicals.At present,Cu is generally considered to be the major monometallic cat... The CO2 electroreduction reaction(CO2RR)is a promising approach of using renewable electricity to synthesize fuels and value-added chemicals.At present,Cu is generally considered to be the major monometallic catalyst capable of producing multicarbon products(C2+)with high current densities from the CO2RR,but it still suffers from the low activity and high overpotential.The challenge of sluggish CO2RR kinetics can be overcome by developing efficient Cu-based catalysts,which undergo the dynamic evolution during the reaction process.The dynamic evolution of the Cu-based catalysts taking place under working conditions makes it difficult to study the structure-activity correlation and reaction mechanism present during CO2RR.Recently,a number of important works have observed and revealed the dynamic evolution process of Cu-based catalysts by operando characterization techniques.This aspect,however,remains less summarized and prospected in the CO2RR literature.In this Review,we summarize the dynamic evolution of Cu-based catalysts during the CO2RR from aspects of structure,composition and oxidation state.We highlight the correlations between evolution behaviors and catalytic properties.Then,we discuss the dynamic deactivation process of Cu-based catalysts during CO2RR,including metal impurities contamination and carbon accumulation.In particular,we introduce recent advancements in in situ characterization techniques those are employed to probe the dynamic evolution under operating conditions.We end the Review by outlining the challenges and offering personal perspectives on the future development opportunities in this field. 展开更多
关键词 Copper-based catalysts CO2electroreduction reaction Dynamic evolution
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Rare earth single atom supported on C2N catalysts for electrochemical CO2reduction:A DFT study 认领 引用
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作者 Yu Ren Qiannan Zhou +4 位作者 Xiaofei Song Yangyang Song Zean Xie Xuehua Yu Zhen Zhao 《Journal of Rare Earths》 SCIE EI CAS CSCD 2026年第4期1085-1090,I0004,共6页
The electrochemical CO2reduction reaction(CO2RR)can convert CO2into high value-added chemicals,which is conducive to improving climate change and energy crisis.Rare earth single-atom catalysts(SACs)have recen... The electrochemical CO2reduction reaction(CO2RR)can convert CO2into high value-added chemicals,which is conducive to improving climate change and energy crisis.Rare earth single-atom catalysts(SACs)have recently been widely studied in the field of CO2reduction due to their unique properties.Herein,a series of rare earth single-atom metals(abbreviated as RM,which are Sc,Y,La,Ce,Pr,Nd,Sm,Eu,Gd,Tb,Dy,Ho,Er,Tm,Yb,Lu)supported on C2N were designed and systematically studied for their CO2RR performance.Results show that CH4is the main product on RM@C2N and the limiting potentials are in range of-0.46 to-0.61 V except for Eu@C2N and Yb@C2N.Among them,Tb@C2N,Sm@C2N,and Gd@C2N show high activity and selectivity with limiting potentials of-0.46,-0.47,and-0.48 V.The binding energy of adsorbed oxygen atoms on rare earth SACs can be used as a good descriptor of activity from volcano plot.These results provide insights into the design of rare earth catalysts for CO2RR and valuable guidance for screening single-atom catalysts in theory. 展开更多
关键词 CO2electroreduction Single-atom catalysts Rare earths Density functional theory C2N
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Chemically stable TMOx@Ti-MgO(TM=Mn and Cu)catalyst enhanced De/hydrogenation kinetics of Mg/MgH2 认领 引用
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作者 Haotian Guan Jiang Liu +2 位作者 Qian Li Yangfan Lu Fusheng Pan 《Journal of Magnesium and Alloys》 SCIE EI CAS CSCD 2026年第2期276-284,共9页
Ti-based catalysts have been identified to be efficient in enhancing hydrogenation and dehydrogenation(de/hydrogenation)kinetics of Mg/MgH2.However,their catalytic activity is constrained by the strong Ti-H bond an... Ti-based catalysts have been identified to be efficient in enhancing hydrogenation and dehydrogenation(de/hydrogenation)kinetics of Mg/MgH2.However,their catalytic activity is constrained by the strong Ti-H bond and chemical instability.Herein,we demonstrate that TMOx@Ti-MgO(TM=Mn and Cu)composite catalysts can simultaneously enhance hydrogen dissociation,diffusion and nucleation processes.MgH2 catalyzed by TMOx@Ti-MgO released 6.03-6.14 wt.%H2 within 5 min at 280℃ and 0.89-1.12 wt.%H2 within 60 min at 180℃.The partially oxidized Ti2+and Ti3+states are stabilized in MgO lattice,accelerating hydrogen adsorption,dissociation and diffusion processes.The TMOx,additionally,serve as the active center for nucleation,further improving de/hydrogenation reactions.The TMOx@Ti-MgO catalysts are characterized by high chemical stability,realizing improved cycle properties.These findings suggest a new approach to achieving controllable Catalyst-Hydrogen bond strengths and optimizing performance in de/hydrogenation reactions. 展开更多
关键词 Ti-based catalyst Mg/MgH2 hydrogen storage hydrogen diffusion nucleation
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The role of copper valence states in CuZnAl catalysts for CO2-to-methanol conversion 认领 引用
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作者 QIU Zhengpu XU Yunzhao +11 位作者 WANG Peng TAO Xiaoxia ZHANG Huimin CHEN Yang LIU Yi YANG Hua CAO Fenghai FU Yajie WU Lizhi TANG Yu XU Xiaoying TAN Li 《燃料化学学报（中英文）》 EI CAS CSCD 北大核心 2026年第4期58-67,共10页
CuZnAl(CZA)is a classic industrial catalyst widely used for the synthesis of methanol from syngas,but its catalytic performance is not optimal for the hydrogenation of CO2 to methanol.Meanwhile,understanding the ca... CuZnAl(CZA)is a classic industrial catalyst widely used for the synthesis of methanol from syngas,but its catalytic performance is not optimal for the hydrogenation of CO2 to methanol.Meanwhile,understanding the catalytic mechanism of Cu species in the CZA catalyst remains a great challenge.In this study,we systematically investigated the valence state change of active Cu species in CZA catalyst and their influence on catalytic performance by modifying the catalysts with varying amounts of electron donor K,thus identifying the catalytic function of Cu species with different valence states.H2-TPR,XPS and HR-TEM characterizations reveal that the highly dispersed K species supported on CZA catalysts will inhibit the reduction of CuO,resulting in a small amount of Cu2O active species being produced under reaction conditions thus causing a decrease in catalytic activity.Furthermore,XRD and Cu LMM spectra show that the proportion of Cu0 in K-modified CZA catalysts increases with K loading,but a higher proportion of Cu0 species on the surface obviously promotes the reverse water gas shift(RWGS)reaction.According to the results of in situ infrared spectroscopy,CZA catalyst follows the reaction pathway mediated by HCOO*in the hydrogenation of CO2 to methanol. 展开更多
关键词 CO2hydrogenation CuZnAl catalysts methanol active species electronic promoter
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Tunable C2selectivity in CO electroreduction via charge-asymmetric dual-metal catalysts on ferroelectric In2Se3 认领 引用
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作者 Dongqiu Zhao Xiao Tang +5 位作者 Yixin Zhang Shuli Liu Di Yuan Chen Long Lin Ju Liangzhi Kou 《Frontiers of physics》 SCIE CSCD 2026年第6期91-100,共10页
The development of efficient catalysts for the electrocatalytic CO reduction reaction toward high-value C2products is critical for addressing pressing energy and environmental challenges.Dual-metal catalysts have e... The development of efficient catalysts for the electrocatalytic CO reduction reaction toward high-value C2products is critical for addressing pressing energy and environmental challenges.Dual-metal catalysts have emerged as promising candidates due to their potential to facilitate C−C coupling,a key step in C2product formation.However,their activity and selectivity are highly dependent on the charge states of the active sites.Modulating asymmetric charge distribution between metal centers offers a viable strategy to enhance C−C coupling efficiency and product selectivity.In this study,we employ density functional theory to investigate heteronuclear dual-atom catalysts(DACs)anchored on ferroelectric In2Se3and impact of polarization on charge states of metal sites.We find that Pd−Nb and Rh−Nb DACs form spatially separated charge centers with opposite signs,which significantly reduce the energy barrier for C−C coupling compared to homonuclear Nb−Nb DACs,enabling thermodynamically favorable C−C bond formation.The Coulomb interaction between oppositely charged centers is identified as a key descriptor governing C−C coupling efficiency.Furthermore,ferroelectric polarization switching of In2Se3offers dynamic modulation of reaction pathways and product selectivity.Pd−Nb@In2Se3under downward polarization(P↓)favors ethane formation with a limiting potential of−1.06 eV,whereas upward polarization(P↑)shifts the reaction toward an alternative C−C coupling pathway with a higher overpotential(−1.47 eV).Similarly,Rh−Nb@In2Se3selectively produces ethanol under P↓,but methane under P↑.Importantly,both Pd−Nb and Rh−Nb DACs exhibit stronger CO adsorption than H adsorption,favoring CORR over the competing hydrogen evolution reaction.These findings underscore the potential of ferroelectric DACs as tunable and selective catalysts for CORR,offering a compelling strategy for the rational design of next-generation electrocatalysts for decarbonization. 展开更多
关键词 electrocatalysis CO reduction reaction dual-atom catalysts polarization switch C2product
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One-pot synthesis of mesoporous NiCe/Al2O3catalysts for enhanced carbon dioxide methanation performance 认领 引用
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作者 Yanyan Feng Yongge Liu +2 位作者 Xinglian Yu Juanjuan Liu Wen Yang 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2026年第2期135-145,共11页
The hydrogenation of carbon dioxide(CO2)to methane(CH4)has become an effective strategy for reducing greenhouse gas emissions due to its high efficiencyand low cost,and ordered mesoporous materials have received... The hydrogenation of carbon dioxide(CO2)to methane(CH4)has become an effective strategy for reducing greenhouse gas emissions due to its high efficiencyand low cost,and ordered mesoporous materials have received considerable interest in CO2methanation applications because of their large specificsurface area and well-ordered pore structure.Herein,a series of the Ce-modifiedordered mesoporous catalysts(NiCe/Al2O3)were prepared through a one-pot approach,and the influenceof Ce doping on the morphology and structure of the catalysts as well as the CO2methanation performance were investigated in detail.The XRD and TEM data revealed that the introduction of Ce could effectively lower the particle size of Ni active components and advance the dispersion of Ni species.The H2-TPR profilesdemonstrated that Ce doping facilitated the catalyst's reduction by greatly decreasing its reduction temperature.In addition,the CO2-TPD and XPS data indicated that the incorporation of Ce provided sufficientbasic sites for CO2activation and adsorption,and the oxygen vacancies of the Cedoped Ni-based catalysts were significantlyenhanced.Obviously,the catalyst 30Ni10Ce/Al2O3achieved the outstanding catalytic performance,achieving CO2conversion of 90.7%and CH4 selectivity of 99.8% at 375℃,and even after 60 h of continuous reaction,it still maintained the stable catalytic activity,which suggested that the Ce-doped Ni-based catalysts can offer significantpromising applications in CO2methanation. 展开更多
关键词 CO2methanation Ni-based catalyst Mesoporous Al2O3 Ce doping Oxygen vacancy
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Hydrogen-driven metal-support interaction in Ni-CeO2 catalysts boosting low-temperature CO2 methanation 认领 引用
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作者 Ru Zhao Siyuan Xu +5 位作者 Junliang Xia Mingxue Wang Xiaoyan Han Yu Xie Qiulin Zhang Ping Ning 《Journal of Rare Earths》 SCIE EI CAS CSCD 2026年第7期2097-2105,I0004,共9页
Converting CO2 to CH4 under mild conditions represents a promising strategy for carbon emission reduction and synthetic natural gas production,yet it remains challenging.In this work,we accelerated low-temperatu... Converting CO2 to CH4 under mild conditions represents a promising strategy for carbon emission reduction and synthetic natural gas production,yet it remains challenging.In this work,we accelerated low-temperature CO2 hydrogenation over Ni-CeO2 catalysts by optimizing metal-support interactions through H2-driven reconstruction.The catalyst reduced at 400℃(Ni-CeO2-400R)achieved 84.3%CO2conversion with 100%CH4 selectivity even at a low temperature of 250℃.Various in situ spectroscopic characterizations(X-ray photoelectron spectroscopy(XPS),Raman,and diffused reflectance infrared Fourier transform spectroscopy(DRIFTS))and H2/D2 isotopic exchange experiments reveal that the appropriate interaction in Ni-CeO2 motivates the dispersion of metallic Ni sites and the generation of oxygen vacancies,thereby promoting the activation of H2 and CO2 molecules,respectively.Therefore,CO2 is efficiently adsorbed and converted into reactive intermediates and finally hydrogenated to CH4through carbonyl and formate pathways simultaneously.These findings underscore the critical role of tailored metal-support interactions in designing advanced CO2 hydrogenation catalysts. 展开更多
关键词 Low-temperature CO2methanation Ni/CeO2catalysts H2treatment Metal-support interaction Rare earths
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CO2hydrogenation to methanol on the incapsulated Cu-Zn catalyst:Effect of the MCM-41 and SBA-15 supports and the method of preparation on catalytic activity 认领 引用
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作者 Anastasiya Shesterkina Christina Zhdanova +5 位作者 Nikolay Davshan Artem Medvedev Konstantin Kalmykov Sergey Dunaev Leonid Kustov Alexander Kustov 《Green Synthesis and Catalysis》 CSCD 2026年第3期328-336,共9页
The catalytic conversion of carbon dioxide to methanol is of great practical and scientific importance in the concept of reducing CO2emissions.Moreover,it can partially solve the problem of human dependence on non-... The catalytic conversion of carbon dioxide to methanol is of great practical and scientific importance in the concept of reducing CO2emissions.Moreover,it can partially solve the problem of human dependence on non-renewable resources.The development of selective and active catalysts for CO2hydrogenation is a key point due to the strong thermodynamic limitations and high chemical stability of CO2.In this work,the influence of the nature of the mesoporous supports,as well as the method of introducing the active component,on the catalytic properties of Cu–Zn catalysts in the CO2hydrogenation to methanol were investigated.A series of bimetallic Cu-Zn catalysts deposited on mesoporous MCM-41 and SBA-15 supports were prepared by two methods:encapsu-lation and incipient wetness impregnation.The obtained catalysts were characterized by N2adsorption,X-ray diffraction(XRD),scanning electron microscopy-energy dispersive X-ray spectroscopy(SEM-EDX),and ther-mogravimetry-differential thermal analysis(TG-DTA)methods.The highest CO2conversion and methanol space-time yield were observed over the encapsulated Cu–Zn catalyst based on the MCM-41 support.The optimal process temperature was 280℃,at which a high selectivity of 92%methanol formation was achieved while maintaining the best CO2conversion.The study demonstrates the prospects of using bimetallic Cu-Zn catalysts encapsulated in MCM-41 for direct CO2hydrogenation for“green”methanol production. 展开更多
关键词 CO2hydrogenation Cu-Zn catalyst Methanol MCM-41 SBA-15
Size-Dependent Hydrogen Dissociation Capacity in Ni/CeO2 Catalysts for Low-Temperature CO2 Methanation 认领 引用
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作者 Yu Xie Zhiyu Li +6 位作者 Xiaoyan Han Mingxue Wang Ru Zhao Siyuan Xu Qiulin Zhang Ping Ning Jiming Hao 《Rare Metals》 SCIE EI CAS CSCD 2026年第2期718-732,共15页
Converting CO2to CH4 under mild conditions is a promising strategy for solving environmental and energy problems,but also a challenge.In this work,the low-temperature CO2 hydrogenation process over Ni/CeO2 ca... Converting CO2to CH4 under mild conditions is a promising strategy for solving environmental and energy problems,but also a challenge.In this work,the low-temperature CO2 hydrogenation process over Ni/CeO2 catalysts was significantly accelerated by optimizing the H2 dissociation ability of Ni through the size effect,thus A-Ni/CeO2 with an average size of 4.9 nm achieved 83.4%CO2conversion with~100%CH4 selectivity even at 225℃.Systematic H2/D2 isotopic exchange experiments,in situ spectroscopic characterizations,and density functional theory(DFT)calculations reveal that the enhanced H2 activation ability not only promoted the creation of oxygen vacancies and hydroxyl group favorable for CO2 adsorption/activation in the pre-reduction process,but also the simultaneous hydrogenation of reactive intermediates belonging to carbonyl and formate pathway into CH4 in the reaction process.This fundamental understanding of the H2 dissociation effect on CO2 activation and hydrogenation provides critical insights for designing catalysts with considerable low-temperature activity,which significantly reduces energy consumption and operating costs for industrial CO2 conversion. 展开更多
关键词 CO2activation H2dissociation low-temperature CO2methanation Ni/CeO2catalysts size effect
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Anion-regulated reconstruction of bismuth-based electrocatalysts for enhanced electrocatalytic CO2 reduction 认领 引用
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作者 Lili Wang Bangwei Deng +5 位作者 Hongtao Xie Xianlong Lu Pengcheng Xiang Xueyang Zhao Yizhao Li Fan Dong 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2026年第2期598-609,I0014,共12页
Elucidating the active site formation mechanism of bismuth(Bi)-based catalysts in electrochemical CO2reduction remains challenging for achieving high activity,selectivity,and long-term stability.Here we confirm thr... Elucidating the active site formation mechanism of bismuth(Bi)-based catalysts in electrochemical CO2reduction remains challenging for achieving high activity,selectivity,and long-term stability.Here we confirm through experimental results that Bi-based catalysts containing halogen ions(I-,Cl-,Br-)and SO42-maintain the system stability,keeping Faraday efficiency of formic acid above90%in the current range of 50-800 mA cm-2.In contrast,anions containing S2-and NO3-in the electrolyte can be reduced to produce by-products.These anions and their by-products could poison the active center,leading to increased side reactions and thus significantly reducing the Faraday efficiency of formic acid.The combination of non-in situ and in situ characterization results revealed that the Bi-based catalysts all underwent the transition from the initial state to the Bi/Bi2O2CO3(BOC)intermediate state in high-concentration KHCO3 solution,and the different anions could selectively modulate the degree of exposure of specific crystalline surfaces of BOC.At the late stage of the reaction,BOC was completely converted to metal Bi and became the real active center.Combined with in situ IR and DFT calculations,it is further verified that*OCHO is the key intermediate on the metallic Bi surface,which is most favorable for formic acid formation.This study reveals the key mechanism by which anions affect the formation of active sites via modulating the catalyst reconstruction process,which provides an important theoretical basis for the design and optimization of test conditions of Bi-based catalysts. 展开更多
关键词 Bismuth-based catalysts Surface reconstruction Electrocatalytic CO2reduction Anion effects In situ spectroscopy
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Cu-Based Catalysts Design Toward Electrochemical CO2 Reduction to Valuable Multi-Carbons Products 认领 引用
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作者 Li‑Qing Li Min‑Xiao Huang +3 位作者 Hong Ke Wei‑Wei Zhu Jing‑Hua Zhao Li‑Hua Zhu 《Rare Metals》 SCIE EI CAS CSCD 2026年第4期284-303,共20页
Electrochemical reduction of CO2 to multi-carbon products(e.g.,C2+ ,ethene,ethanol,etc.)not only effectively decreases the CO2 concentration in atmosphere but also shows great potential economic benefits due ... Electrochemical reduction of CO2 to multi-carbon products(e.g.,C2+ ,ethene,ethanol,etc.)not only effectively decreases the CO2 concentration in atmosphere but also shows great potential economic benefits due to these exploitable value-added products.The Cu-based catalysts have caught much attention in CO2 electroreduction due to the good selectivity to hydrocarbons products.However,designing appropriate Cu-based catalysts is desirable to further improve the energy efficiency and selectivity of specific C2+ product.In this review,primary pathways of CO2 electroreduction to C2+ products are first discussed to summarize the key elementary steps of C2+ products formation.Subsequently,various strategies of catalytic activity regulation of Cu-based catalysts are classified into geometric and electronic structures modification based on the inner correlation between these strategies and the mechanism of C2+ products formation.The review ends with a cross-scale perspective that links the selectivity enhancement of a specific C2+ product and the target design of Cu-based catalysts. 展开更多
关键词 catalytic activity regulation Cu‑based catalysts electrochemical CO2reduction
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Reactive CO2 capture electrolysis at low voltage and high single-pass conversion enabled by ultra-low loading molecular catalyst 认领 引用
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作者 Yuming Wu Guohao Li +7 位作者 Mengxin Liu David Inglis Yasuhiro Sakamoto Lizhuo Wang Zhiqiang Zhao Catherine Stampfl Feng Jiao Yijiao Jiang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2026年第6期728-737,I0018,共10页
Integrating electrochemical CO2 conversion with carbon capture extends the CO2 source beyond pure or point-source streams.By directly interfacing with capture units,reactive CO2 capture electrolysis circumven... Integrating electrochemical CO2 conversion with carbon capture extends the CO2 source beyond pure or point-source streams.By directly interfacing with capture units,reactive CO2 capture electrolysis circumvents the energy-intensive regeneration and compression processes to supply pure CO2 stream,also minimizes the amount of unreacted CO2 through gas-fed CO2 electrolysis.However,the conversion pathway is hampered by high electrolyser voltages and reliance on precious and thick metal catalysts(>2.0 mg cm-2).Here,we report an energy-efficient reactive CO2 capture electrolysis system enabled by an ultra-low loading molecular catalyst(cobalt phthalocyanine anchored onto multi-walled carbon nanotubes,Co Pc/CNT).When the Co Pc/CNT exceeds 0.2 mg cm-2loading on cathode,the thicker Co Pc/CNT layer largely increase electrical and mass transfer resistances.This limits the availability of local CO2 at the catalyst surface,suppressing the formation of adsorbed intermediates(COOH*/CO*)on cobalt centres,as observed by operando Raman spectroscopy.Benefiting from the features,the electrolysis system achieves a single-pass CO2 conversion of 55.1%at 300 m A cm-2 and a faradaic efficiency of CO(FECO)84.7%at a 0.2 mg cm-2.At 100 m A cm-2,the synergistic combination of Co Pc/CNT with a two-layer membrane architecture reduces electrolyser voltage by 30%to widely used bipolar membrane(BPM)-incorporated electrolyser and 17%voltage to metal catalyst-based cathode.This study offers a costeffective molecular catalyst for reactive CO2 capture electrolysis and paves the way for energy-efficient carbon capture and utilisation integrated systems. 展开更多
关键词 Reactive CO2capture Bicarbonate electrolysis CO2capture and utilization Cobalt phthalocyanine Low catalyst loading High conversion yield
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Direct synthesis of long-chain primary alcohols from syngas over Na-driven Co2C-Co catalyst 认领 引用
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作者 Zheng Li Ziang Zhao +7 位作者 Yihui Li Yuan Lyu Li Yan Wenhao Cui Shunbin Zhu Yu Meng Hejun Zhu Yunjie Ding 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2026年第6期371-383,共13页
The direct synthesis of high-value-added long-chain primary alcohols(LPAs,C6+OH)from syngas(CO+H2)is highly attractive.However,low selectivity of targeted products is generally obtained due to competitive dissoc... The direct synthesis of high-value-added long-chain primary alcohols(LPAs,C6+OH)from syngas(CO+H2)is highly attractive.However,low selectivity of targeted products is generally obtained due to competitive dissociative and non-dissociative CO adsorption,as well as uncontrollable chain growth that causes a complex reaction network.Herein,we report that Na-driven Co2C-Co dual active sites could be engineered by loading the Na promoter onto an activated carbon supported Co-based catalyst,achieving total alcohol selectivity of ca.46%with a remarkable LPAs fraction higher than 65%,which represents the first report of high LPA selectivity in literature.Comprehensive characterizations and experiments indicated that electron-rich state of Co2C-Co sites was generated through Na promotion,which enhances the surface basicity of the catalyst and favors chain propagation.Moreover,Na promotes the dissociation of CO to form*C species,facilitating the transformation of metallic Co into Co2C and leading to the formation of Na-driven Co2C-Co active sites that are closely associated with CO insertion.Density functional theory calculations show that Na significantly also promotes C-C coupling while inhibiting hydrogenation and promoting CO insertion,which is deemed to be the intrinsic mechanism behind the high LPAs selectivity.This work elucidates a dual role of Na in constructing active sites and modulating surface reaction energetics,providing a design paradigm to break the LPAs selectivity barrier in syngas conversion. 展开更多
关键词 Syngas conversion Alkali metal Na-driven Co2C-Co catalyst Long-chain primary alcohols Structure-performance relationship
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Core-shell Pd@CeO2/γ-Al2O3 catalysts:Boosting efficiency and durability in stoichiometric natural gas vehicle exhaust treatment 认领 引用
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作者 Run Pan Abubakar Yusuf +10 位作者 Chengjun Wang Jianrong Li Zhiyu Xiao Shuai Liu Yidong Zhong Yong Ren Zheng Wang Hainam Do John L.Zhou George Zheng Chen Jun He 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2026年第3期348-362,共15页
Natural gas vehicles(NGVs)offer significant environmental advantages by reducing pollutant emissions,but effective exhaust treatment remains a challenge due to high methane emissions and catalyst deactivation over tim... Natural gas vehicles(NGVs)offer significant environmental advantages by reducing pollutant emissions,but effective exhaust treatment remains a challenge due to high methane emissions and catalyst deactivation over time.This study introduces a core-shell Pd@CeO2/Al2O3 three-way catalyst(TWC)designed to enhance the efficiency and durability of NGV exhaust treatment.The core-shell structure significantly improves catalytic performance.The optimized Pd@Ce/Al(S-500)catalyst demonstrates excellent low-temperature activity,with T50 values of 336℃ for CH4 and 397℃ for NO.It also achieves remarkable reductions of 113 and 177℃ in the T90 for CH4 and NO conversion,respectively,compared to the non-core-shell counterpart,Pd-Ce/Al(S-500).Characterizations reveal enhanced metal-support interactions,increased oxygen vacancies,and optimized Pd-CeO2 interfaces as key active sites.Density functional theory calculations further demonstrate that the core-shell structure facilitates electron transfer at Pd-CeO2 interfaces and lowers energy barriers for three-way reactions,enhancing catalytic efficiency.Notably,the core-shell Pd@Ce/Al(S-500)catalyst maintains high conversion efficiency for CH4 and NO,with only slight losses(5.5% and 6.6%,respectively)over a 100-h time-on-stream stability test,following 16 h of harsh hydrothermal aging at 800℃,showcasing its long-term stability.These findings provide a deeper understanding of the role of the core-shell Pd@CeO2 structure in Pd-based TWCs and offer valuable insights for designing durable and efficient catalysts to meet the stringent emission standards of NGVs. 展开更多
关键词 Core-shell catalyst Pd@CeO2/Al2O3 Natural gas vehicles Stoichiometric combustion Three-way catalysis Hydrothermal stability
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Tri-functional Ru catalyst drives efficient ammonia synthesis from N2 and H2O 认领 引用
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作者 Ying Hou Wei Hu +6 位作者 Qiao Zhao Yuchuan Tu Guang Yang Yi Cui Wei Liu Liang Yu Dehui Deng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2026年第7期769-775,I0018,共7页
1.Indroduction In light of the global transition toward carbon neutrality,the development of mild-condition ammonia synthesis technologies has gained significant attention as a promising solution to address the inhere... 1.Indroduction In light of the global transition toward carbon neutrality,the development of mild-condition ammonia synthesis technologies has gained significant attention as a promising solution to address the inherent limitations of the traditional Haber-Bosch approach,which remains highly energy-intensive due to the extreme operation conditions(above 350℃ and over 10 MPa)required to activate the robust N≡N bond(945 kJ mol-1).Furthermore,the process is carbon-intensive,as its primary hydrogen source is derived from hydrocarbon reforming with high carbon emissions[1,2]. 展开更多
关键词 NH3 synthesis N and H2O Tri-functional Ru-based catalyst Reversible Li battery
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Preparation and electrochemical performance of nitrogen-doped carbon-coated CuxS nanobox catalyst for hybrid Na-CO2 batteries 认领 引用
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作者 Jing ZHAN Zi-zhuo HUA +1 位作者 Fei-xiang WU Qi-hou LI 《Transactions of Nonferrous Metals Society of China》 SCIE EI CAS CSCD 2026年第3期929-942,共14页
To promote CO2redox kinetics on the cathode of hybrid sodium-carbon dioxide(Na-CO2)batteries,hollow cubic CuS nanoboxes were encapsulated in polypyrrole and polydopamine by in situ polymerization of pyrrole and ... To promote CO2redox kinetics on the cathode of hybrid sodium-carbon dioxide(Na-CO2)batteries,hollow cubic CuS nanoboxes were encapsulated in polypyrrole and polydopamine by in situ polymerization of pyrrole and dopamine monomers,respectively,and coupled with high-temperature heat treatment to obtain nitrogen-carbon encapsulated CuxS@NCPPyand CuxS@NCPDA catalysts.The results show that the encapsulation of nitrogen-doped carbon not only increases the specific surface area and improves the electron affinity but also promotes the synergistic interaction between the CuS-based active species and the defect carbon,thus providing abundant active sites for CO2conversion.The electrochemical performances of the carbon-coated modified samples were all improved,especially the hybrid Na-CO2battery based on CuxS@NCPPy,which showed a low voltage gap of 0.74 V at 0.1 mA/cm2and a high power density of 3.42 mW/cm2. 展开更多
关键词 CO2reutilization copper(I)sulfide catalyst nitrogen-doped carbon high power density Na-CO2batteries
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Synergistic confinement and alloying effects in Pd-based catalysts for efficient and stable CO2reduction 认领 引用
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作者 Yujun Cheng Xi Li +6 位作者 Ziyi Gao Yao Yao Chuan Long Jiasi Zuo Haikun Xu Qi Liu Xiaoqing Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2026年第7期1-11,I0002,共11页
Palladium(Pd)has long been constrained as a potential catalyst for CO2reduction reactions(CO2RR)due to significant deactivation caused by strongly adsorbed carbonaceous intermediates on its surface,severely limi... Palladium(Pd)has long been constrained as a potential catalyst for CO2reduction reactions(CO2RR)due to significant deactivation caused by strongly adsorbed carbonaceous intermediates on its surface,severely limiting its catalytic activity and stability.To address this critical bottleneck,this study proposes and implements a synergistic regulation strategy combining alloying and spatial confinement effects.This approach designs a composite catalyst by encapsulating boron-silver co-doped palladium alloy nanoparticles(B-Ag4Pd6)within hollow porous resin carbon spheres(HPRCS).In an H-cell,this catalyst achieved a CO Faradaic efficiency of 96.19%at jCO=24.8 mA/cm2 and maintained stable performance for 80 h.Even under flow cell conditions,it sustained 91.23%CO selectivity at jCO=157.86 mA/cm2 over 60 h.Experimental comparisons confirmed the significant promoting effect of spatial confinement on CO2RR.Furthermore,in situ ATR-FTIR spectroscopy and density functional theory(DFT)calculations reveal that B/Ag alloying downshifts the Pd d-band center,optimizes(*)^COOH and(*)^CO adsorption,and the confined Hmicroenvironment accelerates CO formation while suppressing hydrogen evolution.This study not only successfully addressed the issue of carbon intermediate poisoning on Pd surfaces through alloying and microenvironmental regulation,but also provides novel insights and approaches for designing high-performance CO2RR catalysts that integrate electronic structure control with microenvironmental engineering. 展开更多
关键词 CO2electroreduction Pd‑based alloy catalysts Confinement effect Interfacial microenvironment engineering
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Thermally Driven Hydrogenation of CO2 to Light Olefins Over Hollow Cubic In2O3-La-ZIF-8 Tandem Catalyst 认领 引用
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作者 Haifeng Tian Haowei Huang +8 位作者 Zhiyu Chen Fei Zha Hongshan Chen Ruiying Ding Yu Zhang Hao Wei Yuzhong Mao Irshad Hussain Zhicheng Zhang 《Rare Metals》 SCIE EI CAS CSCD 2026年第4期471-485,共15页
Thermally driven hydrogenation of CO2 to light olefins(C2=-C4=)using metal oxide-zeolite tandem catalysts is an effective strategy for achieving carbon neutrality.However,progress in this area is constr... Thermally driven hydrogenation of CO2 to light olefins(C2=-C4=)using metal oxide-zeolite tandem catalysts is an effective strategy for achieving carbon neutrality.However,progress in this area is constrained by zeolite pore transport limitations,acidsite inactivation,and surface carbon poisoning.To address these issues,we replaced conventional zeolites with La-modified ZIF-8 and combined it with hollow cubic In2O3 to develop a novel In2O3-La-ZIF-8 tandem catalyst.Our study investigates the effects of the hydrothermal reaction temperature used for synthesizing In2O3 and the La content in ZIF-8 on catalytic performance.We also found that the oxygen vacancy(Ov)concentration in In2O3 can be substantially regulated by adjusting the hydrothermal temperature.The In2O3 sample with the highest Ov concentration not only promotes the formation of reaction intermediates but also markedly reduces the energy barrier of the rate-determining step in methanol synthesis.Comprehensive characterization and simulation analyses indicate that La incorporation enhances the thermal stability of ZIF-8,improves its ability to adsorb and activate reaction intermediates,and effectively adjusts its acid-base properties.Under a reaction pressure of 3.0 MPa and a temperature of 360℃,the hollow cubic In2O3-La-ZIF-8 tandem catalyst achieves 23.5%CO2 conversion with65.3%C2=-C4= selectivity. 展开更多
关键词 CO2hydrogenation In2O3‑La‑ZIF‑8 light olefins oxygen vacancy tandem catalyst
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Carboxylated Carbon Nanotube-Supported Copper-Indium Bimetallic Catalysts for Electroreduction of CO2 to Dimethyl Carbonate via Membrane-Free Cascade Electrosynthesis 认领 引用
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作者 Youjia Wang Xin Ma +4 位作者 Yuxin Tian Wenchao Wang Bochen Tian Yansheng Liu Junwei Hou 《Carbon and Hydrogen》 SCIE CAS CSCD 2026年第2期226-243,共18页
Under the background of the dual carbon strategy,upgrading CO2 electroreduction from C1 products to high-value C3 esters is an important direction for realizing its resource utilization and valorization.In this wor... Under the background of the dual carbon strategy,upgrading CO2 electroreduction from C1 products to high-value C3 esters is an important direction for realizing its resource utilization and valorization.In this work,Cu100In50 bimetallic catalysts supported on carboxylated carbon nanotubes were prepared,and a membrane-free paired electrolytic cell cascade system was constructed to achieve the directional conversion of CO2→CO→dimethyl carbonate(DMC).The catalyst exhibits enhanced CO supply and interfacial mass transfer capability,with the number of CO adsorption sites increased by 1.8 times and the methanol contact angle reduced from 22°to 8°.Electrochemical measurements show that the catalyst achieves a CO Faraday efficiency(FECO)of 60.9%at−1.8 V versus Ag/AgCl,whereas the FEH2 remains as low as 2.1%.In the cascade reaction,the FEDMC reaches 52.3%at−2.2 V and remains at 49.6%after 5 cycles.The system can also be extended to the electrosynthesis of diethyl carbonate(DEC),giving a FEDEC of 27.8%.In situ Raman spectroscopy combined with DFT calculations reveals that In doping shifts the d-band center of Cu by 0.38 eV,regulates the adsorption behavior of key intermediates,and suppresses HER,whereas carboxyl groups optimize the interfacial electronic structure and mass transfer behavior.This work provides an efficient catalytic strategy and mechanistic insight for the cascade valorization of CO2 into high-value carbonates. 展开更多
关键词 carboxylated carbon nanotubes cascade reaction CO2electroreduction copper-indium bimetallic catalyst DFT dimethyl carbonate insitu Raman spectroscopy
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Promotional effect of cerium and niobium doping on Cu/TiO2 catalyst for diethylamine catalytic degradation 认领 引用
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作者 Xiaoqiang Wang Ling Zhou +1 位作者 Yue Liu Zhongbiao Wu 《Journal of Rare Earths》 SCIE EI CAS CSCD 2026年第1期213-219,共7页
In this study,the promotional effect of Ce and Nb doping on Cu/TiO2 catalyst for diethylamine catalytic degradation was investigated.The activity tests reveal that the Ce and Nb modification can facilitate the risi... In this study,the promotional effect of Ce and Nb doping on Cu/TiO2 catalyst for diethylamine catalytic degradation was investigated.The activity tests reveal that the Ce and Nb modification can facilitate the rising of mineralization rate and N2 selectivity during diethylamine degradation,achieving over 90%mineralization rate at 250-450°C,along with N2 selectivity exceeding 80% within 300-400°C.Characterization results show that the co-addition of Ce and Nb induces strong interactions with Cu species and increases surface Brønsted acid sites.Crucially,the enhanced redox capability derived from interactions guarantees good catalytic activity and mineralization rate.Additionally,the increased Brønsted acidity from Nb doping can suppress the formation of NCO(a)species,resulting in less generation of NOx from NCO(a)oxidation.Moreover,the enhanced Brønsted acidity can promote the internal SCR reaction,which also reduces the NOx emission.This work could offer valuable insights for designing catalysts with superior catalytic performance for amine-like volatile organic compounds(VOCs)degradation. 展开更多
关键词 Catalytic degradation Diethylamine Cu/TiO2catalysts Cerium and niobium modification VOCs Rare earths
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