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Au@MoSx boosted carbon nitride for selective photoreforming of plastic waster:synergistic hydrogen production and value-added chemicals generation 认领 引用
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作者 Yadan Luo Danyang Zhang +5 位作者 Jingzhao Cheng Guijie Liang Guangmin Ren Jingsan Xu Hua Tang Shaowen Cao 《Advanced Powder Materials》 EI CAS CSCD 2026年第2期14-23,共10页
Combining the hydrogen production reaction with the photoreforming of plastic waste represents a key strategy for establishing a circular economy.Herein,the Au@MoSx nanoparticles were successfully modified onto car... Combining the hydrogen production reaction with the photoreforming of plastic waste represents a key strategy for establishing a circular economy.Herein,the Au@MoSx nanoparticles were successfully modified onto carbon nitride(CN/Au@MoSx)and employed for efficient hydrogen production,coupled with the high-selectivity upcycling of plastics into value-added products.Comprehensive characterization and density functional theory(DFT)calculations confirm that Au acts as an electron transfer mediator,accelerating charge migration from CN to MoSx.This facilitates the separation of photogenerated electron-hole pairs,thereby enhancing H2 evolution activity while preserving the high oxidation potential of holes on CN,which is favorable for plastic oxidation.Consequently,the optimal photocatalyst showed an H2 production rate of 1.73 mmol g-1 h-1,which is 10.5 times higher than that of CN(0.13 mmol g-1 h-1).Meanwhile,the liquid product achieves a selectivity of 77.9%for glycolic acid in the production of C2 compounds,which is 3.0 times higher than that of CN alone.Therefore,this study proposes a solar-driven“waste-to-wealth”approach that converts plastic waste into clean fuels and highly selective valuable chemical products,thereby addressing plastic pollution and fossil fuel dependency. 展开更多
关键词 Photoreforming Carbon nitride Catalytic mechanism Hydrogen evolution Valuable chemical
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Metal-defficient CoSe2 anchored monodisperse Pt for acidic electrosynthesis of H2O2 认领 引用
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作者 Qian Zhang Jinting Wu +6 位作者 Lijun Tang Yingnan Wang Xingchun Shi Jian Gao Tiansheng Mu Yong-Chao Zhang Xiao-Dong Zhu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2025年第12期143-152,I0005,共10页
Cobalt selenide(CoSe2)anchored monodisperse Pt presents good acidic 2e-oxygen reduction reaction(ORR)performance;however,conventional preparation methods can only yield ultra-low content of Pt atom catalysts.It ... Cobalt selenide(CoSe2)anchored monodisperse Pt presents good acidic 2e-oxygen reduction reaction(ORR)performance;however,conventional preparation methods can only yield ultra-low content of Pt atom catalysts.It is necessary to design catalysts with a high loading of monodisperse Pt to improve the activity and selectivity.Here,we reported anchoring highly reactive Pt atoms by constructing surface Co vacancies on CoSe2(Pt1/md-CoSe2),thereby increasing the co ntent of Pt atoms.The monodisperse Pt is not only a reactive active site but also helps to improve the intrinsic activity of Co around Pt with a suitable electronic structu re,which contributes to the simultaneous enhancement of~*O2 adsorption and lowering of the reaction activation energy,accelerating the 2e-ORR kinetics.The Pt_1/md-CoSe2 with a 0.2 wt%Pt exhibits high performa nce of electrocatalytic acidic 2e-ORR.The H2O2 yield is 1160.2 mmol gcat-1.h-1with a Faraday efficiency(FE)of 95.2%(0 V vs.RHE)at 0.1 M HClO4,superior to most of the reported literature.Moreover,the catalyst did not deactivate after a stability test of 30 h at the high current density of 100 mA cm-2.This work provides guidance for designing catalysts with applications and understanding the action mechanism of monodisperse Pt atoms. 展开更多
关键词 Metal vacancy Monodisperse Pt Intrinsic activity Acidic ORR Hydrogen peroxide
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Identification of abnormal conditions in high-dimensional chemical process based on feature selection and deep learning 认领 引用 被引量：5
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作者 Wende Tian Zijian Liu +2 位作者 Lening Li Shifa Zhang Chuankun Li 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2020年第7期1875-1883,共9页
Identification of abnormal conditions is essential in the chemical process.With the rapid development of artificial intelligence technology,deep learning has attracted a lot of attention as a promising fault identific... Identification of abnormal conditions is essential in the chemical process.With the rapid development of artificial intelligence technology,deep learning has attracted a lot of attention as a promising fault identification method in chemical process recently.In the high-dimensional data identification using deep neural networks,problems such as insufficient data and missing data,measurement noise,redundant variables,and high coupling of data are often encountered.To tackle these problems,a feature based deep belief networks(DBN)method is proposed in this paper.First,a generative adversarial network(GAN)is used to reconstruct the random and non-random missing data of chemical process.Second,the feature variables are selected by Spearman’s rank correlation coefficient(SRCC)from high-dimensional data to eliminate the noise and redundant variables and,as a consequence,compress data dimension of chemical process.Finally,the feature filtered data is deeply abstracted,learned and tuned by DBN for multi-case fault identification.The application in the Tennessee Eastman(TE)process demonstrates the fast convergence and high accuracy of this proposal in identifying abnormal conditions for chemical process,compared with the traditional fault identification algorithms. 展开更多
关键词 Chemical process Deep Belief Networks Fault identification Generative Adversarial Networks Spearman Rank Correlation
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A review of recent progress on CO2hydrogenation to methane by Ni-based catalysts supported on carbon materials 认领 引用
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作者 SUN Yu HUO Kai-xuan +2 位作者 FANG Hai-qiu WANG Yang WU Ming-bo 《新型炭材料（中英文）》 SCIE EI CAS CSCD 北大核心 2025年第6期1201-1218,共18页
Recent research progress on the use of Ni-based catalysts supported by various carbon materials,such as carbon nanotubes,graphene,and activated carbon,for the hydrogenation of CO2to CH4is summarized.The influenc... Recent research progress on the use of Ni-based catalysts supported by various carbon materials,such as carbon nanotubes,graphene,and activated carbon,for the hydrogenation of CO2to CH4is summarized.The influence of additives and surface modification methods on improving their catalytic performance is discussed as is the reaction mechanism,especially the structurefunction relationship produced by the carbon.The review provides a comprehensive directory for the rational design of carbon-supported Ni-based catalysts for the methanation of CO2. 展开更多
关键词 Carbon dioxide hydrogenation Carbon materials Ni-based catalysts Methanation Reaction mechanism
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Microscopic mechanism study and process optimization of dimethyl carbonate production coupled biomass chemical looping gasification system 认领 引用 被引量：2
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作者 Wende Tian Jiawei Zhang +2 位作者 Zhe Cui Haoran Zhang Bin Liu 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2023年第6期291-305,共15页
Biomass chemical looping gasification technology is one of the essential ways to utilize abundant biomass resources.At the same time,dimethyl carbonate can replace phosgene as an environmentfriendly organic material f... Biomass chemical looping gasification technology is one of the essential ways to utilize abundant biomass resources.At the same time,dimethyl carbonate can replace phosgene as an environmentfriendly organic material for the synthesis of polycarbonate.In this paper,a novel system coupling biomass chemical looping gasification with dimethyl carbonate synthesis with methanol as an intermediate is designed through microscopic mechanism analysis and process optimization.Firstly,reactive force field molecular dynamics simulation is performed to explore the reaction mechanism of biomass chemical looping gasification to determine the optimal gasification temperature range.Secondly,steady-state simulations of the process based on molecular dynamics simulation results are carried out to investigate the effects of temperature,steam to biomass ratio,and oxygen carrier to biomass ratio on the syngas yield and compositions.In addition,the main energy indicators of biomass chemical looping gasification process including lower heating value and cold gas efficiency are analyzed based on the above optimum parameters.Then,two synthesis stages are simulated and optimized with the following results obtained:the optimal temperature and pressure of methanol synthesis stage are 150℃ and 4 MPa;the optimal temperature and pressure of dimethyl carbonate synthesis stage are 140℃ and 0.3 MPa.Finally,the pre-separation-extraction-decantation process separates the mixture of dimethyl carbonate and methanol generated in the synthesis stage with 99.11%purity of dimethyl carbonate.Above results verify the feasibility of producing dimethyl carbonate from the perspective of multi-scale simulation and realize the multi-level utilization of biomass resources. 展开更多
关键词 Biomass chemical looping gasification Reactive force field molecular dynamics simulation Separation Multi-scale simulation
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Mechanism analysis and simulation of methyl methacrylate production coupled chemical looping gasification system 认领 引用 被引量：1
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作者 Wende Tian Haoran Zhang +1 位作者 Zhe Cui Xiude Hu 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2021年第9期184-196,共13页
Nowadays,the efficient and cleaner utilization of coal have attracted wide attention due to the rich coal and rare oil/gas resources structure in China.Coal chemical looping gasification(CCLG)is a promising coal utili... Nowadays,the efficient and cleaner utilization of coal have attracted wide attention due to the rich coal and rare oil/gas resources structure in China.Coal chemical looping gasification(CCLG)is a promising coal utilization technology to achieve energy conservation and emission reduction targets for highly pure synthesis gas.As a downstream product of synthesis gas,methyl methacrylate(MMA),is widely used as raw material for synthesizing polymethyl methacrylate and resin products with excellent properties.So this paper proposes a novel system integrating MMA production and CCLG(CCLG-MMA)processes aiming at"energy saving and low emission",in which the synthesis gas produced by CCLG and purified by dry methane reforming(DMR)reaction and Rectisol process reacts with ethylene for synthesizing MMA.Firstly,the reaction mechanism of CCLG is investigated by using Reactive force field(ReaxFF)MD simulation based on atomic models of char and oxygen carrier(Fe2O3)for obtaining optimum reaction temperature of fuel reactor(FR).Secondly,the steady-state simulation of CCLG-MMA system is carried out to verify the feasibility of MMA production.The amount of CO2emitted by CCLG process and DMR reaction is 0.0028(kg CO2)-1·(kg MMA)-1.The total energy consumption of the CCLG-MMA system is 45521 kJ·(kg MMA)-1,among which the consumption of MMA production part is 25293 k(·kg MMA)-1.The results show that the CCLG-MMA system meets CO2emission standard and has lower energy consumption compared to conventional MMA production process.Finally,one control scheme is designed to verify the stability of CCLG-MMA system.The CCLG-MMA integration strategy aims to obtain highly pure MMA from multi-scale simulation perspectives,so this is an optimal design regarding all factors influencing cleaner MMA production. 展开更多
关键词 ReaxFF MD simulation CCLG-MMA system simulation Sensitivity analysis Plant wide control
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Fault monitoring based on mutual information feature engineering modeling in chemical process 认领 引用 被引量：6
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作者 Wende Tian Yujia Ren +2 位作者 Yuxi Dong Shaoguang Wang Lingzhen Bu 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2019年第10期2491-2497,共7页
A large amount of information is frequently encountered when characterizing the sample model in chemical process.A fault diagnosis method based on dynamic modeling of feature engineering is proposed to effectively rem... A large amount of information is frequently encountered when characterizing the sample model in chemical process.A fault diagnosis method based on dynamic modeling of feature engineering is proposed to effectively remove the nonlinear correlation redundancy of chemical process in this paper.From the whole process point of view,the method makes use of the characteristic of mutual information to select the optimal variable subset.It extracts the correlation among variables in the whitening process without limiting to only linear correlations.Further,PCA(Principal Component Analysis)dimension reduction is used to extract feature subset before fault diagnosis.The application results of the TE(Tennessee Eastman)simulation process show that the dynamic modeling process of MIFE(Mutual Information Feature Engineering)can accurately extract the nonlinear correlation relationship among process variables and can effectively reduce the dimension of feature detection in process monitoring. 展开更多
关键词 Big data Fault diagnosis Mutual information TE process Process modeling
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Thermogravimetric characteristics of corn straw and bituminous coal copyrolysis based the ilmenite oxygen carriers 认领 引用 被引量：1
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作者 Pengxing Yuan Xiude Hu +2 位作者 Jingjing Ma Tuo Guo Qingjie Guo 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第4期8-15,共8页
Herein,the co-pyrolysis reaction characteristics of corn straw(CS)and bituminous coal in the presence of ilmenite oxygen carriers(OCs)are investigated via thermogravimetry coupled with mass spectrometry.The results re... Herein,the co-pyrolysis reaction characteristics of corn straw(CS)and bituminous coal in the presence of ilmenite oxygen carriers(OCs)are investigated via thermogravimetry coupled with mass spectrometry.The results reveal that the participation of OCs weakens the devolatilization intensity of co-pyrolysis.When the CS blending ratio is<50%,the mixed fuel exhibits positive synergistic effects.The fitting results according to the Coats-Redfern integral method show that the solid-solid interaction between OCs and coke changes the reaction kinetics,enhancing the co-pyrolysis reactivity at the high-temperature zone(750-950C).The synergistic effect is most prominent at a 30%CS blending ratio,with copyrolysis activation energy in the range of 26.35-40.57 kJ·mol-1. 展开更多
关键词 Oxygen carrier Co-pyrolysis Biomass Coal
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Vertical microbial profiling of water column reveals prokaryotic communities and distribution features of Antarctic Peninsula 认领 引用
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作者 Jiang Li Luying Zhao +4 位作者 Xiaoqian Gu Chengxuan Li Qian Zhang Liping Fu Ao Zhang 《Acta Oceanologica Sinica》 SCIE CAS CSCD 2023年第9期90-100,共11页
Prokaryotic diversity and community composition in the water column of eight stations(63 samples) around the Antarctic Peninsula of the Southern Ocean were investigated. Through pyrosequencing of the V3–V4hypervariab... Prokaryotic diversity and community composition in the water column of eight stations(63 samples) around the Antarctic Peninsula of the Southern Ocean were investigated. Through pyrosequencing of the V3–V4hypervariable regions of the 16S ribosomal RNA gene, we characterized 4 720 089 valid reads representing 48 188operational taxonomic units(OTUs, 97% similarity). The community was dominated by the phyla Pseudomonadota(original name: Proteobacteria, 47%), Oxyphotobacteria(26%), and Bacteroidota(original name: Bacteroidetes, 18%), which comprised an average of 91% of the total OTUs in all samples. The prokaryotic community composition varied vertically within the water column. Water column prokaryotic communities exhibited a clear depth profile, with higher microbial richness and higher diversity observed with increasing water depth. Cluster analysis of the community composition of water column samples exhibited a similar trend with depth. Correlation with environmental factors suggested distinct variation in prokaryotic community composition with changes in depth, salinity, temperature and dissolved oxygen levels. Functional prediction showed presence of active nitrogen, sulphur and methane metabolic cycles along the vertical transect of the studied region. These results will improve our knowledge of prokaryotic diversity and community composition at different depth of water column for better understanding of the microbial ecology and nutrient cycles in Antarctic Peninsula region of the Southern Ocean. 展开更多
关键词 prokaryotic diversity 16S rRNA high-throughput sequencing(HTS) Southern Ocean
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Synthesis of mordenite by solvent-free method and its application in the dimethyl ether carbonylation reaction 认领 引用 被引量：2
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作者 Yinghui Liu Shaoduo Liu +8 位作者 Xiaosheng Wang Hongjing Wang Ranjia Li Changchun Yu Chunming Xu Yuxiang Liu Zhengqiu Xie Yongqiang Wang Pan Tang 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第2期216-223,共8页
Mordenite with different Si/Al ratios were synthesized by solvent-free method and used for dimethyl ether(DME)carbonylation reaction.The influence of Si/Al ratio in the feedstock on the structure,porosity and acid sit... Mordenite with different Si/Al ratios were synthesized by solvent-free method and used for dimethyl ether(DME)carbonylation reaction.The influence of Si/Al ratio in the feedstock on the structure,porosity and acid sites were systematically investigated.The characterization results showed that with the increase of Si/Al ratio in the feedstock,part of silicon species fail to enter the skeleton and the specific surface area and pore volume of the samples decreased.The amount of weak acid and medium strong acid decreased alongside with the increasing Si/Al ratio,and the amount of strong acid slightly increased.The Al atoms preferentially enter the strong acid sites in the 8 member ring(MR)channel during the crystallization process.The high Si/Al ratio sample had more acid sites located in the 8 MR channel,leading to more active sites for carbonylation reaction and higher catalytic performance.Appropriately increasing the Si/Al ratio was beneficial for the improvement of carbonylation reaction activity over the mordenite(MOR)catalyst. 展开更多
关键词 Carbonylation Dimethyl ether Solvent-free Zeolite Synthesis Catalysis
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Fibrous MXene Aerogels with Tunable Pore of Contaminated Seawater 认领 引用
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作者 Fan Wu Siyu Qiang +5 位作者 Xiao-Dong Zhu Wenling Jiao Lifang Liu Jianyong Yu Yi-Tao Liu Bin Ding 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第5期298-312,共15页
The seawater desalination based on solardriven interfacial evaporation has emerged as a promising technique to alleviate the global crisis on freshwater shortage.However,achieving high desalination performance on actu... The seawater desalination based on solardriven interfacial evaporation has emerged as a promising technique to alleviate the global crisis on freshwater shortage.However,achieving high desalination performance on actual,oil-contaminated seawater remains a critical challenge,because the transport channels and evaporation interfaces of the current solar evaporators are easily blocked by the oil slicks,resulting in undermined evaporation rate and conversion efficiency.Herein,we propose a facile strategy for fabricating a modularized solar evaporator based on flexible MXene aerogels with arbitrarily tunable,highly ordered cellular/lamellar pore structures for high-efficiency oil interception and desalination.The core design is the creation of 1D fibrous MXenes with sufficiently large aspect ratios,whose superior flexibility and plentiful link forms lay the basis for controllable 3D assembly into more complicated pore structures.The cellular pore structure is responsible for effective contaminants rejection due to the multi-sieving effect achieved by the omnipresent,isotropic wall apertures together with underwater superhydrophobicity,while the lamellar pore structure is favorable for rapid evaporation due to the presence of continuous,large-area evaporation channels.The modularized solar evaporator delivers the best evaporation rate(1.48 kg m-2h-1)and conversion efficiency(92.08%)among all MXene-based desalination materials on oil-contaminated seawater. 展开更多
关键词 Fibrous MXene aerogels Tunable pore structures Modularized solar evaporator Photothermal desalination
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Transient thermal shock induced radial gradient Cu+ -Ov-Ce3+/Ce4+boosted CO2 electroreduction to C2 products 认领 引用
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作者 Mingwang Wang Xiang Fei +2 位作者 Hui Ning Han Hu Mingbo Wu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2026年第3期639-645,共7页
Electrocatalytic CO2 reduction(CO2 RR)toward multi-carbon compounds is a challenging but meaningful route for carbon cycling.Copper-based catalysts are the most promising candidate for C2+generation due to th... Electrocatalytic CO2 reduction(CO2 RR)toward multi-carbon compounds is a challenging but meaningful route for carbon cycling.Copper-based catalysts are the most promising candidate for C2+generation due to their unique C–C coupling activity,yet the in situ reduction from Cu+ to Cu0 under cathodic potentials causes the catalyst deactivation.Herein,we develop a transient thermal shock strategy to embed Cu+ species into CeO2 lattices,constructing a CuOx/CuCeOxcatalyst with a radial gradient Cu+ -Ov-Ce3+/Ce4+structure.Depth-profiling X-ray photoelectron spectroscopy(XPS)and density functional theory(DFT)calculations reveal that mismatched metal/oxygen diffusion kinetics drive continuous electron transfer from surface Cu+ to bulk Ce3+/Ce4+via oxygen vacancies(Ov),forming a dynamic“self-sacrificial”structure to preserve surface Cu+ states.In CO2-saturated 0.1 M KHCO3,the optimized CuOx/CuCeOx-10 achieves a high C2 Faradaic efficiency(FE)of 85.8%at-1.4 V vs.RHE.In situ attenuated total reflection surface-enhanced infrared adsorption spectroscopy(ATR-SEIRAS)identifies the key intermediates of C2 are*OCCO and*OCCOH,while DFT reveals a drastic reduction of C–C coupling barrier from 0.842 to0.274 eV.This work demonstrates kinetically tailored metal-support interactions,enabling oxidationstate control for pathway-selective catalysis. 展开更多
关键词 Carbon dioxide Metal-support interactions Gradient structure
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Fluorinated poly(p-terphenyl isatin)-based anion exchange membranes with microphase-separated structures for water electrolysis 认领 引用
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作者 Xinji Yu Limin Zhang +3 位作者 Yue Chen Jihai Duan Weiwen Wang Shuguo Qu 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2026年第5期65-77,共13页
In recent years,anion exchange membrane water electrolysis(AEMWE)has garnered significant attention as an efficient technology for hydrogen production.However,anion exchange membranes(AEMs),which are fundamental compo... In recent years,anion exchange membrane water electrolysis(AEMWE)has garnered significant attention as an efficient technology for hydrogen production.However,anion exchange membranes(AEMs),which are fundamental components of AEMWE,continue to face challenges in achieving a balance between ionic conductivity and dimensional integrity.This study successfully synthesized a series of poly(p-terphenyl isatin)-based AEMs,featuring fluorinated main chains and long alkyl side chains(FPTI-N-x-pip),through superacid-catalyzed Friedel-Crafts alkylation,Menshutkin,and nucleophilic substitution reactions.A comparison was also made with poly(p-terphenyl isatin)AEMs containing non-fluorinated main chains(PTI-pip).The incorporation of hydrophobic fluorinated groups into the main chain,coupled with hydrophilic side chains,results in a distinct microphaseseparated structure that enhances both ionic conductivity and dimensional stability.Furthermore,the dual-cation synergistic effect improves the membrane's resistance to alkaline conditions.At 80℃,FPTI-N-50-pip exhibited a maximum ionic conductivity of(158.7±5)mS·cm-1,significantly surpassing that of PTI-pip,which lacks fluorinated groups(80±5)mS·cm-1.Additionally,the introduction of hydrophobic fluorinated groups effectively reduced water uptake,yielding a swelling ratio of only 28.5%at 80℃.After being exposed to 1 mol·L-1 KOH at 80℃for 500 h,the membrane retained 96.3%of its initial conductivity,indicating excellent alkaline stability.Moreover,the AEMWE cell utilizing FPTI-N-50-pip achieved a current density of 1.14 A·cm-2at 2.6 V and 60℃.The characterization results suggest that the synthesized FPTI-N-x-pip membranes hold great potential for applications in AEMWE. 展开更多
关键词 Ion exchange membrane Fluorinated groups Membrances Microphase separation structure Water electrolysis Hydrogen production
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Exposure of V sites on InVO4via rapid Joule-heating for highly efficient photocatalytic N2fixation 认领 引用
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作者 Qianyu Chu Guangmin Ren +3 位作者 Jingdan Zhao Xiangchao Meng Jie Meng Zizhen Li 《Inorganic Chemistry Frontiers》 SCIE EI CAS CSCD 2026年第5期1919-1930,共12页
The photocatalytic nitrogen reduction reaction(NRR)is a sustainable green alternative to the Haber-Bosch process for ammonia production.However,due to the inert properties of dinitrogen,the photocatalytic activity in ... The photocatalytic nitrogen reduction reaction(NRR)is a sustainable green alternative to the Haber-Bosch process for ammonia production.However,due to the inert properties of dinitrogen,the photocatalytic activity in N2 reduction is still pretty low.Based on density functional theory calculations,this study finds that the formation energy of oxygen vacancies around the V site in InVO4was significantly lower than that around the In site.This indicated that the V-O bond was thermodynamically less stable and tends to break preferentially.Therefore,selective cleavage of the V-O bond was achieved by subjecting InVO4to transient high-temperature treatment via rapid Joule heating technology.This resulted in the directed construction of an InVO4-JH catalyst enriched with oxygen vacancies and exposing coordination-unsaturated V sites.The resulting InVO4-JH catalyst delivered a photocatalytic ammonia production rate of up to 35.28μmol g-1h-1under ambient conditions without any sacrificial agent,while exhibiting excellent stability and reaction selectivity.Mechanistic studies and structural characterization confirmed that the formation of oxygen vacancies via V-O bond cleavage releases electrons,which reduce adjacent V5+to V4+.This created localized electron-rich regions at exposed V sites.Theoretical calculations further confirmed that these exposed V sites act as the active centers of the reaction,not only significantly enhancing nitrogen adsorption but also substantially lowering the energy barrier of the hydrogenation step through alternative reaction pathways.This work provides a novel strategy for the rational design of highly efficient defect-engineered catalysts via targeted bond cleavage. 展开更多
关键词 density functional theory calculationsthis ammonia production v o bond cleavage rapid joule heating photocatalytic nitrogen reduction reaction nrr invo oxygen vacancies photocatalytic nitrogen reduction
3D-printed Ti/graphene composite current collectors for high-voltage aqueous zinc-ion batteries 认领 引用
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作者 Yang Zhiqiang Yang Hao +8 位作者 Wang Rui Wan Yi Zhang Yan Liu Chenhao Zhang Zian Li Yuqi Wu Mingbo Hu Han Chen De 《新型炭材料（中英文）》 SCIE EI CSCD 北大核心 2026年第3期641-651,I0048-I0062,共11页
Aqueous zinc-ion batteries(AZIBs)have significant promise as large-scale energy storage devices due to their high safety,low cost,and environmental friendliness.However,their application has been constrained by limite... Aqueous zinc-ion batteries(AZIBs)have significant promise as large-scale energy storage devices due to their high safety,low cost,and environmental friendliness.However,their application has been constrained by limited operational voltage windows.A high-voltage-resistant Ti-graphene-Ti cathode current collector(TGT)was designed and fabricated by three-dimensional(3D)printing.The surface of the TGT has a TixOy protective layer,which effectively suppresses electrolyte decomposition under high voltage conditions so that the voltage window of the battery is extended to 1.0-2.2 V without the obvious formation of by-products.Simultaneously,the graphene layer in the TGT structure significantly improves the adsorption and insertion/extraction kinetics of cations,resulting in a high specific capacity of 307.5 mAh g−1and a prolonged cycling life of the battery.The resultant AZIBs have a stable charge/discharge performance over 400 cycles at a high voltage.Furthermore,the influence of the geometric arrangements of Ti and graphene in the 3D printing process on the energy storage mechanism was investigated and provided novel insight for the development of high-voltage-resistant composite cathode current collectors for AZIBs. 展开更多
关键词 3D printing Aqueous zinc-ion batteries Composite current collectors High-voltage cathodes Wide voltage window
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Investigation into Syngas Generation from Solid Fuel Using CaSO4-based Chemical Looping Gasification Process 认领 引用 被引量：21
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作者 LIU Yongzhuo GUO Qingjie 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2013年第2期127-134,共8页
Chemical-looping gasification(CLG)is a novel process for syngas generation from solid fuels,sharing the same basic principles as chemical-looping combustion(CLC).It also uses oxygen carriers(mainly metal oxide and cal... Chemical-looping gasification(CLG)is a novel process for syngas generation from solid fuels,sharing the same basic principles as chemical-looping combustion(CLC).It also uses oxygen carriers(mainly metal oxide and calcium sulfate)to transfer heat and oxygen to the fuel.In this paper,the primary investigation into the CLG process with CaSO4 as oxygen carrier was carried out by thermodynamic analysis and experiments in the tube reactor.Sulfur-contained gas emission was mainly H2S rather than SO2 in the CLG process,showing some different features from the CLC.The mass and heat balance of CLG processes were calculated thermodynamically to determinate the auto-thermal operating conditions with different CaSO4/C and steam/C molar ratios.It was found that the CaSO4/C molar ratio should be higher than 0.2 to reach auto-thermal balance.The effect of temperature on the reactions between oxygen carrier and coal was investigated based on Gibbs free energy minimum method and ex-perimental results.It indicated that high temperature favored the CLG process in the fuel reactor and part of syngas was consumed to compensate for auto-thermal system. 展开更多
关键词 chemical-looping gasification syngas generation CaSO4oxygen carrier thermodynamic analysis
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Interfacial Ru nanoclusters in tandem with single atoms on oxygen-vacancy regulated CeO2for anion exchange membrane seawater-splitting 认领 引用 被引量：2
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作者 Yue Wang Jing Li +8 位作者 Pengfei Yang Hongdong Li Guangrui Xu Yunmei Du Caixia Li Wei Jin Tianyi Ma Zexing Wu Lei Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2025年第3期618-627,共10页
A hydrogen spillover-bridged water dissociation/hydrogen formation could concurrently promote Volmer/Tafel process and improve the efficiency of hydrogen evolution reaction(HER)under alkaline conditions.However,it is ... A hydrogen spillover-bridged water dissociation/hydrogen formation could concurrently promote Volmer/Tafel process and improve the efficiency of hydrogen evolution reaction(HER)under alkaline conditions.However,it is still challenging to promote occurrence of hydrogen spillover for the large interfacial transport barriers of H2O and hydrogen on active sites.Herein,the strategy of energy barrier gradient to induce hydrogen spillover was proposed by constructing Ru nanoclusters coupled with single atom onto oxygen vacancy cerium dioxide(Ru/CeO2-Ov-2).Density functional theory(DFT)calculations uncover that the adsorption/desorption of H2O occurs at the Ru clusters sites and then the dissociated H*spontaneously overflows from Ru clusters with high binding energy into the adjacent Ru single atom sites with low binding energy,which facilitate the hydrogen formation.Consequently,the synthesized Ru/CeO2-Ov-2 exhibits a small overpotential of 41 mV at 10 mA cm-2and good stability at 500 mA cm-2for 100 h in alkaline seawater,which could be ascribed to the rapid hydrogen spillover and strong coupling interaction between Ru and CeO2-Ov.This work provides a novel insight that synthesizing cooperative sites with energy barrier gradient helps to promote hydrogen spillover and accelerate the Volmer/Tafel process of HER. 展开更多
关键词 Electrocatalyst CeO2 Ru Oxygen vacancy Hydrogen evolution reaction
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Elaborately designed multilayers honeycomb-like MXene/BPQDs hierarchical architecture anode for SIBs with excellent kinetics 认领 引用
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作者 Jin-Hao Zhang Li-Su Zhang +3 位作者 Tian-Sheng Mu Yue Liang Fei-Li Lai Xiao-Dong Zhu 《Rare Metals》 SCIE EI CAS CSCD 2025年第11期8453-8464,共12页
Black phosphorus quantum dots(BPQDs)show great promise as anode material for sodium-ion batteries(SIBs)due to their high theoretical capacity and short ion diffusion pathways.However,the challenges of low electronic c... Black phosphorus quantum dots(BPQDs)show great promise as anode material for sodium-ion batteries(SIBs)due to their high theoretical capacity and short ion diffusion pathways.However,the challenges of low electronic conductivity and aggregation of BPQDs hinder their performance in SIBs.Loading BPQDs onto MXene nanosheets can address these issues,but the two-dimensional nano sheets may restack into a dense film during the filtration process,limiting reaction kinetics.Here,we report,for the first time,a bionic strategy for multilayer honeycomb-like MXene/BPQDs(MLHM/BPQDs)hierarchical architecture anode for SIBs.MXene nanosheets are arranged to ordered honeycomb layers and interlayer channels through the dual-template method.MXene nanosheets are arranged to ordered honeycomb layers and interlayer channels through the dual-templates method,and then,BPQDs are uniformly self-assembled onto the inwalls of the honeycomb.The unique open hierarchical architecture serves as an excellent substrate for rapid electron transport.Its large specific surface area offers more sites for BPQDs loading,preventing aggregation,and provides abundant channels and space for electrolyte infiltration and BPQDs volume change.The-O terminal groups increased after annealing,and the abundant-O/-F terminal groups on the surface of MXene can effectively enhance the binding energy and diffusion rate of Na+.The synergy of structure and surface chemistry accelerates the kinetics for MLHM/BPQDs,delivering a high reversible capacity of653 mAh g-1after 500 cycles at 2 A g-1(94.3%capacity retention),which demonstrates its great potential as a SIBs anode material. 展开更多
关键词 Honeycomb-like structure Black phosphorus quantum dots Sodium storage Self-assembly Excellent kinetics
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Computational particle fluid dynamics simulation of gas–solid flow in a 3 MWth dual-circulation fluidized bed for chemical looping process 认领 引用
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作者 Yankun Li Tuo Guo +4 位作者 Xintong Guo Xiude Hu Qingjie Guo Shengzhong He Zimiao Zhou 《Carbon Resources Conversion》 EI 2024年第4期43-53,共11页
Regulation of gas–solid flow is crucial for optimizing the operation efficiency of dual-circulating fluidized beds that are considered to be the most appropriate type of chemical-looping reactors. Herein, a computati... Regulation of gas–solid flow is crucial for optimizing the operation efficiency of dual-circulating fluidized beds that are considered to be the most appropriate type of chemical-looping reactors. Herein, a computational particle fluid dynamics method was employed to simulate the gas–solid flow in a 3-MWth dual-circulating fluidized bed used for chemical-looping combustion and gasification. The influence of structural difference between units on particle residence time was determined. The multi-parameter control mechanism of pressure, particle circulation, and particle residence time in a whole-loop system was investigated. Results revealed that under stable particle circulation, the particle residence time in the fuel reactor is much longer than that in the air reactor. The axial forces on the particles are reduced upon increasing particle density and size, leading to particle accumulation in the dense-phase zone. When the particle properties are stable, increasing the fluidizing gas flow rates by the same proportion leads to identical pressure drops on the involved two loop seals, which cause symmetrical alterations in the particle circulation rate between the air and fuel reactors. The dual-circulating fluidized bed exhibits certain multi-condition adaptability, which is limited by the stock bin volume. Overall, this study is beneficial for effective and economical optimization of the operation of chemical-looping dual-circulating fluidized beds. 展开更多
关键词 Chemical looping Dual-circulating fluidized bed Computational particle fluid dynamics Gas-solid flow
Rapid anion transporting and mechanically robust cathode-electrolyte interphase for ultrafast and highly reversible dual-ion batteries within a wide temperature range 认领 引用
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作者 Hubiao Pan Xin Gu +4 位作者 Xinyu Lv Fengchun Li Fei Pang Yanli Zhou Mingbo Wu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2025年第10期100-108,共9页
High-voltage dual-ion batteries(DIBs)face significant challenges,including graphite cathode degradation,cathode-electrolyte interphase(CEI)instability,and the thermodynamic instability of conventional carbonate-based ... High-voltage dual-ion batteries(DIBs)face significant challenges,including graphite cathode degradation,cathode-electrolyte interphase(CEI)instability,and the thermodynamic instability of conventional carbonate-based electrolytes,particularly at extreme temperatures.In this study,we develop a stable electrolyte incorporating lithium difluorophosphate(LiDFP)as an additive to enhance the electrochemical performance of DIBs over a wide temperature range.LiDFP preferentially decomposes to form a rapid anion-transporting,mechanically robust CEI layer on graphite,which provides better protection by suppressing graphite's volume expansion,preventing electrolyte oxidative decomposition,and enhancing reaction kinetics.As a result,Li||graphite half cells using LiDFP electrolyte exhibit outstanding rate performance(90.8% capacity retention at 30 C)and excellent cycle stability(82.2% capacity retention after 5000 cycles)at room temperature.Moreover,graphite||graphite full cells with LiDFP electrolyte demonstrate stable discharge capacity across a temperature range of-20 to 40℃,expanding the potential applications of LiDFP.This work establishes a novel strategy for optimizing the interphase through electrolyte design,paving the way for all-climate DIBs with improved performance and stability. 展开更多
关键词 Dual-ion batteries Graphite cathode Electrolyte additive Cathode-electrolyte interphase Wide temperature range
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