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Preparation and characterization of ultrafine Fe-Cu-based catalysts for CO hydrogenation 被引量:4
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作者 Yunlai Su Yingli Wang Zhongmin Liu 《Journal of Natural Gas Chemistry》 EI CAS CSCD 2008年第4期327-331,共5页
The ultrafine particles of a new style Fe-Cu-based catalysts for CO hydrogenation were prepared by impregnating the organic sol of Fe(OH)3 and Cu(OH)2 onto the activated Al2O3, in which the organic sol of Fe(OH)... The ultrafine particles of a new style Fe-Cu-based catalysts for CO hydrogenation were prepared by impregnating the organic sol of Fe(OH)3 and Cu(OH)2 onto the activated Al2O3, in which the organic sol of Fe(OH)3 and Cu(OH)2 were prepared in the microemulsion of dodecylbenzenesulfonic acid sodium(S)/n-butanol(A)/toluene(O)/water with V(A)/V(O) = 0.25 and W(A)/W(S) = 1.50. This catalyst was characterized by particle size analysis, XRD and TG. The results of particle size analysis showed that Fe(OH)3 particles with a mean size of 17.1 nm and Cu(OH)2 particles with an average size of 6.65 um were obtained. TG analysis and XRD patterns suggested that 673 K is the optimal calcination temperature. CO hydrogenation produced C+OH with a high selectivity above 58 wt% by using the ultrafine particles as catalyst, and the total alcohol yield of 0.250 g·ml^-1 ·h^-1 was obtained when the contents of Al2O3 and K were 88.61 wt% and 1.60 wt%, respectively. 展开更多
关键词 MICROEMULSION CONDUCTIVITY ultrafine Fe-cu-based catalyst CO hydrogenation
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Popping of g-C_3N_4 mixed with cupric nitrate: Facile synthesis of Cu-based catalyst for construction of C-N bond 被引量:1
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作者 Shaoyu Yuan Penglei Cui +3 位作者 Yunrui Zhang Hong Zhang Li Huo Yongjun Gao 《Green Energy & Environment》 SCIE 2018年第4期368-374,共7页
A novel strategy to synthesize copper-based nanoparticles supported on carbon nitride(C3 N4) was developed by popping of mixture containing C3 N4 and cupric nitrate. Characterizations such as X-ray photoelectron spect... A novel strategy to synthesize copper-based nanoparticles supported on carbon nitride(C3 N4) was developed by popping of mixture containing C3 N4 and cupric nitrate. Characterizations such as X-ray photoelectron spectroscopy(XPS) and X-ray diffraction(XRD) indicate that the structure of g-C3 N4 maintained although a popping process occurred. High resolution transmission electronic microscopy(HRTEM) characterization illustrated that copper-based nanoparticles with diameter of < 1 nm were well distributed on g-C3 N4. This kind of copper catalyst exhibits high catalytic activity and selectivity in arylation of pyrazole, a simple and effect strategy to construct C-N bond in organic chemistry.According to the results of control experiments and characterizations, cuprous oxide should be the catalytic active phase in the supported coperbased catalyst. 展开更多
关键词 C-N coupling N-ARYLATION Carbon NITRIDE Catalysis COPPER-BASED catalyst
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Carbon Nano-tube Supported Cu-based Catalyst for Methanol Synthesis Developed by Xiamen University
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《China Petroleum Processing & Petrochemical Technology》 SCIE CAS 2008年第4期44-44,共1页
The Chemistry and Chemical Engineering School of Xiamen University has successfully developed the multi-walled nanotube catalyst with small and uniform diameter and has mastered the corresponding technology for manufa... The Chemistry and Chemical Engineering School of Xiamen University has successfully developed the multi-walled nanotube catalyst with small and uniform diameter and has mastered the corresponding technology for manufacture of carbon nanotube. It is learned that this technology has been for the first time developed inside ;and has reached the internationally advanced level with some indicators commanding a globally leading position. 展开更多
关键词 cu-based catalyst Chemical Engineering SCHOOL China multi-walled
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Ultra-stable Cu-based catalyst for dimethyl oxalate hydrogenation to ethylene glycol
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作者 Peipei Ai Huiqing Jin +2 位作者 Jie Li Xiaodong Wang Wei Huang 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2023年第8期186-193,共8页
Dimethyl oxalate(DMO) hydrogenation is a crucial step in the coal to ethylene glycol(CTEG) process.Herein, Cu catalyst supported on fibrous mesoporous silica(Cu/FMS) was synthesized via liquid phase deposition techniq... Dimethyl oxalate(DMO) hydrogenation is a crucial step in the coal to ethylene glycol(CTEG) process.Herein, Cu catalyst supported on fibrous mesoporous silica(Cu/FMS) was synthesized via liquid phase deposition technique and applied for the DMO hydrogenation to EG. The catalyst exhibited a remarkable EG selectivity of 96.95% and maintained its activity without deactivation for 1000 h. Fibers of FMS support and liquid phase deposition technology cooperated to give high dispersion of Cu species in the Cu/FMS catalyst, resulting in a high Cu surface area. The formation of Si—O—Cu during catalyst preparation process increased the Cu^(+)/(Cu^(0)+ Cu^(+)) ratio and enhanced the thermal and valence stability of Cu species.The high Cu^(+) surface area and Cu stability(thermal and valence stability) of the Cu/FMS catalyst were key factors for achieving superior EG selectivity and ultra-high stability. 展开更多
关键词 Stability Cu^(+)surface area Fibrous mesoporous silica catalyst HYDROGENATION
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Electrolyte manipulation on Cu-based electrocatalysts for electrochemical CO_(2) reduction
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作者 Hexin Zhou Wanlong Xi +4 位作者 Peng Yang Huiting Huang Jia Tian Marina Ratova Dan Wu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第12期201-222,共22页
Electrocatalytic reduction of CO_(2)is crucial for environmental sustainability and renewable energy storage,with Cu-based catalysts excelling in producing high-value C_(2+)products.However,a comprehensive analysis of... Electrocatalytic reduction of CO_(2)is crucial for environmental sustainability and renewable energy storage,with Cu-based catalysts excelling in producing high-value C_(2+)products.However,a comprehensive analysis of how specific electrolyte influences Cu-based catalysts is lacking.This review addresses this gap by focusing on how electrolytes impact surface reconstruction and the CO_(2) reduction process on Cu-based electrocatalysts,identifying specific electrolyte compositions that enhance the density and stability of active sites,and providing insights into how different electrolyte environments modulate the selectivity and efficiency of C_(2+)product formation.The review begins by exploring how electrolytes induce favorable surface reconstruction in Cu-based catalysts,affecting surface roughness through dissolution-redeposition of Cu species and interactions with halogens and molecular additives.It also covers changes in crystalline facets of Cu and Cu_(2)O,and oxidation states,highlighting transitions from Cu^(0) to Cu^(δ+)and the stabilization of Cu^(+).The role of electrolytes in the C–C coupling process is examined,emphasizing their effects in modulating mass and charge transfer,CO_(2) adsorption,intermediate evolution,and product desorption.Subsequently,the mechanisms by non-aqueous electrolytes,including organic solvents,ionic liquids,and mixed electrolytes,affecting CO_(2) reduction are analyzed,highlighting the unique advantages and challenges of each type.The review concludes by addressing current challenges,proposing solutions,and research directions,such as optimizing electrolyte composition by integrating diverse cations and anions and employing advanced in-situ characterization techniques.These insights can significantly enhance CO_(2)reduction performance on Cu-based electrocatalysts,advancing efficient and sustainable green energy technologies. 展开更多
关键词 CO_(2)reduction reaction cu-based catalyst ELECTROLYTE Surface reconstruction Intermediates evolution
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Cu-based materials for electrocatalytic CO_(2) to alcohols:Reaction mechanism,catalyst categories,and regulation strategies
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作者 Yaru Lei Yaxin Niu +8 位作者 Xiaolong Tang Xiangtao Yu Xiubing Huang Xiaoqiu Lin Honghong Yi Shunzheng Zhao Jiaying Jiang Jiyue Zhang Fengyu Gao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第10期593-611,I0013,共20页
Electrocatalytic CO_(2) reduction reaction(CO_(2)RR)technology,which enables carbon capture storage and resource utilization by reducing CO_(2) to valuable chemicals or fuels,has become a global research hotspot in re... Electrocatalytic CO_(2) reduction reaction(CO_(2)RR)technology,which enables carbon capture storage and resource utilization by reducing CO_(2) to valuable chemicals or fuels,has become a global research hotspot in recent decades.Among the many products of CO_(2)RR(carbon monoxide,acids,aldehydes and alcohols,olefins,etc.),alcohols(methanol,ethanol,propanol,etc.)have a higher market value and energy density,but it is also more difficult to produce.Copper is known to be effective in catalyzing CO_(2) to high valueadded alcohols,but with poor selectivity.The progress of Cu-based catalysts for the selective generation of alcohols,including copper oxides,bimetals,single atoms and composites is reviewed.Meanwhile,to improve Cu-based catalyst activity and modulate product selectivity,the modulation strategies are straighten out,including morphological regulation,crystalline surface,oxidation state,as well as elemental doping and defect engineering.Based on the research progress of electrocatalytic CO_(2) reduction for alcohol production on Cu-based materials,the reaction pathways and the key intermediates of the electrocatalytic CO_(2)RR to methanol,ethanol and propanol are summarized.Finally,the problems of traditional electrocatalytic CO_(2)RR are introduced,and the future applications of machine learning and theoretical calculations are prospected.An in-depth discussion and a comprehensive review of the reaction mechanism,catalyst types and regulation strategies were carried out with a view to promoting the development of electrocatalytic CO_(2)RR to alcohols. 展开更多
关键词 Electrocatalytic CO_(2)RR cu-based catalyst ALCOHOLS Reaction mechanism Regulation strategies
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Cu-based heterojunction catalysts for electrocatalytic nitrate reduction to ammonia
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作者 HUANG Yitao GUAN Minghao +4 位作者 PEI Jiyuan SONG Yongyi WU Tao HOU Shuandi LU Anhui 《燃料化学学报(中英文)》 EI CAS CSCD 北大核心 2024年第12期1857-1864,I0008-I0010,共11页
Copper-based catalysts have garnered wide attention in the field of electrocatalytic nitrate reduction for ammonia production due to their low hydrogen precipitation activity and high ammonia selectivity.However,they ... Copper-based catalysts have garnered wide attention in the field of electrocatalytic nitrate reduction for ammonia production due to their low hydrogen precipitation activity and high ammonia selectivity.However,they still face challenges pertaining of poor stability and low activity,which hinder their further application.Herein,we present a Cu_(2)O/Cu heterojunction catalyst supported on nitrogen-doped porous carbon for nitrate reduction.High resolution transmission electron microscopy(HRTEM)and X-ray Diffraction(XRD)results confirm the presence of Cu_(2)O/Cu heterojunctions,which serve as an active phase in catalysis.The nitrogen-doped porous carbon as a carrier not only enhances the catalyst’s stability,but also facilitates the exposure and dispersion of active sites.At-1.29 V(vs.RHE),the maximum production rate of ammonia reaches 8.8 mg/(mg·h)with a Faradaic efficiency of 92.8%.This study also elucidates the effect of Cu_(2)O-to-Cu ratio in the heterojunction on catalytic performance,thereby providing valuable insights for designing efficient nitrate reduction catalysts for ammonia production. 展开更多
关键词 ELECTROCATALYSIS nitrate reduction AMMONIA copper-based catalysts
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Rational design strategies of Cu-based electrocatalysts for CO_(2) electroreduction to C_(2) products 被引量:6
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作者 Shuo Liu Baoshan Zhang +1 位作者 Lihong Zhang Jie Sun 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第8期63-82,I0003,共21页
Electrochemical reduction of CO_(2)(CO_(2)RR)to high value-added chemicals is an effective way to remove excess CO_(2) from the atmosphere.Due to the unique propensity of Cu for valuable hydrocarbons,Cu-based electroc... Electrochemical reduction of CO_(2)(CO_(2)RR)to high value-added chemicals is an effective way to remove excess CO_(2) from the atmosphere.Due to the unique propensity of Cu for valuable hydrocarbons,Cu-based electrocatalysts are the most potential catalysts that allow the conversion of CO_(2) into a variety of C_(2) products such as ethylene and ethanol.Rational design of Cu-based catalysts can improve their directional selectivity to C_(2) products.Hence,in this review,we summarize the recent progress in the mechanistic studies of Cu-based catalysts on reducing CO_(2) to C_(2) products.We focus on three key strategies for efficiently enhancing electrocatalytic performance of Cu-based catalysts,including tuning electronic structure,surface structure,and coordination environment.The correlation between the structural characteristics of Cu-based catalysts and their activity and selectivity to C_(2) products is discussed.Finally,we discuss the challenges in the field of CO_(2) electroreduction to C_(2) products and provide the perspectives to design efficient Cu-based catalysts in the future. 展开更多
关键词 Carbon dioxide cu-based catalysts MECHANISMS Active site regulation
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Progress in regulating electronic structure strategies on Cu-based bimetallic catalysts for CO_(2)reduction reaction 被引量:3
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作者 Chunyang Yin Qing Li +6 位作者 Jun Zheng Yaqiong Ni Huiqiong Wu Anna-Lena Kjøniksen Chuntai Liu Yongpeng Lei Yi Zhang 《Advanced Powder Materials》 2022年第4期76-87,共12页
To address the ever-increasing CO_(2)concentration problem in the atmospheric air arisen by massive consumption of fossil fuels,electrocatalytic technologies that reduce CO_(2)to generate high value-added products hav... To address the ever-increasing CO_(2)concentration problem in the atmospheric air arisen by massive consumption of fossil fuels,electrocatalytic technologies that reduce CO_(2)to generate high value-added products have been gaining increasing interest.Cu-based CO_(2)reduction catalysts have attracted widespread attention owing to their capability of generating C1 and C_(2+)products.However,Cu-based catalysts are highly challenged by their low product selectivity.Recently,Cu-based bimetallic catalysts have been found the unique catalytical activity and selectivity in CO_(2)reduction reactions(CO_(2)RR).The incorporation of other metals can change the electronic circumstance of Cu-based catalysts,promoting the adsorption ability of the intermediate products and consequently leading to high selectivity.In this minireview,we intend to summarize recent advances of Cu-based bimetallic catalysts in producing C1 and C_(2+)products,involving designing heterostructure,alloy,defects and surface modification engineering.We pay special attention to the regulation of electronic structure of the composite catalysts,as well as insights into the relationship between electronic property and catalytical performance for Cu-based bimetallic catalysts. 展开更多
关键词 cu-based catalyst CO_(2) RRC_(2+)products Electronic structure regulation Intermetallic synergy
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The newly-assisted catalytic mechanism of surface hydroxyl species performed as the promoter in syngas-to-C2 species on the Cu-based bimetallic catalysts
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作者 Chenyang Li Yuan Zhang +4 位作者 Debao Li Baojun Wang Christopher K.Russell Maohong Fan Riguang Zhang 《Green Energy & Environment》 SCIE EI CSCD 2023年第2期487-498,共12页
In the conversion process of syngas-to-C_(2)species,the OH species are inevitably produced accompanying the production of key intermediates CH_(x)(x=1-3),traditionally,the function of surface OH species is generally a... In the conversion process of syngas-to-C_(2)species,the OH species are inevitably produced accompanying the production of key intermediates CH_(x)(x=1-3),traditionally,the function of surface OH species is generally accepted as the hydrogenating reactive species.This work for the first time proposed and confirmed the assisted catalytic mechanism of surface OH species that performed as the promoter for syngas-to-C_(2)species on Cu-based catalysts.DFT and microkinetic modeling results reveal that the produced OH species accompanying the intermediates CH_(x)production on the MCu(M=Co,Fe,Rh)catalysts can stably exist to form OH/MCu catalysts,on which the presence of surface OH species as the promoter not only presented better activity and selectivity toward CH_(x)(x=1-3)compared to MCu catalysts,but also significantly suppressed CH_(3)OH production,providing enough CH_(x)sources to favor the production of C_(2)hydrocarbons and oxygenates.Correspondingly,the electronic properties analysis revealed the essential relationship between the electronic feature of OH/MCu catalysts and catalytic performance,attributing to the unique electronic micro-environment of the catalysts under the interaction of surface OH species.This new mechanism is called as OH-assisted catalytic mechanism,which may be applied in the reaction systems related to the generation of OH species. 展开更多
关键词 Syngas conversion C_(2)species cu-based catalyst Surface OH species Assisted catalytic mechanism
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Cu-Based Materials for Enhanced C_(2+) Product Selectivity in Photo-/Electro-Catalytic CO_(2) Reduction: Challenges and Prospects 被引量:1
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作者 Baker Rhimi Min Zhou +2 位作者 Zaoxue Yan Xiaoyan Cai Zhifeng Jiang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第4期25-66,共42页
Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues and the energy shortages. Among the materials utilized for ca... Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues and the energy shortages. Among the materials utilized for catalytic reduction of CO_(2), Cu-based materials are highly advantageous owing to their widespread availability, cost-effectiveness, and environmental sustainability. Furthermore, Cu-based materials demonstrate interesting abilities in the adsorption and activation of carbon dioxide, allowing the formation of C_(2+) compounds through C–C coupling process. Herein, the basic principles of photocatalytic CO_(2) reduction reactions(PCO_(2)RR) and electrocatalytic CO_(2) reduction reaction(ECO_(2)RR) and the pathways for the generation C_(2+) products are introduced. This review categorizes Cu-based materials into different groups including Cu metal, Cu oxides, Cu alloys, and Cu SACs, Cu heterojunctions based on their catalytic applications. The relationship between the Cu surfaces and their efficiency in both PCO_(2)RR and ECO_(2)RR is emphasized. Through a review of recent studies on PCO_(2)RR and ECO_(2)RR using Cu-based catalysts, the focus is on understanding the underlying reasons for the enhanced selectivity toward C_(2+) products. Finally, the opportunities and challenges associated with Cu-based materials in the CO_(2) catalytic reduction applications are presented, along with research directions that can guide for the design of highly active and selective Cu-based materials for CO_(2) reduction processes in the future. 展开更多
关键词 Photocatalytic CO_(2)reduction cu-based materials Electrocatalytic CO_(2)reduction
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One-dimensional Cu-based catalysts with layered Cu-Cu20-CuO walls for the Rochow reaction 被引量:4
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作者 Jing Li Zailei Zhang +4 位作者 Yongjun Ji Zheying Jin Shanying Zou Ziyi Zhong Fabing Su 《Nano Research》 SCIE EI CAS CSCD 2016年第5期1377-1392,共16页
A series of copper catalysts with a core-shell or tubular structure containing various contents of Cu, Cu2O, and CuO were prepared via controlled oxidation of Cu nanowires (NWs) and used in the synthesis of dimethyl... A series of copper catalysts with a core-shell or tubular structure containing various contents of Cu, Cu2O, and CuO were prepared via controlled oxidation of Cu nanowires (NWs) and used in the synthesis of dimethyldichlorosilane (M2) via the Rochow reaction. The Cu NWs were prepared from copper (Ⅱ) nitrate using a solution-based reduction method. The samples were characterized by X-ray diffraction, thermogravimetric analysis, temperature-programmed reduction, X-ray photoelectron spectroscopy, transmission electron microscopy, and scanning electron microscopy. It was found that the morphology and composition of the catalysts could be tailored by varying the oxidation temperature and time. During the gradual oxidation of Cu NWs, the oxidation reaction inflated on the outer surface and gradually developed into the bulk of the NWs, leading to the formation of catalysts with various structures and layered compositions, e.g., Cu NWs with surface Cu2O, ternary Cu-Cu2O-CuO core-shell NWs, binary Cu2O-CuO nanotubes (NTs), and single CuO NTs. Among these catalysts, ternary Cu-Cu2O-CuO core-shell NWs exhibited superior M2 selectivity and Si conversion in the Rochow reaction. The enhanced catalytic performance was mainly attributed to improved mass and heat transfer resulting from the peculiar heterostructure and the synergistic effect among layered components. Our work indicated that the catalytic property of Cu-based nanoparticles can be improved by carefully controlling their structures and compositions. 展开更多
关键词 controlled oxidation NANOWIRES core-shell structure NANOTUBES copper-based catalysts Rochow reaction
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Recent advances in Cu-based nanocomposite photocatalysts for CO_2 conversion to solar fuels 被引量:2
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作者 Huan Xie Jingyun Wang +2 位作者 Kemakorn Ithisuphalap Gang Wu Qing Li 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2017年第6期1039-1049,共11页
COconversion via photocatalysis is a potential solution to address global warming and energy shortage.Photocatalysis can directly utilize the inexhaustible sunlight as an energy source to catalyze the reduction of COt... COconversion via photocatalysis is a potential solution to address global warming and energy shortage.Photocatalysis can directly utilize the inexhaustible sunlight as an energy source to catalyze the reduction of COto useful solar fuels such as CO, CH, CHOH, and CHOH. Among studied formulations, Cubased photocatalysts are the most attractive for COconversion because the Cu-based photocatalysts are low-cost and abundance comparing noble metal-based catalysts. In this literature review, a comprehensive summary of recent progress on Cu-based photocatalysts for COconversion, which includes metallic copper, copper alloy nanoparticles(NPs), copper oxides, and copper sulfides photocatalysts, can be found. This review also included a detailed discussion on the correlations of morphology, structure, and performance for each type of Cu-based catalysts. The reaction mechanisms and possible pathways for productions of various solar fuels were analyzed, which provide insight into the nature of potential active sites for the catalysts. Finally, the current challenges and perspective future research directions were outlined, holding promise to advance Cu-based photocatalysts for COconversion with much-enhanced energy conversion efficiency and production rates. 展开更多
关键词 cu-based photocatalyst CO_2 conversion Solar light Solar fuels Quantum efficiency
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Accelerated prediction of Cu-based single-atom alloy catalysts for CO_(2) reduction by machine learning 被引量:2
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作者 Dashuai Wang Runfeng Cao +5 位作者 Shaogang Hao Chen Liang Guangyong Chen Pengfei Chen Yang Li Xiaolong Zou 《Green Energy & Environment》 SCIE EI CAS CSCD 2023年第3期820-830,共11页
Various strategies,including controls of morphology,oxidation state,defect,and doping,have been developed to improve the performance of Cu-based catalysts for CO_(2) reduction reaction(CO_(2)RR),generating a large amo... Various strategies,including controls of morphology,oxidation state,defect,and doping,have been developed to improve the performance of Cu-based catalysts for CO_(2) reduction reaction(CO_(2)RR),generating a large amount of data.However,a unified understanding of underlying mechanism for further optimization is still lacking.In this work,combining first-principles calculations and machine learning(ML)techniques,we elucidate critical factors influencing the catalytic properties,taking Cu-based single atom alloys(SAAs)as examples.Our method relies on high-throughput calculations of 2669 CO adsorption configurations on 43 types of Cu-based SAAs with various surfaces.Extensive ML analyses reveal that low generalized coordination numbers and valence electron number are key features to determine catalytic performance.Applying our ML model with cross-group learning scheme,we demonstrate the model generalizes well between Cu-based SAAs with different alloying elements.Further,electronic structure calculations suggest surface negative center could enhance CO adsorption by back donating electrons to antibonding orbitals of CO.Finally,several SAAs,including PCu,AgCu,GaCu,ZnCu,SnCu,GeCu,InCu,and SiCu,are identified as promising CO_(2)RR catalysts.Our work provides a paradigm for the rational design and fast screening of SAAs for various electrocatalytic reactions. 展开更多
关键词 cu-based single-atom alloy CO adsorption Machine learning First principles CO_(2)reduction reaction
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Tuning Structures and Microenvironments of Cu-Based Catalysts for Sustainable CO_(2) and CO Electroreduction 被引量:1
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作者 Ximeng Lv Zhengzheng Liu +2 位作者 Chao Yang Yali Ji Gengfeng Zheng 《Accounts of Materials Research》 2023年第3期264-274,共11页
CONSPECTUS:The carbon balance has been disrupted by the widespread use of fossil fuels and subsequent excessive emissions of carbon dioxide(CO_(2)),which has become an increasingly critical environmental challenge for... CONSPECTUS:The carbon balance has been disrupted by the widespread use of fossil fuels and subsequent excessive emissions of carbon dioxide(CO_(2)),which has become an increasingly critical environmental challenge for human society.The production and use of renewable energy sources and/or chemicals have been proposed as important strategies to reduce emissions,of which the electrochemical CO_(2)(or CO)reduction reaction(CO_(2)RR/CORR)in the aqueous systems represents a promising approach.Benefitted by the capacity of manufacturing high-value-added products(e.g.,ethylene,ethanol,formic acid,etc.)with a net-zero carbon emission,copper-based CO_(2)RR/CORR powered by sustainable electricity is regarded as a potential candidate for carbon neutrality.However,the diversity of selectivities in copper-based systems poses a great challenge to the research in this field and sets a great obstacle for future industrialization.To date,scientists have revealed that the electrocatalyst design and preparation play a significant role in achieving efficient and selective CO_(2)-to-chemical(or CO-to-chemical)conversion.Although substantial efforts have been dedicated to the catalyst preparation and corresponding electrosynthesis of sustainable chemicals from CO_(2)/CO so far,most of them are still derived from empirical or random searches,which are relatively inefficient and cost-intensive.Most of the mechanism studies have suggested that both intrinsic properties(such as electron states)and extrinsic environmental factors(such as surface energy)of a catalyst can significantly alter catalytic performance.Thus,these two topics are mainly discussed for copper-based catalyst developments in this Account.Here,we provided a concise and comprehensive introduction to the well-established strategies employed for the design of copperbased electrocatalysts for CO_(2)RR/CORR.We used several examples from our research group,as well as representative studies of other research groups in this field during the recent five years,with the perspectives of tuning local electron states,regulating alloy phases,modifying interfacial coverages,and adjusting other interfacial microenvironments(e.g.,molecule modification or surface energy).Finally,we employed the techno-economic assessment with a viewpoint on the future application of CO_(2)/CO electroreduction in manufacturing sustainable chemicals.Our study indicates that when carbon price is taken into account,the electrocatalytic CO_(2)-to-chemical conversion can be more market-competitive,and several potential value-added products including formate,methanol,ethylene,and ethanol can all make profits under optimal operating conditions.Moreover,a downstream module employing traditional chemical industrial processes(e.g.,thermal polymerization,catalytic hydrolysis,or condensation process)will also make the whole electrolysis system profitable in the future.These design principles,combined with the recent advances in the development of efficient copper-based electrocatalysts,may provide a low-cost and long-lasting catalytic system for a profitable industrial-scale CO_(2)RR in the future. 展开更多
关键词 catalyst INTERFACIAL HYDROLYSIS
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NiCu-based catalysts for the low-temperature hydrodeoxygenation of anisole:Effect of the metal ratio on SiO_(2)andγ-Al_(2)O_(3)supports 被引量:1
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作者 Tom Vandevyvere Maarten K.Sabbe +2 位作者 Pedro S.F.Mendes Joris W.Thybaut Jeroen Lauwaert 《Green Carbon》 2023年第2期170-184,共15页
The effects of the metal ratio of NiCu catalysts on the low-temperature hydrodeoxygenation(HDO)of anisole were assessed on a neutral SiO_(2) and an acidicγ-Al_(2)O_(3) support.The activity of SiO_(2)-supported cataly... The effects of the metal ratio of NiCu catalysts on the low-temperature hydrodeoxygenation(HDO)of anisole were assessed on a neutral SiO_(2) and an acidicγ-Al_(2)O_(3) support.The activity of SiO_(2)-supported catalysts increases with the Ni content in the NiCu phase,related to Ni’s hydrogenation capacity.In contrast,on aγ-Al_(2)O_(3) support,the activity decreases with the Ni content.Overall,Al_(2)O_(3)-supported catalysts,exhibiting a smaller NiCu alloy particle size,are more active than SiO_(2)-supported ones.In terms of selectivity,SiO_(2)-supported catalysts mainly hydrogenate anisole to methoxycyclohexane,while,particularly at higher conversions,γ-Al_(2)O_(3)-supported catalysts are able to further convert methoxycyclohexane to cyclohexane,demonstrating the importance of acid sites for low-temperature HDO.The Ni/Cu ratio also steers the selectivity,but not the catalyst stability.Deactivation phenomena are only support dependent:while on SiO_(2)-supported catalysts,active site sintering occurs,attributed to weak stabilization of metal particles by the support,acid catalyzed coking is the main cause of deactivation on theγ-Al_(2)O_(3)-supported catalysts. 展开更多
关键词 BIO-OIL Pyrolysis-oil ANISOLE HYDRODEOXYGENATION Bimetallic catalyst
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Bimetallic Single‑Atom Catalysts for Water Splitting
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作者 Megha A.Deshmukh Aristides Bakandritsos Radek Zbořil 《Nano-Micro Letters》 SCIE EI CAS 2025年第1期1-45,共45页
Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead the global transition to a fossil fuel-independent society.The field of catalysis has been revolutionized by ... Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead the global transition to a fossil fuel-independent society.The field of catalysis has been revolutionized by single-atom catalysts(SACs),which exhibit unique and intricate interactions between atomically dispersed metal atoms and their supports.Recently,bimetallic SACs(bimSACs)have garnered significant attention for leveraging the synergistic functions of two metal ions coordinated on appropriately designed supports.BimSACs offer an avenue for rich metal–metal and metal–support cooperativity,potentially addressing current limitations of SACs in effectively furnishing transformations which involve synchronous proton–electron exchanges,substrate activation with reversible redox cycles,simultaneous multi-electron transfer,regulation of spin states,tuning of electronic properties,and cyclic transition states with low activation energies.This review aims to encapsulate the growing advancements in bimSACs,with an emphasis on their pivotal role in hydrogen generation via water splitting.We subsequently delve into advanced experimental methodologies for the elaborate characterization of SACs,elucidate their electronic properties,and discuss their local coordination environment.Overall,we present comprehensive discussion on the deployment of bimSACs in both hydrogen evolution reaction and oxygen evolution reaction,the two half-reactions of the water electrolysis process. 展开更多
关键词 Single-atom catalysts Single-atom dimers Hydrogen evolution Oxygen evolution Water splitting
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Catalyst–Support Interaction in Polyaniline‑Supported Ni_(3)Fe Oxide to Boost Oxygen Evolution Activities for Rechargeable Zn‑Air Batteries
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作者 Xiaohong Zou Qian Lu +8 位作者 Mingcong Tang Jie Wu Kouer Zhang Wenzhi Li Yunxia Hu Xiaomin Xu Xiao Zhang Zongping Shao Liang An 《Nano-Micro Letters》 SCIE EI CAS 2025年第1期176-190,共15页
Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3... Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3)Fe oxide/PANI)with a robust hetero-interface,which significantly improves oxygen evolution activities with an overpotential of 270 mV at 10 mA cm^(-2)and specific activity of 2.08 mA cm_(ECSA)^(-2)at overpotential of 300 mV,3.84-fold that of Ni_(3)Fe oxide.It is revealed that the catalyst–support interaction between Ni_(3)Fe oxide and PANI support enhances the Ni–O covalency via the interfacial Ni–N bond,thus promoting the charge and mass transfer on Ni_(3)Fe oxide.Considering the excellent activity and stability,rechargeable Zn-air batteries with optimum Ni_(3)Fe oxide/PANI are assembled,delivering a low charge voltage of 1.95 V to cycle for 400 h at 10 mA cm^(-2).The regulation of the effect of catalyst–support interaction on catalytic activity provides new possibilities for the future design of highly efficient OER catalysts. 展开更多
关键词 catalyst-support interaction Supported catalysts HETEROINTERFACE Oxygen evolution reaction Zn-air batteries
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Boosting Oxygen Evolution Reaction Performance on NiFe‑Based Catalysts Through d‑Orbital Hybridization
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作者 Xing Wang Wei Pi +3 位作者 Sheng Hu Haifeng Bao Na Yao Wei Luo 《Nano-Micro Letters》 SCIE EI CAS 2025年第1期281-292,共12页
Anion-exchange membrane water electrolyzers(AEMWEs)for green hydrogen production have received intensive attention due to their feasibility of using earth-abundant NiFe-based catalysts.By introducing a third metal int... Anion-exchange membrane water electrolyzers(AEMWEs)for green hydrogen production have received intensive attention due to their feasibility of using earth-abundant NiFe-based catalysts.By introducing a third metal into NiFe-based catalysts to construct asymmetrical M-NiFe units,the d-orbital and electronic structures can be adjusted,which is an important strategy to achieve sufficient oxygen evolution reaction(OER)performance in AEMWEs.Herein,the ternary NiFeM(M:La,Mo)catalysts featured with distinct M-NiFe units and varying d-orbitals are reported in this work.Experimental and theoretical calculation results reveal that the doping of La leads to optimized hybridization between d orbital in NiFeM and 2p in oxygen,resulting in enhanced adsorption strength of oxygen intermediates,and reduced rate-determining step energy barrier,which is responsible for the enhanced OER performance.More critically,the obtained NiFeLa catalyst only requires 1.58 V to reach 1 A cm^(−2) in an anion exchange membrane electrolyzer and demonstrates excellent long-term stability of up to 600 h. 展开更多
关键词 NiFe-based catalysts d-orbital coupling Oxygen evolution reaction Anion exchange membrane electrolyzer
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Fabrication of highly dispersed carbon doped Cu-based oxides as superior selective catalytic oxidation of ammonia catalysts via employing citric acid-modified carbon nanotubes doping CuAl-LDHs
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作者 Fengrong Li Xuezhen Liu +3 位作者 ZhengYi Zhao Xia An Yali Du Xu Wu 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2023年第11期185-196,共12页
In this work,the CuAl-LDO/c-CNTs catalyst was fabricated via in situ oriented assembly of layered-double hydroxides(LDHs)and citric acid-modified carbon nanotubes(c-CNTs)followed by annealing treatment,and evaluated i... In this work,the CuAl-LDO/c-CNTs catalyst was fabricated via in situ oriented assembly of layered-double hydroxides(LDHs)and citric acid-modified carbon nanotubes(c-CNTs)followed by annealing treatment,and evaluated in the selective catalytic oxidation(SCO)of NH_(3)to N_(2).The CuAl-LDO/c-CNTs catalyst presented better catalytic performance(98%NH_(3)conversion with nearly 90%N_(2)selectivity at 513 K)than other catalysts,such as CuAlO_(x)/CNTs,CuAlO_(x)/c-CNTs and CuAl-LDO/CNTs.Multiple characterizations were utilized to analyze the difference of physicochemical properties among four catalysts.XRD,TEM and XPS analyses manifested that CuO and Cu_(2)O nanoparticles dispersed well on the surface of the Cu Al-LDO/c-CNTs catalyst.Compared with other catalysts,larger specific surface area and better dispersion of CuAl-LDO/c-CNTs catalyst were conducive to the exposure of more active sites,thus improving the redox capacity of the active site and NH_(3)adsorption capacity.In-situ DRIFTS results revealed that the internal selective catalytic reduction(iSCR)mechanism was found over CuAl-LDO/c-CNTs catalyst. 展开更多
关键词 Selective catalytic oxidation of ammonia Layered-double hydroxides cu-based oxides CNTS Citric acid-modified
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