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Recent Advances in Mechanistic Understanding of Metal-Free Carbon Thermocatalysis and electrocatalysis with Model Molecules

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Nano-Micro Letters 2024年第7期16卷 74-97页

作者： Wei Guo Linhui Yu Ling Tang Yan Wan Yangming Lin CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002People’s Republic of China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen 361021People’s Republic of China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002People’s Republic of China Institute of Urban Environment Chinese Academy of SciencesXiamen 361021People’s Republic of China

Metal-free carbon,as the most representative heterogeneous metal-free catalysts,have received considerable interests in electro-and thermo-catalytic reac-tions due to their impressive performance and sustainability.Over the past decade,well-designed carbon catalysts with tunable structures and heteroatom groups coupled with various characterization techniques have proposed numerous reaction mechanisms.However,active sites,key intermediate species,precise structure-activity relationships and dynamic evolution processes of carbon catalysts are still rife with controversies due to the monotony and limitation of used experimental methods.In this Review,we sum-marize the extensive efforts on model catalysts since the 2000s,particularly in the past decade,to overcome the influences of material and structure limitations in metal-free carbon catalysis.Using both nanomolecule model and bulk model,the real contribution of each alien species,defect and edge configuration to a series of fundamentally important reactions,such as thermocatalytic reactions,electrocatalytic reactions,were systematically studied.Combined with in situ techniques,isotope labeling and size control,the detailed reaction mechanisms,the precise 2D structure-activity relationships and the rate-determining steps were revealed at a molecular level.Furthermore,the outlook of model carbon catalysis has also been proposed in this work.

关键词： Metal-free carbon catalysts Model catalyst electrocatalysis Active site Reaction mechanisms

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Research progress on metal-organic framework compounds(MOFs)in electrocatalysis

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Journal of Environmental Sciences 2024年第7期141卷 261-276页

作者： Yutong Guo Shunzheng Zhao Xiaolong Tang Honghong Yi Department of Environmental Science and Engineering School of Energy and Environmental EngineeringUniversity of Science and Technology BeijingBeijing 100083China Beijing Key Laboratory of Resource-oriented Treatment of Industrial Pollutants Beijing 100083China

Metal-organic frameworks(MOFs)have favorable characteristics such as large specific surface area,high porosity,structural diversity,and pore surface modification,giving them great potential for development and attractive prospects in the research area of modern materials electrocatalysis.However,unsatisfactory catalytic activity and poor electronic conductivity are the main challenges facing MOFs.This review focuses on MOF-based materials used in electrocatalysis,based on the types of catalytic reactions that have used MOF-based materials in recent years along with their applications,and also looks at some new electrocatalytic materials and their future development prospects.

关键词： Metal-organic frame compounds electrocatalysis Oxidation-reduction Nitrogen fixation to synthesize ammonia Carbon dioxide reduction

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Wet-chemical synthesis of two-dimensional metal nanomaterials for electrocatalysis

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National Science Review 2022年第5期9卷 37-56页

作者： Zijian Li Li Zhai Yiyao Ge Zhiqi Huang Zhenyu Shi Jiawei Liu Wei Zhai Jinzhe Liang Hua Zhang Department of Chemistry City University of Hong Kong Hong Kong Branch of National Precious Metals Material Engineering Research Center(NPMM) City University of Hong Kong School of Materials Science and Engineering Nanyang Technological University Shenzhen Research Institute City University of Hong Kong

Two-dimensional(2D) metal nanomaterials have gained ever-growing research interest owing to their fascinating physico chemical properties and promising application,especially in the held of ele ctrocatalysis.In this review,we briefly introduce the recent advances in wet-chemical synthesis of 2D metal nanomaterials.Subsequently,the catalytic performances of 2D metal nanomaterials in a variety of electrochemical reactions are illustrated.Finally,we summarize current challenges and highlight our perspectives on preparing high-performance 2D metal electro catalysts.

关键词： two-dimensional metal nanomaterials wet-chemical synthesis phase heterophase electrocatalysis

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Controlling of coordination state of Ru_(x)N_(y) clusters for efficient oxygen reduction electrocatalysis

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Nano Research 2024年第3期17卷 1035-1041页

作者： Weiyang Fu Yihuan Yu Tongtong Liu Yinliang Cao Zhengping Zhang Feng Wang State Key Laboratory of Chemical Resource Engineering Beijing Key Laboratory of Electrochemical Process and Technology for MaterialsBeijing University of Chemical TechnologyBeijing 100029China Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical TechnologyBeijing 100029China Zhejiang Tianneng Hydrogen Energy Technology Co. Ltd.Huzhou 313100China

Ruthenium(Ru)is an attractive potential alternative to platinum as an electrocatalyst for the oxygen reduction reaction(ORR),in virtue of its high catalytic selectivity and relatively low price.In this work,a series of well-dispersed nitrogen-coordinated Ru-clusters on carbon black(Ru_(x)N_(y)/C)were prepared by pyrolyzing different Ru-containing sandwich compounds as the Ru sources.The higher thermal stability of these complexed sandwich precursors(bis(1,2,3,4,5-pentamethylcyclopentadienyl)Ru(II)monomer,dichloro(p-cymene)Ru(II)dimer,and chloro(1,2,3,4,5-pentamethylcyclopentadienyl)Ru(II)tetramer)affords the control of coordinated state for the resulting Ru-clusters,in comparison of that derived from ruthenium chlorides.After the pyrolysis treatment,the Ru coordinated state in Ru_(x)N_(y)/C,with the Ru–N and Ru–Ru bonds,still showed the structural inheritance from the Ru(II)monomer,dimer,and tetramer,but using ruthenium chlorides as the Ru source resulted in the nanoscale Ru agglomerations.The ORR testing exhibited that the Ru_(x)N_(y)/C sample derived from the Ru(II)tetramer(Ru_(x)N_(y)/C-T)presents the higher catalytic activity than the other obtained samples in either alkaline or acidic electrolytes.Even in the acidic electrolyte,Ru_(x)N_(y)/C-T shows the comparable ORR activity to that of Pt/C catalysts,and it shows the superior tolerance against methanol and CO.The X-ray absorption spectroscopy and density functional theory calculations demonstrate that these tetra-nuclear Ru-clusters could be the most active site due to their broadened d-orbital bands and lower energy d-band center than those of other subnano species and nanocrystals,and their favorable Yeager-type adsorption of O_(2)-molecules is also contributed to promoting O–O bond cleavage and accelerating the ORR process.

关键词： ruthenium clusters coordination environment sandwich compounds electrocatalysis oxygen reduction reaction

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Upgrading waste NO_(x)into amino acids via electrocatalysis on Co nanoparticles encapsulated in hollow carbon nanofibers

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Science China Chemistry 2024年第6期67卷 1946-1952页

作者： Jiahui Xian Kaixing Cai Peisen Liao Shihan Wang Guangqin Li Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education LIFMIGCMESchool of ChemistrySun Yat-Sen UniversityGuangzhou510275China

Electrocatalytic conversion of waste nitrogen oxide(NO_(x))into value-added nitrogenous chemicals,especially amino acid,is an emerging strategy to alleviate NO_(x)pollution.However,this process suffers from the coexistence of multiple competitive reactions leading to complex product distribution and low efficiency,and thus the rational design and modulation of efficient catalysts remains a formidable challenge.Herein,well-designed Co nanoparticles encapsulated in hollow carbon nanofiber(CoHCNF)were constructed to promote the amino acid electrosynthesis via dealing waste NO_(x)coupling with biomass-derived keto acids.Ascribed to the rapid reactant diffusion,electron transport and efficient contact with abundant accessible Co catalytic sites stemmed from the unique hollow nanotubular structure,Co-HCNF manifested impressive glycine synthesis performance in one-pot adopting NO as the nitrogen source with Faradaic efficiency(FE)of 41.7%and a corresponding yield rate of 222.3μmol h^(-1)as well as 120 h robust stability.Interestingly,it also demonstrates an excellent performance with the FE of 42.8%for NO_(3)~-solution as the nitrogen source.Specially,this strategy displays a broad universality for the synthesis of other amino acids.This work not only highlights the importance of hollow-structuring electrocatalyst towards upgrading wasted NO_(x)species into amino acids,but also promotes the further development of electrosynthetic systems for high-valued N-containing organic chemicals.

关键词： electrocatalysis NO_(x)reduction amino acid porous materials hollow structure

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Standard-state entropies and their impact on the potential-dependent apparent activation energy in electrocatalysis

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能源化学:英文版 2023年第8期83卷 247-254,I0008页

作者： Kai S.Exner Universty Duisburg-Essen Faculty of ChemstryTheretical Inorganic ChemtryUniversitatsstrae 545141 EssenGemay Cluster of Excellence RESOLV 44801 BochumGermany Center for Nanointegration(CENIDE)Duisburg-Essen 47057 DuisburgGermany

The apparent activation energy,Eapp,is a common measure in thermal catalysis to discuss the activity and limiting steps of catalytic processes on solid-state materials.Recently,the electrocatalysis community adopted the concept of Eappand combined it with the Butler-Volmer theory.Certain observations though,such as potential-dependent fluctuations of Eapp,are yet surprising because they conflict with the proposed linear decrease in Eappwith increasing overpotential.The most common explanation for this finding refers to coverage changes upon alterations in the temperature or the applied electrode potential.In the present contribution,it is demonstrated that the modulation of surface coverages cannot entirely explain potential-dependent oscillations of Eapp,and rather the impact of entropic contributions of the transition states has been overlooked so far.In the case of a nearly constant surface coverage,these entropic contributions can be extracted by a dedicated combination of Tafel plots and temperature-dependent experiments.

关键词： electrocatalysis Standard-state entropy Microkinetic modeling Apparent activation energy Degree of rate control

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Gap engineering of sandwich plasmonic gap nanostructures for boosting plasmon-enhanced electrocatalysis

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Nano Research 2023年第7期16卷 8961-8969页

作者： Lu Cheng Fengxia Wu Yu Tian Xiali Lv Fenghua Li Guobao Xu Hsien-Yi Hsu Yongjun Zhang Wenxin Niu State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Yanshan Branch of Beijing Chemical Research Institute SinopecBeijing 102500China University of Science and Technology of China Hefei 230026Chin a 4 School of Energy and Environment Department of Materials Science and EngineeringCity University of Hong KongKowloon TongHong Kong 999077China Shenzhen Research Institute of City University of Hong Kong Shenzhen 518057China Key Laboratory of Functional Polymer Materials and State Key Laboratory of Medicinal Chemical Biology Institute of Polymer ChemistryCollege of ChemistryNankai UniversityTianjin 300071China

Plasmonic catalysis is emerging as a dynamic field in heterogeneous catalysis and holds great promise for the efficient utilization of solar energy.Central to the development of plasmonic catalysis is the design of efficient plasmonic nanocatalysts.In this report,plasmonic gap nanostructures(PGNs)on the basis of Au@poly(o-phenylenediamine)(POPD)@Pd sandwich nanostructures are synthesized as plasmonic nanocatalysts by an in-situ reduction synthetic strategy,which allows for the precise engineering of the POPD gap size between plasmonic Au and catalytic Pd components.The introduction of conducting POPD nanogap in PGNs not only effectively enhances their light harvesting capability,but also provides an effective charge transfer channel for harnessing the photogenerated hot charge carriers.In this respect,distinct gap-dependent performances in plasmon-enhanced electrocatalysis of ethanol oxidation reactions(EOR)are demonstrated with the PGN nanocatalysts and over 2.5 folds of enhancement can be achieved.A volcano plot is derived to describe the relationship between the catalytic activities and gap size of the PGN nanocatalysts,which is well explained by the interplay of their light harvesting and charge transport capabilities.These results highlight the importance of gap engineering in PGNs for plasmonic catalysis and offer the promise of developing efficient plasmonic nanocatalysts for other heterogeneous catalytic reactions.

关键词： plasmonic gap nanostructures electrocatalysis ethanol oxidation reactions light harvesting charge transport

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Heterojunction interface editing in Co/NiCoP nanospheres by oxygen atoms decoration for synergistic accelerating hydrogen and oxygen evolution electrocatalysis

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Nano Research 2023年第7期16卷 8765-8772页

作者： Yan Lin Xiaojiao Cui Yilin Zhao Zhicheng Liu Guoxin Zhang Yuan Pan College of Energy Storage Technology Shandong University of Science and TechnologyQingdao 266590China State Key Laboratory of Heavy Oil Processing China University of Petroleum(East China)Qingdao 266580China

Controllable designing of well-defined heterojunction nanostructures provides an insightful strategy for accelerating the kinetics of the hydrogen and oxygen evolution reactions(HER/OER),but such task is still challenging.Herein,we proposed a protocol of heterojunction interface editing(HIE)strategy by oxygen atoms decoration for synergistic boosting electrocatalytic HER and OER performances.A novel Co/NiCoP nanospheres(NSs)heterojunction was synthesized by crystal seed template transformation method with Ni_(5)P_(4) microspheres as seeds.The effective oxygen atoms interface editing increased the oxidation state of Co atoms and prolonged the Co-P bond length of Co/NiCoP NSs heterojunction,thus the electron localization on P sites was enhanced,leading to the dramatically elevated HER and OER performances simultaneously.The as-constructed O-Co/NiCoP NSs show excellent electrocatalytic activity with 361 and 430 mV vs.reversible hydrogen electrode(RHE)to arrive high current density of 300 mA·cm^(-2)for HER and OER in 1 M KOH as well as good stability.The proposed HIE concept could provide a new perspective on the catalyst design for energy conversion systems.

关键词： transition metal phosphides heterojunction nanocrystals synthesis bifunctional catalyst electrocatalysis

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Cerium-based nanomaterials for photo/electrocatalysis

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Science China Chemistry 2023年第8期66卷 2204-2220页

作者： Ge Li Ping Wang Miao He Xilin Yuan Lulin Tang Zhenxing Li State Key Laboratory of Heavy Oil Processing College of New Energy and MaterialsChina University of Petroleum(Beijing)Beijing102249China

The localization and incomplete filling of 4f electrons endow cerium(Ce)with the great potential in electrocatalysis and photocatalysis.The unique 5d empty orbital of Ce elements can be used as a hydrogen“trap”site,which is conducive to the recombination of hydrogen ions or atoms and effectively promotes the desorption of hydrogen molecules in electrocatalysis.Meanwhile,due to the stable crystal structure,excellent oxygen mobility,and good optical properties,Ce-based nanomaterials are considered as one of the most desirable photocatalytic catalysts and widely used in atmospheric conditions.Therefore,cerium-based nanomaterials have considerable application prospects in photocatalysis and electrocatalysis.In this review,we summarize the preparation methods of Ce-based nanomaterials,and discuss the application of Ce-based nanomaterials in electrocatalysis and photocatalysis.Among them,electrocatalysis applications include the following:oxygen reduction reaction(ORR),hydrogen evolution reaction(HER),oxygen evolution reaction(OER),CO_(2) reduction reaction(CO_(2)RR),and other electrocatalysis,and photocatalysis applications include HER,CO_(2)RR,photodegradation,and other photocatalysis.Through the summary of present progress in the application of Ce-based nanomaterials in electrocatalytic and photocatalytic reaction,this review provides a reasonable prospect on the Ce-based nanomaterials in electrocatalysis and photocatalysis.

关键词： Ce-based nanomaterials electrocatalysis photocatalysis oxygen reduction reaction hydrogen evolution reaction oxygen evolution reaction carbon dioxide reduction reaction

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Scalable solid-phase synthesis of defect-rich graphene for oxygen reduction electrocatalysis

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Green Energy & Environment 2023年第1期8卷 224-232页

作者： Chunxiao Dong Li Yang Cheng Lian Xiaoling Yang Yihua Zhu Hongliang Jiang Chunzhong Li Shanghai Engineering Research Center of Hierarchical Nanomaterials School of Materials Science and EngineeringEast China University of Science and TechnologyShanghai200237China Key Laboratory for Ultrafine Materials of Ministry of Education School of Chemical EngineeringEast China University of Science and TechnologyShanghai200237China Institutes of Physical Science and Information Technology Anhui UniversityHefeiAnhui230601China School of Chemistry and Molecular Engineering East China University of Science and TechnologyShanghai200237China

Defect-engineered carbon materials have been emerged as promising electrocatalysts for oxygen reduction reaction(ORR)in metal-air batteries.Developing a facile strategy for the preparation of highly active nanocarbon electrocatalysts remains challenging.Herein,a low-cost and simple route is developed to synthesize defective graphene by pyrolyzing the mixture of glucose and carbon nitride.Molecular dynamics simulations reveal that the graphene formation is ascribed to two-dimensional layered feature of carbon nitride,and high compatibility of carbon nitride/glucose systems.Structural measurements suggest that the graphene possesses rich edge and topological defects.The graphene catalyst exhibits higher power density than commercial Pt/C catalyst in a primary Zn-air battery.Combining experimental results and theoretical thermodynamic analysis,it is identified that graphitic nitrogen-modified topological defects at carbon framework edges are responsible for the decent ORR performance.The strategy presented in this work can be can be scaled up readily to fabricate defective carbon materials.

关键词： Carbon materials electrocatalysis Oxygen reduction reaction Solid-phase synthesis Zn-air battery

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