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Nano Research 2024年第4期17卷 2360-2367页

作者： Xiao-Yan Li Manyi Duan Pengfei Ou Department of Electrical and Computer Engineering University of TorontoTorontoOntario M5S 1A4Canada School of Physics and Electronic Engineering Sichuan Normal UniversityChengdu 610101China Department of Chemistry Northwestern UniversityEvanstonIL 60208USA

The discovery of metal-nitrogen centers as the active sites for electrolysis has aroused significant interest in utilizing single-atom catalysts for nitrogen reduction reaction(NRR).Properly designed nanostructured catalysts that strongly interact with nitrogen molecules(N_(2))can promote adsorption and activation,thereby resulting in efficient catalysts with high stability,activity,and selectivity.In this study,using density functional theory calculations,we selected monolayer black phosphorus(BP)as the substrate and screened a series of single-atom transition metals confined in tri-coordinated and tetra-coordinated active centers(without and with N dopants)to electro-catalyze NRR.As a result,we have identified two promising candidates(Hf_(1)-N_(1)P_(2)-1 and Tc_(1)-N_(4)),which exhibit not only low overpotentials of 0.56 and 0.49 V but also high thermodynamic and electrochemical stability,as well as good selectivity towards NRR over the competing hydrogen evolution reaction.We also demonstrate the ability of Hf_(1)-N_(1)P_(2)-1 and Tc_(1)-N_(4) to activate and hydrogenate N_(2) by donating electrons and regulating charge transfer.This study not only predicts new BP-based promising catalysts but also provides guidance for the rational design of high-performance NRR electrocatalysts under ambient conditions.

关键词： N_(2) electroreduction reaction single-atom catalysts black phosphorus density functional theory high-throughput calculations

single-atom catalysts for the electrochemical reduction of carbon dioxide into hydrocarbons and oxygenates

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Carbon Energy 2024年第3期6卷 64-117页

作者： Karl Adrian Gandionco Juwon Kim Lieven Bekaert Annick Hubin Jongwoo Lim Department of Chemistry Seoul National UniversitySeoulRepublic of Korea Research Group Electrochemical and Surface Engineering(SURF) Department of Materials and ChemistryVrije Universiteit BrusselBrusselsBelgium

The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic material and renewable energy-generated electricity drive the conversion of carbon dioxide into high-value chemicals and carbon-neutral fuels.Over the past few years,single-atom catalysts have been intensively studied as they could provide near-unity atom utilization and unique catalytic performance.single-atom catalysts have become one of the state-of-the-art catalyst materials for the electrochemical reduction of carbon dioxide into carbon monoxide.However,it remains a challenge for single-atom catalysts to facilitate the efficient conversion of carbon dioxide into products beyond carbon monoxide.In this review,we summarize and present important findings and critical insights from studies on the electrochemical carbon dioxide reduction reaction into hydrocarbons and oxygenates using single-atom catalysts.It is hoped that this review gives a thorough recapitulation and analysis of the science behind the catalysis of carbon dioxide into more reduced products through singleatom catalysts so that it can be a guide for future research and development on catalysts with industry-ready performance for the electrochemical reduction of carbon dioxide into high-value chemicals and carbon-neutral fuels.

关键词： electrocatalysis electrochemical CO_(2)reduction hydrocarbons oxygenates single-atom catalysts

Shedding light on the reversible deactivation of carbon-supported single-atom catalysts in hydrogenation reaction

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Nano Research 2024年第6期17卷 4807-4814页

作者： Runze Chen Xiaoying Wang Jianfei Dang Songjie Yun Liqiang Wang Fangong Kong You-Nian Liu State Key Laboratory of Biobased Material and Green Papermaking Qilu University of TechnologyJinan 250353China School of Material Science and Engineering Zhengzhou UniversityZhengzhou 450001China School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China Hunan Provincial Key Laboratory of Micro&Nano Materials Interface Science College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China

Carbon-supported single-atom catalysts were found to suffer reversible deactivation in catalytic hydrogenation,but the mechanism is still unclear.Herein,nitro compounds hydrogenation catalyzed by N-doped carbon-supported Co single atom(Co1/NC)was taken as a model to uncover the mechanism of the reversible deactivation phenomenon.Co1/NC exhibited moderate adsorption towards the substrate molecules(i.e.,nitro compounds or related intermediates),which could be strengthened by the confinement effect from the porous structure.Consequently,substrate molecules tend to accumulate within the pore channel,especially micropores that host Co1,making it difficult for the reactants to access the active sites and finally leading to their deactivation.The situation could be even worse when the substrate molecules possess a large size.Nevertheless,the catalytic activity of Co1/NC could be restored via a simple thermal treatment,which could remove the adsorbates within the pore channel,hence releasing active sites that were originally inaccessible to reactants.

关键词： single-atom catalysts porous carbon support reversible deactivation mechanistic study hydrogenation reaction

Selective oxygen electroreduction to hydrogen peroxide in acidic media:The superiority of single-atom catalysts

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Nano Research 2024年第6期17卷 4668-4681页

作者： Ergui Luo Tongtong Yang Jingyi Liang Yuhong Chang Junming Zhang Tianjun Hu Junjie Ge Jianfeng Jia Key Laboratory of Magnetic Molecules and Magnetic Information Materials of Ministry of Education School of Chemistry and Materials ScienceShanxi Normal UniversityTaiyuan 030032China School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China State Key Laboratory of Electroanalytic Chemistry Jilin Province Key Laboratory of Low Carbon Chemistry PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Two-electron oxygen reduction reaction(2e-ORR)provides an environmentally friendly direction for the on-site production of hydrogen peroxide(H_(2)O_(2)).Central to this technology is the exploitation of efficient,economical,and safe 2e-ORR electrocatalysts.This overview starts with the fundamental chemistry of ORR to highlight the decisive role of adsorbing intermediates on the reaction pathway and activity,followed by a comprehensive survey of the tuning strategies to favor 2e-ORR on traditional precious metals.The latest achievements in designing efficient and selective precious-metal-based single-atom catalysts(SACs)and metal-nitrogen-carbon(M-Nx/C)catalysts,from the aspects of material synthesis,theoretical calculations,and mass transport promotion,are systematically summarized.Brief introductions on the evaluation metrics for 2e-ORR catalysts and the primary reactor designs for cathodic H_(2)O_(2)synthesis are also included.We conclude this review with an outlook on the challenges and direction of efforts to advance electrocatalytic 2e-ORR into realistic H_(2)O_(2)production.

关键词： oxygen reduction reaction H_(2)O_(2)production single-atom catalysts selectivity

In-situ observation of structural evolution of single-atom catalysts:From synthesis to catalysis

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ChemPhysMater

ChemPhysMater 2024年第1期3卷 24-35页

作者： Lei Wang Shuyuan Lyu Shuohao Li School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225009China School of Art and Design Huaiyin Institute of TechnologyHuaian 223003China School of Safety Engineering China University of Mining and TechnologyXuzhou 221116China

atomically dispersed single-atom catalysts(SACs)have been extensively studied over the past decade because of their high atom utilization efficiencies and specific selectivities.Although numerous strategies have been proposed to obtain SACs with high densities and stabilities,the transformation mechanism that occurs during the reaction is still unclear.This review summarizes the structural evolution of SACs in the preparation process and reaction with various electron microscopy techniques at atomic scale under environmental conditions.Current state-of-the-art environmental electron microscopy studies on SACs mainly focus on porous carbons,metals or metal oxides,and some specific composite materials.The dynamic evolution of SACs under various reaction conditions is also investigated in this study.Finally,we highlight the challenges and drawbacks of the current studies and the prospects for the future exploration of SACs with environmental strategies.

关键词： single-atom catalysts Structural transformation atomization Environmental electron microscope

MBenes-supported single-atom catalysts for oxygen reduction and oxygen evolution reactions by first-principles study and machine learning

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National Science Open 2024年第2期3卷 56-73页

作者： Erpeng Wang Guanjie Wang Jian Zhou Zhimei Sun School of Materials Science and Engineering Beihang UniversityBeijing 100191China Center for Integrated Computational Materials Engineering International Research Institute for Multidisciplinary ScienceBeihang UniversityBeijing 100191China

Oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)are key catalytic processes in various renewable energy conversion and energy storage technologies.Herein,we systematically investigated the ORR and OER catalytic activity of the single-atom catalysts(SACs)composed of 4d/5d period transition metal(TM)atoms embedded on MBene substrates(TM-M_(2)B_(2)O_(2),M=Ti,Mo,and W).We found that TM dominates the catalytic activity compared to the MBene substrates.The SACs embedded with Rh,Pd,Au,and Ir exhibit excellent ORR or OER catalytic activity.Specifically,Rh-Mo2B2O2and Rh-W2B2O2are promising bifunctional catalysts with ultra-low ORR/OER overpotentials of 0.39/0.21 V and0.19/0.32 V,respectively,lower than that of Pt/RuO_(2)(0.45/0.42 V).Importantly,through machine learning,the models containing 10 element features of SACs were developed to quickly and accurately identify the superior ORR and OER electrocatalysts.Our findings provide several promising SACs for ORR and OER,and offer effective models for catalyst design.

关键词： oxygen reduction reaction oxygen evolution reaction single-atom catalysts catalytic activity machine learning

Recent advances in Fe-N-C single-atom site coupled synergistic catalysts for boosting oxygen reduction reaction

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Electron 2024年第1期2卷 1-38页

作者： Katam Srinivas Jian Zhen Hesheng Yu Dawei Liu Jian Zhen Ou Ming‐qiang Zhu Yuanfu Chen School of Integrated Circuit Science and Engineering and State Key Laboratory of Electronic Thin Films and Integrated DevicesUniversity of Electronic Science and Technology of ChinaChengduSichuanChina College of Mechanical and Electronic Engineering Northwest A&F UniversityYanglingChina School of Engineering RMIT UniversityMelbourneVictoriaAustralia

Metal-air batteries,fuel cells,and electrochemical H_(2)O2 production currently attract substantial consideration in the energy sector owing to their efficiency and eco-consciousness.However,their broader use is hindered by the complex oxygen reduction reaction(ORR)that occurs at cathodes and involves intricate electron transfers.Despite the significant ORR performance of platinum-based catalysts,their high cost,operational limitations,and susceptibility to methanol poisoning hinder broader implementation.This emphasizes the need for efficient nonprecious metal-based ORR electrocatalysts.A promising approach involves utilizing single-atom catalysts(SACs)featuring metal-nitrogen-carbon(M-N-C)coordination sites.SACs offer advantages such as optimal utilization of metal atoms,uniform active centers,precisely defined catalytic sites,and robust metal-support interactions.However,the symmetrical electron distribution around the central metal atom of a single-atom site(M-N4)often results in suboptimal ORR performance.This challenge can be addressed by carefully tailoring the surrounding environment of the active center.This review specifically focuses on recent advancements in the Fe-N4 environment within Fe-N-C SACs.It highlights the promising strategy of coupling Fe-N4 sites with metal clusters and/or nanoparticles,which enhances intrinsic activity.By capitalizing on the interplay between Fe-N4 sites and associated species,overall ORR performance improved.The review combines findings from experimental studies and density functional theory simulations,covering synthesis strategies for Fe-N-C coupled synergistic catalysts,characterization techniques,and the influence of associated particles on ORR activity.By offering a comprehensive outlook,the review aims to encourage research into high-efficiency Fe single-atom sites coupled synergistic catalysts for real-world applications in the coming years.

关键词： electrocatalysis oxygen reduction reaction particle@Fe-N-C single-atom catalysts synergistic catalysts

Progress and perspective of single-atom catalysts for membrane electrode assembly of fuel cells

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Carbon Energy 2023年第7期5卷 38-56页

作者： Zhongxin Song Junjie Li Qianling Zhang Yongliang Li Xiangzhong Ren Lei Zhang Xueliang Sun College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhenChina Department of Mechanical and Materials Engineering The University of Western OntarioLondonOntarioCanada

A fuel cell is an energy conversion device that can continuously input fuel and oxidant into the device through an electrochemical reaction to release electrical energy.Although noble metals show good activity in fuel cell-related electrochemical reactions,their ever-increasing price considerably hinders their industrial application.Improvement of atom utilization efficiency is considered one of the most effective strategies to improve the mass activity of catalysts,and this allows for the use of fewer catalysts,saving greatly on the cost.Thus,single-atom catalysts(SACs)with an atom utilization efficiency of 100%have been widely developed,which show remarkable performance in fuel cells.In this review,we will describe recent progress on the development of SACs for membrane electrode assembly of fuel cell applications.First,we will introduce several effective routes for the synthesis of SACs.The reaction mechanism of the involved reactions will also be introduced as it is highly determinant of the final activity.Then,we will systematically summarize the application of Pt group metal(PGM)and nonprecious group metal(non-PGM)catalysts in membrane electrode assembly of fuel cells.This review will offer numerous experiences for developing potential industrialized fuel cell catalysts in the future.

关键词： fuel cells membrane electrode assembly oxygen reduction reaction reaction mechanism single-atom catalysts

Coordination environments tune the activity of oxygen catalysis on single atom catalysts:A computational study

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Nano Research 2022年第4期15卷 3073-3081页

作者： Gaofan Xiao Ruihu Lu Jianfeng Liu Xiaobin Liao Zhaoyang Wang Yan Zhao State Key Laboratory of Silicate Materials for Architectures International School of Materials Science and EngineeringWuhan University of TechnologyWuhan 430070China The Institute of Technological Sciences Wuhan UniversityWuhan 430072China

Designing highly efficient bifunctional electrocatalysts for oxygen reduction and evolution reaction(ORR/OER)is extremely important for developing regenerative fuel cells and metal-air batteries.single-atom catalysts(SACs)have gained considerable attention in recent years because of their maximum atom utilization efficiency and tunable coordination environments.Herein,through density functional theory(DFT)calculations,we systematically explored the ORR/OER performances of nitrogencoordinated transition metal carbon materials(TM-N_(x)-C(TM=Mn,Fe,Co,Ni,Cu,Pd,and Pt;x=3,4))through tailoring the coordination environment.Our results demonstrate that compared to conventional tetra-coordinated(TM-N_(4)-C)catalysts,the asymmetric tri-coordinated(TM-N_(3)-C)catalysts exhibit stronger adsorption capacity of catalytic intermediates.Among them,Ni-N_(3)-C possesses optimal adsorption energy and the lowest overpotential of 0.29 and 0.28 V for ORR and OER,respectively,making it a highly efficient bifunctional catalyst for oxygen catalysis.Furthermore,we find this enhanced effect stems from the additional orbital interaction between newly uncoordinated d-orbitals and p-orbitals of oxygenated species,which is evidently testified via the change of d-band center and integral crystal orbital Hamilton population(ICOHP).This work not only provides a potential bifunctional oxygen catalyst,but also enriches the knowledge of coordination engineering for tailoring the activity of SACs,which may pave the way to design and discover more promising bifunctional electrocatalysts for oxygen catalysis.

关键词： single-atom catalysts density functional theory oxygen reduction reaction oxygen evolution reaction coordination environments

Computational study of transition metal single-atom catalysts supported on nitrogenated carbon nanotubes for electrocatalytic nitrogen reduction

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Nano Research 2023年第1期16卷 325-333页

作者： Yanyang Qin Yan Li Wenshan Zhao Shenghua Chen Tiantian Wu Yaqiong Su School of Chemistry Xi'an Key Laboratory of Sustainable Energy Materials ChemistryState Key Laboratory of Electrical Insulation and Power EquipmentXi'an Jiaotong UniversityXi'an 710049China Department of Chemistry Tsinghua UniversityBeijing 100084China

Developing efficient and stable catalysts for the electrocatalytic N_(2)reduction reaction(NRR)shows promise in nitrogen fixation.Here,we proposed active and stable single-atom catalysts(SACs)toward NRR,where transition metals are anchored on nitrogenated carbon nanotubes(NCNTs).Among the screened nine common transition metals(Ti,V,Cr,Mn,Fe,Mo,Ru,Rh,and Ag)on(4,4)NCNTs,we found Mo-NCNT possesses the most excellent NRR catalytic activity and selectivity with a low overpotential of 0.29 V.Then,the NRR performance of Mo-NCNT was further engineered by controlling the nanotube diameter,where the lowest overpotential is 0.18 V at a diameter of 9.6Å.In addition,we found a linear scaling relation between*NNH and*NH_(2)on the studied catalysts with the exception of(2,2)and(3,3)Mo-NCNTs,owing to their extremely unstable structures.We attribute the outstanding NRR performance of Mo-NCNT to the moderate adsorption of N_(2)due to the slightly low d-band center of Mo,and the charge donating and accepting capacity of NCNTs.This work has provided a deeper insight into designing highefficiency and stable NRR SACs supported by NCNTs.

关键词： nitrogen reduction single-atom catalysts density functional theory(DFT) carbon nanotubes nitrogen doping