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Electrochemical Energy Reviews 2022年第4期5卷 222-252页

作者： Yiqun Chen Junru Zhang Lijun Yang Xizhang Wang Qiang Wu Zheng Hu Key Laboratory of Mesoscopic Chemistry of MOE School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023JiangsuChina

The carbon dioxide electroreduction reaction(CO_(2)RR)to fuels and/or chemicals is an efficient prospective strategy to realize global carbon management using intermittent electric energy harvested from renewable sources.Highly efficient inexpensive electrocatalysts are required to achieve high energy and Faradaic efficiencies as well as fast conversion.metal-nitrogen-carbon(M-N-C)single-site catalysts(SSCs)are highly competitive over precious metal catalysts in the CO_(2)RR to CO due to their high performance,easy regulation and low cost.In the past six years,intensive studies of M-N-C SSCs for CO_(2)RR to CO have been performed,and great progress has been achieved.This review focuses on the important topic of CO_(2)RR to CO with M-N-C SSCs.We first introduce the reaction mechanism of the CO_(2)RR to CO and the regulation of the electronic structure from a theoretical viewpoint.Then,the construction of M-N-C SSCs and the regulation of the electronic structure are demonstrated experimentally.The up-to-date electrocatalytic performance of M-N-C SSCs with different metal centers(Ni,Fe,Co and others)is summarized and compared systematically to highlight structure-performance correlations that were considered from both theoretical and experimental perspectives.Finally,the opportunities,challenges and future outlooks are summarized to deepen and widen research and applications in this promising field.

关键词： CO_(2)electroreduction reaction metal-nitrogen-carbon Single-site catalysts Electronic structure CO

Single-atom metal-nitrogen-carbon catalysts energize single molecule detection for biosensing

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InfoMat 2023年第6期5卷 44-65页

作者： Xianyang Zhang Pengfei Chen Siwuxie He Bowen Jiang Yong Wang Yonghua Cheng Jian Peng Francis Verpoort John Wang Zongkui Kou State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhanthe People's Republic of China “ZhuCai”Center of Innovation and Entrepreneurship Wuhan University of TechnologyWuhanthe People's Republic of China West China School of Pharmacy Sichuan UniversityChengduthe People's Republic of China Department of Materials Science and Engineering Faculty of EngineeringNational University of SingaporeSingapore Institute of Materials Research and Engineering A*StarSingapore

Biosensors featuring single molecule detection present huge opportunities as well as challenges in food safety inspection,disease diagnosis,and environmental monitoring.Single-molecule detection is largely lacking of high enough activity,precision molecule selectivity,and understanding in the exact operating mechanism.Single-atom catalysts(SACs),especially those metals-nitrogen-carbon that mimic the natural metalloenzyme structure,and with well-defined metal atom bond configurations,high level of molecular selectivity,and easy fabrication,endow single molecule detections with practical-use feasibilities.The recent advances in single-atom catalysts also present new pathways in the key mechanism understandings.In this short review,we will first visit the brief history and advantages of SACs that have been explored only recently for molecule-scale biosensors,where they are analogous and also differentiated from those nanozymes and natural metalloenzymes.Their applications in electrochemical,photochemical,and photoelectrochemical sensors are then discussed comprehensively by focusing on the different molecule-scale sensing modes in achieving local coordination-modulated signal amplifications.Finally,we identify new opportunities and challenges faced by these SACs-based single molecule detections in the further development of biosensors.

关键词： biosensors metal-nitrogen-carbon nanozyme single molecule detection single-atom catalysts

Advanced transition metal/nitrogen/carbon-based electrocatalysts for fuel cell applications

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Science China Chemistry 2020年第11期63卷 1517-1542页

作者： Tang Tang Liang Ding Zhe Jiang Jin-Song Hu Li-Jun Wan Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Molecular Nanostructure and NanotechnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

The development of advanced transition metal/nitrogen/carbon-based(M/N/C)catalysts with high activity and extended durability for oxygen reduction reaction(ORR)is critical for platinum-group-metal(PGM)free fuel cells but still remains great challenging.In this review,we summarize the recent progress in two typical M/N/C catalysts(atomically dispersed metal-nitrogen-carbon(M-N-C)catalysts and carbon-supported metal nanoparticles with N-doped carbon shells(M@NC))with an emphasis on their potential applications in fuel cells.Starting with understanding the active sites in these two types of catalysts,the representative innovative strategies for enhancing their intrinsic activity and increasing the density of these sites are systematically introduced.The synergistic effects of M-N-C and M@NC are subsequently discussed for those M/N/C catalysts combining both of them.To translate the material-level catalyst performance into high-performance devices,we also include the recent progress in engineering the porous structure and durability of M/N/C catalysts towards efficient performance in fuel cell devices.From the viewpoint of industrial applications,the scale-up cost-effective synthesis of M/N/C catalysts has been lastly briefed.With this knowledge,the challenges and perspectives in designing advanced M/N/C catalysts for potential PGM-free fuel cells are proposed.

关键词： electrocatalysis ORR metal-nitrogen-carbon M@NC fuel cells oxygen reduction

Atomic Level Dispersed metal–nitrogen–carbon Catalyst toward Oxygen Reduction Reaction: Synthesis Strategies and Chemical Environmental Regulation

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Energy & Environmental Materials 2021年第1期4卷 5-18页

作者： Hengbo Yin Huicong Xia Shuyan Zhao Kexie Li Jianan Zhang Shichun Mu College of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

For development and application of proton exchange membrane fuel cell(PEMFC) energy transformation technology, the cost performance must be elevated for the catalyst. At present, compared with noble metal-based catalysts, such as Pt-based catalysts, atomically dispersed metal–nitrogen–carbon(M–N–C) catalysts are popularity and show great potential in maximizing active site density, high atom utilization and high activity,making them the first choice to replace Pt-based catalysts. In the preparation of atomically dispersed metal–nitrogen–carbon catalyst, it is difficult to ensure that all active sites are uniformly dispersed, and the structure system of the active sites is not optimal. Based on this, we focus on various approaches for preparing M–N–C catalysts that are conducive to atomic dispersion, and the influence of the chemical environmental regulation of atoms on the catalytic sites in different catalysts. Therefore, we discuss the chemical environmental regulation of the catalytic sites by bimetals, atom clusters, and heteroatoms(B, S, and P). The active sites of M–N–C catalysts are explored in depth from the synthesis and characterization, reaction mechanisms, and density functional theory(DFT)calculations. Finally, the existing problems and development prospects of the current atomic dispersion M–N–C catalyst are proposed in detail.

关键词： atomic-level catalyst chemical environmental effects metal-nitrogen-carbon oxygen reduction reaction synthesis strategy

Molten salt electrochemical modulation of Ni/Co nanoparticles onto N-doped carbon for oxygen reduction

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Journal of Energy Chemistry 2022年第11期31卷 212-217,I0007页

作者： Xinxin Liang Jialin Chen Biao Hong Tingting Wan Wei Weng Wei Xiao College of Chemistry and Molecular Sciences Hubei Key Laboratory of Electrochemical Power SourcesWuhan UniversityWuhan 430072HubeiChina Zijin School of Geology and Mining Fujian Key Laboratory of Green Extraction and High-value Utilization of Energy MetalsFuzhou UniversityFuzhou 350108FujianChina Queen Marry University of London Engineering School Northwestern Polytechnical UniversityXi’an 710129ShaanxiChina

Activation of oxygen over non-precious materials has been an imperative task to develop efficient electrochemical energy storage and conversion such as fuel cells and metal-air batteries.Herein,a molten salt electrochemical modulation of metal-nitrogen-carbon based compounds(M–N–C)is achieved.By electrochemical treatment of polydopamine-coated NiCo_(2)O_(4)(NiCo_(2)O_(4)@PDA)in molten Li_(2)CO_(3)-Na_(2)CO_(3)-K_(2)CO_(3)at 500℃,Ni/Co bimetal-nitrogen-carbon catalyst(denoted as Ni/Co@NC)consisting of Ni-Co nanoparticles anchoring on porous nitrogen-doped carbon is constructed and evaluated as electrocatalysts towards the oxygen reduction reaction(ORR).Experimental and calculation results confirm that alloying of Ni-Co and nitrogen doping to carbon enhances the rate-determining transformation of*OH intermediate during ORR.The Ni/Co@NC hence shows an ORR activity comparable with the commercial Pt/C.

关键词： Oxygen reduction metal-nitrogen-carbon Electrochemistry Molten salt Bimetal modulation

Single-Cu-atoms anchored on 3D macro-porous carbon matrix as efficient catalyst for oxygen reduction and Pt co-catalyst for methanol oxidation

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Chinese Chemical Letters 2022年第5期33卷 2585-2589页

作者： Jin Ma Bin Liu Rongyue Wang Zhiyao Sun Ying Zhang Yubo Sun Zhuang Cai Yao Li Jinlong Zou Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People’s Republic of ChinaSchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080China

Single metal atoms immobilized on a carbon substrate are of great potential for enhancing the catalytic activities for oxygen reduction and methanol oxidation reactions(ORR/MOR)owing to the maximized atom utilization.Herein,single copper atoms(SCAs)are loaded on macro-porous nitrogen-doped carbon(Cu-NC)derived from zeolitic imidazolate framework-8(ZIF-8),which are used as catalysts for ORR and Pt-supports for MOR.For ORR,the catalyst marked as Cu-NC-3 exhibits a higher peak potential of 0.87 V(vs.Reversible hydrogen electrode)than that of commercial Pt/C(0.83 V),mainly attributing to that the 3D macro-porous structure of Cu-NC-3 provides adequate space for uniform dispersion of SCAs as the main active species,and smooth diffusion pathways for fast transport of substances(O_(2),H_(2)O),therefore reducing the overpotential and the intermediate(H_(2)O_(2))generation to enhance ORR activity.For MOR,Pt-Cu-NC-3 has a higher mass activity of 1217.4 mA/mg Pt than that of Pt/C(752.4 mA/mg Pt),and its activity maintenance(decline of 27.6%)is also better than Pt/C(decline of 44.0%)after 5000 cyclic voltammetry(CV)cycles.The interactions between SCAs and Pt nanoparticles should facilitate the generation of OH−from water molecules,which can fast eliminate the adsorbed CO to recover the Pt active sites to improve MOR performance.This synthesis strategy affords a new inspiration to prepare single metal atoms loaded on ZIFs-derived macro-structure with diverse activities for ORR/MOR.

关键词： Defects Electrocatalytic activity Macro-porous structure metal-nitrogen-carbon Single atom catalyst

Boosting the Ni-Zn interplay via O/N dual coordination for high-efficiency CO_(2) electroreduction

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carbon Energy 2023年第4期5卷 68-80页

作者： Ying Zhang Hailei Jiang Anuj Kumar Hongchuan Zhang Zongge Li Tongxin Xu Yuan Pan Yaqun Wang Zhiming Liu Guoxin Zhang Zifeng Yan State Key Laboratory of Heavy Oil Processing College of Chemistry and Chemical EngineeringChina University of Petroleum(East China)QingdaoShandongChina Department of Chemistry Institute of Humanities and Applied ScienceGLA UniversityMathuraIndia College of Chemistry and Chemical Engineering Liaocheng UniversityLiaochengShandongChina Al‐Ion Battery Research Center College of Energy Storage TechnologyShandong University of Science and TechnologyQingdaoShandongChina Shandong Engineering Laboratory for Preparation and Application of High‐performance carbon‐Materials College of Electromechanical EngineeringQingdao University of Science and TechnologyQingdaoShandongChina

Design of supportive atomic sites with a controllably adjusted coordinating environment is essential to advancing the reduction of CO_(2) to value-added fuels and chemicals and to achieving carbon neutralization.Herein,atomic Ni(Zn)sites that are uniquely coordinated with ternary Zn(Ni)/N/O ligands were successfully decorated on formamide-derived porous carbon nanomaterials,possibly forming an atomic structure of Ni(N_(2)O_(1))-Zn(N_(2)O_(1)),as studied by combining X-ray photoelectron spectroscopy and X-ray absorption spectroscopy.With the mediation of additional O coordination,the Ni-Zn dual site induces significantly decreased desorption of molecular CO.The NiZn-NC decorated with rich Ni(N_(2)O_(1))-Zn(N_(2)O_(1))sites remarkably gained>97%CO Faraday efficiency over a wide potential range of -0.8 to -1.1 V(relative to reversible hydrogen electrode).Density functional theory computations suggest that the N/O dual coordination effectively modulates the electronic structure of the Ni-Zn duplex and optimizes the adsorption and conversion properties of CO_(2) and subsequent intermediates.Different from the conventional pathway of using Ni as the active site in the Ni-Zn duplex,it is found that the Ni-neighboring Zn sites in the Ni(N_(2)O_(1))-Zn(N_(2)O_(1))coordination showed much lower energy barriers of the CO_(2) protonation step and the subsequent dehydroxylation step.

关键词： atomic dispersion carbon materials CO_(2)reduction formamide metal-nitrogen-carbon