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Edge-enriched N, S co-doped hierarchical porous carbon for oxygen reduction reaction

Chinese Chemical Letters 2023年第2期34卷 349-354页

作者： Fangfang Chang Panpan Su utsab guharoy Runping Ye Yanfu Ma Huajun Zheng Yi Jia Jian Liu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China Department of Applied Chemistry and Zhejiang Carbon Neutral Innovation Institute Zhejiang University of TechnologyHangzhou 310032China DICP-Surrey Joint Centre for Future Materials Department of Chemical and Process EngineeringUniversity of SurreyGuildfordSurrey GU27XHUnited Kingdom

The development of carbon materials with high electrochemical performance for next-generation energy device is emerging, especially N, S co-doped carbon materials have sparked intensive attention. However,the exploration of N, S co-doped carbon with well-defined active sites and hierarchical porous structures are still limited. In this study, we prepared a series of edge-enriched N, S co-doped carbon materials through pyrolysis of thiourea(TU) encapsulated in zeolitic imidazolate frameworks(TU@ZIF) composites,which delivered very good oxygen reduction reaction(ORR) performance in alkaline medium with onset potential of 0.94 V vs. reversible hydrogen electrode(RHE), good stability and methanol tolerance. Density functional theory(DFT) calculations suggested that carbon atoms adjacent to N and S are probable active sites for ORR intermediates in edge-enriched N, S co-doped carbon materials because higher electron density can enhance O_(2)adsorption, lower formation barriers of intermediates, improving the ORR performance comparing to intact N, S co-doped carbon materials. This study might provide a new pathway for improving ORR activity by the integration engineering of edge sites, and electronic structure of heteroatom doped carbon electrocatalysts.

关键词： Porosity engineering N S co-doped carbon materials Hierarchical porous carbon Edge-enriched carbon Oxygen reduction reaction DFT calculation

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Fe atoms anchored on defective nitrogen doped hollow carbon spheres as efficient electrocatalysts for oxygen reduction reaction

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Nano Research 2021年第4期14卷 1069-1077页

作者： Panpan Su Wenjuan Huang Jiangwei Zhang utsab guharoy Qinggang Du Qiao Sun Qike Jiang Yi Cheng Jie Yang Xiaoli Zhang Yongsheng Liu San Ping Jiang Jian Liu College of Mathematics and Physics Shanghai University of Electric PowerShanghai 200090China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China State Key Laboratory of Radiation Medicine and Protection Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSchool for Radiological and Interdisciplinary SciencesSoochow UniversitySuzhou 215123China Division of Energy Research Resourcesy Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023China Department of Environmental Engineering School of Metallurgy and EnvironmentCentral South UniversityChangsha 410083China WA School of Mines:Minerals Energy and Chemical EngineeringCurtin UniversityPerthWA 6102Australia State Centre for International Cooperation on Designer Low-Carbon&Environmental Materials School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China DICP-Surrey Joint Centre for Future Materials Department of Chemical and Process EngineeringUniversity of SurreyGuildfordSurreyU K

Defective electrocatalysts,especially for intrinsic defective carbon,have aroused a wide concern owing to high spin and charge densities.However,the designated nitrogen species favorable for creating defects by the removal of nitrogen,and the influence of defects for the coordination structure of active site and oxygen reduction reaction(ORR)activity have not been elucidated.Herein,we designed and synthesized a pair of electrocatalysts,denoted as Fe-N/C and Fe-ND/C for coordination sites of atomic iron-nitrogen and iron-nitrogen/defect configuration embedded in hollow carbon spheres,respectively,through direct pyrolysis of their corresponding hollow carbon spheres adsorbed with Fe(acac)3.The nitrogen defects were fabricated via the evaporation of pyrrolic-N on nitrogen doped hollow carbon spheres.Results of comparative experiments between Fe-N/C and Fe-ND/C reveal that Fe-ND/C shows superior ORR activity with an onset potential of 30 mV higher than that of Fe-N/C.Fe-ND sites are more favorable for the enhancement of ORR activity.Density functional theory(DFT)calculation demonstrates that Fe-ND/C with proposed coordination structure of FeN_(4-x)(0

关键词： atom ic iron nitrogen defect coordination environment hollow carbon spheres oxygen reduction reaction

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