异质单原子-团簇协同提升催化活性

Synergistic effect of heterogeneous single atoms and clusters for improved catalytic performance

刘龙 ¹高文婷 ¹马熠灵 ¹梅开男 ¹吴文龙 ¹李洪良 ¹张志荣 ¹曾杰²

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作者信息

1. 中国科学技术大学合肥微尺度物质科学国家研究中心,中国科学院强耦合量子材料物理重点实验室,安徽省教育厅表界面化学与能源催化重点实验室,化学物理系,安徽合肥 230026
2. 中国科学技术大学合肥微尺度物质科学国家研究中心,中国科学院强耦合量子材料物理重点实验室,安徽省教育厅表界面化学与能源催化重点实验室,化学物理系,安徽合肥 230026;安徽工业大学化学与化工学院,安徽马鞍山 243002
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摘要

电解水制氢是一种高效的制氢技术.在电解水制氢过程中,电化学析氧反应(OER)涉及动力学缓慢的四电子转移过程,这限制了电解水制氢的效率.因此,迫切需要开发高活性的电化学析氧反应催化剂来加速反应动力学.耦合单原子和团簇是一种提高电催化性能的有效策略,利用这种策略可以协同优化反应中间体的吸附和构型,提高催化活性.然而,目前这方面的研究较少.本文通过将铱单原子和钴团簇锚定在氢氧化镍纳米片表面构建了异质单原子-团簇系统.铱单原子和钴团簇协同提高了电化学析氧反应催化剂的催化活性.具体而言,ConIr1/Ni(OH)2在10 mA·cm-2电流密度下需要255 mV的过电位,比Con/Ni(OH)2和Ir1/Ni(OH)2分别低60 mV和67 mV.在300 mV过电位下,ConIr1/Ni(OH)2的转换频率为 0.49 s-1,是 Con/Ni(OH)2 的 4.9 倍.

Abstract

Electrocatalytic water splitting provides an efficient method for the production of hydrogen.In electrocatalytic water splitting,the oxygen evolution reaction(OER)involves a kinetically sluggish four-electron transfer process,which limits the efficiency of electrocatalytic water splitting.Therefore,it is urgent to develop highly active OER catalysts to ac-celerate reaction kinetics.Coupling single atoms and clusters in one system is an innovative approach for developing effi-cient catalysts that can synergistically optimize the adsorption and configuration of intermediates and improve catalytic activity.However,research in this area is still scarce.Herein,we constructed a heterogeneous single-atom cluster system by anchoring Ir single atoms and Co clusters on the surface of Ni(OH)2 nanosheets.Ir single atoms and Co clusters syner-gistically improved the catalytic activity toward the OER.Specifically,ConIr1/Ni(OH)2 required an overpotential of 255 mV at a current density of 10 mA·cm-2,which was 60 mV and 67 mV lower than those of Con/Ni(OH)2 and Ir1/Ni(OH)2,respectively.The turnover frequency of ConIr1/Ni(OH)2 was 0.49 s,which was 4.9 times greater than that of Con/Ni(OH)2 at an overpotential of 300 mV.

关键词

单原子-团簇催化剂/协同效应/电化学析氧反应

Key words

single-atom cluster catalysts/synergistic effect/oxygen evolution reaction

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基金项目

National Key Research and Development Program of China(2021YFA1500500)

National Key Research and Development Program of China(2019-YFA0405600)

CAS Project for Young Scientists in Basic Research(YSBR-051)

National Science Fund for Distinguished Young Scholars(21925204)

National Natural Science Foundation of China(22202192)

National Natural Science Foundation of China(U19A2015)

National Natural Science Foundation of China(22221003)

National Natural Science Foundation of China(22250007)

National Natural Science Foundation of China(22163002)

Collaborative Innovation Program of Hefei Science Center,CAS(2022HSC-CIP004)

International Partnership()

DNL Cooperation Fund,CAS(DNL202003)

USTC Research Funds of the Double First-Class Initiative(YD9990002016)

USTC Research Funds of the Double First-Class Initiative(YD999000-2014)

Program of Chinese Academy of Sciences(123GJHZ2022101GC)

Fundamental Research Funds for the Central Universities(WK9990000095)

Fundamental Research Funds for the Central Universities(WK999000-0124)

出版年

2024

中国科学技术大学学报

中国科学技术大学

中国科学技术大学学报

CSTPCD北大核心

影响因子：0.421

ISSN：0253-2778

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