物理化学学报2023，Vol.39Issue(12)：15-38,24.DOI:10.3866/PKU.WHXB202302049
电子自旋效应在电催化剂中的作用
Function of Electron Spin Effect in Electrocatalysts
摘要
Abstract
With the continuous consumption of non-renewable energy and increasing exacerbation in associated environmental problems,there is a growing demand for clean renewable energy.This demand has led to the development of many energy conversion technologies to alleviate the energy crisis and related environmental problems.The development of high-efficiency electrocatalysts is crucial for the progress of renewable energy conversion and storage technologies.Over the past decade,researchers have gradually understood the intrinsic reaction mechanism and structure-performance relationships in electrocatalysis,and made significant progress in synthesizing high-performance electrocatalysts.Detailed analysis of the relationship between the intrinsic activity and electronic structure of active sites,including the deeper levels of electronic spin distribution of catalyst active sites,has been the focus of electrocatalysis research.Spin is an inherent property of particles and can have a unique impact on chemical reactions.Therefore,using electron spin to further study the electronic structure of active sites is expected to bring new development opportunities to catalyst design theory.Spin control in electrocatalysts is undoubtedly an effective method to improve catalytic performance.This review article introduces the progress status of electron spin in electrocatalysis,summarizes the common strategies for controlling electron spin at the active sites in electrocatalysis,and expound the mechanism of spin effect in electrocatalysis from both thermodynamic and kinetic aspects.Further,the article reviews the latest research progress concerning the spin effect on several reactions such as oxygen reduction reaction(ORR),oxygen evolution reaction(OER),nitrogen reduction reaction(NRR)and carbon dioxide reduction reaction(CO2RR).It explains the important role of spin in catalyst activity and catalyst promotion of the aforementioned reactions,and then discusses the spin stability of the catalyst active sites in ORR.In addition,the article reviews the advanced methods widely used for characterizing electron spin in electrocatalysis,such as vibrating sample magnetometry,electron paramagnetic resonance spectroscopy,Mossbauer spectroscopy,and X-ray spectroscopy,and discusses the first-principle calculation methods employed in spin catalysis.Finally,the article summarizes the current development of spin electronics in electrocatalysis and proposes future development directions regarding the spin effect in electrocatalysis.In summary,understanding the role of spin effect is instrumental for improving the understanding of the mechanism of electrocatalytic reaction,and can guide the design of high-efficiency catalysts,which has broad research prospects.This review presents for the first time a comprehensive summary of the latest research progress on the spin effect in the field of electrocatalysis,which provides theoretical guidance for the design of spin-regulated high-efficiency electrocatalysts.关键词
自旋催化/电子自旋/电催化剂/氧还原反应/析氧反应/氮还原反应/二氧化碳还原反应Key words
Spin catalysis/Electron spin/Electrocatalyst/Oxygen reduction reaction/Oxygen evolution reaction/Nitrogen reduction reaction/Carbon dioxide reduction reaction分类
化学引用本文复制引用
李景学,于跃,徐斯然,闫文付,木士春,张佳楠..电子自旋效应在电催化剂中的作用[J].物理化学学报,2023,39(12):15-38,24.基金项目
The project was supported by the National Natural Science Foundation of China(U22A20107,U1967215),the Distinguished Young Scholars Innovation Team of Zhengzhou University(32320275),the Academic Degrees & Graduate Education Reform Project of Henan Province(2021SJGLX093Y),and the Science and Technology Research Support Plan in Henan Province(222301420001).国家自然科学基金(U22A20107,U1967215),郑州大学杰出青年创新团队(32320275),河南省高等教育教学改革研究与实践项目(研究生教育)(2021SJGLX093Y)及河南省省级科技研发计划联合基金(优势学科培育类)(222301420001)资助 （U22A20107,U1967215）
