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Modulating paired Ir-O-Ir via electronic perturbations of correlated Ir single atoms to overcome catalytic selectivity

文献类型：期刊论文

作者Chen, Shi-Hua4,5,6; Yang, Yuan-Fan3,5,6; Song, Zong-Yin3,5,6; Xiao, Xiang-Yu3,5,6; Huang, Cong-Cong3,5,6; Cai, Xin3,5,6; Li, Pei-Hua5,6; Yang, Meng5,6; Chen, Aicheng2; Liu, Wen-Qing1
刊名CHEMICAL SCIENCE
出版日期2023-09-20
卷号14
ISSN号2041-6520
DOI10.1039/d3sc03285j
通讯作者Liu, Wen-Qing(wqliu@aiofm.ac.cn) ; Huang, Xing-Jiu(xingjiuhuang@iim.ac.cn)
英文摘要Single-atom catalysts have been extensively utilized for electrocatalysis, in which electronic metal-support interactions are typically employed to stabilize single atoms. However, this neglects the metal-metal interactions of adjacent atoms, which are essential for the fine-tuning of selective sites. Herein, the high-loading of Ir single atoms (Ir SAs) (8.9 wt%) were adjacently accommodated into oxygen vacancy-rich Co3O4 nanosheets (Ir SAs/Co3O4). Electronic perturbations for both Ir single atoms and Co3O4 supports were observed under electronic metal-support and metal-metal interactions, thus generating Ir-O-Co/Ir units. Electrons were transferred from Co and Ir to O atoms, inducing the depletion of 3d/5d states in Co/Ir and the occupation of 2p states in O atoms to stabilize the Ir SAs. Moreover, the O atoms of Ir-O-Ir functioned as the main active sites for the electrocatalysis of As(iii), which reduced the energy barrier for the rate-determining step. This was due to the stronger electronic affinities for intermediates from reduction of As(iii), which were completely distinct from other coordinated O atoms of Co3O4 or IrO2. Consequently, the resultant Ir SAs/Co3O4 exhibited far more robust electrocatalytic activities than IrO2/Co3O4 and Co3O4 in the electrocatalysis of As(iii). Moreover, there was a strong orbital coupling effect between the coordinated O atoms of Ir SAs and the -OH of H3AsO3, thus exhibiting superior selectivity for As(iii) in contrast to other common heavy metal cations. This work offers useful insights into the rational design of intriguing SACs with high selectivity and stability for the electrocatalysis and electrochemical analysis of pollutants on an electronic level.
WOS关键词METAL-SUPPORT INTERACTIONS ; PLATINUM ; WATER ; GRAPHENE ; SPINELS
资助项目This work was supported by the China Postdoctoral Science Foundation (2022M723188), the Open Research Project of State Key Laboratory of Transducer Technology (SKT2202), the National Natural Science Foundation of China (22306186, 22204166, 22206187), the Y
WOS研究方向Chemistry
语种英语
出版者ROYAL SOC CHEMISTRY
WOS记录号WOS:001065861900001
资助机构This work was supported by the China Postdoctoral Science Foundation (2022M723188), the Open Research Project of State Key Laboratory of Transducer Technology (SKT2202), the National Natural Science Foundation of China (22306186, 22204166, 22206187), the Y
源URL[http://ir.hfcas.ac.cn:8080/handle/334002/132591]  
专题中国科学院合肥物质科学研究院
通讯作者Liu, Wen-Qing; Huang, Xing-Jiu
作者单位1.Chinese Acad Sci, Anhui Inst Opt & Fine Mech, HFIPS, Hefei 230031, Peoples R China
2.Univ Guelph, Dept Chem, Guelph, ON N1G 2W1, Canada
3.Univ Sci & Technol China, Dept Mat Sci & Engn, Hefei 230026, Peoples R China
4.Chinese Acad Sci, Shanghai Inst Microsyst & Informat Technol, State Key Lab Transducer Technol, Shanghai 200050, Peoples R China
5.Chinese Acad Sci, Inst Solid State Phys, Environm Mat & Pollut Control Lab, HFIPS, Hefei 230031, Peoples R China
6.Chinese Acad Sci, Inst Solid State Phys, Key Lab Environm Opt & Technol, HFIPS, Hefei 230031, Peoples R China
推荐引用方式
GB/T 7714		 Chen, Shi-Hua,Yang, Yuan-Fan,Song, Zong-Yin,et al. Modulating paired Ir-O-Ir via electronic perturbations of correlated Ir single atoms to overcome catalytic selectivity[J]. CHEMICAL SCIENCE,2023,14.
APA Chen, Shi-Hua.,Yang, Yuan-Fan.,Song, Zong-Yin.,Xiao, Xiang-Yu.,Huang, Cong-Cong.,...&Huang, Xing-Jiu.(2023).Modulating paired Ir-O-Ir via electronic perturbations of correlated Ir single atoms to overcome catalytic selectivity.CHEMICAL SCIENCE,14.
MLA Chen, Shi-Hua,et al."Modulating paired Ir-O-Ir via electronic perturbations of correlated Ir single atoms to overcome catalytic selectivity".CHEMICAL SCIENCE 14(2023).

入库方式： OAI收割

来源：合肥物质科学研究院

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