Deciphering the contributing motifs of reconstructed cobalt (II) sulfides catalysts in Li-CO<sub>2</sub> batteries

doi:10.1038/s41467-024-46465-8

IMR OpenIR

	Deciphering the contributing motifs of reconstructed cobalt (II) sulfides catalysts in Li-CO₂ batteries
	Liu, Yingqi 1,2; Zhang, Zhiyuan 1,2; Tan, Junyang 1,2; Chen, Biao 3,4; Lu, Bingyi 1,2; Mao, Rui 1,2; Liu, Bilu 1,2; Wang, Dashuai 5,6; Zhou, Guangmin 1,2; Cheng, Hui-Ming 7,8,9
通讯作者	Wang, Dashuai(dswang@zju.edu.cn) ; Zhou, Guangmin(guangminzhou@sz.tsinghua.edu.cn) ; Cheng, Hui-Ming(hm.cheng@siat.ac.cn)
	2024-03-09
发表期刊	NATURE COMMUNICATIONS
卷号	15 期号:1 页码:11
摘要	Developing highly efficient catalysts is significant for Li-CO2 batteries. However, understanding the exact structure of catalysts during battery operation remains a challenge, which hampers knowledge-driven optimization. Here we use X-ray absorption spectroscopy to probe the reconstruction of CoSx (x = 8/9, 1.097, and 2) pre-catalysts and identify the local geometric ligand environment of cobalt during cycling in the Li-CO2 batteries. We find that different oxidized states after reconstruction are decisive to battery performance. Specifically, complete oxidation on CoS1.097 and Co9S8 leads to electrochemical performance deterioration, while oxidation on CoS2 terminates with Co-S4-O2 motifs, leading to improved activity. Density functional theory calculations show that partial oxidation contributes to charge redistributions on cobalt and thus facilitates the catalytic ability. Together, the spectroscopic and electrochemical results provide valuable insight into the structural evolution during cycling and the structure-activity relationship in the electrocatalyst study of Li-CO2 batteries.
资助者	National Natural Science Foundation of China ; Guangdong Innovative and Entrepreneurial Research Team Program ; Shenzhen Science and Technology Program ; Shenzhen Stabilization Support Program ; Guangdong Basic and Applied Basic Research Foundation ; Overseas Research Cooperation Fund ; Interdisciplinary Research and Innovation Fund of Tsinghua Shenzhen International Graduate School ; China Postdoctoral Science Foundation
DOI	10.1038/s41467-024-46465-8
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China[U21A20174] ; Guangdong Innovative and Entrepreneurial Research Team Program[2021ZT09L197] ; Shenzhen Science and Technology Program[KQTD20210811090112002] ; Shenzhen Stabilization Support Program[WDZC20200824091903001] ; Guangdong Basic and Applied Basic Research Foundation[2020B0301030002] ; Overseas Research Cooperation Fund ; Interdisciplinary Research and Innovation Fund of Tsinghua Shenzhen International Graduate School ; China Postdoctoral Science Foundation[2020TQ0159]
WOS研究方向	Science & Technology - Other Topics
WOS类目	Multidisciplinary Sciences
WOS记录号	WOS:001185106800016
出版者	NATURE PORTFOLIO
引用统计	被引频次：25[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/185154
专题	中国科学院金属研究所
通讯作者	Wang, Dashuai; Zhou, Guangmin; Cheng, Hui-Ming
作者单位	1.Tsinghua Univ, Tsinghua Berkeley Shenzhen Inst, Shenzhen 518055, Peoples R China 2.Tsinghua Univ, Tsinghua Shenzhen Int Grad Sch, Shenzhen 518055, Peoples R China 3.Tianjin Univ, Sch Mat Sci & Engn, Tianjin 300350, Peoples R China 4.Tianjin Univ, Tianjin Key Lab Composite & Funct Mat, Tianjin 300350, Peoples R China 5.Inst Zhejiang Univ, Quzhou, Peoples R China 6.Zhejiang Univ, Coll Chem & Biol Engn, Key Lab Biomass Chem Engn, Minist Educ, Hangzhou 310027, Peoples R China 7.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 8.Chinese Acad Sci, Inst Technol Carbon Neutral, Shenzhen Inst Adv Technol, Shenzhen 518055, Peoples R China 9.Shenzhen Univ Adv Technol, Shenzhen 518055, Peoples R China
推荐引用方式 GB/T 7714	Liu, Yingqi,Zhang, Zhiyuan,Tan, Junyang,et al. Deciphering the contributing motifs of reconstructed cobalt (II) sulfides catalysts in Li-CO₂ batteries[J]. NATURE COMMUNICATIONS,2024,15(1):11.
APA	Liu, Yingqi.,Zhang, Zhiyuan.,Tan, Junyang.,Chen, Biao.,Lu, Bingyi.,...&Cheng, Hui-Ming.(2024).Deciphering the contributing motifs of reconstructed cobalt (II) sulfides catalysts in Li-CO₂ batteries.NATURE COMMUNICATIONS,15(1),11.
MLA	Liu, Yingqi,et al."Deciphering the contributing motifs of reconstructed cobalt (II) sulfides catalysts in Li-CO₂ batteries".NATURE COMMUNICATIONS 15.1(2024):11.