High-rate electrochemical H2O2 production over multimetallic atom catalysts under acidic-neutral conditions

doi:10.1002/cey2.378

IMR OpenIR

	High-rate electrochemical H2O2 production over multimetallic atom catalysts under acidic-neutral conditions
	Tong, Yueyu 1,2; Liu, Jiaxin 1; Su, Bing-Jian 3; Juang, Jenh-Yih 3; Hou, Feng 1; Yin, Lichang 4; Dou, Shi Xue 2,5; Liang, Ji 1,6
通讯作者	Liang, Ji(liangji@tju.edu.cn)
	2023-06-12
发表期刊	CARBON ENERGY
页码	19
摘要	Hydrogen peroxide (H2O2) production by the electrochemical 2-electron oxygen reduction reaction (2e(-) ORR) is a promising alternative to the energy-intensive anthraquinone process, and single-atom electrocatalysts show the unique capability of high selectivity toward 2e(-) ORR against the 4e(-) one. The extremely low surface density of the single-atom sites and the inflexibility in manipulating their geometric/electronic configurations, however, compromise the H2O2 yield and impede further performance enhancement. Herein, we construct a family of multiatom catalysts (MACs), on which two or three single atoms are closely coordinated to form high-density active sites that are versatile in their atomic configurations for optimal adsorption of essential OOH species. Among them, the Co-x-Ni MAC presents excellent electrocatalytic performance for 2e(-) ORR, in terms of its exceptionally high H2O2 yield in acidic electrolytes (28.96 mol L-1 g(cat.)(-1) h(-1)) and high selectivity under acidic to neutral conditions in a wide potential region (>80%, 0-0.7 V). Operando X-ray absorption and density functional theory analyses jointly unveil its unique trimetallic Co2NiN8 configuration, which efficiently induces an appropriate Ni-d orbital filling and modulates the OOH adsorption, together boosting the electrocatalytic 2e(-) ORR capability. This work thus provides a new MAC strategy for tuning the geometric/electronic structure of active sites for 2e(-) ORR and other potential electrochemical processes.
关键词	hydrogen peroxide production multiatom catalysts operando X-ray adsorption spectrum reaction mechanism tendency structure-property relation
资助者	National Natural Science Foundation of China ; Australian Research Council ; Natural Science Foundation of Liaoning Province
DOI	10.1002/cey2.378
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China[21905202] ; National Natural Science Foundation of China[22179093] ; National Natural Science Foundation of China[51972312] ; Australian Research Council[DP210102215] ; Natural Science Foundation of Liaoning Province[2020-MS-003]
WOS研究方向	Chemistry ; Energy & Fuels ; Science & Technology - Other Topics ; Materials Science
WOS类目	Chemistry, Physical ; Energy & Fuels ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS记录号	WOS:001004721400001
出版者	WILEY
引用统计	被引频次：27[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/321006/178163
专题	中国科学院金属研究所
通讯作者	Liang, Ji
作者单位	1.Tianjin Univ, Sch Mat Sci & Engn, Key Lab Adv Ceram & Machining Technol, Minist Educ, Tianjin, Peoples R China 2.Univ Wollongong, Inst Superconducting & Elect Mat, Innovat Campus, North Wollongong, NSW, Australia 3.Natl Chiao Tung Univ, Dept Electrophys, Hsinchu, Taiwan 4.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang, Liaoning, Peoples R China 5.Univ Shanghai Sci & Technol, Inst Energy Mat Sci, Shanghai, Peoples R China 6.Tianjin Univ, Sch Mat Sci & Engn, Key Lab Adv Ceram & Machining Technol, Minist Educ, Tianjin 300350, Peoples R China
推荐引用方式 GB/T 7714	Tong, Yueyu,Liu, Jiaxin,Su, Bing-Jian,et al. High-rate electrochemical H2O2 production over multimetallic atom catalysts under acidic-neutral conditions[J]. CARBON ENERGY,2023:19.
APA	Tong, Yueyu.,Liu, Jiaxin.,Su, Bing-Jian.,Juang, Jenh-Yih.,Hou, Feng.,...&Liang, Ji.(2023).High-rate electrochemical H2O2 production over multimetallic atom catalysts under acidic-neutral conditions.CARBON ENERGY,19.
MLA	Tong, Yueyu,et al."High-rate electrochemical H2O2 production over multimetallic atom catalysts under acidic-neutral conditions".CARBON ENERGY (2023):19.