| High-rate electrochemical H2O2 production over multimetallic atom catalysts under acidic-neutral conditions | |
| Tong, Yueyu1,2; Liu, Jiaxin1; Su, Bing-Jian3; Juang, Jenh-Yih3; Hou, Feng1; Yin, Lichang4; Dou, Shi Xue2,5; Liang, Ji1,6 | |
| Corresponding Author | Liang, Ji(liangji@tju.edu.cn) |
| 2023-06-12 | |
| Source Publication | CARBON ENERGY
 |
| Pages | 19 |
| Abstract | 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. |
| Keyword | hydrogen peroxide production multiatom catalysts operando X-ray adsorption spectrum reaction mechanism tendency structure-property relation |
| Funding Organization | National Natural Science Foundation of China ; Australian Research Council ; Natural Science Foundation of Liaoning Province |
| DOI | 10.1002/cey2.378 |
| Indexed By | SCI |
| Language | 英语 |
| Funding Project | 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 Research Area | Chemistry ; Energy & Fuels ; Science & Technology - Other Topics ; Materials Science |
| WOS Subject | Chemistry, Physical ; Energy & Fuels ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary |
| WOS ID | WOS:001004721400001 |
| Publisher | WILEY |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.imr.ac.cn/handle/321006/178163 |
| Collection | 中国科学院金属研究所 |
| Corresponding Author | Liang, Ji |
| Affiliation | 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 |
| Recommended Citation 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. |
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