High-rate electrochemical H2O2 production over multimetallic atom catalysts under acidic-neutral conditions
文献类型：期刊论文
| 作者 | Tong, Yueyu2,3; Liu, Jiaxin2; Su, Bing-Jian1; Juang, Jenh-Yih1; Hou, Feng2; Yin, Lichang4; Dou, Shi Xue3,5; Liang, Ji2,6 |
| 刊名 | CARBON ENERGY
 |
| 出版日期 | 2023-06-12 |
| 页码 | 19 |
| 关键词 | hydrogen peroxide production multiatom catalysts operando X-ray adsorption spectrum reaction mechanism tendency structure-property relation |
| DOI | 10.1002/cey2.378 |
| 通讯作者 | Liang, Ji(liangji@tju.edu.cn) |
| 英文摘要 | 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. |
| 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 |
| 语种 | 英语 |
| WOS记录号 | WOS:001004721400001 |
| 出版者 | WILEY |
| 资助机构 | National Natural Science Foundation of China ; Australian Research Council ; Natural Science Foundation of Liaoning Province |
| 源URL | [http://ir.imr.ac.cn/handle/321006/178162]  |
| 专题 | 金属研究所_中国科学院金属研究所 |
| 通讯作者 | Liang, Ji |
| 作者单位 | 1.Natl Chiao Tung Univ, Dept Electrophys, Hsinchu, Taiwan 2.Tianjin Univ, Sch Mat Sci & Engn, Key Lab Adv Ceram & Machining Technol, Minist Educ, Tianjin, Peoples R China 3.Univ Wollongong, Inst Superconducting & Elect Mat, Innovat Campus, North Wollongong, NSW, Australia 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. |
入库方式： OAI收割
来源：金属研究所
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