Theoretical Insights on Au-based Bimetallic Alloy Electrocatalysts for Nitrogen Reduction Reaction with High Selectivity and Activity
文献类型：期刊论文
| 作者 | Shi, Jun-Lin2; Xiang, Shi-Qin2; Su, Dai-Jian2; Liu, Xiaohong1; Zhang, Wei1 ; Zhao, Liu-Bin2
|
| 刊名 | CHEMSUSCHEM
 |
| 出版日期 | 2021-09-12 |
| 页码 | 12 |
| 关键词 | ammonia bimetallic catalysts electrocatalysis nitrogen reduction reaction thermodynamics |
| ISSN号 | 1864-5631 |
| DOI | 10.1002/cssc.202101462 |
| 通讯作者 | Zhang, Wei(andyzhangwei@163.com) ; Zhao, Liu-Bin(lbzhao@swu.edu.cn) |
| 英文摘要 | Electrochemical reduction of nitrogen to produce ammonia at moderate conditions in aqueous solutions holds great prospect but also faces huge challenges. Considering the high selectivity of Au-based materials to inhibit competitive hydrogen evolution reaction (HER) and high activity of transition metals such as Fe and Mo toward the nitrogen reduction reaction (NRR), it was proposed that Au-based alloy materials could act as efficient catalysts for N-2 fixation based on density functional theory simulations. Only on Mo3Au(111) surface the adsorption of N-2 is stronger than H atom. Thermodynamics combined with kinetics studies were performed to investigate the influence of composition and ratio of Au-based alloys on NRR and HER. The binding energy and reorganization energy affected performance for the initial N-2 activation and hydrogenation process. By considering the free-energy diagram, the computed potential-determining step was either the first or the fifth hydrogenation step on metal catalysts. The optimum catalytic activity could be achieved by adjusting atomic proportion in alloys to make all intermediate species exhibit moderate adsorption. Free-energy diagrams of N-2 hydrogenation via Langmuir-Hinshelwood mechanism and hydrogen evolution via Tafel mechanism were compared to reveal that the Mo3Au surface showed satisfactory catalytic performance by simultaneously promoting NRR and suppressing HER. Theoretical simulations demonstrated that Au-Mo alloy materials could be applied as high-performance electrocatalysts for NRR. |
| 资助项目 | Fundamental Research Funds for the Central Universities[XDJK2019C032] ; Open Funds of State Key Laboratory of Physical Chemistry of Solid Surfaces (Xiamen University)[201929] ; Chongqing Talents Program[CQYC201905041] ; Chongqing Graduate Scientific Research Innovation Project[CYS18115] |
| WOS研究方向 | Chemistry ; Science & Technology - Other Topics |
| 语种 | 英语 |
| WOS记录号 | WOS:000695006800001 |
| 出版者 | WILEY-V C H VERLAG GMBH |
| 源URL | [http://119.78.100.138/handle/2HOD01W0/14258]  |
| 专题 | 中国科学院重庆绿色智能技术研究院 |
| 通讯作者 | Zhang, Wei; Zhao, Liu-Bin |
| 作者单位 | 1.Chinese Acad Sci, Chongqing Inst Green & Intelligent Technol, Chongqing 400714, Peoples R China 2.Southwest Univ, Dept Chem, Sch Chem & Chem Engn, Chongqing 400715, Peoples R China |
| 推荐引用方式 GB/T 7714 | Shi, Jun-Lin,Xiang, Shi-Qin,Su, Dai-Jian,et al. Theoretical Insights on Au-based Bimetallic Alloy Electrocatalysts for Nitrogen Reduction Reaction with High Selectivity and Activity[J]. CHEMSUSCHEM,2021:12. |
| APA | Shi, Jun-Lin,Xiang, Shi-Qin,Su, Dai-Jian,Liu, Xiaohong,Zhang, Wei,&Zhao, Liu-Bin.(2021).Theoretical Insights on Au-based Bimetallic Alloy Electrocatalysts for Nitrogen Reduction Reaction with High Selectivity and Activity.CHEMSUSCHEM,12. |
| MLA | Shi, Jun-Lin,et al."Theoretical Insights on Au-based Bimetallic Alloy Electrocatalysts for Nitrogen Reduction Reaction with High Selectivity and Activity".CHEMSUSCHEM (2021):12. |
入库方式： OAI收割
来源：重庆绿色智能技术研究院
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