Bimetallic PdFe3 Nano-Alloy with Tunable Electron Configuration for Boosting Electrochemical Nitrogen Fixation
文献类型：期刊论文
| 作者 | Mu, Jianjia1; Zhao, Zhiwei2; Gao, Xuan-Wen1; Liu, Zhao-Meng1; Luo, Wen-Bin1; Sun, Zhenhua3; Gu, Qin-Fen4; Li, Feng3 |
| 刊名 | ADVANCED ENERGY MATERIALS
 |
| 出版日期 | 2023-12-15 |
| 页码 | 10 |
| 关键词 | electrocatalyst electrochemical nitrogen fixation electronic configuration PdFe3 nano-alloy |
| ISSN号 | 1614-6832 |
| DOI | 10.1002/aenm.202303558 |
| 通讯作者 | Luo, Wen-Bin(luowenbin@smm.neu.edu.cn) ; Li, Feng(fli@imr.ac.cn) |
| 英文摘要 | Electrocatalyst plays animportant role in electrochemical ammonia synthesis by determining the nitrogen reduction reaction pathway. Featuring the inherent half-filled 3d orbitals, ion-based alloy electrocatalysts have been attracting much more attention owing to the controllable driving force to adsorb and activate N equivalent to N bonds. Besides supplying unoccupied d-orbital to accommodate lone-pair electrons to facilitate nitrogen adsorption, donating d-orbital electrons to nitrogen antibonding orbitals to dissociate N equivalent to N bond is demandedas well. By palladium (Pd) to synthesize PdFe3 nano-alloy, numerous Fe 3d orbitals can be reconstructed via charge polarization between Fe and Pd, simultaneously lowering corresponding work functions. Meanwhile, the positively charged Fesites in PdFe3 can strengthen suppress the proton adsorption by electrostatic repulsion. A considerably optimized ammonia production rate of 29.07 mu g h(-1) mg(cat).(-1) and Faradic efficiency of 22.8% are accomplished at a low overpotential of -0.2 V vs. RHE. Density functional theory combined with in-situ ATR-FTIR results confirmthe electrocatalytic nitrogen reduction follows the associative distalmechanism and the electron-deficient Fe induced through Pd facilitates significantly lowering the first-step-protonation energy barrier of only 0.07 eV (*N-2+ *H ->*NNH). |
| 资助项目 | National Natural Science Foundation of China ; Liaoning Revitalization Talents Program[XLYC2007155] ; [52272194] |
| WOS研究方向 | Chemistry ; Energy & Fuels ; Materials Science ; Physics |
| 语种 | 英语 |
| WOS记录号 | WOS:001127270900001 |
| 出版者 | WILEY-V C H VERLAG GMBH |
| 资助机构 | National Natural Science Foundation of China ; Liaoning Revitalization Talents Program |
| 源URL |  |
| 专题 | 金属研究所_中国科学院金属研究所 |
| 通讯作者 | Luo, Wen-Bin; Li, Feng |
| 作者单位 | 1.Northeastern Univ, Inst Energy Electrochem & Urban Mines Met, Sch Met, Shenyang 110819, Liaoning, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Peoples R China 3.Chinese Acad Sci, Inst Met Res, Shenyang 110819, Liaoning, Peoples R China 4.Australian Synchrotron ANSTO, 800 Blackburn Rd, Clayton, Vic 3168, Australia |
| 推荐引用方式 GB/T 7714 | Mu, Jianjia,Zhao, Zhiwei,Gao, Xuan-Wen,et al. Bimetallic PdFe3 Nano-Alloy with Tunable Electron Configuration for Boosting Electrochemical Nitrogen Fixation[J]. ADVANCED ENERGY MATERIALS,2023:10. |
| APA | Mu, Jianjia.,Zhao, Zhiwei.,Gao, Xuan-Wen.,Liu, Zhao-Meng.,Luo, Wen-Bin.,...&Li, Feng.(2023).Bimetallic PdFe3 Nano-Alloy with Tunable Electron Configuration for Boosting Electrochemical Nitrogen Fixation.ADVANCED ENERGY MATERIALS,10. |
| MLA | Mu, Jianjia,et al."Bimetallic PdFe3 Nano-Alloy with Tunable Electron Configuration for Boosting Electrochemical Nitrogen Fixation".ADVANCED ENERGY MATERIALS (2023):10. |
入库方式： OAI收割
来源：金属研究所
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