| Nitrogen electroreduction performance of transition metal dimers embedded into N-doped graphene: a theoretical prediction | |
| Li, Hongyan1; Zhao, Zhifeng2; Cai, Qinghai1; Yin, Lichang3; Zhao, Jingxiang1 | |
| Corresponding Author | Yin, Lichang(lcyin@imr.ac.cn) ; Zhao, Jingxiang(xjz_hmily@163.com) |
| 2020-02-28 | |
| Source Publication | JOURNAL OF MATERIALS CHEMISTRY A
 |
| ISSN | 2050-7488 |
| Volume | 8Issue:8Pages:4533-4543 |
| Abstract | The electrocatalytic nitrogen reduction reaction (eNRR) under ambient conditions using sustainable energy sources is a fascinating approach for ammonia (NH3) production to replace the industrial Haber-Bosch process with enormous energy input and continuous CO2 emissions. However, the eNRR process remains a coveted goal due to the poor product selectivity, low activity, and stability of traditional catalysts. Inspired by recent experimental advances in dual-atom catalysts, herein, by means of comprehensive spin-polarized density functional theory (DFT) computations, the catalytic performance of various binary transition metals dispersed in nitrogen-doped porous graphene (NPG) for the eNRR was systematically evaluated. Our results revealed that the N atoms around vacancies in the substrate can strongly stabilize the metal dimers by forming metal-N bonds. Among FeFe, FeCo, FeNi, FeCu, FeRh, FeRu, FePd, MoFe, MoCo, MoCu, MoRu, and MoMo, the binary FeRh embedded in NPG was identified as the best catalyst due to its lowest limiting potential (-0.22 V) and high selectivity towards the eNRR. Our results further suggested that the good eNRR catalytic activity of the dispersed FeRh mainly originates from its optimal eNRR intermediates' adsorption/desorption features, obvious suppressing effects on the hydrogen evolution reaction, and great promise for synthesis. Our work not only opens a new door to advance sustainable NH3 production by tailoring the electronic structures of binuclear metal atoms, but also provides deeper insight into the structure-performance relationships of dual sites for eNRR electrocatalysts. |
| Funding Organization | Natural Science Funds for Distinguished Young Scholar of Heilongjiang Province ; National Natural Science Foundation of China ; Project of Introducing Talent of Guangdong University of Petrochemical Technology |
| DOI | 10.1039/c9ta13599e |
| Indexed By | SCI |
| Language | 英语 |
| Funding Project | Natural Science Funds for Distinguished Young Scholar of Heilongjiang Province[JC2018004] ; National Natural Science Foundation of China[51972312] ; National Natural Science Foundation of China[51472249] ; Project of Introducing Talent of Guangdong University of Petrochemical Technology[519614] ; Project of Introducing Talent of Guangdong University of Petrochemical Technology[519162] |
| WOS Research Area | Chemistry ; Energy & Fuels ; Materials Science |
| WOS Subject | Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary |
| WOS ID | WOS:000519704200034 |
| Publisher | ROYAL SOC CHEMISTRY |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.imr.ac.cn/handle/321006/137707 |
| Collection | 中国科学院金属研究所 |
| Corresponding Author | Yin, Lichang; Zhao, Jingxiang |
| Affiliation | 1.Harbin Normal Univ, Minist Educ, Coll Chem & Chem Engn, Key Lab Photon & Elect Bandgap Mat, Harbin 150025, Peoples R China 2.Guangdong Univ Petrochem Technol, Coll Chem, Maoming 525000, Peoples R China 3.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China |
| Recommended Citation GB/T 7714 | Li, Hongyan,Zhao, Zhifeng,Cai, Qinghai,et al. Nitrogen electroreduction performance of transition metal dimers embedded into N-doped graphene: a theoretical prediction[J]. JOURNAL OF MATERIALS CHEMISTRY A,2020,8(8):4533-4543. |
| APA | Li, Hongyan,Zhao, Zhifeng,Cai, Qinghai,Yin, Lichang,&Zhao, Jingxiang.(2020).Nitrogen electroreduction performance of transition metal dimers embedded into N-doped graphene: a theoretical prediction.JOURNAL OF MATERIALS CHEMISTRY A,8(8),4533-4543. |
| MLA | Li, Hongyan,et al."Nitrogen electroreduction performance of transition metal dimers embedded into N-doped graphene: a theoretical prediction".JOURNAL OF MATERIALS CHEMISTRY A 8.8(2020):4533-4543. |
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