| High-Throughput Screening of Nitrogen-Coordinated Bimetal Catalysts for Multielectron Reduction of CO2 to CH4 with High Selectivity and Low Limiting Potential | |
Wang Shuo1; Li Lei6; Li Jing1; Yuan Chengzong1; Kang Yao1; Hui Kwan San7; Zhang Jintao2; Bin F(宾峰)3 ; Fan Xi4; Chen Fuming5; Hui Kwun Nam1
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| Corresponding Author | Li, Lei([email protected]) ; Hui, Kwan San([email protected]) ; Chen, Fuming([email protected]) ; Hui, Kwun Nam([email protected]) |
| Source Publication | JOURNAL OF PHYSICAL CHEMISTRY C
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| 2021-04-08 | |
| Volume | 125Issue:13Pages:7155-7165 |
| ISSN | 1932-7447 |
| Abstract | Significant challenges remain for developing efficient catalysts in an electrochemical multielectron CO2 reduction reaction (CO2RR), which usually suffers from poor activity and selectivity. Motivated by the recent experimental progress in fabricating dual-metal atom catalysts (DMACs) in N-doped graphene materials (graphene-N6V4; N: nitrogen and V: vacancy), we sampled eight types of homonuclear (N6V4-M-2, M = Cr, Mn, Fe, Co, Ni, Cu, Pd, and Ag) catalysts and 28 types of heteronuclear (N6V4-M1M2) catalysts to study CO2RR activity via first-principles high-throughput screening. Using stability, activity, and selectivity as indicators along with the broken conventional scaling relationship, N6V4-AgCr was selected as a promising candidate for deep CO2 reduction to methane with a low overpotential of 0.55 V after two screening rounds. Further analysis showed that a frustrated Lewis pair, formed between metal and the para-N, owing to the difference in the electronic arrangement of the d orbitals of various transition metals, caused a difference in the spin polarization of the systems and affected the catalytic performance of each DMAC. Our work not only provides a solid strategy for screening potential catalysts but also demonstrates that their CO2 reduction activities originate from the various atomic and electronic structures of DMACs. |
| DOI | 10.1021/acs.jpcc.0c10802 |
| Indexed By | SCI ; EI |
| Language | 英语 |
| WOS ID | WOS:000639044400015 |
| WOS Research Area | Chemistry ; Science & Technology - Other Topics ; Materials Science |
| WOS Subject | Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary |
| Funding Project | Science and Technology Development Fund, Macau SAR[0191/2017/A3] ; Science and Technology Development Fund, Macau SAR[0041/2019/A1] ; Science and Technology Development Fund, Macau SAR[0046/2019/AFJ] ; Science and Technology Development Fund, Macau SAR[0021/2019/AIR] ; University of Macau[MYRG2017-00216-FST] ; University of Macau[MYRG2018-00192-IAPME] ; UEA ; Science and Technology Program of Guangzhou[2019050001] ; National Key Research and Development Program of China[2019YFE0198000] ; Pearl River Talent Program[2019QN01L951] |
| Funding Organization | Science and Technology Development Fund, Macau SAR ; University of Macau ; UEA ; Science and Technology Program of Guangzhou ; National Key Research and Development Program of China ; Pearl River Talent Program |
| Classification | 二类 |
| Ranking | 3+ |
| Contributor | Li, Lei ; Hui, Kwan San ; Chen, Fuming ; Hui, Kwun Nam |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://dspace.imech.ac.cn/handle/311007/86462 |
| Collection | 高温气体动力学国家重点实验室 |
| Affiliation | 1.Univ Macau, Inst Appl Phys & Mat Engn, Joint Key Lab Minist Educ, Taipa 999078, Macau, Peoples R China; 2.Shandong Univ, Sch Chem & Chem Engn, Jinan 250100, Peoples R China; 3.Chinese Acad Sci, Inst Mech, State Key Lab High Temp Gas Dynam, Beijing 100190, Peoples R China; 4.Chinese Acad Sci, Ningbo Inst Mat Technol, Engn, Ningbo 315201, Peoples R China; 5.South China Normal Univ, Sch Phys & Telecommun Engn, Guangdong Prov Key Lab Quantum Engn & Quantum Mat, Guangzhou 510006, Guangdong, Peoples R China; 6.Univ Sci & Technol China, Collaborat Innovat Ctr Chem Energy Mat, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China; 7.Univ East Anglia, Sch Engn, Fac Sci, Norwich NR4 7TJ, Norfolk, England |
| Recommended Citation GB/T 7714 | Wang Shuo,Li Lei,Li Jing,et al. High-Throughput Screening of Nitrogen-Coordinated Bimetal Catalysts for Multielectron Reduction of CO2 to CH4 with High Selectivity and Low Limiting Potential[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2021,125,13,:7155-7165.Rp_Au:Li, Lei, Hui, Kwan San, Chen, Fuming, Hui, Kwun Nam |
| APA | Wang Shuo.,Li Lei.,Li Jing.,Yuan Chengzong.,Kang Yao.,...&Hui Kwun Nam.(2021).High-Throughput Screening of Nitrogen-Coordinated Bimetal Catalysts for Multielectron Reduction of CO2 to CH4 with High Selectivity and Low Limiting Potential.JOURNAL OF PHYSICAL CHEMISTRY C,125(13),7155-7165. |
| MLA | Wang Shuo,et al."High-Throughput Screening of Nitrogen-Coordinated Bimetal Catalysts for Multielectron Reduction of CO2 to CH4 with High Selectivity and Low Limiting Potential".JOURNAL OF PHYSICAL CHEMISTRY C 125.13(2021):7155-7165. |
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| Jp2021F172.pdf（6747KB） | 期刊论文 | 出版稿 | 开放获取 | CC BY-NC-SA | View Download | |
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