| Computational Screening of Single Atoms Anchored on Defective Mo2CO2 MXene Nanosheet as Efficient Electrocatalysts for the Synthesis of Ammonia | |
Wang, Shuo1; Li, Lei2; San Hui, Kwan3; Bin F(宾峰)4 ; Zhou, Wei5; Fan, Xi6; Zalnezhad, E.7; Li, Jing1; Hui, Kwun Nam1
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| Corresponding Author | Li, Lei([email protected]) ; San Hui, Kwan([email protected]) ; Li, Jing([email protected]) ; Hui, Kwun Nam([email protected]) |
| Source Publication | ADVANCED ENGINEERING MATERIALS
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| 2021-07-22 | |
| Pages | 8 |
| ISSN | 1438-1656 |
| Abstract | The electrochemical nitrogen reduction reaction (NRR) over single-atom catalysts (SACs) anchored on Mo vacancies of Mo2CO2 MXene nanosheets under ambient conditions suffers from poor selectivity, low yield, and low Faradaic efficiency because of their sluggish kinetics and the competing hydrogen evolution reaction. Herein, density functional theory calculations are performed to improve the understanding of the selectivity and yielding of ammonia through NRR over various isolated SACs, that is, from Sc to Au, anchored on the Mo vacancy of the Mo2CO2 MXene nanosheet (denoted as MO2CO2-M-SA). The potential-determining step of the NRR shows that eight candidates (i.e., Y, Zr, Nb, Hf, Ta, W, Re, and Os) confined on the defective Mo2CO2 layer could promote the electroreduction from N-2 to NH3. Among these, Mo2CO2-Y-SA presented the lowest reported reaction Presents the lowest reported reaction energy barrier (0.08 eV) through the distal pathway and high selectivity to NRR compared with the previously synthesized Mo2CO2-Ru-SA with a relatively high energy barrier (0.65 eV) and poor selectivity. In addition, the formation energy of Mo2CO2-Y-SA is more negative than that of the Mo2CO2-Ru-SA catalyst, suggesting that the experimental preparation of the Mo2CO2-Y-SA catalyst is highly feasible. This work lays a solid foundation for improving the rational design of MXene-based systems as efficient electrocatalysts for the synthesis of ammonia. |
| Keyword | density functional theory calculations electrocatalysis MXene nitrogen reduction reaction single-atom catalysts |
| DOI | 10.1002/adem.202100405 |
| Indexed By | SCI ; EI |
| Language | 英语 |
| WOS ID | WOS:000675530700001 |
| WOS Keyword | HYDROGEN EVOLUTION REACTION ; NITROGEN REDUCTION ; N-2 FIXATION ; CATALYSTS ; MONOLAYER ; NITRIDE |
| WOS Research Area | Materials Science |
| WOS Subject | 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 ; Biomechacin, Texas, USA[BMC200101] |
| Funding Organization | Science and Technology Development Fund, Macau SAR ; University of Macau ; UEA ; Biomechacin, Texas, USA |
| Classification | 二类 |
| Ranking | 3+ |
| Contributor | Li, Lei ; San Hui, Kwan ; Li, Jing ; Hui, Kwun Nam |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://dspace.imech.ac.cn/handle/311007/87065 |
| Collection | 高温气体动力学国家重点实验室 |
| Affiliation | 1.Univ Macau, Inst Appl Phys & Mat Engn, Minist Educ, Joint Key Lab, Ave Univ, Taipa, Macau, Peoples R China; 2.Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Collaborat Innovat Ctr Chem Energy Mat, Hefei 230026, Peoples R China; 3.Univ East Anglia, Fac Sci, Sch Engn, Norwich NR4 7TJ, Norfolk, England; 4.Chinese Acad Sci, Inst Mech, State Key Lab High Temp Gas Dynam, Beijing 100190, Peoples R China; 5.Xiamen Univ, Dept Mech & Elect Engn, Xiamen 361005, Peoples R China; 6.Chinese Acad Sci, Ningbo Inst Mat Technol, Engn, Ningbo 315201, Peoples R China; 7.Univ Texas San Antonio, Dept Chem & Biomed Engn, San Antonio, TX USA |
| Recommended Citation GB/T 7714 | Wang, Shuo,Li, Lei,San Hui, Kwan,et al. Computational Screening of Single Atoms Anchored on Defective Mo2CO2 MXene Nanosheet as Efficient Electrocatalysts for the Synthesis of Ammonia[J]. ADVANCED ENGINEERING MATERIALS,2021:8.Rp_Au:Li, Lei, San Hui, Kwan, Li, Jing, Hui, Kwun Nam |
| APA | Wang, Shuo.,Li, Lei.,San Hui, Kwan.,宾峰.,Zhou, Wei.,...&Hui, Kwun Nam.(2021).Computational Screening of Single Atoms Anchored on Defective Mo2CO2 MXene Nanosheet as Efficient Electrocatalysts for the Synthesis of Ammonia.ADVANCED ENGINEERING MATERIALS,8. |
| MLA | Wang, Shuo,et al."Computational Screening of Single Atoms Anchored on Defective Mo2CO2 MXene Nanosheet as Efficient Electrocatalysts for the Synthesis of Ammonia".ADVANCED ENGINEERING MATERIALS (2021):8. |
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| Jp2021F252.pdf（1142KB） | 期刊论文 | 出版稿 | 开放获取 | CC BY-NC-SA | View Download | |
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