期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 123, 期 36, 页码 22221-22227出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.9b04730
关键词
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资金
- Science and Technology Development Fund from Macau SAR [FDCT-0102/2019/A2]
- Research & Development Office at University of Macau [MYRG2017-00027-FST, MYRG2018-00003-IAPME]
- Natural Science Foundation of Shandong Province, China [ZR2019BA027, ZR2017QA003]
- National Natural Science Foundation of China [51431004, 11634007, 11804006]
Design of novel catalysts for the reduction of N-2 to ammonia has been urgently pursued because of various issues related to the industrial reduction technology. In this work, we perform first-principles calculations on the basis of the density-functional theory to control the edges of two-dimensional (2D) transition-metal disulfides (TMDs), including MoS2, WS2, VS2, NbS2, TiS2, and TaS2, for the achievement of optimal efficiency in nitrogen-fixation. Our calculations show that nitrogen molecules prefer to stay at the bridge-on sites of the metal edges of TMD nanoribbons because of exothermic reactions. The calculated energy barrier at each step illustrates that VS2 has the lowest potential-determining step of 0.16 eV in the distal pathway, leading to its best catalytic activity in the N-2 reduction reaction (NRR). Additionally, we find that the trend of catalytic activity of 2D TMD nanoribbons is as follows: VS2 > NbS2 > TiS2 > MoS2 > WS2 > TaS2. We show that charge transfer is critical to the reduction reaction. We further demonstrate that the edges of TMDs, especially VS2, show a higher selectivity for NRR over the hydrogen evolution reaction (HER) by investigating the competition between HER and NRR Our findings not only reveal the effect of the edges of TMDs on NRR, but also provide theoretical support to the reported experimental results in the literature. It is expectable that the 2D TMD nanoribbons, especially VS2, may find application for efficient N-2-fixation. At the same time, our work may guide the design of new catalysts for NRR.
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