Unveiling the underlying mechanism of nitrogen fixation by a new class of electrocatalysts two-dimensional TM@g-C4N3 monosheets

催化作用 电催化剂 化学 氮气 吸附 选择性 电化学 无机化学 物理化学 电极 生物化学 有机化学
作者
Xiaolin Wang,Li‐Ming Yang
出处
期刊:Applied Surface Science [Elsevier BV]
卷期号:576: 151839-151839 被引量:44
标识
DOI:10.1016/j.apsusc.2021.151839
摘要

The potential of TM atoms embedded g-C4N3 as a new class of electrocatalysts ([email protected]4N3, TM = 3d, 4d and 5d transition metal) towards nitrogen reduction reaction (NRR) were systematically investigated through the combination of high-throughput screening and first-principles calculations. Among 30 candidate materials, [email protected]4N3 (TM = V, Tc, Os, Pt) exhibited the highest activity for electrocatalytic N2 reduction to produce NH3. Particularly, [email protected]4N3 is identified as the most active catalyst for NRR with onset potential of −0.37 V. Interestingly, a volcano curve between Uonset (onset potential) and ΔEads(*N2) (the adsorption energy of N2) is established, and thus ΔEads(*N2) can be used as a descriptor to characterize the activity of catalysts. Among all investigated catalysts, the lowest onset potential of [email protected]4N3 can be attributed to its moderate adsorption energies for N2. After in-deep analysis of the intrinsic properties of the four catalysts, we found that the increasing order of catalytic activity is consistent with the increasing order of d-band center (εd) of the four catalysts. In addition, the excellent thermal stability of the four catalysts is verified via simulated annealing at 500 K for 10 ps. Furthermore, three catalysts [email protected]4N3 (TM = V, Tc, Pt) demonstrate good selectivity. Therefore, [email protected]4N3 is a promising electrocatalyst for NRR. Our work opens the way for g-C4N3 as a new type of support to construct efficient single-atom catalyst for electrocatalytic ammonia synthesis. The predicted [email protected]4N3 catalysts will provide useful guidance for experimental synthesis and rational design of catalysts in future.
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