Single and double boron atoms doped nanoporous C2N-h2D electrocatalysts for highly efficient N2 reduction reaction: a density functional theory study
Single and double boron atoms doped nanoporous C2N-h2D electrocatalysts for highly efficient N2 reduction reaction: a density functional theory study
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用于高效 N-2 还原反应的单硼原子和双硼原子掺杂纳米孔 C2N-h2D 电催化剂：密度泛函理论研究
DOI：
10.1088/1361-6528/ab1d01
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发表时间：
2019-08-16
期刊：
影响因子：
3.5
通讯作者：
Wang, Jianguo
中科院分区：
文献类型：
--
作者：
Cao, Yongyong;Deng, Shengwei;Wang, Jianguo
电催化过程是在环境条件下生产氨（NH3）的最有效方法，但开发高效且低成本的无金属电催化剂仍然是一项重大的科学挑战。因此，设计了单原子和双硼（B）原子掺杂的二维石墨烯类氮化碳（C2 N-h2 D）电催化剂（B@C2N和B-2@C2N），并通过密度泛函理论计算考察了N-2还原反应（NRR）的效率。结果表明，单、双B原子均能牢固地嵌入天然纳米孔C2 N中，对N2-具有上级催化活性。NRR在B@C2N和B-2@C2N上的反应机理均遵循酶促途径，并且B-2@C2N是一种更有效的电催化剂，与B@C2N（0.29 eV）相比具有极低的过电位（0.19 eV）。在低能区，N-2的加氢在热力学上比制氢更有利，从而提高了NRR的选择性。基于这些结果，一种新的双原子策略可能有助于指导高效NRR电催化剂的实验合成。
The electrocatalytical process is the most efficient way to produce ammonia (NH3) under ambient conditions, but developing a highly efficient and low-cost metal-free electrocatalysts remains a major scientific challenge. Hence, single atom and double boron (B) atoms doped 2D graphene-like carbon nitride (C2N-h2D) electrocatalysts have been designed (B@C2N and B-2@C2N), and the efficiency of N-2 reduction reaction (NRR) is examined by density functional theory calculation. The results show that the single and double B atoms can both be strongly embedded in natural nanoporous C2N with superior catalytic activity for N-2 activation. The reaction mechanisms of NRR on the B@C2N and B-2@C2N are both following an enzymatic pathway, and B-2@C2N is a more efficient electrocatalyst with extremely low overpotential of 0.19 eV comparing to B@C2N (0.29 eV). In the low energy region, the hydrogenation of N-2 is thermodynamically more favorable than the hydrogen production, thereby improving the selectivity for NRR. Based on these results, a new double-atom strategy may help guiding the experimental synthesis of highly efficient NRR electrocatalysts.