Single Mo Atom Supported on Defective Boron Nitride Monolayer as an Efficient Electrocatalyst for Nitrogen Fixation: A Computational Study.
Single Mo Atom Supported on Defective Boron Nitride Monolayer as an Efficient Electrocatalyst for Nitrogen Fixation: A Computational Study.
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DOI：
10.1021/jacs.7b05213
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发表时间：
2017-08
影响因子：
15
通讯作者：
Jingxiang Zhao;Zhongfang Chen
中科院分区：
文献类型：
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作者：
Jingxiang Zhao;Zhongfang Chen
在温和条件下由分子二氮（N2）生产氨（NH3）是化学中最具吸引力和挑战性的过程之一。在这里，通过密度泛函理论（DFT）计算，我们系统地研究了潜在的单一过渡金属原子（Sc到Zn，Mo，Ru，Rh，Pd和Ag）的实验可用的缺陷氮化硼（TM-BN）单层与硼单空位作为N2固定电催化剂。我们的计算表明，由有缺陷的BN纳米片支持的单个Mo原子在室温下通过具有0.19 V的相当低的超电势的酶机制表现出最高的N2固定催化活性。高自旋极化、N2 H * 物种的选择性稳定化或不稳定的NH 2 * 物种是负责Mo嵌入的BN纳米片用于N2固定的高活性的原因。这一发现为在环境条件下通过单原子电催化剂生产NH3开辟了一条新途径。
The production of ammonia (NH3) from molecular dinitrogen (N2) under mild conditions is one of the most attractive and challenging processes in chemistry. Here by means of density functional theory (DFT) computations, we systematically investigated the potential of single transition metal atoms (Sc to Zn, Mo, Ru, Rh, Pd, and Ag) supported on the experimentally available defective boron nitride (TM-BN) monolayer with a boron monovacancy as a N2 fixation electrocatalyst. Our computations revealed that the single Mo atom supported by a defective BN nanosheet exhibits the highest catalytic activity for N2 fixation at room temperature through an enzymatic mechanism with a quite low overpotential of 0.19 V. The high spin-polarization, selective stabilization of N2H* species, or destabilizing NH2* species are responsible for the high activity of the Mo-embedded BN nanosheet for N2 fixation. This finding opens a new avenue of NH3 production by single-atom electrocatalysts under ambient conditions.