Considering Electrocatalytic Ammonia Synthesis via Bimetallic Dinitrogen Cleavage
Considering Electrocatalytic Ammonia Synthesis via Bimetallic Dinitrogen Cleavage
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DOI：
10.1021/acscatal.0c02606
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发表时间：
2020-10-02
期刊：
影响因子：
12.9
通讯作者：
Miller, Alexander J. M.
中科院分区：
文献类型：
--
作者：
Bruch, Quinton J.;Connor, Gannon P.;Miller, Alexander J. M.
尽管能够利用质子供体和化学还原剂将氮气还原为氨的分子催化剂的开发取得了进展，但分子电催化剂的发现还很少。这一观点考虑了基于N-2裂解成金属氮化物络合物的机理的电催化剂的发展前景。通过了解控制沿着电化学N-2裂解路径的单个步骤的反应性的因素，确定了新进展的机会。介绍了用于N-2电化学反应、桥联N-2络合物的形成、N-2的热或光化学裂解以及将氮化物配体转化为氨的配体设计原理，重点介绍了最新进展和作者在Re络合物方面的合作工作。
Despite advances in the development of molecular catalysts capable of reducing dinitrogen to ammonia using proton donors and chemical reductants, few molecular electrocatalysts have been discovered. This Perspective considers the prospects of electrocatalyst development based on a mechanism featuring the cleavage of N-2 into metal nitride complexes. By understanding the factors that control the reactivity of individual steps along the electrochemical N-2 cleavage path, opportunities for new advances are identified. Ligand design principles for facile electrochemical N-2 binding, formation of bridging N-2 complexes, thermal or photochemical N-2 cleavage, and conversion of a nitride ligand into ammonia are described, featuring recent advances and the authors' collaborative work on rhenium complexes.