非周期性原子排列实现电化学氮还原和析氧反应性能的增强

Breaking the periodic arrangement of atoms for the enhanced electrochemical reduction of nitrogen and water oxidation

制备低成本的高效电催化剂是缓解目前面临的环境能源危机的重要方式.通过无定型化和构建异质结构可以有效地改变催化剂的电子结构,从而实现电催化性能的稳步提升.但是对于两者之间协同作用的研究则相对较少.在本文中,我们构建了富含异质结构的无定型FeMo基(a-FeMo)电催化剂,并系统评估了该催化剂的氮气还原和析氧反应性能.得益于无定型结构引起的活性位点数目的增多和异质结构引发的电子的重新分布,a-FeMo催化剂表现出优异的电化学催化性能.在-0.1 V vs.RHE的电势下,a-FeMo催化剂表现出29.15%的法拉第效率和71.78μg_(NH_(3)) mg_(cat.)^(-1) h^(-1)的氨气产率.这为合理设计具有低成本优势、高活性和长时间稳定性的优异催化剂提供了有益的参考.

The development of cost-effective and highperformance electrocatalysts has been increasingly studied to mitigate upcoming energy and environmental challenges.Amorphization and heterointerface engineering have played significant roles in the rational design of electrocatalysts and modulation of their electrocatalytic activities.However,the synergistic effect between amorphization and heterointerfaces has been scarcely reported.As a proof-of-concept attempt,we develop amorphous FeMo(a-FeMo)electrocatalysts with an abundance of heterointerfaces that are composed of amorphous components and evaluate their electrocatalytic performances toward the nitrogen reduction reaction and oxygen evolution reaction(OER).Benefitting from the synergistic effect between the amorphous nature of the a-FeMo electrocatalysts,which offer a high density of active sites,and significant electron redistribution at the heterointerfaces,the electrocatalysts exhibit a high Faradaic efficiency of 29.15%,an elevated yield rate of 71.78μg_(NH_(3)) mg_(cat.)^(-1) h^(-1) with long-term stability at a potential of-0.1V vs.reversible hydrogen electrode and excellent electrocatalytic activity toward the OER.This study provides a promising and effective method for the rational design of low-cost heterogeneous catalysts with desirable efficiency,selectivity,and stability.