摘要
氨作为重要的化工产品和化工原料广泛用于工业、农业、医药等行业,在全球经济发展中有不可替代的作用.目前,工业合成氨主要采用传统的哈伯工艺(Haber-Bosch),该工艺消耗大量的化石能源,且平衡转化率相对较低.电催化氮气还原合成氨反应可以在常温常压下将N2与H2O转化为NH3,且操作简易,原料易于获取,成为科研领域重要的研究方向.其中,以d区过渡金属为代表的如非贵金属过渡金属基氧化物、氮化物、硫化物、双金属催化剂和杂原子基催化剂展现出了良好的催化性能.本文重点综述了过渡金属基电催化氮还原反应(E-NRR)电催化制氨的最新进展,包括其面临的挑战、反应机理、E-NRR催化剂的不同材料,重点研究了结构-性能关系.从合成方案、结构修饰、活性、选择性增强和反应机制等方面介绍了提高E-NRR性能的策略和未来发展前景,为E-NRR研究领域提供参考.
Abstract
As an important chemical product and chemical raw material,ammonia is widely used in industry,agriculture,medicine and other industries,and plays an irreplaceable role in global economic development.At present,industrial ammonia synthesis mainly uses the traditional Haber-Bosch process,which consumes a lot of fossil energy and has a relatively low equilibrium conversion rate.Electrocatalytic nitrogen reduction of ammonia synthesis can convert N2 and H2O into NH3 at normal temperature and pressure,and it is easy to operate and easy to obtain raw materials,which has become an important research direction in the scientific research field.Among them,non-precious metal transition metal-based oxides,nitrides,sulfides,bimetal catalysts and heteroatom-based catalysts represented by transition metals in zone d showed good catalytic performance.This paper focuses on the recent progress of electrocatalytic ammonia production by transition metal-based electrocatalytic nitrogen reduction reaction(E-NRR),including its challenges,reaction mechanism,and different materials of E-NRR catalysts,and focuses on the structure-performance relationship.The strategies and prospects for improving the performance of E-NRR were introduced from the aspects of synthesis scheme,structure modification,activity,selective enhancement and reaction mechanism.