摘要
氨是一种重要的化肥生产原料和清洁能源载体,在工业上主要通过哈伯法合成,但该工艺反应条件苛刻,需要高温高压并消耗大量的化石能源。因此,开发能耗低、反应温和的合成氨方法,对于缓解能源和环境的双重压力具有重要的现实意义。近年来,在温和条件下通过电催化氮还原反应(NRR)合成氨有望替代哈伯法,但该技术的重点在于设计合理的电催化反应体系并开发高效的催化剂以提升缓慢的NRR动力学过程。为此,本文从电催化合成氨的反应机理出发,介绍了电催化氮还原体系的构建,综述了近年来电催化氮还原催化剂的发展现状,重点总结了提升NRR催化剂活性的设计策略,并对这一新兴领域面临的挑战和潜在的应用前景进行了合理的展望。
Ammonia(NH3)is one of the most important nitrogen-based fertilizers and chemicals,and is also a novel hydrogen storage material.It is made on an industrial scale via the Haber-Bosch process,which requires high temperature and high pressure to consume a large amount of energy.It is very urgent to find an environmentally benign alternative process to alleviate the crises for energy and environment.Electrocatalytic nitrogen reduction reaction(NRR)has attracted worldwide research interest.However,such process is actually hard to perform due to the inherent inertness of N2 molecules together with the low solubility in aqueous solutions.Although great research efforts have been made to explore and design suitable electrocatalysts for ammonia synthesis,the yield of ammonia is still very low.In addition,the ambiguous mechanism still remains as a major barrier for the development of NRR systems.In this review,we firstly introduced the catalytic reaction mechanisms towards NRR.Then we overviewed of the latest progress of the state-of-art catalysts in the electrocatalytic NRR.Moreover,we put more emphasis on the various rational strategies for electrocatalyst design to enhance the NRR performance,such as size effects,facets regulation,defects engineering,amorphization,which are aiming to increasing the exposed active sites or altering the electronic structure to further improve the apparent or intrinsic activity.Finally,we briefly discussed the main challenges in this field.We hope this review will offer a helpful guidance for the reasonable design of electrocatalysts towards NRR,arouse more interests in the new research field of NRR,and promote the green ammonia synthesis industrialization as soon as possible.
作者
刘晓璐
耿钰晓
郝然
刘玉萍
袁忠勇
李伟
Xiaolu Liu;Yuxiao Geng;Ran Hao;Yuping Liu;Zhongyong Yuan;Wei Li(Key Laboratory of Advanced Energy Materials Chemistry,College of Chemistry,Nankai University,Tianjin 300071,China;National Institute for Advanced Materials,School of Materials Science and Engineering,Nankai University,Tianjin 300350,China)
出处
《化学进展》
SCIE
CAS
CSCD
北大核心
2021年第7期1074-1091,共18页
Progress in Chemistry
基金
国家自然科学基金项目(No.21421001, 21573115, 21875118)资助。
关键词
氮还原反应
电催化
氨合成
催化剂设计
环境条件
nitrogen reduction reaction
electrocatalysis
ammonia synthesis
catalyst design
ambient condition
