无氮铁基电催化氮气分子活化的研究进展  

Research progress of nitrogen-free iron-based electrocatalytic reduction of dinitrogen

作　　者：李梦杰 陈昕煜 臧宏瑛[1] LI Meng-jie;CHEN Xin-yu;ZANG Hong-ying(Faculty of Chemistry,Northeast Normal University,Changchun 130024,China)

机构地区：[1]东北师范大学化学学院,吉林长春130024

出　　处：《分子科学学报》2021年第4期297-310,共14页Journal of Molecular Science

基　　金：国家自然科学基金资助项目(21871042);吉林省自然科学基金资助项目(20200201083JC);吉林省教育厅自然科学基金资助项目(JJKH20201169KJ)。

摘　　要：氨气不仅被广泛应用于制造氮肥,还是一种易液化且无碳的绿色能源载体.工业固氮的Haber-Bosch工艺每年消耗全球超过1%的能耗,还伴随着大量二氧化碳气体的排放等问题,而电催化氮还原反应可以在常温常压下低能耗地合成氨,因此设计高催化性能的氮气分子活化电催化剂成为科研工作者的首要研究目标.受自然界中固氮酶和Haber-Bosch工艺催化剂的启发,价格低廉且含量丰富的铁基催化剂受到广泛关注.但由于含氮催化剂可能导致氮还原假阳性等问题,因此本文综述了无氮铁基电催化剂(氧化物、硫化物、碳化物、磷化物和铁基金属有机骨架等)在氮还原方面的最新研究进展,为研究人员在执行氮还原实验确定氮源的操作中提出合理建议,希望可以为铁基催化剂的设计和开发提供新的研究思路和参考.With the rapid growth of the world′s population, pressing energy problems and growing environmental concerns, ammonia has received widespread attention as an indispensable chemical raw material for nitrogen fertilizer synthesis and chemical production. Besides, ammonia serves as a carbon-free green energy carrier and a potential transportation fuel because it is easily turned into a liquid. Therefore, ammonia is expected to be a candidate for a carbon-free hydrogen economy in the bright future. Currently, artificial nitrogen fixation to synthesize ammonia heavily relies on the Haber-Bosch process. It consumes more than 1% of the world′s energy produced every year, and also emits over 300 million metric tons of carbon dioxide, which causes the greenhouse effect. Accordingly, it is highly desirable to develop more sustainable and less energy-consuming methodologies to replace the Haber-Bosch process for ammonia synthesis. Fortunately, the electrocatalytic reduction of dinitrogen can realize ammonia synthesis with low energy consumption under ambient conditions. It is the primary research goal to design an electrocatalyst with high catalytic performance. Due to their rich content and low price, transition metal electrocatalysts have become an ideal substitute for noble metal catalysts in the field of electrocatalysis. Among the many transition metals, Fe is not only an important catalyst in the Haber-Bosch process, but also a nitrogen activation site in nitrogenase. As a result, low-cost and abundant iron-based catalysts have attracted widespread attention in recent years. However, nitrogen-containing catalysts may cause problems such as false positive nitrogen reduction results. Therefore, we recommend to focus more on the nitrogen-free iron-based electrocatalyst. In this review, we summarize the latest research progress of nitrogen-free iron-based electrocatalysts in nitrogen reduction under mild conditions. Firstly, we briefly discuss the electrocatalytic nitrogen reduction reaction mechanism and analysis the

关 键 词：氮还原 电化学合成氨 铁基催化剂 

分 类 号：O646[理学—物理化学]