Ren Xiang, Zhao Jinxiu, Wei Qin, Ma Yongjun, Guo Haoran, Liu Qian, Wang Yuan, Cui Guanwei, Asiri Abdullah M, Li Baihai, Tang Bo, Sun Xuping
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu, 610054 Sichuan, China.
Key Laboratory of Interfacial Reaction & Sensing Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan, 250022 Shandong, China.
ACS Cent Sci. 2019 Jan 23;5(1):116-121. doi: 10.1021/acscentsci.8b00734. Epub 2018 Dec 19.
The synthesis of NH is mainly dominated by the traditional energy-consuming Haber-Bosch process with a mass of CO emission. Electrochemical conversion of N to NH emerges as a carbon-free process for the sustainable artificial N reduction reaction (NRR), but requires an efficient and stable electrocatalyst. Here, we report that the MoC nanorod serves as an excellent NRR electrocatalyst for artificial N fixation to NH with strong durability and acceptable selectivity under ambient conditions. Such a catalyst shows a high Faradaic efficiency of 8.13% and NH yield of 95.1 μg h mg at -0.3 V in 0.1 M HCl, surpassing the majority of reported electrochemical conversion NRR catalysts. Density functional theory calculation was carried out to gain further insight into the catalytic mechanism involved.
氨的合成主要由传统的耗能哈伯-博施法主导,该过程会排放大量的一氧化碳。将氮电化学转化为氨是一种用于可持续人工固氮反应(NRR)的无碳过程,但需要一种高效且稳定的电催化剂。在此,我们报道碳化钼纳米棒作为一种优异的NRR电催化剂,可在环境条件下将氮人工固定为氨,具有很强的耐久性和可接受的选择性。这种催化剂在0.1 M盐酸中于-0.3 V时显示出8.13%的高法拉第效率和95.1 μg h mg的氨产率,超过了大多数已报道的电化学转化NRR催化剂。进行了密度泛函理论计算以进一步深入了解其中涉及的催化机制。