Chen Chen, Yan Dafeng, Wang Yu, Zhou Yangyang, Zou Yuqin, Li Yafei, Wang Shuangyin
State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, Hunan, 410082, P. R. China.
College of Chemistry and Materials Science, Nanjing Normal University, Nanjing, Jiangsu, 210023, P. R. China.
Small. 2019 Feb;15(7):e1805029. doi: 10.1002/smll.201805029. Epub 2019 Jan 16.
Electrochemical synthesis has garnered attention as a promising alternative to the traditional Haber-Bosch process to enable the generation of ammonia (NH ) under ambient conditions. Current electrocatalysts for the nitrogen reduction reaction (NRR) to produce NH are comprised of noble metals or transitional metals. Here, an efficient metal-free catalyst (BCN) is demonstrated without precious component and can be easily fabricated by pyrolysis of organic precursor. Both theoretical calculations and experiments confirm that the doped BN pairs are the active triggers and the edge carbon atoms near to BN pairs are the active sites toward the NRR. This doping strategy can provide sufficient active sites while retarding the competing hydrogen evolution reaction (HER) process; thus, NRR with high NH formation rate (7.75 µg h mg ) and excellent Faradaic efficiency (13.79%) are achieved at -0.3 V versus reversible hydrogen electrode (RHE), exceeding the performance of most of the metallic catalysts.
作为在环境条件下生成氨（NH₃）的一种有前景的替代传统哈伯-博施法的方法，电化学合成已受到关注。目前用于氮还原反应（NRR）以生产NH₃的电催化剂由贵金属或过渡金属组成。在此，展示了一种不含贵金属成分的高效无金属催化剂（BCN），它可以通过有机前驱体的热解轻松制备。理论计算和实验均证实，掺杂的B-N对是活性触发因素，靠近B-N对的边缘碳原子是NRR的活性位点。这种掺杂策略可以提供足够的活性位点，同时抑制竞争性析氢反应（HER）过程；因此，相对于可逆氢电极（RHE）在-0.3 V时实现了具有高NH₃生成速率（7.75 μg h⁻¹ mg⁻¹）和优异法拉第效率（13.79%）的NRR，超过了大多数金属催化剂的性能。
