Nan Haifeng, Liu Yaping, Li Qingqing, Shen Peng, Chu Ke
School of Materials Science and Engineering, Lanzhou Jiaotong University, Lanzhou 730070, China.
Chem Commun (Camb). 2020 Sep 14;56(71):10345-10348. doi: 10.1039/d0cc04764c. Epub 2020 Aug 6.
The antimony sulfide SbS is firstly explored as a Janus catalyst for highly selective nitrogen reduction reaction (NRR). The developed SbS nanoflowers delivered an excellent faradaic efficiency of 24.1% and a high NH yield of 33.4 μg h mg at -0.3 V. Theoretical calculations revealed that the high NRR selectivity of SbS originated from the Janus role of active Sb centers: on one hand, Sb exhibited a strong Sb5p-N2p hybridization upon initial N protonation, capable of effectively activating the NRR with a low reaction barrier. On the other hand, Sb could concurrently impede the hydrogen evolution by hindering the H adsorption.
首次探索硫化锑(SbS)作为用于高选择性氮还原反应(NRR)的双面催化剂。所制备的SbS纳米花在-0.3 V时表现出24.1%的优异法拉第效率和33.4 μg h mg的高NH产率。理论计算表明,SbS的高NRR选择性源于活性Sb中心的双面作用:一方面,Sb在初始N质子化时表现出强烈的Sb5p-N2p杂化,能够以低反应势垒有效激活NRR。另一方面,Sb可以通过阻碍H吸附同时抑制析氢反应。