Bai Jia-Qi, Xu Jiahui, Ma Mei, Miao Zhengan, Yu Jiawen, Liu Huangfei, Qian Zhangkai, Cai Mengdie, Cheng Qin, Jiang Yong, Sun Song
School of Chemistry and Chemical Engineering, Anhui University, Hefei 230601, Anhui, People's Republic of China.
Sennics Co., Ltd. Anhui, 1111 West Cuihuliu Road, Circulation Economical Industrial Park, Tongling 244000, People's Republic of China.
Langmuir. 2024 Jun 11;40(23):12179-12190. doi: 10.1021/acs.langmuir.4c01132. Epub 2024 May 29.
As haloanilines (HANs) are important organic intermediates and fine chemicals, their preparation over non-noble-metal-based catalysts by catalytic hydrogenation has attracted wide attention. However, the reaction suffers from relatively harsh conditions. Herein, we found that a 3.5%Ni/P25 catalyst exhibited superior photo-thermal catalytic activity with a TOF of 5207 h for hydrogenation of -chloronitrobenzene (-CNB) to -chloroaniline under a 300 W full spectrum, which was much higher than that of photo- and thermal catalysis alone. Moreover, the 3.5%Ni/P25 catalyst could be recycled 4 times and was effective for the hydrogenation of various halonitrobenzenes (HNBs) with superior selectivity. Furthermore, the kinetic research showed that the excellent catalytic performance could be attributed to the better activation and dissociation of H by photo-thermal catalysis and the hydrogenation of -CNB obeyed the condensation routine by ionic hydrogenation over 3.5%Ni/P25.
由于卤代苯胺是重要的有机中间体和精细化学品,通过催化加氢在非贵金属基催化剂上制备卤代苯胺引起了广泛关注。然而,该反应的条件相对苛刻。在此,我们发现3.5%Ni/P25催化剂在300W全光谱下对氯硝基苯(-CNB)加氢生成氯苯胺表现出优异的光热催化活性,其TOF为5207 h-1,远高于单独的光催化和热催化。此外,3.5%Ni/P25催化剂可循环使用4次,对各种卤代硝基苯(HNBs)的加氢反应具有优异的选择性。此外,动力学研究表明,优异的催化性能可归因于光热催化对H的更好活化和解离,并且在3.5%Ni/P25上,-CNB的加氢反应遵循离子加氢的缩合历程。