文献类型：期刊文献

英文题名：Regulating the states of Ni species by controlling the silanols of MCM-41 support to promote the hydrogenation of maleic anhydride

作者：Zhuang, Jianguo[1];Yan, Siyan[1];Zhang, Peng[1];Liu, Xinhui[1];Zhao, Yitao[1];Yu, Yijun[1];Wang, Yuchen[1];Zhao, Qichao[1];Wu, Haidan[1];Zhu, Xuedong[1];Yang, Fan[1]

机构：[1]East China Univ Sci & Technol, Engn Res Ctr Large Scale Reactor Engn & Technol, Minist Educ, Shanghai 200237, Peoples R China

年份：2023

卷号：335

外文期刊名：FUEL

收录：;EI(收录号：20225013239406);WOS:【SCI-EXPANDED(收录号:WOS:000990018700001)】；

基金：The authors are grateful for the financial support from National Natural Science Foundation of China (21776076) and the Fundamental Research Funds for the Central Universities (JKA01211710) . The au- thors also thank Research Center of Analysis and Test of East China University of Science and Technology for the help on the characterizations.

语种：英文

外文关键词：Maleic anhydride; Succinic anhydride; Hydrogenation; Ni-based catalyst; Silanols

摘要：Nickel (Ni) supported on MCM-41 zeolite as hydrogenation catalysts have been widely applied in various reactions, however, the synergism between Ni and the support remains obscure. To prepare more efficient catalysts and reveal the metal-support interaction, MCM-41 zeolite was modified with ammonium hexafluorosilicate (AHFS) before Ni loading. Results show that fluoride ions could selectively convert the vicinal silanols into isolated silanols on MCM-41 surface, which weakens the interactions between Ni precursors and the SiO2 supports. Over the modified MCM-41 zeolites, the attenuated interaction results in the agglomeration of NiO particles that is more easily to be reduced, rather than the formation of nickel phyllosilicate which is extraordinarily difficult towards reduction. The easily-reduced Ni particles provided more adsorption sites for C--C bond instead of C--O bond, and the adsorption strength was also regulated. Therefore, the AHFS modified catalyst demonstrated a notable enhancement in hydrogenation of maleic anhydride (MA) into succinic anhydride (SA), presenting 98.4 % MA conversion and 99.8 % SA selectivity at 90 degrees C under 3.0 MPa H2. Moreover, the optimum catalyst was recycled for 5 runs to analyze the deactivation mechanism, it was found out that the loss of activities stems from the leaching of large Ni particles. Overall, our work shed light on the metal-support interactions for Ni/MCM-41 catalyst, determining the vicinal hydroxyl groups were responsible for the state of Ni species, which is helpful for the rational design of other hydrogenation catalysts.