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Acetylene hydrochlorination over supported ionic liquid phase (SILP) gold-based catalyst: Stabilization of cationic Au species via chemical activation of hydrogen chloride and corresponding mechanisms
Chinese Journal of Catalysis ( IF 15.7 ) Pub Date : 2021-02-01 , DOI: 10.1016/s1872-2067(20)63617-8
Jia Zhao , Saisai Wang , Bolin Wang , Yuxue Yue , Chunxiao Jin , Jinyue Lu , Zheng Fang , Xiangxue Pang , Feng Feng , Lingling Guo , Zhiyan Pan , Xiaonian Li

Abstract The activation of HCl by cationic Au in the presence of C2H2 is important for the construction of active Au sites and in acetylene hydrochlorination. Here, we report a strategy for activating HCl by the Au-based supported ionic liquid phase (Au–SILP) technology with the [N(CN)2−] anion. This strategy enables HCl to accept electrons from [N(CN)2−] anions in Au–[N(CN)2−] complexes rather than from pure [Bmim][N(CN)2], leading to notable improvement in both the reaction path and the stability of the catalyst without changing the reaction triggered by acetylene adsorption. Furthermore, the induction period of the Au–SILP catalyst was shown to be absent in the reaction process due to the high Au(III) content in the Au(III)/Au(I) site and the high substrate diffusion rate in the ionic liquid layer. This work provides a facile method to improve the stability of Au-based catalysts for acetylene hydrochlorination.

中文翻译:

负载型离子液相 (SILP) 金基催化剂上的乙炔氢氯化:通过氯化氢的化学活化和相应机制稳定阳离子 Au 物种

摘要 在 C2H2 存在下,阳离子 Au 对 HCl 的活化对于构建活性 Au 位点和乙炔氢氯化非常重要。在这里,我们报告了一种通过使用 [N(CN)2−] 阴离子的 Au 基负载离子液相 (Au-SILP) 技术激活 HCl 的策略。这种策略使 HCl 能够接受来自 Au-[N(CN)2-] 复合物中的 [N(CN)2-] 阴离子而不是来自纯 [Bmim][N(CN)2] 的电子,从而导致两者的显着改善在不改变乙炔吸附引发的反应的情况下,反应路径和催化剂的稳定性。此外,由于 Au(III)/Au(I) 位点中的高 Au(III) 含量和离子中的高底物扩散速率,Au-SILP 催化剂的诱导期在反应过程中不存在。液体层。
更新日期:2021-02-01
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