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基于锡氮催化剂的乙炔氢氯化反应:氮碳点作为氮前驱体的影响

Acetylene hydrochlorination over tin nitrogen based catalysts: effect of nitrogen carbon-dots as nitrogen precursor.

作者信息

Wu Yibo, Li Fuxiang, Li Qingbin, Li Songtian, Zhao Ganqing, Sun Xuerong, Liu Peisong, He Guoxv, Han Yongjun, Cheng Liping, Luo Shiying

机构信息

College of Chemistry and Enviromental Engineering, Pingding Shan University, Pingding Shan China.

College of Chemistry and Chemical Engineering, Taiyuan University of technology, Taiyuan China.

出版信息

Turk J Chem. 2021 Oct 19;45(5):1463-1475. doi: 10.3906/kim-2102-67. eCollection 2021.

Abstract

The catalysts comprising the main active compounds of Sn-Nx were synthesized using trichlorophenylstannane ((CH)ClSn), nitrogen carbon-dots (NCDs), and activated carbon (AC) as starting materials, and the activity and stability of catalysts was evaluated in the acetylene hydrochlorination. According to the results on the physical and chemical properties of catalysts (TEM, XRD, BET, XPS and TG), it is concluded that NCDs@AC can increase (CH)ClSn dispersity, retard the coke deposition of (CH)ClSn/AC and lessen the loss of (CH)ClSn, thereby further promoting the stability of (CH)ClSn/AC. Based on the characterization results of CH-TPD and HCl adsorption experiments, we proposed that the existence of Sn-N can effectively strengthen the reactants adsorption of catalysts. By combing the FT-IR, CH-TPD and Rideal-Eley mechanism, the catalytic mechanism, in which CH is firstly adsorbed on (CH)ClSn to form (CH)ClSn-CH and then reacted with HCl to produce vinyl chloride, is proposed.

摘要

以三氯苯基锡((CH)ClSn)、氮掺杂碳点(NCDs)和活性炭(AC)为原料合成了含Sn-Nx主要活性化合物的催化剂,并在乙炔氢氯化反应中对催化剂的活性和稳定性进行了评价。根据催化剂的物理和化学性质(TEM、XRD、BET、XPS和TG)结果,得出NCDs@AC可以提高(CH)ClSn的分散性,延缓(CH)ClSn/AC的积炭并减少(CH)ClSn的损失,从而进一步提高(CH)ClSn/AC的稳定性。基于CH-TPD和HCl吸附实验的表征结果,我们提出Sn-N的存在可以有效增强催化剂对反应物的吸附。通过结合FT-IR、CH-TPD和里迪尔-埃利机理,提出了催化机理,即CH首先吸附在(CH)ClSn上形成(CH)ClSn-CH,然后与HCl反应生成氯乙烯。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ad71/8596526/a27521c5ea43/turkjchem-45-1463-fig001.jpg

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