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Constructing the single‐site of pyridine‐based organic compounds for acetylene hydrochlorination: From theory to experiment
Author(s) -
Zhao Chaoyue,
Yi Zenghuimin,
Xue Yinan,
Guan Qingxin,
Li Wei
Publication year - 2021
Publication title -
applied organometallic chemistry
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.53
H-Index - 71
eISSN - 1099-0739
pISSN - 0268-2605
DOI - 10.1002/aoc.6318
Subject(s) - acetylene , chemistry , pyridine , catalysis , vinyl chloride , polymerization , carbonization , chloride , selectivity , polymer , organic chemistry , polymer chemistry , inorganic chemistry , copolymer , adsorption
Acetylene hydrochlorination reaction requires toxic mercuric chloride catalyst, which caused serious environmental pollution by mercury in recent years. Though Au‐based catalysts show the best catalytic activity and high rates of acetylene conversion, much work still needs to be done to reduce the cost before their large‐scale applications. Here, a pure pyridine‐based organic polymer was successfully designed and assembled, which contains only one nitrogen species and exhibits a high activity with acetylene conversion reaching 88% and the selectivity of vinyl chloride above 99%. Both experimental and density functional theory (DFT) studies directly demonstrate that the pyridinic N atom in pyridine ring is the active site of the catalyst and the insertion of acetylene to HCl might be the rate‐determining step. Different from traditional carbonization and aminating treatment at high temperature, the pyridine‐based polymers were obtained by polymerization in liquid phase. Besides, the activity of the catalyst may be determined by these combined effects of surface area, pores structure, and the amount of pyridinic N.