Constructing the single‐site of pyridine‐based organic compounds for acetylene hydrochlorination: From theory to experiment

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 c...

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Bibliographic Details
Published in:Applied organometallic chemistry 2021-09, Vol.35 (9), p.n/a
Main Authors: Zhao, Chaoyue, Yi, Zenghuimin, Xue, Yinan, Guan, Qingxin, Li, Wei
Format: Article
Language:English
Subjects:
Acetylene
acetylene hydrochlorination
Catalysts
Catalytic activity
Catalytic converters
Chemistry
Conversion
Density functional theory
High temperature
Hydrochlorination
Liquid phases
Mercury (metal)
Mercury compounds
metal‐free catalysts
Nitrogen
Organic compounds
polyvinylchloride
pyridinic N
Selectivity
Vinyl chloride
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Summary: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. A polyvinylpyridine material was obtained by polymerization in liquid phase. 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.
ISSN:0268-2605
1099-0739
DOI:10.1002/aoc.6318