Hollow Carbon Nanospheres Decorated with Abundant Pyridinic N+O– for Efficient Acetylene Hydrochlorination

乙炔 催化作用 碳纤维 吸附 杂原子 活动站点 苯胺 化学 化学工程 炭黑 材料科学 无机化学 有机化学 戒指(化学) 复合数 工程类 复合材料 天然橡胶
作者
Feng Li,Haiyang Zhang,Miaomiao Zhang,Linfeng Li,Lisha Yao,Wencai Peng,Jinli Zhang
出处
期刊:ACS Sustainable Chemistry & Engineering [American Chemical Society]
卷期号:10 (1): 194-203 被引量:20
标识
DOI:10.1021/acssuschemeng.1c05661
摘要

Considering the disadvantages of metallic catalyst and benchmark commercial activated carbon for acetylene hydrochlorination, such as considerable cost, metal loss, serious carbon deposition, and insufficient active sites, nonmetal hollow carbon nanospherical materials (PACP-T) with hierarchical porous structures were synthesized by the copolymerization of aniline and pyrrole via a self-templating method. Local active sites were constructed by decorating the carbon material with heteroatomic groups. The synthetic process dispersed active sites at the atomic level, which was promoted by local structural forces. Experiments and DFT calculations showed that most active sites were pyridinic N+O–. The superior activity might have been caused by the synergistic adsorption and activation of reactants by highly electronegative heteroatoms and abundant π-containing functional groups (C═C, N═C═N, aromatic ring, and pyridinic N+O–) at active sites on the catalyst. This promoted rapid reactions and impeded carbon deposition, which promoted the continuous exposure of active sites. The significantly improved activity and stability of the optimized PACP-800 catalyst promote its potential industrial applications.
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