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论文类型：期刊论文

发表时间：2019-12-01

发表刊物：ACS CATALYSIS

收录刊物：SCIE

卷号：9

期号：12

页面范围：10931-10939

ISSN号：2155-5435

关键字：1,2-dichloroethane; surface N-doped porous carbon; electrocatalytic dechlorination; active sites; theoretical calculations

摘要：Nitrogen (N)-doped carbon materials are considered as the most promising alternative to replace noble-metal catalysts for electrocatalytic dechlorination of 1,2-dichloroethane (DCE), which is a promising reaction for industrial production and environmental protection. Unfortunately, the vague cognition of the catalytic active sites limits its further development. Herein, a series of surface N-doped porous carbon materials with adjustable N dopants were synthesized to identify the active sites for electrocatalytic dechlorination of DCE. The as-prepared catalyst showed fascinating DCE electrocatalytic dechlorination activity and ethylene selectivity at -2.75 V (vs SCE) with a current density of 17.94 mA cm(geometry)(-2) and ethylene Faradaic efficiency of 21%. The post hydrogen treatment and X-ray photoelectron spectroscopic analysis experimentally proved that the oxidized N acts as the active site for the dechlorination of DCE to CH2CH2, which was further theoretically confirmed by first-principles calculations. This work would open avenues for the development of N-doped carbon and the production of ethylene in an efficient and environmentally benign manner.