Identification of Catalytic Active Sites in Nitrogen-Doped Carbon for Electrocatalytic Dechlorination of 1,2-Dichloroethane,ACS Catalysis

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Identification of Catalytic Active Sites in Nitrogen-Doped Carbon for Electrocatalytic Dechlorination of 1,2-Dichloroethane
ACS Catalysis ( IF 11.3 ) Pub Date : 2019-11-04 , DOI: 10.1021/acscatal.9b02853
Guoqiang Gan ₁ , Xinyong Li _{1,

2} , Liang Wang ₁ , Shiying Fan ₁ , Ji Li ₁ , Feng Liang ₁ , Aicheng Chen ₂

Affiliation

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^–2_geometry 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.

中文翻译：

氮掺杂碳中1,2-二氯乙烷电催化脱氯的催化活性位点的确定

氮（N）掺杂的碳材料被认为是最有希望的替代物，以代替贵金属催化剂对1，2-二氯乙烷（DCE）进行电催化脱氯，这对于工业生产和环境保护是有希望的反应。不幸的是，对催化活性位点的模糊认识限制了它的进一步发展。本文中，合成了一系列具有可调N掺杂剂的表面N掺杂多孔碳材料，以识别DCE电催化脱氯的活性位点。所制备的催化剂在−2.75 V（vs SCE）下具有令人着迷的DCE电催化脱氯活性和乙烯选择性，电流密度为17.94 mA cm ^–2_几何乙烯法拉第效率为21％。氢气后处理和X射线光电子能谱分析实验证明，被氧化的N充当DCE脱氯成CH ₂ CH ₂的活性位点，这在理论上得到了第一性原理的证实。这项工作将为开发掺氮碳和以有效和环境友好的方式生产乙烯开辟道路。

更新日期：2019-11-04

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