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

Abstract

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.

Active Sites in Single-Atom Fe–Nx–C Nanosheets for Selective Electrochemical Dechlorination of 1,2-Dichloroethane to Ethylene

“…Furthermore, with the in situ addition of SCN – during the ongoing process, the current density and C 2 H 4 production rate decline to the same level as those of the Fe–N x –Cns–800 poisoned by SCN – . It is worth noting that the catalyst cannot be completely poisoned by SCN – , and the remaining activity may be contributed by N-doped graphene as reported in our previous work . The two tests indicate that the Fe–N x site in the Fe–N x –Cns is supposed to be the dominating catalytic sites for the DCEDR.…”

“…The electrochemical dechlorination of 1,2-dichloroethane (DCE) has been proved to be a promising and economic strategy for production of high-value ethylene and vinyl chloride. − However, the DCE dechlorination reaction (DCEDR) is generally challenged in practice because of the harsh dechlorination conditions, unclear reaction mechanism, and poor selectivity. , We have concentrated on the exploitation of advanced materials for DCEDR to produce ethylene for a long while. We have found that nitrogen-doped carbon showed excellent dechlorination performance and the oxidized N acted as a catalytic site for electrochemical production of ethylene . Nevertheless, advanced electrocatalysts with high performance are still urgently needed.…”

Functionalized Activated Carbon for Competing Adsorption of Volatile Organic Compounds and Water

“…Figure e shows a typical type-IV curve with an H1-type hysteresis loop, which suggests dominant development of large mesopores. The steep increase for N 2 absorbed at low relative pressure ( P / P 0 < 0.1) implies the existence of micropores. − The specific surface areas of OAC and SACs are 2254, 1748, 1343, and 1257 m 2 g –1 (Table S2). Also, the pore size tends to decrease with the increase of the modifier dosage due to the blocking of the pores by a hydrophobic layer (Figure f).…”

Advances in photocatalytic and electrocatalytic removal of chlorinated volatile organic compounds

“…. 在此基础上, 研究者对 金属单质电催化剂进行了一系列研究 [91,94,95] , 均发现其 有一些报道, 取得了一系列的研究成果 [69,71,100,101] . 其 中, Mitch课题组 [69,71] 3基于Cl-VOCs物质的分子结构去预测其反应的电子转…”

“…氮掺杂碳材料电催化1,2-二氯乙烷脱氯反应的理论计算结果. 1,2-二氯乙烷脱氯反应的能垒图: (a) 乙烯; (b) 氯乙烯; (c) 表面N掺杂碳材料 的分波态密度(PDOS)图; (d) 1,2-二氯乙烷在活性中心氧化N位点催化脱氯反应过程示意图[101] …”