Single-Ni-atom catalyzes aqueous phase electrochemical reductive dechlorination reaction

Yinghua Xu; Zeqing Yao; Zhechuan Mao; Meiqin Shi; Xiaoyong Zhang; Feng Cheng; Hong Bin Yang; Hua bing Tao; Bin Liu

doi:10.1016/j.apcatb.2020.119057

Single-Ni-atom catalyzes aqueous phase electrochemical reductive dechlorination reaction

Yinghua Xu^*
, Zeqing Yao
, Zhechuan Mao
, Meiqin Shi
, Xiaoyong Zhang
, Feng Cheng
, Hong Bin Yang^*
, Hua bing Tao
, Bin Liu^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

82 Citations (Scopus)

Abstract

Electrochemical dechlorination offers a promising strategy to convert refractory chlorinated organic pollutants (COPs) to biodegradable chlorine-free organics under mild conditions. In this work, we report atomically dispersed nickel anchored on nitrogenated graphene (A-Ni-NG) as an efficient dechlorination catalyst, and study its underlying dechlorination pathway and catalytic mechanism, using chloroacetic acids (CAAs) as the model COPs. The A-Ni-NG exhibits higher catalytic activity than state-of-the-art Pd and Ag catalysts. Using A-Ni-NG as a catalyst, complete dechlorination of CAAs to acetic acid can be achieved at pH 3, 7 and 11. The Cl atoms in CAAs are eliminated sequentially through a direct dechlorination mechanism. The exceptional electrocatalytic activity of A-Ni-NG stems from the specific interactions between A-Ni-NG and the substrate as well as the primary intermediate generated from the first electron transfer (ET) step, and the ET step occurs in a stepwise manner with breaking C–Cl bond. © 2020 Elsevier B.V.

Original language	English
Article number	119057
Journal	Applied Catalysis B: Environmental
Volume	277
Online published	4 May 2020
DOIs	https://doi.org/10.1016/j.apcatb.2020.119057
Publication status	Published - 15 Nov 2020
Externally published	Yes

Funding

This research was supported by the National Natural Science Foundation of China (21576238, 21106133), the Natural Science Foundation of Zhejiang Province, China (LY16B060012), Hangzhou Science and Technology Development Foundation of China (20190101A02), the financial support from Jiangsu Specially-Appointed Professor program, and Singapore Ministry of Education Academic Research Fund (AcRF) Tier 1: RG10/16 and RG111/15, and Tier 2: MOE2016-T2-2-004.

Research Keywords

Catalytic mechanism
Chloroacetic acids
Dechlorination pathway
Reductive dechlorination
Single atom catalyst

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title = "Single-Ni-atom catalyzes aqueous phase electrochemical reductive dechlorination reaction",

abstract = "Electrochemical dechlorination offers a promising strategy to convert refractory chlorinated organic pollutants (COPs) to biodegradable chlorine-free organics under mild conditions. In this work, we report atomically dispersed nickel anchored on nitrogenated graphene (A-Ni-NG) as an efficient dechlorination catalyst, and study its underlying dechlorination pathway and catalytic mechanism, using chloroacetic acids (CAAs) as the model COPs. The A-Ni-NG exhibits higher catalytic activity than state-of-the-art Pd and Ag catalysts. Using A-Ni-NG as a catalyst, complete dechlorination of CAAs to acetic acid can be achieved at pH 3, 7 and 11. The Cl atoms in CAAs are eliminated sequentially through a direct dechlorination mechanism. The exceptional electrocatalytic activity of A-Ni-NG stems from the specific interactions between A-Ni-NG and the substrate as well as the primary intermediate generated from the first electron transfer (ET) step, and the ET step occurs in a stepwise manner with breaking C–Cl bond. {\textcopyright} 2020 Elsevier B.V.",

keywords = "Catalytic mechanism, Chloroacetic acids, Dechlorination pathway, Reductive dechlorination, Single atom catalyst",

author = "Yinghua Xu and Zeqing Yao and Zhechuan Mao and Meiqin Shi and Xiaoyong Zhang and Feng Cheng and Yang, \{Hong Bin\} and Tao, \{Hua bing\} and Bin Liu",

year = "2020",

month = nov,

day = "15",

doi = "10.1016/j.apcatb.2020.119057",

language = "English",

volume = "277",

journal = "Applied Catalysis B: Environmental",

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TY - JOUR

T1 - Single-Ni-atom catalyzes aqueous phase electrochemical reductive dechlorination reaction

AU - Xu, Yinghua

AU - Yao, Zeqing

AU - Mao, Zhechuan

AU - Shi, Meiqin

AU - Zhang, Xiaoyong

AU - Cheng, Feng

AU - Yang, Hong Bin

AU - Tao, Hua bing

AU - Liu, Bin

PY - 2020/11/15

Y1 - 2020/11/15

N2 - Electrochemical dechlorination offers a promising strategy to convert refractory chlorinated organic pollutants (COPs) to biodegradable chlorine-free organics under mild conditions. In this work, we report atomically dispersed nickel anchored on nitrogenated graphene (A-Ni-NG) as an efficient dechlorination catalyst, and study its underlying dechlorination pathway and catalytic mechanism, using chloroacetic acids (CAAs) as the model COPs. The A-Ni-NG exhibits higher catalytic activity than state-of-the-art Pd and Ag catalysts. Using A-Ni-NG as a catalyst, complete dechlorination of CAAs to acetic acid can be achieved at pH 3, 7 and 11. The Cl atoms in CAAs are eliminated sequentially through a direct dechlorination mechanism. The exceptional electrocatalytic activity of A-Ni-NG stems from the specific interactions between A-Ni-NG and the substrate as well as the primary intermediate generated from the first electron transfer (ET) step, and the ET step occurs in a stepwise manner with breaking C–Cl bond. © 2020 Elsevier B.V.

AB - Electrochemical dechlorination offers a promising strategy to convert refractory chlorinated organic pollutants (COPs) to biodegradable chlorine-free organics under mild conditions. In this work, we report atomically dispersed nickel anchored on nitrogenated graphene (A-Ni-NG) as an efficient dechlorination catalyst, and study its underlying dechlorination pathway and catalytic mechanism, using chloroacetic acids (CAAs) as the model COPs. The A-Ni-NG exhibits higher catalytic activity than state-of-the-art Pd and Ag catalysts. Using A-Ni-NG as a catalyst, complete dechlorination of CAAs to acetic acid can be achieved at pH 3, 7 and 11. The Cl atoms in CAAs are eliminated sequentially through a direct dechlorination mechanism. The exceptional electrocatalytic activity of A-Ni-NG stems from the specific interactions between A-Ni-NG and the substrate as well as the primary intermediate generated from the first electron transfer (ET) step, and the ET step occurs in a stepwise manner with breaking C–Cl bond. © 2020 Elsevier B.V.

KW - Catalytic mechanism

KW - Chloroacetic acids

KW - Dechlorination pathway

KW - Reductive dechlorination

KW - Single atom catalyst

UR - https://www.scopus.com/pages/publications/85086160765

UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-85086160765&origin=recordpage

U2 - 10.1016/j.apcatb.2020.119057

DO - 10.1016/j.apcatb.2020.119057

M3 - RGC 21 - Publication in refereed journal

SN - 0926-3373

VL - 277

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

M1 - 119057

ER -

Single-Ni-atom catalyzes aqueous phase electrochemical reductive dechlorination reaction

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