期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 277, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2020.119057
关键词
Reductive dechlorination; Chloroacetic acids; Single atom catalyst; Dechlorination pathway; Catalytic mechanism
资金
- National Natural Science Foundation of China [21576238, 21106133]
- Natural Science Foundation of Zhejiang Province, China [LY16B060012]
- Hangzhou Science and Technology Development Foundation of China [20190101A02]
- Jiangsu Specially-Appointed Professor program
- Singapore Ministry of Education Academic Research Fund (AcRF) Tier 1 [RG10/16, RG111/15]
- Singapore Ministry of Education Academic Research Fund (AcRF) Tier 2 [MOE2016-T2-2-004]
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.
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