Mimicking reductive dehalogenases for efficient electrocatalytic water dechlorination

Yuan Min, Shu-Chuan Mei, Xiao-Qiang Pan, Jie-Jie Chen (), Han-Qing Yu () and Yujie Xiong ()
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Yuan Min: University of Science and Technology of China
Shu-Chuan Mei: University of Science and Technology of China
Xiao-Qiang Pan: University of Science and Technology of China
Jie-Jie Chen: University of Science and Technology of China
Han-Qing Yu: University of Science and Technology of China
Yujie Xiong: University of Science and Technology of China

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Electrochemical technology is a robust approach to removing toxic and persistent chlorinated organic pollutants from water; however, it remains a challenge to design electrocatalysts with high activity and selectivity as elaborately as natural reductive dehalogenases. Here we report the design of high-performance electrocatalysts toward water dechlorination by mimicking the binding pocket configuration and catalytic center of reductive dehalogenases. Specifically, our designed electrocatalyst is an assembled heterostructure by sandwiching a molecular catalyst into the interlayers of two-dimensional graphene oxide. The electrocatalyst exhibits excellent dechlorination performance, which enhances reduction of intermediate dichloroacetic acid by 7.8 folds against that without sandwich configuration and can selectively generate monochloro-groups from trichloro-groups. Molecular simulations suggest that the sandwiched inner space plays an essential role in tuning solvation shell, altering protonation state and facilitating carbon−chlorine bond cleavage. This work demonstrates the concept of mimicking natural reductive dehalogenases toward the sustainable treatment of organohalogen-contaminated water and wastewater.

Date: 2023
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DOI: 10.1038/s41467-023-40906-6

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