Publications

Introducing Water-Network-Assisted Proton Transfer for Boosted Electrocatalytic Hydrogen Evolution with Cobalt Corrole

Li, X. and Lv, B. and Zhang, X.-P. and Jin, X. and Guo, K. and Zhou, D. and Bian, H. and Zhang, W. and Apfel, U.-P. and Cao, R.

ANGEWANDTE CHEMIE - INTERNATIONAL EDITION
Volume: 61 Pages:
DOI: 10.1002/anie.202114310
Published: 2022

Abstract
Proton transfer is vital for many biological and chemical reactions. Hydrogen-bonded water-containing networks are often found in enzymes to assist proton transfer, but similar strategy has been rarely presented by synthetic catalysts. We herein report the Co corrole 1 with an appended crown ether unit and its boosted activity for the hydrogen evolution reaction (HER). Crystallographic and 1H NMR studies proved that the crown ether of 1 can grab water via hydrogen bonds. By using protic acids as proton sources, the HER activity of 1 was largely boosted with added water, while the activity of crown-ether-free analogues showed very small enhancement. Inhibition studies by adding 1) external 18-crown-6-ether to extract water molecules and 2) potassium ion or N-benzyl-n-butylamine to block the crown ether of 1 further confirmed its critical role in assisting proton transfer via grabbed water molecules. This work presents a synthetic example to boost HER through water-containing networks. © 2021 Wiley-VCH GmbH

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