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Under the support of the National Natural Science Foundation of China (Grant Nos.
21773146, 22003036, 22102092), Professor Cao Rui's team from Shaanxi Normal University cooperated with overseas scholars to use intramolecular crown ether groups to build water clusters around the cobalt corrole catalytic center The hydrogen bond network assists proton transfer and significantly promotes the electrocatalytic hydrogen evolution reaction
For many important chemical reactions, such as water desorption, hydrogen evolution, oxygen evolution, oxygen reduction, carbon dioxide reduction and nitrogen reduction, the proton transfer efficiency plays a decisive role in the overall reaction efficiency
.
In biological systems, metalloprotein catalytic active centers often utilize water cluster hydrogen bond networks to achieve efficient and directed proton transfer, such as in hydrogenases, photosystem II oxygen-releasing centers, and cytochrome c oxidase catalytic centers (Figure a).
Based on the fact that cobalt-corrole complexes can effectively catalyze the hydrogen evolution reaction, the researchers designed and synthesized crown ether-modified cobalt-corrole complexes as a model for electrocatalytic hydrogen evolution by taking advantage of the meso position of corrole ligands to facilitate modification of various substituents.
(Fig.
b)
.
Through X-ray single crystal diffraction, 1H NMR and DOSY NMR spectroscopy and infrared spectroscopy, it was proved that the modification of the crown ether group on the catalyst molecular structure can effectively construct the intramolecular water cluster hydrogen bond network through the hydrogen bond interaction with the water molecule.
The findings have important scientific implications for artificially regulating many other catalytic small molecule activation reactions involving proton transfer
