The lower electricity consumption (EC) and higher value-added products are much desired yet still challenging for the development of CO2 coupling electrocatalytic systems. Herein, we give insight into the inherent nature of the retrenchment of EC by exploring the photo-assisted co-electrolysis of methanol and CO2 system using a kind of hydroxyl-rich covalent organic frameworks (Dha-COF-Co) with well-tuned pore structure and morphology. Specifically, the hydroxyl induced hydrogen bond interaction in Dha-COF-Co enables to simultaneously regulate the pore microenvironment and nanoribbon morphology of COFs for performance boosting. Notably, the obtained Dha-COF-Co nanoribbon exhibits an overall EC retrenchment of ~41.2% (highest in porous crystalline materials to date) when replacing the anodic OER with MOR in the photo-electrocatalytic MOR-CO2RR coupling system, as well as superior FEHCOOH (anode, ~100%) and FECO (cathode, >95%) at 1.8 V. Combined theoretical calculations with various characterizations, the vital role of hydroxyl group in both microenvironment and morphology tuning that can facilitate the CO2RR and MOR kinetics to retrench the EC has been intensively discussed.
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Nano Research Energy
Published: 09 December 2024
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