Study of Non-Noble-Metal-Based Metal-Nitrogen-Carbon Catalysts for Formic Acid Dehydrogenation

Formic acid (FA) is a safe, renewable, and promising hydrogen carrier. Acritical challenge is the effective screening of the suitable non-noble-metal-based catalysts forFA dehydrogenation to substitute expensive noble-metal-based ones. Here, a study of allpossible catalysts with M-N-C structures (M = 12 metals,-N-C = nitrogen-dopedgraphene-like surface) for FA dehydrogenation has been conducted using density functionaltheory (DFT) and followed by experimental analysis. Based on the adsorption energy ofcritical intermediates, preliminary screening suggests Co as a possible active metal for M-N-C. Experiment and further DFT calculations suggest that atomically dispersed Co sites (Co-N1-C3,Co-N2-C2,andCo-N3-C) are preferable for FA dehydrogenation. Theappropriate N contents are critical to the catalytic activity, whose amount can be tuned bychoosing different sacrifice templates and the pyrolysis temperature.

Automated summary

This study investigates the application of all possible M-N-C catalysts in formic acid dehydrogenation using density functional theory and experimental analysis. The results suggest that atomically dispersed Co sites exhibit good catalytic activity for formic acid dehydrogenation, and the appropriate nitrogen content plays a critical role in catalytic activity.