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Pyrrolic Nitrogen Boosted H 2 Generation from an Aqueous Solution of HCHO at Room Temperature by Metal-Free Carbon Catalysts.

Yu SunYiting XiaoLei RenZiheng ChengYaning NiuZhichu LiSai Zhang
Published in: The journal of physical chemistry letters (2024)
Hydrogen production from organic hydrides represents a promising strategy for the development of safe and sustainable technologies for H 2 storage and transportation. Nonetheless, the majority of existing procedures rely on noble metal catalysts and emit greenhouse gases such as CO 2 /CO. Herein, we demonstrated an alternative N-doped carbon (CN) catalyst for highly efficient and robust H 2 production from an aqueous solution of formaldehyde (HCHO). Importantly, this process generated formic acid as a valuable byproduct instead of CO 2 /CO, enabling a clean H 2 generation process with 100% atom economy. Mechanism investigations revealed that the pyrrolic N in the CN catalysts played a critical role in promoting H 2 generation via enhancing the transformation of O 2 to generate • OO - free radicals. Consequently, the optimized CN catalysts achieved a remarkable H 2 generation rate of 13.6 mmol g -1 h -1 at 30 °C. This finding is anticipated to facilitate the development of liquid H 2 storage and its large-scale utilization.
Keyphrases
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