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Highly efficient continuous gas-phase dehydrogenation of formic acid by Ni induces β-Mo2C to α-MoC structural transformation
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DOI：10.1016/j.gerr.2026.100173.png)
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Abstract
En 中文
Formic acid (FA) is a promising hydrogen storage carrier for high power density hydrogen fuel cells. However, dehydrogenation of FA usually produces CO by-products that poison the catalyst. The prevention of FA decomposition into CO within high-temperature proton exchange membrane (HT-PEM) systems operating at 130-200 degrees C remains a formidable scientific challenge. Here, we propose a Ni doping-induced active phase transition of molybdenum carbide on carbon-based catalysts, enhancing hydrogen production from FA. Ni-MoC/ NC achieves complete FA conversion at 190 degrees C, maintaining stable catalytic performance over 170 h. In MoC/NC, Mo primarily exists as R-Mo2C and gamma-Mo2N, while in Ni-MoC/NC, it predominantly forms alpha-MoC and gamma-Mo2N. XRD and XPS analyses reveal that Ni doping induces the transformation of R-Mo2C into alpha-MoC, improving catalytic performance. Mechanistic studies identify HCOO* as a key intermediate in FA dehydrogenation on Ni-MoC/NC. The catalyst promotes the dissociation of HCOOH* into HCOO*, reduces the energy barrier for HCOO* conversion to CO2*, and inhibits CO by-product formation, accelerating FA dehydrogenation. These findings highlight Ni-MoC/NC as a robust catalyst for efficient hydrogen production.
Keywords:
Carbon-based catalyst
Active phase
FA
Dehydrogenation
Hydrogen storage
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