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Solar-Driven Syngas Generation From Formic Acid Via K+ Intercalated Carbon Nitride
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DOI：10.1002/cctc.70896.png)
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Abstract
En 中文
Solar-driven dehydrogenation of formic acid (FA), a liquid phase organic hydrogen repository, is a promising paradigm for sustainable green H2 generation. Herein, we demonstrated photo-reforming of FA to produce CO along with H2 production using potassium intercalated (K+) carbon nitride (KPCN) as an organic semiconductor. Among the prepared photocatalysts, Pt/0.5KPCN exhibited the highest photocatalytic activity, achieving H2 and CO production rates of 323 and 242 µmol.h−1.g−1, respectively, with a H2/CO ratio of 1:3. The overall AQY for syngas (AQYH2 + AQYCO) production was estimated as 1.34% at λ = 400 nm. Moreover, CO2-TPD analysis unveiled increased basicity upon K+ intercalation in Pt/0.5KPCN, facilitating a stronger structural activity relationship with the acidic FA and steering the formation of CO and H2. 13C isotopic labeling experiment using 13C-labeled FA confirms that CO originates exclusively from the photo reforming of FA. Further, EPR and DFT studies confirm the formation of CO2•− radical and reveal the mechanistic insights into syngas formation, elucidating the reaction pathway. This work presents a more viable and sustainable strategy to expedite FA as a dual source of H2 and CO production, an important precursor for Fischer–Tropsch synthesis (FTS).
Keywords:
formic acid
K+ intercalated carbon nitride
photocatalysis
syngas
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