Methane (CH) photocatalytic upgrading to value-added chemicals, especially C products, is significant yet challenging due to sluggish energy/mass transfer and insufficient chemical driven-force in single photochemical process. Herein, we realize solar-driven CH oxidation to ethanol (CHOH) on crystalline carbon nitride (CCN) modified with CuS and Cu single atoms (CuS/Cu-CCN). The integration of photothermal effect and photocatalysis overcomes CH-to-CHOH conversion bottlenecks, with CuS as a hotspot to convert solar-energy to heat. In-situ characterizations demonstrate that Cu single atoms play as electron acceptor for O reduction to ·OOH/ · OH, while CuS acts as hole acceptor and site for CH adsorption, C - H activation, and C - C coupling. Theoretical calculations demonstrate that CuS/Cu-CCN reduces C - C coupling energy barrier by stabilizing ·CH and ·CHO. Impressively, CHOH productivity reaches 549.7 μmol g h, with selectivity of 94.8% and apparent quantum efficiency of 0.9% (420 nm). This work provides a sustainable avenue for CH conversion to value-added chemcials.
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| http://dx.doi.org/10.1038/s41467-024-54835-5 | DOI Listing |
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