Site-defined Cu-O ensembles enable hydrogen-conserving light-driven ethane upgrading.
basic_science · Level V
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- Record sourced from PubMed, PMID 41803124.
- Also identified by DOI 10.1038/s41467-026-70416-0.
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Abstract
Upgrading light alkanes to value-added olefins is a long-standing challenge, owing to the high stability of C-H bonds and the tendency for overoxidation at elevated temperatures. Here, we introduce a light-driven strategy for ethane dehydrogenation using Cu-doped TiO<sub>2</sub>, in which atomically dispersed Cu coordinated to bridging oxygen (O<sub>br-Cu</sub>) creates well-defined [Cu-O] ensembles that orchestrate site-specific, stepwise C-H activation. Photogenerated holes localize at O<sub>br-Cu</sub> sites to initiate the first C-H cleavage, while adjacent Cu centers mediate β-H elimination and H<sub>2</sub> evolution. In contrast, minor β-H activation at O<sub>br-Ti</sub> sites generates *H species that cannot desorb due to a prohibitive coupling barrier with *H on O<sub>br-Cu</sub>, leading to Cu reduction and progressive deactivation. Co-feeding CO<sub>2</sub> restores the active Cu coordination environment and suppresses this deactivation process without perturbing the primary reaction pathway. This cooperative design achieves a C<sub>2</sub>H<sub>4</sub> production rate of 21.1 mmol g<sup>-1</sup> h<sup>-1</sup> with nearly stoichiometric H<sub>2</sub> evolution and an apparent quantum efficiency of 6.1% under 365 nm irradiation. These findings establish a site-defined, hydrogen-conserving route for photocatalytic alkane upgrading, offering a general blueprint for selective C-H bond transformations with long-term stability.