ArticleJournal of the American Chemical Society2026
Highly Selective Methane Photooxidation to Formaldehyde by Constructing Symmetry-Breaking Sites.
Article in Journal of the American Chemical Society, 2026. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.
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7 authors.
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Abstract
Solar-driven direct conversion of methane (CH4) and water to formaldehyde (HCHO) offers a sustainable route for hydrocarbon production under mild conditions. However, thermodynamic parallels between HCHO and methanol (CH3OH) formation limit product selectivity. Using titanium dioxide (TiO2), we have engineered symmetry-breaking sites to overcome this constraint. The studies reveal that symmetry-breaking sites generate surface hole-trapping states, enabling rapid hole migration (∼8 ps). This process combines with adsorbed hydroxyl groups to produce hydroxyl radicals (•OH), which cleave titanium-oxygen (Ti-O) bonds in methoxy intermediates. The resulting methoxy radicals (•OCH3) drive a single-step pathway that entirely bypasses CH3OH formation, achieving 93.7% HCHO selectivity with HCHO accounting for 100% of liquid products. In sharp contrast, symmetric sites follow a two-step pathway involving substantial CH3OH coproduction via slower electron transfer (>4 ns), yielding only ∼42.8% HCHO selectivity. This work demonstrates a breakthrough in sustainable HCHO production, with symmetry-breaking site engineering commandeering photoinduced charge dynamics to eliminate selectivity barriers.
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