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Atomically dispersed low-valent Au boosts photocatalytic hydroxyl radical production.

Zhenyuan TengHongbin YangQi-Tao ZhangWenan CaiYing-Rui LuKosaku KatoZhenzong ZhangJie DingHan SunSixiao LiuChengyin WangPeng ChenAkira YamakataTing-Shan ChanChenliang SuTeruhisa OhnoBin Liu
Published in: Nature chemistry (2024)
Providing affordable, safe drinking water and universal sanitation poses a grand societal challenge. Here we developed atomically dispersed Au on potassium-incorporated polymeric carbon nitride material that could simultaneously boost photocatalytic generation of ·OH and H 2 O 2 with an apparent quantum efficiency over 85% at 420 nm. Potassium introduction into the poly(heptazine imide) matrix formed strong K-N bonds and rendered Au with an oxidation number close to 0. Extensive experimental characterization and computational simulations revealed that the low-valent Au altered the materials' band structure to trap highly localized holes produced under photoexcitation. These highly localized holes could boost the 1e - water oxidation reaction to form highly oxidative ·OH and simultaneously dissociate the hydrogen atom in H 2 O, which greatly promoted the reduction of oxygen to H 2 O 2 . The photogenerated ·OH led to an efficiency enhancement for visible-light-response superhydrophilicity. Furthermore, photo-illumination in an onsite fixed-bed reactor could disinfect water at a rate of 66 L H 2 O m -2 per day.
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