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Superexchange-induced Pt-O-Ti <sup>3+</sup> site on single photocatalyst for efficient H <sub>2</sub> production with organics degradation in wastewater

Tao Zhang, Zhiyong Zhao, Dongpeng Zhang, Xingyu Liu, Pengfei Wang, Yi Li, Sihui Zhan

2023Proceedings of the National Academy of Sciences45 citationsDOIOpen Access PDF

Abstract

Efficient photocatalytic H 2 production from wastewater instead of pure water is a dual solution to the environmental and energy crisis, but due to the rapid recombination of photoinduced charge in the photocatalyst and inevitable electron depletion caused by organic pollutants, a significant challenge of dual-functional photocatalysis (simultaneous oxidative and reductive reactions) in single catalyst is designing spatial separation path for photogenerated charges at atomic level. Here, we designed a Pt-doped BaTiO 3 single catalyst with oxygen vacancies (BTPO v ) that features Pt-O-Ti 3+ short charge separation site, which enables excellent H 2 production performance (1519 μmol·g −1 ·h −1 ) while oxidizing moxifloxacin ( k = 0.048 min −1 ), almost 43 and 98 times than that of pristine BaTiO 3 (35 μmol·g −1 ·h −1 and k = 0.00049 min −1 ). The efficient charge separation path is demonstrated that the oxygen vacancies extract photoinduced charge from photocatalyst to catalytic surface, and the adjacent Ti 3+ defects allow rapid migration of electrons to Pt atoms through the superexchange effect for H * adsorption and reduction, while the holes will be confined in Ti 3+ defects for oxidation of moxifloxacin. Impressively, the BTPO v shows an exceptional atomic economy and potential for practical applications, a best H 2 production TOF (370.4 h −1 ) among the recent reported dual-functional photocatalysts and exhibiting excellent H 2 production activity in multiple types of wastewaters.

Topics & Concepts

PhotocatalysisCatalysisOxidizing agentWater splittingHydrogen productionPhotochemistryChemistryOxygenMaterials sciencePoint of zero chargeAdsorptionInorganic chemistryPhysical chemistryOrganic chemistryAdvanced Photocatalysis TechniquesCovalent Organic Framework ApplicationsPerovskite Materials and Applications