Perovskite photoelectrocatalysis enables solar-driven conversion of CO_(2)to value-added chemicals,but instability in water and insufficient C–C coupling still constrain performance.Herein,we present a synergistic ap...Perovskite photoelectrocatalysis enables solar-driven conversion of CO_(2)to value-added chemicals,but instability in water and insufficient C–C coupling still constrain performance.Herein,we present a synergistic approach for aqueous-phase CO_(2)conversion that combines perovskite-based photoelectrocatalysis with localized surface plasmon resonance(LSPR)enhancement.To address the inherent instability of lead-halide perovskites,we developed a modified hot-injection route that enables the in situ formation of water-stable CsPbBr_(3)@TiO_(2)core–shell nanoparticles.Titanium butoxide and water were introduced after Cs-oleate injection,enabling controlled TiO_(2)shell growth without post-treatment.Electron microscopy,XRD,and XPS confirm the core–shell architecture,while optical/electrical probes indicate efficient charge separation across the CsPbBr_(3)/TiO_(2)junction.Subsequently,we investigated electrocatalytic,photocatalytic,and photoelectrochemical carbon dioxide reduction(CO_(2)RR)on CsPbBr_(3)@TiO_(2)/Au and CsPbBr_(3)@TiO_(2).Gas chromatography revealed tunable product selectivity,yielding H_(2),CO,CH_(4),and multicarbon(C_(2),C_(3))products including C_(2)H_(4)(ethylene)and C_(3)H_(6)(propene).Our main findings indicate that the CsPbBr_(3)@TiO_(2)/Au exhibits high selectivity toward C_(3)(propene)in photocatalysis and C_(2)(ethylene)in photoelectrochemistry,reaching up to 70%and 58%,respectively.These results highlight perovskite heterostructures as a viable platform for efficient CO_(2)utilization and the sustainable production of value-added C_(2)/C_(3)chemicals.展开更多
基金financially supported by the National Natural Science Foundation of China(Project No.62350610272)the Department of Science and Technology of Shandong Province(Grant KY0020240040)+1 种基金the Priority 2030 Federal Academic Leadership Programthe support from the Ministry of Science and Higher Education of the Russian Federation(Project No.FSRZ 2023-0006)。
文摘Perovskite photoelectrocatalysis enables solar-driven conversion of CO_(2)to value-added chemicals,but instability in water and insufficient C–C coupling still constrain performance.Herein,we present a synergistic approach for aqueous-phase CO_(2)conversion that combines perovskite-based photoelectrocatalysis with localized surface plasmon resonance(LSPR)enhancement.To address the inherent instability of lead-halide perovskites,we developed a modified hot-injection route that enables the in situ formation of water-stable CsPbBr_(3)@TiO_(2)core–shell nanoparticles.Titanium butoxide and water were introduced after Cs-oleate injection,enabling controlled TiO_(2)shell growth without post-treatment.Electron microscopy,XRD,and XPS confirm the core–shell architecture,while optical/electrical probes indicate efficient charge separation across the CsPbBr_(3)/TiO_(2)junction.Subsequently,we investigated electrocatalytic,photocatalytic,and photoelectrochemical carbon dioxide reduction(CO_(2)RR)on CsPbBr_(3)@TiO_(2)/Au and CsPbBr_(3)@TiO_(2).Gas chromatography revealed tunable product selectivity,yielding H_(2),CO,CH_(4),and multicarbon(C_(2),C_(3))products including C_(2)H_(4)(ethylene)and C_(3)H_(6)(propene).Our main findings indicate that the CsPbBr_(3)@TiO_(2)/Au exhibits high selectivity toward C_(3)(propene)in photocatalysis and C_(2)(ethylene)in photoelectrochemistry,reaching up to 70%and 58%,respectively.These results highlight perovskite heterostructures as a viable platform for efficient CO_(2)utilization and the sustainable production of value-added C_(2)/C_(3)chemicals.
