Highly efficient and stable photocatalytic CO2 and H2O reduction into methanol at lower temperatures through an elaborate gas–liquid–solid interfacial system
It is extraordinarily exigent to solve the efficiency of 6H+/6e− photoreduction of CO2 and H2O into methanol as the major product, which is limited by the severe photogenerated carrier recombination, the reoxidation of methanol at high temperature, and photocorrosion of catalysts. Herein, we developed an elaborate gas–liquid–solid system assembled by using a novel multicomponent SrTiO3 (La Cr)/Cu@Ni/SiO2/TiN (STO/Cu@Ni/SiO2/TiN) heterojunction, realizing a highly efficient and robust photocatalytic CO2 reduction to methanol at low temperature. STO/Cu@Ni/SiO2/TiN exhibits excellent light absorption and high charge carriers separation nature, and the evolution of methanol is 25.8 μmol (h gcat.)−1 roughly not only 173 folds higher than those observed compared with the STO counterpart, but also is 50 times that those of traditional gas–solid two-phase system. Of note, these improved performances are attributed to the enhancement of the local surface plasmonic resonance of Cu@Ni nanoparticles by changing the local medium dielectric constant and prolonged carrier's lifetime originating from heterostructure. Moreover, plasmonic TiN nanoparticles play an important role in remaining the triphase interfacial system temperature at 90 °C and increasing methanol production excellently. While, the ionic liquid in the gas–liquid–solid system can activate CO2 molecules, thereby greatly improves the yield of methanol. In situ Fourier transform infrared (FTIR) spectra and 13C isotope labeling tests reveal the reaction path of CO2 on the photocatalyst surface. This work may provide a new direction for the efficient photoreduction of CO2 to methanol.
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