An in-depth understanding of fast interfacial electron transfer in amide-bonded photocatalyst for boosting photoreduction of CO2

The photocatalytic reduction of CO2 is typically slow due to inert charge kinetics and low CO2 affinity. This research aimed to enhance the photocarrier transfer/separation and CO2 adsorption/activation process over amine-functionalized TiO2 nanoparticles/GO (f-TGO). Density functional theory (DFT) calculations established models of TGO and f-TGO (with CO2 adsorbed on the top, middle, and bottom), proving that the presence of the amino group fortifies the adsorption/activation of CO2, while the amido bond acts as a charge delivery channel to accelerate electron transfer in f-TGO. The optimized f-TGO demonstrated good performance in photocatalytic CO2RR under mild conditions, achieving a turnover frequency (TOF) of 40.9 and 19.9 & mu;mol g - 1h- 1for CO and CH4, respectively, outperforming most reported TiO2-based catalysts. In addition, in situ DRIFTS and theoretical calculation revealed the reaction intermediates, demonstrated the kinetic behaviors of the reaction pathway, and thus laid the groundwork for investigating the CO2RR mechanism. This study proposes a viable approach to modify the electronic structure of photocatalysts and provides new insight for designing high-performance photocatalysts, focusing particularly on how interfacial carrier transfer affects photoreduction CO2.

Automated summary

This research aimed to enhance the photocarrier transfer/separation and CO2 adsorption/activation process over amine-functionalized TiO2 nanoparticles/GO (f-TGO). The optimized f-TGO demonstrated good performance in photocatalytic CO2RR under mild conditions, achieving a turnover frequency (TOF) of 40.9 and 19.9 μmol g-1h-1 for CO and CH4, respectively, outperforming most reported TiO2-based catalysts. This study proposes a viable approach to modify the electronic structure of photocatalysts and provides new insight for designing high-performance photocatalysts, focusing particularly on how interfacial carrier transfer affects photoreduction CO2.