Journal
CHEMICAL ENGINEERING JOURNAL
Volume 389, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2019.123450
Keywords
CO2 reduction; Flame synthesis; Hydrogenation; Pt/TiO2; Strong electronic metal-support interaction
Categories
Funding
- National Science Foundation [CBET 1705864]
- Department of Energy [DEFE0029161]
- NIH [R01CA208623]
- Optical Spectroscopy Core Facility [NIH 1S10RR031621]
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This work for the first time reports the promoting effect of strong electronic metal-support interaction (EMSI) in N/TiO2-V-O (V-O: oxygen vacancy) for gas-phase CO2 photoreduction. A novel in-situ surface hydrogenation was developed to prepare hydrogenated N/TiO2-V-O in a continuous, high throughput diffusion flame aerosol reactor. The combined results of various characterization techniques confirmed the presence of EMSI between N and defective TiO2-V-O resulted in the enhanced electronic density of N nanoparticles. Both the modulated electronic structure of N and surface oxygen vacancies simultaneously promoted the activation of surface adsorbed carbon intermediates and facilitated the separation of photogenerated charges, eventually boosting the photocatalytic activity of N/TiO2-V-O. The optimized N/TiO2-V-O demonstrated a high quantum yield of 1.49% with high CH4 selectivity (81%), which rendered 5.8- and 1.2-fold enhancements over its counterparts of TiO2-V-O and N/TiO2. More significantly, the EMSI also played a critical role in preserving the surface metallic Pt-0 and oxygen vacancies, and in sustaining high activity of the Pt/TiO2-V-O, whereas rapid catalytic deactivation are observed for both TiO2-V-O and Pt/TiO2.
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