A mechanistic study of molecular CO2 interaction and adsorption on carbon implanted SnS2 thin film for photocatalytic CO2 reduction activity

Citation:
Billo, T, Shown I, kumar Anbalagan A, Effendi TA, Sabbah A, Fu F-Y, Chu C-M, Woon W-Y, Chen R-S, Lee C-H, Chen K-H, Chen L-C.  2020.  A mechanistic study of molecular CO2 interaction and adsorption on carbon implanted SnS2 thin film for photocatalytic CO2 reduction activity, 2020. 72:104717.

Abstract:

Gas-phase photocatalytic reactions to convert carbon dioxide and water into oxygen and hydrocarbons are the foundation of life on earth. However, the efficiency of photosynthesis is relatively low (~1%), which leaves much room for artificial photosynthesis to reach the benchmark of the solar cells (>15%). In this work, carbon implanted SnS2 thin films (C–SnS2) were prepared to study photocatalytic activity and adsorbate-catalyst surface interactions during CO2 photoreduction. The electron density distribution in C–SnS2 and its contribution toward the photogenerated charge transfer process has been analyzed by the angle-dependent X-ray absorption near-edge structure (XANES) study. The C–SnS2 surface affinity toward the CO2 molecule was monitored by in-situ dark current and Raman spectroscopy measurements. By optimizing the dose during ion implantation, SnS2 thin film with 1 wt% carbon incorporation shows 108 times enhancement in the CO2 conversion efficiency and more than 89% product selectivity toward CH4 formation compared with the as-grown SnS2 without carbon incorporation. The improved photocatalytic activity can be ascribed to enhanced light harvesting, pronounced charge-transfer between SnS2 and carbon with improved carrier separation and the availability of highly active carbon sites that serve as favorable CO2 adsorption sites.

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