Engineering the Charge Density on an In2.77S4/Porous Organic Polymer Hybrid Photocatalyst for CO2-to-Ethylene Conversion Reaction

Das, R and Paul, R and Parui, A and Shrotri, A and Atzori, C and Lomachenko, KA and Singh, AK and Mondal, J and Peter, SC (2022) Engineering the Charge Density on an In2.77S4/Porous Organic Polymer Hybrid Photocatalyst for CO2-to-Ethylene Conversion Reaction. In: Journal of the American Chemical Society .

PDF jou_ame_che_2022.pdf - Published Version Restricted to Registered users only Download (8MB) | Request a copy

Abstract

The development of an efficient photocatalyst for C2 product formation from CO2 is of urgent importance toward the deployment of solar-fuel production. Here, we report a template-free, cost-effective synthetic strategy to develop a carbazole-derived porous organic polymer (POP)-based composite catalyst. The composite catalyst is comprised of In2.77S4 and porous organic polymer (POP) and is held together by induced-polarity-driven electrostatic interaction. Utilizing the synergy of the catalytically active In centers and light-harvesting POPs, the catalyst showed 98.9 selectivity toward the generation of C2H4, with a formation rate of 67.65 μmol g-1 h-1. Two different oxidation states of the In2.77S4 spinel were exploited for the C-C coupling process, and this was investigated by X-ray photoelectron spectroscopy (XPS), X-ray absorption spectroscopy (XAS), and density functional theory (DFT) calculations. The role of POP was elucidated via several photophysical and photoelectrochemical studies. The electron transfer was mapped by several correlated approaches, which assisted in establishing the Z-scheme mechanism. Furthermore, the mechanism of C2H4 formation was extensively investigated using density functional theory (DFT) calculations from multiple possible pathways. © 2022 American Chemical Society.

Item Type:	Journal Article
Publication:	Journal of the American Chemical Society
Publisher:	American Chemical Society
Additional Information:	The copyright for this article belongs to the American Chemical Society.
Department/Centre:	Division of Chemical Sciences > Materials Research Centre
Date Deposited:	31 Jan 2023 06:36
Last Modified:	31 Jan 2023 06:36
URI:	https://eprints.iisc.ac.in/id/eprint/79596

Actions (login required)

View Item