Photocatalytic Activation and Reduction of CO2 to CH4 over Single Phase Nano Cu3SnS4: A Combined Experimental and Theoretical Study

Neha Sharma, Tilak Das, Santosh Kumar, Reshma Bhosale, Mubul Kabir, Satishchandra Ogale

Research output: Contribution to journalArticlepeer-review

14 Citations (Scopus)
15 Downloads (Pure)

Abstract

In view of their ability to absorb visible light and their high surface catalytic activity, metal sulfides are rapidly emerging as promising candidates for CO 2 photoreduction, scoring over the traditional oxide-based systems. However, their low conversion efficiencies due to serious radiative recombination issues and poor stability restrict their real-life applicability. Enhancing their performance by coupling them with other semiconductor-based photocatalysts or precious noble metals as cocatalysts makes the process cost intensive. Herein, we report the single-phase ternary sulfide Cu 3SnS 4 (CTS) as a robust visible-light photocatalyst for selective photoreduction of CO 2 to CH 4. It showed a remarkable 80% selectivity for CH 4 evolution with the rate of 14 μmol/g/h, without addition of any cocatalyst or scavenger. The mechanistic pathway for catalytic activity is elucidated by first principle calculations and in situ ATR, which imply a formaldehyde pathway of hydrocarbon production. The Cu-Sn termination of the surface is shown to be the key factor for competent CO 2 absorption and activation as confirmed from our X-ray spectroscopy measurements and first principle calculations. This study provides a foundation and insights for the rational design of sulfide-based photocatalysts to produce renewable fuel.

Original languageEnglish
Pages (from-to)5677-5685
Number of pages9
JournalACS Applied Energy Materials
Volume2
Issue number8
Early online date1 Jul 2019
DOIs
Publication statusPublished - 26 Aug 2019

Keywords

  • CO reduction
  • Cu SnS
  • Cu-Sn-terminated surface
  • photocatalysis
  • solar fuels

ASJC Scopus subject areas

  • Chemical Engineering (miscellaneous)
  • Energy Engineering and Power Technology
  • Electrochemistry
  • Materials Chemistry
  • Electrical and Electronic Engineering

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