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 journalArticle

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

Cite this

Photocatalytic Activation and Reduction of CO2 to CH4 over Single Phase Nano Cu3SnS4: A Combined Experimental and Theoretical Study. / Sharma, Neha; Das, Tilak; Kumar, Santosh; Bhosale, Reshma; Kabir, Mubul; Ogale, Satishchandra.

In: ACS Applied Energy Materials, Vol. 2, No. 8, 26.08.2019, p. 5677-5685.

Research output: Contribution to journalArticle

Sharma, Neha ; Das, Tilak ; Kumar, Santosh ; Bhosale, Reshma ; Kabir, Mubul ; Ogale, Satishchandra. / Photocatalytic Activation and Reduction of CO2 to CH4 over Single Phase Nano Cu3SnS4: A Combined Experimental and Theoretical Study. In: ACS Applied Energy Materials. 2019 ; Vol. 2, No. 8. pp. 5677-5685.
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