Carbon Nitride-Based Ruthenium Single Atom Photocatalyst for CO2 Reduction to Methanol

Priti Sharma, Subodh Kumar, Ondrej Tomanec, Martin Petr, Johnny Zhu Chen, Jeffrey T. Miller, Rajender S. Varma, Manoj B. Gawande, Radek Zbořil

Research output: Contribution to journalArticlepeer-review

161 Scopus citations

Abstract

With increasing concerns for global warming, the solar-driven photocatalytic reduction of CO2 into chemical fuels like methanol is a propitious route to enrich energy supplies, with concomitant reduction of the abundant CO2 stockpiles. Herein, a novel single atom-confinement and a strategy are reported toward single ruthenium atoms dispersion over porous carbon nitride surface. Ruthenium single atom character is well confirmed by EXAFS absorption spectrometric analysis unveiling the cationic coordination environment for the single-atomic-site ruthenium center, that is formed by Ru-N/C intercalation in the first coordination shell, attaining synergism in N–Ru–N connection and interfacial carrier transfer. From time resolved fluorescence decay spectra, the average carrier lifetime of the RuSA–mC3N4 system is found to be higher compared to m-C3N4; the fact uncovering the crucial role of single Ru atoms in promoting photocatalytic reaction system. A high yield of methanol (1500 µmol g-1 cat. after 6 h of the reaction) using water as an electron donor and the reusability of the developed catalyst without any significant change in the efficiency represent the superior aspects for its potential application in real industrial technologies.

Original languageEnglish
Article number2006478
JournalSmall
Volume17
Issue number16
DOIs
StatePublished - 22 Apr 2021
Externally publishedYes

Bibliographical note

Publisher Copyright:
© 2021 Wiley-VCH GmbH

Funding

P.S. and S.K. contributed equally to this work. The authors gratefully acknowledge the support by the Operational Program Research, Development and Education—European Regional Development Fund (project no. CZ.02.1.01/0.0/0.0/16_019/0000754) and by the ERDF project “Development of pre‐applied research in nanotechnology and biotechnology” (project no. CZ.02.1.01/0.0/0.0/17_048/0007323) of the Ministry of Education, Youth and Sports of the Czech Republic. R.Z. acknowledges the support from the Czech Science Foundation, project No. 19‐27454X. The authors thank to Ms. J. Stráská and Ms. P. Bazgerová for TEM analysis. Use of the Advanced Photon Source was supported by the U.S. Department of Energy Office of Basic Energy Sciences under contract no. DE‐AC02‐06CH11357. MRCAT operations, beamline 10‐BM, are supported by the Department of Energy and the MRCAT member institutions.

FundersFunder number
Operational Program Research, Development and Education
U.S. Department of Energy Office of Basic Energy SciencesDE‐AC02‐06CH11357
U.S. Department of Energy
Ministerstvo Školství, Mládeže a Tělovýchovy
Grantová Agentura České Republiky19‐27454X
European Regional Development FundCZ.02.1.01/0.0/0.0/17_048/0007323

    Keywords

    • carbon nitride
    • photocatalysts
    • photocatalytic reduction of carbon dioxide
    • single atom

    Fingerprint

    Dive into the research topics of 'Carbon Nitride-Based Ruthenium Single Atom Photocatalyst for CO2 Reduction to Methanol'. Together they form a unique fingerprint.

    Cite this