Facet-dependent active sites of a single Cu2O particle photocatalyst for CO2 reduction to methanol

Yimin A. Wu, Ian McNulty, Cong Liu, Kah Chun Lau, Qi Liu, Arvydas P. Paulikas, Cheng-Jun Sun, Zhonghou Cai, Jeffrey R. Guest, Yang Ren, Vojislav Stamenkovic, Larry A. Curtiss, Yuzi Liu () and Tijana Rajh ()
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Yimin A. Wu: Center for Nanoscale Materials, Argonne National Laboratory
Ian McNulty: Center for Nanoscale Materials, Argonne National Laboratory
Cong Liu: Chemical Sciences and Engineering Division, Argonne National Laboratory
Kah Chun Lau: Materials Science Division, Argonne National Laboratory
Qi Liu: City University of Hong Kong
Arvydas P. Paulikas: Materials Science Division, Argonne National Laboratory
Cheng-Jun Sun: Advanced Photon Source, Argonne National Laboratory
Zhonghou Cai: Advanced Photon Source, Argonne National Laboratory
Jeffrey R. Guest: Center for Nanoscale Materials, Argonne National Laboratory
Yang Ren: Advanced Photon Source, Argonne National Laboratory
Vojislav Stamenkovic: Materials Science Division, Argonne National Laboratory
Larry A. Curtiss: Materials Science Division, Argonne National Laboratory
Yuzi Liu: Center for Nanoscale Materials, Argonne National Laboratory
Tijana Rajh: Center for Nanoscale Materials, Argonne National Laboratory

Nature Energy, 2019, vol. 4, issue 11, 957-968

Abstract: Abstract Atomic-level understanding of the active sites and transformation mechanisms under realistic working conditions is a prerequisite for rational design of high-performance photocatalysts. Here, by using correlated scanning fluorescence X-ray microscopy and environmental transmission electron microscopy at atmospheric pressure, in operando, we directly observe that the (110) facet of a single Cu2O photocatalyst particle is photocatalytically active for CO2 reduction to methanol while the (100) facet is inert. The oxidation state of the active sites changes from Cu(i) towards Cu(ii) due to CO2 and H2O co-adsorption and changes back to Cu(i) after CO2 conversion under visible light illumination. The Cu2O photocatalyst oxidizes water as it reduces CO2. Concomitantly, the crystal lattice expands due to CO2 adsorption then reverts after CO2 conversion. The internal quantum yield for unassisted wireless photocatalytic reduction of CO2 to methanol using Cu2O crystals is ~72%.

Date: 2019
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DOI: 10.1038/s41560-019-0490-3

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