@article{6cd873aafd834f588384f9d001865b7a,
title = "Facet-dependent active sites of a single Cu2O particle photocatalyst for CO2 reduction to methanol",
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%.",
author = "Wu, {Yimin A.} and Ian McNulty and Cong Liu and Lau, {Kah Chun} and Qi Liu and Paulikas, {Arvydas P.} and Sun, {Cheng Jun} and Zhonghou Cai and Guest, {Jeffrey R.} and Yang Ren and Vojislav Stamenkovic and Curtiss, {Larry A.} and Yuzi Liu and Tijana Rajh",
note = "Funding Information: This work was performed at the Center for Nanoscale Materials, a US Department of Energy, Office of Science, Basic Energy Sciences, under Contract no. DE-AC02-06CH11357. Use of the Advanced Photon Source was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract no. DE-AC02-06CH11357. This work is partially supported by Laboratory Directed Research and Development (LDRD) funding from Argonne National Laboratory, provided by the Director, Office of Science, of the US Department of Energy under Contract no. DE-AC02-06CH11357. The computational studies were supported by the US Department of Energy, Basic Energy Sciences, Division of Materials Science and Engineering. C.L., K.C.L. and L.A.C. acknowledge grants of computer time through the LCRC Blues Cluster at Argonne National Laboratory. Cong Liu acknowledges the financial support by US Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences, under Contract no. DE-AC02-06CH11357. We acknowledge discussions with and the assistance of P. Fuesz, M. Holt, S. Lapidus, E. Rozhkova, C. Fry, R. Zhang, L. Li and M. Chan. Publisher Copyright: {\textcopyright} 2019, This is a U.S. government work and not under copyright protection in the U.S.; foreign copyright protection may apply.",
year = "2019",
month = nov,
day = "1",
doi = "10.1038/s41560-019-0490-3",
language = "English (US)",
volume = "4",
pages = "957--968",
journal = "Nature Energy",
issn = "2058-7546",
publisher = "Springer Nature",
number = "11",
}