Copper carbon dioxide reduction electrocatalysts studied by in situ soft X-ray spectro-ptychography

Li, 2021, Recent advances in metal-based electrocatalysts with hetero-interfaces for CO2 reduction reaction, Chem Catal., 12, 262 Zhang, 2022, Chemical Structure and Distribution in Nickel–Nitrogen–Carbon Catalysts for CO2 Electroreduction Identified by Scanning Transmission X-ray Microscopy, ACS Catal., 12, 8746, 10.1021/acscatal.2c01255 Chou, 2020, Controlling the oxidation state of the Cu electrode and reaction intermediates for electrochemical CO2 reduction to ethylene, J. Am. Chem. Soc., 142, 2857, 10.1021/jacs.9b11126 Gibbons, 2020, In situ X-ray absorption spectroscopy disentangles the roles of copper and silver in a bimetallic catalyst for the oxygen reduction reaction, Chem. Mater., 32, 1819, 10.1021/acs.chemmater.9b03963 De Luna, 2019, What would it take for renewably powered electrosynthesis to displace petrochemical processes?, Science, 364, eaav3506, 10.1126/science.aav3506 Yang, 2022, Operando Resonant Soft X-ray Scattering Studies of Chemical Environment and Interparticle Dynamics of Cu Nanocatalysts for CO2 Electroreduction, Surg. Endosc., 36, 8927, 10.1007/s00464-022-09341-4 Tabassum, 2022, Surface engineering of Cu catalysts for electrochemical reduction of CO2 to value-added multi-carbon products, Chem Catal., 2, 1561, 10.1016/j.checat.2022.04.012 Hahn, 2017, Engineering Cu surfaces for the electrocatalytic conversion of CO2: Controlling selectivity toward oxygenates and hydrocarbons, Proc. Natl. Acad. Sci. USA, 114, 5918, 10.1073/pnas.1618935114 Timoshenko, 2022, Steering the structure and selectivity of CO2 electroreduction catalysts by potential pulses, Nat. Catal., 5, 259, 10.1038/s41929-022-00760-z Arán-Ais, 2020, The role of in situ generated morphological motifs and Cu (i) species in C2+ product selectivity during CO2 pulsed electroreduction, Nat. Energy, 5, 317, 10.1038/s41560-020-0594-9 Timoshenko, 2021, In situ/operando electrocatalyst characterization by X-ray absorption spectroscopy, Chem. Rev., 121, 882, 10.1021/acs.chemrev.0c00396 Nitopi, 2019, Progress and perspectives of electrochemical CO2 reduction on copper in aqueous electrolyte, Chem. Rev., 119, 7610, 10.1021/acs.chemrev.8b00705 Kibria, 2019, Electrochemical CO2 reduction into chemical feedstocks: from mechanistic electrocatalysis models to system design, Adv. Mater., 31, 10.1002/adma.201807166 Cheng, 2021, The nature of active sites for carbon dioxide electroreduction over oxide-derived copper catalysts, Nat. Commun., 12, 395, 10.1038/s41467-020-20615-0 Eilert, 2017, Subsurface oxygen in oxide-derived copper electrocatalysts for carbon dioxide reduction, J. Phys. Chem. Lett., 8, 285, 10.1021/acs.jpclett.6b02273 Wang, 2022, Direct Evidence of Subsurface Oxygen Formation in Oxide-Derived Cu by X-ray Photoelectron Spectroscopy, Angew. Chem., Int. Ed. Engl., 61 Fields, 2018, Role of subsurface oxygen on Cu surfaces for CO2 electrochemical reduction, J. Phys. Chem. C, 122, 16209, 10.1021/acs.jpcc.8b04983 Scott, 2019, Absence of oxidized phases in Cu under CO reduction conditions, ACS Energy Lett., 4, 803, 10.1021/acsenergylett.9b00172 Lum, 2018, Stability of residual oxides in oxide-derived copper catalysts for electrochemical CO2 reduction investigated with 18O labeling, Angew. Chem., Int. Ed. Engl., 57, 551, 10.1002/anie.201710590 Grosse, 2021, Dynamic transformation of cubic copper catalysts during CO2 electroreduction and its impact on catalytic selectivity, Nat. Commun., 12, 6736, 10.1038/s41467-021-26743-5 Arán-Ais, 2020, Imaging electrochemically synthesized Cu2O cubes and their morphological evolution under conditions relevant to CO2 electroreduction, Nat. Commun., 11, 3489, 10.1038/s41467-020-17220-6 Alnoush, 2021, Judicious selection, validation, and use of reference electrodes for in situ and operando electrocatalysis studies, Chem Catal., 1, 997, 10.1016/j.checat.2021.07.001 Velasco-Velez, 2020, Revealing the active phase of copper during the electroreduction of CO2 in aqueous electrolyte by correlating in situ X-ray spectroscopy and in situ electron microscopy, ACS Energy Lett., 5, 2106, 10.1021/acsenergylett.0c00802 Hitchcock, 2021, In situ and Operando Studies with Soft X-Ray Transmission Spectromicroscopy, Microsc. Microanal., 27, 59, 10.1017/S1431927621013295 Yang, 2023, Operando studies reveal active Cu nanograins for CO2 electroreduction, Nature, 15, 262, 10.1038/s41586-022-05540-0 Ade, 2008, NEXAFS microscopy and resonant scattering: Composition and orientation probed in real and reciprocal space, Polymer, 49, 643, 10.1016/j.polymer.2007.10.030 Hitchcock, 2012, 745 Stöhr, 2013, 25 Nelson Weker, 2015, Emerging In Situ and Operando Nanoscale X-Ray Imaging Techniques for Energy Storage Materials, Adv. Funct. Mater., 25, 1622, 10.1002/adfm.201403409 Lim, 2016, Origin and hysteresis of lithium compositional spatiodynamics within battery primary particles, Science, 353, 566, 10.1126/science.aaf4914 Chourasia, 2022, In Situ/Operando Characterization Techniques: The Guiding Tool for the Development of Li–CO2 Battery, Small Methods, 6, 10.1002/smtd.202200930 Prabu, 2018, Instrumentation for in situ flow electrochemical scanning transmission X-ray microscopy (STXM), Rev. Sci. Instrum., 89, 10.1063/1.5023288 Zhang, 2023, In-situ studies of copper-based CO2 reduction electrocatalysts by scanning transmission soft X-ray microscopy, ACS Nano, 10.1021/acsnano.3c05964 Mefford, 2021, Correlative operando microscopy of oxygen evolution electrocatalysts, Nature, 593, 67, 10.1038/s41586-021-03454-x Jacobsen, 2019 Pfeiffer, 2018, X-ray ptychography, Nat. Photonics, 12, 9, 10.1038/s41566-017-0072-5 Mille, 2022, Ptychography at the carbon K-edge, Commun. Mater., 3, 8, 10.1038/s43246-022-00232-8 Vijayakumar, 2023, Soft X-ray spectro-ptychography of boron nitride nanobamboos, carbon nanotubes and permalloy nanorods, J. Synchrotron Radiat., 30, 746, 10.1107/S1600577523003399 Shapiro, 2014, Chemical composition mapping with nanometre resolution by soft X-ray microscopy, Nat. Photonics, 8, 765, 10.1038/nphoton.2014.207 Shapiro, 2020, An ultrahigh-resolution soft x-ray microscope for quantitative analysis of chemically heterogeneous nanomaterials, Sci. Adv., 6, 10.1126/sciadv.abc4904 Xu, 2017, Low-dose, high-resolution and high-efficiency ptychography at STXM beamline of SSRF Journal of Physics: Conference Series, IOP Publishing, 849 Xia, 2022, Molecular insights into roles of dissolved organic matter in Cr (III) immobilization by coprecipitation with Fe (III) probed by STXM-Ptychography and XANES spectroscopy, Environ. Sci. Technol., 56, 2432, 10.1021/acs.est.1c07528 Desjardins, 2019, Characterization of a back-illuminated CMOS camera for soft x-ray coherent scattering, 2054 Desjardins, 2020, Backside-illuminated scientific CMOS detector for soft X-ray resonant scattering and ptychography, J. Synchrotron Radiat., 27, 1577, 10.1107/S160057752001262X Urquhart, 2022, X-ray Spectroptychography, ACS Omega, 7, 11521, 10.1021/acsomega.2c00228 Grote, 2022, Imaging Cu2O nanocube hollowing in solution by quantitative in situ X-ray ptychography, Nat. Commun., 13, 4971, 10.1038/s41467-022-32373-2 Thibault, 2008, High-resolution scanning x-ray diffraction microscopy, Science, 321, 379, 10.1126/science.1158573 Fam, 2019, A versatile nanoreactor for complementary in situ X-ray and electron microscopy studies in catalysis and materials science, J. Synchrotron Radiat., 26, 1769, 10.1107/S160057751900660X Hoppe, 2013, High-resolution chemical imaging of gold nanoparticles using hard x-ray ptychography, Appl. Phys. Lett., 102, 10.1063/1.4807020 Baier, 2017, Stability of a bifunctional Cu-based core@ zeolite shell catalyst for dimethyl ether synthesis under redox conditions studied by environmental transmission electron microscopy and in situ X-ray ptychography, Microsc. Microanal., 23, 501, 10.1017/S1431927617000332 Sun, 2021, Soft X-ray ptychography chemical imaging of degradation in a composite surface-reconstructed Li-rich cathode, ACS Nano, 15, 1475, 10.1021/acsnano.0c08891 Wise, 2016, Nanoscale chemical imaging of an individual catalyst particle with soft X-ray ptychography, ACS Catal., 6, 2178, 10.1021/acscatal.6b00221 Kränzlin, 2015, Mechanistic Studies as a Tool for the Design of Copper-Based Heterostructures, Adv. Mater. Interfac., 2, 10.1002/admi.201500094 Kvashnina, 2007, Changes in electronic structure of copper films in aqueous solutions, J. Phys. Condens. Matter, 19, 10.1088/0953-8984/19/22/226002 Jiang, 2013, Experimental and theoretical investigation of the electronic structure of Cu2O and CuO thin films on Cu (110) using x-ray photoelectron and absorption spectroscopy, J. Chem. Phys., 138 Koprinarov, 2002, Quantitative mapping of structured polymeric systems using singular value decomposition analysis of soft X-ray images, J. Phys. Chem. B, 106, 5358, 10.1021/jp013281l Roberts, 2015, High selectivity for ethylene from carbon dioxide reduction over copper nanocube electrocatalysts, Angew. Chem., 54, 5179, 10.1002/anie.201412214 Roberts, 2016, Electroreduction of carbon monoxide over a copper nanocube catalyst: surface structure and pH dependence on selectivity, ChemCatChem, 8, 1119, 10.1002/cctc.201501189 Higgins, 2018, Guiding electrochemical carbon dioxide reduction toward carbonyls using copper silver thin films with interphase miscibility, ACS Energy Lett., 3, 2947, 10.1021/acsenergylett.8b01736 Belkhou, 2015, HERMES: a soft X-ray beamline dedicated to X-ray microscopy, J. Synchrotron Radiat., 22, 968, 10.1107/S1600577515007778 Kilcoyne, 2003, Interferometer-controlled scanning transmission X-ray microscopes at the Advanced Light Source, J. Synchrotron Radiat., 10, 125, 10.1107/S0909049502017739 Favre-Nicolin, 2020, PyNX: high-performance computing toolkit for coherent X-ray imaging based on operators, J. Appl. Crystallogr., 53, 1404, 10.1107/S1600576720010985 Jacobsen, 2000, Soft X-ray spectroscopy from image sequences with sub-100 nm spatial resolution, J. Microsc., 197, 173, 10.1046/j.1365-2818.2000.00640.x Hitchcock, 2023, Analysis of X-ray Images and Spectra (aXis2000): a toolkit for the analysis of X-ray spectromicroscopy data, J. Electron. Spectrosc. Relat. Phenom., 266, 10.1016/j.elspec.2023.147360