Abstract
Copper-based catalyst is uniquely positioned to catalyze the hydrocarbon formations through electrochemical CO2 reduction. The catalyst design freedom is limited for alloying copper with H-affinitive elements represented by platinum group metals because the latter would easily drive the hydrogen evolution reaction to override CO2 reduction. We report an adept design of anchoring atomically dispersed platinum group metal species on both polycrystalline and shape-controlled Cu catalysts, which now promote targeted CO2 reduction reaction while frustrating the undesired hydrogen evolution reaction. Notably, alloys with similar metal formulations but comprising small platinum or palladium clusters would fail this objective. With an appreciable amount of CO-Pd1 moieties on copper surfaces, facile CO* hydrogenation to CHO* or CO-CHO* coupling is now viable as one of the main pathways on Cu(111) or Cu(100) to selectively produce CH4 or C2H4 through Pd-Cu dual-site pathways. The work broadens copper alloying choices for CO2 reduction in aqueous phases.
| Original language | English |
|---|---|
| Article number | 3075 |
| Journal | Nature Communications |
| Volume | 14 |
| Issue number | 1 |
| DOIs | |
| State | Published - Dec 2023 |
Funding
M.Y. thanks the support provided by the start-up fund and the Creative Inquiry Program (CI#2186) of Clemson University, NASA EPSCoR (SC-80NSSC22M020), and the use of 12-BM beamline of the Advanced Photon Source is supported by the U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by the Argonne National Laboratory under Contract No. DE-AC02-06CH11357. The Electron microscopy facility was supported by Drs. Laxmikant Saraf and Haijun Qian at Clemson University Electron Microscopy Facility. Instruments were supported by Dr. Rakesh Sachdeva at the Department of Chemistry at Clemson University. Post-reaction sample scanning transmission electron microscopy research was supported by the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. M.C. thanks Clemson University for postdoctoral research funding. Z.J. and M.Y. thanks for the support from Hitachi High-Tech, USA 2022 Fellowship, Creative Inquiry program of Clemson University. F.C. thanks the support from the institutional faculty start-up funds from the University of Massachusetts Lowell and National Science Foundation for partial support (award #2103478). M.W. and F.C. acknowledge the computational resources provided by the Massachusetts Green High-Performance Computing Center (MGHPCC). M.W. and F.C also acknowledge the Extreme Science and Engineering Discovery Environment (XSEDE) at Texas Advanced Computing Center (TACC) Dell/Intel Knights Landing, Skylake System (Stampede2) and San Diego Supercomputer Center Expense through allocation CHE200083 Renewal for the computational facility support. Yang Group would like to thank the entire Rachel Getman Group for the fun and constructive discussions of catalysis science that we had at those joint group meetings at Clemson. M.Y. wishes good friend Dr. Rachel the best in her new endeavor in Ohio. M.Y. thanks the support provided by the start-up fund and the Creative Inquiry Program (CI#2186) of Clemson University, NASA EPSCoR (SC-80NSSC22M020), and the use of 12-BM beamline of the Advanced Photon Source is supported by the U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by the Argonne National Laboratory under Contract No. DE-AC02-06CH11357. The Electron microscopy facility was supported by Drs. Laxmikant Saraf and Haijun Qian at Clemson University Electron Microscopy Facility. Instruments were supported by Dr. Rakesh Sachdeva at the Department of Chemistry at Clemson University. Post-reaction sample scanning transmission electron microscopy research was supported by the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. M.C. thanks Clemson University for postdoctoral research funding. Z.J. and M.Y. thanks for the support from Hitachi High-Tech, USA 2022 Fellowship, Creative Inquiry program of Clemson University. F.C. thanks the support from the institutional faculty start-up funds from the University of Massachusetts Lowell and National Science Foundation for partial support (award #2103478). M.W. and F.C. acknowledge the computational resources provided by the Massachusetts Green High-Performance Computing Center (MGHPCC). M.W. and F.C also acknowledge the Extreme Science and Engineering Discovery Environment (XSEDE) at Texas Advanced Computing Center (TACC) Dell/Intel Knights Landing, Skylake System (Stampede2) and San Diego Supercomputer Center Expense through allocation CHE200083 Renewal for the computational facility support. Yang Group would like to thank the entire Rachel Getman Group for the fun and constructive discussions of catalysis science that we had at those joint group meetings at Clemson. M.Y. wishes good friend Dr. Rachel the best in her new endeavor in Ohio.
| Funders | Funder number |
|---|---|
| Center for Nanophase Materials Sciences | |
| NASA EPSCoR | SC-80NSSC22M020 |
| National Science Foundation | 2103478 |
| U.S. Department of Energy | |
| Office of Science | |
| Argonne National Laboratory | DE-AC02-06CH11357 |
| Oak Ridge National Laboratory | |
| Clemson University | |
| Massachusetts Green High Performance Computing Center | |
| University of Massachusetts Lowell |
