期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 317, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2022.121681
关键词
CO2 reduction reaction; Transition metal phosphides; Imidazolium; in-situ Raman; Ethanol electrosynthesis
资金
- National Science Foundation (NSF) Catalysis [CBET-2135173]
- Advanced Research Projects Agency-Energy (ARPA-E), United States (U.S.) Department of Energy [DE-AR0001581]
- Materials Research Science and Engineering Centers (MRSEC) program at the Materials Research Center [DMR-1121262]
- Nanoscale Science and Engineering Center at the International Institute for Nanotechnology [EEC 0647560]
- State of Illinois, through the International Institute for Nanotechnology
- NSF [DMR-1809439]
- Major Research Instrumentation Program (MRI-R2) grant from the National Science Foundation [DMR-0959470]
- Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division
- U.S. Department of Energy
- MRCAT
- DOE Office of Science
- U.S. Department of Energy Office of Science laboratory [DE-AC02-06CH11357]
This study found a catalytic system using molybdenum phosphide nanoparticles covered by imidazolium-functionalized ionomer, which effectively reduces carbon dioxide to ethanol. The imidazolium-functionalized ionomer improves the diffusion of CO2 and balances the water content in the catalyst layer, resulting in higher CO2-to-water ratio and fine-tuning of the electronic properties of the catalyst surface.
An effective electrochemical carbon dioxide reduction reaction (eCO(2)RR) requires the discovery of a catalytic system that is highly active and selective for multi-carbon products together with superior CO2 diffusion at a catalyst layer to minimize the reduction barriers. Here, we found a catalytic system that uses molybdenum phosphide (MoP) nanoparticles covered by imidazolium-functionalized ionomer (Im) that promotes CO2 diffusion at the catalyst layer toward the catalyst surface, where CO2 is reduced to ethanol (C2H5OH). The electrochemical results with the MoP-Im co-catalyst show a C2H5OH production Faradaic efficiency and a cathodic energy efficiency of 77.4% and 63.3%, respectively, at a potential as low as - 200 mV vs. RHE. The electrochemical experiments along with our physicochemical characterizations indicate that the Im improves CO2 diffusion and balances water content resulting in a higher CO2-to-water ratio at the catalyst layer and fine-tunes the electronic properties of Mo atoms at the MoP surface. In-situ Raman spectroscopy reveals that a high number of adsorbed *CO intermediates on the surface and a higher binding strength of *CO intermediates on the Mo surface sites in the presence of imidazolium molecules are the main reasons for a superior C-C coupling and thereby the improved C2H5OH formation.
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