期刊
ADVANCED FUNCTIONAL MATERIALS
卷 30, 期 17, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202000407
关键词
CO2 electroreduction; density functional theory; palladium; single-atom catalysis; X-ray absorption spectroscopy
类别
资金
- US Department of Energy, Basic Energy Science, Catalysis Science Program [DE-FG02-13ER16381]
- National Synchrotron Light Source II (NSLS-II) [DE-SC0012704]
- Center for Functional Nanomaterials (CFN) [DE-SC0012704]
- National Science Foundation [ACI-1548562, TG-CHE190032]
- National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility [DE-AC02-05CH11231]
- National Key R&D Program of China [2017YFA0303500]
- China Scholarship Council (CSC) [201806340016, 201806010243]
The electrochemical conversion of carbon dioxide (CO2) into value-added chemicals is regarded as one of the promising routes to mitigate CO2 emission. A nitrogen-doped carbon-supported palladium (Pd) single-atom catalyst that can catalyze CO2 into CO with far higher mass activity than its Pd nanoparticle counterpart, for example, 373.0 and 28.5 mA mg(Pd)(-1), respectively, at -0.8 V versus reversible hydrogen electrode, is reported. A combination of in situ X-ray characterization and density functional theory (DFT) calculation reveals that the Pd-N-4 site is the most likely active center for CO production without the formation of palladium hydride (PdH), which is essential for typical Pd nanoparticle catalysts. Furthermore, the well-dispersed Pd-N-4 single-atom site facilitates the stabilization of the adsorbed CO2 intermediate, thereby enhancing electrocatalytic CO2 reduction capability at low overpotentials. This work provides important insights into the structure-activity relationship for single-atom based electrocatalysts.
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