Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 28, Pages 11345-11348Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202003625
Keywords
carbon dioxide reduction reaction; density functional theory; interfacial energy; metal nitrides; palladium hydride
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Funding
- US Department of Energy, Basic Energy Science, Catalysis Science Program [DE-FG02-13ER16381]
- Center for Functional Nanomaterials (CFN) in Brookhaven National Laboratory [DE-SC0012704]
- China Scholarship Council [201806010243, 201808740001]
- Advanced Photon Source (APS) in Argonne National Laboratory [DE-AC02-06CH11357]
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The electrochemical carbon dioxide reduction reaction (CO2RR) to produce synthesis gas (syngas) with tunable CO/H-2 ratios has been studied by supporting Pd catalysts on transition metal nitride (TMN) substrates. Combining experimental measurements and density functional theory (DFT) calculations, Pd-modified niobium nitride (Pd/NbN) is found to generate much higher CO and H-2 partial current densities and greater CO Faradaic efficiency than Pd-modified vanadium nitride (Pd/VN) and commercial Pd/C catalysts. In-situ X-ray diffraction identifies the formation of PdH in Pd/NbN and Pd/C under CO2RR conditions, whereas the Pd in Pd/VN is not fully transformed into the active PdH phase. DFT calculations show that the stabilized *HOCO and weakened *CO intermediates on PdH/NbN are critical to achieving higher CO2RR activity. This work suggests that NbN is a promising substrate to modify Pd, resulting in an enhanced electrochemical conversion of CO2 to syngas with a potential reduction in precious metal loading.
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