Transition Metal Nitrides as Promising Catalyst Supports for Tuning CO/H2 Syngas Production from Electrochemical CO2 Reduction

The electrochemical carbon dioxide reduction reaction (CO2RR) to produce synthesis gas (syngas) with tunable CO/H2 ratios has been studied by supporting Pd catalysts on transition metal nitride (TMN) substrates. Combining experimental measurements and density functional theory (DFT) calculations, Pd...

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Published in:Angewandte Chemie (International ed.) 2020-07, Vol.59 (28), p.11345-11348
Main Authors: Liu, Yumeng, Tian, Dong, Biswas, Akash N., Xie, Zhenhua, Hwang, Sooyeon, Lee, Ji Hoon, Meng, Hong, Chen, Jingguang G.
Format: Article
Language:English
Subjects:
Carbon dioxide
carbon dioxide reduction reaction
Catalysts
Chemical reduction
Density functional theory
Electrochemistry
ENERGY STORAGE
interfacial energy
Intermediates
Mathematical analysis
Metal nitrides
Niobium
Niobium nitride
Palladium
palladium hydride
Substrates
Synthesis gas
Transition metals
Vanadium
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Summary:The electrochemical carbon dioxide reduction reaction (CO2RR) to produce synthesis gas (syngas) with tunable CO/H2 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 H2 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. Palladium‐modified transition metal nitrides are investigated as electrochemical CO2 reduction reaction (CO2RR) catalysts. Combined in‐situ X‐ray characterization and DFT results demonstrate niobium nitride as an effective support material to enhance CO2RR activity.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202003625