Transition Metal Nitrides as Promising Catalyst Supports for Tuning CO/H 2 Syngas Production from Electrochemical CO 2 Reduction
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- Department of Chemical Engineering Columbia University 821 Mudd Building New York NY 10027 USA, School of Advanced Materials Peking University Shenzhen Graduate School Peking University Shenzhen Guangdong Province 518055 China
- Department of Chemical Engineering Columbia University 821 Mudd Building New York NY 10027 USA, State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization/Faculty of Metallurgical and Energy Engineering Kunming University of Science and Technology Kunming Yunnan Province 650093 China
- Department of Chemical Engineering Columbia University 821 Mudd Building New York NY 10027 USA
- Chemistry Division Brookhaven National Laboratory Building 555 Upton NY 11973 USA
- Center for Functional Nanomaterials Brookhaven National Laboratory Upton NY 11973 USA
- School of Advanced Materials Peking University Shenzhen Graduate School Peking University Shenzhen Guangdong Province 518055 China
- Department of Chemical Engineering Columbia University 821 Mudd Building New York NY 10027 USA, Chemistry Division Brookhaven National Laboratory Building 555 Upton NY 11973 USA
Abstract The electrochemical carbon dioxide reduction reaction (CO 2 RR) 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 CO 2 RR 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 CO 2 RR activity. This work suggests that NbN is a promising substrate to modify Pd, resulting in an enhanced electrochemical conversion of CO 2 to syngas with a potential reduction in precious metal loading.
- Sponsoring Organization:
- USDOE
- Grant/Contract Number:
- FG02-13ER16381; SC0009476
- OSTI ID:
- 1617984
- Journal Information:
- Angewandte Chemie, Journal Name: Angewandte Chemie Vol. 132 Journal Issue: 28; ISSN 0044-8249
- Publisher:
- Wiley Blackwell (John Wiley & Sons)Copyright Statement
- Country of Publication:
- Germany
- Language:
- English
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