Transition Metal Nitrides as Promising Catalyst Supports for Tuning CO/H2 Syngas Production from Electrochemical CO2 Reduction
Abstract
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.
- Authors:
-
[1];
[2];
[3];
[4];
[5];
[3];
[6];
[7]
- Columbia Univ., New York, NY (United States); Peking Univ., Beijing (China)
- Columbia Univ., New York, NY (United States); Kunming Univ. of Science and Technology (China)
- Columbia Univ., New York, NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
- Peking Univ., Beijing (China)
- Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1618410
- Alternate Identifier(s):
- OSTI ID: 1617980
- Report Number(s):
- BNL-215927-2020-JAAM
Journal ID: ISSN 1433-7851
- Grant/Contract Number:
- SC0012704; FG02-13ER16381; SC0009476
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 59; Journal Issue: 28; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; carbon dioxide reduction reaction; density functional theory; interfacial energy; metal nitrides; palladium hydride
Citation Formats
Liu, Yumeng, Tian, Dong, Biswas, Akash N., Xie, Zhenhua, Hwang, Sooyeon, Lee, Ji Hoon, Meng, Hong, and Chen, Jingguang G. Transition Metal Nitrides as Promising Catalyst Supports for Tuning CO/H2 Syngas Production from Electrochemical CO2 Reduction. United States: N. p., 2020.
Web. doi:10.1002/anie.202003625.
Liu, Yumeng, Tian, Dong, Biswas, Akash N., Xie, Zhenhua, Hwang, Sooyeon, Lee, Ji Hoon, Meng, Hong, & Chen, Jingguang G. Transition Metal Nitrides as Promising Catalyst Supports for Tuning CO/H2 Syngas Production from Electrochemical CO2 Reduction. United States. https://doi.org/10.1002/anie.202003625
Liu, Yumeng, Tian, Dong, Biswas, Akash N., Xie, Zhenhua, Hwang, Sooyeon, Lee, Ji Hoon, Meng, Hong, and Chen, Jingguang G. Tue .
"Transition Metal Nitrides as Promising Catalyst Supports for Tuning CO/H2 Syngas Production from Electrochemical CO2 Reduction". United States. https://doi.org/10.1002/anie.202003625. https://www.osti.gov/servlets/purl/1618410.
@article{osti_1618410,
title = {Transition Metal Nitrides as Promising Catalyst Supports for Tuning CO/H2 Syngas Production from Electrochemical CO2 Reduction},
author = {Liu, Yumeng and Tian, Dong and Biswas, Akash N. and Xie, Zhenhua and Hwang, Sooyeon and Lee, Ji Hoon and Meng, Hong and Chen, Jingguang G.},
abstractNote = {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.},
doi = {10.1002/anie.202003625},
journal = {Angewandte Chemie (International Edition)},
number = 28,
volume = 59,
place = {United States},
year = {Tue Apr 14 00:00:00 EDT 2020},
month = {Tue Apr 14 00:00:00 EDT 2020}
}
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