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

Liu, Yumeng; Tian, Dong; Biswas, Akash N.; Xie, Zhenhua; Hwang, Sooyeon; Lee, Ji Hoon; Meng, Hong; Chen, Jingguang G.

doi:10.1002/anie.202003625

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

Journal Article · Tue Apr 14 00:00:00 EDT 2020 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202003625· OSTI ID:1618410

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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)

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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704; FG02-13ER16381; SC0009476

OSTI ID:: 1618410

Alternate ID(s):: OSTI ID: 1617980

Report Number(s):: BNL-215927-2020-JAAM

Journal Information:: Angewandte Chemie (International Edition), Vol. 59, Issue 28; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 83 works

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25 ENERGY STORAGE
carbon dioxide reduction reaction
density functional theory
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Title: Transition Metal Nitrides as Promising Catalyst Supports for Tuning CO/H2 Syngas Production from Electrochemical CO2 Reduction

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