Accelerating CO2 Electroreduction to CO Over Pd Single-Atom Catalyst
Abstract
The electrochemical conversion of carbon dioxide (CO2) into value-added chemicals is regarded as one of the promising routes to mitigate CO2 emission. A nitrogen-doped carbon-supported palladium (Pd) single-atom catalyst that can catalyze CO2 into CO with far higher mass activity than its Pd nanoparticle counterpart, for example, 373.0 and 28.5 mA mg–1Pd, respectively, at –0.8 V versus reversible hydrogen electrode, is reported herein. A combination of in situ X-ray characterization and density functional theory (DFT) calculation reveals that the Pd–N4 site is the most likely active center for CO production without the formation of palladium hydride (PdH), which is essential for typical Pd nanoparticle catalysts. Furthermore, the well-dispersed Pd–N4 single-atom site facilitates the stabilization of the adsorbed CO2 intermediate, thereby enhancing electrocatalytic CO2 reduction capability at low overpotentials. This work provides important insights into the structure-activity relationship for single-atom based electrocatalysts.
- Authors:
-
[2];
[6];
[9]
- Columbia Univ., New York, NY (United States); Univ. of Science and Technology of China, Hefei (China)
- Columbia Univ., New York, NY (United States)
- Nanyang Technological Univ. (Singapore)
- Department of Chemical EngineeringColumbia University New York NY 10027 USA
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
- Florida A & M University, Tallahassee, FL (United States)
- Univ. of Science and Technology of China, Hefei (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). National Synchrotron Light Source II (NSLS-II) and Center for Functional Nanomaterials (CFN); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); National Key Research and Development Program of China; China Scholarship Council (CSC)
- OSTI Identifier:
- 1604621
- Alternate Identifier(s):
- OSTI ID: 1602349
- Report Number(s):
- BNL-213730-2020-JAAM
Journal ID: ISSN 1616-301X
- Grant/Contract Number:
- SC0012704; FG02-13ER16381; ACI-1548562; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Functional Materials
- Additional Journal Information:
- Journal Volume: 30; Journal Issue: 17; Journal ID: ISSN 1616-301X
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; CO2 electroreduction; density functional theory; palladium; single‐atom catalysis; X‐ray absorption spectroscopy
Citation Formats
He, Qun, Lee, Ji Hoon, Liu, Daobin, Liu, Yumeng, Lin, Zhexi, Xie, Zhenhua, Hwang, Sooyeon, Kattel, Shyam, Song, Li, and Chen, Jingguang G. Accelerating CO2 Electroreduction to CO Over Pd Single-Atom Catalyst. United States: N. p., 2020.
Web. doi:10.1002/adfm.202000407.
He, Qun, Lee, Ji Hoon, Liu, Daobin, Liu, Yumeng, Lin, Zhexi, Xie, Zhenhua, Hwang, Sooyeon, Kattel, Shyam, Song, Li, & Chen, Jingguang G. Accelerating CO2 Electroreduction to CO Over Pd Single-Atom Catalyst. United States. https://doi.org/10.1002/adfm.202000407
He, Qun, Lee, Ji Hoon, Liu, Daobin, Liu, Yumeng, Lin, Zhexi, Xie, Zhenhua, Hwang, Sooyeon, Kattel, Shyam, Song, Li, and Chen, Jingguang G. Sun .
"Accelerating CO2 Electroreduction to CO Over Pd Single-Atom Catalyst". United States. https://doi.org/10.1002/adfm.202000407. https://www.osti.gov/servlets/purl/1604621.
@article{osti_1604621,
title = {Accelerating CO2 Electroreduction to CO Over Pd Single-Atom Catalyst},
author = {He, Qun and Lee, Ji Hoon and Liu, Daobin and Liu, Yumeng and Lin, Zhexi and Xie, Zhenhua and Hwang, Sooyeon and Kattel, Shyam and Song, Li and Chen, Jingguang G.},
abstractNote = {The electrochemical conversion of carbon dioxide (CO2) into value-added chemicals is regarded as one of the promising routes to mitigate CO2 emission. A nitrogen-doped carbon-supported palladium (Pd) single-atom catalyst that can catalyze CO2 into CO with far higher mass activity than its Pd nanoparticle counterpart, for example, 373.0 and 28.5 mA mg–1Pd, respectively, at –0.8 V versus reversible hydrogen electrode, is reported herein. A combination of in situ X-ray characterization and density functional theory (DFT) calculation reveals that the Pd–N4 site is the most likely active center for CO production without the formation of palladium hydride (PdH), which is essential for typical Pd nanoparticle catalysts. Furthermore, the well-dispersed Pd–N4 single-atom site facilitates the stabilization of the adsorbed CO2 intermediate, thereby enhancing electrocatalytic CO2 reduction capability at low overpotentials. This work provides important insights into the structure-activity relationship for single-atom based electrocatalysts.},
doi = {10.1002/adfm.202000407},
journal = {Advanced Functional Materials},
number = 17,
volume = 30,
place = {United States},
year = {Sun Mar 01 00:00:00 EST 2020},
month = {Sun Mar 01 00:00:00 EST 2020}
}
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