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Title: 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:
 [1]; ORCiD logo [2];  [3];  [2];  [4];  [5]; ORCiD logo [6];  [7];  [8]; ORCiD logo [9]
  1. Columbia Univ., New York, NY (United States); Univ. of Science and Technology of China, Hefei (China)
  2. Columbia Univ., New York, NY (United States)
  3. Nanyang Technological Univ. (Singapore)
  4. Department of Chemical EngineeringColumbia University New York NY 10027 USA
  5. Brookhaven National Lab. (BNL), Upton, NY (United States)
  6. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  7. Florida A & M University, Tallahassee, FL (United States)
  8. Univ. of Science and Technology of China, Hefei (China)
  9. 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 Lab. (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 R&D 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. doi: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. doi: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 = {2020},
month = {3}
}

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