Doping palladium with tellurium for the highly selective electrocatalytic reduction of aqueous CO2 to CO
Abstract
Designing highly selective and energy-efficient electrocatalysts to minimize the competitive hydrogen evolution reaction in the electrochemical reduction of aqueous CO2 remains a challenge. In this study, we report that doping Pd with a small amount of Te could selectively convert CO2 to CO with a low overpotential. The PdTe/few-layer graphene (FLG) catalyst with a Pd/Te molar ratio of 1 : 0.05 displayed a maximum CO faradaic efficiency of about 90% at –0.8 V (vs. a reversible hydrogen electrode, RHE), CO partial current density of 4.4 mA cm–2, and CO formation turnover frequency of 0.14 s–1 at –1.0 V (vs. a RHE), which were 3.7-, 4.3-, and 10-fold higher than those of a Pd/FLG catalyst, respectively. Density functional calculations showed that Te adatoms preferentially bind at the terrace sites of Pd, thereby suppressing undesired hydrogen evolution, whereas CO2 adsorption and activation occurred on the high index sites of Pd to produce CO.
- Authors:
-
[1];
[3];
[4];
[2];
[3];
[1]
- Beijing Univ. of Chemical Technology (China)
- Chinese Academy of Sciences (CAS), Beijing (China)
- Korea Advanced Inst. Science and Technology (KAIST), Daejeon (Korea, Republic of)
- Univ. of Oxford (United Kingdom)
- Publication Date:
- Research Org.:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE; Chinese Academy of Sciences; National Research Foundation of Korea (NRF)
- OSTI Identifier:
- 1719125
- Report Number(s):
- PNNL-SA-127588
Journal ID: ISSN 2041-6539
- Grant/Contract Number:
- AC05-76RL01830; OIC-201503005; BUCTRC201525; BNLMS20160133; NRF-2017R1A2B3010176; 2016M3D1A1021147; 2015R1A2A1A15055539
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemical Science (Online)
- Additional Journal Information:
- Journal Name: Chemical Science (Online); Journal Volume: 9; Journal Issue: 2; Journal ID: ISSN 2041-6539
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Tao, Hengcong, Sun, Xiaofu, Back, Seoin, Han, Zishan, Zhu, Qinggong, Robertson, Alex W, Ma, Tao, Fan, Qun, Han, Buxing, Jung, Yousung, and Sun, Zhenyu. Doping palladium with tellurium for the highly selective electrocatalytic reduction of aqueous CO2 to CO. United States: N. p., 2017.
Web. doi:10.1039/C7SC03018E.
Tao, Hengcong, Sun, Xiaofu, Back, Seoin, Han, Zishan, Zhu, Qinggong, Robertson, Alex W, Ma, Tao, Fan, Qun, Han, Buxing, Jung, Yousung, & Sun, Zhenyu. Doping palladium with tellurium for the highly selective electrocatalytic reduction of aqueous CO2 to CO. United States. https://doi.org/10.1039/C7SC03018E
Tao, Hengcong, Sun, Xiaofu, Back, Seoin, Han, Zishan, Zhu, Qinggong, Robertson, Alex W, Ma, Tao, Fan, Qun, Han, Buxing, Jung, Yousung, and Sun, Zhenyu. Mon .
"Doping palladium with tellurium for the highly selective electrocatalytic reduction of aqueous CO2 to CO". United States. https://doi.org/10.1039/C7SC03018E. https://www.osti.gov/servlets/purl/1719125.
@article{osti_1719125,
title = {Doping palladium with tellurium for the highly selective electrocatalytic reduction of aqueous CO2 to CO},
author = {Tao, Hengcong and Sun, Xiaofu and Back, Seoin and Han, Zishan and Zhu, Qinggong and Robertson, Alex W and Ma, Tao and Fan, Qun and Han, Buxing and Jung, Yousung and Sun, Zhenyu},
abstractNote = {Designing highly selective and energy-efficient electrocatalysts to minimize the competitive hydrogen evolution reaction in the electrochemical reduction of aqueous CO2 remains a challenge. In this study, we report that doping Pd with a small amount of Te could selectively convert CO2 to CO with a low overpotential. The PdTe/few-layer graphene (FLG) catalyst with a Pd/Te molar ratio of 1 : 0.05 displayed a maximum CO faradaic efficiency of about 90% at –0.8 V (vs. a reversible hydrogen electrode, RHE), CO partial current density of 4.4 mA cm–2, and CO formation turnover frequency of 0.14 s–1 at –1.0 V (vs. a RHE), which were 3.7-, 4.3-, and 10-fold higher than those of a Pd/FLG catalyst, respectively. Density functional calculations showed that Te adatoms preferentially bind at the terrace sites of Pd, thereby suppressing undesired hydrogen evolution, whereas CO2 adsorption and activation occurred on the high index sites of Pd to produce CO.},
doi = {10.1039/C7SC03018E},
journal = {Chemical Science (Online)},
number = 2,
volume = 9,
place = {United States},
year = {Mon Nov 06 00:00:00 EST 2017},
month = {Mon Nov 06 00:00:00 EST 2017}
}
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