Boosted CO2 photoreduction to methane: Via Co doping in bismuth vanadate atomic layers

Kefu Wang, Ling Zhang, Yang Su, Songmei Sun, Qianqian Wang, Haipeng Wang, Wenzhong Wang

Research output: Contribution to journalArticle

6 Citations (Scopus)

Abstract

CO2 photoreduction to valuable hydrocarbons is attractive and promising. Nevertheless, the photoactivity has been pretty low to date, and deeper insights into improving CO2 conversion efficiency remain a challenge. Here, BiVO4 atomic layers have been synthesized as ideal platforms to investigate the correlation between the electronic structures and activities for CO2 photoreduction. Cobalt (Co) is then deliberately doped in BiVO4 atomic layers to adjust the electronic structures. XPS analysis, CO2 TPD and electrochemical experiments indicate that Co doping makes the electron densities around O anions increase, which could likely facilitate CO2 activation and electron transfer to CO2 molecules, while photoelectrochemical and photocatalytic oxygen evolution experiments demonstrate that Co doping could also promote water oxidation reactions. Further investigations by density functional theory calculation reveal that Co doping results in the generation of new defect levels above the Fermi level, inferring that a higher hole concentration is favorable for water oxidation, and the doped Co 3d orbits located at the top of valence bands might serve as active centers for water oxidation. As a result, Co-doped BiVO4 atomic layers achieve an efficient and stable CH4 production rate of 23.8 μmol g-1 h-1 under atmospheric CO2 concentration (400 ppm), which is about three times the activity of pristine BiVO4 atomic layers. This work might help to gain deeper insights into the design of CO2 photoreduction catalysts.

Original languageEnglish
Pages (from-to)3115-3122
Number of pages8
JournalCatalysis Science and Technology
Volume8
Issue number12
DOIs
Publication statusPublished - Jan 1 2018
Externally publishedYes

Fingerprint

Methane
Cobalt
Bismuth
Doping (additives)
Oxidation
Electronic structure
Water
Hole concentration
Temperature programmed desorption
Hydrocarbons
Valence bands
Fermi level
Conversion efficiency
Density functional theory
Anions
Carrier concentration
bismuth vanadium tetraoxide
Orbits
Negative ions
X ray photoelectron spectroscopy

All Science Journal Classification (ASJC) codes

  • Catalysis

Cite this

Boosted CO2 photoreduction to methane : Via Co doping in bismuth vanadate atomic layers. / Wang, Kefu; Zhang, Ling; Su, Yang; Sun, Songmei; Wang, Qianqian; Wang, Haipeng; Wang, Wenzhong.

In: Catalysis Science and Technology, Vol. 8, No. 12, 01.01.2018, p. 3115-3122.

Research output: Contribution to journalArticle

Wang, K, Zhang, L, Su, Y, Sun, S, Wang, Q, Wang, H & Wang, W 2018, 'Boosted CO2 photoreduction to methane: Via Co doping in bismuth vanadate atomic layers', Catalysis Science and Technology, vol. 8, no. 12, pp. 3115-3122. https://doi.org/10.1039/c8cy00513c
Wang, Kefu ; Zhang, Ling ; Su, Yang ; Sun, Songmei ; Wang, Qianqian ; Wang, Haipeng ; Wang, Wenzhong. / Boosted CO2 photoreduction to methane : Via Co doping in bismuth vanadate atomic layers. In: Catalysis Science and Technology. 2018 ; Vol. 8, No. 12. pp. 3115-3122.
@article{9642030de2d6493c903d2d2209326940,
title = "Boosted CO2 photoreduction to methane: Via Co doping in bismuth vanadate atomic layers",
abstract = "CO2 photoreduction to valuable hydrocarbons is attractive and promising. Nevertheless, the photoactivity has been pretty low to date, and deeper insights into improving CO2 conversion efficiency remain a challenge. Here, BiVO4 atomic layers have been synthesized as ideal platforms to investigate the correlation between the electronic structures and activities for CO2 photoreduction. Cobalt (Co) is then deliberately doped in BiVO4 atomic layers to adjust the electronic structures. XPS analysis, CO2 TPD and electrochemical experiments indicate that Co doping makes the electron densities around O anions increase, which could likely facilitate CO2 activation and electron transfer to CO2 molecules, while photoelectrochemical and photocatalytic oxygen evolution experiments demonstrate that Co doping could also promote water oxidation reactions. Further investigations by density functional theory calculation reveal that Co doping results in the generation of new defect levels above the Fermi level, inferring that a higher hole concentration is favorable for water oxidation, and the doped Co 3d orbits located at the top of valence bands might serve as active centers for water oxidation. As a result, Co-doped BiVO4 atomic layers achieve an efficient and stable CH4 production rate of 23.8 μmol g-1 h-1 under atmospheric CO2 concentration (400 ppm), which is about three times the activity of pristine BiVO4 atomic layers. This work might help to gain deeper insights into the design of CO2 photoreduction catalysts.",
author = "Kefu Wang and Ling Zhang and Yang Su and Songmei Sun and Qianqian Wang and Haipeng Wang and Wenzhong Wang",
year = "2018",
month = "1",
day = "1",
doi = "10.1039/c8cy00513c",
language = "English",
volume = "8",
pages = "3115--3122",
journal = "Catalysis Science and Technology",
issn = "2044-4753",
publisher = "Royal Society of Chemistry",
number = "12",

}

TY - JOUR

T1 - Boosted CO2 photoreduction to methane

T2 - Via Co doping in bismuth vanadate atomic layers

AU - Wang, Kefu

AU - Zhang, Ling

AU - Su, Yang

AU - Sun, Songmei

AU - Wang, Qianqian

AU - Wang, Haipeng

AU - Wang, Wenzhong

PY - 2018/1/1

Y1 - 2018/1/1

N2 - CO2 photoreduction to valuable hydrocarbons is attractive and promising. Nevertheless, the photoactivity has been pretty low to date, and deeper insights into improving CO2 conversion efficiency remain a challenge. Here, BiVO4 atomic layers have been synthesized as ideal platforms to investigate the correlation between the electronic structures and activities for CO2 photoreduction. Cobalt (Co) is then deliberately doped in BiVO4 atomic layers to adjust the electronic structures. XPS analysis, CO2 TPD and electrochemical experiments indicate that Co doping makes the electron densities around O anions increase, which could likely facilitate CO2 activation and electron transfer to CO2 molecules, while photoelectrochemical and photocatalytic oxygen evolution experiments demonstrate that Co doping could also promote water oxidation reactions. Further investigations by density functional theory calculation reveal that Co doping results in the generation of new defect levels above the Fermi level, inferring that a higher hole concentration is favorable for water oxidation, and the doped Co 3d orbits located at the top of valence bands might serve as active centers for water oxidation. As a result, Co-doped BiVO4 atomic layers achieve an efficient and stable CH4 production rate of 23.8 μmol g-1 h-1 under atmospheric CO2 concentration (400 ppm), which is about three times the activity of pristine BiVO4 atomic layers. This work might help to gain deeper insights into the design of CO2 photoreduction catalysts.

AB - CO2 photoreduction to valuable hydrocarbons is attractive and promising. Nevertheless, the photoactivity has been pretty low to date, and deeper insights into improving CO2 conversion efficiency remain a challenge. Here, BiVO4 atomic layers have been synthesized as ideal platforms to investigate the correlation between the electronic structures and activities for CO2 photoreduction. Cobalt (Co) is then deliberately doped in BiVO4 atomic layers to adjust the electronic structures. XPS analysis, CO2 TPD and electrochemical experiments indicate that Co doping makes the electron densities around O anions increase, which could likely facilitate CO2 activation and electron transfer to CO2 molecules, while photoelectrochemical and photocatalytic oxygen evolution experiments demonstrate that Co doping could also promote water oxidation reactions. Further investigations by density functional theory calculation reveal that Co doping results in the generation of new defect levels above the Fermi level, inferring that a higher hole concentration is favorable for water oxidation, and the doped Co 3d orbits located at the top of valence bands might serve as active centers for water oxidation. As a result, Co-doped BiVO4 atomic layers achieve an efficient and stable CH4 production rate of 23.8 μmol g-1 h-1 under atmospheric CO2 concentration (400 ppm), which is about three times the activity of pristine BiVO4 atomic layers. This work might help to gain deeper insights into the design of CO2 photoreduction catalysts.

UR - http://www.scopus.com/inward/record.url?scp=85049031856&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85049031856&partnerID=8YFLogxK

U2 - 10.1039/c8cy00513c

DO - 10.1039/c8cy00513c

M3 - Article

AN - SCOPUS:85049031856

VL - 8

SP - 3115

EP - 3122

JO - Catalysis Science and Technology

JF - Catalysis Science and Technology

SN - 2044-4753

IS - 12

ER -