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Title: Selective CO Production by Photoelectrochemical Methane Oxidation on TiO2

Abstract

The inertness of the C–H bond in CH4 poses significant challenges to selective CH4 oxidation, which often proceeds all the way to CO2 once activated. Selective oxidation of CH4 to high-value industrial chemicals such as CO or CH3OH remains a challenge. Presently, the main methods to activate CH4 oxidation include thermochemical, electrochemical, and photocatalytic reactions. Of them, photocatalytic reactions hold great promise for practical applications but have been poorly studied. Existing demonstrations of photocatalytic CH4 oxidation exhibit limited control over the product selectivity, with CO2 as the most common product. The yield of CO or other hydrocarbons is too low to be of any practical value. In this work, we show that highly selective production of CO by CH4 oxidation can be achieved by a photoelectrochemical (PEC) approach. Under our experimental conditions, the highest yield for CO production was 81.9%. The substrate we used was TiO2 grown by atomic layer deposition (ALD), which features high concentrations of Ti3+ species. The selectivity toward CO was found to be highly sensitive to the substrate types, with significantly lower yield on P25 or commercial anatase TiO2 substrates. Moreover, our results revealed that the selectivity toward CO also depends on the applied potentials. Basedmore » on the experimental results, we proposed a reaction mechanism that involves synergistic effects by adjacent Ti sites on TiO2. Spectroscopic characterization and computational studies provide critical evidence to support the mechanism. Furthermore, the synergistic effect was found to parallel heterogeneous CO2 reduction mechanisms. Our results not only present a new route to selective CH4 oxidation, but also highlight the importance of mechanistic understandings in advancing heterogeneous catalysis.« less

Authors:
 [1];  [1];  [2]; ORCiD logo [1];  [3]; ORCiD logo [1];  [3]; ORCiD logo [1];  [1]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Boston College, Chestnut Hill, MA (United States)
  2. Univ. of California, Riverside, CA (United States)
  3. Yale Univ., New Haven, CT (United States)
Publication Date:
Research Org.:
Yale Univ., New Haven, CT (United States); Univ. of California, Riverside, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1498722
Grant/Contract Number:  
FG02-05ER15646; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
ACS Central Science
Additional Journal Information:
Journal Volume: 4; Journal Issue: 5; Journal ID: ISSN 2374-7943
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Li, Wei, He, Da, Hu, Guoxiang, Li, Xiang, Banerjee, Gourab, Li, Jingyi, Lee, Shin Hee, Dong, Qi, Gao, Tianyue, Brudvig, Gary W., Waegele, Matthias M., Jiang, De-en, and Wang, Dunwei. Selective CO Production by Photoelectrochemical Methane Oxidation on TiO2. United States: N. p., 2018. Web. doi:10.1021/acscentsci.8b00130.
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Li, Wei, He, Da, Hu, Guoxiang, Li, Xiang, Banerjee, Gourab, Li, Jingyi, Lee, Shin Hee, Dong, Qi, Gao, Tianyue, Brudvig, Gary W., Waegele, Matthias M., Jiang, De-en, & Wang, Dunwei. Selective CO Production by Photoelectrochemical Methane Oxidation on TiO2. United States. https://doi.org/10.1021/acscentsci.8b00130
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Li, Wei, He, Da, Hu, Guoxiang, Li, Xiang, Banerjee, Gourab, Li, Jingyi, Lee, Shin Hee, Dong, Qi, Gao, Tianyue, Brudvig, Gary W., Waegele, Matthias M., Jiang, De-en, and Wang, Dunwei. Mon . "Selective CO Production by Photoelectrochemical Methane Oxidation on TiO2". United States. https://doi.org/10.1021/acscentsci.8b00130. https://www.osti.gov/servlets/purl/1498722.
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@article{osti_1498722,
title = {Selective CO Production by Photoelectrochemical Methane Oxidation on TiO2},
author = {Li, Wei and He, Da and Hu, Guoxiang and Li, Xiang and Banerjee, Gourab and Li, Jingyi and Lee, Shin Hee and Dong, Qi and Gao, Tianyue and Brudvig, Gary W. and Waegele, Matthias M. and Jiang, De-en and Wang, Dunwei},
abstractNote = {The inertness of the C–H bond in CH4 poses significant challenges to selective CH4 oxidation, which often proceeds all the way to CO2 once activated. Selective oxidation of CH4 to high-value industrial chemicals such as CO or CH3OH remains a challenge. Presently, the main methods to activate CH4 oxidation include thermochemical, electrochemical, and photocatalytic reactions. Of them, photocatalytic reactions hold great promise for practical applications but have been poorly studied. Existing demonstrations of photocatalytic CH4 oxidation exhibit limited control over the product selectivity, with CO2 as the most common product. The yield of CO or other hydrocarbons is too low to be of any practical value. In this work, we show that highly selective production of CO by CH4 oxidation can be achieved by a photoelectrochemical (PEC) approach. Under our experimental conditions, the highest yield for CO production was 81.9%. The substrate we used was TiO2 grown by atomic layer deposition (ALD), which features high concentrations of Ti3+ species. The selectivity toward CO was found to be highly sensitive to the substrate types, with significantly lower yield on P25 or commercial anatase TiO2 substrates. Moreover, our results revealed that the selectivity toward CO also depends on the applied potentials. Based on the experimental results, we proposed a reaction mechanism that involves synergistic effects by adjacent Ti sites on TiO2. Spectroscopic characterization and computational studies provide critical evidence to support the mechanism. Furthermore, the synergistic effect was found to parallel heterogeneous CO2 reduction mechanisms. Our results not only present a new route to selective CH4 oxidation, but also highlight the importance of mechanistic understandings in advancing heterogeneous catalysis.},
doi = {10.1021/acscentsci.8b00130},
journal = {ACS Central Science},
number = 5,
volume = 4,
place = {United States},
year = {Mon Apr 23 00:00:00 EDT 2018},
month = {Mon Apr 23 00:00:00 EDT 2018}
}
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https://doi.org/10.1021/acscentsci.8b00130
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Figures / Tables:

Figure 1 Figure 1: (a) Schematic illustration of selective CH4 oxidation to CO on a TiO2 photoelectrode, starting with charge separation between O2− and Ti4+ to produce −•O−Ti3+ upon illumination. The separation of the redox half reactions permitted us to focus on CH4 oxidation. (b) Dependence of the CO efficiency and selectivitymore » on the applied potentials (left axis, efficiency, %; right axis, selectivity of CO over all carbonaceous products, %). PEC bulk electrolysis was conducted on ALD TiO2 in CH4-saturated 1.0 M NaOH electrolyte at the corresponding applied potentials.« less
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Heterogeneous Catalysis: Understanding for Designing, and Designing for Applications
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Formaldehyde Oxidation over Ag Catalysts
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Role of Ti3+ in CS2 conversion over TiO2 Claus catalyst
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Heterogeneous Catalysis: A Central Science for a Sustainable Future
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Catalytic Reforming of Oxygenates: State of the Art and Future Prospects
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Direct Conversion of Methane to Value-Added Chemicals over Heterogeneous Catalysts: Challenges and Prospects
journal, March 2017

Probing the Interfacial Chemistry of Ultrathin ALD-Grown TiO 2 Films: An In-Line XPS Study
journal, March 2017

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Catalytic Methane Monofunctionalization by an Electrogenerated High-Valent Pd Intermediate
journal, October 2017

Raman Spectroscopic Investigation of CH4 and N2 Adsorption in Metal−Organic Frameworks
journal, July 2007

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Photocatalysis on TiO2 Surfaces: Principles, Mechanisms, and Selected Results
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journal, September 2012

  • Shimura, Katsuya; Kawai, Hiromasa; Yoshida, Tomoko
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Selective Heterogeneous CO 2 Electroreduction to Methanol
journal, January 2015

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Electrochemically assisted photocatalysis: titania particulate film electrodes for photocatalytic degradation of 4-chlorophenol
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journal, June 2012

  • Schouten, Klaas Jan P.; Qin, Zisheng; Pérez Gallent, Elena
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TiO 2 /TiSi 2 Heterostructures for High-Efficiency Photoelectrochemical H 2 O Splitting
journal, March 2009

  • Lin, Yongjing; Zhou, Sa; Liu, Xiaohua
  • Journal of the American Chemical Society, Vol. 131, Issue 8
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Solubility of CCl2F2, CClF3, CF4, and CH4 in Water and Seawater at 288.15-303.15 K and 101.325 kPa
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Light-Induced Charge Separation in Anatase TiO 2 Particles
journal, April 2005

  • Berger, T.; Sterrer, M.; Diwald, O.
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Hydrogen Production from Methane and Water on Platinum Loaded Titanium Oxide Photocatalysts
journal, March 2008

  • Yoshida, Hisao; Hirao, Kazuhisa; Nishimoto, Jun-ichi
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Understanding Methane Adsorption in Porous Aromatic Frameworks: An FTIR, Raman, and Theoretical Combined Study
journal, May 2014

  • Errahali, M.; Gatti, G.; Tei, L.
  • The Journal of Physical Chemistry C, Vol. 118, Issue 19
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Acid–Base Interaction and Its Role in Alkane Dissociative Chemisorption on Oxide Surfaces
journal, November 2014

  • Chrétien, Steeve; Metiu, Horia
  • The Journal of Physical Chemistry C, Vol. 118, Issue 47
  • DOI: 10.1021/jp507207b

Photocatalytic Steam Reforming of Methane over Sodium Tantalate
journal, February 2010

  • Shimura, Katsuya; Kato, Satoru; Yoshida, Tomoko
  • The Journal of Physical Chemistry C, Vol. 114, Issue 8
  • DOI: 10.1021/jp902761x

Photocatalytic oxidation of methane over silver decorated zinc oxide nanocatalysts
journal, July 2016

  • Chen, Xuxing; Li, Yunpeng; Pan, Xiaoyang
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms12273

Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction
journal, January 2018

Construction of Pd-Zn dual sites to enhance the performance for ethanol electro-oxidation reaction
journal, September 2021

Photocatalytic conversion of methane
journal, January 2008

  • Yuliati, Leny; Yoshida, Hisao
  • Chemical Society Reviews, Vol. 37, Issue 8
  • DOI: 10.1039/b710575b

Simultaneously photodeposited rhodium metal and oxide nanoparticles promoting photocatalytic hydrogen production
journal, January 2011

  • Shimura, Katsuya; Kawai, Hiromasa; Yoshida, Tomoko
  • Chemical Communications, Vol. 47, Issue 31
  • DOI: 10.1039/c1cc12287h

Renewable energy based catalytic CH4 conversion to fuels
journal, January 2014

  • Baltrusaitis, J.; Jansen, I.; Schuttlefield Christus, J. D.
  • Catalysis Science & Technology, Vol. 4, Issue 8
  • DOI: 10.1039/c4cy00294f

Active sites for CO 2 hydrogenation to methanol on Cu/ZnO catalysts
journal, March 2017

Selective anaerobic oxidation of methane enables direct synthesis of methanol
journal, May 2017

  • Sushkevich, Vitaly L.; Palagin, Dennis; Ranocchiari, Marco
  • Science, Vol. 356, Issue 6337
  • DOI: 10.1126/science.aam9035

Aqueous Au-Pd colloids catalyze selective CH 4 oxidation to CH 3 OH with O 2 under mild conditions
journal, September 2017

  • Agarwal, Nishtha; Freakley, Simon J.; McVicker, Rebecca U.
  • Science, Vol. 358, Issue 6360
  • DOI: 10.1126/science.aan6515

Electrochemical Methane Activation and Conversion to Oxygenates at Room Temperature
journal, October 2013

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    Atomically Thin 2D Transition Metal Oxides: Structural Reconstruction, Interaction with Substrates, and Potential Applications
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