Aqueous Photoelectrochemical CO 2 Reduction to CO and Methanol over a Silicon Photocathode Functionalized with a Cobalt Phthalocyanine Molecular Catalyst

Shang, Bo; Rooney, Conor L.; Gallagher, David J.; Wang, Bernie T.; Krayev, Andrey; Shema, Hadar; Leitner, Oliver; Harmon, Nia J.; Xiao, Langqiu; Sheehan, Colton; Bottum, Samuel R.; Gross, Elad; Cahoon, James F.; Mallouk, Thomas E.; Wang, Hailiang

doi:10.1002/ange.202215213

Title: Aqueous Photoelectrochemical CO ₂ Reduction to CO and Methanol over a Silicon Photocathode Functionalized with a Cobalt Phthalocyanine Molecular Catalyst

Abstract

Abstract We report a precious‐metal‐free molecular catalyst‐based photocathode that is active for aqueous CO ₂ reduction to CO and methanol. The photoelectrode is composed of cobalt phthalocyanine molecules anchored on graphene oxide which is integrated via a (3‐aminopropyl)triethoxysilane linker to p‐type silicon protected by a thin film of titanium dioxide. The photocathode reduces CO ₂ to CO with high selectivity at potentials as mild as 0 V versus the reversible hydrogen electrode (vs RHE). Methanol production is observed at an onset potential of −0.36 V vs RHE, and reaches a peak turnover frequency of 0.18 s ⁻¹ . To date, this is the only molecular catalyst‐based photoelectrode that is active for the six‐electron reduction of CO ₂ to methanol. This work puts forth a strategy for interfacing molecular catalysts to p‐type semiconductors and demonstrates state‐of‐the‐art performance for photoelectrochemical CO ₂ reduction to CO and methanol.

Authors:

Shang, Bo ^[1]; Rooney, Conor L. ^[1]; Gallagher, David J. ^[1]; Wang, Bernie T. ^[1]; Krayev, Andrey ^[2]; Shema, Hadar ^[3]; Leitner, Oliver ^[1]; Harmon, Nia J. ^[1]; Xiao, Langqiu ^[4]; Sheehan, Colton ^[4]; Bottum, Samuel R. ^[5]; Gross, Elad ^[3]; Cahoon, James F. ^[5]; Mallouk, Thomas E. ^[4];

^[1]

Department of Chemistry Yale University New Haven CT 06520 USA, Energy Sciences Institute Yale University West Haven CT 06516 USA
HORIBA Instruments Inc. 359 Bel Marin Keys Blvd, Suite 18 Novato CA 94949 USA
Institute of Chemistry and Center for Nanoscience and Nanotechnology Hebrew University of Jerusalem Jerusalem 91904 Israel
Department of Chemistry University of Pennsylvania Philadelphia PA 19104 USA
Department of Chemistry University of North Carolina at Chapel Hill Chapel Hill NC 27599-3290 USA

Publication Date:: Tue Dec 20 00:00:00 EST 2022

Sponsoring Org.:: USDOE

OSTI Identifier:: 1905917

Grant/Contract Number:: SC0021173

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Angewandte Chemie

Additional Journal Information:: Journal Name: Angewandte Chemie Journal Volume: 135 Journal Issue: 4; Journal ID: ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Shang, Bo, Rooney, Conor L., Gallagher, David J., Wang, Bernie T., Krayev, Andrey, Shema, Hadar, Leitner, Oliver, Harmon, Nia J., Xiao, Langqiu, Sheehan, Colton, Bottum, Samuel R., Gross, Elad, Cahoon, James F., Mallouk, Thomas E., and Wang, Hailiang. Aqueous Photoelectrochemical CO 2 Reduction to CO and Methanol over a Silicon Photocathode Functionalized with a Cobalt Phthalocyanine Molecular Catalyst.  Germany: N. p., 2022. 
Web.  doi:10.1002/ange.202215213.

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                    Shang, Bo, Rooney, Conor L., Gallagher, David J., Wang, Bernie T., Krayev, Andrey, Shema, Hadar, Leitner, Oliver, Harmon, Nia J., Xiao, Langqiu, Sheehan, Colton, Bottum, Samuel R., Gross, Elad, Cahoon, James F., Mallouk, Thomas E., & Wang, Hailiang. Aqueous Photoelectrochemical CO 2 Reduction to CO and Methanol over a Silicon Photocathode Functionalized with a Cobalt Phthalocyanine Molecular Catalyst.  Germany.  https://doi.org/10.1002/ange.202215213

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                    Shang, Bo, Rooney, Conor L., Gallagher, David J., Wang, Bernie T., Krayev, Andrey, Shema, Hadar, Leitner, Oliver, Harmon, Nia J., Xiao, Langqiu, Sheehan, Colton, Bottum, Samuel R., Gross, Elad, Cahoon, James F., Mallouk, Thomas E., and Wang, Hailiang. Tue .  
"Aqueous Photoelectrochemical CO 2 Reduction to CO and Methanol over a Silicon Photocathode Functionalized with a Cobalt Phthalocyanine Molecular Catalyst".  Germany.  https://doi.org/10.1002/ange.202215213.

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@article{osti_1905917,

  title        = {Aqueous Photoelectrochemical CO 2 Reduction to CO and Methanol over a Silicon Photocathode Functionalized with a Cobalt Phthalocyanine Molecular Catalyst},

  author       = {Shang, Bo and Rooney, Conor L. and Gallagher, David J. and Wang, Bernie T. and Krayev, Andrey and Shema, Hadar and Leitner, Oliver and Harmon, Nia J. and Xiao, Langqiu and Sheehan, Colton and Bottum, Samuel R. and Gross, Elad and Cahoon, James F. and Mallouk, Thomas E. and Wang, Hailiang},

  abstractNote = {Abstract We report a precious‐metal‐free molecular catalyst‐based photocathode that is active for aqueous CO 2 reduction to CO and methanol. The photoelectrode is composed of cobalt phthalocyanine molecules anchored on graphene oxide which is integrated via a (3‐aminopropyl)triethoxysilane linker to p‐type silicon protected by a thin film of titanium dioxide. The photocathode reduces CO 2 to CO with high selectivity at potentials as mild as 0 V versus the reversible hydrogen electrode (vs RHE). Methanol production is observed at an onset potential of −0.36 V vs RHE, and reaches a peak turnover frequency of 0.18 s −1 . To date, this is the only molecular catalyst‐based photoelectrode that is active for the six‐electron reduction of CO 2 to methanol. This work puts forth a strategy for interfacing molecular catalysts to p‐type semiconductors and demonstrates state‐of‐the‐art performance for photoelectrochemical CO 2 reduction to CO and methanol.},

  doi          = {10.1002/ange.202215213},

  journal      = {Angewandte Chemie},

  number       = 4,

  volume       = 135,

  place        = {Germany},

  year         = {Tue Dec 20 00:00:00 EST 2022},

  month        = {Tue Dec 20 00:00:00 EST 2022}

}

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Title: Aqueous Photoelectrochemical CO 2 Reduction to CO and Methanol over a Silicon Photocathode Functionalized with a Cobalt Phthalocyanine Molecular Catalyst

Abstract

Citation Formats

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Title: Aqueous Photoelectrochemical CO ₂ Reduction to CO and Methanol over a Silicon Photocathode Functionalized with a Cobalt Phthalocyanine Molecular Catalyst

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