Heterogenized Pyridine-Substituted Cobalt(II) Phthalocyanine Yields Reduction of CO2 by Tuning the Electron Affinity of the Co Center

Alberto De Riccardis; Michelle Lee; Roman V. Kazantsev; Alejandro J. Garza; Guosong Zeng; David M. Larson; Ezra L. Clark; Peter Lobaccaro; Paul W.W. Burroughs; Ermelinda Bloise; Joel W. Ager; Alexis T. Bell; Martin Head-Gordon; Giuseppe Mele; Francesca M. Toma

doi:10.1021/acsami.9b18924

Heterogenized Pyridine-Substituted Cobalt(II) Phthalocyanine Yields Reduction of CO₂ by Tuning the Electron Affinity of the Co Center

Alberto De Riccardis, Michelle Lee, Roman V. Kazantsev, Alejandro J. Garza, Guosong Zeng, David M. Larson, Ezra L. Clark, Peter Lobaccaro, Paul W.W. Burroughs, Ermelinda Bloise, Joel W. Ager, Alexis T. Bell, Martin Head-Gordon, Giuseppe Mele, Francesca M. Toma

Chemical Engineering

Research output: Contribution to journal › Review article › peer-review

27 Scopus citations

Abstract

Conversion of CO₂ to reduced products is a promising route to alleviate irreversible climate change. Here we report the synthesis of a Co-based phthalocyanine with pyridine moieties (CoPc-Pyr), which is supported on a carbon electrode and shows Faradaic efficiency ?90% for CO at 490 mV of overpotential (-0.6 V vs reversible hydrogen electrode (RHE)). In addition, its catalytic activity at -0.7 V versus RHE surpasses other Co-based molecular and metal-organic framework catalysts for CO₂ reduction at this bias. Density functional theory calculations show that pyridine moieties enhance CO₂ adsorption and electron affinity of the Co center by an inductive effect, thus lowering the overpotential necessary for CO₂ conversion. Our study shows that CoPc-Pyr reduces CO₂ at lower overpotential and with higher activity than noble metal electrodes, such as silver.

Original language	English (US)
Pages (from-to)	5251-5258
Number of pages	8
Journal	ACS Applied Materials and Interfaces
Volume	12
Issue number	5
DOIs	https://doi.org/10.1021/acsami.9b18924
State	Published - Feb 5 2020

All Science Journal Classification (ASJC) codes

Materials Science(all)

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De Riccardis, A., Lee, M., Kazantsev, R. V., Garza, A. J., Zeng, G., Larson, D. M., Clark, E. L., Lobaccaro, P., Burroughs, P. W. W., Bloise, E., Ager, J. W., Bell, A. T., Head-Gordon, M., Mele, G., & Toma, F. M. (2020). Heterogenized Pyridine-Substituted Cobalt(II) Phthalocyanine Yields Reduction of CO₂ by Tuning the Electron Affinity of the Co Center. ACS Applied Materials and Interfaces, 12(5), 5251-5258. https://doi.org/10.1021/acsami.9b18924

@article{4abe737bb6064b969f3d62771e179374,

title = "Heterogenized Pyridine-Substituted Cobalt(II) Phthalocyanine Yields Reduction of CO2 by Tuning the Electron Affinity of the Co Center",

abstract = "Conversion of CO2 to reduced products is a promising route to alleviate irreversible climate change. Here we report the synthesis of a Co-based phthalocyanine with pyridine moieties (CoPc-Pyr), which is supported on a carbon electrode and shows Faradaic efficiency ?90% for CO at 490 mV of overpotential (-0.6 V vs reversible hydrogen electrode (RHE)). In addition, its catalytic activity at -0.7 V versus RHE surpasses other Co-based molecular and metal-organic framework catalysts for CO2 reduction at this bias. Density functional theory calculations show that pyridine moieties enhance CO2 adsorption and electron affinity of the Co center by an inductive effect, thus lowering the overpotential necessary for CO2 conversion. Our study shows that CoPc-Pyr reduces CO2 at lower overpotential and with higher activity than noble metal electrodes, such as silver.",

author = "{De Riccardis}, Alberto and Michelle Lee and Kazantsev, {Roman V.} and Garza, {Alejandro J.} and Guosong Zeng and Larson, {David M.} and Clark, {Ezra L.} and Peter Lobaccaro and Burroughs, {Paul W.W.} and Ermelinda Bloise and Ager, {Joel W.} and Bell, {Alexis T.} and Martin Head-Gordon and Giuseppe Mele and Toma, {Francesca M.}",

note = "Funding Information: This material is based on work performed at the Joint Center for Artificial Photosynthesis, a Department of Energy (DOE) Energy Innovation Hub, supported through the Office of Science of the U.S. DOE under Award No. DE-SC00004993. The computational work presented here used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. DOE under Contract No. DE-AC02-05CH11231. Publisher Copyright: Copyright {\textcopyright} 2020 American Chemical Society.",

year = "2020",

month = feb,

day = "5",

doi = "10.1021/acsami.9b18924",

language = "English (US)",

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De Riccardis, A, Lee, M, Kazantsev, RV, Garza, AJ, Zeng, G, Larson, DM, Clark, EL, Lobaccaro, P, Burroughs, PWW, Bloise, E, Ager, JW, Bell, AT, Head-Gordon, M, Mele, G & Toma, FM 2020, 'Heterogenized Pyridine-Substituted Cobalt(II) Phthalocyanine Yields Reduction of CO₂ by Tuning the Electron Affinity of the Co Center', ACS Applied Materials and Interfaces, vol. 12, no. 5, pp. 5251-5258. https://doi.org/10.1021/acsami.9b18924

TY - JOUR

T1 - Heterogenized Pyridine-Substituted Cobalt(II) Phthalocyanine Yields Reduction of CO2 by Tuning the Electron Affinity of the Co Center

AU - De Riccardis, Alberto

AU - Lee, Michelle

AU - Kazantsev, Roman V.

AU - Garza, Alejandro J.

AU - Zeng, Guosong

AU - Larson, David M.

AU - Clark, Ezra L.

AU - Lobaccaro, Peter

AU - Burroughs, Paul W.W.

AU - Bloise, Ermelinda

AU - Ager, Joel W.

AU - Bell, Alexis T.

AU - Head-Gordon, Martin

AU - Mele, Giuseppe

AU - Toma, Francesca M.

N1 - Funding Information: This material is based on work performed at the Joint Center for Artificial Photosynthesis, a Department of Energy (DOE) Energy Innovation Hub, supported through the Office of Science of the U.S. DOE under Award No. DE-SC00004993. The computational work presented here used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. DOE under Contract No. DE-AC02-05CH11231. Publisher Copyright: Copyright © 2020 American Chemical Society.

PY - 2020/2/5

Y1 - 2020/2/5

N2 - Conversion of CO2 to reduced products is a promising route to alleviate irreversible climate change. Here we report the synthesis of a Co-based phthalocyanine with pyridine moieties (CoPc-Pyr), which is supported on a carbon electrode and shows Faradaic efficiency ?90% for CO at 490 mV of overpotential (-0.6 V vs reversible hydrogen electrode (RHE)). In addition, its catalytic activity at -0.7 V versus RHE surpasses other Co-based molecular and metal-organic framework catalysts for CO2 reduction at this bias. Density functional theory calculations show that pyridine moieties enhance CO2 adsorption and electron affinity of the Co center by an inductive effect, thus lowering the overpotential necessary for CO2 conversion. Our study shows that CoPc-Pyr reduces CO2 at lower overpotential and with higher activity than noble metal electrodes, such as silver.

AB - Conversion of CO2 to reduced products is a promising route to alleviate irreversible climate change. Here we report the synthesis of a Co-based phthalocyanine with pyridine moieties (CoPc-Pyr), which is supported on a carbon electrode and shows Faradaic efficiency ?90% for CO at 490 mV of overpotential (-0.6 V vs reversible hydrogen electrode (RHE)). In addition, its catalytic activity at -0.7 V versus RHE surpasses other Co-based molecular and metal-organic framework catalysts for CO2 reduction at this bias. Density functional theory calculations show that pyridine moieties enhance CO2 adsorption and electron affinity of the Co center by an inductive effect, thus lowering the overpotential necessary for CO2 conversion. Our study shows that CoPc-Pyr reduces CO2 at lower overpotential and with higher activity than noble metal electrodes, such as silver.

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U2 - 10.1021/acsami.9b18924

DO - 10.1021/acsami.9b18924

M3 - Review article

C2 - 31971360

AN - SCOPUS:85078883486

SN - 1944-8244

VL - 12

SP - 5251

EP - 5258

JO - ACS applied materials & interfaces

JF - ACS applied materials & interfaces

IS - 5

ER -

Heterogenized Pyridine-Substituted Cobalt(II) Phthalocyanine Yields Reduction of CO₂ by Tuning the Electron Affinity of the Co Center

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