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

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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

General Materials Science

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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

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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 = "Publisher Copyright: Copyright {\textcopyright} 2020 American Chemical Society.",

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month = feb,

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doi = "10.1021/acsami.9b18924",

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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.

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

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