Energy efficient electrochemical reduction of CO                         2                          to CO using a three-dimensional porphyrin/graphene hydrogel

Jaecheol Choi; Jeonghun Kim; Pawel Wagner; Sanjeev Gambhir; Rouhollah Jalili; Seoungwoo Byun; Sepidar Sayyar; Yong Min Lee; Douglas R. MacFarlane; Gordon G. Wallace; David L. Officer

doi:10.1039/c8ee03403f

Energy efficient electrochemical reduction of CO ₂ to CO using a three-dimensional porphyrin/graphene hydrogel

Jaecheol Choi, Jeonghun Kim, Pawel Wagner, Sanjeev Gambhir, Rouhollah Jalili, Seoungwoo Byun, Sepidar Sayyar, Yong Min Lee, Douglas R. MacFarlane, Gordon G. Wallace, David L. Officer

Department of Chemical and Biomolecular Engineering

Research output: Contribution to journal › Article › peer-review

94 Citations (Scopus)

Abstract

Although electrochemical CO ₂ reduction is one of the most promising ways to convert atmospheric CO ₂ into value-added chemicals, there are still numerous limitations to overcome to achieve highly efficient CO ₂ conversion performance. Herein, we report for the first time the development and use of a three-dimensional iron porphyrin-based graphene hydrogel (FePGH) as an electrocatalyst for extremely efficient robust CO ₂ reduction to CO. Electrocatalytic CO ₂ conversion was performed in aqueous medium with FePGH, which has a highly porous and conductive 3D graphene structure, resulting in high catalytic activity for CO production with ∼96.2% faradaic efficiency at a very low overpotential of 280 mV. Furthermore, FePGH showed considerable catalytic durability maintaining a consistent CO yield (96.4% FE) over 20 h electrolysis at the same overpotential, corresponding to the highest cathodic energy efficiency yet observed of 79.7% compared to other state-of-the-art immobilised metal complex electrocatalysts. This approach to fabricating a 3D graphene-based hydrogel electrocatalyst should provide an exciting new avenue for the development of other kinds of molecular electrocatalysts.

Original language	English
Pages (from-to)	747-755
Number of pages	9
Journal	Energy and Environmental Science
Volume	12
Issue number	2
DOIs	https://doi.org/10.1039/c8ee03403f
Publication status	Published - 2019 Feb

Bibliographical note

Funding Information:
This work was supported by the ARC Centre of Excellence Scheme (Project Number CE 140100012). JC also thanks the University of Wollongong (UOW) for a University Postgraduate Award. DRM is grateful for support from the Australian Research Council for his Australian Laureate Fellowship (Grant Number FL120100019). The authors thank Dr Patricia Hayes for assistance with Raman spectroscopy, and the Materials Node of the Australian National Fabrication Facility (ANFF) and the UOW Electron Microscopy Centre for their facilities and research support.

Publisher Copyright:
© 2019 The Royal Society of Chemistry.

All Science Journal Classification (ASJC) codes

Environmental Chemistry
Renewable Energy, Sustainability and the Environment
Nuclear Energy and Engineering
Pollution

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1039/c8ee03403f

Cite this

Choi, J., Kim, J., Wagner, P., Gambhir, S., Jalili, R., Byun, S., Sayyar, S., Lee, Y. M., MacFarlane, D. R., Wallace, G. G., & Officer, D. L. (2019). Energy efficient electrochemical reduction of CO ₂ to CO using a three-dimensional porphyrin/graphene hydrogel Energy and Environmental Science, 12(2), 747-755. https://doi.org/10.1039/c8ee03403f

@article{e27b06e2b8fc465a81e65ef7a3d3b17b,

title = " Energy efficient electrochemical reduction of CO 2 to CO using a three-dimensional porphyrin/graphene hydrogel ",

abstract = " Although electrochemical CO 2 reduction is one of the most promising ways to convert atmospheric CO 2 into value-added chemicals, there are still numerous limitations to overcome to achieve highly efficient CO 2 conversion performance. Herein, we report for the first time the development and use of a three-dimensional iron porphyrin-based graphene hydrogel (FePGH) as an electrocatalyst for extremely efficient robust CO 2 reduction to CO. Electrocatalytic CO 2 conversion was performed in aqueous medium with FePGH, which has a highly porous and conductive 3D graphene structure, resulting in high catalytic activity for CO production with ∼96.2% faradaic efficiency at a very low overpotential of 280 mV. Furthermore, FePGH showed considerable catalytic durability maintaining a consistent CO yield (96.4% FE) over 20 h electrolysis at the same overpotential, corresponding to the highest cathodic energy efficiency yet observed of 79.7% compared to other state-of-the-art immobilised metal complex electrocatalysts. This approach to fabricating a 3D graphene-based hydrogel electrocatalyst should provide an exciting new avenue for the development of other kinds of molecular electrocatalysts.",

author = "Jaecheol Choi and Jeonghun Kim and Pawel Wagner and Sanjeev Gambhir and Rouhollah Jalili and Seoungwoo Byun and Sepidar Sayyar and Lee, {Yong Min} and MacFarlane, {Douglas R.} and Wallace, {Gordon G.} and Officer, {David L.}",

note = "Funding Information: This work was supported by the ARC Centre of Excellence Scheme (Project Number CE 140100012). JC also thanks the University of Wollongong (UOW) for a University Postgraduate Award. DRM is grateful for support from the Australian Research Council for his Australian Laureate Fellowship (Grant Number FL120100019). The authors thank Dr Patricia Hayes for assistance with Raman spectroscopy, and the Materials Node of the Australian National Fabrication Facility (ANFF) and the UOW Electron Microscopy Centre for their facilities and research support. Publisher Copyright: {\textcopyright} 2019 The Royal Society of Chemistry.",

year = "2019",

month = feb,

doi = "10.1039/c8ee03403f",

language = "English",

volume = "12",

pages = "747--755",

journal = "Energy and Environmental Science",

issn = "1754-5692",

publisher = "Royal Society of Chemistry",

number = "2",

}

Choi, J, Kim, J, Wagner, P, Gambhir, S, Jalili, R, Byun, S, Sayyar, S, Lee, YM, MacFarlane, DR, Wallace, GG & Officer, DL 2019, ' Energy efficient electrochemical reduction of CO ₂ to CO using a three-dimensional porphyrin/graphene hydrogel ', Energy and Environmental Science, vol. 12, no. 2, pp. 747-755. https://doi.org/10.1039/c8ee03403f

Energy efficient electrochemical reduction of CO ₂ to CO using a three-dimensional porphyrin/graphene hydrogel . / Choi, Jaecheol; Kim, Jeonghun; Wagner, Pawel et al.

In: Energy and Environmental Science, Vol. 12, No. 2, 02.2019, p. 747-755.

Research output: Contribution to journal › Article › peer-review

TY - JOUR

T1 - Energy efficient electrochemical reduction of CO 2 to CO using a three-dimensional porphyrin/graphene hydrogel

AU - Choi, Jaecheol

AU - Kim, Jeonghun

AU - Wagner, Pawel

AU - Gambhir, Sanjeev

AU - Jalili, Rouhollah

AU - Byun, Seoungwoo

AU - Sayyar, Sepidar

AU - Lee, Yong Min

AU - MacFarlane, Douglas R.

AU - Wallace, Gordon G.

AU - Officer, David L.

N1 - Funding Information: This work was supported by the ARC Centre of Excellence Scheme (Project Number CE 140100012). JC also thanks the University of Wollongong (UOW) for a University Postgraduate Award. DRM is grateful for support from the Australian Research Council for his Australian Laureate Fellowship (Grant Number FL120100019). The authors thank Dr Patricia Hayes for assistance with Raman spectroscopy, and the Materials Node of the Australian National Fabrication Facility (ANFF) and the UOW Electron Microscopy Centre for their facilities and research support. Publisher Copyright: © 2019 The Royal Society of Chemistry.

PY - 2019/2

Y1 - 2019/2

N2 - Although electrochemical CO 2 reduction is one of the most promising ways to convert atmospheric CO 2 into value-added chemicals, there are still numerous limitations to overcome to achieve highly efficient CO 2 conversion performance. Herein, we report for the first time the development and use of a three-dimensional iron porphyrin-based graphene hydrogel (FePGH) as an electrocatalyst for extremely efficient robust CO 2 reduction to CO. Electrocatalytic CO 2 conversion was performed in aqueous medium with FePGH, which has a highly porous and conductive 3D graphene structure, resulting in high catalytic activity for CO production with ∼96.2% faradaic efficiency at a very low overpotential of 280 mV. Furthermore, FePGH showed considerable catalytic durability maintaining a consistent CO yield (96.4% FE) over 20 h electrolysis at the same overpotential, corresponding to the highest cathodic energy efficiency yet observed of 79.7% compared to other state-of-the-art immobilised metal complex electrocatalysts. This approach to fabricating a 3D graphene-based hydrogel electrocatalyst should provide an exciting new avenue for the development of other kinds of molecular electrocatalysts.

AB - Although electrochemical CO 2 reduction is one of the most promising ways to convert atmospheric CO 2 into value-added chemicals, there are still numerous limitations to overcome to achieve highly efficient CO 2 conversion performance. Herein, we report for the first time the development and use of a three-dimensional iron porphyrin-based graphene hydrogel (FePGH) as an electrocatalyst for extremely efficient robust CO 2 reduction to CO. Electrocatalytic CO 2 conversion was performed in aqueous medium with FePGH, which has a highly porous and conductive 3D graphene structure, resulting in high catalytic activity for CO production with ∼96.2% faradaic efficiency at a very low overpotential of 280 mV. Furthermore, FePGH showed considerable catalytic durability maintaining a consistent CO yield (96.4% FE) over 20 h electrolysis at the same overpotential, corresponding to the highest cathodic energy efficiency yet observed of 79.7% compared to other state-of-the-art immobilised metal complex electrocatalysts. This approach to fabricating a 3D graphene-based hydrogel electrocatalyst should provide an exciting new avenue for the development of other kinds of molecular electrocatalysts.

UR - http://www.scopus.com/inward/record.url?scp=85061914651&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85061914651&partnerID=8YFLogxK

U2 - 10.1039/c8ee03403f

DO - 10.1039/c8ee03403f

M3 - Article

AN - SCOPUS:85061914651

SN - 1754-5692

VL - 12

SP - 747

EP - 755

JO - Energy and Environmental Science

JF - Energy and Environmental Science

IS - 2

ER -