High-Rate and Efficient Ethylene Electrosynthesis Using a Catalyst/Promoter/Transport Layer

Adnan Ozden; Fengwang Li; F. Pelayo Garcĺa De Arquer; Alonso Rosas-Hernández; Arnaud Thevenon; Yuhang Wang; Sung Fu Hung; Xue Wang; Bin Chen; Jun Li; Joshua Wicks; Mingchuan Luo; Ziyun Wang; Theodor Agapie; Jonas C. Peters; Edward H. Sargent; David Sinton

doi:10.1021/acsenergylett.0c01266

High-Rate and Efficient Ethylene Electrosynthesis Using a Catalyst/Promoter/Transport Layer

Adnan Ozden, Fengwang Li, F. Pelayo Garcĺa De Arquer, Alonso Rosas-Hernández, Arnaud Thevenon, Yuhang Wang, Sung Fu Hung, Xue Wang, Bin Chen, Jun Li, Joshua Wicks, Mingchuan Luo, Ziyun Wang, Theodor Agapie^*, Jonas C. Peters^*, Edward H. Sargent^*, David Sinton^*

^*Corresponding author for this work

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

115 Citations (Scopus)

Abstract

Carbon dioxide (CO2) electroreduction to valuable chemicals such as ethylene is an avenue to store renewable electricity and close the carbon cycle. Membrane electrode assembly (MEA) electrolyzers have attracted recent interest in light of their high stability and despite low productivity (a modest partial current density in CO2-to-ethylene conversion of approximately 100 mA cm-2). Here we present an adlayer functionalization catalyst design: a catalyst/tetrahydro-phenanthrolinium/ionomer (CTPI) interface in which the catalytically active copper is functionalized using a phenanthrolinium-derived film and a perfluorocarbon-based polymeric ionomer. We find, using electroanalytical tools and operando spectroscopies, that this hierarchical adlayer augments both the local CO2 availability and the adsorption of the key reaction intermediate CO on the catalyst surface. Using this CTPI catalyst, we achieve an ethylene Faradaic efficiency of 66% at a partial current density of 208 mA cm-2 - a 2-fold increase over the best prior MEA electrolyzer report - and an improved full-cell energy efficiency of 21%.

Original language	English
Journal	ACS Energy Letters
Volume	5
Issue	9
Pages (from-to)	2811-2818
Number of pages	8
DOIs	https://doi.org/10.1021/acsenergylett.0c01266
Publication status	Published - 11 Sept 2020
Externally published	Yes

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Ozden, A., Li, F., Garcĺa De Arquer, F. P., Rosas-Hernández, A., Thevenon, A., Wang, Y., Hung, S. F., Wang, X., Chen, B., Li, J., Wicks, J., Luo, M., Wang, Z., Agapie, T., Peters, J. C., Sargent, E. H., & Sinton, D. (2020). High-Rate and Efficient Ethylene Electrosynthesis Using a Catalyst/Promoter/Transport Layer. ACS Energy Letters, 5(9), 2811-2818. https://doi.org/10.1021/acsenergylett.0c01266

@article{ae8af0eb690244c9ac140b733435a79e,

title = "High-Rate and Efficient Ethylene Electrosynthesis Using a Catalyst/Promoter/Transport Layer",

abstract = "Carbon dioxide (CO2) electroreduction to valuable chemicals such as ethylene is an avenue to store renewable electricity and close the carbon cycle. Membrane electrode assembly (MEA) electrolyzers have attracted recent interest in light of their high stability and despite low productivity (a modest partial current density in CO2-to-ethylene conversion of approximately 100 mA cm-2). Here we present an adlayer functionalization catalyst design: a catalyst/tetrahydro-phenanthrolinium/ionomer (CTPI) interface in which the catalytically active copper is functionalized using a phenanthrolinium-derived film and a perfluorocarbon-based polymeric ionomer. We find, using electroanalytical tools and operando spectroscopies, that this hierarchical adlayer augments both the local CO2 availability and the adsorption of the key reaction intermediate CO on the catalyst surface. Using this CTPI catalyst, we achieve an ethylene Faradaic efficiency of 66% at a partial current density of 208 mA cm-2 - a 2-fold increase over the best prior MEA electrolyzer report - and an improved full-cell energy efficiency of 21%. ",

author = "Adnan Ozden and Fengwang Li and {Garc{\'l}a De Arquer}, {F. Pelayo} and Alonso Rosas-Hern{\'a}ndez and Arnaud Thevenon and Yuhang Wang and Hung, {Sung Fu} and Xue Wang and Bin Chen and Jun Li and Joshua Wicks and Mingchuan Luo and Ziyun Wang and Theodor Agapie and Peters, {Jonas C.} and Sargent, {Edward H.} and David Sinton",

year = "2020",

month = sep,

day = "11",

doi = "10.1021/acsenergylett.0c01266",

language = "English",

volume = "5",

pages = "2811--2818",

journal = "ACS Energy Letters",

issn = "2380-8195",

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Ozden, A, Li, F, Garcĺa De Arquer, FP, Rosas-Hernández, A, Thevenon, A, Wang, Y, Hung, SF, Wang, X, Chen, B, Li, J, Wicks, J, Luo, M, Wang, Z, Agapie, T, Peters, JC, Sargent, EH & Sinton, D 2020, 'High-Rate and Efficient Ethylene Electrosynthesis Using a Catalyst/Promoter/Transport Layer', ACS Energy Letters, vol. 5, no. 9, pp. 2811-2818. https://doi.org/10.1021/acsenergylett.0c01266

High-Rate and Efficient Ethylene Electrosynthesis Using a Catalyst/Promoter/Transport Layer. / Ozden, Adnan; Li, Fengwang; Garcĺa De Arquer, F. Pelayo et al.
In: ACS Energy Letters, Vol. 5, No. 9, 11.09.2020, p. 2811-2818.

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaper › Journal article › Research › peer-review

TY - JOUR

T1 - High-Rate and Efficient Ethylene Electrosynthesis Using a Catalyst/Promoter/Transport Layer

AU - Ozden, Adnan

AU - Li, Fengwang

AU - Garcĺa De Arquer, F. Pelayo

AU - Rosas-Hernández, Alonso

AU - Thevenon, Arnaud

AU - Wang, Yuhang

AU - Hung, Sung Fu

AU - Wang, Xue

AU - Chen, Bin

AU - Li, Jun

AU - Wicks, Joshua

AU - Luo, Mingchuan

AU - Wang, Ziyun

AU - Agapie, Theodor

AU - Peters, Jonas C.

AU - Sargent, Edward H.

AU - Sinton, David

PY - 2020/9/11

Y1 - 2020/9/11

N2 - Carbon dioxide (CO2) electroreduction to valuable chemicals such as ethylene is an avenue to store renewable electricity and close the carbon cycle. Membrane electrode assembly (MEA) electrolyzers have attracted recent interest in light of their high stability and despite low productivity (a modest partial current density in CO2-to-ethylene conversion of approximately 100 mA cm-2). Here we present an adlayer functionalization catalyst design: a catalyst/tetrahydro-phenanthrolinium/ionomer (CTPI) interface in which the catalytically active copper is functionalized using a phenanthrolinium-derived film and a perfluorocarbon-based polymeric ionomer. We find, using electroanalytical tools and operando spectroscopies, that this hierarchical adlayer augments both the local CO2 availability and the adsorption of the key reaction intermediate CO on the catalyst surface. Using this CTPI catalyst, we achieve an ethylene Faradaic efficiency of 66% at a partial current density of 208 mA cm-2 - a 2-fold increase over the best prior MEA electrolyzer report - and an improved full-cell energy efficiency of 21%.

AB - Carbon dioxide (CO2) electroreduction to valuable chemicals such as ethylene is an avenue to store renewable electricity and close the carbon cycle. Membrane electrode assembly (MEA) electrolyzers have attracted recent interest in light of their high stability and despite low productivity (a modest partial current density in CO2-to-ethylene conversion of approximately 100 mA cm-2). Here we present an adlayer functionalization catalyst design: a catalyst/tetrahydro-phenanthrolinium/ionomer (CTPI) interface in which the catalytically active copper is functionalized using a phenanthrolinium-derived film and a perfluorocarbon-based polymeric ionomer. We find, using electroanalytical tools and operando spectroscopies, that this hierarchical adlayer augments both the local CO2 availability and the adsorption of the key reaction intermediate CO on the catalyst surface. Using this CTPI catalyst, we achieve an ethylene Faradaic efficiency of 66% at a partial current density of 208 mA cm-2 - a 2-fold increase over the best prior MEA electrolyzer report - and an improved full-cell energy efficiency of 21%.

UR - http://www.scopus.com/inward/record.url?scp=85091024723&partnerID=8YFLogxK

U2 - 10.1021/acsenergylett.0c01266

DO - 10.1021/acsenergylett.0c01266

M3 - Journal article

AN - SCOPUS:85091024723

SN - 2380-8195

VL - 5

SP - 2811

EP - 2818

JO - ACS Energy Letters

JF - ACS Energy Letters

IS - 9

ER -

High-Rate and Efficient Ethylene Electrosynthesis Using a Catalyst/Promoter/Transport Layer

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