Single site porphyrine-like structures advantages over metals for selective electrochemical CO2 reduction

Alexander Bagger; Wen Ju; Ana Sofia Varela; Peter Strasser; Jan Rossmeisl

doi:10.1016/j.cattod.2017.02.028

Single site porphyrine-like structures advantages over metals for selective electrochemical CO₂ reduction

Alexander Bagger, Wen Ju, Ana Sofia Varela, Peter Strasser, Jan Rossmeisl^*

^*Corresponding author af dette arbejde

Kemisk Institut

55 Citationer (Scopus)

Abstract

Currently, no catalysts are completely selective for the electrochemical CO2 Reduction Reaction (CO2RR). Based on trends in density functional theory calculations of reaction intermediates we find that the single metal site in a porphyrine-like structure has a simple advantage of limiting the competing Hydrogen Evolution Reaction (HER). The single metal site in a porphyrine-like structure requires an ontop site binding of hydrogen, compared to the hollow site binding of hydrogen on a metal catalyst surface. The difference in binding site structure gives a fundamental energy-shift in the scaling relation of ∼0.3 eV between the COOH* vs. H* intermediate (CO2RR vs. HER). As a result, porphyrine-like catalysts have the advantage over metal catalyst of suppressing HER and enhancing CO2RR selectivity

Originalsprog	Engelsk
Tidsskrift	Catalysis Today
Vol/bind	288
Sider (fra-til)	74-78
Antal sider	5
ISSN	0920-5861
DOI	https://doi.org/10.1016/j.cattod.2017.02.028
Status	Udgivet - 2017

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10.1016/j.cattod.2017.02.028

Citationsformater

@article{2752da727f4f46b79e357455cbdc7851,

title = "Single site porphyrine-like structures advantages over metals for selective electrochemical CO2 reduction",

abstract = "Currently, no catalysts are completely selective for the electrochemical CO2 Reduction Reaction (CO2RR). Based on trends in density functional theory calculations of reaction intermediates we find that the single metal site in a porphyrine-like structure has a simple advantage of limiting the competing Hydrogen Evolution Reaction (HER). The single metal site in a porphyrine-like structure requires an ontop site binding of hydrogen, compared to the hollow site binding of hydrogen on a metal catalyst surface. The difference in binding site structure gives a fundamental energy-shift in the scaling relation of ∼0.3eV between the COOH* vs. H* intermediate (CO2RR vs. HER). As a result, porphyrine-like catalysts have the advantage over metal catalyst of suppressing HER and enhancing CO2RR selectivity.",

keywords = "CO reduction reaction, Electrochemistry, Porphyrine structures, Scaling relation",

author = "Alexander Bagger and Wen Ju and Varela, {Ana Sofia} and Peter Strasser and Jan Rossmeisl",

year = "2017",

doi = "10.1016/j.cattod.2017.02.028",

language = "English",

volume = "288",

pages = "74--78",

journal = "Catalysis Today",

issn = "0920-5861",

publisher = "Elsevier",

}

TY - JOUR

T1 - Single site porphyrine-like structures advantages over metals for selective electrochemical CO2 reduction

AU - Bagger, Alexander

AU - Ju, Wen

AU - Varela, Ana Sofia

AU - Strasser, Peter

AU - Rossmeisl, Jan

PY - 2017

Y1 - 2017

N2 - Currently, no catalysts are completely selective for the electrochemical CO2 Reduction Reaction (CO2RR). Based on trends in density functional theory calculations of reaction intermediates we find that the single metal site in a porphyrine-like structure has a simple advantage of limiting the competing Hydrogen Evolution Reaction (HER). The single metal site in a porphyrine-like structure requires an ontop site binding of hydrogen, compared to the hollow site binding of hydrogen on a metal catalyst surface. The difference in binding site structure gives a fundamental energy-shift in the scaling relation of ∼0.3eV between the COOH* vs. H* intermediate (CO2RR vs. HER). As a result, porphyrine-like catalysts have the advantage over metal catalyst of suppressing HER and enhancing CO2RR selectivity.

AB - Currently, no catalysts are completely selective for the electrochemical CO2 Reduction Reaction (CO2RR). Based on trends in density functional theory calculations of reaction intermediates we find that the single metal site in a porphyrine-like structure has a simple advantage of limiting the competing Hydrogen Evolution Reaction (HER). The single metal site in a porphyrine-like structure requires an ontop site binding of hydrogen, compared to the hollow site binding of hydrogen on a metal catalyst surface. The difference in binding site structure gives a fundamental energy-shift in the scaling relation of ∼0.3eV between the COOH* vs. H* intermediate (CO2RR vs. HER). As a result, porphyrine-like catalysts have the advantage over metal catalyst of suppressing HER and enhancing CO2RR selectivity.

KW - CO reduction reaction

KW - Electrochemistry

KW - Porphyrine structures

KW - Scaling relation

U2 - 10.1016/j.cattod.2017.02.028

DO - 10.1016/j.cattod.2017.02.028

M3 - Journal article

AN - SCOPUS:85014116510

SN - 0920-5861

VL - 288

SP - 74

EP - 78

JO - Catalysis Today

JF - Catalysis Today

ER -

Single site porphyrine-like structures advantages over metals for selective electrochemical CO2 reduction

Abstract

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Single site porphyrine-like structures advantages over metals for selective electrochemical CO₂ reduction