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 for this work

Department of Chemistry

55 Citations (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 ∼0.3eV 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.

Original language	English
Journal	Catalysis Today
Volume	288
Pages (from-to)	74-78
Number of pages	5
ISSN	0920-5861
DOIs	https://doi.org/10.1016/j.cattod.2017.02.028
Publication status	Published - 2017

Keywords

CO reduction reaction
Electrochemistry
Porphyrine structures
Scaling relation

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10.1016/j.cattod.2017.02.028

Cite this

@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",

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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