Achieving Near-Unity CO Selectivity for CO2 Electroreduction on an Iron-Decorated Carbon Material

Xin Ming Hu; Daniela Mendoza; Monica Rohde Madsen; Dorian Joulié; Benedikt Lassalle-Kaiser; Marc Robert; Steen U. Pedersen; Troels Skrydstrup; Kim Daasbjerg

doi:10.1002/cssc.202001311

Achieving Near-Unity CO Selectivity for CO₂ Electroreduction on an Iron-Decorated Carbon Material

Xin Ming Hu, Daniela Mendoza, Monica Rohde Madsen, Dorian Joulié, Benedikt Lassalle-Kaiser, Marc Robert, Steen U. Pedersen, Troels Skrydstrup, Kim Daasbjerg^*

^*Corresponding author for this work

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

10 Citations (Scopus)

Abstract

A straightforward procedure has been developed to prepare a porous carbon material decorated with iron by direct pyrolysis of a mixture of a porous polymer and iron chloride. Characterization of the material with X-ray diffraction, X-ray absorption spectroscopy, and electron microscopy indicates the presence of iron carbide nanoparticles encapsulated inside the carbon matrix, and elemental mapping and cyanide poisoning experiments demonstrate the presence of atomic Fe centers, albeit in trace amounts, which are active sites for electrochemical CO₂ reduction. The encapsulated iron carbide nanoparticles are found to boost the catalytic activity of atomic Fe sites in the outer carbon layers, rendering the material highly active and selective for CO₂ reduction, although these atomic Fe sites are only present in trace amounts. The target material exhibits near-unity selectivity (98 %) for CO₂-to-CO conversion at a small overpotential (410 mV) in water. Furthermore, the material holds potential for practical application, as a current density over 30 mA cm⁻² and a selectivity of 93 % can be achieved in a flow cell.

Original language	English
Journal	ChemSusChem (Print)
Volume	13
Issue	23
Pages (from-to)	6360-6369
Number of pages	10
ISSN	1864-5631
DOIs	https://doi.org/10.1002/cssc.202001311
Publication status	Published - Dec 2020

Keywords

CO reduction
electrocatalysis
iron
nanoparticles
porous polymers
ELECTROREDUCTION
ACTIVE-SITES
ELECTROCATALYSTS
REDUCTION
CO(2)reduction
METAL
EFFICIENT
POROUS CARBONS

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10.1002/cssc.202001311

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title = "Achieving Near-Unity CO Selectivity for CO2 Electroreduction on an Iron-Decorated Carbon Material",

abstract = "A straightforward procedure has been developed to prepare a porous carbon material decorated with iron by direct pyrolysis of a mixture of a porous polymer and iron chloride. Characterization of the material with X-ray diffraction, X-ray absorption spectroscopy, and electron microscopy indicates the presence of iron carbide nanoparticles encapsulated inside the carbon matrix, and elemental mapping and cyanide poisoning experiments demonstrate the presence of atomic Fe centers, albeit in trace amounts, which are active sites for electrochemical CO2 reduction. The encapsulated iron carbide nanoparticles are found to boost the catalytic activity of atomic Fe sites in the outer carbon layers, rendering the material highly active and selective for CO2 reduction, although these atomic Fe sites are only present in trace amounts. The target material exhibits near-unity selectivity (98 %) for CO2-to-CO conversion at a small overpotential (410 mV) in water. Furthermore, the material holds potential for practical application, as a current density over 30 mA cm−2 and a selectivity of 93 % can be achieved in a flow cell.",

keywords = "CO reduction, electrocatalysis, iron, nanoparticles, porous polymers, ELECTROREDUCTION, ACTIVE-SITES, ELECTROCATALYSTS, REDUCTION, CO(2)reduction, METAL, EFFICIENT, POROUS CARBONS",

author = "Hu, {Xin Ming} and Daniela Mendoza and Madsen, {Monica Rohde} and Dorian Jouli{\'e} and Benedikt Lassalle-Kaiser and Marc Robert and Pedersen, {Steen U.} and Troels Skrydstrup and Kim Daasbjerg",

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year = "2020",

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doi = "10.1002/cssc.202001311",

language = "English",

volume = "13",

pages = "6360--6369",

journal = "ChemSusChem (Print)",

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publisher = "Chemistry Europe - European Chemical Societies Publishing",

number = "23",

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Achieving Near-Unity CO Selectivity for CO₂ Electroreduction on an Iron-Decorated Carbon Material. / Hu, Xin Ming; Mendoza, Daniela; Madsen, Monica Rohde et al.
In: ChemSusChem (Print), Vol. 13, No. 23, 12.2020, p. 6360-6369.

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

TY - JOUR

T1 - Achieving Near-Unity CO Selectivity for CO2 Electroreduction on an Iron-Decorated Carbon Material

AU - Hu, Xin Ming

AU - Mendoza, Daniela

AU - Madsen, Monica Rohde

AU - Joulié, Dorian

AU - Lassalle-Kaiser, Benedikt

AU - Robert, Marc

AU - Pedersen, Steen U.

AU - Skrydstrup, Troels

AU - Daasbjerg, Kim

PY - 2020/12

Y1 - 2020/12

N2 - A straightforward procedure has been developed to prepare a porous carbon material decorated with iron by direct pyrolysis of a mixture of a porous polymer and iron chloride. Characterization of the material with X-ray diffraction, X-ray absorption spectroscopy, and electron microscopy indicates the presence of iron carbide nanoparticles encapsulated inside the carbon matrix, and elemental mapping and cyanide poisoning experiments demonstrate the presence of atomic Fe centers, albeit in trace amounts, which are active sites for electrochemical CO2 reduction. The encapsulated iron carbide nanoparticles are found to boost the catalytic activity of atomic Fe sites in the outer carbon layers, rendering the material highly active and selective for CO2 reduction, although these atomic Fe sites are only present in trace amounts. The target material exhibits near-unity selectivity (98 %) for CO2-to-CO conversion at a small overpotential (410 mV) in water. Furthermore, the material holds potential for practical application, as a current density over 30 mA cm−2 and a selectivity of 93 % can be achieved in a flow cell.

AB - A straightforward procedure has been developed to prepare a porous carbon material decorated with iron by direct pyrolysis of a mixture of a porous polymer and iron chloride. Characterization of the material with X-ray diffraction, X-ray absorption spectroscopy, and electron microscopy indicates the presence of iron carbide nanoparticles encapsulated inside the carbon matrix, and elemental mapping and cyanide poisoning experiments demonstrate the presence of atomic Fe centers, albeit in trace amounts, which are active sites for electrochemical CO2 reduction. The encapsulated iron carbide nanoparticles are found to boost the catalytic activity of atomic Fe sites in the outer carbon layers, rendering the material highly active and selective for CO2 reduction, although these atomic Fe sites are only present in trace amounts. The target material exhibits near-unity selectivity (98 %) for CO2-to-CO conversion at a small overpotential (410 mV) in water. Furthermore, the material holds potential for practical application, as a current density over 30 mA cm−2 and a selectivity of 93 % can be achieved in a flow cell.

KW - CO reduction

KW - electrocatalysis

KW - iron

KW - nanoparticles

KW - porous polymers

KW - ELECTROREDUCTION

KW - ACTIVE-SITES

KW - ELECTROCATALYSTS

KW - REDUCTION

KW - CO(2)reduction

KW - METAL

KW - EFFICIENT

KW - POROUS CARBONS

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AN - SCOPUS:85090436333

SN - 1864-5631

VL - 13

SP - 6360

EP - 6369

JO - ChemSusChem (Print)

JF - ChemSusChem (Print)

IS - 23

ER -

Achieving Near-Unity CO Selectivity for CO₂ Electroreduction on an Iron-Decorated Carbon Material

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