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Kristian Birk Buhl

Selective CO2 Reduction to CO in Water using Earth-Abundant Metal and Nitrogen-Doped Carbon Electrocatalysts

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Selective CO2 Reduction to CO in Water using Earth-Abundant Metal and Nitrogen-Doped Carbon Electrocatalysts. / Hu, Xin-Ming; Hval, Halvor Hoen; Bjerglund, Emil Tveden; Dalgaard, Kirstine Junker; Madsen, Monica Rohde; Pohl, Marga-Martina; Welter, Edmund; Lamagni, Paolo; Buhl, Kristian Birk; Bremholm, Martin; Beller, Matthias; Pedersen, Steen Uttrup; Skrydstrup, Troels; Daasbjerg, Kim.

I: ACS Catalysis, Bind 8, Nr. 7, 06.07.2018, s. 6255-6264.

Publikation: Bidrag til tidsskrift/Konferencebidrag i tidsskrift /Bidrag til avisTidsskriftartikelForskningpeer review

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@article{302ce97009dd4c2fb592bf93bdb4fbdc,
title = "Selective CO2 Reduction to CO in Water using Earth-Abundant Metal and Nitrogen-Doped Carbon Electrocatalysts",
abstract = "Earth-abundant transition metal (Fe, Co, or Ni) and nitrogen doped porous carbon electrocatalysts (M-N-C, where M denotes the metal) were synthesized from cheap precursors via silica-templated pyrolysis. The effect of the material composition and structure (i.e., porosity, nitrogen doping, metal identity, and oxygen functionalization) on the activity for the electrochemical CO2 reduction reaction (CO2RR) was investigated. The metal-free N-C exhibits a high selectivity but low activity for CO2RR Incorporation of the Fe and Ni, but not CO2 sites in the N-C material is able to significantly enhance the activity. The general selectivity order for CO2-to-CO conversion in water is found to be Ni > Fe >> Co with respect to the metal in M-N-C, while the activity follows Ni, Fe >> Co. Notably, the Ni-doped carbon exhibits a high selectivity with a faradaic efficiency of 93{\%} for CO production. Tafel analysis shows a change of the rate-determining step as the metal overtakes the role of the nitrogen as the most active site. Recording the X-ray photoelectron spectra and extended X-ray absorption fine structure demonstrates that the metals are atomically dispersed in the carbon matrix, most likely coordinated to four nitrogen atoms and with carbon atoms serving as a second coordination shell. Presumably, the carbon atoms in the second coordination shell of the metal sites in M-N-C significantly affect the CO2RR activity because the opposite reactivity order is found for carbon supported metal meso-tetraphenylporphyrin complexes. From a better understanding of the relationship between the CO2RR activity and the material structure, it becomes possible to rationally design high-performance porous carbon electrocatalysts involving earth-abundant metals for CO2 valorization.",
keywords = "CO2 reduction, carbon, iron/cobalt/nickel doping, electrocatalysis, structure-activity relationship, ELECTROCHEMICAL REDUCTION, ORGANIC FRAMEWORKS, OXYGEN REDUCTION, HIGHLY EFFICIENT, CO2-TO-CO CONVERSION, DIOXIDE, IRON, ELECTROREDUCTION, SITES, IMMOBILIZATION",
author = "Xin-Ming Hu and Hval, {Halvor Hoen} and Bjerglund, {Emil Tveden} and Dalgaard, {Kirstine Junker} and Madsen, {Monica Rohde} and Marga-Martina Pohl and Edmund Welter and Paolo Lamagni and Buhl, {Kristian Birk} and Martin Bremholm and Matthias Beller and Pedersen, {Steen Uttrup} and Troels Skrydstrup and Kim Daasbjerg",
year = "2018",
month = "7",
day = "6",
doi = "10.1021/acscatal.8b01022",
language = "English",
volume = "8",
pages = "6255--6264",
journal = "A C S Catalysis",
issn = "2155-5435",
publisher = "American Chemical Society",
number = "7",

}

RIS

TY - JOUR

T1 - Selective CO2 Reduction to CO in Water using Earth-Abundant Metal and Nitrogen-Doped Carbon Electrocatalysts

AU - Hu, Xin-Ming

AU - Hval, Halvor Hoen

AU - Bjerglund, Emil Tveden

AU - Dalgaard, Kirstine Junker

AU - Madsen, Monica Rohde

AU - Pohl, Marga-Martina

AU - Welter, Edmund

AU - Lamagni, Paolo

AU - Buhl, Kristian Birk

AU - Bremholm, Martin

AU - Beller, Matthias

AU - Pedersen, Steen Uttrup

AU - Skrydstrup, Troels

AU - Daasbjerg, Kim

PY - 2018/7/6

Y1 - 2018/7/6

N2 - Earth-abundant transition metal (Fe, Co, or Ni) and nitrogen doped porous carbon electrocatalysts (M-N-C, where M denotes the metal) were synthesized from cheap precursors via silica-templated pyrolysis. The effect of the material composition and structure (i.e., porosity, nitrogen doping, metal identity, and oxygen functionalization) on the activity for the electrochemical CO2 reduction reaction (CO2RR) was investigated. The metal-free N-C exhibits a high selectivity but low activity for CO2RR Incorporation of the Fe and Ni, but not CO2 sites in the N-C material is able to significantly enhance the activity. The general selectivity order for CO2-to-CO conversion in water is found to be Ni > Fe >> Co with respect to the metal in M-N-C, while the activity follows Ni, Fe >> Co. Notably, the Ni-doped carbon exhibits a high selectivity with a faradaic efficiency of 93% for CO production. Tafel analysis shows a change of the rate-determining step as the metal overtakes the role of the nitrogen as the most active site. Recording the X-ray photoelectron spectra and extended X-ray absorption fine structure demonstrates that the metals are atomically dispersed in the carbon matrix, most likely coordinated to four nitrogen atoms and with carbon atoms serving as a second coordination shell. Presumably, the carbon atoms in the second coordination shell of the metal sites in M-N-C significantly affect the CO2RR activity because the opposite reactivity order is found for carbon supported metal meso-tetraphenylporphyrin complexes. From a better understanding of the relationship between the CO2RR activity and the material structure, it becomes possible to rationally design high-performance porous carbon electrocatalysts involving earth-abundant metals for CO2 valorization.

AB - Earth-abundant transition metal (Fe, Co, or Ni) and nitrogen doped porous carbon electrocatalysts (M-N-C, where M denotes the metal) were synthesized from cheap precursors via silica-templated pyrolysis. The effect of the material composition and structure (i.e., porosity, nitrogen doping, metal identity, and oxygen functionalization) on the activity for the electrochemical CO2 reduction reaction (CO2RR) was investigated. The metal-free N-C exhibits a high selectivity but low activity for CO2RR Incorporation of the Fe and Ni, but not CO2 sites in the N-C material is able to significantly enhance the activity. The general selectivity order for CO2-to-CO conversion in water is found to be Ni > Fe >> Co with respect to the metal in M-N-C, while the activity follows Ni, Fe >> Co. Notably, the Ni-doped carbon exhibits a high selectivity with a faradaic efficiency of 93% for CO production. Tafel analysis shows a change of the rate-determining step as the metal overtakes the role of the nitrogen as the most active site. Recording the X-ray photoelectron spectra and extended X-ray absorption fine structure demonstrates that the metals are atomically dispersed in the carbon matrix, most likely coordinated to four nitrogen atoms and with carbon atoms serving as a second coordination shell. Presumably, the carbon atoms in the second coordination shell of the metal sites in M-N-C significantly affect the CO2RR activity because the opposite reactivity order is found for carbon supported metal meso-tetraphenylporphyrin complexes. From a better understanding of the relationship between the CO2RR activity and the material structure, it becomes possible to rationally design high-performance porous carbon electrocatalysts involving earth-abundant metals for CO2 valorization.

KW - CO2 reduction

KW - carbon

KW - iron/cobalt/nickel doping

KW - electrocatalysis

KW - structure-activity relationship

KW - ELECTROCHEMICAL REDUCTION

KW - ORGANIC FRAMEWORKS

KW - OXYGEN REDUCTION

KW - HIGHLY EFFICIENT

KW - CO2-TO-CO CONVERSION

KW - DIOXIDE

KW - IRON

KW - ELECTROREDUCTION

KW - SITES

KW - IMMOBILIZATION

U2 - 10.1021/acscatal.8b01022

DO - 10.1021/acscatal.8b01022

M3 - Journal article

VL - 8

SP - 6255

EP - 6264

JO - A C S Catalysis

JF - A C S Catalysis

SN - 2155-5435

IS - 7

ER -