Restructuring Metal–Organic Frameworks to Nanoscale Bismuth Electrocatalysts for Highly Active and Selective CO2 Reduction to Formate

Paolo Lamagni; Matteo Miola; Jacopo Catalano; Mathias S. Hvid; Mohammad Aref H. Mamakhel; Mogens Christensen; Monica R. Madsen; Henrik S. Jeppesen; Xin Ming Hu; Kim Daasbjerg; Troels Skrydstrup; Nina Lock

doi:10.1002/adfm.201910408

Restructuring Metal–Organic Frameworks to Nanoscale Bismuth Electrocatalysts for Highly Active and Selective CO₂ Reduction to Formate

Paolo Lamagni, Matteo Miola, Jacopo Catalano, Mathias S. Hvid, Mohammad Aref H. Mamakhel, Mogens Christensen, Monica R. Madsen, Henrik S. Jeppesen, Xin Ming Hu^*, Kim Daasbjerg, Troels Skrydstrup, Nina Lock

^*Corresponding author for this work

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

128 Citations (Scopus)

Abstract

Recently, a large number of nanostructured metal-containing materials have been developed for the electrochemical CO₂ reduction reaction (eCO₂RR). However, it remains a challenge to achieve high activity and selectivity with respect to the metal load due to the limited concentration of surface metal atoms. Here, it is reported that the bismuth-based metal–organic framework Bi(1,3,5-tris(4-carboxyphenyl)benzene), herein denoted Bi(btb), works as a precatalyst and undergoes a structural rearrangement at reducing potentials to form highly active and selective catalytic Bi-based nanoparticles dispersed in a porous organic matrix. The structural change is investigated by electron microscopy, X-ray diffraction, total scattering, and spectroscopic techniques. Due to the periodic arrangement of Bi cations in highly porous Bi(btb), the in situ formed Bi nanoparticles are well-dispersed and hence highly exposed for surface catalytic reactions. As a result, high selectivity over a broad potential range in the eCO₂RR toward formate production with a Faradaic efficiency up to 95(3)% is achieved. Moreover, a large current density with respect to the Bi load, i.e., a mass activity, up to 261(13) A g⁻¹ is achieved, thereby outperforming most other nanostructured Bi materials.

Original language	English
Article number	1910408
Journal	Advanced Functional Materials
Volume	30
Issue	16
Number of pages	11
ISSN	1616-301X
DOIs	https://doi.org/10.1002/adfm.201910408
Publication status	Published - Apr 2020

Keywords

bismuth electrocatalysts
electrocatalysis
formate production
metal–organic frameworks
selective CO reduction

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10.1002/adfm.201910408

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Lamagni, P., Miola, M., Catalano, J., Hvid, M. S., Mamakhel, M. A. H., Christensen, M., Madsen, M. R., Jeppesen, H. S., Hu, X. M., Daasbjerg, K., Skrydstrup, T., & Lock, N. (2020). Restructuring Metal–Organic Frameworks to Nanoscale Bismuth Electrocatalysts for Highly Active and Selective CO₂ Reduction to Formate. Advanced Functional Materials, 30(16), Article 1910408. https://doi.org/10.1002/adfm.201910408

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title = "Restructuring Metal–Organic Frameworks to Nanoscale Bismuth Electrocatalysts for Highly Active and Selective CO2 Reduction to Formate",

abstract = "Recently, a large number of nanostructured metal-containing materials have been developed for the electrochemical CO2 reduction reaction (eCO2RR). However, it remains a challenge to achieve high activity and selectivity with respect to the metal load due to the limited concentration of surface metal atoms. Here, it is reported that the bismuth-based metal–organic framework Bi(1,3,5-tris(4-carboxyphenyl)benzene), herein denoted Bi(btb), works as a precatalyst and undergoes a structural rearrangement at reducing potentials to form highly active and selective catalytic Bi-based nanoparticles dispersed in a porous organic matrix. The structural change is investigated by electron microscopy, X-ray diffraction, total scattering, and spectroscopic techniques. Due to the periodic arrangement of Bi cations in highly porous Bi(btb), the in situ formed Bi nanoparticles are well-dispersed and hence highly exposed for surface catalytic reactions. As a result, high selectivity over a broad potential range in the eCO2RR toward formate production with a Faradaic efficiency up to 95(3)% is achieved. Moreover, a large current density with respect to the Bi load, i.e., a mass activity, up to 261(13) A g−1 is achieved, thereby outperforming most other nanostructured Bi materials.",

keywords = "bismuth electrocatalysts, electrocatalysis, formate production, metal–organic frameworks, selective CO reduction",

author = "Paolo Lamagni and Matteo Miola and Jacopo Catalano and Hvid, {Mathias S.} and Mamakhel, {Mohammad Aref H.} and Mogens Christensen and Madsen, {Monica R.} and Jeppesen, {Henrik S.} and Hu, {Xin Ming} and Kim Daasbjerg and Troels Skrydstrup and Nina Lock",

year = "2020",

month = apr,

doi = "10.1002/adfm.201910408",

language = "English",

volume = "30",

journal = "Advanced Functional Materials",

issn = "1616-301X",

publisher = "Wiley-VCH Verlag",

number = "16",

}

Lamagni, P, Miola, M, Catalano, J, Hvid, MS, Mamakhel, MAH , Christensen, M, Madsen, MR, Jeppesen, HS, Hu, XM, Daasbjerg, K , Skrydstrup, T & Lock, N 2020, 'Restructuring Metal–Organic Frameworks to Nanoscale Bismuth Electrocatalysts for Highly Active and Selective CO₂ Reduction to Formate', Advanced Functional Materials, vol. 30, no. 16, 1910408. https://doi.org/10.1002/adfm.201910408

Restructuring Metal–Organic Frameworks to Nanoscale Bismuth Electrocatalysts for Highly Active and Selective CO₂ Reduction to Formate. / Lamagni, Paolo; Miola, Matteo; Catalano, Jacopo et al.
In: Advanced Functional Materials, Vol. 30, No. 16, 1910408, 04.2020.

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

TY - JOUR

T1 - Restructuring Metal–Organic Frameworks to Nanoscale Bismuth Electrocatalysts for Highly Active and Selective CO2 Reduction to Formate

AU - Lamagni, Paolo

AU - Miola, Matteo

AU - Catalano, Jacopo

AU - Hvid, Mathias S.

AU - Mamakhel, Mohammad Aref H.

AU - Christensen, Mogens

AU - Madsen, Monica R.

AU - Jeppesen, Henrik S.

AU - Hu, Xin Ming

AU - Daasbjerg, Kim

AU - Skrydstrup, Troels

AU - Lock, Nina

PY - 2020/4

Y1 - 2020/4

N2 - Recently, a large number of nanostructured metal-containing materials have been developed for the electrochemical CO2 reduction reaction (eCO2RR). However, it remains a challenge to achieve high activity and selectivity with respect to the metal load due to the limited concentration of surface metal atoms. Here, it is reported that the bismuth-based metal–organic framework Bi(1,3,5-tris(4-carboxyphenyl)benzene), herein denoted Bi(btb), works as a precatalyst and undergoes a structural rearrangement at reducing potentials to form highly active and selective catalytic Bi-based nanoparticles dispersed in a porous organic matrix. The structural change is investigated by electron microscopy, X-ray diffraction, total scattering, and spectroscopic techniques. Due to the periodic arrangement of Bi cations in highly porous Bi(btb), the in situ formed Bi nanoparticles are well-dispersed and hence highly exposed for surface catalytic reactions. As a result, high selectivity over a broad potential range in the eCO2RR toward formate production with a Faradaic efficiency up to 95(3)% is achieved. Moreover, a large current density with respect to the Bi load, i.e., a mass activity, up to 261(13) A g−1 is achieved, thereby outperforming most other nanostructured Bi materials.

AB - Recently, a large number of nanostructured metal-containing materials have been developed for the electrochemical CO2 reduction reaction (eCO2RR). However, it remains a challenge to achieve high activity and selectivity with respect to the metal load due to the limited concentration of surface metal atoms. Here, it is reported that the bismuth-based metal–organic framework Bi(1,3,5-tris(4-carboxyphenyl)benzene), herein denoted Bi(btb), works as a precatalyst and undergoes a structural rearrangement at reducing potentials to form highly active and selective catalytic Bi-based nanoparticles dispersed in a porous organic matrix. The structural change is investigated by electron microscopy, X-ray diffraction, total scattering, and spectroscopic techniques. Due to the periodic arrangement of Bi cations in highly porous Bi(btb), the in situ formed Bi nanoparticles are well-dispersed and hence highly exposed for surface catalytic reactions. As a result, high selectivity over a broad potential range in the eCO2RR toward formate production with a Faradaic efficiency up to 95(3)% is achieved. Moreover, a large current density with respect to the Bi load, i.e., a mass activity, up to 261(13) A g−1 is achieved, thereby outperforming most other nanostructured Bi materials.

KW - bismuth electrocatalysts

KW - electrocatalysis

KW - formate production

KW - metal–organic frameworks

KW - selective CO reduction

UR - http://www.scopus.com/inward/record.url?scp=85083689755&partnerID=8YFLogxK

U2 - 10.1002/adfm.201910408

DO - 10.1002/adfm.201910408

M3 - Journal article

AN - SCOPUS:85083689755

SN - 1616-301X

VL - 30

JO - Advanced Functional Materials

JF - Advanced Functional Materials

IS - 16

M1 - 1910408

ER -

Restructuring Metal–Organic Frameworks to Nanoscale Bismuth Electrocatalysts for Highly Active and Selective CO₂ Reduction to Formate

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Keywords

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