Journal
ADVANCED FUNCTIONAL MATERIALS
Volume 30, Issue 16, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.201910408
Keywords
bismuth electrocatalysts; electrocatalysis; formate production; metal-organic frameworks; selective CO2 reduction
Categories
Funding
- Danish National Research Foundation (Carbon Dioxide Activation Center) [DNRF 118]
- VILLUM Foundation Young Investigator Programme [VKR023449]
- Carlsberg Foundation [CF14-0506]
- Independent Research Fund Denmark (Danish Center for Synchrotron and Neutron Science-Danscatt)
- Faculty of Science and Technology at Aarhus University (ST Synergy grant)
- Independent Research Fund Denmark [DFF-IPD 9059-00008B]
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Recently, a large number of nanostructured metal-containing materials have been developed for the electrochemical CO2 reduction reaction (eCO(2)RR). 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 eCO(2)RR 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.
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