Highly stable two-dimensional bismuth metal-organic frameworks for efficient electrochemical reduction of CO2

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We report a unique 2D bismuth metal-organic framework (Bi-MOF) that possesses permanent accessible porosity for efficient electrochemical CO2 reduction (ECR) to HCOOH. The 2D open-framework structure with helical Bi-O rods bridged by tritopic carboxylate ligands exhibits a remarkable Faradaic efficiency for HCOOH formation over a broad potential window, reaching 92.2 % at similar to -0.9 V (vs. reversible hydrogen electrode, RHE) with excellent durability over 30 h. The mass-specific HCOOH partial current density is up to 41.0 mA mg(Bi)(-1), exceeding 4 times higher than that of commercial Bi2O3 and Bi sheets at similar to -1.1 V (vs. RHE). Operando and ex-situ X-ray absorption fine structure spectroscopy revealed a structural feature associated with Bi-MOF to preserve Bi (3 + ) during and after long-term ECR. Theoretical calculations further showed that the crystallographically channels with abundant Bi active sites in the MOF structure favor the formation of *HCOO while suppressing the side-reaction of hydrogen evolution, thereby leading to the high selectivity for HCOOH.
Publisher
ELSEVIER
Issue Date
2020-11
Language
English
Article Type
Article
Citation

APPLIED CATALYSIS B-ENVIRONMENTAL, v.277, pp.119241

ISSN
0926-3373
DOI
10.1016/j.apcatb.2020.119241
URI
http://hdl.handle.net/10203/281843
Appears in Collection
CBE-Journal Papers(저널논문)
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