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Title: Fe-porphyrin-based metal–organic framework films as high-surface concentration, heterogeneous catalysts for electrochemical reduction of CO 2

Realization of heterogeneous electrochemical CO 2-to-fuel conversion via molecular catalysis under high-flux conditions requires the assembly of large quantities of reactant-accessible catalysts on conductive surfaces. As a proof of principle, we demonstrate that electrophoretic deposition of thin films of an appropriately chosen metal–organic framework (MOF) material is an effective method for immobilizing the needed quantity of catalyst. For electrocatalytic CO 2 reduction, we used a material that contains functionalized Fe-porphyrins as catalytically competent, redox-conductive linkers. The approach yields a high effective surface coverage of electrochemically addressable catalytic sites (~10 15 sites/cm 2). The chemical products of the reduction, obtained with ~100% Faradaic efficiency, are mixtures of CO and H 2. The results validate the strategy of using MOF chemistry to obtain porous, electrode-immobilized, networks of molecular catalysts having competency for energy-relevant electrochemical reactions.
 [1] ;  [2] ;  [1] ;  [2] ;  [3] ;  [4]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Univ. of California at San Diego, La Jolla, CA (United States)
  3. Northwestern Univ., Evanston, IL (United States); King Abdulaziz Univ., Jeddah (Saudi Arabia)
  4. Northwestern Univ., Evanston, IL (United States); Argonne National Lab., Argonne, IL (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357; SC0001059; FA9550-10-1-0572
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Name: ACS Catalysis; Journal ID: ISSN 2155-5435
American Chemical Society
Research Org:
Argonne National Laboratory (ANL), Argonne, IL (United States; Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO2 reduction; electrocatalysis; metal organic frameworks; Fe-porphyrin; solar fuel; redox conductivity
OSTI Identifier:
Alternate Identifier(s):
OSTI ID: 1224209