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Title: A spongy nickel-organic CO 2 reduction photocatalyst for nearly 100% selective CO production

Solar-driven photocatalytic conversion of CO 2 into fuels has attracted a lot of interest; however, developing active catalysts that can selectively convert CO 2 to fuels with desirable reaction products remains a grand challenge. For instance, complete suppression of the competing H 2 evolution during photocatalytic CO 2-to-CO conversion has not been achieved before. We design and synthesize a spongy nickel-organic heterogeneous photocatalyst via a photochemical route. The catalyst has a crystalline network architecture with a high concentration of defects. It is highly active in converting CO 2 to CO, with a production rate of ~1.6 × 10 4 μmol hour –1 g –1. No measurable H 2 is generated during the reaction, leading to nearly 100% selective CO production over H 2 evolution. When the spongy Ni-organic catalyst is enriched with Rh or Ag nanocrystals, the controlled photocatalytic CO 2 reduction reactions generate formic acid and acetic acid. As a result, achieving such a spongy nickel-organic photocatalyst is a critical step toward practical production of high-value multicarbon fuels using solar energy.
Authors:
ORCiD logo [1] ; ORCiD logo [2] ; ORCiD logo [3] ; ORCiD logo [4] ; ORCiD logo [5] ; ORCiD logo [6] ; ORCiD logo [7] ;  [1] ; ORCiD logo [7] ; ORCiD logo [7] ; ORCiD logo [8] ; ORCiD logo [1] ; ORCiD logo [2] ;  [1]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Nanyang Technological Univ. (Singapore); SinBeRISE (Singapore-Berkeley Research Initiative for Sustainable Energy) CREATE (Singapore)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of Science and Technology Beijing, Beijing (People's Republic of China)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States)
  6. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
  7. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  8. Leiden Univ., Leiden (Netherlands)
Publication Date:
Report Number(s):
BNL-114699-2017-JA
Journal ID: ISSN 2375-2548; R&D Project: 16060; 16060; KC0403020
Grant/Contract Number:
SC0012704; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 3; Journal Issue: 7; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Research Org:
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; CO2 reduction photocatalyst; Center for Functional Nanomaterials
OSTI Identifier:
1419436
Alternate Identifier(s):
OSTI ID: 1409644