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Title: Three-Dimensional Phthalocyanine Metal-Catecholates for High Electrochemical Carbon Dioxide Reduction

Abstract

The synthesis of a new anionic 3D metal-catecholate framework, termed MOF-1992, is achieved by linking tetratopic cobalt phthalocyanin-2,3,9,10,16,17,23,24-octaol linkers with Fe 3(-C 2O 2-) 6(OH 2) 2 trimers into an extended framework of roc topology. MOF-1992 exhibits sterically accessible Co active sites together with charge transfer properties. Cathodes based on MOF-1992 and carbon black (CB) display a high coverage of electroactive sites (270 nmol cm -2) and a high current density (-16.5 mA cm -2; overpotential, -0.52 V) for the CO 2 to CO reduction reaction in water (faradaic efficiency, 80%). Finally, over the 6 h experiment, MOF-1992/CB cathodes reach turnover numbers of 5800 with turnover frequencies of 0.20 s -1 per active site.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [4]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States)
  2. Consejo Superior de Investigaciones Científicas, Madrid (Spain)
  3. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States); Sungkyunkwan Univ. (SKKU), Suwon (Korea)
  4. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States); King Abdulaziz City for Science and Technology, Riyadh (Saudi Arabia)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); King Abdulaziz City for Science and Technology; Fundacion Ruamon Areces; Swiss National Science Foundation (SNSF)
OSTI Identifier:
1634054
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 141; Journal Issue: 43; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
crystal structure; electrical properties; electrodes; metal organic frameworks; catalysts

Citation Formats

Matheu, Roc, Gutierrez-Puebla, Enrique, Monge, M. Ángeles, Diercks, Christian S., Kang, Joohoon, Prévot, Mathieu S., Pei, Xiaokun, Hanikel, Nikita, Zhang, Bing, Yang, Peidong, and Yaghi, Omar M. Three-Dimensional Phthalocyanine Metal-Catecholates for High Electrochemical Carbon Dioxide Reduction. United States: N. p., 2019. Web. doi:10.1021/jacs.9b09298.
Matheu, Roc, Gutierrez-Puebla, Enrique, Monge, M. Ángeles, Diercks, Christian S., Kang, Joohoon, Prévot, Mathieu S., Pei, Xiaokun, Hanikel, Nikita, Zhang, Bing, Yang, Peidong, & Yaghi, Omar M. Three-Dimensional Phthalocyanine Metal-Catecholates for High Electrochemical Carbon Dioxide Reduction. United States. doi:10.1021/jacs.9b09298.
Matheu, Roc, Gutierrez-Puebla, Enrique, Monge, M. Ángeles, Diercks, Christian S., Kang, Joohoon, Prévot, Mathieu S., Pei, Xiaokun, Hanikel, Nikita, Zhang, Bing, Yang, Peidong, and Yaghi, Omar M. Tue . "Three-Dimensional Phthalocyanine Metal-Catecholates for High Electrochemical Carbon Dioxide Reduction". United States. doi:10.1021/jacs.9b09298. https://www.osti.gov/servlets/purl/1634054.
@article{osti_1634054,
title = {Three-Dimensional Phthalocyanine Metal-Catecholates for High Electrochemical Carbon Dioxide Reduction},
author = {Matheu, Roc and Gutierrez-Puebla, Enrique and Monge, M. Ángeles and Diercks, Christian S. and Kang, Joohoon and Prévot, Mathieu S. and Pei, Xiaokun and Hanikel, Nikita and Zhang, Bing and Yang, Peidong and Yaghi, Omar M.},
abstractNote = {The synthesis of a new anionic 3D metal-catecholate framework, termed MOF-1992, is achieved by linking tetratopic cobalt phthalocyanin-2,3,9,10,16,17,23,24-octaol linkers with Fe3(-C2O2-)6(OH2)2 trimers into an extended framework of roc topology. MOF-1992 exhibits sterically accessible Co active sites together with charge transfer properties. Cathodes based on MOF-1992 and carbon black (CB) display a high coverage of electroactive sites (270 nmol cm-2) and a high current density (-16.5 mA cm-2; overpotential, -0.52 V) for the CO2 to CO reduction reaction in water (faradaic efficiency, 80%). Finally, over the 6 h experiment, MOF-1992/CB cathodes reach turnover numbers of 5800 with turnover frequencies of 0.20 s-1 per active site.},
doi = {10.1021/jacs.9b09298},
journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 43,
volume = 141,
place = {United States},
year = {2019},
month = {10}
}

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