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

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.

doi:10.1021/jacs.9b09298

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 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.

Authors:

^[1]; Gutierrez-Puebla, Enrique ^[2];

^[2];

^[1];

^[3];

^[1];

^[1]; Yaghi, Omar M. ^[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)
Consejo Superior de Investigaciones Científicas, Madrid (Spain)
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)
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:: Tue Oct 15 00:00:00 EDT 2019

Research Org.:: Lawrence Berkeley National Laboratory (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:: 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:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 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.

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                    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.  https://doi.org/10.1021/jacs.9b09298

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                    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.  https://doi.org/10.1021/jacs.9b09298.  https://www.osti.gov/servlets/purl/1634054.

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@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},

  number       = 43,

  volume       = 141,

  place        = {United States},

  year         = {Tue Oct 15 00:00:00 EDT 2019},

  month        = {Tue Oct 15 00:00:00 EDT 2019}

}

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https://doi.org/10.1021/jacs.9b09298

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Figure 1: Single crystal X-ray structure of MOF-1992 based on Fe trimers and Co phthalocyanine catechol linkers (CoPc). Atom color scheme: C, black; O, red; N, green; Co, orange; Fe, blue polyhedra. Hydrogen atoms and chlorido ligands (Section S3) are omitted. The anionic charge of [Fe₆(OH₂)₄(CoPc)₃]^6-, MOF-1992, is balanced bymore »

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

Abstract

Citation Formats

Figures / Tables:

The frontiers of energy journal, January 2016

Materials for solar fuels and chemicals journal, December 2016

What would it take for renewably powered electrosynthesis to displace petrochemical processes? journal, April 2019

Electrochemical CO 2 Reduction to Hydrocarbons on a Heterogeneous Molecular Cu Catalyst in Aqueous Solution journal, June 2016

A Local Proton Source Enhances CO 2 Electroreduction to CO by a Molecular Fe Catalyst journal, October 2012

Electrocatalytic reduction of carbon dioxide by nickel cyclam2+ in water: study of the factors affecting the efficiency and the selectivity of the process journal, November 1986

The Homogeneous Reduction of CO 2 by [Ni(cyclam)] + : Increased Catalytic Rates with the Addition of a CO Scavenger journal, March 2015

Highly selective and active CO2 reduction electrocatalysts based on cobalt phthalocyanine/carbon nanotube hybrid structures journal, March 2017

CO2 electrochemical catalytic reduction with a highly active cobalt phthalocyanine journal, August 2019

Efficient electrolyzer for CO 2 splitting in neutral water using earth-abundant materials journal, May 2016

Molecular electrocatalysts can mediate fast, selective CO 2 reduction in a flow cell journal, July 2019

Introduction to Reticular Chemistry journal, January 2019

The role of reticular chemistry in the design of CO2 reduction catalysts journal, February 2018

Fe-Porphyrin-Based Metal–Organic Framework Films as High-Surface Concentration, Heterogeneous Catalysts for Electrochemical Reduction of CO 2 journal, September 2015

Metal–Organic Frameworks for Electrocatalytic Reduction of Carbon Dioxide journal, October 2015

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Electrically Conductive Porous Metal-Organic Frameworks journal, January 2016

Electrocatalysis by metal phthalocyanines in the reduction of carbon dioxide journal, January 1974

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The frontiers of energy
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Materials for solar fuels and chemicals
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journal, March 2017

Electrically Conductive Porous Metal-Organic Frameworks
journal, January 2016

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journal, January 1974

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