DataVXACS Applied Materials & InterfacesPaper
journal article·2022-01-12

Metallated Isoindigo–Porphyrin Covalent Organic Framework Photocatalyst with a Narrow Band Gap for Efficient CO2 Conversion

Tina Skorjanc, Dinesh Shetty, Mahmoud Elcheikh Mahmoud, Felipe Gándara, Jose Ignacio Martinez, Abdul Khayum Mohammed, Sandra Boutros, Areej Merhi, Elissa O. Shehayeb, Christa A. Sharabati, Patrick Damacet, Jesus Raya, Sandra Gardonio, Mohamad Hmadeh, Bilal R. Kaafarani, Ali Trabolsi

ACS Applied Materials & Interfaces· Volume 14· Issue 1
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Source abstract

Abstract

Photocatalytic CO2 reduction into formate (HCOO–) has been widely studied with semiconductor and molecule-based systems, but it is rarely investigated with covalent organic frameworks (COFs). Herein, we report a novel donor–acceptor COF named Co-PI-COF composed of isoindigo and metallated porphyrin subunits that exhibits high catalytic efficiency (∼50 μmol formate g–1 h–1) at low-power visible-light irradiation and in the absence of rare metal cocatalysts. Density functional theory calculations and experimental diffuse-reflectance measurements are used to explain the origin of catalytic efficiency and the particularly low band gap (0.56 eV) in this material. The mechanism of photocatalysis is also studied experimentally and is found to involve electron transfer from the sacrificial agent to the excited Co-PI-COF. The observed high-efficiency conversion could be ascribed to the enhanced CO2 adsorption on the coordinatively unsaturated cobalt centers, the narrow band gap, and the efficient transfer of the charge originating from the postsynthetic metallation. It is anticipated that this study will pave the way toward the design of new simple and efficient catalysts for photocatalytic CO2 reduction into useful products.
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Research context

Electronic materialsCatalysis & surfaces

OpenAlex topics: Covalent Organic Framework Applications · Metal-Organic Frameworks: Synthesis and Applications · Advanced Photocatalysis Techniques

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Science Division, New York University Abu Dhabi, Saadiyat Island, 129188 Abu Dhabi, United Arab Emirates

Materials Research Laboratory, University of Nova Gorica, Vipavska 11c, 5270 Ajdovscina, Slovenia

Department of Chemistry & Center for Catalysis and Separations (CeCaS), Khalifa University of Science and Technology, P.O. Box 127788 Abu Dhabi, United Arab Emirates

American University of Beirut, P.O. Box 11-0236, 1107 2020 Riad El-Solh, Beirut, Lebanon

Instituto de Ciencia de Materiales de Madrid-CSIC, C. Sor Juana Inés de la Cruz 3, 28049 Madrid, Spain

Department of Natural Sciences, Lebanese American University, P.O. Box 13-5053, 1102 2801 Chouran Beirut, Lebanon

Membrane Biophysics and NMR, Institute of Chemistry, University of Strasbourg─CNRS, Rue Blaise Pascal 1, 67081 Strasbourg, France

NYUAD Water Research Center, New York University Abu Dhabi (NYUAD), Saadiyat Island, P.O. Box 129188 Abu Dhabi, United Arab Emirates

Funding

Khalifa University of Science, Technology and Research · American University of Beirut · Horizon 2020 Framework Programme · New York University Abu Dhabi

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