A novel π-d conjugated cobalt tetraaza[14]annulene based atomically dispersed electrocatalyst for efficient CO2 reduction
Liang, Zhifu (Institut Català de Nanociència i Nanotecnologia)
Zhang, Ting (Institut Català de Nanociència i Nanotecnologia)
Cao, Pengfei (Peter Grünberg Institute Forschungszentrum Jülich GmbH)
Yoshida, Takefumi (The University of Electro-Communications. Innovation Research Center for Fuel Cells)
Tang, Weiqiang (East China University of Science and Technology)
Wang, Xiang (Institut de Recerca en Energia de Catalunya)
Zuo, Yong (Institut de Recerca en Energia de Catalunya)
Tang, PengYi (Shanghai Institute of Microsystem and Information Technology)
Heggen, Marc (Peter Grünberg Institute Forschungszentrum Jülich GmbH)
Dunin-Borkowski, Rafal E. (Peter Grünberg Institute Forschungszentrum Jülich GmbH)
Morante, Joan Ramon (Institut de Recerca en Energia de Catalunya)
Cabot i Codina, Andreu (Institució Catalana de Recerca i Estudis Avançats)
Yamashita, Masahiro (Tohoku University. Department of Chemistry)
Arbiol i Cobos, Jordi (Institut Català de Nanociència i Nanotecnologia)

Date:	2022
Abstract:	Tetraaza[14]annulenes (TAA) are synthetic macrocycles which are analogue to porphyrins. However, there are almost no reports about the synthesis of polymers based on TAA and neither on their use as electrocatalysts. The study of new catalysts to promote an efficient electrochemical conversion of carbon dioxide to valuable chemicals is a promising approach to relieve the pressure of carbon emissions and realize the carbon cycle. Herein, we first report the synthesis of a novel tetraaza[14]annulene (TAA) based organic polymeric metal complex (PMC) by a non-template method. This PMC is used as ligand to construct a π-d conjugated cobalt coordination polymer (Poly-TAA-Co) with CoN structure which is supported on multi-wall carbon nanotubes (CNTs) to work as an atomically dispersed efficient electrocatalyst for the CO reduction reaction (CORR). The resulting catalyst (Poly-TAA-Co-CNT) exhibits excellent performance, with a 90% CO faradaic efficiency, a low overpotential (390 mV) and good stability in 0. 5 M KHCO aqueous solution. Density functional theory calculations confirmed that the cobalt tetra[14]annulene is an excellent active site for electrocatalytic CORR. This work not only inspires the design of novel TAA based macromolecules, but also paves the way to the development and application of new molecular-based catalysts for electrocatalytic CORR.
Grants:	Agencia Estatal de Investigación PID2020-116093RB-C43 Agencia Estatal de Investigación PID2019-105490RB-C32 Agencia Estatal de Investigación ENE2016-77798-C4-3-R Ministerio de Economía y Competitividad SEV-2017-0706 Ministerio de Economía y Competitividad SEV-2013-0295-17-1 Agència de Gestió d'Ajuts Universitaris i de Recerca 2017/SGR-327 Agència de Gestió d'Ajuts Universitaris i de Recerca 2017/SGR-1246
Note:	Altres ajuts: the present work was supported by MCIN with funding from European Union NextGenerationEU (PRTR-C17.I1) and the Government of Catalonia. ICN2 and IREC are funded by the CERCA Programme /Generalitat de Catalunya.
Rights:	Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, la comunicació pública de l'obra i la creació d'obres derivades, fins i tot amb finalitats comercials, sempre i quan es reconegui l'autoria de l'obra original.
Language:	Anglès
Document:	Article ; recerca ; Versió publicada
Subject:	Tetraaza[14]annulene ; π-d Conjugated ; Atomically dispersed Co catalyst ; Electrocatalytic CO2 reduction
Published in:	Chemical engineering journal (1996), Vol. 442, part. 2 (Aug. 2022) , art. 136129, ISSN 1873-3212

DOI: 10.1016/j.cej.2022.136129

11 p, 4.4 MB

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Research literature > UAB research groups literature > Research Centres and Groups (research output) > Experimental sciences > Catalan Institute of Nanoscience and Nanotechnology (ICN2)
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Articles > Published articles