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@ARTICLE{Liang:907450,
author = {Liang, Zhifu and Zhang, Ting and Cao, Pengfei and Yoshida,
Takefumi and Tang, Weiqiang and Wang, Xiang and Zuo, Yong
and Tang, Pengyi and Heggen, Marc and Dunin-Borkowski, Rafal
E. and Morante, Joan Ramon and Cabot, Andreu and Yamashita,
Masahiro and Arbiol, Jordi},
title = {{A} novel π-d conjugated cobalt tetraaza[14]annulene based
atomically dispersed electrocatalyst for efficient {CO}2
reduction},
journal = {The chemical engineering journal},
volume = {442},
issn = {1385-8947},
address = {Amsterdam},
publisher = {Elsevier},
reportid = {FZJ-2022-02042},
pages = {136129 -},
year = {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
CoN4 structure which is supported on multi-wall carbon
nanotubes (CNTs) to work as an atomically dispersed
efficient electrocatalyst for the CO2 reduction reaction
(CO2RR). 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
KHCO3 aqueous solution. Density functional theory
calculations confirmed that the cobalt tetra[14]annulene is
an excellent active site for electrocatalytic CO2RR. 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 CO2RR.},
cin = {ER-C-1},
cid = {I:(DE-Juel1)ER-C-1-20170209},
pnm = {5351 - Platform for Correlative, In Situ and Operando
Characterization (POF4-535)},
pid = {G:(DE-HGF)POF4-5351},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000799842600004},
doi = {10.1016/j.cej.2022.136129},
url = {https://juser.fz-juelich.de/record/907450},
}