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@ARTICLE{Singh:626265,
author = {Singh, Ashish and Barman, Soumitra and Rahimi, Faruk Ahamed
and Dey, Anupam and Jena, Rohan and Kumar, Ravi and Mathew,
Nijita and Bhattacharyya, Dibyendu and Maji, Tapas Kumar},
title = {{A}tomically dispersed {C}o$^{2+}$ in a redox-active {COF}
for electrochemical {CO}$_2$ reduction to ethanol:
unravelling mechanistic insight through operando studies},
journal = {Energy $\&$ environmental science},
volume = {17},
number = {6},
issn = {1754-5692},
address = {Cambridge},
publisher = {RSC Publ.},
reportid = {PUBDB-2025-01344},
pages = {2315 - 2325},
year = {2024},
abstract = {Designing cheap, stable, and efficient electrocatalysts for
selective CO$_2$ reduction to ethanol is a green and
sustainable approach for converting the greenhouse gas into
value-added products. In this context, developing
single-atom-based electrocatalysts (SAEs) could be
advantageous because of their maximum atom utilization.
Here, we report the design and synthesis of a
donor–acceptor-based redox-active covalent organic
framework (COF), TAPA-OPE, obtained by condensation between
tris-(4-aminophenyl) amine (TAPA) and
oligo-(p-phenyleneethynylenes) (OPE) based dialdehyde. Owing
to the presence of suitable metal chelating sites, TAPA-OPE
was utilized for covalent grafting of atomic Co$^{2+}$
(Co-TAPA-OPE), which has been confirmed by EXAFS,
HAADF-STEM, and XPS studies. Co-TAPA-OPE acts as a stable
SAE for selective reduction of CO$_2$ to ethanol at −0.67
V vs. RHE. Faradaic efficiency (FE) for the ethanol
formation is calculated to be 66.8\%. The in situ XAS study
discloses that the single Co-site transiently changes its
oxidation state and coordination environment during the
electrocatalytic reduction process. Furthermore, an in situ
FTIR study is performed to track the intermediates during
the CO$_2$ reduction reaction (CO$_2$RR), which eventually
assists in elucidating a plausible reaction mechanism
through density functional theory (DFT).},
cin = {FS DOOR-User},
ddc = {690},
cid = {$I:(DE-H253)FS_DOOR-User-20241023$},
pnm = {6G3 - PETRA III (DESY) (POF4-6G3) / INDIA-DESY - INDIA-DESY
Collaboration $(2020_Join2-INDIA-DESY)$},
pid = {G:(DE-HGF)POF4-6G3 / $G:(DE-HGF)2020_Join2-INDIA-DESY$},
experiment = {EXP:(DE-H253)P-P64-20150101},
typ = {PUB:(DE-HGF)16},
UT = {WOS:001175941800001},
doi = {10.1039/D3EE02946H},
url = {https://bib-pubdb1.desy.de/record/626265},
}