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000626265 1001_ $$0P:(DE-H253)PIP1032409$$aSingh, Ashish$$b0
000626265 245__ $$aAtomically dispersed Co$^{2+}$ in a redox-active COF for electrochemical CO$_2$ reduction to ethanol: unravelling mechanistic insight through operando studies
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000626265 520__ $$aDesigning cheap, stable, and efficient electrocatalysts for selective CO$_2$ reduction to ethanol is a green and sustainable approach for converting the greenhouse gas into value-added products. In this context, developing single-atom-based electrocatalysts (SAEs) could be advantageous because of their maximum atom utilization. Here, we report the design and synthesis of a donor–acceptor-based redox-active covalent organic framework (COF), TAPA-OPE, obtained by condensation between tris-(4-aminophenyl) amine (TAPA) and oligo-(p-phenyleneethynylenes) (OPE) based dialdehyde. Owing to the presence of suitable metal chelating sites, TAPA-OPE was utilized for covalent grafting of atomic Co$^{2+}$ (Co-TAPA-OPE), which has been confirmed by EXAFS, HAADF-STEM, and XPS studies. Co-TAPA-OPE acts as a stable SAE for selective reduction of CO$_2$ to ethanol at −0.67 V vs. RHE. Faradaic efficiency (FE) for the ethanol formation is calculated to be 66.8%. The in situ XAS study discloses that the single Co-site transiently changes its oxidation state and coordination environment during the electrocatalytic reduction process. Furthermore, an in situ FTIR study is performed to track the intermediates during the CO$_2$ reduction reaction (CO$_2$RR), which eventually assists in elucidating a plausible reaction mechanism through density functional theory (DFT).
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000626265 7001_ $$00000-0002-8193-2816$$aBarman, Soumitra$$b1
000626265 7001_ $$0P:(DE-H253)PIP1098320$$aRahimi, Faruk Ahamed$$b2
000626265 7001_ $$0P:(DE-H253)PIP1098284$$aDey, Anupam$$b3
000626265 7001_ $$0P:(DE-H253)PIP1098283$$aJena, Rohan$$b4
000626265 7001_ $$aKumar, Ravi$$b5
000626265 7001_ $$0P:(DE-H253)PIP1102994$$aMathew, Nijita$$b6
000626265 7001_ $$00000-0002-3653-7657$$aBhattacharyya, Dibyendu$$b7
000626265 7001_ $$0P:(DE-H253)PIP1098153$$aMaji, Tapas Kumar$$b8$$eCorresponding author
000626265 773__ $$0PERI:(DE-600)2439879-2$$a10.1039/D3EE02946H$$gVol. 17, no. 6, p. 2315 - 2325$$n6$$p2315 - 2325$$tEnergy & environmental science$$v17$$x1754-5692$$y2024
000626265 8564_ $$uhttps://bib-pubdb1.desy.de/record/626265/files/d3ee02946h.pdf
000626265 8564_ $$uhttps://bib-pubdb1.desy.de/record/626265/files/Manuscript_accepted%20version.pdf$$yPublished on 2024-01-31. Available in OpenAccess from 2025-01-31.
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