Polyethylene
terephthalate (PET) is the most used polymer, but
its natural degradation kinetics is sluggish; therefore, its disposal
poses an environmental threat. Here, we demonstrate electrocatalytic
PET upcycling with full recyclability with a cobalt containing one-dimensional
(1D) coordination polymer as an electrocatalyst that can operate at
a low onset potential of 1.27 V vs. RHE, affording terephthalic acid
(TPA) in 100% yield and potassium diformate (KDF) with ∼80%
selectivity as isolated products, along with the coproduction of hydrogen.
The mechanistic analysis, as obtained from systematic studies with
PET, its oligomer, and monomer revealed a pathway for a side reaction
generating carbonate (CO3
2–) that follows
a formate oxidation instead of an oxalate oxidation pathway. The catalytic
performance and the mechanistic insight gained from the study, are
useful in developing the PET upcycling technologies with maximized
formate/KDF production.
Luminescent nickel(ii) complexes have been synthesized using redox-active azo-oximes. The superior π-acidity of the organic backbone is a key to the isolation of Ni(ii) anion radicals.
A pair of tridentate ligands incorporating heterocyclic hydrazones of 9,10‐phenanthrenequinone viz,. pyridyl‐hydrazino‐phenathrenequinone HLPy 1a and benzothiazolyl‐hydrazino‐phenathrenequinone HLBenz 1b have been synthesized and both behave as monoanionic towards nickel(II), forming meridional octahedral complexes of type [Ni(LPy)2] 2a and [Ni(LBenz)2] 2b as evident from single crystal X‐ray diffraction studies. The complexes are electro‐active in solution and nature of redox orbitals has been analysed by theoretical means. They display two oxidative and two reductive responses that have been ascribed to the redox processes of coordinated ligands. The electronic absorption spectral patterns of two complexes are analogous barring the fact that lower energy transition for 2b is marginally bathochromically shifted relative to that of 2a and it has been clarified by TD‐DFT studies. Anti‐bacterial efficacy of the ligands HLPy 1a, HLBenz 1b and complexes [Ni(LPy)2] 2a, [Ni(LBenz)2] 2b against four Gram‐positive and four Gram‐negative strains has been explored. [Ni(LPy)2] 2a exhibits more pronounced efficacy than [Ni(LBenz)2] 2b and these are greater than those of the corresponding ligands. The mode of action of 2a is essential via DNA damage while protein leakage and membrane lipid damage were observed upon treatment with 2b.
Coordination diversity of an aromatic diamine with Rh(iii) is presented together with the elucidation of the molecular and electronic structures, electron transfer, and electronic transitions.
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