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1.
Spectrochim Acta A Mol Biomol Spectrosc ; 308: 123772, 2024 Mar 05.
Article in English | MEDLINE | ID: mdl-38128326

ABSTRACT

Reuse and/or recycling of spent adsorbents is taking a central role in modern thinking and catalyzed carbonization is the way forward. Herein we explore the carbonization of adsorbed acetamiprid, in an inert atmosphere, as a way of recycling and producing nitrogen-rich carbon material for potential use in supercapacitors. Added value material and the reuse of the adsorbent were achieved by carbonization at 700 °C under argon. The formation of a nitrogen-doped carbon layer as an active material on the adsorbent, bonded through a C-Si linkage, has been conclusively verified through elemental composition quantification using XPS and EDX measurements. Two-stage catalytic decomposition and condensation of the adsorbed pesticide is followed by TGA and TPD-MS. Attained carbon-based materials give stable Faradaic capacitance with a slight dependency on the number of adsorbing cycles. Capacitance calculated with respect to the adlayer carbon material reaches values as high as 610 F g-1. Galvanostatic Charge/Discharge measurement confirmed the stability of explored materials with a slight increase in capacitance over 1000 cycles. The presented results envisage electroactive materials preparation from environmental pollutants, adding value to spent adsorbents.

2.
Spectrochim Acta A Mol Biomol Spectrosc ; 301: 122987, 2023 Nov 15.
Article in English | MEDLINE | ID: mdl-37327500

ABSTRACT

Herein we unequivocally identify the mechanism of zeolite-catalysed thermal degradation of pesticide, employing Fourier-transform infrared spectroscopy (FTIR), Raman and mass spectrometry following temperature decomposition (TPDe/MS). We demonstrate that Y zeolite can effectively adsorb a significant amount of acetamiprid both in a single trial (168 mg/g) and in 10 cycles (1249 mg/g) with intermittent thermal regeneration at 300 °C. Sectional vibrational analysis of acetamiprid two-stage thermal degradation is performed for pristine and supported pesticide. The acetamiprid Raman spectral changes appear at 200 °C, while partial carbonization occurs at 250 °C. The gradual disappearance of the FTIR bands of acetamiprid is seen up to 270 °C when two Raman signature bands for carbonised material emerged. The TPDe/MS profiles reveal the evolution of mass fragments - in the first step, cleavage of the CC bond occurs between the aromatic core of the molecule and its tail-end, followed by cleavage of the CN bond. The mechanism of adsorbed acetamiprid degradation follows the same step, at significantly lower temperatures, as the process is catalysed by the interaction of acetamiprid nitrogens and zeolite support. Reduced temperature degradation allows for a quick recovery process that leaves 65% efficacy after 10 cycles. After numerous cycles of recovery, a subsequent one-time heat treatment at 700 °C completely restores initial efficacy. The efficient adsorption, novel details on degradation mechanism and ease of regeneration procedure place the Y zeolite at the forefront of future all-encompassing environmental solutions.


Subject(s)
Pesticides , Zeolites , Zeolites/chemistry , Neonicotinoids , Temperature
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