Dataset Information

Pauling-type adsorption of O₂ induced electrocatalytic singlet oxygen production on N-CuO for organic pollutants degradation.

ABSTRACT: Due to environmentally friendly operation and on-site productivity, electrocatalytic singlet oxygen (¹O₂) production via O₂ gas is of immense interest in environment purification. However, the side-on configuration of O₂ on the catalysts surface will lead to the formation of H₂O, which seriously limits the selectivity and activity of ¹O₂ production. Herein, we show a robust N-doped CuO (N-CuO) with Pauling-type (end-on) adsorption of O₂ at the N-Cu-O₃ sites for the selective generation of ¹O₂ under direct-current electric field. We propose that Pauling-type configuration of O₂ not only lowers the overall activation energy barrier, but also alters the reaction pathway to form ¹O₂ instead of H₂O, which is the key feature determining selectivity for the dissociation of Cu-O bonds rather than the O-O bonds. The proposed N dopant strategy is applicable to a series of transition metal oxides, providing a universal electrocatalysts design scheme for existing high-performance electrocatalytic ¹O₂ production.

SUBMITTER: Xie L

PROVIDER: S-EPMC9500010 | biostudies-literature | 2022 Sep

REPOSITORIES: biostudies-literature

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Pauling-type adsorption of O2 induced electrocatalytic singlet oxygen production on N-CuO for organic pollutants degradation.

Xie Liangbo L Wang Pengfei P Li Yi Y Zhang Dongpeng D Shang Denghui D Zheng Wenwen W Xia Yuguo Y Zhan Sihui S Hu Wenping W

Nature communications 20220922 1

Due to environmentally friendly operation and on-site productivity, electrocatalytic singlet oxygen (1O2) production via O2 gas is of immense interest in environment purification. However, the side-on configuration of O2 on the catalysts surface will lead to the formation of H2O, which seriously limits the selectivity and activity of 1O2 production. Herein, we show a robust N-doped CuO (N-CuO) with Pauling-type (end-on) ...[more]

PMID: 36138010

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Project description:In this work, we report the facile, environmentally friendly, room-temperature (RT) synthesis of porous CuO nanosheets and their application as a photocatalyst to degrade an organic pollutant/food dye using NaBH4 as the reducing agent in an aqueous medium. Ultrahigh-resolution field effect scanning electron microscopy images of CuO displayed a broken nanosheet-like (a length of ∼160 nm, a width of ∼65 nm) morphology, and the lattice strain was estimated to be ∼1.24 × 10-3 using the Williamson-Hall analysis of X-ray diffraction plots. Owing to the strong quantum size confinement effect, CuO nanosheets resulted in an optical energy band gap of ∼1.92 eV, measured using Tauc plots of the ultraviolet-visible (UV-vis) spectrum, resulting in excellent photocatalytic efficiency. The RT synthesized CuO catalyst showed a high Brunauer-Emmet-Teller surface area of 30.88 ± 0.2313 m2/g (a correlation coefficient of 0.99972) with an average Barrett-Joyner-Halenda pore size of ∼20.385 nm. The obtained porous CuO nanosheets exhibited a high crystallinity of 73.5% with a crystallite size of ∼12 nm and was applied as an efficient photocatalyst for degradation of the organic pollutant/food dye, Allura Red AC (AR) dye, as monitored by UV-vis spectrophotometric analysis and evidenced by a color change from red to colorless. From UV-vis spectra, CuO nanosheets exhibited an efficient and ultrafast photocatalytic degradation efficiency of ∼96.99% for the AR dye in an aqueous medium within 6 min at RT. According to the Langmuir-Hinshelwood model, photodegradation reaction kinetics followed a pseudo-first-order reaction with a rate constant of k = 0.524 min-1 and a half-life (t 1/2) of 2.5 min for AR dye degradation in the aqueous medium. The CuO nanosheets showed an outstanding recycling ability for AR degradation and would be highly favorable and an efficient catalyst due to the synergistic effect of high adsorption capability and photodegradation of the food dye.

Project description:Microplastics (MPs) are persistent tiny pieces of plastic material in the environment that are capable of adsorbing environmental organic pollutants from their surroundings. The interaction of MPs with organic pollutants alters their environmental behavior, i.e., their adsorption, degradation and toxicity, etc. Polyethylene (PE) is the most widely used plastic material. The environmental weathering of PE results in changes to its surface chemistry, making the polymer a much better vector for organic pollutants than virgin PE. In this study, a laboratory-accelerated weathering experiment was carried out with a virgin PE film and an oxidatively degradable PE (OXO-PE) film, i.e., PE modified by the addition of a pro-oxidant catalyst. The degradation of PE and OXO-PE was assessed through Fourier transform infra-red (FTIR) spectroscopy and their wettability was measured by contact angle (CA) measurements. Their thermal properties and morphology were studied using thermogravimetric analyses (TGA) and scanning electron microscopy (SEM), respectively. Further, the adsorption of two model organic pollutants onto weathered and virgin PE was analyzed. Triclosan (TCS) and methylparaben (MeP) were chosen as model organic pollutants for the adsorption experiment due to their frequent use in the cosmetics industry, their uncontrolled release into the environment and their toxicity. The adsorption of both model pollutants onto PE and OXO-PE MP was analyzed by using gas chromatography with a flame ionization detector (GC-FID). The adsorption of MeP onto OXO-PE was higher than onto PE MPs. However, TCS showed insignificant adsorption onto PE and OXO-PE. When both pollutants were present simultaneously, the adsorption of TCS onto both PE and OXO-PE was significantly influenced by the presence of MeP. This result demonstrates that the adsorption behavior of one pollutant can be significantly altered by the presence of another pollutant. Both the effect of weathering on the adsorption of organic pollutants as well as the interaction between organic pollutants adsorbing onto MPs is highly relevant to actual MP pollution in the environment, where MPs are exposed to weathering conditions and mixtures of organic pollutants.

Dataset Information

Pauling-type adsorption of O₂ induced electrocatalytic singlet oxygen production on N-CuO for organic pollutants degradation.

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Pauling-type adsorption of O<sub>2</sub> induced electrocatalytic singlet oxygen production on N-CuO for organic pollutants degradation.

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