PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2023
·Vol. 25
·期 12
·8913-8920
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IF 3.3
Zhen Chi,Jia Xu,Shida Luo,Xia Ran,Xiaojuan Wang,Pingan Liu,Yulu He,Yanmin Kuang,Lijun Guo
Triplet energy transfer (TET) from semiconductor quantum dots (QDs) to molecular triplets has potential applications in photon up-conversion and singlet oxygen generation. Here, we have constructed a complex consisting of CdTe QDs as the donor and 9-anthracenecarboxylic acid (ACA) as the triplet acceptor, and studied the TET pathways and enhanced singlet oxygen generation properties. The results from steady-state and time-resolved spectroscopy demonstrate efficient TET with a total efficiency of over 80% from photoexcited CdTe QDs to ACA. Dynamical analysis clearly indicates two distinctive TET channels – hot electron exchange and thermalized electron exchange – mediating the TET process in the CdTe QDs–ACA complex. The TET efficiencies from hot electron exchange at high energetic levels and thermalized electron exchange on the lowest exciton state can reach ∼27% and ∼85%, respectively, following 530 nm excitation. This efficient TET endows the CdTe QDs–ACA complex with a good capability of generating singlet oxygen species with a yield of up to ∼59%. These findings contribute further insights to the mechanisms of interfacial TET processes and are significant in designing efficient TET systems based on semiconductor nanoparticles and triplet molecules.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
·
IF 13.6
Chen Wang,Huanran Liu,Peng Sun,Jingjing Cai,Mingxing Sun,Haijiao Xie,Guoqing Shen
Single-atom dispersed catalysts (SACs) have gained considerable attention in organic contaminants remediation due to their superior reactivity and stability. However, the complex and costly synthesis processes limit their practical applications in environmental protection. Herein, a facile and cost-effective single-atom iron catalyst (Fe-SA/NC) anchored on nitrogen-doped porous carbon was first fabricated by using waste biomass as a carbon source. The Fe-SA/NC catalyst exhibited outstanding performance with a high turnover frequency of 1.72 min −1 toward antibiotics degradation via peroxymonosulfate activation . ECOSAR program and algae growth experiments demonstrated that the byproducts produced during the sulfamethoxazole degradation process were not detrimental to the aquatic environment. Radical quenching and electron paramagnetic resonance experiments revealed that Fe-SA/NC remarkably promoted 1 O 2 production in PMS-assisted reaction, and thus 1 O 2 contributed as much as 78.77% to sulfamethoxazole degradation. As indicated by experiment and density functional theory (DFT) calculations, FeN 2 O 2 configuration serves as the active site. DFT calculations further presented the most rational generation route of 1 O 2 as PMS→OH* →O* → 1 O 2 . We also designed Fe-SA/NC embedded spherical pellets for contaminants elimination at the device level. This study offers new insights into the synthesis of SACs from waste biomass and their practical application in environmental remediation.
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JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Mingyu Wei,Xiaowen Shi,Ling Xiao,Haifei Zhang
Polyimide-modified carbon nanotubes (PI/CNTs) were synthesized via a solvent-free thermal method and used as a metal-free catalyst to activate peroxymonosulfate for organic contaminant degradation without light irradiation. The characterization results suggested that PI was loaded onto the surface of CNTs . The catalytic ability of the PI/CNTs was strongly correlated with the content of PI in the catalysts. The PI/CNTs (22% of PI) showed the highest catalytic efficiency for organic pollutant degradation at room temperature. The degradation efficiency of acid orange 7 (AO7) dye was significantly enhanced to 98.9% within 15 min, compared to the efficiency of 2.2% exhibited by pure PI. The radical quenching tests and electron paramagnetic resonance spectrometry proved that singlet oxygen, instead of hydroxyl radicals or sulfate radicals, played a dominant role during the catalytic oxidation of AO7. The influences of operation parameters including temperature and catalyst amount were investigated. The PI/CNTs metal-free catalyst exhibited high catalytic activity under a broad range of pH values. The recycling study of four repeated reactions demonstrated good stability of the PI/CNTs. This work provided a promising metal-free catalyst for degradation of organic pollutants in aqueous solutions, contributing to the development of green materials for sustainable remediation.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Nguyen Trung Dung,Vu Dinh Thao,Nguyen Phuong Thao,Cao Thi Minh Thuy,Nguyen Hong Nam,Le Viet Ngan,Kun-Yi Andrew Lin,Ta Cong Khiem,Nguyen Nhat Huy
Biochar is an environmentally friendly material with various potential applications in water treatment. Herein, nitrogen and sulfur co-doped biochars (N,S-BCD-X) were fabricated from durian peel as an agricultural waste by coupling with thiourea via thermal treatment to activate peroxymonosulfate (PMS) for degradation of ofloxacin (OFX) in water. The OFX removal using PMS activated by N,S-BCD-800 was over 85 % after 120 min of reaction, which was 17.78 times higher than that by pure BCD. The OFX degradation was not inhibited over a wide pH range of 3 to 9. Through radical quenching tests, electron paramagnetic resonance, and DFT calculations, 1 O 2 was revealed as the key reactive species in the N,S-BCD-800/PMS system because of PMS’s elongated O-O bond-induced promoted generation of • OH and SO 4 • - with an insignificant contribution and the generation of 1 O 2 via various reactions associated with • OH, SO 4 • - , and PMS. The boosted catalytic activity of N,S-BCD-800 mainly came from synergetic effect of N and S co-doping due to the enhanced electron-donating capability caused by decrease in the work function. Furthermore, the increase in electrostatic potential and the difference in electron density and atomic charge could also account for stronger adsorption and activation of PMS on N,S-BCD-800 to generate more 1 O 2 besides the N,S-BCD-800/PMS complex as a minor species responsible for the degradation of OFX via electron transfer. Finally, the attainment of high efficiency of N,S-BCD/PMS for OFX degradation in various water matrices as well as after 5 cycles proved that N,S-BCD had high stability and applicability.
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WATER RESEARCH
·
2025
·
IF 12.4
Mengdi Zhao,Zibo Xu,Xiaoguang Duan,Nigel J.D. Graham,Hua Zhong,Daniel C.W. Tsang
Single-atom catalysts have attracted tremendous research interest in advanced oxidation water treatment, while their efficiency and recyclability were restricted by speciation. Deliberate manipulation of single-atom (SAs) accumulation and distribution to tune the catalyst efficiency and route constitutes an area of great interest but a challenging pursuit. Here, we developed a series of novel spherical porous carbon materials from biomass waste with a three-dimensional distribution of Fe. Fe SAs and atomic clusters (ACs) are simultaneously formed in catalysts, and their distribution from the outer surface to the inner core varies with pyrrolic N content. The cooperation of SAs and ACs serves as a pair of redox sites linked with graphitic carbon to coordinate the electron circulation with peroxymonosulfate (PMS), generating radical and singlet oxygen for antibiotic degradation. The confined environment and the cooperation of dual sites perpendicular to the carbon plane were first reported, which enhanced the generation of reactive species. These advantages afforded efficient degradation (up to 229 % improved in kinetics and 133 % improved in degradation) with heightened recyclability (up to 150 % improved) compared to surface-doped SAs or ACs-dominated catalyst. Furthermore, this approach achieved efficient utilization of atomic metal sites compared to previously documented metal-based atomically dispersed catalysts. This study reveals the synergy of SAs and ACs in a confined environment for cyclic electron transfer and inspires a new version for designing atomically dispersed Fe within the 3D structure for advanced water decontamination.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 22
·期 27
·15340-15353
·
IF 3.43
Genxing Zhu,Jialu Zhu,Xinlong Fu,Qi Liu,Fengyi Cao,Yu-nan Li,Qi Qin,Mingli Jiao
In this study, Co nanoparticle-embedded N,O-codoped porous carbon nanospheres (C@Co) with abundant N and O doping, high graphitization, large specific surface area (319 m2 g−1) and a well-developed mesoporous structure were synthesized and characterized thoroughly, and were applied to activate peroxymonosulfate (PMS) for the degradation of methylene blue (MB). Various influential factors affecting the catalytic performance including C@Co dosage, PMS dosage, MB concentration, initial pH, temperature, and co-existing common anions and humic acid (HA) on the MB degradation were systematically investigated. The increase of the C@Co dosage (15–60 mg), PMS dosage (25–100 mg) and reaction temperature (278–308 K) promoted the MB degradation in the C@Co/PMS system. The best performance of the C@Co/PMS system was observed under weakly acidic or nearly neutral conditions. Both the MB concentration (25–100 mg L−1) and Cl− (5–100 mM), NO3− (10–500 mM), CO32− (10–300 mM), HCO3− (1–30 mM) and HA (2–40 mg L−1) had an inhibitory effect on MB degradation, and the degree of decrease in MB degradation increased as their concentrations were enhanced. Interestingly, HPO42− (1–100 mM) had an overall inhibitory effect on the degradation process of MB; however, in comparison with lower concentrations (1–10 mM), an attenuation of the inhibitory effect at higher concentrations (50–100 mM) could be observed. Moreover, the C@Co/PMS system also exhibited general applicability in eliminating various organic pollutants from water such as methyl orange, malachite green, safranine T, Congo red, Rhodamine B, ofloxacin and tetracycline. Classical radical-quenching tests and EPR measurements showed that both the non-radical pathway (major route, involving 1O2) and radical pathway (minor route, involving ˙OH, ˙SO4− and ˙O2−) contribute to the MB degradation. DFT calculations disclosed that the combination of Co–C interactions with graphitic N doping brought in catalytically active sites in C@Co where the charge states of some C atoms were significantly increased. The degradation intermediates of MB during the catalytic reaction were also identified by HPLC-MS and the possible degradation pathway was proposed. Overall, the resultant C@Co can be developed as a novel and efficient heterogeneous catalyst for activating PMS to degrade organic pollutants, and has potential application in environmental remediation.
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ACS Applied Bio Materials
·
2021
·
IF 0
Xiaoxiao Hu,Qiang Zhang,Xiaomei Dai,Junyong Sun,Feng Gao
The pH environment in cancer cells has been demonstrated to display vital influences on the therapeutic effect of photodynamic therapy (PDT). It is very interesting to develop pH-responsive probes for simultaneous pH sensing and dynamics monitoring of the effects of PDT, and therefore assessing the correlation between them. In this study, a multifunctional fluorescence probe, dual-emission carbonized polymer dot (CPD) in blue and red regions, which uses ethylene imine polymer (PEI) and 4,4′,4″,4‴-(porphine-5, 10, 15, 20-tetrayl) tetrakis (benzoic acid) (TCPP) as precursors through a one-step hydrothermal amide reaction, has been designed for ratiometric pH sensing, generating pH-dependent 1O2 for PDT of cancer cells, and investigating the dynamics effects of PDT through pH-guided imaging. The prepared CPDs were successfully used for ratiometric pH response, pH-dependent generation of 1O2, and dynamics monitoring PDT in HeLa cells. This study may provide an alternative strategy to prepare CPD-based theranostic integrated nanoprobes for PDT through the rational design of precursors.
研究领域:
生物医学工程
·
肿瘤学
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纳米医学
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CHEMOSPHERE
·
2024
·
IF 8.1
Que Wu,Yongqing Zhang,Hong Meng,Xuefeng Wu,Yuqi Liu,Li Li
The non-free radical oxidation pathway (PMS-NOPs) of peroxymonosulfate (PMS) holds significant promise for practical wastewater treatment applications, owing to its low oxidation potential, high PMS utilization rate, and robust anti-interference capability in the degradation of pollutants. A novel activator copper nitrogen co-doped porous biochar (Cu-N-BC) with rich defect edges and functional groups was obtained by adding Cu and N to the biochar matrix generated by sodium alginate through pyrolysis in this study. Under the condition of 1 mM PMS, 30 mg/L activator was used to activate PMS and achieve efficient degradation of 10 mg/L paracetamol (PCT) within 15 min, with a high reaction rate constants (k obs ) of 0.391 min −1 . The activation mechanism of the Cu-N-BC/PMS/PCT system was a non-radical activation pathway with the dominance of singlet oxygen ( 1 O 2 ) and the presence of catalyst-mediated electron transfer. The graphite nitrogen, pyridine nitrogen, and Cu–N coordination introduced by Cu/N co-doping, as well as the carbon skeleton and C O functional group of biochar, were considered active sites that promote the 1 O 2 generation. The Cu-N-BC/PMS system exhibits strong stability, eco-friendliness, effective mineralization, and interference resistance across diverse pH levels (3–11) and interfering ions, including Cl − , H 2 PO 4 − , NO 3 − , SO 4 2− , and humic acid. Remarkably, it efficiently degrades PCT in tap and lake water, achieving a notable 63.73% TOC mineralization rate, with leached copper ions below 0.02 mg/L. This research introduces a novel method for obtaining metal nitrogen carbon activators and enhances understanding of PMS non-radical activation pathways and active sites.
研究领域:
环境科学
·
废水处理
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2026
·
IF 7.1
Taotao Qiang,Jie Xiong,Chen Mi,Xi Zhang,Huaqing Liu,Xiaonan Ruan,Bing Shi,Qingshuang Zhu,Fei Cheng,Longfang Ren
Covalent organic framework (COF) photocatalysts have attracted considerable attention for their highly efficient and selective oxidation to sulfides, but they still suffer from high charge recombination rates, wide band gaps, and low electron-transfer efficiencies. Therefore, two kinds of high-performance porphyrin-based D-A type COFs photocatalysts were designed by employing tetraaminoporphyrin as the electron donor (D) and two distinct linkers as electron acceptors (A). The D-A architecture facilitates the enhancement of charge transfer and the effective separation of photogenerated electron-hole pairs, so that the COFs exhibit exceptional charge separation efficiency which is evidenced by significantly reduced steady-state photoluminescence (PL) intensity and prolonged fluorescence lifetimes. The singlet oxygen radicals generated by COFs enables the selective oxidation of sulfides with the conversion rate of 99% and the selectivity of 99%. The narrow band gap (Eg = 1.73 eV) further achieves the adjusting of carrier mobility, thereby accelerating the electron transfer rate. Through precise regulation of the reaction pathway, the toxic by-products during oxidation are significantly reduced, highlighting that the COFs have great potential as visible-light-driven heterogeneous catalysts. This study offers a promising strategy for environmentally friendly and sustainable production of chemicals.
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TALANTA
·
2021
·
IF 6.057
Hong Huang,Biyun Chen,Lifen Li,Yuan Wang,Zhangfeng Shen,Yangang Wang,Xi Li
Endoplasmic reticulum (ER) is an indispensable organelle responsible for protein synthesis , transportation, and maintenance of Ca 2+ homeostasis in eukaryotic cells. Recent studies highlighted that ER-targeted photosensitizers with high yield of singlet oxygen ( 1 O 2 ) are effective in selectively disrupting ER function and are promising candidates for anticancer therapy. Unfortunately, no ER targetable fluorescent probes for determining 1 O 2 photosensitized in this photodynamic therapy process is available. In this work, we synthesized an ER-targetable, two-photon fluorescence probe, ER- 1 O 2 , for fluorescence turn-on sensing of 1 O 2 . ER- 1 O 2 demonstrated high sensitivity to 1 O 2 sensing with a wide detection range (0–2.75 μM) and a low detection limit (0.11 μM). ER- 1 O 2 also displayed excellent selectivity toward 1 O 2 out of other ROS and metal ions . Notably, ER- 1 O 2 exhibited low cytotoxicity but with specific ER targetable capability. On account of these advantageous features, fluctuations of 1 O 2 in living cells and brain tissues were effectively visualized by ER- 1 O 2 .
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Photodiagnosis and Photodynamic Therapy
·
2021
·
IF 3.631
Xianglian Liao,Chunxiu Yang,Huiyun Lin,Buhong Li
Background Singlet oxygen ( 1 O 2 ) is highly reactive to biological components such as lipids, proteins and DNA, which induces oxidative damage to cells and tissues. Natural antioxidants may function as 1 O 2 quencher to prevent 1 O 2 involved photosensitized oxidation in biological system. Methods Time-resolved measurement of 1 O 2 luminescence was employed to evaluate the 1 O 2 quenching abilities of natural antioxidants in air-statured phosphate buffered saline (PBS), including (-)-Epigallocatechin gallate (EGCG), Proanthocyanidins, L-carnosine and Vitamin C. The 1 O 2 quenching effects and rate constant of EGCG were investigated by detecting the absorption, fluorescence and 1 H-NMR spectroscopy and 1 O 2 luminescence decay curves, respectively. In addition, the protective activity of EGCG against 1 O 2 oxidative damage caused by Ce6-mediated photodynamic therapy (PDT) was verified in cells. Results EGCG, proanthocyanidins, L-carnosine and Vitamin C efficiently quenched 1 O 2 luminescence at 1270 nm. The triplet-state quenching rate constants of EGCG for Rose Bengal (RB), Chlorin e6, AlPcS and HiPorfin are 2.21 × 10 9 , 4.90 × 10 8 , 3.30 × 10 8 , 1.78 × 10 9 M −1 s −1 , while the 1 O 2 quenching rate constants are 2.80 × 10 8 , 1.50 × 10 8 , 1.30 × 10 8 , 1.70 × 10 8 M −1 s −1 , respectively. Furthermore, EGCG could effectively quench 1 O 2 production to prevent NIH/3T3 cells oxidative damage induced by Ce6-mediated PDT. Conclusions EGCG is an efficient quencher for both triplet-state photosensitizers and 1 O 2 . The quenching ability of EGCG during photosensitization for selected photosensitizers is: RB > HiPorfin > Ce6 > AlPcS. EGCG could be used to protect normal cells and tissue against oxidative damage.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Yi Hu,Dezhi Chen,Rui Zhang,Yuan Ding,Zhong Ren,Maosheng Fu,Xiukun Cao,Guisheng Zeng
Waste-derived biochar has been emerged as promising catalysts to activate peroxymonosulfate (PMS) for the degradation of organic contaminants . Herein, passion fruit shell derived biochar (PFSC) was prepared by a one-pot pyrolysis method and used as a metal-free catalyst to activate PMS for the degradation of tetracycline hydrochloride (TC). The batch experiments indicated that the pyrolysis temperature could influence the efficiency of PFSC for the activation of PMS. In the PFSC-900 (prepared at 900 °C)/PMS system, the degradation rate of TC can reach 90.91%. The quenching test and electron paramagnetic resonance spectra revealed that the high catalytic performance of PFSC-900/PMS system was mainly attributed to the non-free radical reaction pathway containing a carbon bridge, and the TC degradation was controlled primarily by singlet oxygen-mediated oxidation . Moreover, the carboxyl group of ketones and the graphite-N atoms on PFSC-900 are the possible active sites of the non-free radical pathway including direct electron transfer or the formation of O 2 •- / 1 O 2 . This study not only shows a new type of biochar as an efficient catalyst for PMS activation but also provides a way of value-added reuse of passion fruit shell.
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危险品化学品经营许可证（带存储）