ENVIRONMENTAL POLLUTION
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2022
·
IF 9.988
Yao Tang,Jibo Dou,Zhijiang Lu,Jianming Xu,Yan He
The sluggish Fe 3+ /Fe 2+ cycle was the rate-limiting step in the Fenton-like reaction, and metal-free carbonaceous materials are considered as emerging alternatives to solve this problem. However, the effect of carbon material properties on the distribution of reactive species remains poorly understood. This study investigated the possibility and mechanism of using biochar to accelerate the Fe 3+ /Fe 2+ cycle to overcome the low efficiency of Fe 3+ /persulfate (PS) catalytic oxidation of phenanthrene . More importantly, the contribution of reactive species in the reaction systems with the variation of biochar pyrolysis temperatures was quantitatively studied. The results showed that medium-temperature derived biochar (BC500) had the greatest ability to enhance the Fenton-like system compared to the low- and high-temperature (BC350/700), and the first-order rate constant achieved 5.2 and 35.7-fold increase against the biochar/PS and Fe 3+ /PS systems, respectively. Using electrochemical evidence, sulfoxide probe tests, and steady-state concentration calculations, radicals yields were found to rise and then reduce with decreasing pyrolysis temperature, while the nonradical contribution of Fe(IV) increased to 56.3%. Electron paramagnetic resonance, Boehm titration, and Raman spectroscopy unraveled that the enhanced effect of biochar resulted from itself persistent free radicals, phenolic-OH, and edge defects, which enabled electron transfer between Fe 3+ and biochar. Fe 2+ was thus continuously generated and effectively activated the PS. This work enables a better understanding of the Fe 3+ -mediated Fenton-like reaction in the presence of biochar and provides a sustainable green strategy for Fenton chemistry with potential applications.
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CHEMOSPHERE
·
2022
·
IF 8.943
Yingjie Wen,Xu Chen,Linfeng Su,Shuqian Dong,Li Yi,Peilei He,Wen Yang,Zhiyi Lu
The catalytic ozonation-based advanced oxidation process (AOP) is applied to remove nondegradable chemical oxygen demand (COD), while the application in industry is limited by the economics and activity of catalysts. In this study, we demonstrate that by taking atrazine (ATZ) as a model pollutant, the removal rates of catalytic ozonation were negatively correlated with the interlayer water content of metal-modified montmorillonite (M x @MMT), instead of the loadings metals. Among the modified MMT, Zn 0.1 @MMT achieved 83.2% degradation of ATZ within 15 min, and corresponding removal rates of COD and total organic carbon (TOC) reached 40.3% and 46.5%, respectively. Detailed EPR and quenching experiments identified that hydroxyl radicals (HO•) were the main reactive oxygen species and QTOF/MS/MS analysis helped to propose a possible degradation pathway of ATZ. Moreover, the catalytic performance of Zn 0.1 @MMT under different conditions was also systematically evaluated.
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ACS Nano
·
2022
·
IF 18.027
Shikai Liu,Linyang Fang,He Ding,Yangyang Zhang,Wenting Li,Bin Liu,Shuming Dong,Boshi Tian,Lili Feng,Piaoping Yang
The emergence of X-ray-induced photodynamic therapy (X-PDT) holds tremendous promise for clinical deep-penetrating cancer therapy. However, the clinical application of X-PDT in cancer treatment is still limited due to the hypoxic property of cancerous tissue, the inherent antioxidant system of tumor cells, and the difficulty in matching the absorption spectra of photosensitizers. Herein, a versatile core–shell radiosensitizer (SCNPs@DMSN@CeOx-PEG, denoted as SSCP) was elaborately designed and constructed to enhance X-PDT by coating tunable mesoporous silica on nanoscintillators, followed by embedding the cerium oxide nanoparticles in situ. The obtained SSCP radiosensitizer demonstrated a distinct blue-shift in the ultraviolet light region, so that it could perfectly absorb the ultraviolet light converted by the SCNPs core, resulting in the formation of photoinduced electron–hole (e–-h+) pairs separation to generate reactive oxygen species (ROS). In addition, the cerium oxide exhibits high glutathione consumption to heighten ROS accumulation, and catalase-like activity to alleviate the hypoxia, which further enhances the efficiency of radiotherapy. Benefiting from the abundant Lu and Ce elements, the computed tomography imaging performance of SSCP is about 3.79-fold that of the clinical contrast agent (iohexol), which has great potential in both preclinical imaging and clinical translation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Mengmeng Xu,Yuan Liu,Wanru Luo,Fangrong Tan,Donghua Dong,Weichang Li,LinGe Wang,Qianqian Yu
A multi-functional nanocatalytic system based on combined therapies has attracted considerable research attention in recent years due to its potential in the treatment of cancer. Herein, ZnO 2 @ [email protected] nanoparticles (NPs) based on hydroxyl radical (•OH) mediated chemodynamic therapy (CDT) and glucose-exhausting starvation therapy (ST) were constructed. Specifically, in the acidic tumor microenvironment (TME), the pH responsive decomposition of the shell ZIF-67 triggered the release of the Fenton-like catalyst Co 2+ , after which the exposed zinc peroxide (ZnO 2 ) reacted with H 2 O (H + ) to generate O 2 and hydrogen peroxide (H 2 O 2 ). The generated O 2 could alleviate hypoxia in the TEM and interact with ultra-small Au NPs originally coated on ZnO 2 to catalyze intracellular glucose and to produce another source of H 2 O 2 . While the glucose consumption caused the starvation of tumor cells, the generated H 2 O 2 from dual sources reacted with the catalyst Co 2+ to generate highly toxic •OH for CDT. Systematic in vitro and in vivo experiments were carried out to evaluate this nanocatalytic system, and the results showed an enhanced efficacy of this cancer therapy.
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JOURNAL OF MOLECULAR LIQUIDS
·
2022
·
IF 6.633
Chenyue Zhang,Zheng Wang,Fulin Li,Jiahao Wang,Nannan Xu,Yannan Jia,Shiwei Gao,Tian Tian,Wei Shen
CuFe 2 O 4 is often loaded onto biochar (BC) to prepare activated peroxodisulfate (PDS) catalysts for the removal of persistent organic pollutants from water. However, the activation mechanism remains unclear. Therefore, in this study, a BC-loaded CuFe 2 O 4 (CuFe 2 O 4 @BC) system that activates PDS was constructed and used to degrade the antibiotic tetracycline (TC). The synthesized materials were fully characterized, and the optimal reaction conditions of the system were determined to be a CuFe 2 O 4 @BC dosage and PDS concentration of 0.1 mg/L and 10 mM, respectively, under acidic conditions, achieving a TC removal of 30 mg/L. Under these conditions, the removal efficiency reaches 96.0 %. The synergistic effect of CuFe 2 O 4 and BC greatly improves catalytic performance and avoids the agglomeration of the metallic nanoparticles. The PDS-activation mechanism was studied through electron paramagnetic resonance and quenching experiments, revealing that TC is degraded under the combined effects of sulfate radicals (SO 4 •− ), hydroxyl radicals (•OH), and singlet oxygen ( 1 O 2 ). Two plausible degradation pathways of TC are proposed. Overall, this study provides a deeper understanding of metal-modified biochar activated PDS and provides a new strategy for the degradation of TC in this catalytic system.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Waseem Hayat,Yongqing Zhang,Ze-hua Liu,Xiaodong Du
The high leachability and solubility of methomyl (MET; C 5 H 10 N 2 O 2 S) result in water pollution; while, the polluted water channels can be depolluted by environmentally-friendly and highly-effective degradation technique. Therefore, MET degradation in water by peroxydisulfate (PDS) oxidation was investigated in this study employing the two most naturally-abundant iron species i.e. pyrite (PyR) and zero-valent iron (ZVI) as activators for PDS activation. The experiments were conducted at different activators’ dosage, pollutant concentration, oxidant concentration, initial pH and initial temperature for comparative assessment of degradation-efficiencies of PyR/PDS and ZVI/PDS systems. Using 0.25 g/L PyR/ZVI and 1.0 mmol/L PDS, PyR/PDS and ZVI/PDS systems respectively led to 98.8 % and 97.5 % degradation of 20.0 mg/L MET in 20 min, which became rapid by increasing the activators’ dosage and oxidant concentration in both systems. Further, the degradation has been more than 90.0 % at initial pH 3.0 to 11.0, which slowed with increasing the MET concentration in two systems. The free-radicals quenching analysis showed that degradation by PyR/PDS system was mainly executed by sulfate (SO 4 •− ) and hydroxyl ( • OH) radicals; while, SO 4 •− and super oxide radical anion (O 2 •− ) were dominant during degradation by ZVI/PDS system. PyR/PDS system had low stability and applicability, which supports the employment of ZVI/PDS system for efficient degradation of MET in water.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2022
·
IF 6.437
Fupeng Huang,Dongmei Bi,Shanjian Liu,Weiming Yi,Jiawen Zhang,Di Yao
Biochar contains environmentally persistent free radicals (EPFRs), a class of pollutants whose regulation and influencing factors need to be studied. In this study, electron paramagnetic resonance (EPR) signals were observed for biochar samples obtained by the pyrolysis of wheat straw, corn straw, peanut shell, and cotton stalk. The effects of pyrolysis temperature, residence time, and alkali/alkaline earth metals (AAEMs) on EPFRs in biochar were investigated. The adsorption effect of diethyl phthalate (DEP) on biochar obtained from the pyrolysis of wheat straw impregnated with K, Na, Ca, and Mg was also studied. The concentration of EPFRs increased first and then decreased upon increasing the pyrolysis temperature within the rage of 300–700 ℃, conforming to a Gaussian fit. Residence time experiments showed that the concentration of EPFRs was the highest at a residence time of 10 min. The effect of AAEMs on the EPFRs concentration followed the order Mg > K > Ca > Na due to the catalysis of a secondary reaction. Because of hole-filling and electrostatic attraction, biochar obtained by pyrolysis of wheat straw impregnated with MgCl 2 (WS Mg ) had the highest DEP removal rate of 95.969%. DEP removal efficiency of the five adsorbents followed the order WS Mg > WS Ca (88.701%) > WS (68.867%) > WS Na (53.852%) > WS K (50.845%). Hydroxyl radicals (•OH) signals were detected in these five adsorption systems, showing that EPFRs could activated H 2 O 2 to produce •OH. However, the five •OH signals had similar intensities, indicating that AAEMs had not significantly effects on the process of activation of H 2 O 2 to produce •OH by EPFRs. The results of this study are of great significance for understanding the formation and regulation of EPFRs and the utilization of biochar.
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CHEMOSPHERE
·
2022
·
IF 8.943
Lidong Kou,Qingfeng Fan,Yuhong Yang,Xianying Duan,Kai Jiang,Jing Wang
N -doped carbons have attracted extensive attention as catalysts for peroxymonosulfate (PMS) activation towards environmental remediation. However, synthesis of N -rich carbocatalysts is challenging and PMS activation mechanism is still unclear. Herein, novel N -rich porous carbocatalysts ( C -P x CN-T) were synthesized by carbonization of polyaniline nanorods coated g-C 3 N 4 . C –P 50 CN-900 (polyaniline content 50%) calcined at 900 °C had high surface area (358 m 2 /g), product yield (27.1%) and N content (12.27 at%). It showed superior performance in activating PMS to degrade and mineralize various phenolic pollutants in a wide pH range (2–11) and with the co-existence of water constituents. A positive correlation was observed between phenol oxidation rates and contents of C O, C –C/C C and graphitic N, which served as active sites to facilitate adsorption of pollutants and PMS on C –P 50 CN-900 and subsequent electron-transfer from pollutants to PMS. Overall, this study provides new insights into rational design of N -doped carbocatalysts and elucidation of electron transfer pathway in PMS activation.
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CARBOHYDRATE POLYMERS
·
2022
·
IF 10.723
Biyang Zhu,Yifan Chen,Shiyuan Chang,Huamai Qiu,Lijun You
Kinetic models and mechanism of isomaltooligosaccharides (IMOs) by hydroxyl ( OH) radicals-driven degradation in ultraviolet/hydrogen peroxide system were investigated. Electron paramagnetic resonance spectra indicated that UV radiation played an important role in the steady generation of OH radicals. The OH radicals could effectively decrease the molecular weight of IMOs and significantly oxidize hydroxy group into carbonyl and carboxy groups . Main components of IMOs were separated and identified by HPAEC-PAD and UHPLC-MS/MS methods. Degradation behaviors of IMOs were well fitted to pseudo first-order kinetics. The hydrogen abstraction by OH radicals from different C H sites at pyranose ring began a cascade reaction leading to cleavage of α-glycosidic linkage or C C bonds with formation of stable uronic/aldonic acids. Degradation rate was closely influenced by the degree of polymerization (DP) of IMOs, the initial concentrations of IMOs and H 2 O 2 . The results would pave the way for free radicals-driven degradation of polysaccharides .
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ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Jinxin Li,Dan Zhong,Yiru Chen,Kefei Li,Wencheng Ma,Shaobo Zhang,Jingna Zhang,Aoshuang Sun,Haijiao Xie
Coal pyrolysis wastewater (CPW) contained all kinds of toxic and harmful components, which would seriously threaten the natural environment and human health. However, the traditional advanced oxidation processes frequently failed to remove phenolic substances. An A 2 BO 4 -type perovskite (La 2 CuO 4 ) was successfully synthesized through sol-gel process and first applied in the treatment of CPW. More than 90% of 3, 5-dimethylphenol (DMP) was removed within 200 min at neutral conditions. Moreover, La 2 CuO 4 also displayed excellent catalytic activity and stability in the actual CPW treatment process. Results demonstrated that DMP was removed through the attack of ∙OH, ∙O 2 − and 1 O 2 in La 2 CuO 4 /H 2 O 2 system. The La 2 CuO 4 were more favorable for H 2 O 2 activation and have a lower adsorption energy than LaFeO 3 . XPS of fresh and spent La 2 CuO 4 illustrated that the decomposition of hydrogen peroxide (H 2 O 2 ) was mainly due to the redox cycle between surface copper and oxygen species. Moreover, the possible degradation pathway of DMP was deduced by identifying degradation products and analyzing density functional theory (DFT) calculations. This research provided a novel strategy for the development of perovskite-based catalytic materials on the treatment of practical CPW.
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ChemSusChem
·
2022
·Vol. 16
·期 3
·e202201496
·
IF 9.14
Cuiyu Huang,Jin Lin,Heqing Tang,Qin Wang,Tetsuro Majima,Nan Wang,Zhihong Luo,Lihua Zhu
Graphical Grind and sonicate : A green mechanochemical process is developed to prepare edge-selectively hydroxylated graphene (EHG) nanosheets. As-prepared EHG nanosheets have abundant OH groups at the edges and low defects in the basal planes, yielding good dispersibility in water, high near-IR photothermal conversion efficiency at 1064 nm, and excellent electrochemical performance. The production of water-dispersed graphene with low defects remains a challenge. The dry ball milling of graphite with additives produces edge-selectively functionalized graphene. However, the “inert” additives require a long milling time and cause inevitable in-plane defects. Here, the mechanochemical reaction of graphite with persulfate solved the above drawback and produced edge-selectively hydroxylated graphene (EHG) nanosheets through a 2 h ball-milling and a subsequent 0.5 h sonication. The mechanochemical cleavage of persulfate yielded SO 4 ⋅ − to spontaneously oxidize graphite to form the carbon radical cations selectively at edges, followed by hydroxylation with water of moisture. Because the O−O bond dissociation energy of persulfate is 20 % of the graphitic C−C bond, the rather low milling energy allowed the hydroxylation of graphite at edges with nearly no in-plane defects. The obtained EHG showed high water-dispersibility and excellent photothermal and electrochemical properties, thereby opening up a new door to fabricate graphene-based composites.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2022
·
IF 5.895
Rong Tian,Lan Zhou,Naihao Lu
The interactions between quercetin and bovine (or human) hemoglobin (Hb) were systematically investigated by fluorescence, UV–vis absorption spectroscopy, and molecular docking to demonstrate the structural mechanism by which quercetin affected the Hb redox state and stability. Quercetin could interact with the central cavity of the Hb molecule with one binding site to generate an Hb–quercetin complex, and the hydrophobic interaction played an important role in the formation of the complex. The binding constant for the Hb–quercetin complex at 298 K was observed to be 1.25 × 104 M–1. In addition, quercetin effectively inhibited Hb-induced lipid oxidation in liposomes or washed muscles, which was ascribed to the conversion to oxy-Hb and decreased hemin dissociation from met-Hb. Consistent with its lower abilities to bind Hb and scavenge free radicals, rutin (i.e., quercetin-3-rhamnosylglucsoside) did not significantly influence the redox state of Hb nor reduce hemin release from Hb, and subsequently, it less effectively inhibited Hb-induced lipid oxidation than quercetin. Altogether, the results herein provide novel insights into the antioxidant mechanism for quercetin and are beneficial to the application of natural quercetin in Hb-containing foods.
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