CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Xuantong Chen,Zhen Guo,Juemiao Liu,Fei Wu,Cheng Cheng,Heng Lin,Wei Ren,Hui Zhang
Waste herb residue biochar (WBC) was synthesized to activate peroxydisulfate (PDS) for the removal of different micropollutants. WBC prepared at 700 °C (WBC700) exhibits discrepant adsorption and PDS catalytic performance to three pharmaceuticals and four phenolic compounds. At 60 min reaction time, the adsorptive removal by 0.5 g/L WBC700 varied from 31.3% (clofibric acid) to 97.6% (4-chlorophenol), while the apparent removal ranged from 36.1% (clofibric acid) to 99.5% (4-chlorophenol) when 0.5 g/L WBC700 and 1.0 mM PDS were applied. The oxidation of the micropollutants involves electron transfer mechanism via the surface-confined metastable reactive complexes (WBC-PDS*), which was verified by electrochemical tests, quenching experiments, electron paramagnetic resonance, Fourier transform infrared and in-situ Raman spectroscopy. The observed pseudo first-order kinetic constant ( k obs ) of organic removal did not exhibit a good correlation with its electrochemical redox descriptor (half-wave potential, φ 1/2 , for example) as reported in the previous studies. Instead, the surface oxidation rate constant ( k oxid ), determined from a dynamic model considering liquid-solid mass transfer of micropollutant and the sequent surface oxidation by WBC-PDS* complexes, was highly related to φ 1/2 . In parallel, the liquid-solid mass transfer coefficient ( K L a) of micropollutant was obtained from a similar model excluding the surface oxidation, and k obs showed a more significant association with K L a than with adsorption capacity ( Q e ). This study provides a promising approach to understand the role of adsorption and surface oxidation in an electron transfer-dominated persulfate activation process.
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BIORESOURCE TECHNOLOGY
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2022
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IF 11.889
Nan Jiang,Jinling He,Ai Zhang,Yongquan Zhou,Ming Zheng,Xianbao Xu,Andere Clement Miruka,Xiang Li,Yanan Liu,Gang Xue
In this study, the combination of dielectric barrier discharge plasma (DBD) with calcium peroxide (CaO 2 ) achieved significant synergistic effects in promoting hydrolysis of waste activated sludge (WAS) and short-chain fatty acid (SCFA) production during anaerobic fermentation. Compared with the control, DBD/CaO 2 pretreatment increased SCFA production by 116 %, acetic acid ratio by 39 %, and sludge reduction by 30 % under the optimal conditions (discharge power = 76.5 W, CaO 2 dosage = 0.05 g/g VSS). Mechanism investigations elucidated that DBD/CaO 2 enhanced the generation of •OH, 1 O 2 , and •O 2 − , synergistically promoted decomposing extracellular polymeric substances (EPS), lysing cells, releasing biodegradable substances, and enhancing acetic acid-enriched SCFA accumulation from fermentation. Meanwhile, Illumina MiSeq sequencing analysis revealed that the enrichment of hydrolytic and SCFAs-forming bacteria and the decrease in SCFAs-consuming bacteria by DBD/CaO 2 treatment also contributed. This work provides an effective method to boost the SCFA production from WAS fermentation.
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ACS Applied Materials & Interfaces
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2022
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IF 10.383
Wenjie Feng,Wanrui Shi,Ze Wang,Yanqi Cui,Xinxin Shao,Shuwei Liu,Li Rong,Yi Liu,Hao Zhang
Ferroptosis has been considered as a promising pathway to overcome apoptosis-induced tumor chemoresistance. However, the antitumor efficacy of ferroptosis-inducing agents is still limited because of the complexity and diversity of tumor microenvironments. Herein, we demonstrate a triple ferroptosis amplification strategy for tumor therapy by associating iron-based nanocarriers, ferroptosis molecular drugs, and H2O2-producing enzymes. Fe(III)-Shikonin (FeShik) metal-polyphenol-coordinated networks are employed to load a ferroptosis inducer of sorafenib (SRF) inside and glucose oxidase (GOx) outside, thus producing SRF@FeShik-GOx supramolecular nanomedicines (SNs). After delivering into glutathione (GSH)-overexpressed tumor cells, FeShik will disassemble and release Fe2+ to induce cell death via ferroptosis. At the same time, GOx executes its catalytic activity to produce an acid environment and plenty of H2O2 for stimulating •OH generation via the Fenton reaction. Moreover, SRF will suppress the biosynthesis of GSH by inhibiting system Xc–, further deactivating the enzymatic activity of glutathione peroxidase 4 (GPX4). Up-regulation of the oxidative stress level and down-regulation of GPX4 expression can dramatically accelerate the accumulation of lethal lipid peroxides, leading to ferroptosis amplification of tumor cells. The current strategy that utilizes ferroptosis-inducing agents as both nanocarriers and cargoes provides a pathway to enhance the efficacy of ferroptosis-based tumor therapy.
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高影响因子
POLYMERS FOR ADVANCED TECHNOLOGIES
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2022
·Vol. 33
·期 10
·3718-3727
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IF 3.348
Yang You,Anna Zheng,Dafu Wei,Xiang Xu,Yong Guan,Jianding Chen
As an essential elastomer used in edge technologies, fluorosilicone rubber (FSR) suffers serious oxidative aging problem when serving at high temperature. In this study, a small amount of reduced graphene oxide (rGO) was added to FSR, and the resulting rGO/FSR compounds were vulcanized using 2,5-dimethyl-2,5-di(tert-butyl) peroxyhexane as the vulcanizer. The dispersion of rGO was investigated using scanning electron microscope. The mechanical properties and thermal-oxidative stability of the rGO/FSR vulcanizates were investigated via thermal aging test at 230°C for 72 h, thermogravimetric analysis (TGA), and isothermal degradation test at 280, 320, and 350°C. The results showed the small addition of rGO (0.5 wt%) significantly improved the thermo-oxidative stability of FSR. In particular, the FSR incorporating of 0.5 wt% of rGO could maintain more than 85% of tensile strength after aging at 230°C for 72 h. The FSR incorporating of 0.5 wt% of rGO can maintain more than 90% of initial weight after aging at 350°C for 12 h. The experiment of scavenging hydroxyl radical by rGO, and quantum chemistry calculation indicated rGO containing aryloxy radicals can scavenge the initial radicals during thermal degradation of FSR, which might be prime reason for the antioxidant properties of rGO.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Mengjie Pu,Daqi Ye,Jinquan Wan,Bentuo Xu,Wei Sun,Wei Li
A novel peroxymonosulfate (PMS) catalyst, zinc-based metal–organic framework electrospinning (ES) nanofibers membrane (short for ZIF-65/PAN) was firstly fabricated and used for the degradation of aqueous ciprofloxacin (CIP). Physicochemical properties, catalytic performance, stability, reusability, and the regeneration of ZIF-65/PAN was observed and conducted. Influence of various parameters including ZIF-65 loading content, reaction temperature, initial pH, and competitive organic molecules on CIP degradation was investigated. Reactive active species and degradation intermediates that involved in ZIF-65/PAN/PMS/CIP process were identified. Corresponding reaction mechanisms were speculated. The results indicate that the easy-separation ZIF-65/PAN nanofibers exhibit high efficiency for PMS activation, 89.2 % of CIP was degraded within 60 min, with up to 87.5 % of PMS utilization efficiency. ZIF-65/PAN was renewable through simple layer-by-layer self-assembly, thus shows good prospect in future applications. 26.4 % of surface Zn 2+ of ZIF-65/PAN exists in the form of + III oxidation state after activation, indicating the role of zinc catalytic site. Through activation, oxidative active species SO 4 ·− , ·OH, and 1 O 2 was generated, CIP was thus degraded through mainly-three pathways. This study provides novel ideas for the application of MOF-based membrane on PMS based advanced oxidation processes.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Chu Dai,Xike Tian,Yulun Nie,Wei Fu,Jiatang Wang
Most researches focus on design and optimization of heterogeneous Fenton catalyst itself to drive H 2 O 2 decomposition into • OH radicals. In this study, we reported the significant impact of the interaction mode of H 2 O 2 and CuMnO 2 (namely H 2 O 2 occurrence form) on the Fenton-like performance. The interaction mode of H 2 O 2 largely exposed to Cu atom active site (CMH-L) led to a superior ofloxacin (OFX) degradation efficiency of 93% compared with H 2 O 2 middle exposed around the Cu atoms (CMH-M, 84%) and small part exposed around the Cu atoms (CMH-S, 50%). The effect of H 2 O 2 occurrence forms on catalytic activity were confirmed by analyzing their fraction and the relevant rate constant with the correlation was 98%. And the relevant interfacial reaction mechanism was detailed explored based on density functional theory calculation, a series of probe experiments and quantitative analysis of H 2 O 2 utilization efficiency and • OH generation. It revealed that Cu atom arrangement on CuMnO 2 can induce the different H 2 O 2 occurrence form, and compared with CMH-M especially CMH-S (1.486 and 1.591 Å), CMH-L has the shortest elongation of O-O bond (1.477 vs. 1.468 Å in free H 2 O 2 ) together with the smallest O-H 1 and O-H 2 (0.988, 1.022 Å), which were more likely to decomposition H 2 O 2 into • OH, while it was more likely to inefficient transformation H 2 O 2 into O 2 in CMH-S system. Thus, this work provided a new insight for improving the heterogeneous Fenton catalytic performance via altering the interaction mode of H 2 O 2 and catalyst, which should be the fundamental reason for efficient H 2 O 2 activation into O 2 or • OH.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Tong Liu,Yang Liu,Peng Zhou,Zhaokun Xiong,Heng Zhang,Chuanshu He,Ye Du,Gang Yao,Bo Lai
As one of the most promising advanced oxidation processes , the activation of S(IV) by iron-based materials to produce SO 4 •− has become a hot technology for the degradation of organic pollutants . However, the mechanism of radical chain reactions has not been clearly explored. Herein, we established a novel AOP system based on the combination of zero-valent iron (ZVI) and potassium pyrosulfite (PPS). Combined with the degradation trends of CBZ and the change of DO concentration, the system was proposed to be divided into a slow initiation stage in 5 min and a rapid degradation stage in 5 − 10 min. Through a series of quenching experiments, electron paramagnetic resonance tests and several probe experiments, the mechanisms of two radical chain reactions were proposed between ZVI and PPS: the first one produced O 2 •− and HO • , and the other produced SO 3 •− , SO 5 •− , SO 4 •− and HO • . The two-stage reaction and two radical production paths of the ZVI/PPS system were proposed for the first time, which provided theoretical guidance for the practical application of the ZVI/PPS system. The ZVI/PPS system has been found to have excellent environmental adaptability in the treatment of industrial wastewater .
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BIOMACROMOLECULES
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2022
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IF 6.978
Xueping Kong,Qiuyan Chen,Guofeng Wan,Yimeng Yang,Huimei Yu,Bao Li,Lixin Wu
To enhance the efficacy of tumor therapy, the collection of functional components into a targeting system shows advantages over most homogeneous materials in inducing apoptosis of cancer cells. The security and targeting of therapeutic agents also require the effect combination of additional components. However, the construction of multifunctional composites in a simple system with intelligent cooperative responsiveness remains a challenge. Herein, a reduced polyanionic cluster (rP2W18) bearing the absorption at the near infrared (NIR) II region is used as a core carrier to bind the positively charged doxorubicin hydrochloride (DOX) through ionic interaction. To reduce the physiological toxicity, hyaluronic acid grafting β-cyclodextrin side chains is used to cover the ionic complex through host–guest inclusion to DOX. When the nanocomposite is activated by local laser exposure, the final three-component therapeutic agent is demonstrated to present targeted photothermal conversion capability and chemodynamic activity together with chemotherapy. With the controlled release of DOX under the stimulation of mild acidity in the tumor region and photothermal effect, the exposed rP2W18 is aroused by hydrogen peroxide overexpressed in a tumor microenvironment to produce toxic reactive oxygen species, 1O2. This work presents an opportunity for the development of a nanocomposite in NIR-II photothermal/chemo-therapy and chemodynamic synergistic therapy.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Xin Liu,Peng Xu,Shiqi Xie,Lei Wang,Zhuoyu Yang,Pengfei Zhu,Jingwei Ma,Qiulai He,John C. Crittenden
Zero-valent copper particles (Cu 0 ) used to degrade pollutant due to its in-site generation and activation of hydrogen peroxide (H 2 O 2 ), while the disproportionation of Cu + limited the efficacy. In this study, spiking chloride ion (Cl − ) into zero-valent copper (Cu 0 ) system (Cl − /Cu 0 system) enhanced greatly acetaminophen degradation. The addition of Cl − not only reduced the dismutation reaction of Cu + , but also helped the comproportionation reaction of Cu 0 and Cu 2+ , leading to much generation of Cu + and H 2 O 2 . Hydroxyl radical ( OH) and reactive chlorine species were identified as the dominant reactive oxidants in the Cl − /Cu 0 system with its contribution ratio of degrading acetaminophen being respectively 73.4 % and 23.8 %. In the Cl − /Cu 0 system, Cu + was released by H + corrosion from Cu 0 , and then Cu + coupled with Cl − forming Cu-Cl complexes; Meanwhile, the reaction of O 2 and the species of Cu + (e. g. Cu-Cl complexes and Cu + ) produced H 2 O 2 and, then the species of Cu + catalyzed H 2 O 2 to form OH; Thereinto, partial OH was shifted by Cl − to reactive chlorine species. Except for fulvic acid , coexisting substrates such as sulphate, nitrate and phosphate ions had no obvious inhibition impact on oxidizing acetaminophen in the Cl − /Cu 0 system. Furthermore, the Cl − /Cu 0 system presented a good removal rate of acetaminophen in three actual water samples. Moreover, three kinds of dyes and painkillers was removed over 78 % in the Cl − /Cu 0 system. The residual total dissolved copper was under II-level of environmental quality standards for surface water in China by alkali precipitation and filtration after reaction. Therefore, the study provided a new idea to enhance Cu 0 for the purification of pollutants.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Yan Xiao,Liangliang Xiong,Yin Xu,Hui Zhang
In recent years, visible light assisted advanced oxidation processes (AOPs) are appealing in the elimination of pollutants. Herein, an innovative and eco-friendly visible light enhanced Fe 3+ -nitrilotriacetic acid system for the activation of peroxydisulfate (Vis/Fe 3+ -NTA/PDS) was proposed for the removal of bisphenol A (BPA). Fe 3+ -NTA could be dissociated through ligand-to-metal charge transfer (LMCT) to realize the generation of Fe 2+ for the continuous activation of PDS to remove BPA. The use of 0.10 mM Fe 3+ , 0.10 mM NTA and 1.00 mM PDS led to 97.5% decay of 0.05 mM BPA and 66.3% of TOC removal in 30 min with the illumination of visible light at initial pH 3.0. The sulfate and hydroxyl radicals were proved to be the dominant species leading to BPA removal by means of radical scavenging experiments, radical probes and electron paramagnetic resonance (EPR) technique. The effects of various operating parameters, natural water constituents as well as different water matrices on BPA abatement were explored. The intermediate products of BPA degradation were identified and a possible transformation pathway was proposed. Briefly, this research provides an attractive strategy for the remediation of refractory wastewater using NTA assisted with visible light in the homogeneous Fe 3+ /PDS system.
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JOURNAL OF MEMBRANE SCIENCE
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2022
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IF 10.53
Jianyong Feng,Xing Li,Hang Li,Yanling Yang
Membrane biofouling is a challenge for biocarriers facilitated gravity-driven membrane (GDM) systems to achieve high-efficiency filtration in decentralized drinking water treatment . The purpose of this study was to investigate the effects of vacuum ultraviolet (VUV) as a pretreatment on membrane fouling , permeate water quality and bacterial communities. VUV pretreatment was found to significantly reduce the cake layer resistance by 24.4% and the membrane pore resistance by 40.0% ( p < 0.05), resulting in a 22.2% increase in stable flux. The removal of low molecular weight neutrals and protein-like materials was enhanced by 22.5% and 40.1% respectively after VUV pretreatment. The heterogeneity of the biofouling layer was improved by VUV pretreatment, and the porosity and roughness were increased by 227.5% and 46.5%, respectively. The application of VUV pretreatment resulted in a larger nanoparticle size in the biofouling layer suspension (peak at 85.4 nm), improvement in the membrane hydrophilicity, and a decrease in protein-like substances adhesion. The richness and diversity of the bacterial community were decreased by VUV pretreatment. The bacterial community structure had the highest mantel correlation with biopolymers (r = 0.89). Overall, VUV pretreatment can be a promising strategy to effectively alleviate membrane biofouling in biocarriers facilitated GDM systems.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Lu Yang,Haixia Zhu,Ruoxi Zhao,Zhijia Zhang,Bin Liu,Haijiang Gong,Yanlin Zhu,He Ding,Shili Gai,Lili Feng
Activatable nanosystem for cancer therapy are of considerable attention in the field of theranostics. Nevertheless, constructing activatable nanosystem with specific response performance and turn “on–off” treatment mode still remains an enormous challenge. Here, we developed a cascade reaction nanomedicine for highly efficient cancer theranostics by constructing and delivering multifunctional activatable nanocapsules into the tumor region. 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS, activatable agent) and camptothecin (CPT, chemotherapeutic drug) have been encapsulated into large pore-sized dendritic macroporous silica coated Fe 3 O 4 nanocapsules (Fe 3 O 4 @DMSN), further modified with poly(vinylpyrrolidone) (PVP) to improve the solubility and biocompatibility, defined as [email protected] NCs. The prepared nanocapsules can be specifically responded to tumor microenvironment by a nanozyme-catalyzed two-step acceleration process to turn on its hyperthermia effect and imaging performance due to the production of oxidized ABTS, simultaneously. Moreover, the generating hydroxyl radicals are attributed to the overexpressed H 2 O 2 in the tumor microenvironment and the self-depletion intracellular GSH endow [email protected] with the capability of promoted chemodynamic therapy, therefore resulting in significant therapeutic effect in connection with chemotherapy and tumor microenvironment-mediated photothermal therapy. What’s more, the H 2 O 2 -activated and tumor microenvironment improved profiles endow the nanocapsules to be specific to tumors, avoiding the damage to normal tissue. These prominent characteristics of [email protected] NCs may open up a new trail to explore activatable nanoplatform for imaging-directed smart, precise, and noninvasive tumor theranostics.
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