Polymers
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2022
·Vol. 14
·期 14
·2959
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IF 4.967
Jun Wang,Xiaocui Wen,Shaojun Jiang,Tao Chen
Inappropriate disposal of leaching residues from the lead-zinc tailings recovery process may result in environmental pollution. Its recycling and reuse remain a prevalent topic in environmental science and technology. It was roasted to prepare leaching residues-based materials (TLRS) in this work, and the TLRS were creatively used as the catalyst to active sodium persulfate (PS) to degrade organic pollutants. Degradation of tetracycline using the TLRS–PS system was evaluated, and the treating parameters were optimized. Roasting resulted in the exposure of active sites on TLRS surface, in which transition metals can donate electrons to PS to form SO4·−. SO4·−can further react with OH−to form ·OH. Formation of these radicals was confirmed by both quenching experiments and EPR analysis. Under optimized conditions, 85% of the TC can be degraded in 3.0 h, and ~50% of degraded TC was mineralized to CO2and H2O. The performance of TLRS barely changed after four reuses, suggesting the chemical stability of TLRS. The presence of dissolved substance in the water matrix could weaken the performance of the TLRS–PS system. A mechanism of TC degradation was proposed based on the experimental results and literature. These preliminary results provide us new insight on the reuse of lead-zinc flotation tailings.Keywords:leaching residues;tetracycline;persulfate activation;oxidative degradation;solid waste
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Huizhong Chi,Wenbiao Jin,Jianqiao Zhang,Yibin Xiu,Tao Xu
In recent years, there has been growing interest in the mechanism (radical or nonradical) of persulfate activation processes. In this study, the enhancement of naproxen (NPX) degradation in a Cu 0 /peroxymonosulfate (PMS) system by complexing reagents was investigated. Surprisingly, neocuproine (NCP) alters the nature of reactive species in the Cu 0 /PMS system. A high-valent copper species, Cu(III)-NCP, was found to dominate NPX degradation rather than radicals under acid conditions for the first time. Moreover, systematically designed experiments revealed that the Cu(III)-NCP complex was a strong selective oxidant that reacted with organics through a single electron transfer pathway. Meanwhile, the degradation efficiency of NPX was highly dependent on the solution pH and dosage of Cu 0 and NCP, but was irrelevant to the concentration of NPX. Additionally, the enhancement of NCP on other copper based PMS activation systems (i.e., Cu 2+ /HA/PMS and Cu 0 /HA/PMS systems) was investigated. Considering that the released copper can be removed by a simple precipitation method to meet the effluent standards, the new complex-enhanced Cu 0 /PMS system provided a new method to enhance the degradation efficiencies of pollutants by a copper-catalyzed Fenton-like system.
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Acta Biomaterialia
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2022
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IF 10.633
Kai Sun,Jiaying Yu,Jinzhong Hu,Jian Chen,Jia Song,Zhixin Chen,Zhuoer Cai,Zhuoxuan Lu,Liming Zhang,Zhifei Wang
The delivery of salicylic acid or its derivatives to tumor tissue in the form of nanomedicine is critical for the studies on their potential synergistic mechanism in tumor therapy and chemoprevention considering the dangerous bleeding in the high-dose oral administration. To deepen the understanding of their role in adjusting immunosuppressive tumor microenvironment (ITM), herein, we firstly developed a hypoxia-sensitive Fe-5,5′-azosalicylic acid nanoscale coordination polymer nanomedicines (FeNCPs) via a “old drugs new tricks” strategy for synergistic chemodynamic therapy (CDT) and remodulation of ITM to elevate antitumor immunotherapy effect. PEGylated FeNCPs could be reductively cleaved to release 5-aminosalicylic acid (5-ASA) and ferric ions by azo-reductase under hypoxic conditions, which could induce tumor cell death by Fenton reaction-catalysis enhanced CDT and 5-ASA-converted carboxylquinone to promote the production of •OH. Meanwhile, cyclooxygenase-2 (COX-2) and its enzymatic product prostaglandin E 2 (PGE 2 ), as immune negative regulatory molecules, can promote tumor progression and immune tolerance . The released 5-ASA as a COX inhibitor could suppress the expression of PGE 2 , and Fe 3+ was employed to reeducate M2-like tumor-associated macrophages (TAMs) to M1-like phenotype, which could initiate antitumor immune response to reach better antitumor immunotherapy. This work broadens the application of salicylic acid derivatives in antitumor immunotherapy, and provides a new strategy for their “old drugs new tricks”. Statement of Significance Cyclooxygenase-2 (COX-2) and its enzymatic product prostaglandin E2 (PGE 2 ), as immune negative regulatory molecules, facilitate the differentiation of immune cells into immunosuppressive cells to build the immunosuppressive tumor microenvironment, which can promote tumor progression and immune tolerance. Thus, down-regulation of COX-2/PGE 2 expression may be a key approach to tumor treatments. Meanwhile, as a class of inhibitors of COX-2/PGE 2 , the potential mechanism of aspirin or 5-aminosalicylic acid has been a mystery in tumor therapy and chemoprevention. To expand the application of aspirin family nanomedicine in biomedicine , herein, we firstly developed a hypoxia-sensitive Fe-5,5′-azosalicylic acid nanoscale coordination polymer nanomedicines via a “old drugs new tricks” strategy for synergistic chemodynamic therapy and remodulation of immunosuppressive tumor microenvironment to elevate antitumor immunotherapy effect.
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Journal of Water Process Engineering
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2022
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IF 7.34
Wenchao Liao,Shuyi Liao,Su Xu,Qingsong Li,Linbo Han
A chemical-less microwave enhanced photolysis process (named MW/UV) was established for sulfamethoxazole (SMX) degradation and the mechanisms were specifically studied. 96.7% of SMX could be removed in an extremely short reaction time of 140 s under 400 W of microwave and 23.0 mW/cm 2 of UV light at 254 nm. The half-live of SMX was greatly shortened to 5 s in MW/UV process, compared with 67 s in UV process and 1386 s in MW process. MW/UV process was also effective when applied to complex real water matrices, such as river water, seawater, and synthetic waste water. Non-thermal effects of microwave were found to play an essential role in elevating photolysis degradation efficiency. The ROS formation detected by quenching experiments and EPR test showed that SMX degradation by MW/UV followed non-radicals dominated method, although 1 O 2 and OH co-existed in this system. 16 intermediates in total were detected by HPLC-Q-TOF and three degradation pathways based on 1 O 2 and OH oxidation were proposed according to the structural characteristics of the intermediates. Besides, toxicity evaluation of SMX and its intermediates revealed that MW/UV process could effectively reduce the toxicity of SMX. This study provides an efficient and promising scheme for practical SMX degradation.
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MICROCHIMICA ACTA
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2022
·Vol. 189
·期 6
·1-11
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IF 6.408
Guo Jingjing,Liu Yangyang,Mu Zhao,Wu Shu,Wang Jueyu,Yang Yue,Zhao Min,Wang Yan
A bifunctional Ni-MOF nanosheet was synthesized and developed for label-free fluorescent detection of H 2 O 2 and glucose. The Ni-MOF exhibited intrinsic peroxidase-like activity and its catalytic activity was demonstrated to be originated from the hydroxyl radicals (•OH) produced in catalytic process. Since the generated •OH enabled terephthalic acid, the non-fluorescent organic ligand of Ni-MOF, to form a strongly fluorescent 2-hydroxy terephthalic acid, the Ni-MOF nanozyme was endowed with dual-function properties of mimicking peroxidase and emitting fluorescence. Based on this bifunctional Ni-MOF nanozyme, the proposed label-free fluorescence sensing strategy was applied to detecting H 2 O 2 and glucose with wide linear ranges of 0.1–20 mM and 8–30 μM, and low detection limits of 4.0 × 10 −5 M and 4.0 × 10 −6 M, respectively. Furthermore, the bifunctional Ni-MOF-based label-free sensing platform was successfully used for the glucose detection in human serum samples, showing good reproducibility and high accuracy. This strategy provides a green and sensitive method for the determination of small biomolecules in practical applications by the combination of enzyme cascade reaction. Graphical abstract
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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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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Jing Liao,Yuke Wu,Xueshan Chen,Huimin Yu,Yao Lin,Ke Huang,Jinyi Zhang,Chengbin Zheng
Hexavalent chromium (Cr(VI)), a confirmed human respiratory carcinogen, has attracted widespread attention due to its high toxicity and mobility in natural water systems. However, the developed catalytic colorimetric probes for Cr(VI) detection remain challenging, such as various species of Cr(VI) coexisting in water or acid buffer, the obvious interference from oxidizing ions at acidic pH, the synthesis of complex materials, and the consumption of hydrogen peroxide. In this work, a phenomenon of UV light-triggered chromate to produce singlet oxygen under neutral pH was found. An environmentally-friendly method based on the rapid oxidation of chromogenic substrates was thus developed for the highly specific and accurate detection of Cr(VI). Cr(VI) serves as both the active center and the target of this system, which ensures the rapidity, simplicity, and environmental protection of the proposed colorimetric strategy. Importantly, the neutral catalytic condition ensures that the predominant species CrO 4 2- can be accurately quantified and avoids the interference of oxidizing ions. Subsequently, a portable analytical system integrating an array of LED lamps, a miniature color reading device, and a developed smartphone-based program was successfully developed to accomplish high-throughput and on-site analysis of Cr(VI) in natural water. The proposed method provides a rapid screening and water quality assessment tool for the faster, more cost-effective, and accurate detection of Cr(VI) in the water system.
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Journal of Cleaner Production
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2022
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IF 11.072
Wenli Yao,Mingzhe Li,Changduo Sun,Yanlong Liu,Mengling Ma,Fengjuan Chen,Lei Zhou,Yian Zheng
Removal of perfluorinated compounds (PFCs) from the environment is a major challenge due to their refractory, persistent and bioaccumulative properties. In this study, trace Co coupled via Co–P coordination and tourmaline (TM) doped g-C 3 N 4 was fabricated (marked as Co/TM/g-C 3 N 4 ) and used as the catalyst for activating peroxymonosulfate (PMS) to remove emerging PFOA under visible light irradiation. Several affecting parameters were systematically investigated, inlcuding Co/TM/g-C 3 N 4 dosage, PMS concentration, initial pH, as well as coexisting Cl − , HC O 3 − , H 2 P O 4 − , N O 3 − and humic acid . Under the conditions of 0.5 g/L Co/TM/g-C 3 N 4 , 2.5 g/L PMS and pH 3.0, the developed synergistic system had the ability for 81.11% removal of PFOA within 4 h, 67.64% removal after the fourth run, and also could be effectively applied in actual water bodies. During the degradation process , π-π*, N–C N and graphite N played the vital role, with the final defluorination rate of 31.12% at 4 h. Free radical quenching and quantitative analysis, as well as electron paramagnetic resonance was used to verify the free radical and non-free radical pathways for PFOA removal, with the findings that S O 4 • − (2.61 μM at 1 h), •OH (0.067 μM at 4 h), O 2 • − , h + , and O 1 2 were involved with possible time-dependent. By liquid chromatography-mass spectrometry analysis, the short-chain intermediates of C3–C7 were proposed and identified. From this study, trace Co coupled and TM doped g-C 3 N 4 demonstrated higher catalytic potential to activate PMS for visible-light synergistic PFOA removal, with the expectation of achieving a cleaner water environment for human beings.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Xinyu Hu,Juntao Wang,Jing Wang,Yao Deng,Huidi Zhang,Tao Xu,Wenlei Wang
In this work, a high-energy β electron beam was applied to promote the generation and directional inward migration of surface oxygen defects. The valence band potential changed to a high potential due to the transfer of surface oxygen vacancies on BiVO 4 /Bi 2 O 3−x . Interface oxygen vacancies have significant advantages in inducing the formation of oxygen vacancy levels and reducing the band gap energy. Surface oxygen vacancy and vacancy levels can prevent the recombination of photogenerated carriers. The electrons enriched in the surface oxygen vacancies can remarkably activate PMS with O−O bonds to degrade ciprofloxacin (CIP). The degradation kinetic constant and CIP mineralization rate of BiVO 4 /Bi 2 O 3−x -450/PMS were 2.09 and 1.51 times higher than those of BiVO 4 /Bi 2 O 3−x /PMS, respectively. BiVO 4 /Bi 2 O 3−x -450 with a lower relative content of surface oxygen vacancies (24.70%) exhibited a stronger activation ability. Obviously, the change of band structure caused by interface oxygen vacancies is the reason for increasing photoactivation efficiency of PMS.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2022
·Vol. 30
·期 1
·1386-1398
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IF 5.19
Yan Shiquan,Lai Xinting,Fan Lingling,Wang Tianhao,Yao Yuyuan,Wang Wentao
Wastewater containing organic pollutants with high toxicity and poor biodegradability poses a considerable threat to human health and the ecosystem. Although adsorption and advanced oxidation processes (AOPs) are currently the most widely used technologies for wastewater treatment, limitations of these two independent processes make the treatment effect unsatisfactory. Herein, a system of integrating adsorption and subsequent in situ AOPs is established by a 3D carbon aerogel embedded with Fe-doped carbonitrides (Fe-NC/CAG). The SEM and BET analysis demonstrate that Fe-NC/CAG possesses porous structures with a specific surface area of 518.7 m 2 /g. The XRD result indicates the formation of Fe 0 and Fe 3 O 4 in Fe-NC/CAG. The impacts of operational parameters such as Fe-NC/CAG dosage, pollutants concentration, temperature, initial pH, and inorganic ions on the adsorption efficiency are investigated. The adsorption kinetics is predominantly based on the pseudo-second-order model. After adsorbing organic pollutants, the Fe-NC/CAG is immersed in peroxymonosulfate (PMS) solution. The adsorbed pollutants are in situ degraded by PMS-based AOPs, leading to the regeneration of Fe-NC/CAG. At optimum conditions, the integrating process established by Fe-NC/CAG achieves over 90% removal of antibiotics, phenolics, and dyes as well as keeps stable performance even after 6 cycles. This integrating adsorption and AOPs system is expected to open up a rich field for wastewater treatment.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Jia Xie,Yingpeng Yang,Hao Zhang,Saisai Chen,Zhengjun Lv,Yujun Zhou,Junwen Qi,Xiuyun Sun,Jiansheng Li
Advanced oxidation processes (AOPs) were appealing wastewater treatment options yet practices were hampered by reactor design and diminished performance in complex water matrices. Herein, one-step-pyrolysis strategy was proposed for large-scale synthesis of ZIF-67 derived conductive Co/N carbon hollow fiber ultrafiltration membrane to achieve exceptional availability of catalytic sites and interference prevention from macro molecular substances by size exclusion. Benefitting from the microenvironment modulation and electric field assistance (−1 V, membrane as the cathode), the bisphenol A (as a model micropollutant) can be efficiently removed with enhanced mass transfer of flow-through process (modified apparent reaction rate constant of 1260 μM g cat -1 s −1 ) and the active cobalt species were cycled via electroreduction thus showing exceptional sustainability with nearly zero Co leaching even after 24 h operation. The synergy effects between separation and catalysis alleviated the deteriorated AOPs efficiency and membrane fouling caused by macromolecular organic matter. The integrated membrane system provides new insight into rational design of catalytic membrane and system engineering for advanced water purification.
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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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