CHEMOSPHERE
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2021
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IF 7.086
Yong Chen,Junfeng Zhao,Lu Hu,Jing Tian,Yong Liu
Most metal-organic frameworks (MOFs) are synthesized from carboxylate and metal precursors by hydrothermal process, which will consume a large amount of solvent and carboxylate. To address this issue, a new strategy for Cu-based MOFs was developed, in which the Cu-based MOFs was obtained by using abundant natural polymer (tannic acid) as one of the precursors and using high-energy ball milling to achieve a self-assembly of tannic acid and copper sulfate. Based on this strategy, a novel Cu-based MOFs derivative (Cu x O@C composite) was synthesized by high-temperature sintering of Cu-based MOFs and used for sulfamerazine (SMR) removal via O 2 activation. The BET specific surface area and average pore size of Cu x O@C composite were 110.34 m 2 g −1 and 21.06 nm, respectively, which made Cu x O@C composite had the maximum adsorption capacity ( Q max ) for SMR of 104.65 mg g −1 and favored the subsequent degradation of SMR. The results from XRD and XPS indicated that Cu x O@C composite contained a lot of Cu 0 and Cu 2 O with the sizes of 76.6 nm and 9.8 nm, respectively, which led to its high performance of O 2 activation. The removal efficiency of SMR and 90.2% TOC achieved 100% and 90.2%, respectively in the Cu x O@C/air system at initial pH of 4.0, air flow rate of 100 mL min −1 , Cu x O@C dosage of 1 g L −1 and reaction time of 30 min. Reactive species, including H 2 O 2 , OH and O 2 - radicals were detected in the Cu x O@C/air system, and OH and O 2 - were mainly responsible for the degradation of SMR.
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CARBOHYDRATE POLYMERS
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2021
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IF 9.381
Wentao Wang,Qicheng Zhang,Ming Zhang,Xintong Lv,Zihan Li,Mohsen Mohammadniaei,Ninglin Zhou,Yi Sun
Wound bacterial infections and tumor recurrence are the main reasons for the poor prognosis after primary tumor resection. Here, we fabricated a novel therapeutic nanocomposite using chitosan (CS) hydrogel combined with black phosphate nanosheets (BPNSs) and in situ grown copper nanoparticles (CuNPs). The obtained hydrogel ( [email protected] @CuNPs), possessing a remarkable temperature-sensitive spongy-like state, offered 24.98 % blood clotting index. The released [email protected] could produce reactive oxygen species (ROS) to kill infected invasive bacteria (98.1 %) and inhibit local residual tumor cell regeneration (11.3 %). Moreover, by coupling the photothermal properties of BPNSs , the [email protected] showed 19.6 % penetration rate to cross the blood tumor barrier (BTB) for treating brain tumors. The hydrogel platform was further combined with aPD-L1-based immunotherapy to employ its synergetic therapeutic effect in the prevention of tumors. The in vivo studies showed that biodegradable hydrogel could hold a great potential as a novel strategy for improving postoperative therapy and multi-tumor treatments.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Jie-xia Li,Ling-min Zhang,Cheng-cheng Liu,Qian-ni Wu,Song-pei Li,Xue-ping Lei,Yu-gang Huang,Gui-ning Feng,Xi-yong Yu,Xian-qiang Sun,Zhao-ming Guo,Ji-jun Fu
In recent years, chemodynamic therapy (CDT) has gained increasing interest in cancer treatment. In contrast to photodynamic therapy and sonodynamic therapy, extrinsic excitations such as laser or ultrasound are not required in CDT. As a result, the CDT performance is not limited by the penetration depth of the external irritation. However, CDT relies heavily on hydrogen peroxide (H 2 O 2 ) in the tumour microenvironment (TME). Insufficient H 2 O 2 in the TME limits the CDT performance, and the most reported methods to produce H 2 O 2 in the TME are dependent on oxygen supply, which is restricted by the hypoxic TME. In this study, H 2 O 2 self-providing copper nanodots were proposed, and the drug doxorubicin (DOX) was successfully loaded to construct DOX-nanodots. Our results showed that the nanodots produced H 2 O 2 in the weakly acidic TME due to the peroxo group and further generated the most active hydroxyl radical ( OH) through the Fenton-like reaction. This process was pH-dependent and did not occur in a neutral environment. In addition to OH, the nanodots also produced singlet oxygen ( 1 O 2 ) and superoxide anions (O 2 – ) in the cancer cells. The copper nanodots performed promising CDT against breast cancer in vitro and in vivo, with enhanced cell apoptosis and decreased cell proliferation . The combination of chemotherapy and CDT using DOX-nanodots further improved the therapeutic effects. The treatments showed good biocompatibility with no obvious toxicity in major tissues, possibly due to the specific OH generation in the weakly acidic TME. In summary, the H 2 O 2 self-providing copper nanodots in combination with DOX showed promising cancer-curing effects due to the oxygen-independent and tumour-specific production of reactive oxygen species and the cooperation of chemotherapy.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
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IF 8.128
Wenlan Jia,Fuping Tian,Mengjie Zhang,Xinyi Li,Sheng Ye,Yanfu Ma,Wangyin Wang,Yifu Zhang,Changgong Meng,Guang Zeng,Jian Liu
Developing low-cost non-precious metals as efficient catalysts for the reduction of toxic 4-nitrophenol (4-NP) to useful 4-aminophenol (4-AP) have received increasing attention in recent years. Herein, a novel and efficient Cu-based catalyst Cu/Cu x O@CN (carbon doped with nitrogen) was prepared via a facile method from pyrolysis of bi-ligand MOFs material Cu 2 (BDC) 2 (BPY) (BDC = p-Phthalic acid, BPY = 4,4′-bipyridyl) in Ar atmosphere. Characterization results revealed that N doping in carbon matrix favors the development of mesoporous structure, the formation of more defect sites in carbon matrix, better dispersion of Cu/Cu x O nano particles, and maintenance of Cu species in metallic Cu state (the active site), all of which contribute to a superior catalytic activity for 4-NP reduction with a pseudo-first-order rate constant as high as 0.126 s −1 (the molar ratio of NaBH 4 to 4-NP is 400), nearly 11 times higher than its counterpart Cu/Cu x O@C without N doping (0.011 s −1 ). The activation energy for 4-NP reduction to 4-AP catalyzed by Cu/Cu x O@CN was determined as 55.6 kJ mol −1 (the molar ratio of NaBH 4 to 4-NP is 100). In addition, Cu/Cu x O@CN showed excellent reusability in successive 6 cycles. The facile synthesis and superior catalytic activity make Cu/Cu x O@CN a promising catalyst in industrial applications for many other similar reaction systems.
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ACS Biomaterials Science & Engineering
·
2021
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IF 4.749
Zu-E. Hu,Jun Li,Zhe-Ning Wu,Yun-Jie Wei,Yan-Hong Liu,Na Wang,Xiao-Qi Yu
Chemodynamic therapy (CDT) is a kind of method utilizing hydroxyl radicals (•OH) generated by Fenton or Fenton-like reactions in situ to kill tumor cells. Copper, a cofactor of many intracellular enzymes, which has good biocompatibility, is a transition metal with extremely high efficiency in the Fenton-like reaction. However, when the intracellular free copper exceeds the threshold, it will bring serious side effects. Hence, we used the chelation between glutathione (GSH) and copper ions to produce a nanocatalytic drug, which was named as Cu–GSSG NPs, to fix free copper. With the aid of hydrogen peroxide (H2O2) in vitro, Cu–GSSG NPs catalyzed it to •OH radicals, which could be confirmed by the electron spin resonance spectrum and the degradation experiment of methylene blue. Based on these results, we further studied the intracellular properties of Cu–GSSG NPs and found that Cu–GSSG NPs could react with the overexpressed H2O2 in tumor cells to produce •OH radicals effectively by the Fenton-like reaction to induce cell death. Therefore, Cu–GSSG NPs could be a kind of potential “green” nanocatalytic drug with good biocompatibility to achieve CDT.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Huan Xia,Hailan Qin,Yushan Zhang,Hang Yin,Qiang Li,Fei Pan,Dongsheng Xia,Dongya Li,Haiming Xu
Enhance the concentration of singlet oxygen ( 1 O 2 ) to ameliorate the photocatalytic performance is a promising strategy. Therefore, Z-scheme Mo 2 S 3 /BiOCl heterostructure with rational oxygen vacancies (OVs) was successfully synthesized by in-situ template method to tackle these issues. Characterization results reveal that the OVs were efficiently passivated by forming Mo–O bond at the interface of Mo 2 S 3 and BiOCl. Moreover, the photocatalytic mechanism research reflects that the interfacial electric field not only enhance the spatial separation and migration efficiency of the photo-induced carriers but also benefit producing abundant 1 O 2 , and thus TC-HCl was purified 90.8% in 90 min. Meanwhile, the contribution of the reactive oxygen species to the photocatalytic activity and the formation path of 1 O 2 were comprehensively studied for the first time. This work provides a new avenue to study the formation path of 1 O 2 and offer a polishing strategy to mend the photocatalytic activity by modulate the concentration of 1 O 2 .
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NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 13
·6108-6119
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IF 3.591
Siyi Li,Xuehui Zhao,Hongwei Zhang
It is very important to reduce the oxidation of free radicals in organic membrane materials for the stability and safety of drinking water production treatment processes. This paper presents a new method for the qualitative and quantitative determination of free radicals in sodium hypochlorite solution by electron spin resonance (ESR) and salicylic acid spectrophotometry. Experiments show that the free radical scavenging rate reaches over 86% after the addition of 0.5 wt% nano-particles. PVDF–PVP/TiO2 and PVDF–PVP/CNT modified membranes are prepared by blending polyvinylidene fluoride (PVDF) with nano titanium dioxide (nano-TiO2) and carboxyl-modified multi-wall carbon nanotubes (MWCNTs-COOH), and are treated in 2000 ppm sodium hypochlorite solution for 30 days. Through surface chemistry (FTIR, XRD), surface morphology (SEM), surface hydrophilicity (contact angle), surface electronegative (zeta potential) and mechanical properties tests, the changes of membrane properties are analyzed during aging. The experimental results show that the nano-particles have a quenching effect on free radicals and inhibit defluorination. It has been proved that under the action of nano-additives, the erosion of free radicals on the membrane material is reduced, the aging rate of the membrane material is decreased, and the chemical stability of the membrane material is improved. In this paper, the reason and mechanism of anti-aging of the nano-particle modified membrane are analyzed, which provides theoretical support for future membrane cleaning technology and prolonging the service life of the membrane.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Min Yu,Changduo Sun,Luhan Wang,Kun Zang,Mingzhe Li,Lei Zhou,Yian Zheng
Semi-coke (SC) is a solid waste of coal chemical process, and the comprehensive utilization of SC is a challenging issue. Based on physicochemical characteristics, SC was firstly utilized as a mineral biochar for activating persulfate (PS) to promote simultaneous degradation of sulfadiazine (SDZ) and tetracycline (TC) in a binary mixture. The influencing parameters were systematically investigated. The dominant reactive oxygen species (ROS) were identified by combination of quenching experiments and electron spin resonance (EPR) analysis. Subsequently, possible activation mechanism and degradation pathways were also proposed. With the evolution of SDZ and TC in SC/PS system, the Vibrio fischeri was used to examine the acute toxicity to explore the detoxification efficiency. The experimental results indicated that in such a binary system, a mutually promoted degradation occurred between SDZ and TC, and at optimized conditions of 0.75 g/L PS, 0.50 g/L SC, pH 3.0 and 30 ℃, the developed SC/PS system had high degradation ability for simultaneous removal of SDZ (97.8%) and TC (97.2%). The polar groups and defects of SC were conducive to the adsorption; the oxygen-containing functional groups, pyridine N and graphite C on SC surface could be used as active sites for activating PS to produce ROS. During the degradation process, both radical (•OH and SO 4 •− ) and non-radical ( 1 O 2 ) pathways coexisted. SC exhibited an excellent reusability, with the degradation efficiency of 84.5% for SDZ and 95.9% for TC after 4 cycles, and high mineralization efficiency of 67.5% after 4 h, demonstrating that such a unique SC/PS system exhibited a great potential for simultaneously efficient removal of different kinds of antibiotics in actual wastewaters.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Tao Zhou,Yi Han,Wei Xiang,Chen Wang,Xiaohui Wu,Juan Mao,Mingjie Huang
Heterogeneous catalytic activation mechanisms of peroxydisulfate (PDS) by transition metal oxides are generally attributed to the interactions between catalysts and PDS, however, the role of the co-existed organic substrate was largely overlooked in the past studies. In this work, phenol was selected as the target organic pollutant in a CuO/PDS system to evaluate its deep-seated role in participating in the effective activation of PDS. First, optimized reaction conditions as pH of 6.0, CuO of 5.96 g·L −1 and PDS of 2.5 mM were obtained by the response surface methodology (RSM) with a phenol degradation efficiency of 84.0%. It was further found that pre-adsorption of phenol or PDS led to obviously different performances in the phenol degradation with/without the radical scavengers. Two different activation pathways of PDS, i.e., the non-radical pathway mediated by surface deprotonated phenol to generate 1 O 2 and the radical pathway mediated by structural Cu(I)/Cu(II) to produce SO 4 − , were therefore proposed, and the former was predominant in the CuO/PDS/phenol system. In addition, HCO 3 − and HPO 4 2− could strongly inhibit the phenol degradation while Cl − and NO 3 − only performed negligible effects. NaOH washing could regenerate the surface hydroxyl groups and recover the catalytic ability of CuO. The result of this study integrated the interactions among the catalyst, oxidant and substrate, providing new insights into environmental-friendly PDS activation processes.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zhijie Guan,Yanping Guo,Zhenhua Huang,Xiaojian Liao,Shaojin Chen,Xuelian Ou,Shuiyu Sun,Jialin Liang,Yongfeng Cai,Wenren Xie,Jiao Xian
In the industrial electroless metal plating process, efficient removal of organic-Ni and -Cu complexes from electroless plating effluent (EPE) remains a huge challenge. In this study, a novel and feasible process of heterogeneous catalytic ozonation combined with heavy metal chelation is proposed for the effective removal of organic-Ni and -Cu complexes from EPE. The method was evaluated in a continuous pilot-scale system (CPSS). Results show that the adoption of synchronous bi-directional flow enhanced the removal of total Ni and Cu. Under optimal conditions, the total Ni and Cu in the effluent decreased to 0.1 and 0.3 mg L −1 , respectively, meeting the Chinese discharge standard requirements. The CPSS indicated that efficient removal of total Ni and Cu ( > 95%) was consistently achieved for 300 days using the proposed process. Mechanistic analysis demonstrated that ethylenediamine tetraacetic acid-Ni (EDTA-Ni) and citrate-Cu (CA-Cu) were the main complexes present in EPE. Furthermore, there were 10 transformation products and their related pathways were also identified. The decomplexation of EDTA-Ni was found to be difficult, with its final products principally existing in the complexed states, while CA-Cu was readily broken down, releasing Cu (II) that can be easily chelated. Overall, these findings provide valuable and novel insights into the removal of organic-Ni and -Cu, supporting the practical application of the proposed process in advanced EPE treatment and other industrial wastewater treatment systems.
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JOURNAL OF MEMBRANE SCIENCE
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2021
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IF 8.742
Jiaojiao Chen,Senqing Fan,Yu Chen,Yilin Wang,Ke Bai,Zenghui Mai,Zeyi Xiao
An electrocatalytic composite membrane with deep-permeation nano structure (DPNS) has been fabricated by flowing synthesis. The nano electrocatalyst MnO 2 is in situ successfully assembled in membrane pores and uniformly immobilized in membrane pores along the direction of membrane thickness. The size of MnO 2 nanoparticles immobilized in membrane pores is in the range of 33–35 nm, which is one-tenth of that immobilized on the membrane surface. The increased current density and the lower charge transfer resistance of the electrocatalytic composite membrane implied that a fast electron transfer can be achieved. As a concept-of-proof, the removal of phenol was applied to test the catalytic performance of the electrocatalytic composite membrane under the flow-through reaction mode, and the removal rate of phenol of being over 97% can be achieved under the condition of membrane flux of being 13.5 L m −2 h −1 . The apparent reaction rate constant could be increased by 2–3 orders of magnitude, owing to the enhanced contact by uniform distribution of membrane pores, as well as the confined space effect of membrane pores and the flow-through synergism enhancing mass transfer. The species of free radical can be determined as ·OH via ESR measurements for phenol oxidation . This electrocatalytic composite membrane (ECCM) with DPNS has good reusability and can provide a promising prospect for industrial application.
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Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 37
·7686-7697
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IF 6.331
Jingmei Guo,Yue Xu,Miaodeng Liu,Jian Yu,Hongye Yang,Wenlong Lei,Cui Huang
The validity and biocompatibility of irrigating agents are imperative for the success of root canal therapy. The imperfections in the currently available irrigants highlight the fact that more advanced technologies and strategies are required for complete disinfection in endodontic treatments. In the present study, a Fenton reaction-enhanced antimicrobial sonodynamic therapy (SDT) platform was fabricated for root canal disinfection. Firstly, mesoporous silica nanoparticles (MSNs) were synthesized, grafted with an amino group and then conjugated with sonosensitizer protoporphyrin IX (PpIX). Iron ions were then anchored (M@P-Fe) to initiate a Fenton reaction. Nanoparticle characterization by size and zeta potential measurements, scanning electron microscopy, transmission electron microscopy and thermogravimetric analysis confirmed that the platform was successfully developed. Reactive oxygen species (ROS) generation assessment, methylene blue degradation and electron spin resonance assays illustrated upon ultrasound (US) irradiation, that augmented ROS, can be produced by US activated PpIX and iron mediated Fenton reactions from low concentration H2O2 (0.01%). In vitro anti-Enterococcus faecalis efficacy was demonstrated by growth curve and colony forming unit measurements. Confocal laser scanning microscopy and scanning electron microscopy observations illustrated the effectiveness of the platform on in situ biofilm eradication in root canal. Owing to the stronger oxidizing capability and short lifetime of ROS, the Fenton reaction-enhanced SDT can induce detrimental oxidative damage to bacteria upon activation of US while avoiding nonspecific toxicity to cells, which was verified by cytotoxicity evaluations using CCK-8 assay and morphology observation of MC3T3-E1 cells. Compared to commonly used NaClO, this nanoplatform displayed desirable anti-bacterial, anti-biofilm abilities and better biocompatibility. These results highlight that the integrated M@P-Fe + US + H2O2 platform is a promising candidate for US enhanced root canal irrigation and disinfection.
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