Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Yuge Wang,Huiyu Duan,Hao Li,Jianzheng Zhen,Weiyang Lv
The application of MoS 2 as an emerging cocatalyst in wastewater treatment is of great significance, but the efficiency of cocatalyst is often limited due to its easy agglomeration and insufficient interaction with the catalyst. Here, we used layered double hydroxide (LDH) as the catalyst and the growth template of MoS 2 to achieve an efficient combination of catalyst and cocatalyst in the removal of organic pollutants by peroxymonosulfate (PMS) activation. The outcomes showed that the MoS 2 intercalated LDH composite samples (MLDH) owned excellent phenol degradation performance, reaching nearly 100% removal within 10 min, and the calculated apparent rate constants were 2.3, 5.6, 17.7 and 19.8 times higher than that of the samples of directly growing MoS 2 on the LDH (M@LDH), physically blended MoS 2 and LDH samples, LDH and MoS 2 , respectively. Based on the results of electron paramagnetic resonance (EPR) and X-ray photoelectron spectroscopy (XPS), SO 4 •- had a major impact on the elimination of phenol, Mo(Ⅳ) in MoS 2 also participated in and encouraged the Fe(Ⅲ)/Fe(Ⅱ) redox cycle, providing the driving force for the further activation of PMS . Moreover, the effects of pH value, anions, cations and water environment of MLDH during the activation of PMS were also determined, and it was found that under various catalytic environments, MLDH always maintained a high removal rate of phenol and showed strong anti-interference ability. Collectively, the results of this research would offer more possibilities and suggestions for creating highly effective catalysts for wastewater cleanup.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF NANOBIOTECHNOLOGY
·
2023
·Vol. 21
·期 1
·1-18
·
IF 10.2
Cao Yameng,Cheng Kai,Yang Mei,Deng Zhichao,Ma Yana,Yan Xiangji,Zhang Yuanyuan,Jia Zhenzhen,Wang Jun,Tu Kangsheng,Liang Jie,Zhang Mingzhen
Background Inflammatory bowel disease (IBD) is a chronic nonspecific disease with unknown etiology. Currently, the anti-inflammatory therapeutic approaches have achieved a certain extent of effects in terms of inflammation alleviation. Still, the final pathological outcome of intestinal fibrosis has not been effectively improved yet.Results In this study, dextran-coated cerium oxide (D-CeO2) nanozyme with superoxide dismutase (SOD) and catalase (CAT) activities was synthesized by chemical precipitation. Our results showed that D-CeO2 could efficiently scavenge reactive oxide species (ROS) as well as downregulate the pro-inflammatory cytokines (IL-1β, IL-6, TNF-α, and iNOS) to protect cells from H2O2-induced oxidative damage. Moreover, D-CeO2 could suppress the expression of fibrosis-related gene levels, such as α-SMA, and Collagen 1/3, demonstrating the anti-fibrotic effect. In both TBNS- and DSS-induced colitis models, oral administration of D-CeO2 in chitosan/alginate hydrogel alleviated intestinal inflammation, reduced colonic damage by scavenging ROS, and decreased inflammatory factor levels. Notably, our findings also suggested that D-CeO2 reduced fibrosis-related cytokine levels, predicting a contribution to alleviating colonic fibrosis. Meanwhile, D-CeO2 could also be employed as a CT contrast agent for noninvasive gastrointestinal tract (GIT) imaging.Conclusion We introduced cerium oxide nanozyme as a novel therapeutic approach with computed tomography (CT)-guided anti-inflammatory and anti-fibrotic therapy for the management of IBD. Collectively, without appreciable systemic toxicity, D-CeO2 held the promise of integrated applications for diagnosis and therapy, pioneering the exploration of nanozymes with ROS scavenging capacity in the anti-fibrotic treatment of IBD.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Qianqian Zhou,Peidong Hong,Xu Shi,Yulian Li,Ke Yao,Wanqi Zhang,Chengming Wang,Junyong He,Kaisheng Zhang,Lingtao Kong
In order to solve the problem of easy aggregation of copper oxides in environmental remediation, it is an effective method to confine copper oxides to suitable substrates. Herein, we design a novel Cu 2 O/Cu@MXene composite with a nanoconfinement structure, and it can effectively activate peroxymonosulfate (PMS) to produce . OH for degradation tetracycline (TC). Results indicated that the MXene with extraordinary multilayer structure and surface negativity could fix the Cu 2 O/Cu nanoparticles in the layer spaces and suppress the agglomeration of nanoparticles. The removal efficiency of TC reached 99.14 % within 30 min, and the pseudo-first-order reaction kinetic constant was 0.1505 min −1 , which was 3.2 times that of Cu 2 O/Cu alone. The outstanding catalytic performance attributed that the MXene based on Cu 2 O/Cu@MXene could promote the adsorption of TC and electron transmittal between Cu 2 O/Cu nanoparticles. Furthermore, the degradation efficiency of TC was still over 82 % after five cycles. In addition, based on the degradation intermediates provided by LC-MS, two specific degradation pathways were proposed. This study provides a new reference for suppressing the agglomeration of nanoparticles, and broadens the application of MXene materials in the field of environmental remediation.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Acta Biomaterialia
·
2023
·
IF 9.7
Yiyu Chen,Ping Liu,Chunze Zhou,Tao Zhang,Tianxing Zhou,Dandan Men,Guihua Jiang,Lifeng Hang
Photothermal therapy (PTT), photodynamic therapy (PDT), and chemodynamic therapy (CDT) can cause cancer cell death through an immunogenic process. However, the study of second near-infrared window (NIR-II)-triggered PTT and PDT combined with CDT to induce an immune response has not been recently reported. Here, we integrated gold nanobipyramids and copper sulfide in a core/shell architecture (AuNBP@CuS). The material displays both photodynamic and photothermal properties under irradiation with a NIR-II laser. The released Cu 2+ from CuS under an acidic tumor microenvironment can be converted to Cu + by glutathione following a Fenton-like reaction with hydrogen peroxide to generate highly toxic hydroxyl radicals in the tumor region. Both in vitro and in vivo results demonstrated that such multifunctional nanoplatforms could achieve enhanced efficiency for image-guided tumor suppression based on the NIR-II photo/chemodynamic therapy. We found that damage-associated molecular pattern molecules such as adenosine triphosphate, pre-apoptotic calreticulin , and high mobility group box-1 in dying cells induced by the NIR-II photo/chemodynamic therapy could simultaneously trigger adaptive immune responses. This is the first report revealing that NIR-II photo/chemodynamic therapy based on AuNBP@CuS had promising performance on tumor suppressor with an effective immunogenic cell death process. Statement of significance 1. AuNBP@CuS displays both NIR-II photodynamic and photothermal properties. 2. Cu + following a Fenton-like reaction to generate highly toxic hydroxyl radicals. 3. The NIR-II photo/chemodynamic therapy can trigger adaptive immune responses. 4. Such multifunctional nanoplatforms could achieve enhanced efficiency for tumor suppression.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yahan Yu,Chunxiu Yu,Zelin Wu,Bingkun Huang,Peng Zhou,Heng Zhang,Wen Liu,Yucheng Liu,Zhaokun Xiong,Bo Lai
Concurrently elevating the degradation efficiency of pollutants and realizing the reduction of iron sludge in Fe-based catalytic ozonation is important but still challenging. Herein, we developed an electrocatalytic ozonation (ECO) system with iron plate cathode and graphite felt anode (ECO-Fe-cathode), which was free from added chemical reagents. Unlike the iron plate as a sacrificial anode in the ECO (ECO-Fe-anode) system, this delicately designed system shows a much higher degradation rate of ibuprofen ( k obs = 1.490 min −1 ) than that of the ECO-Fe-anode system ( k obs = 0.345 min −1 ). Simultaneously, the effluent was totally limpid without the corrosion of iron plates and the formation of iron sludge in the ECO-Fe-cathode system. Unexpectedly, the generation of singlet oxygen ( 1 O 2 ) which is indirectly generated by the single-electron transfer derived from superoxide ion (O 2 •- ) is the primary reactive oxygen species (ROS) in the ECO-Fe-cathode system, which is different from the ECO-Fe-anode system with hydroxyl radicals ( • OH). Moreover, linear sweep voltammetry (LSV) was applied to reveal the oxygen evolution reaction (OER) performance of the iron plate and graphite felt, and the results showed that graphite felt as anode has better electrocatalytic performance. The electrochemical analysis and density functional theory (DFT) calculation revealed that ozone adsorbed on the iron plate surface is more conducive to facilitating and triggering subsequent reactions. Finally, the different degradation pathways of ibuprofen in both systems were proposed. This work represents a fundamental breakthrough toward the design of an efficient and harmless ECO system for wastewater treatment.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Ke Zhang,Yajing Wei,Hongyang Cao,Yue Xin,Chuanyi Wang
Tuning reactive oxygen species in peroxymonosulfate (PMS) activation by the structure of catalysts has been extensively studied. But in photocatalysis , the photothermal effect is lack of attention on the alteration of reactive species produced by PMS activation. In this work, ZnFe 2 O 4 /C photocatalyst with oxygen vacancy (ZFO v /C) was synthesized via the calcination of bimetallic Zn/Fe-metal–organic framework. The photocatalytic performance of the catalyst had been studied under several conditions, and the experimental results demonstrated that the photocatalytic reaction rate constant of ZFO v /C photocatalyst without temperature control was 21.3 % higher than that under temperature control. Reactive species quenching experiments and electron paramagnetic resonance indicated that 1 O 2 and h + are the primary reactive species without temperature control, while only 1 O 2 are the dominant reactive species under temperature control conditions. The possible activation site was speculated by in-situ Raman spectroscopy , XPS spectra and cycling experiment. This paper analyzes the reasons for photocatalysis to improve the degradation rate of pollutant from the perspective of the change of reactive species generated by photothermal effect on PMS activation, which may open up opportunities to explore the maximum utilization of sunlight in PMS activation.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yong Liu,Le Zhang,Ting Liu,Jianlong Wang
The selective oxidation of ammonium nitrogen (NH 4 + -N) to dinitrogen (N 2 ) by advanced oxidation processes (AOPs) is of paramount significance, but it is still a great challenge. In this study, a novel composite (FeO x -MgO) was synthesized to activate persulfate (PS) for selective oxidation of ammonium (NH 4 + ) to N 2 under simulated solar-light irradiation ( hv ). The results demonstrated that the conversion of NH 4 + to ammonia (NH 3 ) on the basic sites of FeO x -MgO was a key step for the selective oxidation of NH 4 + . Fe(IV) species formed in FeO x -MgO/PS/ hv system could enhance both the efficiency and N 2 selectivity of the NH 4 + -N oxidation through the oxidation of ammonia hydride to N 2 . The 100 % NH 4 + -N removal and over 95.5 % N 2 selectivity could be achieved after 30 min when initial pH was in range of 2–10, and the initial NH 4 + -N concentration was 30 mg N/L. This study could provide a promising technology for the selective oxidation of NH 4 + -N to N 2 in water and wastewater.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Limin Duan,Huihao Jiang,Wenhao Wu,Daohui Lin,Kun Yang
Introducing crystal defects into iron based metal-organic frameworks (Fe-MOFs) is regarded as a promising strategy to enhance Fenton-like performance. However, developing a facile and effective strategy to construct defective Fe-MOFs as highly efficient Fenton-like catalyst is still a challenge. Herein, MIL-100(Fe) (Def-MIL-100(Fe)) with missing ligands defects was synthesized by a simple heterogeneous reaction using zero-valent iron. The bisphenol A degradation efficiency in the Def-MIL-100(Fe)/H 2 O 2 system reached up to 91.26% within 10 min at pH 4 with a low catalyst dosage of 0.05 g/L, while the perfect MIL-100(Fe) has almost no Fenton-like performance. It was observed that missing ligands defects in the Def-MIL-100(Fe) play a key role in the Fenton-like reaction. The missing ligands defects could increase the Lewis acidity for fast H 2 O 2 adsorption and accelerate the electron transfer between Fe II and Fe III cycling, leading to faster and more·OH generation. Moreover, the missing ligands defects could promote the mass transfer for improving·OH utilization efficiency. This work provides a novel strategy to construct defective Fe-MOFs as highly efficient Fenton-like catalyst to degrade organic pollutants in water.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Rong Ji,Yuming Dong,Hui Zhao,Chengsi Pan,Guangli Wang,Yongfa Zhu,Junshan Li
Fenton technology has been famous on antibiotics removal, but seriously restricted by the extra addition of H 2 O 2 and low mineralization efficiency. Herein, we develop a novel cobalt-iron oxide/perylene diimide organic supermolecule (CoFeO/PDIsm) Z-scheme heterojunction under photocatalysis-self-Fenton system, in which the holes (h + ) of photocatalyst can mineralize organic pollutants and the photo-generated electrons (e − ) are used to in-situ H 2 O 2 production with high efficiency. The CoFeO/PDIsm exhibits superior in-situ H 2 O 2 production at a rate of 281.7 µmol g −1 h −1 in contaminating solution, correspondingly of total organic carbon (TOC) removal rate of ciprofloxacin (CIP) is 63.7 %, far exceeding current photocatalysts. The high H 2 O 2 production rate and remarkable mineralization ability are ascribed to great charge separation in Z-scheme heterojunction. This work provides a novel Z-scheme heterojunction with photocatalysis-self-Fenton system for environmental-friendly removing the organic containment.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ying Wu,Chi Song,Xinyan Yu,Xianbao Shen,Lijie Xu,Ying Zhang,Han Gong,Changlei Xia,Lu Gan
In this study, waste polyethylene (PP) obtained from obsoleting water purifier filter was mixed with ferric chloride hexahydrate (FeCl 3 ·6H 2 O) to prepare a series of single crystal phased iron compound incorporated carbon composites (Fe/PP-C). The prepared Fe/PP-Cx catalysts were then utilized to degrade sulfamethoxazole (SMX) in water by activating peroxymonosulfate (PMS). The results showed that with the assistance of pyrolysis temperature regulation, waste PP filter could control the crystalline phase of the iron compound in the prepared Fe/PP-Cx through releasing distinct gaseous atmospheres at respective pyrolysis temperature. When the pyrolysis temperature was set at 600 °C and 900 °C, pure phase ferric oxide (Fe 3 O 4 ) and zero-valent iron (ZVI) incorporated carbon catalysts were obtained, respectively. 0.2 g/L of Fe/PP-Cx could completely degrade 0.02 mM of SMX within 20 min, in which the toxicity of the reaction solution was also effectively reduced. In both Fe/PP-Cx/PMS systems, non-radical mechanisms dominated the SMX degradation, in which singlet oxygen played the dominant role in the Fe/PP-C600/PMS system, whereas electron transfer process was primarily responsible for SMX degradation in the Fe/PP-C900/PMS system. High-valent iron-oxo species was also involved in SMX degradation in the Fe/PP-C900/PMS system. Since Fe/PP-C600 and Fe/PP-C900 respectively activated PMS via heterogeneous and homogeneous routes, Fe/PP-C600 maintained higher longtime use stability. This study aims to present a simple approach to manipulate the nonradical organic pollutant degradation mechanisms in PMS activated system, which also provides a new strategy of utilizing waste polymer.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Shiwen Dong,Wen Xu,Qingqing Guo,Kai Luo,Haijun Cheng,Juntao Tang,Da Wang,Zhiqiao He,Lizhang Wang,Shuang Song,Jun Ma
Designing efficient and environmentally friendly catalysts is essential to activating ozonation for wastewater remediation. This study prepared soybean biochar (SB), adzuki beans biochar (AB), and mung beans biochar (MB) catalysts using moldy legumes as precursors. The biochars were characterized to investigate the surface characters’ effect on ozone activation toward 2, 6-dimethylpyrazine (2,6-DMP) degradation. All prepared samples drastically facilitated the degradation more than with sole ozonation. It was found that at pH 7 with 10 mg L −1 catalysts, the removal rates of 5 μM 2,6-DMP were 88.3 %, 90.7 %, and 87.3 % by SB, MB, and AB at 30 min, respectively. The surface-area-normalized reaction rate constants (k obs /S BET ) showed that AB exhibited the best catalytic activity with the rate of 1.5 × 10 −2 mg·m 2 ·min −1 , which is 2.3- and 23.1-fold higher than that of SB and MB, respectively. Further characterization confirmed that oxygen- (C–O/C = O and –OH) and nitrogen-containing groups (pyridine N and pyrrole N) were crucial to the catalytic degradation, as electron transfer was promoted to form more ROS. In addition, the quenching test and electron paramagnetic resonance (EPR) revealed OH, O 2 − , and 1 O 2 as the main reactive oxygen species (ROS) during the heterogeneous catalytic ozonation (HCO), indicating that 2,6-DMP degradation followed the radical and non-radical oxidation pathways. Overall, this study helped to understand the relationship between surface functional groups and intrinsic activity. It also provided a new direction for utilizing agricultural waste.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Sainan Wang,Chao Yuan,Wei Chen,Yifan Niu,Yexi Yan,Fan Li,Hongmei Jiang
A series of CuO@g-C 3 N 4 composites with different contents of g-C 3 N 4 and different morphologies of CuO have been designed and prepared by hydrothermal method and applied to activate peroxymonosulfate (PMS) for the removal 2,4,6-trichlorophenol (2,4,6-TCP). The results showed that 3D spherical shape CuO-1@g-C 3 N 4 -3, being able to activate PMS to produce a large amount of singlet oxygen ( 1 O 2 ), not only had good catalytic performance, but also reduced the dissolution of Cu 2+ . By comparing the morphological characteristics, catalytic performance, free radical species, decomposition rate of PMS and surface properties of three kinds of CuO, the generation mechanism of 1 O 2 and key reasons of CuO for producing 1 O 2 were deeply explored and finally deduced. Besides, under the conditions of initial pH 7.0, catalyst dosage 50 mg·L −1 , PMS dosage 0.3 mmol·L −1 and initial concentration of 2,4,6-TCP 10 mg·L −1 , the removal rate of 2,4,6,-TCP reached 94 % at 25 min in the first cycle, and 85 % in the fifth cycle. When CuO-1@g-C 3 N 4 was applied in actual water samples, 65 % of 2,4,6-TCP was removed in the Yangtze River, and 60 % of 2,4,6-TCP in Xuanwu and Yueya Lake in 40 min. Quenching experiments and electron paramagnetic resonance (EPR) were used to indentify active species during degradation process and the degradation intermediates of 2,4,6-TCP and possible degradation pathways were determined and proposed by high performance liquid chromatography-time of flight-mass spectrometry (HPLC-TOF-MS 2 ). This study shed light on the 1 O 2 generation mechanism of catalyst and provided theoretical basis and guidance for the design of 1 O 2 catalysts rich in non-radical active species.
✓ 已验证
产品关联
DOI
高影响因子