WATER RESEARCH
·
2023
·
IF 12.8
Xixi Chen,Wanyi Fu,Zhichao Yang,Yulong Yang,Yanjun Li,Hui Huang,Xihui Zhang,Bingcai Pan
Hydrogen peroxide (H 2 O 2 ) is the most commonly used oxidant in advanced oxidation processes for emerging organic contaminant degradation. However, the activation of H 2 O 2 to generate reactive oxygen species is always accompanied by O 2 generation resulting in H 2 O 2 waste. Here, we prepare a Ti doped Mn 3 O 4 /Fe 3 O 4 ternary catalyst (Ti-Mn 3 O 4 /Fe 3 O 4 ) to create abundant oxygen vacancies (OVs), which yields electron delocalization impacts on enhancing the electrical conductivity, accelerating the activation of O 2 to produce H 2 O 2 . In Ti-Mn 3 O 4 /Fe 3 O 4 /H 2 O 2 system, OVs-mediated O 2 /O 2 •− /H 2 O 2 redox cycles trigger the activation of locally generated O 2 , boost the regeneration of O 2 •− and on site produce H 2 O 2 for replenishment. This leads to a 100% removal of tiamulin in 30 min at an unprecedented H 2 O 2 utilization efficiency of 96.0%, which is 24 folds higher than that with Fe 3 O 4 /H 2 O 2 . Importantly, further integration of Ti-Mn 3 O 4 /Fe 3 O 4 catalysts into membrane filtration achieved high rejections of tiamulin (> 83.9%) from real surface water during a continuous 12-h operation, demonstrating broad pH adaptability, excellent catalytic stability and leaching resistance. This work demonstrates a feasible strategy for developing OVs-rich catalysts for improving H 2 O 2 utilization efficiency via activation of locally generated oxygen during the Haber-Weiss reaction.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yibo Shen,Baolong Wang,Da Li,Weihao Yuan,Yudong Huang,Zhen Hu
Widely used traditional thermosets have drawn great attention due to their advantageous features such as excellent stability, mechanical reliability etc. However, brittleness is still the weak point in their extensive applications. Herein, a synthetic strategy to incorporate catechol groups into polymer structures via thiol-epoxy click chemistry was developed, the covalent and iron-catechol coordination bonds are combined to build up the material consisting of two types of crosslinks. As an important design feature of thermoset, catechol moiety provided the potential of gaining recoverable hysteretic energy dissipation through iron-catechol complexes. Favorable thermal properties comparable to commercial resin were retained, and mechanical testing revealed the thermoset exhibited high extensibility, such that it can be stretched to over 100 % with a fracture strength of 31.16 MPa, along with the tensile strength can be maintained 90.53 % after 5 cycles at the strain of 50 %. The synergistic interaction additionally providing the possibility of shape memory response to specific environmental changes, either by heat or by ultraviolet light. These behaviors further highlight the utility of dynamic coordinate bonds in the preparation of versatile thermosets, which could be potentially applied in smart devices and advanced materials.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Qihui Wang,Zeyu Guan,Yi Xiong,Dongya Li
Lower reaction speed and excessive oxidant inputs impede the removal of contaminants from water via the advanced oxidation processes based on peroxymonosulfate. Herein, we report a new confined catalysis paradigm via the hollow hetero-shell structured CN@C (H-CN@C), which permits effective decontamination through polymerization with faster reaction rates and lower oxidant dosage. The confined space structures regulated the C N and C O and electron density of the inner shell, which increased the electron transfer rate and mass transfer rate. As a result, C N in H-CN@C-10 reacted with peroxymonosulfate in preference to C O to generate singlet oxygen, improving the second-order reaction kinetics by 503 times. The identification of oxidation products implied that bisphenol AF could effectively remove by polymerization, which could reduce carbon dioxide emissions. These favorable properties make the nanoconfined catalytic polymerization of contaminants a remarkably promising nanocatalytic water purification technology.
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JOURNAL OF POLYMER RESEARCH
·
2022
·Vol. 29
·期 11
·1-13
·
IF 3.061
Xu Jingmei,Meng Lingxin,Shi Qingyuan,Ren Qiang,Wang Zhe
In this study, sulfonated poly (ether ketone sulfone)s polymers with long sulfonic acid alkyl side chains and amino groups were prepared by free radical and polycondensation reaction. Poly (ether ketone)s with carboxyl groups were used for macromolecule crosslinking agent to prepare cross-linked membranes by amidation reaction. This series of membranes were characterized by FT-IR and 1 H NMR. Meanwhile, cross-linked composite membranes possessed excellent mechanical properties, methanol resistance performance and thermal stability. The highest proton conductivity of 0.096 S cm −1 was observed for APD-3/CP at 80 °C. The range of methanol permeation coefficients for the prepared membranes (2.89 × 10 −7 cm 2 s −1 —4.95 × 10 −7 cm 2 s −1 ) was far lower as compared to that of Nafion 117 (24.1 × 10 −7 cm 2 s −1 ). The results of morphology, swelling ratio and proton conductivity showed that the hydrophilic-hydrophobic phase separation structure effectively improved the properties of the membrane namely water uptake, dimensional stability and proton conductivity. Long-side chains functionalized cross-linked sulfonated poly (ether ketone sulfone)s proton exchange membranes had good candidate for application in fuel cells.
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ANALYST
·
2022
·Vol. 147
·期 24
·5655-5662
·
IF 5.227
Ying Zhou,Ruichun Li,Guomei Zhang,Yan Zhang,Caihong Zhang,Shaomin Shuang
Metal–organic frameworks (MOFs) have emerged as interesting nanomaterials owing to their large surface area, high porosity, tunable pore architecture and easy functionalization. However, an inferior electrical conductivity hinders their application in electrochemical sensing. In this paper, gold–palladium alloy/UiO-66-NH2/graphene (AuPd/UiO-66-NH2/GN) composites were synthesized by loading alloys on the surfaces of MOFs and then attaching them to the graphene surface. The addition of metal nanoparticles and graphene enhanced the electron transfer ability of MOFs. Then, composites were used to modify a glassy carbon electrode (GCE) to construct a sensitive dopamine (DA) electrochemical sensor. The developed sensor manifested two linear relationships in lower concentration ranges and in higher concentration ranges with a 0.21 × 10−6 mol L−1 low detection limit (3σ/k) under optimal conditions. The results certified that the constructed sensor had high selectivity, excellent reproducibility and good stability, and had been used successfully for DA detection in actual human serum samples.
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ACS ES&T Water
·
2022
·
IF 0
Yi Zhou,Xia Li,Xinyu Chen,Jian Lu,Yanbo Zhou
Manganese dioxide (MnO2) is often used to treat pollutants in water owing to its high oxidative activity. Bisulfite (BS) as an activator can promote the degradation efficiency of MnO2. However, the mechanism of different crystalline MnO2 in the presence of BS is still controversial. The oxidation performance of the tunnel type (α-MnO2, β-MnO2) and the two-dimensional lamellar type (δ-MnO2) in the presence of BS was investigated. β-MnO2/BS exhibited the highest oxidative activity under optimal conditions. The bisphenol A (BPA) oxidation kinetic constant of β-MnO2/BS (0.737 min–1) was 6 and 2.3 times higher than that of δ-MnO2/BS and α-MnO2/BS, respectively. The mineralization efficiency of BPA reached 80.05% within 15 min, owing to the high content of Mn(IV) in β-MnO2. BS could rapidly reduce β-MnO2 to produce a high concentration of Mn(III). Soluble Mn(III) directly participates in the BPA oxidation, and the surface Mn(III) can react with the surface adsorbed oxygen molecules (Oad) to generate superoxide radicals (O2•–) to promote the deep mineralization of target contaminants. Moreover, the β-MnO2/BS system can efficiently oxidate various phenolic organic pollutants even in natural water. This research can provide new insights for better understanding of the oxidation process of different crystalline-phase MnO2/BS.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Menglu Xu,Yibing Zhang,Huaqin Yin,Jinnan Wang,Aimin Li,Philippe François-Xavier Corvini
Co-ZFO@Mn-CN with 1 O 2 and O 2 •− as main reactive oxygen species was synthesized for catalytic ozonation , which could efficiently degrade organic pollutants . EPR and XPS analysis indicated that lattice doping of Co induced formation of abundant of OVs, which could provide localized electrons for O 3 activation with the generation of HO 2 • /O 2 •− . 1 O 2 and H 2 O 2 were produced by the recombination of HO 2 • /O 2 •− . DFT calculation demonstrated that H 2 O 2 was deprotonated to generate HOO − , which preferred to form HOO-Mn-N X bonds with Co-ZFO@Mn-CN. Under the attack of O 3 , HOO-Mn-N X bonds were broken with the generation of HO 2 • and HO 3 • /O 3 •− , not only accelerating 1 O 2 production for organics degradation but also avoiding Mn(Ⅱ) sites oxidation . Combining advantages of OVs and HOO-Mn-N X , Co-ZFO@Mn-CN achieved 70–100% mineralization for different organic pollutants . Thus, this work provided a simple and efficient way for enhancing the utilization of O 3 by the synergistic effect of OVs and HOO-Mn-N X bonds, also improving ROS transformation.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yujun Ju,Jianwei Zhang,Qinyu Cai,Zhengze Zhang,Yan Zhao,Jianguo Cui,Ruien Hou,Yi Wei,Zhiqiang Liang,Fengjuan Chen
Polluted water caused by antibiotics leads to serious risks to human health and ecosystem. Rapidly and efficiently treating antibiotic pollutions to make it safe is urgently needed for environmental protection and public health. Herein, we report that ZIF-67 derived nano-cube Co 3 O 4 as model catalysts were immobilized in the rotary-angle three-dimensional (3D) printed multilayer reduced graphene oxide/carbon nanotubes (Co 3 O 4 /R-rGO/CNTs) membrane for the highly efficient degradation of antibiotic pollutants through sulfate radical-based advanced oxidation process (SR-AOP). The macropores in the designed Co 3 O 4 /R-rGO/CNTs membrane are distributed in a rotationally staggered arrangement, which increases the opportunity for contaminant contact with the catalyst. The micro-cellular structures formed by the freeze-casting treatment in Co 3 O 4 /R-rGO/CNTs membrane provide abundant anchor sites for catalysts as-well-as plentiful active sites for catalytic reactions. The degradation efficiency of the designed membrane toward aureomycin hydrochloride (CTC) reached 99.3% at a flux rate of 636.9 L m −2 h −1 , which is increased by 100% comparing with the traditional 3D printing membrane with vertical macroporous arrays. This strategy put forward a new idea for the efficient degradation of antibiotic pollutants and has great application prospects in the field of environmental remediation.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Rui Ji,Zhuzhu Zhang,Lechen Tian,Liujun Jin,Qingfeng Xu,Jianmei Lu
A novel BiOI-incorporated NH 2 -UiO-66 composite photocatalyst, NH 2 -UiO-66@BiOI, was prepared using an in-situ successive ion-insertion method. The in situ grown BiOI nanosheets exhibited an ultrathin structure and were uniformly dispersed on NH 2 -UiO-66. The formation of tight heterojunctions, characteristics of enhanced visible light absorption and availability of abundant exposed active sites facilitated the efficient activation of peroxymonosulfate and the rapid degradation of Bisphenol A in water (12 min). Surprisingly, the photocatalyst maintained a fast degradation rate of Bisphenol A under the interference of different conditions. The research explored the charge transfer pathways and radical species between the heterojunction components, indicating that the heterojunction type of the NH 2 -UiO-66@BiOI was Z-scheme. In addition, the degraded intermediate components and high mineralization rate indicated that Bisphenol A was deeply degraded. In conclusion, this study synthesized metal–organic framework-based photocatalysts through a simple preparation method, which has potential application value in the rapid degradation of bisphenol A.
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JOURNAL OF CHROMATOGRAPHY A
·
2022
·
IF 4.601
Jin-Yu Qiao,Yue-Hong Pang,Zhu-Ying Yan,Xiao-Fang Shen
Bisphenols (BPs), one of the endocrine disrupting chemicals (EDCs), are harmful to health with the potential carcinogenicity, teratogenicity and neurotoxicity. In this paper, we developed an electro-enhanced solid-phase microextraction with membrane protection method to enrich BPs. The extraction time can be shortened to 10 min with the electric field, and the prepared fiber can be repetitively used 100 times with the membrane protection. The factors affecting extraction such potential, pH, extraction temperature and extraction time were optimized. Under optimal conditions, the linear ranges were 2-600 ng mL −1 for BPAF and 2-800 ng mL −1 for the other four BPs (BPB, BPF, BPA, BPZ), and the limits of detection (S/N=3) were from 0.09 (BPAF) to 0.41 (BPA) ng mL −1 , with intra-day and inter-day precisions <5.16% and 9.29%, respectively. The developed method has been applied to the determination of trace BPs in canned meat with the recoveries of 73%-117%, showing a promising application for pretreatment in complex samples.
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ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Wenfang Du,Jie Liu,Hong Li,Chenyi Deng,Jie Luo,Qianqian Feng,Yan Tan,Shengyuan Yang,Zhaoyang Wu,Fubing Xiao
Bisphenol A (BPA), one of the most abundantly produced endocrine disrupting chemicals, is widely used in everyday plastic products and thus must be monitored. Multimode sensing platforms are able to combine the advantages of different strategies while solving the issues of inaccurate test results of single signal sensing. However, the exploration in this field is limited due to the compromise of sensing conditions and inevitable mutual interferences of different systems. Herein, we constructed a two-dimensional photonic crystal dually cross-linked supramolecular hydrogel (2DPCDCSH) by utilizing a host–guest pair of β-cyclodextrin (β-CD) and tert-butyl (t-Bu) as the second cross-linking for colorimetric and fluorescent dual-mode sensing of BPA. Based on the fact that BPA can act as a competitive guest to break the host–guest interaction between β-CD and t-Bu, the cross-linking density decreased and an expansion-induced structural color change occurred. Sensitive and selective BPA detection can be easily achieved by measuring the Debye diffraction ring diameter or observing the color change of 2DPC with a detection limit of 1 μg mL–1. Moreover, the formation of the β-CD/BPA complex gave a significant enhancement of the intrinsic fluorescence of BPA, obtaining a detection limit of 0.001 μg mL–1. The two sensing systems can share the same reaction condition and yield a wider dynamic response range than the single signal strategy. Overall, the proposed method presented an efficient, rapid, cost-effective, and regenerative dual-mode method for BPA analysis and shed new insights for the design of diversified sensing platforms.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Zhuoyue Liu,Ke Wang,Danyang Li,Zhenxin Wang,Shengjiong Yang,Heliang Pang,Gen Wang,Dahu Ding,Delu Miao
Mesoporous carbon materials are promising catalysts for peroxydisulfate (PDS) activation for degrading aqueous organic pollutants but limited by the intrinsic inertness. Herein, co-doping of iron and nitrogen into the mesoporous carbon framework was performed via thermal conversion of metal-polyphenol coordination polymers (Fe-TA) to synthesize Fe/N co-doped mesoporous carbon for efficient PDS activation. Owing to the large surface area, high graphitization degree and defective configurations, the Fe/N co-doped mesoporous carbon (Fe/N-MCs) exhibited superior catalytic performance toward the degradation of organic pollutants . Electron paramagnetic resonance tests, chemical quenching experiments, electrochemical analysis and spectra measurements revealed that the degradation of organic pollutants over the Fe/N-MCs followed a nonradical oxidation pathway based on electron transfer process. Graphite nitrogen and hydroxyl (C-OH) groups on the defective edges of Fe/N-MCs were proved to be possible active sites for PDS activation. PDS catalyzed by the Fe/N-MCs exhibited strong anti-interference capability to surrounding inorganic ions (such as Cl – , CO 3 2– , NO 3 – and SO 4 2– ) and natural organic matters, making it a promising candidate for the degradation of organic pollutants. This work provides a new prospect for developing highly active mesoporous carbon materials via heteroatom doping for PDS activation for wastewater decontamination .
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