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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2020 · IF 7.489

Development of highly permeable and antifouling ultrafiltration membranes based on the synergistic effect of carboxylated polysulfone and bio-inspired co-deposition modified hydroxyapatite nanotubes

Yongfeng Mu,Han Feng,Shuling Zhang,Chongyang Zhang,Nan Lu,Jiashuang Luan,Guibin Wang

Hybridization has become a powerful toolbox for developing ultrafiltration membranes with superior properties. However, it remains challenging to give full play to the utility of nanofillers because of poor bonding strength between polymers and inorganic nanomaterials . Herein, hydroxyapatite nanotubes (HANTs) were modified via bio-inspired polydopamine (PDA) and polyethylenimine (PEI) co-deposition. Meanwhile, polysulfone with carboxylation degree of 30% (PSF-COOH-30%) was synthesized by nucleophilic substitution reaction and employed as the membrane matrix. The results showed that when 0.3 wt% HANTs@PDA/PEI was incorporated, the pure water flux of the hybrid membrane achieved about 3.2 times that of the unfilled membrane and the rejection rate of bovine serum albumin (BSA) and humic acid (HA) remained 94.5% and 97.8%, respectively. Meanwhile, the flux recovery ratio for BSA and HA solutions (1 g/L) reached 90.8% and 93.7%, respectively. Specifically, the superiority of UF performance benefited from the synergistic effect of both the carboxylated polymer and the nanofiller. On one hand, the incorporation of HANTs@PDA/PEI promoted the formation of more porous membrane structure and improved the hydrophilicity of the membrane. On the other hand, due to the existence of COOH, the electrostatic repulsion between the membranes and contaminants enhanced the fouling resistance for BSA and HA. Conspicuously, the ease and versatility of co-deposition provide new ideas in the construction of nanohybrid and the favorable improvement renders that appropriate combination of polymer and additive is an effective way for developing future ultrafiltration membranes.

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Materials Today Communications · 2020 · IF 2.678

Preparation and adsorption properties of rosin-based bisphenol A molecularly imprinted microspheres

Caili Yu,Jianhang Shan,Yong Chen,Jintao Shao,Faai Zhang

Rosin-based bisphenol A (BPA) molecular imprinted polymer (P-MIP) microspheres were prepared by suspension polymerization using rosin-based isophorone diisocyanate polyurethane as the primary monomer, methacrylic acid as the functional monomer, and BPA as the template molecule. The structure, morphology, particle size and adsorption properties of the microspheres were characterized and analyzed by means of infrared spectroscopy, scanning electron microscopy, laser particle size analysis and ultraviolet-visible spectrophotometry. The results showed that the imprinted microspheres exhibited a spherical shape with an average particle size of 123 μm. The adsorption behavior of BPA on the P-MIP microspheres followed a pseudo-first-order kinetic model, corresponding to physical adsorption. The isothermal adsorption model conformed to the Freundlich model, indicating that the binding sites were non-uniform. The imprinting factors ( σ ) of the P-MIP microspheres for BPA, para-tert-butyl phenol, hydroquinone and phenol were 2.69, 1.53, 1.26 and 1.10, respectively, indicating that the P-MIP microspheres had specific adsorption properties for BPA. After the imprinted microspheres were repeatedly used for five times, the adsorption rate was 96 %, indicating good repeatability.

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JOURNAL OF MEMBRANE SCIENCE · 2020 · IF 7.183

Hierarchical poly(vinylidene fluoride)/active carbon composite membrane with self-confining functional carbon nanotube layer for intractable wastewater remediation

Zhongming Chen,Sakil Mahmud,Lirong Cai,Zijun He,Yang Yang,Lei Zhang,Shuaifei Zhao,Zhu Xiong

The efficient removal of trace micro pollutants and heavy metals from wastewater has been deemed as major challenge in the field of water treatment. Membrane composites have shown promises for the removal of these contaminants via green chemistry principles (i.e. membrane filtration). However, membrane composites normally lack appropriate surface porosity which hinders their performance, and it oftentimes causes membrane fouling . In this work, in order to ensure simultaneous removal of trace micro pollutants and heavy metals, a multi-functional active carbon inlayed poly(vinylidene fluoride) (PVDF) composite membrane with antifouling surface of polyacryloyl hydrazide (PAH)-grafted-carbon nanotubes (CNTs) layer is fabricated for the cross-flowing separation of oil/water emulsion, and heavy metals removal . The as-prepared PVDF-membrane composite with highly porous structure is integrated with powdered activated carbon (PAC) inlayed via the delayed liquid-liquid de-mixing process. The system shows high dynamic adsorption capacity towards the removal of toxic micro pollutants such as nitro-phenol, sulfamerazine and bisphenol A. In addition, micro/nano-hierarchical surface is constructed on the PVDF membrane via phase inversion. This enables successful anchorage of PAH-grafted-CNTs as antifouling layer on the surface of the PVDF-membrane. The reductive hydrophilic PAH brush on CNTs adsorbs different kinds of trace heavy metals (i.e. Cu 2+ , Ni + , and Cr 3+ ) through reduction process. The PAH-grafted-CNTs also endows the composite membrane with excellent antifouling towards proteins.

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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2020 · IF 7.864

Enhancing the Fenton-like Catalytic Activity of nFe2O3 by MIL-53(Cu) Support: A Mechanistic Investigation

Yi Ren,Mengqi Shi,Weiming Zhang,Dionysios D. Dionysiou,Junhe Lu,Chao Shan,Yanyang Zhang,Lu Lv,Bingcai Pan

A novel Fenton-like catalyst was synthesized by immobilizing nano-Fe2O3 (nFe2O3) on MIL-53(Cu). The pseudo-first-order rate constant of bisphenol A degradation in the nFe2O3/MIL-53(Cu)/H2O2 system reached 0.0123 min–1, while the values in MIL-53(Cu)/H2O2 and nFe2O3/H2O2 systems were only 0.0026 and 0.0040 min–1, respectively. The characterization of nFe2O3/MIL-53(Cu) reveals that the supreme catalytic activity of this material could be ascribed to iron–copper synergy, smaller size, and better dispersion of nFe2O3 particles. Moreover, a method of trapping Cu(I) by neocuproine was developed, which could shield Cu(I) from interacting with iron and H2O2, and thus allow quantitative differentiation of the contribution to the enhanced catalytic activity by each of the factors. Using this method, 19% of the enhancement was determined to be contributed by synergistic effect, while 24% of the enhancement was due to the smaller size and better dispersion of the nFe2O3 particles on MIL-53(Cu) support. In addition, the performance of nFe2O3/MIL-53(Cu) only dropped 10.7% after five treatment cycles in real wastewater, showing good potential in practical application. We believe this study sheds light on the tailored design of Fenton-like catalysts and elucidates the catalytic mechanisms of supported bimetallic catalysts.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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MICROCHIMICA ACTA · 2020 ·Vol. 187 ·期 7 ·1-11 · IF 6.232

High-throughput screening of bisphenols using magnetic covalent organic frameworks as a SELDI-TOF-MS probe

Sun Qianqian,Gao Chaohong,Ma Wende,He Yanting,Wu Jie,Luo Kailong,Ouyang Dan,Lin Zian,Cai Zongwei

Core-shell structured magnetic covalent organic framework (Fe 3 O 4 @COF) nanospheres were rapidly synthesized at room temperature using the monodisperse Fe 3 O 4 nanoparticles (NPs) as magnetic core and benzene-1,3,5-tricarbaldehyde (BTA) and 3,3′-dihydroxybenzidine (DHBD) as two building blocks (denoted as Fe 3 O 4 @BTA-DHBD), respectively. They can serve as a mass spectrometry probe for rapid and high-throughput screening of bisphenols (BPs) from pharmaceuticals and personal care products (PPCPs) by surface-enhanced laser desorption/ionization time-of-flight mass spectrometry (SELDI-TOF-MS). The Fe 3 O 4 @BTA-DHBD nanospheres showed some superior features involving average pore size distribution (2.82 nm), high magnetization values (42.5 emu g −1 ), high specific surface area (82.96 m 2  g −1 ), and good chemical/thermal stability. It was used as both ideal adsorbent for enrichment of BPs and new substrate to assist ionization in SELDI-TOF-MS. The method exhibited good linearity in the range 0.05–4000 ng mL −1 with correlation coefficients ( r ) higher than 0.9920. Low limits of detection (LODs) (500 pg mL −1 for bisphenol A (BPA), 2 pg mL −1 for bisphenol B (BPB), 28 pg mL −1 for bisphenol C (BPC), 60 pg mL −1 for bisphenol F (BPF), 33 pg mL −1 for bisphenol AF (BPAF), 200 pg mL −1 for bisphenol BP (BPBP), 10 pg mL −1 for bisphenol S (BPS), 90 pg mL −1 for tetrabromobisphenol A (BPA(Br) 4 ), and 380 pg mL −1 for tetrabromobisphenol S (BPS(Br) 4 )) and good recoveries (80.6–115%) of BPs in PPCPs were achieved. The relative standard deviations (RSDs) of spot-to-spot ( n  = 10) and sample-to-sample ( n  = 5) were in the ranges 5–11% and 5–12%, respectively. The dual-function platform was successfully applied to the quantitative determination of BPs in PPCPs. It not only expanded the scope of the application of COFs but also provided an alternative strategy for the determination of hazardous compounds in PPCPs. Schematic representation of the synthesis of core-shell structured magnetic covalent organic framework nanospheres (Fe 3 O 4 @COFs) and its application in the analysis of bisphenols by using Fe 3 O 4 @BTA-DHBD nanospheres as a MS probe based on surface-enhanced laser desorption/ionization time-of-flight mass spectrometry.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Gravity-driven biomimetic membrane (GDBM): An ecological water treatment technology for water purification in the open natural water system

Zhenzhou Zhu,Zhe Chen,Xiao Luo,Wenxiang Zhang,Shujuan Meng

As an environmental water treatment technology, membrane technology has been prevalent for water purification in the closed membrane reactor system. Can membrane technology be applied as an ecological water treatment technology for water purification in the open natural water system? In this study, the feasibility of water purification in the open natural water system with gravity-driven biomimetic membrane (GDBM) was explored, focusing on the filtration driving force for providing the superior filtration efficiency and stability of long-term operation for improving the practicability. During GDBM preparation process, laccase was immobilized by carrier, then they were filtrated and deposited on microfiltration, thus a biomimetic layer with high permeability was formed. Its filtration process could be driven by the gravity of its own hydrostatic height. Above all, activated carbon, graphene oxide (GO) and carbon nanotube were utilized as carrier materials. Because of more stable immobilization effect for laccase and greater permeable structure, GO-GDBM possessed the better BPA removal rate and higher permeate flux. It even reached 72.1 L m −2 h −1 at 12 cm of hydrostatic height, and its fouling rate kept at a low hydrostatic height by the analysis of critical flux theory. Moreover, filtration experiments with BPA micro-polluted water were performed with various carrier dosages, laccase dosages, and BPA concentrations. Under different operating conditions, the filtration performance still kept a desirable degree. With an optimized condition (6 cm of hydrostatic height, 30 g m −2 of carrier dosage, and 100 g m −2 of laccase dosage), GO-GDBM sustained above 27~42 L m −2 h −1 of permeate flux and 55~70% of BPA removal rate during 30 days’ operation. In addition, GDBM was proved to be effective to treat real micro-polluted water (natural water body polluted by soy sauce pollutants). Thus, GDBM could obtain sufficient filtration driving force, demonstrate a good capacity of resisting the change of operating conditions, and maintain high stability of long-term operation in the open natural water system. This study demonstrates an example of a niche application, where GDBM is expected to transform membrane technology from environmental water treatment technology to a highly efficient and cost-effective ecological water treatment technology.

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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Uniform N-coordinated single-atomic iron sites dispersed in porous carbon framework to activate PMS for efficient BPA degradation via high-valent iron-oxo species

Yang Li,Ting Yang,Shaohui Qiu,Wanqi Lin,Jinting Yan,Shisuo Fan,Qi Zhou

Iron-mediated activation of peroxymonosulfate (PMS) has been widely investigated for recalcitrant pollutants. However, maximizing the dispersion degree of the active iron sites in the catalysts is still a great challenge and attracting tremendous attention. Herein, we demonstrated that well-dispersed single atomic Fe sites embedded into N-doped porous carbon (Fe SA -N-C), which derived from chemically Fe-doped zeolitic imidazolate frameworks, could work as Fe-based catalyst for efficient catalytic oxidation of recalcitrant organics via PMS activation. As expected, Fe SA -N-C exhibited remarkably higher degradation activity (8.1 times faster) to BPA (a model pollutant) than that of Fe based nanoparticles-loaded N-doped carbon (Fe NP -N-C). The sufficient Fe-N x sites with single Fe atom as the building units were proposed to be the main active sites for PMS activation. Based on that, unlike the traditional sulfate radical-based advanced oxidation processes, BPA degradation was achieved via high-valent iron-oxo species. More particularly, it could be used over a wide range of pH 3.0–7.5 with almost no loss of degradation efficiency. This study will provide insights into the design of heterogeneous Fenton-like catalysts.

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International Journal of Environmental Research and Public Health · 2020 ·Vol. 17 ·期 3 ·1075 · IF 2.849

Adsorption Characteristics and Mechanism of Bisphenol A by Magnetic Biochar

Jinpeng Wang,Ming Zhang

In this paper, biochar (BC) was prepared from discarded grapefruit peel and modified to prepare magnetic biochar (MBC). Physical and chemical properties of BC and MBC were characterized, and the results showed that the type of iron oxide loaded by MBC was γ-Fe2O3. Compared with BC, MBC has a larger specific surface area and pore volume, with more oxygen-containing functional groups on the surface. BC and MBC were used to adsorb and remove endocrine-disrupting chemical (EDC) bisphenol A (BPA) from simulated wastewater. The results showed that the adsorption kinetics and adsorption isotherm of BPA adsorption by BC and MBC were mainly in accordance with the pseudo-second-order kinetics model and the Langmuir model. This indicates that the adsorption of BPA on BC and MBC is mainly a chemically controlled monolayer adsorption. Adsorption thermodynamics show that BC and MBC adsorption of BPA is a spontaneous exothermic reaction, and lowering the temperature is conducive to the adsorption reaction. The effect of solution pH on the adsorption of BPA by both was significant. The optimum pH for BC and MBC to absorb BPA was 6 and 3, respectively. The concentration of Na+in the range of 0–0.10 mol·L−1can promote the adsorption of BPA to MBC. MBC loaded with γ-Fe2O3not only has excellent magnetic separation ability, but can also reach about 80% of the initial adsorption capacity after four cycles of adsorption. By analyzing the adsorption mechanism, it was found that the H-bond and the π–π electron donor–acceptor interaction (EDA) were the main forces for BC and MBC to adsorb BPA.Keywords:biochar;magnetic biochar;adsorption;bisphenol A;γ-Fe2O3

CAS / MDL: 80-05-7
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2020 · IF 7.489

One-step electroreduction preparation of multilayered reduced graphene oxide/gold-palladium nanohybrid as a proficient electrocatalyst for development of sensitive hydrazine sensor

Huanfang Zhou,Limin Chen,Shuting Li,Songqing Huang,Yingying Sun,Yanhong Chen,Zhao Wang,Wei Liu,Xinchun Li

A facile and green method for preparation of gold/palladium (Au/Pd) bimetallic nanoparticles interleaved reduced graphene oxide (rGO) composite was presented. One-step electroreduction of Au/Pd precursors and graphene oxide synergistically produced a multilayered and well-structured nanohybrid on glassy carbon electrode, which was explored as a highly efficient electrocatalyst . This operation is easy and controllable, as compared with time-consuming and procedure-tedious hydrothermal synthesis . The morphology and chemical constituents were meticulously characterized. The remarkable electrocatalytic performance of the prepared nanohybrid was demonstrated by detection of a high-risk carcinogen pollutant, hydrazine. By optimizing the preparation condition and investigating the electrochemical behavior, we achieved the sensitive analysis of hydrazine with ultralow oxidation overpotential. Amperometry was employed for constructing the quantitative calibration curve ; the steady-state current originating from hydrazine oxidation was proportional to the analytical concentration ranging from 0.1 μM to 200 μM, with the detection limit of 16 nM. Moreover, the nanohybrid displayed considerable anti-interfering ability with respect to hydrazine detection, as a variety of potentially coexisting substances produced negligible electrochemical response in the given analytical condition. Advantages including easy-to-preparation, high sensitivity and favorable selectivity , as well as broad linear response make the present method feasible for monitoring of hydrazine in water environment.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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JOURNAL OF MEMBRANE SCIENCE · 2020 · IF 7.183

Bidirectional molecularly imprinted membranes for selective recognition and separation of pyrimethamine: A double-faced loading strategy

Jian Lu,Yingying Qin,Yilin Wu,Minjia Meng,Zeqing Dong,Chao Yu,Yongsheng Yan,Chunxiang Li,Felix Kwame Nyarko

Molecularly imprinted membranes (MIMs) inspired from biological semi-permeable membranes are playing promising roles in molecularly selective recognition and separation due to its remarkable and customizable selectivity. In this research, the bidirectional pyrimethamine molecularly imprinted membranes (PMIMs) have been fabricated for selective separation of pyrimethamine (PMM). PMM was selected as the target resulting from the potential threat to human health and reusable value in aquaculture industry. The carbon nanotubes double-faced loading strategy was implemented based on polydopamine and κ-carrageenan for the improvement of effective platform. By photo-initiated “click chemistry”, specific recognition sites were facilely and efficiently formed on membranes using methacrylic acid as functional monomers . Notably, results indicated that the PMIMs possess desirable rebinding selectivity ( α  = 3.24, 3.53 and 3.78) and permselectivity ( β  = 3.99, 4.03 and 4.21) towards PMM despite the interference of competitors or analogues (sulfadiazine, diaveridine, and bisphenol A). High regeneration rate (>90% after ten cycles of regeneration) proved the potentials of PMIMs for practical applications. During the designed bidirectional filtration, the PMIMs showed a stable performance in separation of PMM from practical samples. The PMIMs and preparation strategy developed here will provide significant potentials for selective separation and extraction of harmful or reusable constituents form wastewater.

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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2020 · IF 3.99

N doped carbon quantum dots modified defect-rich g-C3N4 for enhanced photocatalytic combined pollutions degradation and hydrogen evolution

Haiping Liu,Jing Liang,Shuai Fu,Li Li,Jiehu Cui,Penghui Gao,Fengying Zhao,Jianguo Zhou

Exploiting metal-free cocatalysts is of huge interest for photocatalytic technology in environmental wastewater remediation and water splitting fields. The N doped carbon quantum dots (NCDs) modified defect-rich g-C 3 N 4 (DCN) was prepared through impregnation method. The structural, optical and electronic properties of NCDs/DCN were systematically investigated. The NCDs/DCN with outstanding visible light absorption, narrowed gap and electron transfer ability were conducive to combined pollutions photocatalytic removal and simultaneous H 2 production and rhodamine B (RhB) degradation. The resulting NCDs/DCN performed much higher removal efficiency in different combined pollutions systems containing OFL/Cr (VI), BPA/Cr (VI) and CIP/Cr (VI) than in single system owing to the synergistic effect between organic pollution oxidation and Cr (VI) reduction. The free-radical quenching experiments, spectral technology and electron spin resonance (ESR) confirmed that Cr(VI) can be reduced by the conduction band (CB) electrons, and the h + and O 2 − radicals dominated OFL degradation. The optimized NCDs/DCN displayed excellent simultaneously photocatalytic H 2 production activity and RhB degradation with the H 2 evolution rate of 3.68 μmol‧h −1 ‧g −1 and 100% RhB removal efficiency. The photocatalytic activity of simultaneous combined pollutions removal and synergistic H 2 generation and RHB degradation provides a promising strategy for real wastewater remediation applications and energy utilization.

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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

In-situ formed N-doped bamboo-like carbon nanotubes encapsulated with Fe nanoparticles supported by biochar as highly efficient catalyst for activation of persulfate (PS) toward degradation of organic pollutants

Ke Zhu,Qiong Bin,Yaqian Shen,Jin Huang,Dongdong He,Wenjin Chen

In this study, N-doped bamboo-like carbon nanotubes encapsulated with Fe nanoparticles (Fe NPs) on the surface of soybean dregs-derived biochar (Fe@NCNT − BC) was synthesized via a low-cost and facile strategy. The unique composites behaved as efficient catalysts for the degradation of various organic pollutants by the activation of persulfate (PS). Under the conditions of [PS] = 5 mM, [RhB] = 20 mg/L, [Fe@NCNT-BC-800] = 1.0 g/L, pH = 7.0, the RhB degradation rate was very fast reaching up to 100% within 10 min. The system also exhibited significant high activity in a broad pH window (3.0–11.0). Meanwhile, the recycling experiments and Fe leaching tests further demonstrated the stability of Fe@NCNT − BC during the activation of PS. Most interestingly, the Fe nanoparticles played a key role in promoting the degree of graphitization and the formation of bamboo-like N-doped carbon nanotubes. Besides, the introduction of biochar significantly improved the dispersion ability to the Fe@NCNT − BC. The competitive radical quenching tests and electron paramagnetic resonance measurements (ESR) illustrated that instead of the traditional radicals (sulfate radicals and hydroxyl radicals), the non-radical singlet oxygen ( 1 O 2 ) was the dominant reactive oxidative species (ROS) in the Fe@NCNT-BC/PS system. A mechanistic study suggested that pyridinic N, graphitic N, sp 2 -hybridized carbon structure and C = O bond in the Fe@NCNT − BC − 800 promoted the generation of the ROS. This study successfully provides an economic and feasible method for synthesis of a novel catalyst as an eco-friendly and efficient material for the degradation of organic pollutants in the environment.

CAS / MDL: 80-05-7 68-35-9
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