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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2019 · IF 6.361

Negatively-charged nanofiltration membrane and its hexavalent chromium removal performance

Xiu-Zhen Wei,Zhi-Qiang Gan,Yu-Jie Shen,Ze-Lin Qiu,Li-Feng Fang,Bao-Ku Zhu

To enhance hexavalent chromium (Cr(VI)) removal performance under acidic conditions, the nanofiltration (NF) membrane with enhanced negative charge was fabricated via introducing 2, 5-diaminobenzenesulfonic acid (DABSA) into polyamide layer. The control membrane (NF-P) was directly prepared from piperazine and 1, 3, 5-benzenetricarbonyltrichloride. Surface chemical compositions , morphology, surface charge, pore size, permeability and pH-dependent separation performance of the fabricated membranes were characterized. The membranes showed the similar water permeance (∼11.5 L m -2  h −1  bar −1 ) and Na 2 SO 4 rejections (∼98%) under neutral environments. The DABSA introduced NF membrane (NF-PD) was negatively charged in the pH range of 2.5–11, while the isoelectric point for NF-P was ∼pH 4.0. Cr(VI) removal ability was then evaluated under various concentrations and pH environments. The results indicated that NF-PD showed the better Cr(VI) rejection performance in all tested conditions than NF-P, especially under acidic environments (e.g., pH 4 and pH 5). Moreover, there was a fluctuation of the rejection with the increase of Cr(VI) concentration under acidic environments, which was mainly caused by the formation of Cr 2 O 7 2− species. The harmful Cr(VI) was efficiently removed by the NF membrane with enhanced negative charge under acidic environments, which indicated the wider application range of the NF membrane.

研究领域: 环境科学 · 材料科学
✓ 已验证 DOI PubMed 高影响因子
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY · 2024 · IF 5.9

Leaf-like ZIF-L as self-sacrificed template via acid induced removal for stronger negatively charged PES membranes based on RTIPS method

Yi Guo,Jinchao Chen,Chunmei Gao,Shifeng Ji,Yunqing Xing,Wenjing Tan

In this paper, ZIF-L was blended with citric acid (CA) and polyethersulfone (PES) to prepare a casting solution. A novel negatively charged ultrafiltration (UF) membrane (ZIF-L/CA/PES) was obtained using the reverse thermally induced phase separation (RTIPS) method. The hydrophilic carboxyl groups present in CA not only imparted high hydrophilicity and negative charge to the membrane surface, enhancing the membrane’s selectivity and contamination resistance, but also created an acidic environment to attack the Zn atoms in ZIF-L by the ionized H + from CA, resulting in the generation of micro-defective pores and an improvement in permeability. Additionally, the results showed that membranes generated through the RTIPS process exhibit uniform porous surfaces and spongy cross-sections, enhancing membrane performance. The optimized membranes demonstrated the capability to achieve a pure water flux of up to 2267 L/m 2 h with 93.1 % humic acid (HA) retention, and a remarkable membrane flux recovery rate of 75.8 %, suggesting the crucial roles played by CA and ZIF-L in the separation process. In conclusion, hydrophilic anti-fouling UF membranes with a high negative charge and excellent permeation selectivity were fabricated by establishing micro-defective channels through the incorporation of carboxylic acid and ZIF-L, combined with the RTIPS process.

CAS / MDL: 1415-93-6 693-98-1
研究领域: 材料科学 · 环境工程 · 膜技术
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JOURNAL OF HAZARDOUS MATERIALS · 2021 · IF 10.588

Cadmium removal by FeOOH nanoparticles accommodated in biochar: Effect of the negatively charged functional groups in host

Shunli Wan,Yan Li,Shuo Cheng,Guowei Wu,Xuan Yang,Yu Wang,Liangmin Gao

Metallic oxide nanoparticles (NPs) anchored in biochar provide a promising measure forward into the scaled-up application of these NPs in water treatment , and reducing the size of the dwelled NPs is expected to boost the adsorption performance of biochar-based composites because of the size and surface effect. Nevertheless, it is still of great challenge to regulate the size of the impregnated NPs due to their intrinsic self-agglomeration caused by high surface energy . In this study, we fabricated the charged biochar (C-BC) bearing high-density negatively charged groups (i.e., carboxyl and hydroxyl groups) via HNO 3 oxidization to load the model metal oxide FeOOH NPs. The average sizes of anchored FeOOH NPs were ultrasmall, ranging from 19.9 ± 1.5 to 3.1 ± 0.5 nm, and decreased with the increased amount of carboxyl and hydroxyl groups in C-BC. Whether in batch adsorption or fixed-bed column setting, adsorption of Cd(II) onto the as-made composites was greatly enhanced by carboxyl and hydroxyl groups in carrier. The normalized adsorption capacities of Cd(II) by ferric mass of the loaded FeOOH were 499.9–724.9 mg/g-Fe, approximately 18.6–27.1 and 2.51–3.64 folds over the bulky FeOOH and FeOOH-impregnated biochar. Our study results should provide a significant reference on how to acquire highly efficient biochar-based composites for water decontamination .

研究领域: 环境科学 · 材料科学
✓ 已验证 DOI PubMed 高影响因子
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JOURNAL OF MEMBRANE SCIENCE · 2019 · IF 7.015

Layer-by-layer assembly of high negatively charged polycarbonate membranes with robust antifouling property for microalgae harvesting

Rui Huang,Zhiquan Liu,Boyin Yan,Yaqiong Li,Huarui Li,Dongmei Liu,Peng Wang,Fuyi Cui,Wenxin Shi

To tailor low-biofouling membranes remains one of the most problematic issues in filtration for microalgae harvesting. The aim of this study is to develop a high negatively charged and hydrophilic membrane to reduce membrane fouling via bioinspired design and Layer-by-layer (LBL) self-assembly technique for the application in microalgae harvesting. Bioinspired adhesive based on the polydopamine and polyethylenimine (PDA/PEI) composite was first linked onto the neutrally charged PC membrane substrates, then the poly-(styrenesulfonate) (PSS)/poly-(diallyldimethylammonium chloride) (PDADMAC) layers were uniformly assembled by electrostatic attraction. The resultant highly negatively charged and hydrophilic PC membranes exhibit a zeta potential of -66.1 mV and a water contact angle of 26°. Moreover, the modified membranes present a high average flux (133.1 L m 2  h -1 ·bar -1 ) in 1-h microalgae filtration, a high algae retention (~100%) as well as a high flux recovery rate (over 94%). Meanwhile, the resultant membranes exhibit excellent chemical stability in high salty solutions, the low pH solutions and tolerance to long-time running in DI water. The combination of bioinspired construction method and LBL self-assembly technique could be expected to be a universal way to endow neutrally charged materials with highly negative or positive surface charge for various applications.

研究领域: 环境科学 · 材料科学 · 生物工程
✓ 已验证 DOI 高影响因子
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VIBRATIONAL SPECTROSCOPY · 2022 · IF 2.382

SERS detection of negatively charged molecules by interface-induced self-assembly of PDDA modified Ag nanoparticles

Yuanjie Teng,Zhenni Wang,Weihao Huang,Yuanbin She

Some noble metal colloids with negative charges were mostly used as surface-enhanced Raman scattering (SERS) substrates, that the Raman signals of negatively charged molecules are hard to be detected because of the electrostatic repulsion among them and the negatively charged metal nanoparticles . Herein, Ag nanoparticles (Ag NPs) with positive charges and its Ag nanofilm were prepared by poly dimethyl diallyl ammonium chloride (PDDA) to realize the SERS detection of negatively charged molecules directly. The zeta potential and its particle sizes were characterized to select the optimum condition of PDDA. In addition, the morphology of positive Ag NPs and Ag nanofilm was characterized by UV–Vis spectroscopy and transmission electron microscopy . The SERS effect of negatively charged thiamphenicol on positively charged Ag nanofilm was significantly enhanced at the optimum condition and its sensitivity was significantly improved compared with normal Ag nanofilm. The proposed novel positively charged Ag nanofilm can be further applied to detect other negatively charged molecules by SERS.

研究领域: 分析化学 · 纳米科学 · 光谱学
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ACS Catalysis · 2022 · IF 13.7

Negatively Charged Single-Atom Pt Catalyst Shows Superior SO2 Tolerance in NOx Reduction by CO

Yongjun Ji,Shaomian Liu,Shaojia Song,Wenqing Xu,Liang Li,Yu Zhang,Wenxing Chen,Huifang Li,Jingang Jiang,Tingyu Zhu,Zhenxing Li,Ziyi Zhong,Dingsheng Wang,Guangwen Xu,Fabing Su

Pt-based catalysts are promising for the selective catalytic reduction of NOx by CO (CO-SCR), but some technical issues hinder their practical application, including the high Pt loading needed, high reduction temperature, and the low tolerance toward SO2. Here, we report a novel Pt catalyst for CO-SCR, which has negatively charged single-atom Pt embedded on CuO squares, and the latter is supported on CoAlO nanosheets. This Pt–CuO/CoAlO catalyst with an ultra-low Pt loading (0.02 wt %) exhibited 91% NO conversion and 80% N2 selectivity in 3% O2 at 200 °C. More importantly, it showed almost no activity loss in 200 ppm SO2 over a 15 h test. The theoretical calculations reveal that the negatively charged Pt has a stronger NO adsorption ability than the positively charged Pt, and Cu serves as the CO adsorption site. The much-weakened SO2 adsorption on Pt–CuO/CoAlO relative to the NO and CO adsorption effectively avoids the catalyst poisoning by SO2.

CAS / MDL: 10026-22-9
研究领域: 催化化学 · 环境科学
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MOLECULAR PHARMACEUTICS · 2018 · IF 4.556

Negative Surface Shielded Polymeric Micelles with Colloidal Stability for Intracellular Endosomal/Lysosomal Escape

Yun Zhu,Tingting Meng,Yanan Tan,Xiqin Yang,Yupeng Liu,Xuan Liu,Fangying Yu,Lijuan Wen,Suhuan Dai,Hong Yuan,Fuqiang Hu

The critical process and step in achieving effective antitumor therapies is facilitating endosomal escape, which can enhance the intracellular target delivery of therapeutics. However, the normally adopted approaches tend to result in colloidal instability as a result of the inevitable interactions between the resulting positively charged surfaces of micelles and proteins in vivo. Herein, negatively charged surface shielded polymeric micelles, consisting of polymethylacrylamide derivatives and hydrophilic chitosan (Mw = 18.8 kDa) linked by 3,3′-dithiodipropionic, are constructed. Until the pH decreases to less than 4.5, the DOX-loaded polymeric micelles (CSO-SS-PDPA/DOX) retain a negative surface charge as a result of the abundant amide groups, which could resist formation of the protein “corona” as visualized by transmission electron microscopy. Robust endosomal escape within tens of minutes due to protonated amine groups and specific redox-responsive drug release is visualized by confocal microscopy. The superior therapeutic efficacy in both 3D tumor spheroids and MCF-7 bearing mice further suggested that the prepared CSO-SS-PDPA/DOX is a promising approach for maintaining colloidal stability while achieving intracellular endosomal/lysosomal escape, which opens new opportunities for drug delivery.

研究领域: 药剂学 · 生物医学工程 · 肿瘤学
✓ 已验证 DOI PubMed 高影响因子
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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Novel negatively charged nanofiltration membrane based on 4,4′-diaminodiphenylmethane for dye removal

Chengyu Yang,Weixing Xu,Yang Nan,Yiguang Wang,Xianhong Chen

Membrane separation processes constitute an economical and efficient technology for the effective treatment of dye wastewater. In this study, 4,4′-diaminodiphenylmethane and 1,3,5-benzenetricarbonyl trichloride were used as monomers to prepare polyamide-based nanofiltration (NF) membranes by interfacial polymerization, for dye removal. The preparation parameters of the NF membrane were optimized by investigating the effects of the concentrations of two monomers, the soaking time of the carrier in aqueous solution of monomer, and the polymerization time on the membrane performance. The surface roughness of optimized membrane was found to be only 5.08 nm, and the stabilized contact angle was about 25°, indicating very high hydrophilicity. When the pH was in the range from 3 to 10, the membrane surface became electronegative, which resulted in a high rejection rate toward various negatively charged dyes. For the congo red dye solution, the membrane showed a flux of 36.81 L m −2 h −1 and a rejection rate of 99%. The rejection rate of the other two negatively charged dyes investigated herein was also above 95%. Moreover, the filtration experiment of bovine serum albumin solution showed that the flux recovery rate of the membrane was up to 89.85%, indicating good stability and antifouling performance.

研究领域: 环境科学 · 材料科学
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Highly negatively charged nanofiltration membrane prepared with a novel diamino-sulfonamide aqueous monomer for efficient removal of anionic dyes

Tengteng Xie,Kuo Chen,Hongxue Xie,Congcong Miao,Muan Yu,Feiyang Li,Yuhao Chen,Xiujie Yang,Peng Li,Q. Jason Niu

Nanofiltration (NF) membranes with negative surface charge are of critical significance for the efficient removal of anionic dyes from wastewater. In this work, a novel negatively charged NF membrane was prepared from a new sulfonamide monomer , 2,4,6-trimethyl-3,5-diaminobenzenesulfonamide (TMDBSA) and trimesoyl chloride (TMC) via interfacial polymerization. The unique diamino-sulfonamide structure of TMDBSA would be conducive to the formation of a poly (amide-sulfonamide) (PASA) layer with enhanced negative charge while maintaining the appropriate degree of crosslinking. The TMDBSA-TMC membrane prepared at optimized condition exhibits both high water permeability (19.6 L m −2 h −1 bar −1 ) and superior rejections of anionic dyes with different molecular weights (e.g. 98.3% rejection for methyl blue), reveals that Donnan exclusion dominates the rejection mechanism. More importantly, benefiting from the strong negatively charged surface and PASA structure, the TMDBSA-TMC membrane shows separation stability for the removal of methyl blue in a broad pH range, even under a harsh acid environment. Meanwhile, the membrane has excellent antifouling performance and long-term stability during the filtration tests. The newly developed negatively charged NF membrane demonstrates great practical application potential for the removal of anionic dyes with small molecular weights.

CAS / MDL: 25322-68-3
研究领域: 环境科学 · 材料科学 · 化学工程
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DESALINATION · 2020 · IF 7.098

How to fabricate a negatively charged NF membrane for heavy metal removal via the interfacial polymerization between PIP and TMC?

Jiayu Tian,Hailin Chang,Shanshan Gao,Ruijun Zhang

The potential toxicity of heavy metals arising from the discharge of industrial wastewater has become a serious public concern. Fabrication of a thin film composite (TFC) NF membrane with desirable rejection of heavy metal ions is an attracting route to solve this problem. Hereon, we proposed a facile strategy for fabricating a TFC NF membrane with excellent heavy metal removal. The ratio of PIP and TMC was greatly enlarged by decreasing the concentration of TMC to an exceptional low extent. Thus a polyamide film with weak electronegativity and small pore size was successfully constructed on an ultrafiltration substrate membrane. Comprehensive characterizations were adopted to reveal the micro-variation of the resulted NF membranes when regulating TMC concentration . The optimized membrane prepared only with PIP and TMC can exhibit a high pure water permeability of 14.6 L m −2  h −1  bar −1 , desirable rejection of over 98% against Ni 2+ , Zn 2+ , Cu 2+ , and >92.7% against Cd 2+ . This performance could go beyond most of the reported candidates which were prepared with other complicated methods. The simplicity, low cost and scaling up feasibility of the current strategy is expected to well meet the requirements of industrial production of TFC NF membrane for heavy metal removal.

研究领域: 环境科学 · 材料科学
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JOURNAL OF CHROMATOGRAPHY A · 2025 · IF 4

Enhanced extraction of negatively charged emerging contaminants by amine-modified amphiphilic materials-based solid phase microextraction fibers

Wei Jiao,Xinyi He,Ziang Zhang,Zongli Huo,Feng Zhu,Qing Zhou

The solid phase microextraction (SPME) technique is an efficient method for emerging contaminants (ECs) detection, however, many commercial fibers are not suitable for extracting negatively charged ECs. Herein, three amine-functionalized amphiphilic materials(MAM) were synthesized via a high-speed shear dispersion emulsification technique. These materials were employed as SPME fiber coatings to enhance the selectivity for negatively charged ECs, attributed to their substantial specific surface area (679-693 m 2 /g), high ion-exchange capacity (1.55-2.57 mmol/g) and good hydrophilicity (contact Angle of 63.8-83.9°). The MAM-PIP coating demonstrates superior selectivity and efficiency for negatively charged compounds across a broad spectrum of polarities compared to Oasis® WAX, commercial C18, and CAR coatings. A novel analytical method employing SPME (piperazine-modified MAM) in conjunction with LC-MS/MS was developed. The enrichment factors for 21 ECs ranged from 408 to 7,129. The method exhibited excellent linearity within the concentration range of 10-5,000 ng/L, with limits of detection (LOD) ranging from 0.03 to 2.59 ng/L and limits of quantitation (LOQ) from 0.1 to 8.62 ng/L. The relative standard deviations were consistently below 15%. Comparative analysis with existing literature indicates that the developed method holds significant potential for commercial application in extracting ECs from environmental water samples.

研究领域: 环境科学 · 分析化学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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Catalysis Science & Technology · 2016 ·Vol. 7 ·期 2 ·387-395 · IF 5.287

Chemical and photochemical water oxidation catalyzed by novel ruthenium complexes comprising a negatively charged NCNHCO ligand

Wei Su,Hussein A. Younus,Kui Zhou,Zafar A. K. Khattak,Somboon Chaemcheun,Cheng Chen,Francis Verpoort

Incorporation of negatively charged moieties into complexes is a promising strategy to develop water oxidation catalysts with high stability and low over-potentials. We reported here the synthesis of a novel pincer-type ligand precursor, 1-(pyridin-2-ylmethyl)-3-methylcarboxylate-imidazolium (1). Deprotonation of C2-H of 1 resulted in formation of NCNHCO, a negatively charged asymmetric N-heterocyclic carbene (NHC). Complexes [Ru(NCNHCO)(terpy)]+ (2) and RuCl(NCNHCO)(DMSO)(pic) (3) were prepared and capable of decomposing water chemically and photo-chemically. Under acidic conditions, 4-picoline/H2O exchange in 3 was detected by UV-vis and 1H NMR, forming the corresponding Ru–aqua complex. In a typical three-component light-induced water oxidation, a turnover number of 273 was attained employing 3, which demonstrated catalytic ability comparable to those state-of-the-art catalysts.

研究领域: 化学 · 催化科学
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