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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Hollow Hierarchical Porous and Antihydrolytic Spherical Zeolitic Imidazolate Frameworks for Enzyme Encapsulation and Biocatalysis

Baozhu Zhao,Haowen Yang,Jin Mao,Qi Zhou,Qianchun Deng,Lei Zheng,Jie Shi

The creation of a new metal–organic framework (MOF) with a hollow hierarchical porous structure has gained significant attention in the realm of enzyme immobilization. The present work employed a novel, facile, and effective combinatorial technique to synthesize modified MOF (N-PVP/HZIF-8) with a hierarchically porous core–shell structure, allowing for the preservation of the structural integrity of the encapsulated enzyme molecules. Scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, confocal laser scanning microscopy, and other characterization tools were used to fully explore the changes of morphological structure and surface properties in different stages of the preparation of immobilization enzyme CRL-N-PVP/HZIF-8, thus showing the superiority of N-PVP/HZIF-8 as an enzyme immobilization platform and the logic of the immobilization process on the carrier. Additionally, the maximum enzyme loading was 216.3 mg mL–1, the relative activity of CRL-N-PVP/HZIF-8 increased by 15 times compared with the CRL@ZIF-8 immobilized in situ, and exhibited quite good thermal, chemical, and operational stability. With a maximal conversion of 88.8%, CRL-N-PVP/HZIF-8 demonstrated good catalytic performance in the biosynthesis of phytosterol esters as a proof of concept. It is anticipated that this work will offer fresh concepts from several perspectives for the creation of MOF-based immobilized enzymes for biotechnological uses.

研究领域: 材料科学 · 生物化学 · 生物技术 · 催化
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CHEMICAL ENGINEERING SCIENCE · 2025 · IF 4.3

The preparation of electrospun PVDF membranes and their applications in the removal of dyes, heavy metals and oil-water separation

Zixuan Xu,Liqiang Qi,Song Wang,Gaoshan Xing,Wen Wang,Zhaoyang Liu

The PVDF/PVP/SiO 2 /CS nanofibrous membrane was synthesized using polyvinylidene fluoride (PVDF), polyvinylpyrrolidone (PVP), nanosilica (SiO 2 ), and chitosan (CS) as raw materials through a one-step electrospinning process, specifically developed for the treatment of complex oily wastewater. The membrane exhibited exceptional hydrophilicity, underwater oil repellency, self-cleaning properties, and a porous fiber structure. Its pure water flux reached 7894.50 L·m −2 ·h −1 ·bar −1 , with an average fiber diameter of 130 nm and an underwater oil contact angle exceeding 140°. The hydration layer enabled the membrane to effectively separate oil–water mixtures and emulsions composed of engine oil, carbon tetrachloride (CCl 4 ), toluene (C 7 H 8 ), soybean oil, cyclohexane (C 6 H 12 ), and other oil agents from water, achieving an efficiency greater than 99 %. Furthermore, the PVDF/PVP/SiO 2 /CS nanofiber membrane successfully captured dyes and heavy metal ions through hydration, hydrogen bonding (HB), electrostatic interactions (ESI), π-π interactions, and chelation mechanisms. The retention efficiencies of the membrane for Rhodamine B (RB), chromium ions (Cr 6+ ), methyl orange (MO), methylene blue (MB), malachite green (MG), and lead ions (Pb 2+ ) were 71.4 %, 74.0 %, 83.3 %, 85.6 %, 88.5 %, and 95.1 %, respectively. After filtration, the membrane flux values were 6042.64, 6653.40, 5689.85, 5865.40, 5732.68, and 6652.70 L·m −2 ·h −1 ·bar −1 , with a maximum membrane flux loss of no more than 25 %. The membrane demonstrated retention efficiencies of 72.4 %, 75.3 %, 79.4 %, 81.2 %, 84.3 %, and 92.3 % for the removal of RB, Cr 6+ , MO, MB, MG, and Pb 2+ from wastewater containing dual pollutants of oil–water emulsions with heavy metal ions and dyes. The separation efficiency for oil–water emulsions in the dual-pollutant wastewater exceeded 99 %.

研究领域: 环境科学 · 材料科学 · 化学工程 · 纳米技术 · 水处理 · 膜技术
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Polymer Chemistry · 2015 ·Vol. 6 ·期 21 ·3926-3933 · IF 5.52

Unraveling the forming mechanism of hierarchical helices via self-assembly of an achiral supramolecular polymer brush

Shanshan Liu,Qibin Chen,Yujie Sheng,Jincheng Shen,Changjun Peng,Honglai Liu

Developing supramolecular helical assemblies with a controlled helix sense and revealing the forming mechanism of hierarchical helices for mimicking biological self-organization and physiological processes remain major challenges. In this work, a bottlebrush-like supramolecular polymer is prepared through the formation of a hydrogen bond between the keto group of polyvinylpyrrolidone (PVP) and the phenolic hydroxyl group of p-dodecylphenol (PDP), characterized by 1H NMR and FT-IR spectroscopy. CD spectra show an unsplit Cotton effect, suggesting the emergence of a helical structure in this supramolecular polymer brush (PVP–PDP). In particular, straightforward experimental evidence for the formation of hierarchical helices is obtained via TEM and AFM methods. We propose a detailed structural transition of the hierarchical helix or superhelix of PVP–PDP from primary to secondary, tertiary and even quaternary structures, resulting from the incorporation of bulky pendant PDP into the PVP backbone and the binding site of the hydrogen bond at ortho-position.

研究领域: 超分子化学 · 高分子科学 · 材料科学 · 纳米技术 · 生物物理学
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ACS Applied Nano Materials · 2023 · IF 5.9

Simultaneous Modification of Dragon fruit-like TiO2 Nanoarchitectures to Enhance Lithium Storage

Zhitong Jia,Songyuan Sun,Ao Li,Huigui Wu,Guoqiang Qin,Tong Liu,Pengpeng Lv,Jingbo Chen

Titanium dioxide (TiO2) is a promising anode material for lithium-ion batteries with the characteristics of highly stable structure and excellent safety, while the application is constrained by its inferior electrical conductivity and sluggish lithium-ion diffusion kinetics. Herein, H2Ti4O9 was prepared as a precursor, and it was wrapped with polyvinylpyrrolidone (PVP) as the nitrogen and carbon sources. Then, the N-doped carbon-filled TiO2 nanocrystals (N-TiO2/C), which had a unique dragon fruit structure with TiO2 nanocrystals acting as seeds and carbon acting as the flesh, were successfully prepared from PVP-coated H2Ti4O9 by one-step heat treatment. It is noteworthy that four modification methods, including carbon filling, nanosizing, nitrogen doping, and morphological designing, are all accomplished simultaneously during this process. The N-TiO2/C composite exhibits an outstanding stable capacity of 444.6 mAh g–1 after 600 cycles at 1 A g–1, and it possesses a reversible capacity of 146.7 mAh g–1 at 5 A g–1. The superior electrochemical capacity can be attributed to the distinctive dragon fruit structure along with nitrogen doping and carbon filling. The ingenious modification strategy can extend to the investigation on the other oxide anode materials.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米技术
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DESIGNED MONOMERS AND POLYMERS · 2022 · IF 3.718

Design of novel temperature-resistant and salt-tolerant acrylamide-based copolymers by aqueous dispersion polymerization

Xiang Li,Ye Ju,Yongkang Jia,Fenggang Liu,Guangpu Liu,Shuo Wang,Haoyi Wang,Shihua Mao,Jintao Yang,Guangyan Du

Development of polymer-based flooding technology to improve oil recovery efficiency, water dispersion copolymerization of acrylamide, cationic monomer methacryloxyethyltrimethyl ammonium chloride (METAC), and anionic monomer acrylic acid (AA) were carried out in aqueous ammonium sulfate solution with polyvinyl pyrrolidone (PVP) as the stabilizer. The copolymers were characterized by 1H-NMR, FT-IR, TG, and SEM to confirm that they were prepared successfully and exhibited excellent salt-resistant property. Moreover, the effect of the aqueous solution of ammonium sulfate (AS) concentration, stabilizer concentration, and initiator concentration on the viscosity and size were systematically investigated. To further improve the thermal endurance properties of copolymer, hydrophobic monomers with different alkyl chain lengths were added to the above system. The acrylamide-based quadripolymer possessed prominent thermal and salt endurance properties by utilizing the advantages of zwitterionic structure and hydrophobic monomer. With the temperature rising, the viscosity retention could reach 70.2% in the water and 63.8% in the saline. This work had expected to provide a new strategy to design polymers with excellent salinity tolerance and thermal-resistance performances.

研究领域: 高分子科学 · 石油工程 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Fabrication of micro/nano spherulitic hierarchical energetic materials via noncrystallographic branching induced by polymer additives: A case study of 2,2′,4,4′,6,6′-hexanitrostilbene (HNS)

Min Li,Ying Wang,Xin Zhou,Qi Zhang,Mingyang Chen,Dandan Han,Junbo Gong,Hongzhen Li

In this work, the micro/nano spherulitic hierarchical 2,2′,4,4′,6,6′-hexanitrostilbene (HNS) with the excellent specific surface area was prepared for the first time, which was expected to overcome the agglomeration problems of nanoscale HNS. In detail, poly( N -isopropyl acrylamide) (PNIPAM), polysuccinimide (PSI), and polyvinylpyrrolidone (PVP) were selected as additives to induce forming spherulitic HNS. Leaflike crystals were obtained in the presence of PNIPAM, while spherulitic HNS could be fabricated in the presence of PSI or PVP. And the prepared spherulitic HNS owned nearly 6 times the specific surface area of the raw HNS, with decreased impact sensitivity and advanced melting and decomposition temperatures, demonstrating a good desensitization effect, and a favorable energy release of the hierarchical structure. Moreover, morphological changes under the effect of the molecular weight and concentration of PVP were explored. The approximated morphological evolution of spherulitic HNS was consistent with the classical spherulitic growth by noncrystallographic branching. Furthermore, it was verified that preferential adsorption of PVP and PSI on the HNS inhibits the growth steps of the (200) face and introduces stress to generate crystal defects, which triggers noncrystallographic branching and further spherulitic growth. Overall, the strategy of fabricating micro/nano spherulitic hierarchical energetic materials via polymer-additive induced noncrystallographic branching is promising to solve the problems of nanoscale energetic materials in agglomeration and microscale bulk crystals in low activity.

研究领域: 材料科学 · 高能材料 · 聚合物科学 · 纳米技术
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

A novel kind of hollow SiO2@g-C3N4@TiO2 microspheres for rapid removal of dyes and antibiotics in water under sunlight

Hao-Yu Zhou,Bai-Yu Feng,Zhen-bin Pang,Guo-Zhi Han

In this paper, using PVP-modified polystyrene microspheres as template, tetrabutyl titanate (TEOT), tetraethyl orthosilicate (TEOS) and melamine as precursor, we developed a facile one-pot two-step method to preparing a novel kind of mesoporous hollow SiO 2 @TiO 2 @g-C 3 N 4 ternary composite microspheres with plush surface, in which highly active black titanium dioxide (TiO 2 ) was formed by simple calcination without further chemical reduction treatment. The structure and morphology of the composite microspheres were detailed characterized for understanding the formation mechanism. Research results indicated that the hollow SiO 2 microspheres can promote the formation of oxygen vacancies in TiO 2 , and the ternary combination narrowed the bandgap width of the black hollow composite microspheres to 1.43 eV, thus endowing it with excellent broad-spectrum catalytic performance for rapid photo-degradation of persistent organic pollutants (POPs) such as dyes and antibiotics in water under sunlight. The removal rates of dyes reached more than 70 %, as well as that of antibiotics more than 50 % within one hour. Finally, a plausible catalytic degradation mechanism was discussed.

研究领域: 环境科学 · 材料科学 · 化学工程 · 水处理
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Advanced Healthcare Materials · 2025 · IF 9.6

A Multifunctional Janus Electrospinning Dressing with Sequential Drug-releasing Property for Programmed Treatments of Chronic Infected Wounds

Zhi Qu,Yang Wang,Zequan Liu,Wenzhan Fu,Xinmeng Li,Shenglin Ma,Lingwan Hao,Yu Wang,Weihua Liu,Rujian Jiang

Wound dressings equipped with disinfection and wound tissue regeneration capabilities demonstrate significant potential in chronic wound management. However, current multifunctional dressings can rarely accommodate multiple repair processes accurately due to the time-dependent variational wound microenvironment. Herein, a Janus wound dressing is developed based on electrospun nanofibrous scaffold featuring programmed drug release performance and asymmetrical wettability. Specifically, polyvinylidene fluoride (PVDF) nanofiber membrane as the outer layer to resist the external biofouling and provide essential mechanical support for the inner layer was firstly constructed. Subsequently, the inner layer composed of polyvinyl pyrrolidone (PVP) and polylactic acid (PLA) fibers which are separately loaded with bacterial-targeted nanoparticles (VHA NPs) and composite particle of zeolite imidazolate frameworks-8 containing deferoxamine (ZD NPs) is fabricated on the PVDF membrane. Experimental results demonstrated that the degradation rate of the inner layer could be precisely controlled to sequentially deliver the loaded drugs into the wound site. Taking advantages of the synergistic therapeutic effects including significant antibacterial activity, admired antioxidant property and remarkable angiogenesis performances, the fabricated Janus dressing (PF/PHPD) achieves superior performance for promoting infected wound healing in a full-thickness skin wound model, much better than that of conventional bandage and clinical antibiotic treated wound.

CAS / MDL: 1898-66-4
研究领域: 生物材料 · 组织工程 · 伤口愈合 · 纳米技术 · 药物递送系统 · 生物医学工程
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