POLYMER
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2022
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IF 4.432
Jing Yan,Jianghao Yao,Yinghui Hu,Diping Huang,Dongdong Yao,Fangzhou Wu,Qiuyu Zhang,Yi Yan
To enrich the building block and function as well as the preparation methodology of metallopolymer system, functioned inorganic polyoxometalate clusters were introduced by using their intrinsic acidity induced multiple interactions with triblock copolymers . In the designed triblock copolymer PEG- b -PDMAEMA- b -PTEPM, the POMs clusters can be immobilized through in-situ protonation of the PDMAEMA block induced electrostatic interaction and the self-gelation of the PTEPM block, while the PEG block can improve the water solubility and dispersion of the final polyoxometalate-based hybrid catalyst (PHC). The selective oxidation activity of PHC is comparable with the homogeneous POMs catalyst as demonstrated by the model reaction of the selective oxidation of methyl phenyl sulfide (MPS) to methyl phenyl sulfoxide (MPSO). By optimizing the ratio between PHC and oxidant H 2 O 2 , the selectivity for MPSO can achieve as high as 99% with conversion above 95%. Furthermore, the multiple interactions between POMs and the polymer substrate also enhance the stability of PHC and enable the recycling of PHC. Therefore, the methodology of in-situ protonation and self-gelation by the acidity of POMs provides a facile and general strategy to prepare robust POMs-based metallopolymers, paving a new avenue towards cluster-based materials and devices.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Chao Wang,Min Chen,Huimin Hu,Junwei Huang,Ting Jiang,Lei Peng,Qing Shi,Qiwu Zhang
The deep treatment of monovalent thallium (Tl + ) and the study of Tl + incorporation mechanism are of great value for water safety. However, current research objectives have focused on how to oxidize or precipitate Tl + , while neglecting to investigate the underlying mechanisms of the direct immobilization and stable storage state of Tl + . Therefore, the present study examines in detail how Tl + is directly incorporated and stably stored by silicate minerals. In this study, an idea is proposed to enhance the purification of Tl-containing wastewater by using mechanically activated mica to stabilize Tl + in the silicate structure in the form of lattice residue state. Elucidation of the removal mechanism was first performed with focus on Tl + exchange with interlayer K + and H(H 2 O) + inside the silicate mineral based on the quantitative data and a series of characterizations such as XRD, XPS, FTIR, SEM-EDS and TG. As adsorbents for Tl-containing wastewater, both activated phlogopite and biotite for the purification of target wastewater demonstrated excellent performances at a dose of 2 g/L and a reaction time of 240 min, reaching quantitatively down to 23.88 μg/L and nearly 0 μg/L respectively, from an initial Tl + concentration of 1203 μg/L, so that the effluent concentrations would meet the requirements of US EPA and Chinese discharge standards for industrial wastewater and drinking water. In addition, density functional theory (DFT) calculation was used to quantify the adsorption energy of Tl + being solidified in the interlayer structure to further give insight into the mechanism of Tl + immobilization by silicate mineral.
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CHINESE JOURNAL OF CATALYSIS
·
2023
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IF 16.5
Suwei Xia,Qixing Zhou,Ruoxu Sun,Lizhang Chen,Mingyi Zhang,Huan Pang,Lin Xu,Jun Yang,Yawen Tang
The ingenious design and feasible fabrication of affordable, active and robust electrocatalysts toward the oxygen reduction reaction (ORR) is imperative importance for the advancement of advanced sustainable energy technologies. The electronic structure modulation via the establishment of Mott- Schottky heterojunctions offers a powerful leverage to realize the boosted electrocatalytic intrinsic activity, yet remaining challenging. Herein, an ingenious self-sacrificial template strategy is developed for the fabrication of an advanced hybrid Mott-Schottky electrocatalyst composed of CoNi alloyed nanoparticles in-situ implanted within N-doped carbon nanotube/nanowire-integrated hierarchical superstructures (CoNi@N-CNT/NWs). The combinations of experimental and theoretical studies demonstrate that the rectifying contact of CoNi nanoalloys and N-CNT/NWs can induce the self- driven charge transfer across the Mott-Schottky heterojunctions, giving rise to the improved electron transfer rate, reconfigured charge distribution, and boosted intrinsic activity. Moreover, the “branches”/“trunk“- structured carbon substrates can offer the tight structural interconnectivity and highly accessible channels for active site exposure, thus dramatically facilitating the mass transfer during the electrocatalytic process. As anticipated, the as-prepared CoNi@N-CNT/NWs exhibit prominent ORR performance with a half-wave potential ( E 1/2 ) of 0.86 V and exceptional long-term stability in 0.1 mol L −1 KOH. The innovational manipulation of electronic state via the of Mott-Schottky heterojunctions can enlighten the rational design of electrocatalysts with excellent performance.
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CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Yuan Sun,Wei-Ming Yin,Yan Wang,Nian-Dan Zhao,Xin-Yu Wang,Ji-Guo Zhang,Yuan-Ru Guo,Shujun Li,Qing-Jiang Pan
To remedy the heavy metal ion (HMI) pollution, unravel the relationship of material microstructure and removal performance and clarify relevant mechanism, magnesium-aluminum layered double oxide (MgAl-LDO) has been fabricated via a template method using cellulose. The variously performed characterizations show that ultra-thin flakes of about 5 nm are successfully accessible with the size of 50 ~ 100 nm. They are smaller than the ones prepared without the addition of cellulose. The distinctive structural feature endows the newly-synthesized LDO with large removal capacity for HMIs. Towards Cd 2+ , Pb 2+ and Cu 2+ , the removal capacity reaches as high as 1422.3, 1336.8 and 1135.4 mg·g −1 , respectively. Moreover, the highly achieved durability makes our LDO applicable to treating the polluted water. The mechanism of cation exchange along with deposition has been postulated. The Mg-OH moiety in the sample is found to dominate the HMI removal. The experimental findings are borne out by the first-principle density functional theory calculations on geometries, thermodynamics and electronic structures.
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ACS Applied Materials & Interfaces
·
2021
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IF 9.229
Jiang Wu,Junyi Zhu,Qiuji Wu,Ying An,Kangning Wang,Tengxiao Xuan,Junwen Zhang,Wenxiang Song,Huacheng He,Liwan Song,Jie Zheng,Jian Xiao
Efficient reconstruction of a fully functional skin after wounds requires multiple functionalities of wound dressing due to the complexity of healing. In these regards, topical administration of functionalized nanoparticles capable of sustainably releasing bioactive agents to the wound site may significantly accelerate wound repair. Among the various nanoparticles, superparamagnetic iron oxide (Fe3O4) nanoparticles gain increasing attractiveness due to their intrinsic response to an external magnetic field (eMF). Herein, based on the Fe3O4 nanoparticle, we developed a fibroblast growth factor (bFGF)-loaded Fe3O4 nanoparticle using a simple mussel-inspired surface immobilization method. This nanoparticle, named as bFGF-HDC@Fe3O4, could stabilize bFGF in various conditions and exhibited sustained release of bFGF. In addition, an in vitro study discovered that bFGF-HDC@Fe3O4 could promote macrophage polarization toward an anti-inflammatory (pro-healing) M2 phenotype especially under eMF. Further, in vivo full-thickness wound animal models demonstrated that bFGF-HDC@Fe3O4 could significantly accelerate wound healing through M2 macrophage polarization and increased cell proliferation. Therefore, this approach of realizing sustained the release of the growth factor with magnetically macrophage regulating behavior through modification of Fe3O4 nanoparticles offers promising potential to tissue-regenerative applications.
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PubMed
高影响因子
BIOPROCESS AND BIOSYSTEMS ENGINEERING
·
2019
·Vol. 43
·期 1
·21-31
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IF 2.371
Zhang Xiao-Jian,Wang Wen-Zhong,Zhou Rong,Liu Zhi-Qiang,Zheng Yu-Guo
Abstract tert -Butyl (3 R ,5 S ) - 6-chloro-3,5-dihydroxyhexanoate [(3 R ,5 S )-CDHH] is the key chiral intermediate to synthesize the side chain of the lipid-lowering drug rosuvastatin. Carbonyl reductases showed excellent activity for the biosynthesis of (3 R ,5 S )-CDHH. The requirement of cofactor NADH/NADPH leads to high cost for the industrial application of carbonyl reductases. In this study, a self-sufficient biocatalyst based on carbonyl reductase and NADP + co-immobilization strategy was developed on an amino resin carrier LX-1000HAA (SCR-NADP + @LX-1000HAA). The self-sufficient biocatalyst achieved in situ cofactor regeneration and showed the activity recovery of 77.93% and the specific activity of 70.45 U/g. Asymmetric synthesis of (3 R ,5 S )-CDHH using SCR-NADP + @LX-1000HAA showed high enantioselectivity (> 99% e.e.) and yield (98.54%). Batch reactions were performed for ten cycles without extra addition of NADP + , and the total yield of (3 R, 5 S )-CDHH achieved at 10.56 g/g biocatalyst. The present work demonstrated the potential of the self-sufficient biocatalyst for the asymmetric biosynthesis of rosuvastatin intermediate. Graphic abstract
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PubMed
高影响因子
BIORESOURCE TECHNOLOGY
·
2019
·
IF 6.669
Konglong Feng,Zaocheng Huang,Bo Peng,Weijie Dai,Yunqi Li,Xiaoai Zhu,Yunjiao Chen,Xing Tong,Yaqi Lan,Yong Cao
Deacidification of high-acid soy sauce residue (SSR) oil is crucial to utilization of SSR oil. Aspergillus niger lipase (ANL) has been widely applied for such purpose while its immobilization still has large room for improvement. ANL was immobilized onto six different macroporous acrylic resins, accounting the effect of the different textural properties of resins on stability and their potential for application in enzymatic deacidification. The resin MARE with lower porosity, higher bulk density, and medium hydrophobicity, was chosen as the best carrier for the best thermostability and reusability. ANL-MARE is a promising catalyst than Novozym 40086, which not only exhibited higher deacidification activity and good thermostability, but also was continuously reused for 15 cycles and efficiently catalyzed from high-acid SSR oil into diacylglycerol-enriched oil. Therefore, immobilized ANL was a novel, low-cost and recyclable biocatalyst that could be used as a good alternative to higher-cost commercial lipases in industrial applications.
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PubMed
高影响因子
CORROSION SCIENCE
·
2019
·
IF 6.355
Yanhui Cao,Dajiang Zheng,Jingsong Luo,Fan Zhang,Cheng Wang,Shigang Dong,Yanlong Ma,Zhaoyuan Liang,Changjian Lin
In this work, a novel in-situ grown layered double hydroxide (LDH) film co-intercalated with inhibitors (vanadates) and low surface energy substance (laurates) was immobilized on Al substrates. A long-term monitoring of electrochemical impedance spectra (EIS) of the various samples in 3.5 wt.% NaCl solution demonstrated the synergetic protection of the intercalated two functional species. Meanwhile, the X-ray diffraction (XRD) result of the samples after immersion in NaCl solution for a long time presented the anion-exchange process between vanadates/laurates and chlorides. The synergetic effect of the two species loaded film significantly contributed to the enhanced long-term corrosion protection of aluminum.
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高影响因子
Food & Function
·
2019
·Vol. 10
·期 9
·5461-5472
·
IF 3.241
Xilian Yang,Yanli Ma,Lirong Li
β-Glucosidase (BG) was immobilized on the surface of bifunctionalized nano-magnetic iron oxide with silica and amine groups (Fe3O4@SiO2-NH2). The aroma and flavonoid aglycone enhancement effect of BG in tea soup was investigated. The immobilized BG-synthesized nanocomposite morphology and structure were characterized by using different analytical techniques, including Fourier transform infrared spectroscopy and scanning electron microscopy. The immobilized BG showed enhanced pH and temperature endurance at an optimum pH of 5.0 and temperature of 65 °C. After seven cycles of reuse, immobilized BG showed 51.8% initial activity. Immobilized-BG treatment in green tea and black tea soup elevated the aroma content by approximately 16% and 48%, respectively. In addition, flavonoid aglycones, such as myricetin, kaempferol, and quercetin, in green tea and black tea soup increased by approximately 65- and 5-fold, respectively. These results suggested that immobilized BG showed excellent potential in the enhancement of aroma and effectively hydrolyzed the flavonoid glycosides to release flavonoid aglycones in tea soup. Hence, this study provides a green and sustainable approach for the tea industry to efficiently enhance tea soup properties.
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高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2019
·
IF 4.784
Qingmei Yu,Zhou Wang,Yewang Zhang,Ruijiang Liu
Magnetic Ni 0.5 Zn 0.5 Fe 2 O 4 @SiO 2 nanocomposite was prepared via the rapid combustion process, and its surface was modified to obtain amino-functionalized magnetic Ni 0.5 Zn 0.5 Fe 2 O 4 @SiO 2 -NH 2 nanocomposite. The modified nanocomposite was loaded on graphene oxide (GO), on which penicillin G acylase (PGA) was covalently immobilized. The structure for docking was visualized between PGA and penicillin G using the PyMol program, which revealed the configuration of the active site. Selections of immobilization conditions including immobilization concentration and time of fixation, were explored. The catalytic performance of the immobilized PGA was characterized. The immobilized and free PGA had the highest activity at pH 8.0 and 45 °C. Compared with the activity of the free PGA, the activity of the immobilized PGA was affected less by pH and temperature. The immobilized PGA exhibited the high-effective activity and good stability. V max and K m of immobilized PGA were 0.8123 mol·min −1 and 0.0399 mol·L −1 , respectively. Free PGA's V max and K m were 0.6854 mol·min −1 and 0.0328 mol·L −1 . Immobilized PGA remained >70% in relative activity after 9 successive cycles.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Dingsheng Wu,Quan Feng,Tao Xu,Anfang Wei,Hao Fong
The aim of this study is to develop high-performance carrier/support for immobilization of enzyme ( e.g. , laccase). The hypothesis is that electrospun blend nanofiber membrane consisting of polyurethane (PU), amidoxime polyarcylonitrile (AOPAN), and β-cyclodextrin (β-CD) would possess the desired morphological, mechanical, and chemical properties for the coordination/chelation of Fe(III) ions and the subsequent immobilization of laccase molecules. To test this hypothesis, the Fe(III)-PU/AOPAN/β-CD nanofiber membrane has been prepared and characterized first; thereafter, the membrane’s performance as laccase immobilization carrier/support has been investigated. The results indicate that the prepared nanofiber membrane can efficiently immobilize laccase, and it also possesses excellent morphological/mechanical properties and regeneration capability. In specific, the membrane’s immobilization amount of laccase reaches a high value of 186.34 mg/g; moreover, the immobilized laccase exhibits reasonably high catalytic activity and significantly improved resistance against the variations of temperature and p H value than the free laccase. Additionally, thermal stability, storage stability, and reusability of the immobilized laccase are substantially improved; and the membrane carrier/support can also be regenerated/reused for several times. Therefore, the developed electrospun PU/AOPAN/β-CD blend nanofiber membrane is a high-performance carrier/support for efficient and reusable immobilization of laccase.
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RSC Advances
·
2017
·Vol. 7
·期 5
·2650-2657
·
IF 3.108
Zhike Wang,Cunling Ye,Lingyun Chen,Haili Wu
Adsorptive removals of naphthols are often interfered by some coexisting anions of aqueous solutions. In this work, 1-vinyl-3-octadecylimidazolium cations and p-styrenesulphonate anions were chemically co-modified on silica (denoted as Sil-PImC18-SS) via the click chemistry reaction and were characterized. This material was created with the aim to explore the feasibility of removal of 1-naphthol (1-NAP) and 2-naphthol (2-NAP) from aqueous solutions. The prepared Sil-PImC18-SS was used as an adsorbent to remove 1-NAP and 2-NAP from aqueous solutions and the effects of various variables for the adsorption of 1-NAP and 2-NAP were systematically studied. Among the coexisting anions tested, 0.2 mol L−1 background NaCl or Na2SO4 aqueous solutions had no significant effect on the adsorption of 1-NAP and 2-NAP. The adsorption behaviors of 1-NAP and 2-NAP were well described by the pseudo-second order kinetic and the Dubinin–Radushkevich models with the maximum adsorption capacities of 84.4 mg g−1 and 71.9 mg g−1 for 1-naphthol and 2-naphthol, respectively. The adsorption was a spontaneous and exothermic process, and an adsorption mechanism was speculated to be the cooperative contributions from the hydrophobic interaction, hydrogen bonding interaction, and π–π stacking. Thus, Sil-PImC18-SS can be potentially used as an effective adsorption material for naphthol pollutant removal from the water environment.
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