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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Biochar accelerated Fenton process for roxarsone oxidation, inorganic arsenic adsorption and simultaneous immobilization of arsenic-iron sludge

Siqi Wang,Jia Wang,Lingzhi He,Fang Luo,Zhuwei Liao,Yi Wu,Zhuo Liu,Yu He,Zhuqi Chen

Complete remediation of organoarsenics from environmental matrix hits the bottleneck, that is, the sluggish efficiency of oxidative degradation towards organoarsenics and unsatisfying immobilization performance towards generated inorganic arsenic. Herein, we establish a biochar accelerated Fenton (BA-Fenton) process to decontaminate water from roxarsone (ROX). In comparison with Fe 2+ /H 2 O 2 process (10 μΜ/0.2 mM), the incorporation of 0.5 g L -1 biochar promoted ROX degradation from 48.2% to 98.2% and total arsenic elimination from 67.6% to 97.3%, respectively. In BA-Fenton process, •OH as the dominant reactive oxygen species (ROS), exhibited a cumulative concentration of 0.42 mM, three times higher than that in classical Fenton process. Crucially, the presence of biochar in Fenton process significantly enhanced the stability of arsenic-iron sludge, whereas the secondary leaching of total arsenic decreased from 433.8 μg-As L -1 to 13.9 μg-As L -1 , meeting the prescribed environmental quality standards for surface water in China (50 μg-As L -1 , GB 3838-2002). Mechanistic studies unveiled ROX remediation mechanism by BA-Fenton process, highlighting the dual functionality of biochar. On one hand, biochar efficiently reduced Fe 3+ to Fe 2+ with a rate constant of 0.225 min -1 , overcoming the rate-determining step of classical Fenton process for •OH production, consequently promoting the transformation of ROX to As(V). On the other hand, molecular spectroscopy analysis elucidated that in-situ formed As(V) was adsorbed by ferric hydroxides with the formation of arsenic-iron sludge. Subsequently, biochar immobilized arsenic-iron sludge through hydrogen bonds, electrostatic attraction and surface complexation. Furthermore, real water studies demonstrated the effective remediation of organoarsenics by BA-Fenton process in tap water, lake water and chicken manure leachate. This “Two Birds with One Stone” strategy with low-cost, environmental-friendly and sustainable biochar holds great promise for the ultimate disposal of industrial wastewater containing organoarsenics.

CAS / MDL: 7705-08-0 1415-93-6
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2024 · IF 7.7

Biomimetic immobilization of α-glucosidase inspired by antibody-antigen specific recognition for catalytic preparation of 4-methylumbelliferone

Shuang Guo,Shuo Liu,Chang Liu,Yi Wang,Dongyu Gu,Jing Tian,Yi Yang

Immobilization technology plays an important role in enhancing enzyme stability and environmental adaptability. Despite its rapid development, this technology still encounters many challenges such as enzyme leakage, difficulties in large-scale implementation, and limited reusability. Drawing inspiration from natural paired molecules, this study aimed to establish a method for immobilized α-glucosidase using artificial antibody-antigen interaction. The proposed method consists of three main parts: synthesis of artificial antibodies, synthesis of artificial antigens, and assembly of the artificial antibody-antigen complex. The critical step in this method involves selecting a pair of structurally similar compounds: catechol as a template for preparing artificial antibodies and protocatechualdehyde for modifying the enzyme to create the artificial antigens. By utilizing the same functional groups in these compounds, specific recognition of the antigen by the artificial antibody can be achieved, thereby immobilizing the enzymes. The results demonstrated that the immobilization amount, specific activity, and enzyme activity of the immobilized α-glucosidase were 25.09 ± 0.10 mg/g, 5.71 ± 0.17 U/mg protein and 143.25 ± 1.71 U/g carrier , respectively. The immobilized α-glucosidase not only exhibited excellent reusability but also demonstrated remarkable performance in catalyzing the hydrolysis of 4-methylumbelliferyl-α-D-glucopyranoside.

CAS / MDL: 609-99-4
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Nanoscale · 2024 · IF 5.8

Co-immobilization of a bi-enzymatic cascade into hierarchically porous MIL-53 for efficient 6′-sialyllactose production

Xinlv Peng,Caixia Pei,Eika W. Qian,Yuguang Du,Jian-Jun Li

6′-Sialyllactose (6′-SL), the most abundant sialylated human milk oligosaccharide, has attracted attention for its potential application in supplementary infant formulas. Herein, we report a facile strategy to construct a cascade bioreactor for the enzymatic synthesis of 6′-SL by co-immobilizing an enzymatic module consisting of CMP–sialic acid synthase and α-2,6-sialyltransferase into hierarchically porous MIL-53 (HP-MIL-53). The as-prepared HP-MIL-53 showed high enzyme immobilization capacity, reaching 226 mg g−1. Furthermore, the co-immobilized enzymes exhibited higher initial catalytic efficiency, and thermal, pH and storage stability than the free ones. Finally, the 6′-SL yield remained >80% after 13 cycles of use. We expect that HP-MIL-53 would have potential industrial applications in the enzymatic modular synthesis of 6′-SL and other glycans.

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International Journal of Nanomedicine · 2015 · IF 4.383

Immobilization of collagen peptide on dialdehyde bacterial cellulose nanofibers via covalent bonds for tissue engineering and regeneration

Xiaoxiao Wen,Yudong Zheng,Jian Wu,Lu-Ning Wang,Zhenya Yuan,Jiang Peng,Haoye Meng

Bacterial cellulose (BC) is an alternative nanostructured biomaterial to be utilized for a wide range of biomedical applications. Because of its low bioactivity, which restricted its practical application, collagen and collagen hydrolysate were usually composited into BC. It is necessary to develop a new method to generate covalent bonds between collagen and cellulose to improve the immobilization of collagen on BC. This study describes a facile dialdehyde BC/collagen peptide nanocomposite. BC was oxidized into dialdehyde bacterial cellulose (DBC) by regioselective oxidation, and then composited with collagen peptide (Col-p) via covalent bonds to form Schiff’s base type compounds, which was demonstrated by the results of microstructures, contact angle, Col-p content, and peptide-binding ratio. The peptide-binding ratio was further affected by the degree of oxidation, pH value, and zeta potential. In vitro desorption measurement of Col-p suggested a controlled release mechanism of the nanocomposite. Cell tests indicated that the prepared DBC/Col-p composite was bioactive and suitable for cell adhesion and attachment. This work demonstrates that the DBC/Col-p composite is a promising material for tissue engineering and regeneration.

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JOURNAL OF MEMBRANE SCIENCE · 2015 · IF 5.056

In situ immobilization of silver nanoparticles for improving permeability, antifouling and anti-bacterial properties of ultrafiltration membrane

Lichuan Huang,Song Zhao,Zhi Wang,Junhui Wu,Jixiao Wang,Shichang Wang

In this work, silver nanoparticles (AgNPs) were in situ immobilized on polysulfone (PSf) ultrafiltration membrane via polydopamine (PDA) deposition and in situ reduction of silver ammonia aqueous solution (Ag(NH 3 ) 2 OH). The adhesive and reductive PDA layer existing on the membrane surface induced the reduction of Ag + on the site of surface without surface pore blockage, and also favored to the firm attachment and uniform distribution of AgNPs onto the membrane. The diameter and density of the immobilized AgNPs were regulated by changing [Ag(NH 3 ) 2 ] + ion concentration, which exerted an influence on membrane hydrophilicity and permeation flux. The prepared AgNPs-PDA/PSf membranes were characterized by X-ray photoelectron spectroscopy (XPS), scanning election microscope (SEM), atomic force microscopy (AFM), water contact angle measurement and thermogravimetric analysis (TGA). The results indicated that AgNPs were immobilized on the surface as well as the top layer cross section of the membranes. The increase of Ag + ion concentration led to an increase in the size and density of AgNPs anchored onto the membrane. Compared with PSf membrane, AgNPs-PDA/PSf (20   mM) membrane showed higher water flux, slower flux decline rate during BSA solution filtration and higher flux recovery ratio after simple water flushing. The AgNPs-PDA/PSf (20   mM) membrane possessed excellent stability with little release of silver during the filtrate operation or static immersion in water for 12 days. Besides, AgNPs-PDA/PSf (20   mM) membrane displayed excellent anti-bacterial and ani-biofouling properties against E . coli and B . subtilis .

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RSC Advances · 2017 ·Vol. 7 ·期 45 ·28114-28123 · IF 3.108

Immobilization of tyrosinase on polyacrylonitrile beads: biodegradation of phenol from aqueous solution and the relevant cytotoxicity assessment

Qiao Wu,Zhiqun Xu,Yunjian Duan,Yincan Zhu,Minrui Ou,Xiaoping Xu

An economical and stabilized immobilized-enzyme method was developed for the removal of phenol in wastewater. Tyrosinase was immobilized on the PAN-based beads with glutaraldehyde as was confirmed successfully by a series of characterizations involving Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), and energy dispersive X-ray spectroscopy (EDS). The biodegradation of phenol was investigated by using the immobilized beads and compared to free tyrosinase. The optimum pH and temperature were determined to be 7.0 and 40 °C, respectively. Experiments showed that the immobilized tyrosinase was much more stable than the free tyrosinase in storage and that the immobilized tyrosinase could even retain about 78% of its original activity after repeated use 6 times in a batch system. Furthermore, the comparative in vitro cytotoxicity of phenol/treated solutions were evaluated in LO2 and HepG2 cells by using the CCK-8 assay for cell viability along with flow cytometry detection for apoptosis. The results showed that the toxicity of the phenol solutions only exerted toxicity on cells in a certain concentration range (>0.5 mM for LO2 and HepG2 cells) and that the toxicity of the phenol solutions was greatly decreased after treatment with the tyrosinase-immobilized beads. Thereby, the results confirm that we have established a suitable strategy with promising application to remove phenol economically and efficiently, which could even lower the toxicity of phenol at the cellular level.

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BIOCHEMICAL ENGINEERING JOURNAL · 2016 · IF 2.463

Monolithic biocatalytic systems with enhanced stabilities constructed through biomimetic silicification-induced enzyme immobilization on rGO/FeOOH hydrogel

Dong Yang,Jingjing Zhao,Xueyan Wang,Jiafu Shi,Shaohua Zhang,Zhongyi Jiang

In this study, we present a green and facile method of utilizing biomimetic silicification to trigger enzyme immobilization on the surface of the rGO/FeOOH hydrogel for constructing stable monolithic biocatalytic systems. In brief, the rGO/FeOOH hydrogel is firstly prepared through metal ion-induced reduction/assembly of graphene oxide (GO) nanosheets, which is then utilized to adsorb cationic polyethyleneimine (PEI). This cationic PEI, as the mineralization-inducing agent, catalyzes the condensation of silicate to form silica (biomimetic silicification) on the rGO surface, where enzyme is simultaneously entrapped. The resultant rGO/FeOOH/silica hydrogel shows an extraordinary three-dimensional (3D) porous structure. The silica content on the rGO surface can be facilely tailored through changing the silica precursor concentration. Combined with monolithic macroscale of the rGO/FeOOH/silica hydrogel, the acquired monolithic biocatalytic systems display easy recyclability and elevated pH/thermal/recycling/storage stabilities during the catalytic production of 6-aminopenicillanic acid (6-APA) in comparison to enzyme in free form and enzyme adsorbed on rGO/FeOOH hydrogel. Notably, the activity can be retained up to 93.3% of its initial activity after 11 reaction cycles for our biocatalytic systems.

CAS / MDL: 9002-98-6
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Chemistry-An Asian Journal · 2017 ·Vol. 12 ·期 24 ·3162-3171 · IF 4.083

Step-Up Synthesis of Periodic Mesoporous Organosilicas with a Tyrosine Framework and Performance in Horseradish Peroxidase Immobilization

Jianqiang Wang,Wenqi Zhang,Changqing Gu,Wenpei Zhang,Man Zhou,Zhiwei Wang,Cheng Guo,Linbing Sun

Graphical Tyr'd out : Novel periodic mesoporous organosilicas with a tyrosine framework (Tyr-PMOs) are constructed. Tyrosine units are incorporated into the framework at the same time as phenolic hydroxy groups as binding centers are introduced within the channels. A long storage time and conventional stability are found for the Tyr-PMOs after the immobilization of horseradish peroxidase (HRP). New amino-acid-bridged periodic mesoporous organosilicas (PMOs) were constructed by hydrolysis and condensation reactions under acid conditions in the presence of a template. The tyrosine bissilylated organic precursor (TBOS) was first prepared through a multistep reaction by using tyrosine (a natural amino acid) as the starting material. PMOs with the tyrosine framework (Tyr-PMOs) were constructed by simultaneously using TBOS and tetraethoxysilane as complex silicon sources in the condensation process. All the Tyr-PMOs materials were characterized by XRD, FTIR spectroscopy, N 2 adsorption–desorption, TEM, SEM, and solid-state 29 Si NMR spectroscopy to confirm the structure. The horseradish peroxidase (HRP) enzyme was first immobilized on these new Tyr-PMOs materials. Optimal conditions for enzyme adsorption included a temperature of 40 °C, a time of 8 h, and a pH value of 7. Furthermore, the novel Tyr-PMOs materials could store HRP for approximately 40 days and maintained the enzymatic activity, and the Tyr-PMOs–10 % HRP with the best immobilization effect could be reused at least eight times.

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MATERIALS RESEARCH BULLETIN · 2015 · IF 2.288

Immobilization of Candida rugosa lipase on ZnO nanowires/macroporous silica composites for biocatalytic synthesis of phytosterol esters

Chuan-Yang Shang,Wei-Xun Li,Rui-Feng Zhang

ZnO nanowires were successfully introduced into a macroporous SiO 2 by in-situ hydrothermal growth in 3D pores. The obtained composites were characterized by SEM and XRD, and used as supports to immobilize Candida rugosa lipase (CRL) through adsorption. The high specific surface area (233   m 2 /g) and strong electrostatic interaction resulted that the average loading amount of the composite supports reached 287.2   mg/g. Both adsorption capacity and the activity of the CRL immobilized on the composite supports almost kept unchanged as the samples were soaked in buffer solution for 48   h. The immobilized CRL exhibited better thermal stability, reusability and pH adaptability in comparison to free CRL. The immobilized CRL was used as biocatalyst for the preparation of phytosterol esters by the esterification of phytosterol and oleic acid. A maximum molar conversion of 96.5% was achieved under the optimal condition. After twelve recycles the immobilized lipase could retain 89.9% of its initial activity.

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SOLID STATE SCIENCES · 2014 · IF 1.679

Immobilization and catalytic properties of candida lipolytic lipase on surface of organic intercalated and modified MgAl-LDHs

Lijun Dong,Chunling Ge,Peiyong Qin,Yan Chen,Qinghong Xu

In this study, MgAl-LDHs (layered double hydroxides) intercalated with sodium dodecyl sulfate and outside surface modified with (3-aminopropyl)triethoxysilane (KH550) were prepared. The existence of organic part in LDHs improved immobilization efficiency and activity recovery of candida lipolytic lipase loaded. Also the positive charge in framework of LDHs was found to be beneficial to the enzyme immobilization. An immobilization efficiency of 56.4% and an activity recovery over 69.2% of the enzyme were obtained after it was loaded on the intercalated and modified LDHs, and catalytic activity of the immobilization can be kept at least five times. Moreover, the immobilized enzyme was found to have higher temperature resistance, wider pH value and better thermostability in reactive activity.

CAS / MDL: 919-30-2
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CHEMICAL ENGINEERING JOURNAL · 2013 · IF 3.473

Facile fabrication of hollow hydridosilica nanoparticles with mesoporous shell and their dual effect in Pd nanoparticles immobilization

Na Li,Jingjing Du,Lijian Xu,Jianxiong Xu,Tie-hong Chen

Synthesis of hollow hydridosilica nanoparticles with mesoporous shell (HMHNs) employing a mixture of cationic fluorocarbon surfactant (FC-04) and nonionic triblock copolymer surfactant (P123) as template and triethoxysilane as silica precursor is reported. It is found that the content of the FC-04 in the surfactant mixture greatly influences the aggregation state of the FC-04 and P123 surfactant template and therefore influences the morphology of the synthesized hydridosilica nanoparticles. HMHNs can be synthesized with proper amount of FC-04 surfactants due to the formation of FC-04 and P123 complex micelle, where FC-04 surfactant locates at the outer shell and the P123 constructs the inner core. Ascribed to the inherent hydride sites within the HMHNs, facile immobilization of Pd nanoparticles is achieved by using HMHNs as both the reducing agent and scaffold. The lesser processes produce some smaller Pd nanoparticles (2–3   nm) within the pore voids and relatively larger Pd nanoparticles (10–15   nm) on the outer surfaces of HMHNs. The catalytic hydrogenation of 4-nitrophenol demonstrates that the heterogeneous Pd catalyst is efficient.

CAS / MDL: 71-36-3
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PROGRESS IN NUCLEAR ENERGY · 2015 · IF 1.119

Adsorption and immobilization of actinides using novel SiO2–ZrO2-calcium alginate aerogels from high level liquid waste

Junchuan Zhao,Xingeng Ding,Cheng Meng,Chunrong Ren,Huiqin Fu,Hui Yang

The novel SiO 2 –ZrO 2 -calcium alginate aerogels were prepared by Sol–Gel process with phase separation method for investigating the adsorption and immobilization performance of the plutonium and minor actinides from high-level liquid waste (HLLW). The materials contained porous network structure with high surface area (233.44–481.08 m 2 /g) and pore volume (0.50–1.26 m 3 /g). The aerogels were superior adsorbents for the removal of plutonium and minor actinides, the maximum adsorption capacity and adsorption rate (35 °C, 75 rpm) reached 231.5 mg/g and 99.2%. For all the waste forms, SiO 2 , ZrO 2 and Ca 2 SiO 4 phases were simultaneously observed in the matrix. Moreover, Ce entered into Ca sites of Ca 2 SiO 4 and Zr sites of ZrO 2 . The substitution of Ca and Zr by Ce in the Ca 2 SiO 4 and ZrO 2 implies a promising disposal measure of actinides.

CAS / MDL: 25322-68-3 7699-43-6
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