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Science of Advanced Materials · 2015 ·Vol. 7 ·期 6 ·1021-1027 · IF 2.598

Chemical Attachment of Hydrogen Iodide to Carbon Nanotubes

Yu Jin-Gang,Chen Na,Jiao Fei-Peng,Liu Qi,Jiang Xin-Yu,Jiang Jian-Hui,Chen Xiao-Qing

A novel and facile method for preparing iodinated carbon nanotubes, with iodine and hydrogen simultaneously covalently bound to the surface of nanotubes, has been developed. The functionalized carbon nanotubes were fully characterized using Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, Raman spectroscopy, energy-dispersive X-ray (EDX) spectroscopy and thermogravimetric analyses. This is the first report on the successful functionalization of single-walled carbon nanotubes using hydroiodic acid.

研究领域: 材料科学 · 化学
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INDUSTRIAL CROPS AND PRODUCTS · 2023 · IF 5.9

Modular design of vegetable polyphenols enables covalent bonding with collagen for eco-leather

Yuanhang Xiao,Chunhua Wang,Jiajing Zhou,Jianhui Wu,Wei Lin

Natural renewable materials have been engineered to synthesize functional products because of their wide availability and excellent biodegradability. Particularly, vegetable polyphenols have been regarded as sustainable tanning agents in the leather industry. However, the non-covalent binding nature and high consumption of polyphenols in the leather matrix have limited its potential for replacing chrome tannage. In this work, we developed a series of new polyphenol derivatives by selectively conjugating cyanuric chloride (CC) with phenolic group, and therefore introduced covalent binding moieties in polyphenol for the tanning process. Specifically, polyphenols with different molecular sizes, i.e., tannic acid (TA), ellagic acid (EA), and gallic acid (GA), were modified and evaluated in a comparative study. The obtained triazine-conjugated polyphenol derivatives (i.e., GACC, EACC, and TACC) exhibited appropriate molecular weight (460−1130 Da) and superior stability in the tanning bath (pH ∼8.0), which can effectively penetrate collagen networks. We further investigated the tanning performance of GACC, EACC, TACC, and a commercial triazine tanning agent (i.e., SACC). These polyphenol derivatives exhibited covalent and non-covalent synergistic interaction with collagen, endowing leather with excellent fiber dispersion and overall performance (i.e., thermal stability, organoleptic and physical properties). Of note, the tanning system effectively reduced the dosage of polyphenols and organic carbon emission and improved the biodegradability of wastewater. Together with these outstanding results, we envision that this work will pave the promising way for eco-leather manufacturing.

研究领域: 材料科学 · 生物学 · 环境科学
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ACS Biomaterials Science & Engineering · 2016 · IF 0

Covalent Bonding of Heparin on the Crystallized Poly(lactic acid) (PLA) Membrane to Improve Hemocompability via Surface Cross-Linking and Glycidyl Ether Reaction

Zhu Xiong,Fu Liu,Haibo Lin,Jinglong Li,Yi Wang

The hemocompatibility of the dialysis membrane has been considered the key factor influencing the dialysis performance for curing the kidney malfunction. In this work, the commonly used anticoagulant heparin in the clinic was directly bonded to the poly(lactic acid) (PLA) membrane to improve the hemocompatibility via the glycidyl ether reaction. A novel precopolymer P(VP-VTES-GMA) was first prepared via free radical polymerization. The surface cross-linking of the precopolymer containing GMA segments enabled the membrane to anchor heparin through the glycidyl ether reaction. The chemical structure of the precopolymer was confirmed by 1H NMR. The surface chemistry was analyzed by XPS, toluidine blue staining, and solubility tests. The crystallization behavior, heat resistance, morphology, hydrophilicity, pore size, and pure water flux were investigated. The hemocompatibility was comprehensively investigated via APTT, PRT, PT, FIB, and platelet adhesion tests. The simulated dialysis performances relating to urea, creatinine, lysozyme, and BSA clearance were measured. All results demonstrated that the covalent bonding of heparin provided the PLA membrane with excellent hemcompatibility, hydrophilicity, heat resistance, and dialysis performance as well.

研究领域: 生物医学工程 · 材料科学
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JOURNAL OF HAZARDOUS MATERIALS · 2021 · IF 10.588

Removal of emulsified oil from water by using recyclable chitosan based covalently bonded composite magnetic flocculant: Performance and mechanism

Jiangya Ma,Xue Fu,Wei Xia,Rui Zhang,Kun Fu,Genyu Wu,Bangtao Jia,Sha Li,Jincheng Li

In this work, a novel recyclable covalently bonded magnetic flocculant (FS-MC) was successfully prepared by combining chitosan-based modified polymers (MCS) with Fe 3 O 4 @SiO 2 through a silane coupling agent. The covalent bond Fe–O–Si–O–C and the core–shell structure of FS-MC were confirmed through several characterization methods. The emulsified oily wastewater flocculation performance and mechanism by using FS-MC were evaluated and studied. Results showed that 94.47%, 93.95%, and 92.98% of emulsified oil could be removed by using FS-MC1, FS-MC2 and FS-MC3 at dosages of 2.0, 2.5, and 2.0 mg/L, respectively. Furthermore, FS-MC exhibited an excellent behavior on the removal of organic compounds with molecular weight > 10 kDa, including long chain alkanes, cycloalkanes , and aromatic hydrocarbon compounds. In addition, triple-phase separation of oil, water and flocculants was achieved by using magnetic FS-MC. Due to the introduction of cationic and hydrophobic groups in FS-MC, charge neutralization, compression double electric-layer action, hydrophobic interaction, interfacial adsorption bridging and sweep-flocculation synergistically contributed and enhanced the removal of emulsified oil. Recycling experiments also showed that no obvious decrease of oil removal rate was observed by using magnetic FS-MC flocculants in five cycles.

研究领域: 环境科学 · 材料科学
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DIAMOND AND RELATED MATERIALS · 2022 · IF 3.806

Improving the thermal conductivity of natural rubber by constructing three-dimensional thermal conductivity networks and chemically bonded filler-matrix interaction

Xiaoyuan Duan,Rizheng He,Dong An,Jie He,Rongyao Tao,Yiwen Cui,Chaobo Liang,Zhijian Sun,Yaqing Liu,Chingping Wong

It has become the mainstream way to take advantage of the new carbon materials to modify polymer matrix to prepare thermal interface materials (TIMs) with excellent comprehensive properties for the modern electronic packaging materials. Yet, how to make full use of the properties of new carbon materials is still facing the severe challenges. Herein, thiol-functionalized carbon nanotubes/natural rubber (CNTs-SH/NR) TIMs with three-dimensional networks (3D) and covalently bonded filler/matrix interactions were fabricated through the surface chemical treatment as well as ice-templated approach. The results proved that CNTs-SH/NR TIMs could achieve a high through-plane thermal conductivity of 1.22 W m −1  K −1 with CNTs-SH content was 25 wt%. Simultaneously, it showed sensitive heat response capacity. The improvement of filler/matrix interface and 3D networks were of great importance in abating the total thermal resistance . Moreover, the method provide a novel route to design high-performance thermal conductive TIMs and apply for the thermal management of electronics.

CAS / MDL: 4420-74-0 1310-73-2
研究领域: 材料科学 · 电子封装材料
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RSC Advances · 2015 ·Vol. 5 ·期 39 ·30631-30639 · IF 3.84

Anthraquinone chromophore covalently bonded blocked waterborne polyurethanes: synthesis and application

Haiyan Mao,Fan Yang,Chaoxia Wang,Youjiang Wang,Donggang Yao,Yunjie Yin

Dye-bonded blocked waterborne polyurethanes were developed to synchronously realize coloring and finishing of textiles and improve colorfastness using an anthraquinone chromophore and a methyl ethyl ketoxime blocking agent. The number-average molecular weight of the dye-bonded blocked polyurethane is 2303 g mol−1 and the polydispersity is 1.06, indicating a narrow molecular weight distribution. The maximum absorption wavelengths do not shift after the monomolecular chromophores are bonded to the polyurethane. The self-colored polyurethanes provide better centrifugal stability and water solubility than the dye-mixed blocked polyurethanes. The dye-bonded blocked polyurethane offers good thermal stability below 100 °C and undertakes de-blocking at about 150 °C. The covalent bonding of the anthraquinone moiety with the polyurethane chain and temporary blocking of the terminal isocyanate groups are conducive to enhancing the tinting strength and colorfastness of the treated cotton fabrics. The self-colored blocked polyurethanes with good elasticity and toughness can improve the recovery angle of the treated cotton up to 120°, which can also endow the fabric with wrinkle resistance.

研究领域: 材料科学 · 纺织化学 · 染料化学
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MOLECULES · 2016 ·Vol. 21 ·期 7 ·895 · IF 2.465

Site-Specific, Covalent Immobilization of Dehalogenase ST2570 Catalyzed by Formylglycine-Generating Enzymes and Its Application in Batch and Semi-Continuous Flow Reactors

Hui Jian,Yingwu Wang,Yan Bai,Rong Li,Renjun Gao

Formylglycine-generating enzymes can selectively recognize and oxidize cysteine residues within the sulfatase sub motif at the terminus of proteins to form aldehyde-bearing formylglycine (FGly) residues, and are normally used in protein labeling. In this study, an aldehyde tag was introduced to proteins using formylglycine-generating enzymes encoded by a reconstructed set of the pET28a plasmid system for enzyme immobilization. The haloacid dehalogenase ST2570 fromSulfolobus tokodaiiwas used as a model enzyme. The C-terminal aldehyde-tagged ST2570 (ST2570CQ) exhibited significant enzymological properties, such as new free aldehyde groups, a high level of protein expression and improved enzyme activity. SBA-15 has widely been used as an immobilization support for its large surface and excellent thermal and chemical stability. It was functionalized with amino groups by aminopropyltriethoxysilane. The C-terminal aldehyde-tagged ST2570 was immobilized to SBA-15 by covalent binding. The site-specific immobilization of ST2570 avoided the chemical denaturation that occurs in general covalent immobilization and resulted in better fastening compared to physical adsorption. The site-specific immobilized ST2570 showed 3-fold higher thermal stability, 1.2-fold higher catalytic ability and improved operational stability than free ST2570. The site-specific immobilized ST2570 retained 60% of its original activity after seven cycles of batch operation, and it was superior to the ST2570 immobilized to SBA-15 by physical adsorption, which loses 40% of its original activity when used for the second time. It is remarkable that the site-specific immobilized ST2570 still retained 100% of its original activity after 10 cycles of reuse in the semi-continuous flow reactor. Overall, these results provide support for the industrial-scale production and application of site-specific, covalently immobilized ST2570.

研究领域: 生物化学 · 酶工程 · 材料科学
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MACROMOLECULAR CHEMISTRY AND PHYSICS · 2016 ·Vol. 218 ·期 4 ·1600449 · IF 2.495

Efficient and Robust Reactions for Polyethylene Covalently Grafted Carbon Nanotubes

Yongjie Zhang,Qian Li,Wenbo Wang,Anru Guo,Jie Li,Huayi Li

Surface modification of carbon nanotubes (CNTs) with long polymer chains has attracted great attention since it promises high performance nanomaterials. However, due to the chemical inertness of both polyethylene (PE) and CNT, it still remains a challenge to covalently conjugate CNT with PE in a facile manner. In this report, trimethoxysilane terminated PE (TMS-PE) and trimethoxysilane modified multiwall carbon nanotube (TMS-MWNT) is prepared through radical mediated thiol-ene addition reaction between (3-mercaptopropyl)trimethoxysilane and vinyl terminated PE or pristine carbon nanotube, respectively. Subsequently, organotin-catalyzed hydrolytic co-condensation of TMS-PE and TMS-MWNT lead to PE covalently grafted mutliwall CNT (PE-Si-MWNT) with high graft ratio (17.5 wt%). Such reactions are robust and efficient and the reaction conditions are mild. In addition, the authors provide the very first evidence that end-grafted PE chains in PE-Si-MWNT, which are clearly observed in TEM images, can render high compatibility and good interfacial interactions between CNT and low density PE (LDPE) matrix and thus promote homogeneous dispersion of CNT into LDPE matrix as shown by scanning electron microscopy (SEM) characterization of brittle fracture surfaces of LDPE/PE-Si-MWNT nanocomposites.

CAS / MDL: 94-36-0 78-04-6
研究领域: 材料科学 · 化学工程
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2023 · IF 4.2

Optimization of Flexible Nacre-Like Cellulose Nanofiber Films by a Covalent Overlapping Method: Excellent Thermal Conductivity and Superior Flame Resistance

Jiachen Guo,Zhiyuan Peng,Hu Wang,Liu Yang,Ling Zhang,Chunzhong Li

Facing the explosive growth of heat flux in microelectronic equipment, advanced thermal management materials should not only ensure the safe and stable operation of equipment, but also have the ability to withstand fire risks. Carbon materials such as graphene are subject to many restrictions in use due to their inherent high conductivity. Hexagonal boron nitride (h-BN) is often used to blend with polymers to prepare flexible thermal management materials due to its excellent electrical insulation and thermal conductivity. However, its further application is limited by its insufficient flame resistance and limited improvement of thermal conductivity at low filling levels. In this paper, urea-assisted ball milling is used to achieve the amination of boron nitride nanosheets (BNNS) and black phosphorus (BP), which creates the covalent bond between the filler and the cellulose. With the overlapping between small-size BP and large-size BNNS, the thermal conductivity, flame resistance, and mechanical properties of the film are significantly enhanced. Accordingly, the cellulose nanofiber (CNF)-based film has a high thermal conductivity of 42.29 W m–1 K–1 at 50 wt % loading (40 wt % BNNS-NH2 and 10 wt % BP-NH2), which is 777% higher than that of pure CNF. In addition, the peak heat release rate and total heat release of CBP10 decrease by 80.3 and 64.7%, respectively, compared with pure CNF, and the residue is more complete and denser, indicating that the film can effectively reduce and delay the fire hazard.

研究领域: 材料科学 · 热管理技术
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Nano Research · 2020 ·Vol. 13 ·期 10 ·2665-2672 · IF 8.183

An efficient visible-light photocatalyst for CO2 reduction fabricated by cobalt porphyrin and graphitic carbon nitride via covalent bonding

Tian Shufang,Chen Sudi,Ren Xitong,Hu Yaoqing,Hu Haiyan,Sun Jiajie,Bai Feng

Nanoparticle photosensitizers possess technical advantages for photocatalytic reactions due to enhanced light harvesting and efficient charge transport. Here we report synthesis of semiconductor nanoparticles through covalent coupling and assembly of metalloporphyrin with condensed carbon nitride. The resultant nanoparticles consist of light harvesting component from the condensed carbon nitride and photocatalytic sites from the metalloporphyrins. This synergetic particle system effectively initiates efficient charge separation and transport and exhibits excellent photocatalytic activity for CO 2 reduction. The CO production rate can reach up to 57 µmol/(gh) with a selectivity of 79% over competing H 2 evolution. Controlled experiments demonstrate that the combination of light harvesting with photocatalytic activity via covalent assembly is crucial for the high photocatalytic activity. Due to effective charge separation and transfer, the resultant nanoparticle photocatalysts show exceptional photo stability against photo-corrosion under light irradiation, enabling for long-term utilization. This research opens a new way for the development of stable, effective nanoparticle photocatalysts using naturally abundant porphyrin pigments.

研究领域: 材料科学 · 环境科学 · 化学
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CELLULOSE · 2021 ·Vol. 28 ·期 8 ·4793-4805 · IF 5.044

Immobilization of laccases onto cellulose nanocrystals derived from waste newspaper: relationship between immobilized laccase activity and dialdehyde content

Xing Xinyue,Han Ying,Jiang Qiwen,Sun Yang,Wang Xing,Qu Guiyang,Sun Guangwei,Li Yao

The purpose of this work is to evaluate the possibility of using cellulose nanocrystals (CNC) derived from waste newspaper as a carrier for immobilizing laccases. Firstly, the cellulose nanocrystals extracted from waste newspaper were oxidized with sodium periodate, and the hydroxyl groups on the second and third carbons (C2 and C3) of the CNC molecules were converted to dialdehyde groups. Then, the laccase was successfully immobilized on the dialdehyde-modified cellulose nanocrystals (DMC) through covalent bonding. The DMC was characterized using zeta potential, Fourier-transform infrared spectroscopy, X-ray diffraction, scanning electron microscopy, and transmission electron microscopy, and the relationship between the activity of the immobilized laccase and the dialdehyde group content of the DMC was thoroughly investigated. It was found that the yield of the laccase immobilization is 64.94%, and the highest activity of the immobilized laccase (1.108 U/mg) is obtained at an aldehyde content of the DMC equal to 50.64%, a mass ratio of the carrier to the laccase equal to 45:3, a pH of 4.5, and a reaction time of 2 h. Compared to the free laccase, the immobilized laccase exhibits excellent stability in a wider range of pH values and temperatures. Furthermore, the immobilized laccase showed excellent reusability as evidenced by its retained relative activity of 67% after 6 cycles. Graphic abstract

CAS / MDL: 7790-28-5 28752-68-3
研究领域: 生物技术 · 酶工程 · 材料科学
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Journal of Materials Chemistry C · 2018 ·Vol. 6 ·期 8 ·2139-2147 · IF 5.976

A well-organized graphene nanostructure for versatile strain-sensing application constructed by a covalently bonded graphene/rubber interface

Quanquan Guo,Yongyue Luo,Jize Liu,Xinxing Zhang,Canhui Lu

Graphene/rubber nanocomposites have attracted increasing attention for their fantastic applications in varied wearable electronics. However, the mechanical and functional properties of graphene/rubber nanocomposites are often limited by their weak interfacial interactions, such as ionic and hydrogen bonding. Here, we propose a covalently bonded graphene/rubber nanocomposite with a well-organized graphene nanostructure for versatile strain-sensing applications. Briefly, biological phytic acid was chosen as a covalent-bonding bridge to co-crosslink graphene oxide nanosheets and epoxidized natural rubber chains via the ring-opening reaction of epoxy groups. Benefiting from the covalently bonded interface, the obtained nanocomposite exhibited dramatically enhanced mechanical properties. Compared with the sulfur-cured sample, the tensile strength and elongation at break increased by 67.43% and 116.55%, respectively. Moreover, the covalent linkage facilitates the formation of a well-organized graphene network, which remarkably enhances the sensitivity and stability of the as-prepared strain sensors. The resultant sensors can monitor both large-scale and tiny human motion and exhibit great potential in the application of sign language recognition. This covalently bonded graphene/rubber interface opens the door to tailored design and low-cost fabrication of well-organized graphene nanostructures for multifunctional applications in electronic sensors, electromagnetic shielding materials, actuators for artificial muscles, etc.

研究领域: 材料科学 · 电子工程 · 纳米技术
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