ACS Applied Materials & Interfaces
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2014
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IF 5.9
Xiangsheng Liu,Nan Huang,Huan Li,Haibo Wang,Qiao Jin,Jian Ji
Gold nanorods (AuNRs), because of their strong absorption of near-infrared (NIR) light, are very suitable for in vivo photothermal therapy of cancer. However, appropriate surface modification must be performed on AuNRs before their in vivo application because of the high toxicity of their original stabilizer cetyltrimethylammonium bromide. Multidentate ligands have attracted a lot of attention for modification of inorganic nanoparticles (NPs) because of their high ligand affinity and multifunctionality, while the therapeutic effect of multidentate ligands modified NPs in vivo remains unexplored. Here, we modified AuNRs with a polythiol PEG-based copolymer. The multidentate PEG coated AuNRs (AuNR-PTPEGm950) showed good stabilities in high saline condition and wide pH range. And they had much stronger resistance to ligand competition of dithiothreitol (DTT) than AuNRs coated by monothiol-anchored PEG. The AuNR-PTPEGm950 had very low cytotoxicity and showed high efficacy for the ablation of cancer cells in vitro. Moreover, the AuNR-PTPEGm950 showed good stability in serum, and they had a long circulation time in blood that led to a high accumulation in tumors after intravenous injection. In vivo photothermal therapy showed that tumors were completely cured without reoccurrence by one-time irradiation of NIR laser after a single injection of these multidentate PEG modified AuNRs.
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LANGMUIR
·
2013
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IF 4.187
Junyang Shen,Chongyi Chen,Wenxin Fu,Linqi Shi,Zhibo Li
Poly(ethylene glycol)-block-poly(γ-(2-methoxyethoxy)esteryl-l-glutamate) (PEG-b-poly-l-EG2Glu) was synthesized via ring-opening polymerization (ROP) of l-EG2Glu N-carboxyanhydride (NCA) using PEG-NH2 as macroinitiator. This diblock contained a thermo-responsive poly-l-EG2Glu block, which adopted primarily helical conformation in pristine aqueous solution. We found that PEG-b-poly-l-EG2Glu diblock can display two levels of self-assembly behaviors associated with hydrophobic interactions and conformation-specific reassembly, respectively. Upon temperature increase, the PEG-b-poly-l-EG2Glu diblock formed wormlike micelles, in which the poly-l-EG2Glu formed the micelle core and maintained helical conformation. However, extension of thermal annealing time drove the secondary structure transformation of the poly-l-EG2Glu block from helical conformation to β-sheet, which accounted for an assembly structure transition from wormlike micelles to nanoribbons. The critical factor was that poly-l-EG2Glu block can undergo thermo-induced hydrophobicity and conformation transformation, which offered an additional parameter to tune the nature of molecular interactions, i.e., intermolecular versus intramolecular hydrogen bonding interactions. The corresponding conformation and assembly structure changes were characterized using FTIR and electron microscopy, respectively.
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BIORESOURCE TECHNOLOGY
·
2014
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IF 5.039
Jifeng Pang,Mingyuan Zheng,Ruiyan Sun,Lei Song,Aiqin Wang,Xiaodong Wang,Tao Zhang
The effects of typical inorganic impurities on the catalytic conversion of cellulose to ethylene glycol (EG) were investigated, and the mechanism of catalyst deactivation by certain impurities were clarified. It was found that most impurities did not affect the EG yield, but some non-neutral impurities or Ca and Fe ions greatly decreased the EG yield. Conditional experiments and catalyst characterization showed that some impurities changed the pH of the reaction solution and affected the cellulose hydrolysis rate; Ca and Fe cations reacted with tungstate ions and suppressed the retro-aldol condensation. To obtain a high EG yield, the pH of the reaction solution and the concentration of tungstate ions should be respectively adjusted to 5.0–6.0 and higher than 187 ppm. For raw biomass conversion, negative effects were eliminated by suitable pretreatments, and high EG yields comparable to those from pure cellulose were obtained.
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CATALYSIS LETTERS
·
2014
·Vol. 144
·期 10
·1728-1734
·
IF 2.291
Wang Shengpei,Chen Jinzhu,Chen Limin
Abstract A multifunctional catalyst of ruthenium supported on NENU-3 [a hybrid of phosphotungstic acid (PTA) and HKUST-1] is developed. An ethylene glycol (EG) yield of 50.2 % can be directly obtained from cellulose with Ru/NENU-3 as catalyst under optimized conditions. As a multifunctional catalyst of Ru/NENU-3, the presence of both the active specie of PTA for cellulose hydrolysis and subsequent C–C bond cleavage of cellulose-derived sugars, and the active specie of Ru for glycolaldehyde hydrogenation is indispensible for the formation of EG from cellulose. Graphical Abstract
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CHINESE JOURNAL OF CATALYSIS
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2017
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IF 2.813
Cong Zhao,Shengxin Chen,Ruirui Zhang,Zihang Li,Ruixia Liu,Baozeng Ren,Suojiang Zhang
A series of acetate ionic liquids were synthesized using a typical two-step method. The ionic liquids were used as environmentally benign catalysts in the production of propylene glycol ethers from propylene oxide and alcohols under mild conditions. The basic strengths of the ionic liquids were evaluated by determination of their Hammett functions, obtained using ultraviolet-visible spectroscopy, and the relationship between their catalytic activities and basicities was established. The catalytic efficiencies of the ionic liquids were higher than that of the traditional basic catalyst NaOH. This can be attributed to the involvement of a novel reaction mechanism when these ionic liquids are used. A possible electrophilic-nucleophilic dual activation mechanism was proposed and confirmed using electrospray ionization quadrupole time-of-flight mass spectrometry . In addition, the effects of significant reaction parameters such as concentration of catalyst, molar ratio of alcohol to propylene oxide, reaction temperature, and steric hindrance of the alcohol were investigated in detail.
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Materials Science & Engineering C-Materials for Biological Applications
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2017
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IF 4.164
Jianbing Wu,Xusheng Xie,Zhaozhu Zheng,Gang Li,Xiaoqin Wang,Yansong Wang
The effects of changing solution pH in the range of 3.6–10.0 during a one-step silk microsphere preparation process, by mixing silk and polyethylene glycol (PEG), was assessed. The microspheres prepared at low pH (3.6) showed a more homogeneous size (1–3 μm) and less porous texture than those prepared at neutral pH. High pH (10.0) inhibited microsphere formation, yielding small and inhomogeneous microspheres. Compared to neutral pH, low pH also increased the content of silk crystalline β-sheet structure from approx. 30% to above 40%. As a result, the microspheres produced at low pH were more thermally stable as well as resistant to chemical (8 M urea) and enzymatic (protease XIV) degradation when compared to microspheres prepared at neutral pH. Doxorubicin hydrochloride (DOX) and curcumin (CUR) were successfully loaded in silk microspheres via control of solution pH. The loading efficiency of DOX was approx. 95% at pH 7.0 and approx. 60% for CUR at pH 3.6, attributed to charge-charge interactions and hydrophobic interactions between the silk and drug molecules, respectively. When PBS, pH 7.4, was used as a medium for release studies, the pH 3.6 microspheres released both drugs more slowly than the pH 7.0 microspheres, likely due to the high content of crystalline β-sheet structure that enhanced drug-silk interactions as well as restricted drug molecule diffusion.
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Biomedical Materials
·
2015
·Vol. 10
·期 6
·065022
·
IF 3.697
Weiping Wang,Xin Huang,Haiyan Yin,Wenling Fan,Tao Zhang,Lei Li,Chun Mao
In this study, polyethylene glycol acrylate (PEGA) was introduced onto the surface of polysulphone (PSF) membrane to prepare PSF–PEGA membranes through low-temperature plasma technology for haemocompatibility improvement of artificial lungs. The effects of plasma power, PEGA solution concentration and dipcoating temperature on surface modification were systematically investigated. Results of Fourier transform infrared spectroscopy, x-ray photoelectron spectroscopy and PEGA grafting degree confirmed that PEGA was successfully grafted onto the PSF membranes. Contact angle values showed that the hydrophilicity of the PSF–PEGA membrane surface increased by 21.5%. The results of the protein adsorption, platelet adhesion and coagulation tests further showed the excellent haemocompatibility of the modified membrane. Gas exchange tests also revealed that at a porcine blood flow rate of 5 l min−1, O2 and CO2 exchange rates through the PSF–PEGA membrane were 198.6 and 170.9 ml min−1, respectively; approximately this is the gas exchange capacity of commercial respiratory assistance devices.
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Heritage Science
·
2024
·Vol. 12
·期 1
·1-9
·
IF 2.6
Liu Jiaojiao,Dong Wenqiang,Yang Junchang,Chen Zhongwei,Cao Jing,Chen Ran
Owing to the instability of gelatine in hygrothermal environments, gelatine-based cultural heritage undergo various deterioration processes, such as cracking, peeling, warping, curling and fracture, posing significant threats to its long-term preservation. Building on previous research, this study investigates the stability of polyol glycidyl ether–gelatine composite films under high-humidity and high-temperature conditions using ethylene glycol diglycidyl ether (EGDE) as a model compound. The hygrothermal ageing properties of EGDE–gelatine composite films are evaluated in terms of macrosize, mesoscopic structure, surface properties and mechanical properties. Results indicate that EGDE enhances the dimensional stability and swelling ratios of the composite films, stabilizes the pore structure and distribution and maintains the hydrophilicity and molecular structural stability under hygrothermal ageing conditions. Furthermore, the incorporation of EGDE leads to superior stress–strain properties of the composite films in such challenging environments. This study provides valuable experimental data for the preparation and conservation applications of gelatine-based cultural heritage materials.
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Advanced Science
·
2024
·
IF 14.3
Likun Luan,Yingfang Zhang,Xiuling Ji,Boxia Guo,Shaoyu Song,Yuhong Huang,Suojiang Zhang
Multi-enzymatic cascade reaction provides a new avenue for C─C coupling directly from CO 2 under mild conditions. In this study, a new pathway with four enzymes including formate dehydrogenase (PaFDH), formaldehyde dehydrogenase (BmFADH), glycolaldehyde synthase (PpGALS), and alcohol dehydrogenase (GoADH) is developed for directly converting CO 2 gas molecules to ethylene glycol (EG) in vitro. A rhodium-based NADH regeneration electrode is constructed to continuously provide the proton and electron of this multi-enzymatic cascade reaction. The prepared electrode can reach the Faradaic Efficiency (FE) of 82.9% at −0.6 V (vs. Ag/AgCl) and the NADH productivity of 0.737 mM h −1 . Shortening the reaction path is crucial for multi-enzymatic cascade reactions. Here, a hydrogen-bonded organic framework (HOF) nano-reactor is successfully developed to immobilize four enzymes in one pot with a striking enzyme loading capacity (990 mg enzyme g −1 material). Through integrating and optimization of NADH electro-regeneration and enzymatic catalysis in one pot, 0.15 mM EG is achieved with an average conversion rate of 7.15 × 10 −7 mmol CO 2 min −1 mg −1 enzymes in 6 h. These results shed light on electro-driven multi-enzymatic cascade conversion of C─C coupling from CO 2 in the nano-reactor.
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ACS Central Science
·
2024
·
IF 12.7
Yaqi Li,Yixin Sun,Qing Wang,Shuo Wang,Cuiyun Liu,Yuetong Huang,Wenxin Zhong,Xiyan Wang,Wenjing Wang,Shiyi Zuo,Xianbao Shi,Xiaohui Pu,Jin Sun,Zhonggui He,Bingjun Sun
Prodrug-based nanoassemblies are promising platforms for cancer therapy. Prodrugs typically consist of three main components: drug modules, intelligent response modules, and modification modules. However, the available modification modules are usually hydrophobic aliphatic side chains, which affect the activation efficiency of the prodrugs. Herein, hydrophilic ethylene glycol fragments were inserted between the modification modules and the response modules, and the important effects of hydrophilic fragments on the assembly, drug release, and therapeutic index of the prodrugs were investigated. Notably, the introduction of hydrophilic fragments affected the intermolecular forces of the prodrugs and increased the interaction of hydrogen bonding. In addition, hydrophilic fragments significantly improved the redox drug release profiles, which affected the therapeutic index of the prodrug nanoassemblies. PTX-SS-OA NPs with hydrophilic fragments exhibited increased redox sensitivity, enhanced cytotoxicity, and superior antitumor efficacy. In comparison, PTX-SS-OAL NPs without hydrophilic fragments showed limited redox sensitivity and cytotoxicity but displayed better safety. Overall, the hydrophilic fragment is a critical determinant in modulating the therapeutic index of the prodrug nanoassemblies, which contributes to the development of advanced prodrug nanodelivery systems.
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PROCESS BIOCHEMISTRY
·
2024
·
IF 3.7
Wenjing Liu,Kexin Qiang,Peipei Ye,Xin Li,Xiaoman Zhao,Jianhan Hong,Yafeng Duan
Polyethylene terephthalate (PET) fabric was enzymatically modified with polyethylene glycol (PEG). Lipase from Aspergillus oryzae was used as a catalyst. The wetting behavior of the modified PET fabric was characterized by the water contact angle , water adsorption dynamics and moisture regain. The initial water contact angle of the modified fabric decreased from 129.3° to 74.9°. The water absorption dynamics results indicated that the equilibrium water absorption amount of the modified fabric was approximately 10 times greater than that of the untreated sample. The initial absorption rate ( V init ) of the modified fabric was almost 30 times higher than that of the untreated fabric. The moisture regain reached 3.52 % after modification. Scanning electron microscopy revealed granular and sheet coatings on the surface of the modified fabric. Chemical linkage of PEG onto the PET fibers was confirmed by attenuated total reflection–Fourier transform infrared spectroscopy. The modification had no significant effect on the thermal properties of the PET fabrics according to the thermogravimetric curve and differential scanning calorimetry results. The mechanical properties of the modified fabric were slightly improved. Therefore, in situ enzymatic transesterification between PET and PEG could be a potential novel modification approach for adding value to PET fiber textiles .
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2024
·
IF 2.6
Li Xiaogang,Zhou Yanhui,Tu Huan,Wang Zongnan,Wu Rui,Lu Yaokang,Zong Yujie,Liu Qian,He Jie,Qian Li,Song Siyu,Zhang Yixian,Meng Chunfeng,Yuan Aihua
Aqueous zinc-ion batteries (AZIBs) are considered promising candidates for scalable and sustainable energy storage devices due to their low cost and high safety advantages. However, the practical application of AZIBs is subject to the limits of the reversibility of the Zn 2+ stripping/plating, such as the growth of Zn dendrites, corrosion of Zn anode, and hydrogen evolution reaction (HER). Herein, we propose a solution to the issues of AZIBs by creating a versatile electrolyte via the addition of polyethylene glycol (PEG). PEG additive changes the coordination environment of Zn 2+ and disturbs the solvation structure of H 2 O, which is beneficial to alleviate the side reactions triggered by water molecules in the Zn 2+ solvation structure. In addition, the Zn 2+ nucleation behavior is optimized by texturing the hexagonal deposition plane and inducing the compact-grained deposition manner to resist corrosion reactions and dendrite aggravation. The solvation structure of Zn 2+ is optimized to improve the reversibility of the Zn anode. As a result, improved reversibility of Zn plating/stripping on the Cu-working electrode is achieved by 20% PEG electrolyte with high Coulombic efficiency (CE) of 99.43% at 1 mA cm −2 , stably cycled for 750 cycles. Furthermore, the Zn||Zn symmetrical half-cell with 20% PEG electrolyte shows stable plating/stripping overpotentials for more than 1400 h. Finally, the Zn||V 2 O 5 full-cells exhibit excellent long cycling stability for over 180 cycles even at 1000 mA g −1 with a high reversible capacity of 168 mAh g −1 . This work provides valuable insights into designing electrolytes for aqueous zinc metal batteries.
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