ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Jinyi Zhang,Jie Wang,Jing Liao,Yao Lin,Chengbin Zheng,Juewen Liu
Catalytic cascades have drawn much attention by avoiding the isolation of intermediates and due to high atom economy. Yet, developing an efficient, one-pot biocatalytic cascade remains challenging. Combined with the selectivity of biological enzymes and tunable activity of nanozymes, we herein demonstrate an effective bio-nanozyme cascade formed by glucose oxidase (GOx) and in situ-generated nanoceria. The prepared H2O2–nanoceria complex shows strong oxidative activity for common chromogenic substrates under physiological conditions, which are the optimal reaction conditions for most biological enzymes. Interestingly, GOx not only provides H2O2 for the second step reaction but also simultaneously leads to 7.4-fold enhancement of activity. We characterized the process of in situ generation of nanoceria at pH 7.0 and how proteins boost the activity by enhancing product desorption. In addition, the proposed one-pot bio-nanozyme cascade shows high stability and analytical performance for serum glucose with a detection limit of 5 μM.
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高影响因子
ACS Applied Polymer Materials
·
2021
·
IF 4.089
Ye Yuan,He Zhang,Jinqing Qu
The smart fluorescent hydrogels exhibiting tunable fluorescence have been used as biosensors, probes, light-emitting devices, and information storage and confidentiality. However, they usually show single stimuli responsiveness and possess weak mechanical properties, which limit their applications. Herein, we report a pyridine-dicarbohydrazone-based polyacrylate hydrogel (the As-prepared hydrogel and Eu-hydrogel) showing strong mechanical property, tunable fluorescence ability, and thermal and pH stimuli responsiveness. The As-prepared hydrogel is prepared by light-induced micellar copolymerization, and Eu-hydrogel is obtained after the formation of Eu3+-(pyridine-dicarbohydrazone) coordination. The As-prepared hydrogel could be made in large size (side length of 15 cm), exhibiting a tensile strength of 1.55 MPa and a fracture tensile strain of 800%. The fluorescence intensity of Eu-hydrogel is tunable by [Eu3+] (approaching 655% of the minimum state at [Eu3+] = 0.1 mol). It is demonstrated that Eu-hydrogels display force-induced fluorochromic response during stretching. The transmittance temperature of the As-prepared hydrogel ranges from 36 to 42 °C. Reversible Eu3+-(pyridine-dicarbohydrazone) coordination enables Eu-hydrogels to have excellent fatigue resistance. The pH stimuli responsiveness of the As-prepared hydrogel and Eu-hydrogel is triggered by switchable covalent hydrozone bonds. In terms of the shape-memory ability, the As-prepared hydrogel could be reconstructed by Eu3+ and Eu-hydrogel could be deformed by H+. This mechanically strong (pyridine-dicarbohydrazone)-based polyacrylate hydrogel with multistimuli responsive behaviors is promising to be used in information transmission, smart windows, load-bearing devices, energy-absorbing materials, and soft wearable devices.
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高影响因子
FOOD CHEMISTRY
·
2015
·
IF 3.391
Zhenhua Zhang,Yueyu Zou,Taigang Wu,Caihuan Huang,Kehan Pei,Guangwen Zhang,Xiaohua Lin,Weibin Bai,Shiyi Ou
Chlorogenic acid (CGA) is a phenolic acid that ubiquitously exists in fruits. This work aims to investigate whether and how CGA influences HMF formation during heating fructose alone, or with an amino acid. The results showed that that CGA increased 5-hydroxymethylfurfural (HMF) formation. At pH 5.5 and 7.0, the addition of 5.0 μmol/ml CGA increased HMF formation by 49.4% and 25.2%, respectively when heating fructose alone, and by 9.0% and 16.7%, respectively when heating fructose with aspartic acid. CGA significantly increased HMF formation by promoting 3-deoxosone formation, and its conversion to HMF by inhibiting HMF elimination, especially in the Maillard reaction system. A comparison of the catalytic capacity of CGA with its six analogous compounds showed that both its di-hydroxyphenyl and carboxyl groups function in increasing HMF formation.
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高影响因子
CELLULOSE
·
2020
·Vol. 27
·期 11
·6367-6381
·
IF 4.21
Cui Li,Hu Jin-jing,Wang Wei,Yan Chao,Guo Yi,Tu Chao
Abstract A kind of smart calcium alginate fiber having pH indicating properties was proposed to monitor wound healing. The smart calcium alginate fiber was prepared by dyeing the hydroxypropyl trimethyl ammonium chloride chitosan (HACC) modified calcium alginate fiber with alizarin dye and anthocyanin dye, respectively. It was worth noting that modification of calcium alginate fibers with HACC enhanced the dyeing and antibacterial properties, simultaneously. When the concentration of HACC was 10 g/L, the modified calcium alginate fiber had the best dyeing performance. At the same time, the dyeing process had no significant influence on the mechanical properties of the fibers with the strength loss only around 0.2 cN/dtex. The smart calcium alginate fibers exhibited a rapid and significant color change and reversible color response at pH 2–11. Moreover, the color change could be easily observed by naked eye. Therefore, the prepared calcium alginate fibers could be a good candidate for intelligent wound dressings for visual monitoring of wound healing. Graphic abstract
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
·
IF 4.539
Peizhang Zhou,Yuanyang Yan,Jiang Cheng,Cailong Zhou
In this work, stainless steel mesh coated with stearic acid and tetradecanedioic acid modulated ZIF-67 (SA+TDA/mZIF-67@SSM) was prepared via facile electrodeposition . The composite modulators supply defect engineering on the MOFs , endowing the as-prepared meshes with pH-switchable wettability . The ratio of modulators significantly affected the crystal morphology and wetting property of SA+TDA/mZIF-67@SSM, resulting from the competitive coordination between the modulation and crystal growth process. The SA+TDA/mZIF-67@SSM exhibited highly hydrophobic, while it became amphiphilic after soaked in alkaline solution because some exposed carboxylic acid groups on the mesh were deprotonated. The SA+TDA/mZIF-67@SSM achieved efficient and adjustable organic liquids separation, with the separation efficiency both up to 98% before and after the wettability transition. In addition, the SA+TDA/mZIF-67@SSM could realize the separation of oil/water/oil mixtures, with the separation efficiency larger than 98%. This work introduces a new technique of modulated MOFs coated mesh with pH-responsivity for separating organic liquids based on defect engineering.
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高影响因子
Small
·
2022
·Vol. 18
·期 47
·2204557
·
IF 15.153
Jian Zhang,Jiandong Li,Huajie Huang,Wei Chen,Yan Cui,Yonghua Li,Weiwei Mao,Xinbao Zhu,Xing'ao Li
Defect engineering of transition metal dichalcogenides (TMDCs) is important for improving electrocatalytic hydrogen evolution reaction (HER) performance. Herein, a facile and scalable atomic-level di-defect strategy over thermodynamically stable VSe 2 nanoflakes, yielding attractive improvements in the electrocatalytic HER performance over a wide electrolyte pH range is reported. The di-defect configuration with controllable spatial relation between single-atom (SA) V defects and single Se vacancy defects effectively triggers the electrocatalytic HER activity of the inert VSe 2 basal plane. When employed as a cathode, this di-defects decorated VSe 2 electrocatalyst requires overpotentials of 67.2, 72.3, and 122.3 mV to reach a HER current density of 10 mA cm −2 under acidic, alkaline, and neutral conditions, respectively, which are superior to most previously reported non-noble metal HER electrocatalysts. Theoretical calculations reveal that the reactive microenvironment consists of two adjacent SA Mo atoms with two surrounding symmetric Se vacancies, yielding optimal water dissociation and hydrogen desorption kinetics. This study provides a scalable strategy for improving the electrocatalytic activity of other TMDCs with inert atoms in the basal plane.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Shen Zhang,Yuan Rui,Xing Zhang,Rongjia Sa,Feng Zhou,Ruihu Wang,Xiaoju Li
The exploration of the inexpensive and efficient substitutes for platinum-based electrocatalysts is of great challenges for hydrogen evolution reaction (HER). Here, we presented a facile method to achieve highly active, cost-effective and stable HER catalysts, which are composed of ultrafine Co-Ru alloy nanoparticles embedded in heteroatom-free graphitic carbon (Co 1-x Ru x /GC). The optimum catalyst with ruthenium content of 0.93 wt% exhibits remarkable HER activity and the excellent durability, low overpotentials of 14, 39 and 44 mV at −10 mA cm −2 are achieved in alkaline, neutral and acidic media, respectively, which can compete with those in commercial 20 wt% Pt/C and majority of the reported platinum-free catalysts. It has been validated that the confinement effect of SBA-15 induces the formation of ultrafine alloy nanoparticles for generating more active sites. The theoretical simulations reveal that Co-Ru alloy regulates hydrogen adsorption energy to the optimum level, thus resulting in high HER activity. This work provides new methods for the fabrication of ultrafine alloy nanoparticles for the electrocatalysis and other application.
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高影响因子
BIOCONJUGATE CHEMISTRY
·
2018
·
IF 4.485
Chao-Ran Xu,Liang Qiu,Cai-Yuan Pan,Chun-Yan Hong,Zong-Yao Hao
In this study, an efficient method is proposed for the synthesis of polymer prodrug with acid-liable linkage via thiol–acrylate Michael addition reaction of the camptothecin with tethering acrylate group and polymer scaffold containing multiple thiol groups. The polymer scaffold P(HEO2MA)-b-P(HEMA-DHLA) is prepared by reversible addition–fragmentation chain transfer (RAFT) polymerization of the methacrylate of lipoic acid (HEMA-LA) using poly(2-(2-hydroethoxy) ethyl methacrylate) (PHEO2MA) as macro-RAFT agent followed by reduction of the disulfides in lipoic acid (LA) groups to give polymer scaffold with dihydrolipoic acid (DHLA) pendent groups. Acrylate-tethering camptothecin (ACPT) is connected to P(HEO2MA)-b-P(HEMA-DHLA) via Michael addition reaction between thiol and acrylate with a high coupling efficiency (95%). Amphiphilic polymer prodrug P(HEO2MA)-b-P(HEMA-DHLA-CPT) spontaneously self-assembles into nanoparticles in an aqueous solution and exhibits a CPT loading content as high as 40.1%. The prodrug nanoparticles with the acid-liable β-thiopropionate linkages can release CPT under acidic conditions, and the prodrug nanoparticles show similar cytotoxicity to HeLa cells as free CPT. Overall, the prodrug nanoparticles with high drug loading contents and acid-liable linkages are promising for pH-responsive anticancer therapy.
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高影响因子
Polymer Chemistry
·
2017
·Vol. 8
·期 43
·6675-6687
·
IF 5.375
Da Huang,Yaqiang Wang,Fei Yang,Hong Shen,Zuquan Weng,Decheng Wu
Recently, nanoparticles self-assembled from amphiphilic supramolecular linear-dendritic block copolymers (LDBCs) have attracted great interest, since the combination of linear and dendritic polymers can incorporate the unique properties of the different segments but avoid some inherent drawbacks of dendrimers, not to mention that the components can be flexibly adjusted to enrich their functionality. In this study, LDBCs formed by host–guest recognition of polyacetal dendrimers with a β-cyclodextrin core and adamantane-terminated zwitterionic poly(sulfobetaine) could self-assemble into micelles and vesicles by varying the hydrophilic/hydrophobic ratio. Owing to the acid-labile characteristic of the dendritic segments, the micelles and vesicles were degradable and could release their payloads in a pH-responsive manner. The incorporation of zwitterionic linear segments gave the micelles and vesicles a charge-reversal ability and excellent resistivity to protein absorption, leading to higher affinity to cell membranes than conventional PEG-coated nanoparticles. In addition, the potential of these nanoparticles as anticancer drug carriers was preliminarily evaluated by using doxorubicin as a model drug and the results indicated that the DOX-loaded micelles and vesicles exhibited remarkable anticancer activity. This study cast a new light on the application of dendrimers and these micelles and vesicles constructed from LDBCs may be promising candidates as anticancer drug delivery platforms for cancer therapy.
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高影响因子
MICROCHIMICA ACTA
·
2016
·Vol. 183
·期 5
·1779-1786
·
IF 4.831
Li Huihui,Zhu Shuqiang,Cheng Ting,Wang Shuxia,Zhu Bin,Liu Xiaoyan,Zhang Haixia
Boronate affinity materials have been widely used for selective capture of cis-diols such as nucleosides. Adsorbents with features of low binding pH and high adsorption capacity are highly desired. However, most reported materials only possess one of the two features. We have synthesized a 1,3,5-triazine-containing binary boronic acid by reacting cyanuric chloride with 3-aminophenylboronic acid, and the product was then grafted onto attapulgite (a fibrous aluminum-magnesium silicate). The resulting functionalized attapulgite exhibit low binding pH (5.0) and display high adsorption capacity (19.5 ± 1.1 mg⋅g −1 for adenosine). The material exhibits high selectivity for cis-diols even in the presence of a 1000-fold excess of interferences. It was applied to the selective extraction of nucleosides from human urine. Typical features of the method include (a) limits of detection in the range from 4 to 17 ng⋅mL −1 , (b) limits of quantification between 13 and 57 ng⋅mL −1 , (c) relative standard deviations of ≤9.1 %, and (d) recoveries of nucleosides from spiked human urine between 85.0 and 112.9 %. In our perception, the material and method offer a promising strategy for selective capture of cis-diols in the areas of proteomics, metabolomics and glycomics.
We have prepared 1,3,5-triazine-containing binary boronic acid-functionalized attapulgite. The material exhibited low binding pH (5.0) and high adsorption capacity (19.5 ± 1.1 mg⋅g‾ 1 for adenosine).
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
·
IF 4.539
Mengnan Qu,Yajie Pang,Jiehui Li,Rong Wang,Dan He,Zhanxia Luo,Fan Shi,Lei Peng,Jinmei He
Smart materials with controllable wettability have become one of the current research hotspots. Among them, the pH-responsive superwetting material is considered an ideal material because of its rapid response process and simple response mechanism. However, the pH-responsive materials reported previously could only perform wettability conversion in a single direction. In order to meet the demands of practical applications, it is indispensable to prepare the pH-bidirectional responsive superwetting material which can flexibly transform wettability in both directions. Based on this, a fluorine free and eco-friendly superwetting fabric with pH-bidirectional responsiveness was prepared by free radical polymerization and the combination of micro-nano hierarchical structure. A series of test results verified that the prepared fabric possessed excellent mechanical durability and chemical stability, satisfactory flux and separation efficiency. In addition, this work also successfully employed the prepared pH-bidirectional responsive superwetting fabric to realize the separation of three-phase oil-water-oil mixture. Surprisingly, the prepared fabric was also proved to be effective for the separation of multiple organic components, which was rarely reported in previous researches. Therefore, such pH-bidirectional responsive superwetting fabric will have broad application prospects in the field of oil-water separation and multi-organic components separation under the actual complex environment.
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高影响因子
MICROCHIMICA ACTA
·
2023
·Vol. 190
·期 4
·1-9
·
IF 5.7
Du Ning,Zhang Guohui,Hou Pengkun,Zhang Hao,Guan Ruifang
An organic fluorescent probe, citric acid-1,3-Propanediamine-Rhodamine B ( CPR ) was synthesized to determine pH of ordinary Portland cement requiring only a small sample size (less than 500 μL cement leachate). The SEM, XRD, and FTIR investigations demonstrate that citric acid-1,3-Propanediamine are polymer dots with a fusiform structure. Ratio pH probe is constructed by rhodamine B with polymer dots, which exhibits a linear response in high alkaline range. A 6-fold increase in fluorescence intensity (455 nm) is achieved at pH from 12.00 to 13.25. Combined with measurements of the isothermal calorimeter, mineral composition, and microscopic morphology, variation of pH is used to evaluate the changes of components during hydration. Furthermore, CPR can be applied to measure pH of high-dose pulverized fuel ash blending systems, the non-pure cement with slightly lower alkalinity. Graphical
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高影响因子
危险品化学品经营许可证（带存储）