Advanced Healthcare Materials
·
2022
·Vol. 11
·期 20
·2200938
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IF 11.092
Lei Zhou,Haifeng Liang,Yuxiang Ge,Wang Ding,Qing Chen,Taiwei Zhang,Lan Xiao,Yulin Li,Jian Dong,Xiaowen He,Fengfeng Xue,Libo Jiang
Although immune checkpoint inhibitors (ICIs) have been widely applied to treat non-small cell lung cancer (NSCLC), a significant proportion of patients, especially those with spinal metastasis (NSCLC-SM), are insensitive to anti-programmed death 1 (PD-1)/programmed death ligand 1 (PD-L1) ICIs. A drug delivery nano-controller of PD-L1 that targets NSCLC-SM can solve this problem, however, none have been developed to date. In this study, it is shown that integrin β 3 ( β 3-int) is strongly upregulated in NSCLC-SM. Its inhibitor RGDyK promotes PD-L1 ubiquitination, indicating the potential application of RGDyK as a new PD-L1 inhibitor in nano-controller and a targeting peptide for NSCLC-SM treatment. According to the synergistic effect of photodynamic therapy and ICIs on T-cell activation through the release of tumor antigens, RGDyK-modified and zinc protoporphyrin (ZnPP)-loaded mesoporous silicon nanoparticles (ZnPP@MSN-RGDyK) are fabricated. The ZnPP@MSN-RGDyK nanoparticles precisely target β 3-int to inhibit PD-L1, exhibiting high photodynamic therapy efficiency, and excellent immunotherapeutic effects in an NSCLC-SM mouse model. Collectively, the findings indicate that ZnPP@MSN-RGDyK is a promising immunotherapeutic agent for treating NSCLC-SM.
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POLYMER BULLETIN
·
2022
·Vol. 80
·期 5
·5587-5605
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IF 2.843
Zhou Jiacheng,Wu Linlin,Ge Yongxin,Gao Yifeng,Ma Xiaofeng,Fang Ying
Deep eutectic solvent (DES)-based gels, with their biocompatibility, non-volatility, low cost, and electrochemical stability, have attracted widespread interest as novel solid-state ionic conductor for flexible devices. However, fabrication of tough and stretchable DES gels is challenging due to the insufficient understanding of the interactions between polymers and DES. The development of tough DES gels based on hydrogen bonding is attractive but also challenging due to the possible competitive hydrogen bonds between the hydrogen bond-rich choline chloride-based polar DES and polymers. Herein, tough copolymer-supported DES gels with dual-cross-linked dissipative network were fabricated through copolymerization of methacrylic acid and N , N -dimethylacrylamide monomers with good and poor compatibility with DES to promote the formation of stable hydrogen bonds between polymers in the DES. The resulting DES gels were stiff, tough, stretchable, and self-recoverable, with tensile strength, breaking strain, Young's modulus, toughness, and recovery ratio being 2.08 MPa, 792%, 1.76 MPa, 12.88 MJ m −3 , and 76%, respectively. The mechanical properties of DES gels could be widely tuned by varying the monomer ratio and solvent structure changes. The carbon-based supercapacitor based on the DES gel shows stable voltage window to 2 V and exhibits the specific capacitance of 93.25 F g −1 at 2 A g −1 . Graphical abstract An ultratough and stretchable copolymer-supported DES gel ionic conductor with high tensile strength of 2.08 Mpa, high toughness of 12.88 MJ m −3 , stretchability of 792%, and excellent recovery properties are facile fabricated for flexible electronics through copolymerization of two monomer pairs of methacrylic acid and N , N -dimethylacrylamide that can form stable hydrogen bonds in the DES environment with a small amount of chemical cross-linker to form a dual-crosslinked dissipative network.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Qinzhi Wang,Yijian Zhao,Tong Bu,Xin Wang,Zhihao Xu,Hui Zhangsun,Li Wang
Surface-enhanced Raman scattering (SERS) with its outstanding performance in ultra-sensitivity has been applied in contaminants monitoring. Herein, a facile strategy of integrating oriented layered MOF nanoarray with controlled electrodeposition of gold nanoparticles via semi-sacrificial template method was proposed to fabricate a versatile self-supporting MOF chip ( [email protected] ) for efficient SERS detection of food contaminants. The S-MOF was ingeniously formed by directly using flexible Ni sheet as both metal source and scaffold, which in favour of greatly improving intrinsic electrical conductivity during electrodeposition process as well as endowing prepared chip with uniform distribution of gold nanoparticles and high stability. Furthermore, amounts of SERS “hot spots” in the oriented layered [email protected] can yield strong electromagnetic field for Raman amplification with superior reproducibility. By virtue of good flexibility and pre-concentration effect of [email protected] , tartrazine (TA), chloramphenicol (CP), imidacloprid (IDP) and crystal violet (CV) in food samples were sensitively detected using three collected approaches (drip coating, soaking and wiping) with low limits of detection (1.0 × 10 −9 M for TA, 8.0 × 10 −11 M for CP, 6.4 × 10 −11 M for IDP and 5.0 × 10 −12 M for CV), wide linear detection ranges (1.0 × 10 −8 – 1.0 × 10 −3 M for TA, 1.0 × 10 −10 – 1.0 × 10 −6 M for CP, 1.0 × 10 −10 – 1.0 × 10 −7 M for IDP and 1.0 × 10 −11 – 1.0 × 10 −7 M for CV) and satisfactory recoveries (96.2 – 125.1%). This method provides a novel strategy to develop an advanced SERS platform for efficient food contaminants monitoring.
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ADVANCED MATERIALS
·
2021
·Vol. 34
·期 5
·2101976
·
IF 30.849
Zhizhan Dai,Zhiwei Bao,Song Ding,Chuanchuan Liu,Haoyang Sun,He Wang,Xiang Zhou,Yuchen Wang,Yuewei Yin,Xiaoguang Li
The developments of next-generation electric power systems and electronics demand for high temperature (≈150 °C), high energy density, high efficiency, scalable, and low-cost polymer-based dielectric capacitors are still scarce. Here, the nanocomposites based on polyimide-poly(amic acid) copolymers with a very low amount of boron nitride nanosheets are designed and synthesized. Under the actual working condition in hybrid electric vehicles of 200 MV m −1 and 150 °C, a high energy density of 1.38 J cm −3 with an efficiency higher than 96% is achieved. This is about 2.5 times higher than the room temperature energy density (≈0.39 J cm −3 under 200 MV m −1 ) of the commercially used biaxially oriented polypropylene, the benchmark of dielectric polymer. Especially, the energy density and efficiency at 150 °C show no sign of degradation after 20 000 cycles of charge-discharge test and 35 days’ high-temperature endurance test. This research provides an effective and low-cost strategy to develop high-temperature polymer-based capacitors.
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POLYMER
·
2021
·
IF 4.43
Hualong Zhang,Wen Xu,Zhigang Wu,Chao Liu,Chunyan Hong
In this study, an efficient strategy was presented to prepare monocyclic polymers via combination of reversible addition-fragmentation chain transfer (RAFT) polymerization and light-induced cycloaddition reaction, and tadpole-shaped copolymer was further synthesized via ring-opening polymerization (ROP) using cyclic polystyrene (C-PS) as macroinitiator. A series of well-defined α, ω-hetero bifunctional homopolymers with furan-protected maleimide and o-methylbenzaldehyde terminals, including polystyrene (PS), poly ( N, N -dimethylacrylamide) (PDMA) and poly ( N -isopropylacrylamide) (PNIPAAm) were prepared via RAFT polymerization. After deprotection, highly active maleimide group at the end of linear polymer coupled intramolecularly with photoenol structure (photoisomer of o-methylbenzaldehyde) via Diels-Alder cycloaddition reaction under 365 nm UV irradiation in dilute solution, leading to the formation of cyclic polymer. The monocyclic polymers were characterized with 1 H NMR, UV–Vis spectroscopy, gel permeation chromatography (GPC) and MALDI-TOF MS. Furthermore, the C-PS containing hydroxyl group was used as macroinitiator to prepare tadpole-shaped copolymer CPS- b -PCL via the ROP of ε-caprolactone.
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Journal of the Taiwan Institute of Chemical Engineers
·
2021
·
IF 5.876
Liu Yang,Yu-Long Liu,Xian-Xian Ji,Cheng-Guo Liu,Ying Fu,Fei Ye
Background A novel luminescent sensor with dual-emitting platforms, Tb@UiO-66 , was used for highly detecting Sm 3+ and teflubenzuron. Methods Tb@UiO-66 was synthesized on basis of the exchange of guest molecules, where Tb 3+ ions were encapsulated into the cages of UiO-66 . Significant finds The results of multiband fluorescence originated from the linker-to-cluster charge transfer and the characteristic emission of Tb III . Tb@UiO-66 displayed luminescence enhancements or quenches according to small molecules. Especially for Sm 3+ and teflubenzuron, the characteristic peaks of Tb@UiO-66 at 490, 545, 585, and 621 nm increased with the increasing of the concentration of the analytes, where Tb@UiO-66 exhibited the effect of luminescence enhancement. The detection limits for detecting Sm 3+ and teflubenzuron were 0.09 μM and 0.21 μM, and the changes of luminescence intensities could be observed by naked eyes under the UV light at 365 nm. Tb@UiO-66 could also be used to detect teflubenzuron in real water samples. Tb@UiO-66 could be reused for at least 5 cycles for the detection of Sm 3+ and teflubenzuron with the framework of Tb@UiO-66 uncollapsed. These results implied that the integration of Ln III luminescent materials and Zr-MOFs by doping method provided a new strategy for fabricating novel luminescent sensors for detecting polluting small molecules.
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LANGMUIR
·
2021
·
IF 3.882
Ya Liu,Li Wang,Hongsheng Lu,Zhiyu Huang
Hydrogels and organogels, as two crucial representatives of soft materials, have attracted immense interest. However, they develop independently along two parallel lines, and these gels with single networks have their inherent drawbacks. For example, hydrogels tend to freeze, and organogels are usually brittle. Herein, organogels were incorporated into a hydrogel matrix for the synthesis of organohydrogels GOHs through polymerization in Pickering emulsion. The rigid organogel domains contribute to enhancing the strength of organohydrogels. Besides this, the organogels derived from 12-HAS self-assembly behavior exhibit a gel–sol transition when the temperature reaches 70 °C, thus leading to a thermo-softening behavior in the GOHs. Due to the phase transition of organogel domains and the elastic hydrogel network, the resultant organohydrogels demonstrate high-strain shape-memory performance (over 1000%) which could help achieve full recovery in seconds. Consequently, GOHs are endowed with the potential of practical application in soft robots, wearable devices, and biological materials.
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REACTIVE & FUNCTIONAL POLYMERS
·
2021
·
IF 3.975
Yong Gao,Amin Deng,Xionghui Wu,Changsheng Sun,Chenze Qi
Injectable multi-responsive hydrogels are very important and exhibit many potential applications in biologically relevant fields. In this work, the preparation of injectable multi-responsive hydrogels at near-physiological conditions and their applications as durg carriers were demonstrated. Diol-capped poly( N, N -dimethylacrylamide)- b -poly( N -isopropylacrylamide) ((OH) 2 -PDMA- b -PNIPAM) diblock copolymers containing a disulfide linkage on the backbone and N, N -dimethylacrylamide- stat -(2-acrylamidophenylboronic acid) (DMA- stat -2APBA) copolymers were separatedly synthesized. Hydrogels were then prepared by a solution-based mixing of DMA- stat -2APBA with (OH) 2 -PDMA- b -PNIPAM diblock copolymers in PBS (pH 7.4) solution at a given temperature, i.e. 37 °C. Above the lower critical solution temperature (LCST) of diblock copolymers at around 32 °C, (OH) 2 -PDMA- b -PNIPAM copolymers self-assembled into core-shell structured macromolecular micelles with numerous diol groups on hydrophilic cornoas. Subsequent complexiation of diols with lateral PBA groups of DMA- stat -2APBA copolymers led to the formation of hydrogels. Due to the integration of a library of responsive units including boronate ester and disulfide DCBs together with thermal responsive PNIPAM blocks within the same system, the as-prepared hydrogels indicated multiple stimuli-responsiveness to pH, temperature, glucose and redox reaction as well as the mechanical field. Such multi-responsive hydrogels could be applied as potential drug carriers. The encapsulation and the stimuli-responsive release of a model drug of Rh B were demonstrated.
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ACS Applied Energy Materials
·
2021
·
IF 6.024
Zhen Wang,Shuqi Hu,Asad Ali,Hongling Chen,Pei Kang Shen
The development of highly active and stable catalysts is a critical challenge which affects the practical application of the direct methanol fuel cells. Alloying Pt with other metals is an effective strategy to form the bimetallic or trimetallic catalysts, which not only decreases the consumption of Pt but also optimizes the electronic structure of Pt, in turn enhancing the catalytic activity. Herein, we use a facile one-pot solvothermal reduction method to synthesize Ag nanocubes (NCs) enclosed by PtRh nanoparticles as a trimetallic Ag@PtRhAg NC core–shell catalyst toward methanol oxidation reaction (MOR). Notably, the core–shell structure is formed because of the presence of N,N-dimethylacetamide, which promotes the preferential reduction of Ag by reducing the reduction potential of Ag atoms. Meanwhile, the bromide ions originating from cetyltrimethylammonium bromide controlled the growth of the cubic morphology. Benefiting from the pleated exterior providing more active sites and the synergistic effect between Pt, Rh, and Ag, the mass and specific activities of Ag@PtRhAg NCs are 4.22 and 3.78 times higher than those of commercial Pt/C, respectively. More impressively, because of the better CO tolerance, Ag@PtRhAg NCs display strengthened durability by maintaining 84.9% mass activity after 1000 MOR cycles compared to the initial value. The present work provides a one-step strategy to synthesize a core–shell nanostructure catalyst for enhancing the MOR activity.
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EUROPEAN POLYMER JOURNAL
·
2020
·
IF 3.862
Lei Wang,Xiaofeng Ma,Linlin Wu,Ye Sha,Bo Yu,Xiaoyu Lan,Yanlong Luo,Yijun Shi,Yan Wang,Zhenyang Luo
Fabrication strategies for photo-responsive ion gels have attracted attention owing to their precise spatial and temporal control with predetermined responses to light stimuli. In this work, a reversible light-driven method was introduced to devise photo-responsive ion gels by harnessing coumarin-based building blocks under 365 nm irradiation. A series of random copolymers composed of N, N -dimethylacrylamide (DMA) and 7-(2′-methacryloyloxyethoxy)–4-methylcoumarin (MAOEMC), namely P(DMA- r -MAOEMC), were synthesized through reversible addition-fragmentation chain transfer (RAFT) polymerization with sufficient molecular weight (≈100 kDa). The coumarin moieties in those polymers exhibited a reversible photo-induced dimerization and photocleavage behavior in 1-ethyl-3-methylimidazolium bis (trifluoromethylsufonyl) imide ([C 2 mim][NTf 2 ]). Those polymers - ionic liquid system at high polymer concentration (20 wt%) under suitable wavelength UV light irradiation led to sol–gel transition, which could be functionalized as photo-healable material and photo-controlled adhesion agents. Notably, the photo-controlled adhesiveness was reversible and can be mediated from 1.2 MPa to 0.2 MPa. This work opens new avenues to develop multifunctional ion gels using dynamic covalent bonds.
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DRUG DEVELOPMENT AND INDUSTRIAL PHARMACY
·
2020
·
IF 2.365
Zhongjuan Wang,Yueqin Liang,Yanqiu Liu,Hongying Xia,Jianqi Liu,Xingfang Jin,Zhongkun Li
Multi-drug resistance (MDR) is one of the major challenges in the successful chemotherapy of non-small cell lung cancer (NSCLC). Although RNA interference (RNAi) has been widely used to silence resistance-related genes, the effect remains unsatisfactory. In this study, we attempted to overcome MDR of NSCLC by simultaneously interfering with two RNAs that have different functions. A new pH-triggered polyglutamate brush polymer dimethylmaleic anhydride-poly(ethyleneglycol) monomethyl ether-b-polyglutamate-g-spermine (DMA-mPEG-b-PG-g-spermine, DPPGS) was designed and synthesized. The DPPGS/small interfering RNA (siRNA) complex nanoparticles (DPPGSN) were prepared. The results demonstrated that DPPGSN could be transformed from a negatively charged form into a positively charged form in the slightly acidic tumor extracellular environment. The siRNA targeting MDR1 mRNA (siMDR1) and siRNA targeting survivin mRNA (siSurvivin) could be efficiently co-delivered by DPPGS to simultaneously interfere with two genes (p < 0.01). Furthermore, DPPGS co-delivery of siMDR1 and siSurvivin lowered the IC50 value of cisplatin (DDP) in A549/DDP (p < 0.01) cells and increased the apoptosis rate of the cells (p < 0.01). Therefore, co-delivery of siMDR1 and siSurvivin using DPPGS would be a promising approach for overcoming MDR of NSCLC.
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BIOMACROMOLECULES
·
2020
·
IF 6.092
Shuyue Zhao,Wenjun Huang,Changrong Wang,Yaping Wang,YuFeng Zhang,Zhanpeng Ye,Jianhua Zhang,Liandong Deng,Anjie Dong
The amphiphilic cationic polymers that mimic antimicrobial peptides have received increasing attention due to their excellent antibacterial activity. However, the relationship between the structure of cationic polymers and its antibacterial effect remains unclear. In our current work, a series of PEG blocked amphiphilic cationic polymers composed of hydrophobic alkyl-modified and quaternary ammonium salt (QAS) moieties have been prepared. The structure–antibacterial activity relationship of these cationic polymers was investigated against E. coli and S. aureus, including PEGylation, random structure, molecular weights, and the content and lengths of the hydrophobic alkyl side chains. The results indicated that PEGylated random amphiphilic cationic copolymer (mPB35/T57) showed stronger antibacterial activity and better biocompatibility than the random copolymer without PEG (PB33/T56). Furthermore, mPB35/T57 with appropriate mole fraction of alkyl side chains (falkyl = 0.38), degree of polymerization (DP = 92), and four-carbon hydrophobic alkyl moieties was found to have the optimal structure that revealed the best antibacterial activities against both E. coli (MIC = 8 μg/mL, selectivity > 250) and S. aureus (MIC = 4 μg/mL, selectivity > 500). More importantly, mPB35/T57 could effectively eradicate E. coli biofilms by killing the bacteria embedded in the biofilms. Therefore, the structure of mPB35/T57 provided valuable information for improving the antibacterial activity of cationic polymers.
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