Biomaterials Advances
·
2025
·
IF 6
Chen Wang,Yin Li,Xiaoxue Shen,Shiwei Xiao,Huiying Du,Qianye Zhao,Ying Wang,Qiangtao Zhang,Shuxin Wen
Background Patients with locally advanced head and neck squamous cell carcinoma (HNSCC) exhibit poor survival due to tumor microenvironment (TME) barriers and systemic toxicity of chemo-immunotherapy associated with chemo-immunotherapy. Methods An injectable thermoresponsive hydrogel was engineered by crosslinking D-α-tocopheryl polyethylene glycol succinate (TPGS) with Na₂CO₃ (15 % w/v TPGS: 9 % w/v Na₂CO₃). This platform co-encapsulated doxorubicin-loaded nanoparticles (DOX NP) synthesized via PEI-cis-aconitic acid conjugation and CpG-loaded adjuvant nanoparticles (CpG NP) prepared through genipin-mediated PEI crosslinking. The hydrogel exhibited rapid temperature-triggered gelation, shear-thinning injectability, and a macroporous architecture that enabled dual drug retention and immune cell infiltration. Results In vitro , the hydrogel provided the sustained release of DOX NP with pH-responsive acceleration in acidic TME. In vivo , localized delivery of Gel-DOX NP-CpG NP significantly suppressed tumor growth ( p < 0.05) and enhanced cytotoxic CD8 + T-cell infiltration in TME (3.1-fold) and spleens (2.4-fold). RNA sequencing revealed 88 immune-related differentially expressed genes, including downregulated immunosuppressors and enriched cytokine pathways. Conclusion This TPGS/Na₂CO₃ hydrogel platform coordinates chemotherapy-induced immunogenic cell death (DOX NP) with CpG-driven innate immunity, overcoming TME barriers to enhance localized and systemic anti-tumor responses in HNSCC.
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Ming-feng Sun,Ting Wang,Li-guang Wu,Yu-xing Wang
This study attempted to enhance the permeation and antifouling performance of polyvinylidene fluoride (PVDF) ultrafiltration membranes. Reverse microemulsion containing cobalt and iron (Co–Fe) bimetallic hydroxide nanoparticles was blended with the PVDF membranes to construct a novel PVDF hybrid membrane. The permeation performance, antifouling property, and long-term operational stability of the hybrid membranes were evaluated via ultrafiltration process of water flux and bovine serum albumin (BSA) rejection. Structural characterization showed that the protection endowed by reverse microemulsion made the hydroxide nanoparticles to distribute uniformly in the PVDF polymeric matrix. The introduction of well-distributed bimetallic hydroxide nanoparticles substantially improved the pore structures and hydrophilicity of the PVDF hybrid membranes, thereby enhancing their permeation performance and antifouling property. The optimal water flux of the PVDF hybrid membranes (MD-10) reached 328 L·m −2 ·h −1 and was 5.4-fold higher than that of neat PVDF. Moreover, the MD-10 membrane had a high a high BSA rejection rate (91.04%). After four cycles of successive fouling-cleaning processes, the water flux of the MD-10 membrane still exceeded 160 L·m −2 ·h −1 and was fourfold higher than that of neat PVDF. However, excessive amounts of the microemulsion could not be uniformly mixed with the PVDF membranes, thereby decreasing the permeation and antifouling performance of the PVDF hybrid membranes.
研究领域:
膜科学
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纳米技术
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材料科学
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环境工程
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DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2023
·
IF 6
Zihao Dong,Yajuan Qu,Yuyang Jiao,Ke Xue,Wenguang Zhu,Hai Liu,Jianguang Qi,Yinglong Wang
A series of poly(1-vinyl-3-methylimidazole dimethyl phosphate- co -N-isopropylacrylamide) oligomers was synthesized by reversible addition-fragmentation chain transfer polymerization. The co-oligomers exhibited a pH-tunable lower critical solution temperature (LCST) phase transition in aqueous solutions. By changing the pH of the aqueous solution (HCI), the hydrogen bonding between the internal molecules of the co-oligomers and water molecules was weakened, which effectively reduced the cloud-point temperature. Poly(1-vinyl-3-methylimidazole dimethyl phosphate- co - N -isopropylacrylamide) oligomers exhibit an upper critical solution temperature (UCST) type of phase transition in an ester solution, which is associated with the formation and breaking of hydrogen bonds within the co-oligomers molecules. FT-IR analysis revealed the effect of temperature on hydrogen bonding between the functional groups. Energy decomposition, Electrostatic Potential (ESP), Atoms-in-Molecules (AIM), and Interaction region indicator (IRI) analyses demonstrated the presence of hydrogen bond donors N–H and imidazole ring C–H, and hydrogen bond acceptors C = O and P = O in the co-oligomers. The sites of hydrogen bonding between the co-oligomers and the solvent molecules as well as intermolecular forces were found to be the main factors contributing to the LCST/UCST-type phase transition.
研究领域:
高分子化学
·
物理化学
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
·
IF 7.2
Xiaowei Guo,Yang Yuan,Shanshan Li,Jingwen Wang,Zhengyu Bai,Lin Yang
Owing to the unique geometric and electronic structure, design and synthesis of electrocatalysts with well defined heterointerfaces are essential for clean energy technologies, for instance water-splitting and Zn-air batteries. Herein, a bifunctional electrocatalyst assembled by Co/MnO nanoparticles and nitrogen doping double-sphere carbon (denoted as Co/MnO@N-DSC), was fabricated via a solvothermal and pyrolysis strategy. The Co/MnO@N-DSC catalysts exhibit an enhanced bifunctional oxygen electrocatalytic performance for Oxygen reduction reaction (ORR) (E 1/2 , 0.84 V vs . RHE) and oxygen evolution reaction (OER) (E onset , 1.54 V vs . RHE). As an air cathode catalyst, the Co/MnO@N-DSC-based Zn-air battery can afford prime performance, over the commercial noble-metal-based Zn-air battery. Theoretical calculation results indicate that the synergism of Co (111)/MnO (200) heterointerfaces can enhance charge transfer and provide extra electrons for the reaction processes. This work provides a promising manoeuvre to uplift bifunctional catalytic activity by increasing the synergy from heterointerfaces of transition-metal/metal oxide in oxygen electrocatalysis .
研究领域:
能源材料
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电催化
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纳米材料
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可再生能源技术
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电池技术
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DOI
高影响因子
DALTON TRANSACTIONS
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2025
·Vol. 54
·期 19
·7753-7764
·
IF 3.3
Feiyang Tian,Ruixue Cheng,Yujing Shang,Le Pan,Xiuyun Cui,Xuekai Jiang,Kai Chen,Huajun Zhao,Kuiyuan Wang
Cucurbit[n]urils, owing to their unique structural features, exhibit versatility in performing tasks such as adsorption, detection, and catalysis. However, the scope of their catalytic applications remains limited, primarily because most cucurbituril-based catalytic reactions take place in either aqueous or organic phases. In this study, we have successfully synthesized porous honeycomb composites of cucurbit[6]uril with cobalt and nickel (denoted as Co@Q[6] and Ni@Q[6], respectively) and applied them in a photothermal synergistic heterogeneous gas–solid reaction for the reduction of nitrogen to ammonia under mild conditions. This represents a groundbreaking achievement, as it is the first instance where a cucurbit[n]uril-based material has demonstrated catalytic functionality in its solid-state form, thereby introducing a novel concept for the design and application of cucurbit[n]uril-based photocatalysts. To characterize the structure of these composites, we employed a range of techniques including X-ray absorption fine structure (XAFS) analysis, transmission electron microscopy (TEM), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and hydrogen temperature-programmed reduction (H2-TPR). Our findings revealed that Ni@Q[6] exhibits higher photothermal catalytic ammonia synthesis activity compared to Co@Q[6]. This enhanced activity is attributed to the strong metal–support interaction (MSI) between Ni and Q[6], which facilitates electron transfer and nitrogen activation. Furthermore, the thermal source promotes the transition of electrons from the valence band to the conduction band, thereby enhancing the cleavage of the NN bond. Notably, the band gaps of Co@Q[6] and Ni@Q[6] are significantly reduced. In particular, Ni@Q[6] demonstrates the highest efficiency in electron–hole pair separation, as evidenced by photoluminescence (PL) and electrochemical impedance spectroscopy (EIS) measurements. Overall, Co/Ni@Q[6] provides an effective pathway for nitrogen reduction under mild conditions and advances the application of cucurbituril-based materials in photothermal catalysis. This work also contributes to the development of environmentally sustainable ammonia synthesis technology.
研究领域:
材料科学
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无机化学
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催化
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纳米技术
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环境科学
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光化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2021
·
IF 5.316
Haiyang Zhang,Junchuan Wang,Ying Sun,Xueqin Zhang,Hong Yang,Baoping Lin
The exploration of an inexpensive, low-energy consumption and environmentally friendly preparation process to synthesize high capacitance performance MOF-based electrode materials is an important prerequisite for their commercialization. We propose a non-calcined strategy to synthesize nanowire microsphere shaped Co-BTC (CBNWM). Making MOF into one-dimensional nanowire structure can effectively increase its active sites and the ion transfer rate. After the MOF nanowires are entangle and reunite into microspheres, their mechanical property and chemical stability are improved. Therefore, compared with Co-BTC crystal (CBC), the electrochemical properties of CBNWM have been significantly improved. The specific capacity of CBNWM reaches 1020 F g −1 at 5 mV s −1 or 657 F g −1 at 0.5 A g −1 with the capacity remains 81.4% after 3000 cycles. Subsequently, a flexible asymmetric device of CBNWM//AC was fabricated, whose maximum energy density can achieve 34.4 W h kg −1 with the related power density of 375.3 W kg −1 .
研究领域:
材料科学
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电化学
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能源存储
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DOI
高影响因子
JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY
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2012
·Vol. 50
·期 23
·4871-4878
·
IF 3.919
Lijun Fan,Hou Chen,Zhihai Hao,Zhi Tan
A novel high oil-absorbing crosslinked gel was synthesized by copolymerization of butyl methacrylate (BMA) with a small amount of pentaerythritol triacrylate (PETA) crosslinker using single electron transfer-living radical polymerization (SET–LRP) initiated with carbon tetrachloride (CCl 4 ) and catalyzed by Cu(0)/hexamethylenetetramine (HMTA) in N, N-dimethylformamide (DMF). The polymerization followed first-order kinetics as indicated by linear increase of monomer concentration with reaction time. Effects of reaction temperature, crosslinker, initiator, and catalyst on the oil-absorbing properties of the crosslinked gel were investigated in detail. The oil absorptions of the crosslinked gel to chloroform, toluene could reach 51.9, 34.5 g/g, respectively. © 2012 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem, 2012
研究领域:
高分子化学
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功能材料
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环境修复
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石油泄漏处理
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聚合物科学
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DOI
高影响因子
Journal of Materials Chemistry B
·
2022
·Vol. 10
·期 19
·3723-3733
·
IF 7.571
Qing Hao,Jinghong Wang,Jie Shen,Rong Gu,Yu Rao,Jian Feng,Huanhuan Wang,John L. Brash,Hong Chen
In analogy with adsorbed protein films, we have fabricated a family of 2D nanofilms composed of poly(N-vinyl caprolactam-co-vinylimidazole) (PNVCL) nanogels. NVCL was copolymerized with 1-vinylimidazole (VIM), and then cross-linked with α,ω-dibromoalkanes with 2 to 8 carbons via quaternization to form the nanogels. The swelling ratio of the gels was precisely controlled by regulating the inter-chain spacing of the polymers at the level of the carbon atom chain length of the cross-linker. The short-chain alkanes used are relatively rigid and their dimensions provide an accurate estimate of the chain spacing in the nanogels. It was shown that small differences in the carbon atom number of the cross-linking agent led to significant differences in the mechanical properties of the nanogels, in particular in the softness, deformability, and contact area (in film form), all of which increased with increasing carbon number. Films of the softer gels not only showed good adhesion to a number of substrates, but were also mechanically robust. In addition, the films showed excellent light transmission and nontoxicity to L929 cells. Nanogels of intermediate softness were shown to inhibit the adhesion of bacteria and human umbilical vein smooth muscle cells (HUVSMCs), and to be resistant to the adsorption of the plasma protein fibrinogen, indicating strong anti-biofouling properties. Gels that were either too stiff or too soft showed somewhat weaker anti-fouling activity in terms both of HUVSMCs adhesion and protein adsorption.
研究领域:
材料科学
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生物医学工程
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纳米技术
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生物材料
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DOI
PubMed
高影响因子
EES Catalysis
·
2025
·
IF 8.1
Jie Yang,Lifang Chen,Xuya Zhu,Wenwen Shi,Mengxue Huang,Chang Liu,Ruimin Ding,Lin Gan,Xi Yin
H2O2 -related electrochemical reactions, including two-electron oxygen reduction reaction (2e-ORR), H2O2 oxidation reaction (HPOR), and H2O2 reduction reaction (HPRR), have received significant attention for the electrosynthesis H2O2 and energy storage. Understanding the complex structure-activity relationships among 2e-ORR/ HPOR/HPRR and their connections is crucial for further developing highly efficient catalysts and working systems. Herein, we unveil these intricacies by employing model Co-N-C catalysts with well-defined active site configuration (Co-N4-pyrrolic and Co-N4- pyridinic ) in a combined experimental and computational approach. We report the higher 2e-ORR/HPOR but lower HPRR activity of CoN4-pyrrolic site than the CoN4-pyridinic site based on their reaction free energy landscapes remodeled considering the chemisorption steps of O2 and H2O2 . The results reveal that the binding free energy of *OOH (ΔG*OOH ) can only be utilized as a reliable descriptor for 2e-ORR/HPOR activity, but not indicative of HPRR activity, regardless of the scaling relationship of the common reaction intermediates ( *OOH or *OH). The HPRR activity of CoN 4 sites strongly depends on the H2O2 adsorption strength and configuration. These findings provide valuable insights into the design of catalysts for H2O2 -related electrochemical energy conversion and storage systems.
研究领域:
电化学
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催化
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材料科学
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能量转换与存储
·
计算化学
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产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2016
·
IF 4.803
Na Li,ChunYi Zhi,Haiyan Zhang
The preparation of high specific-capacity pseudocapacitive transition-metal-oxide/hydroxide (TMH) materials into transparent micro-structure electrodes is a great challenge and has become the bottleneck restricting the performance of transparent flexible supercapacitors . Beyond that, extending the operating voltage window is an urgent need for improving energy density . Here, Co(OH) 2 nanosheets and amorphous FeOOH nanowires were prepared into transparent films through a simple and scalable bio-inspired method at the air-solution interface. Both nanostructures are enwrapped in graphene shells (Co@Gr-TFandFe@Gr-TF) for use as transparent asymmetric pseudocapacitive electrodes. The unique encapsulation structures (1) provide pseudocapacitive electrode materials, especially an amorphous FeOOH structure cathode, (2) build up rapid three-dimensional electron and ion transport pathways together with the underlying ITO layer, (3) alleviate the exfoliation and dissolution of the active materials into electrolyte, and (4) extend the potential window of the FeOOH cathode from −0.8 ∼ 0 V to −1.2 ∼ 0 V with minimal cycling stability degradation. The asymmetric transparent and flexible supercapacitor based on Co@Gr-TF//Fe@Gr-TF operated at 1.8 V exhibits good transparency (50.5% at 550 nm), high specific capacitance (25.5 mF cm −2 , one order higher than the maximum value reported for FFT-GP), and high energy density (1.04 mWh cm −3 , comparable to that of nontransparent devices) as well as a long cycle life (10 000 cycles) with high-capacity retention (83.5%).
研究领域:
材料科学
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纳米科技
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电化学
·
能源存储
·
柔性电子学
·
功能薄膜
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DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·Vol. 141
·期 36
·e55915
·
IF 2.7
Tianyuan Liu,Weihao Wang,Tian Yin,Zhikui Jiang,Zhichao Zhen,Guochun Yan,Junhui Ji
The application and promotion of biodegradable plastics are hindered by the imbalance between their mechanical and degradation performance imbalance, as well as high costs. Herein, a series of poly(ethylene adipate-co-terephthalate) (PEAT) copolyesters with excellent mechanical and degradation properties are synthesized by one-step melt polycondensation. The influence of the proportion of aliphatic groups in the molecular chain on the structure and properties, especially the degradation performance, of the copolyesters was studied. The molecular chain flexibility and degradability of PEAT increases with increasing of adipic acid content and decreasing of ET fragment length ( L ET ). The comprehensive mechanical properties of PEAT60 can be comparable to traditional packaging material poly(butylene adipateco-terephthalate) (PBAT). The degradation performance of PEAT can be adjusted the molecular chain structure. PEAT with L ET < 3 exhibit degradation performance, and PEAT with L ET < 2.2 exhibit significant degradation acceleration. The excellent mechanical and degradable properties of PEAT copolyester make it expected to be used in degradable packaging and other fields to help solve plastic pollution, while its lower cost will aid in the promotion of degradable materials.
研究领域:
材料科学
·
高分子化学
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环境科学
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DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·
IF 3.9
Jialu Wei,Jingyu Wang,Wei Zhang,Yuezhen Mao,Chunwen Sun
Graphical A ZAB with Co–N–C–PBMCRO cathodic catalyst achieves a remarkable cycling stability for 788 h. The perovskite Pr 0.5 Ba 0.5 Mn 0.8 Co 0.1 Ru 0.1 O 2.5+δ (PBMCRO) composite was constructed by in situ exsolved CoRu nanoparticles and Co–N–C with more exposing active sites. A conductive pathway for oxygen ions and electrons was built, thereby enhancing the electrochemical bifunctional properties. This rational design strategy shows great potential for facilitating synthesis of perovskite based catalysts for energy conversion and storage applications. Bifunctional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are essential components of rechargeable zinc-air batteries. In this study, we synthesized a Pr 0.5 Ba 0.5 Mn 0.8 Co 0.1 Ru 0.1 O 2.5+δ (PBMCRO) perovskite composite with in situ exsolved CoRu nanoparticles and Co–N–C, functioning as an efficient bifunctional electrocatalyst for zinc-air batteries. The in situ exsolution of CoRu nanoparticles from the perovskite oxide was facilitated by the reducing action of 2-methylimidazole (2-MIM). Concurrently, Co–N–C was used to decorate PBMCRO, forming a novel bifunctional composite electrode of Co–N–C–PBMCRO. The incorporation of CoRu nanoparticles introduces a significant number of electrochemically active oxygen vacancies in the perovskite matrix, enhancing ORR and OER performance. Additionally, the Co–N–C synergistically improves electrochemical activity while preserving the structural stability of the perovskite oxide. The prepared Co–N–C–PBMCRO catalyst demonstrates significantly enhanced bifunctional performance compared to the undecorated pristine perovskite Pr 0.5 Ba 0.5 MnO 3−δ (PBMO). The zinc-air battery with Co–N–C–PBMCRO catalyst achieve a peak power density of approximately 90 mW/cm 2 and exhibit remarkable cycling stability for 788 h. This study presents a novel and effective strategy to enhance the catalytic performance of perovskite-based air electrodes for rechargeable metal-air batteries.
研究领域:
材料科学
·
电化学
·
能源存储与转换
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DOI
高影响因子