Acta Biomaterialia
·
2024
·
IF 9.4
Lianying Zhang,Xiaotong Chen,Beixian Zhou,Wei Meng,Haifeng Zeng,Yongjian Chen,Guoqin Huang,Yingshan Zhang,Huimin Wang,Ming Chen,Jinxiang Chen
Immunotherapy has emerged as a highly promising strategy in the realm of cancer treatment, wherein immunogenic cell death (ICD) is considered a potential trigger for anti-tumor immunity by inducing adaptive immunity to dying cell antigens. This process is often accompanied by the exposure, active secretion, or passive release of a large number of damage-associated molecular patterns (DAMPs), which activate dendritic cells (DCs) and enhance their antigen-presenting capacity. Subsequently, it promotes the recruitment and activation of cytotoxic T lymphocytes, ultimately leading to tumor growth inhibition. In addition, polarizing the M2 phenotype of tumor-associated macrophages (TAMs) to the M1 phenotype is another way to activate anti-tumor immunity, which can further enhance the effect of anti-tumor immunotherapy. In this study, we engineered a composite nanoparticle of UiO-66-NH 2 @Gold nanoshells@GOx-P-Arg (denoted as UGsGP). The gold nano shells in UGsGP exhibit a broad Near-Infrared-II (NIR-II) absorption to give a high photothermal conversion efficiency and achieve photothermal therapy (PTT). The GOx in UGsGP involves the breakdown of glucose, which results in a decrease in ATP levels and an inhibition of HSP90 and HSP70 production, ultimately enhancing the heat sensitivity of the tumor for PTT. In addition, GOx-mediated starvation therapy by glucose exhaustion produces a substantial amount of hydrogen peroxide (H 2 O 2 ), which can then react with P-Arg to produce intratumoral NO Thus, the synergistic effect of PTT resensitization, the photothermally-enhanced GOx-mediated starvation, and NO-based gas therapy promote the induction of ICD and the polarization of TAMs. The combination therapy exhibits significant antitumor effects both in vitro and in vivo. Statement of significance (1) Gold nanoshells on the surface of UiO-66-NH 2 display a broad absorption spectrum ranging from 900 to 1700 nm, combined with a high photothermal conversion efficiency of 74.0 %, demonstrating their remarkable ability to harness and convert light energy into heat for effective tumor ablation. (2) Under laser irradiation, GOx within the UGsGPs effectively consumes glucose, increasing intratumoral H 2 O 2 levels, which then reacts with P-Arg to produce NO within the tumor. Concurrently, the reduction in ATP levels suppresses HSP90 and HSP70 production, thereby enhancing the tumor's sensitivity to photothermal therapy. (3) The synergistic combination of NO gas therapy, starvation therapy, and PTT promotes ICD induction and TAM polarization, thereby improving the therapeutic outcomes for primary and distant tumors.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Kunpeng Song,Xue Bi,Chuang Yu,Ye-Tang Pan,Henri Vahabi,Vera Realinho,Jiyu He,Rongjie Yang
Up to now, metal–organic frameworks (MOFs) with open nanostructures have shown outstanding capabilities in trapping smoke particles compared to the original MOFs. However, only a few MOF-based strategies have been reported to synthesize hierarchical porous cages thus far, which are mainly restricted to environmentally unfriendly wet-chemical liquid methods. Herein, as a proof-of-concept, a gas-steamed metal–organic framework approach was designed to fabricate a series of cheeselike open cages with hierarchical porosity. Briefly, zeolitic imidazolate framework-67 (ZIF-67) and phytic acid were employed as precursor and etchant, respectively. Abandoning the conventional wet-chemical method, the coordination bond of ZIF-67 was cleaved by acidic steam, forming an open framework with a high specific surface area and a hierarchical porous structure. The universality of this method was also confirmed by the selection of different etchants. Impressively, they also show outstanding fume-toxic adsorption capability and labyrinth effects based on abundant and complex porous channels. At only 5 wt % loading, Co3O4@open ZIF-67 cage-2 (Co3O4@OZC-2) imparted polyurea (PUA) composites with a 21.2% limiting oxygen index, and the peak of heat release rate, total heat release, and total smoke production were reduced by around 37.5, 25.5, and 40.4%, respectively, compared to neat PUA. This work will shed light on the advanced structural design of polymer composites with high fire safety, especially smoke suppression performance, so as to obtain more feasible applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Qingping Xin,Yucheng Pan,Chao Zhang,Lei Zhang,Chensheng Dong,Ligang Lin,Lizhi Zhao,Hui Ye,Yuzhong Zhang
The CH 4 /N 2 high-efficiency membrane separation technology is capable of effectively enriching CH 4 from natural gas, and holds great potential for application in the fields of biogas purification and natural gas pipeline leak detection. However, preparing high-performance separation membranes is challenging due to the similarity between CH 4 and N 2 molecules. To enhance the CH 4 /N 2 separation performance, block polyetheramide copolymer (Pebax)/EVA blended membranes were fabricated in this study. Additionally, a novel gas leakage detection tube was prepared. The EVA14 (14 wt% VA) membrane exhibits an optimal transport-facilitated channel among a series of pure EVA membranes, resulting in a CH 4 permeability of 21.41 Barrer and CH 4 /N 2 selectivity reaches 1.80 under mixed-gas feed conditions at 35 °C. The CH 4 permeability of Pebax/EVA (30 wt%) reaches 120.5 Barrer by physical blending, and the CH 4 permeability is increased by 191 % in comparison with pure EVA14 membrane. The Pebax/EVA (10 wt%) membrane exhibits the optimum CH 4 /N 2 selectivity, and compared with pure EVA membrane increased by 35.5 %. EVA and Pebax polymers are blended for the first time for CH 4 /N 2 separation, and the blending of block polyetheramide copolymer intensifies the membrane's separation performance comprehensively. The natural gas leak detection tube was fabricated with a membrane, offering a new and efficient CH 4 /N 2 separation strategy.
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ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Qianfeng Wang,Jiayi Li,Yunxiao Dong,Han Hu,Drow Lionel OYoung,Di Hu,Yufang Zhang,Dong-Qing Wei,Jinggang Wang,Jin Zhu
2,5-Thiophenedicarboxylic acid (TDCA) is a biobased building block for aromatic–aliphatic copolyesters. This study synthesized poly(propylene succinate-co-thiophenedicarboxylate) (PPSTh) and poly(propylene adipate-co-thiophenedicarboxylate) (PPATh) via two-step melt polycondensation. PPATh70 exhibits the highest melting temperature at 144.8 °C. Crystallization kinetics indicate that diol-TDCA segments primarily form crystalline phases in PPXThs, with long aliphatic units enhancing crystallization. PPXThs containing over 50 mol % TDCA have a higher tensile modulus than poly(butylene adipate-co-terephthalate) (PBAT) and possess excellent gas barrier properties, outperforming PBAT by over 200 times. Dynamic mechanical analysis links the superior gas barrier properties to reduced free volumes. PPAThs degrade faster than PPSThs, with hydrolytic differences explained by Fukui function analysis and DFT calculations. Molecular dynamics simulations clarified the degradation mechanism catalyzed by Candida antarctica lipase B, showing that residues at the entrance interact with PPXTh50 residues, hindering the carbonyl carbon from approaching the catalytic nucleophile, while the flexible PPXTh40 more easily achieves an ideal Bürgi–Dunitz angle for nucleophilic attack.
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CHINESE JOURNAL OF ANALYTICAL CHEMISTRY
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2015
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IF 0.754
Liang HAO,Da-Peng WU,Ya-Feng GUAN
The method of micro-pressurized liquid extraction (μ-PLE) coupled with gas chromatography-mass spectrometer (GC-MS) for analysis of 4 dicarboxylic acids (DCAs, including malonic acid, succinic acid, glutaric acid, and adipic acid) in fine atmospheric particles was developed. PM 2.5 filter sample was extracted by μ-PLE at a pressure of 8 MPa and temperature of 80 °C using methanol as extraction solution. After two static 5-min extractions and a rinsing step with 100 μL methanol, about 500 μL of extraction solution was obtained. The extraction solution was then blown to dry with high purity nitrogen and submitted to a silylation reaction at 60 °C for 30 min. After internal standard (IS) was added, the derivatization solution was directly injected for GC-MS analysis. For quantification of 4 normally DCAs in fine atmospheric particles, the calibration curve was obtained with a good linear relationship in the range of 0.2–20 ng μL −1 . The limits of quantification (LOQs, S/N = 10) were in the range of 0.15–0.47 ng m −3 . The relative recoveries were between 92% and 122% with the RSDs between 2.6% and 11.8% for spiked filter samples. The method developed here was used to determine malonic acid, succinic acid, glutaric acid, and adipic acid in real PM 2.5 samples collected from Xinghai Bay of Dalian city, and the results were determined to be 64.6, 50.0, 41.8 and 20.2 ng m −3 , respectively.
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GREEN CHEMISTRY
·
2016
·Vol. 18
·期 24
·6493-6500
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IF 8.506
Jian Chen,He Li,Mingmei Zhong,Qihua Yang
CO2 capture and utilization is one of the most attractive and challenging topics of the twenty-first century. The direct conversion of CO2 using flue gas as a feedstock is an energy saving process, but it has been rarely reported. Herein, we report an efficient CO2 cycloaddition reaction using diluted gas (20% CO2 and 80% N2, simulating flue gas) as a feedstock, catalyzed by a 2,2′-bipyridine zinc(II) based hierarchical meso/microporous polymer, Bp-Zn@MA. Bp-Zn@MA, constructed via a template-free polycondensation reaction without using any catalyst, can efficiently catalyze the cycloaddition of propylene oxide with a TOF of up to 1580 h−1 (100 °C) and 8041 h−1 (150 °C), using diluted gas and pure CO2, respectively. This is among the best performing solid catalysts ever reported for the CO2 cycloaddition reaction. The high catalytic activity of the polymer, especially when diluted CO2 was employed, can be mainly attributed to its hierarchical meso/microporous structure, which contains mesopores for facilitating the diffusion of reactants and micropores for CO2 enrichment. The construction of this hierarchical structured porous material provides an efficient approach for realizing CO2 conversion using flue gas as a feedstock.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2016
·
IF 8.328
Dong Jiang,Wenzhong Wang,Yali Zheng,Ling Zhang
Hydrogenation has been widely employed in solar-driven photocatalysis, to enhance the light absorption and photon-to-electron (PE) conversion of semiconductors. However, there still remain controversies in this field, such as the precise roles of bulk and surface oxygen vacancies (V O ). Furthermore, the influence of hydrogenation on surface reactions in photocatalysis at gas-solid interface has been rarely discussed. Herein, gray CeO 2 was prepared by treating pristine CeO 2 in H 2 /Ar, presenting surface plasma resonance (SPR) like visible light absorption. No modifications on microstructural surface disordering or valence band edge were detected in gray CeO 2 . Hydrogenation induced abundant V O inside both the bulk lattice and the surface layer. Gray CeO 2 presented much enhanced performance as well as improved water resistance in photocatalytic oxidation of gaseous hydrocarbons. Additional post-annealing in air was applied to remove surface V O and discolored the material. With series of characterization including XPS, Raman, EPR and in-situ FTIR, it was found bulk V O mostly contributes to the enhanced PE conversion, while surface V O is mainly responsible for the improved water resistance. Our results unambiguously confirmed hydrogenation as an efficient approach to simultaneously optimize oxide semicomductors in various elementary steps of photocatalysis.
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TALANTA
·
2017
·
IF 4.162
Shuyao Huang,Jianqiao Xu,Jiayi Wu,Haojia Hong,Guosheng Chen,Ruifen Jiang,Fang Zhu,Yuan Liu,Gangfeng Ouyang
The concentration of five rapidly metabolized anesthetics in living tilapias was determined in this study, by the presented method coupling in vivo solid phase microextraction (SPME) to gas chromatography-mass spectrometry (GC-MS), which was the first time that in vivo sampling method was adapted in detecting the anesthetic residue in the living aquatic product. The analytical performance of the developed method was evaluated in homogenized tilapia dorsal muscle, and the results demonstrated that the present method possessed low detection limits 1.7–9.4 ng g −1 ), wide linear ranges (10 or 30–5000 ng g −1 ), and satisfactory reproducibility (relative standard deviations no more than 8.1% and 10.8% for inter-fiber and intra-fiber assays, respectively). Standard curves were established in homogenized tilapia dorsal muscle for calibrating in vivo SPME in living tilapias. And the concentrations determined by in vivo SPME were close to those determined by the liquid extraction. By using the present method, one anesthetic residue was detected above the detection limit in tilapias from the local markets. Comparing to traditional methods, the present one exhibited superior time-efficiency and cost performance, as the extraction time was only ten minutes, which was short to successfully avoid the possible loss of analytes caused by elimination and sample storage. In addition, owing to the time-efficiency of the present method, the elimination of the anesthetics in tilapias was traced successfully in the laboratory.
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ADVANCED FUNCTIONAL MATERIALS
·
2017
·Vol. 27
·期 22
·1700653
·
IF 12.124
Jia Yan,Marco-Tulio F. Rodrigues,Zhilong Song,Hongping Li,Hui Xu,Huan Liu,Jingjie Wu,Yuanguo Xu,Yanhua Song,Yang Liu,Peng Yu,Wei Yang,Robert Vajtai,Huaming Li,Shouqi Yuan,Pulickel M. Ajayan
Many unique properties arise when the 3D stacking of layered materials is disrupted, originating nanostructures. Stabilization, and further reorganization of these individual layers into complex 3D structures, can be essential to allow these properties to persist in macroscopic systems. It is demonstrated that a simple hydrothermal process, assisted by ionic liquids (ILs), can convert bulk g-C 3 N 4 into a stable hydrogel. The gelation occurs through delamination of the layered structure, driven by particular interactions between the IL and the carbon nitride sheets, forming an amphiphilic foam-like network. This study employs spectroscopic and computational tools to unravel the gelation mechanism, and provides a rational approach toward the stabilization of 2D materials in hydrogels. The solution-processable hydrogels can also be used as building blocks of complex devices. Chemiresistive gas sensors employing g-C 3 N 4 3D hydrogels exhibit superior response at room temperature, enabling effective gas sensing under low power conditions.
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ELECTROCHIMICA ACTA
·
2017
·
IF 4.798
Yan Zhang,Mingming Gao,Shu-Guang Wang,Weizhi Zhou,Yuanhua Sang,Xin-Hua Wang
In this study, we developed an electro-Fenton (EF) system with a Fe 3 O 4 /gas diffusion electrode (Fe 3 O 4 /GDE) as the rotating cathode, realizing the simultaneous processes of O 2 diffusion, H 2 O 2 generation and activation at the cathode for the first time. In this system, H 2 O 2 was effectively electro-generated on the rotating cathode without external aeration, and then in suit activated to hydroxyl radical by the immobilized Fe 3 O 4 . Experimental results showed that 50 mg L −1 of tetracycline was completely degraded in 120 min, with the total organic carbon removal efficiency of 56.7%, which was accelerated by 1.7 times compared with the mobilized Fe 3 O 4 as catalyst. This enhancement was ascribed to the increased catalytic ability of immobilized Fe 3 O 4 in the presence of electric field. The effects of some important parameters such as Fe 3 O 4 loading, initial pH, applied potential and the rotation speed were evaluated. Computational fluid dynamics simulation suggested that the rotating disk mode greatly enhanced the mass transfer. Further investigation indicated that the immobilized Fe 3 O 4 contributed to the decomposition of H 2 O 2 predominately, while the effects of leaching iron could be ignored. The hydroxyl radical was considered as the primary reactive oxidants, and the degradation mechanism of tetracycline was proposed combined with the analysis of intermediates by ion chromatograph technology. These findings demonstrated the feasibility of establishing an efficient EF system with a simple and cost-effective integrated cathode based on iron immobilization and rotating GDE for environmental remediation.
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RSC Advances
·
2015
·Vol. 6
·期 4
·2703-2711
·
IF 3.84
Zhong-Liang Sun,Sheng-Zhang Xue,Cheng-hu Yan,Wei Cong,De-Zhu Kong
CO2 supplementation is usually a limiting factor in microalgal culture systems, especially when flue gases are used as the carbon source. In this study, tris(hydroxymethyl)aminomethane (THAM) was applied as a gas carrier to increase CO2 storage capacity in the culture medium and enhance microalgal biomass production. Abiotic experiments showed that the amount of CO2 absorbed by the medium within the same absorption time increased with increasing THAM concentration, and the gas absorptivity maintained a higher level (>60%) under the neutral pH conditions. Cell growth in shaker flasks illustrated that the biomass productivities of Scenedesmus dimorphus were significantly improved (31 to 66%) when the medium contained 2–8 mmol L−1 THAM. Meanwhile, THAM was not biodegraded during the cultivation. The biomass productivities achieved with 6 mmol L−1 THAM were much higher (32 to 33%) than that with routine culture when it was applied into an open raceway reactor system (2 m2), and the CO2 utilisation efficiency also increased by 6 to 12%. The results show that the addition of THAM as a gas carrier for enhancing CO2 input could be an easy-to-use and cost-effective approach for mass cultivation of microalgae.
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Energy Technology
·
2017
·Vol. 5
·期 10
·1836-1843
·
IF 2.789
Haoxin Wang,Ze Yu,Xiao Jiang,Jiajia Li,Bin Cai,Xichuan Yang,Licheng Sun
The inorganic p-type semiconductor CuI possesses several unique characteristics such as high transparency, low-production cost, high hole mobility, and good chemical stability and is a promising hole-transporting material candidate that can be explored in solar-cell devices. Herein, we adopt a simple solid–gas reaction method to fabricate a uniform CuI film by exposing a thermally evaporated copper film to iodine vapor and apply it as a hole-transporting layer (HTL) in inverted planar perovskite solar cells (PSCs). The optimized devices display a promising power conversion (PCE) efficiency of 14.7 %, with an open-circuit voltage of 1.04 V, a short-circuit current density of 20.9 mW cm −2 , and a fill factor of 0.68. This is one of the highest PCE values reported so far for CuI-based HTL in PSCs. Moreover, the devices studied also exhibit good long-term stability at ambient atmosphere, arising from the hydrophobicity of CuI HTL. The results highlight that CuI fabricated using the simple and low-temperature processing method presented here holds great promise as low-cost alternative HTL material for the development of efficient and stable inverted planar PSCs in the future.
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