MACROMOLECULES
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2023
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IF 5.5
Bingxue Jiang,Yisong Wang,Zhengqi Peng,Khak Ho Lim,Qingyue Wang,Shengbin Shi,Jieyuan Zheng,Xuan Yang,Pingwei Liu,Wen-Jun Wang
As one of the most promising biodegradable polymers, poly(butylene adipate-co-terephthalate) (PBAT) has attracted immense attention in packaging and mulching film applications. However, their slow degradation performance in aqueous environments remains a great challenge. In this work, we focused on tailoring the chain structure of PBAT by introducing poly(glycolic acid) (PGA) into the copolyester backbone. The PBAT-co-PGA copolyesters with molar percentages of butylene terephthalate of 36.2–50.3 mol % and GA of 8.0–20.2 mol % and number-average sequence lengths of poly(butylene terephthalate) of 1.55–1.97 and PGA of 1.06–1.11 were synthesized using a melt copolycondensation. The number-average sequence length of the PBAT-co-PGAs can be tailored while maintaining the same monomer composition. The PBAT-co-PGAs exhibit higher Young’s modulus (88 MPa) and tensile strength (35 MPa) owing to their better crystallization ability compared with PBAT at the same terephthalic acid fraction. The incorporation of more terephthalic acid and glycolic acid results in an increase of glass transition temperature and the formation of a more rigid chain structure, which is beneficial to improving the water vapor barrier properties of the copolyesters. Importantly, the PBAT-co-PGA copolyesters show enhanced degradation properties in water environments without sacrificing their aging resistance. The synthetic strategy proposed here endows the PBAT-co-PGA copolyesters with a broad chain structure tailoring window, which renders them to exhibit excellent mechanical properties, water barrier, aging resistance, and, most importantly, accelerated hydrolysis performances in aqueous environments.
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RSC Advances
·
2023
·Vol. 13
·期 45
·31785-31794
·
IF 3.9
Yi Yu,Kai Shao,Chonghui Niu,Mingjie Dan,Yingying Wang,Xiourong Zhu,Xianke Zhang,Yeqing Wang
In recent years, more and more attention has been paid to optical temperature sensing, and how to improve its accuracy is the most important issue. Herein, a new temperature sensing material, SrGd2Al2O7:Bi3+,Mn4+, based on fluorescence intensity ratio was designed in this work. It has both blue-purple and red luminescence under 300 nm excitation, and the dual-emitting centers with distinct colors, the different thermal sensitivities of Bi3+ and Mn4+, and the energy transfer between Bi3+ and Mn4+ give it excellent signal resolution and accurate temperature detection. The Sa of SrGd2Al2O7:0.04Bi3+,0.003Mn4+ phosphor reaches a maximum value of 8.573% K−1 at 473 K, and the corresponding Sr is 1.927% K−1, both of which are significantly better than those of most other reported optical temperature sensing materials. Taking all the results into account, the SrGd2Al2O7:0.04Bi3+,0.003Mn4+ phosphor can be regarded as a prominent FIR-type temperature sensing material.
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2023
·
IF 2.6
Qiang Gao,Ali Farajtabar
The shake-flask technique was used to test the solubility of glyburide in mixtures of acetone + water and ethyl acetate + methanol/ethanol/isopropanol under 101.0 kPa. For a fixed temperature, the glyburide solubility positively increased with the mass fraction of acetone in the acetone + water mixture, and reached a maximum value of 8.805 × 10 −6 at 298.15 K. The solubility magnitudes reach their peak when the mass fraction of ethyl acetate in solutions containing ethyl acetate plus methanol/ethanol/isopropanol is approximately 0.3, which correspond to 5.703 × 10 −4 , 5.235 × 10 −4 and 4.307 × 10 −4 , respectively, at 298.15 K. Two models-the Jouyban-Acree and modified van't Hoff-Jouyban-Acree were employed to correlate the solutility and produced the biggest relative average deviation of 7.78 %. The local composition (solvents) around the drug molecule was investigated at 298.15 K using an inverse Kirkwood-Buff integrals. The positive preferred solvation parameters of glyburide were observed in the medium and rich compositions of methanol/ n -propanol/isopropanol/acetonitrile/PG/NMP (taken from published works)/acetone, signifying that glyburide was preferentially solvated by these solvents; while they had negative magnitudes in ethyl acetate + methanol/ethanol/isopropanol systems throughout the whole ethyl acetate compositions. The solubility of glyburide in the ten solutions was properly described by an extended Hildebrand solubility parameter approach, with relative average errors of no more than 5.32 %. In addition, the electrostatic characteristics of the basicity/acidity of glyburide molecule were highlighted with the help of quantitative study of molecular surface. Because of their lowest (-158.0 kJˑmol −1 to −136.6 kJˑmol −1 ) and largest (156.6 kJˑmol −1 to 182.8 kJˑmol −1 ) global electrostatic potentials, the > C = O and > NH groups are the main targets of electrophilic and nucleophilic assault. Visual examination of the weak interactions between glyburide and the neat solvents (methanol, ethanol, isopropanol, acetone, ethyl acetate, and water) was done using the Hirshfeld partition analysis-based independent gradient model.
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JOURNAL OF RARE EARTHS
·
2023
·
IF 4.9
Danyu Zhang,Yuxuan Luo,Junyu Chen,Lianjie Li,Hai Guo
Dual-excitation and dual-emission Y 4 GeO 8 :Bi 3+ ,Sm 3+ phosphors were manufactured by traditional solid-phase sintering technique. The X-ray diffraction, morphology, photoluminescence, energy transfer process and temperature sensing properties of Y 4 GeO 8 :Bi 3+ ,Sm 3+ samples were comprehensively evaluated. The Y 4 GeO 8 :Bi 3+ ,Sm 3+ phosphors exhibit characteristic emissions of Bi 3+ ( 3 P 1 → 1 S 0 ) and Sm 3+ ( 4 G 5/2 → 6 H) under both 290 and 347 nm excitations. In fluorescence intensity ratio and Commission International de L'Eclairage coordinates modes, Y 4 GeO 8 :Bi 3+ ,Sm 3+ samples present excellent temperature measurement performance. The maximum relative sensitivity ( S r-max ) values of the former are 1.55 %/K (460 K, 290 nm excitation) and 0.82 %/K (506 K, 347 nm excitation). The S r-max ( x ) values of the latter are 0.21 %/K (437 K, 290 nm excitation) and 0.15 %/K (513 K, 347 nm excitation). These results illustrate that Y 4 GeO 8 :Bi 3+ ,Sm 3+ phosphors can be used as a candidate material for a dual-mode optical thermometer under dual-excitation.
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Molecular Catalysis
·
2023
·
IF 4.6
Jie Huang,Wenhao Yang,Sen Zhang,Jingjie Luo,Changhai Liang
Catalytic hydrogenation of adiponitrile to hexamethylenediamine (HMDA) via alkali-free processes is essential to produce high-value downstream chemicals. In this work, we synthesized a series of Co@C CNT x catalysts using CNT promotion to strength the carbon skeleton derived by ZIF-67. Compared to the Co@C without CNT promotion, great enhancement of HMDA yield was achieved by Co@C CNT x . Characterizations suggested that CNT in the precursor modified the crystallization of the active Co centers as well as the surface composition in the Co@C CNT x . Strong Co-carbon interaction was formed via Co-N coordination caused by the facilitated re-dispersion of N- containing functionalities. The ethanol contact angle on Co@C CNT x was changed for better mass transfer and diffusion of reaction liquid on the catalyst. As a final result, the oxidation of cobalt sites was greatly suppressed in Co@C CNT 0.3 and Co@C CNT 0.5 , which was proved an essential factor for their fast reaction rates. 88 % yield of HMDA with the rate of 4.5 mol HMDA /mol Co /h was reached under a much higher utilization rate of Co center.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Shipeng Geng,Liming Chen,Lianmei Kang,Ruchun Li,Haixin Chen,Luo Cheng,Dandan Cai,Yi Wang,Shuqin Song
Developing efficient and durable non-precious metal electrocatalysts with industrial current density is urgent for hydrogen evolution reaction from alkaline water/seawater but remains challenging. Here, a heterostructured Co/W 5 N 4 catalyst with porous structure is innovatively constructed. The theoretical calculations confirm the strong d-p hybridization between Co and N at the interface of Co/W 5 N 4 with the modulation of d‐band center of Co sites. The synergistic effect between Co and W 5 N 4 is disclosed that H 2 O can rapidly dissociate on the W sites to generate H* adsorbed at the Co sites for favorable H 2 production. Consequently, the Co/W 5 N 4 catalyst affords low overpotentials of 113 and 118 mV to drive current density of 100 mA cm −2 in alkaline water/seawater electrolytes, respectively, which are even superior to those of commercial Pt/C. More importantly, it can also present outstanding HER stability at large current density of 500 mA cm −2 for over two weeks (350 h) in alkaline water/seawater electrocatalysis.
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Advanced Healthcare Materials
·
2023
·
IF 10
Dongyan Shao,Ting Bai,Bobo Zhu,Xiaojia Guo,Kai Dong,Junling Shi,Qingsheng Huang,Jie Kong
Natural killer (NK) cells have emerged as an important contributor to cancer immunotherapy, but their antitumor efficacy remains suboptimal. While cytokine-based priming shows promise in enhancing NK-cell activity, its clinical translation faces many challenges, including co-activation of multiple cytokines, poor pharmacokinetics, and limited mechanistic understanding. Here, we developed a polymeric micelle-based IL-15/IL-2 codelivery system (IL-15/2-PEG-PTMC) for NK-cell activation. In vivo studies demonstrated that the half-life of IL-15 and IL-2 as well as the recruitment of NK cell within tumor tissue was significantly increased after PEG-PTMC loading. Coupled with the coactivation effect of IL-15 and IL-2 conferred by this polymeric micelle-based system, it noticeably delayed the growth of tumors in mice compared to conventional NK cell activation approach, that was free IL-15 and IL-2. We also surprisingly found that cholesterol metabolism was highly involved in the NK cell activation by IL-15/2-PEG-PTMC. Following stimulation with IL-15/2-PEG-PTMC or IL-15, NK cells underwent a series of cholesterol metabolism reprogramming, which elevated the cholesterol levels on the NK cell membrane. This in turn promoted the formation of lipid rafts and actived immune synapse, effectively contributing to the enhancement of the NK cell's anti-tumor activity. We believe this will open a new avenue for improving the efficacy of NK cell immunotherapy by regulating cholesterol metabolism. This article is protected by copyright. All rights reserved
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FUEL
·
2023
·
IF 7.4
Jia Li,Sheng He,Le Li,Zhiyuan Shen,Junyi Li,Congling Shi,Bobo Shi,Xiaoyu Chen,Fubao Zhou
Rapid removing toxic CO for methane-air mixture explosions is essential in reducing casualties, but relevant research is rare. This paper proposed a novel approach for efficient CO removal and explosion suppression for methane-air mixture explosions using Co 3 O 4 powder. The effect of Co 3 O 4 powder on the explosion characteristics and basic parameters to quantify the CO removal performance have been studied, mainly including maximum explosion pressure (P m ), combustion time (t c ), flame propagation velocity, and average CO removal rate (R ave. ). Results indicated that explosion intensity and CO concentration decreased significantly with Co 3 O 4 powder, due to increased heat absorption capacity and the active site of CO catalytic oxidation . However, the average CO removal rate decreased as the Co 3 O 4 powder usage and CH 4 partial pressure increased, which could reduce the dispersion degree of the Co 3 O 4 dust cloud. The CO removal was achieved through the CH 4 catalytic combustion and CO catalytic oxidation, which could reduce the CO generation and oxidize the generated CO to harmless CO 2 , respectively. This work provides a novel routine to lessen the explosion hazards and has promising applications in emergency rescue.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Can-Wen Yu,Cong-Yi Du,Ting Ouyang,Xi-Ting Zhang,Zhao-Qing Liu
Physical structure change of catalysts based on the electronic metal-support interaction (EMSI) effects is a prospective strategy to regulate the surface electronic structure of catalysts and further enhance their catalytic performance. To optimize the constrained intrinsic oxygen evolution reaction/oxygen reduction reaction (OER/ORR) activity of spinel MnCo 2 O 4 , we present a facile hydrothermal and photoreduction strategy to synthesize the Ag and MnCo 2 O 4 supported on N-doped carbon nanotubes (Ag-MnCoO/NCNTs) with the EMSI effect. Ag-MnCoO/NCNTs as catalyst shows enhanced performance for OER (overpotential of 340 mV) and ORR (half-wave potential of 0.80 V). Furthermore, a zinc-air battery is assembled based on Ag-MnCoO/NCNTs cathode, which affords an open circuit potential of 1.49 V and favorable cycling performance for 200 h. Theoretical calculations illustrate the introduction of Ag reduces the charge density of the tetrahedral Co site along the direction of the dangling bonds and optimizes the adsorption of oxygen intermediates on tetrahedral Co, thus lowering the reaction activation energy and improving its oxygen catalytic activity. This work provides new insights to guide the fabrication of advanced oxygen electrocatalysts.
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Weiting Gao,Xuelang Gao,Qiugen Zhang,Aimei Zhu,Qinglin Liu
Building well-developed ion-conductive highways is highly desirable for anion exchange membranes (AEMs). Grafting side chain is a highly effective approach for constructing a well-defined phase-separated morphological structure and forming unblocked ion pathways in AEMs for fast ion transport. Fluorination of side chains can further enhance phase separation due to the superhydrophobic nature of fluorine groups. However, their electronic effect on the alkaline stability of side chains and membranes is rarely reported. Here, fluorine-containing and fluorine-free side chains are introduced into the polyaromatic backbone in proper configuration to investigate the impact of the fluorine terminal group on the stability of the side chains and membrane properties. The poly(binaphthyl-co-p-terphenyl piperidinium) AEM (QBNpTP) has the highest molecular weight and most dimensional stability due to its favorable backbone arrangement among ortho- and meta-terphenyl based AEMs. Importantly, by introducing both a fluorinated piperidinium side chain and a hexane chain into the p-terphenyl-based backbone, the prepared AEM (QBNpTP-QFC) presents an enhanced conductivity (150.6 mS cm −1 ) and a constrained swelling at 80 °C. The electronic effect of fluorinated side chains is contemplated by experiments and simulations. The results demonstrate that the presence of strong electro-withdrawing fluorine groups weakens the electronic cloud of adjacent C atoms, increasing OH − attack on the C atom and improving the stability of piperidinium cations. Hence QBNpTP-QFC possesses a robust alkaline stability at 80 °C (95.3% conductivity retention after testing in 2 M NaOH for 2160 h). An excellent peak power density of 1.44 W cm −2 and a remarkable durability at 80 °C (4.5% voltage loss after 100 h) can be observed.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2023
·
IF 6.1
Renjie Xie,Jianbin Lu,Jian Wang
The detection of dissolved gases in the oil of oil-immersed transformers is essential to evaluate the operating status of oil-immersed transformers. In this study, a CuO/TiO 2 /N-MWCNTs composites-based sensor was fabricated by hydrothermal method for the detection of dissolved CO gas in oil. The introduction of N-MWCNTs with high specific surface area, high electrical conductivity and multiple adsorption sites effectively improved the response value and response/recovery performance for CO. The response can reach 4.33 at a CO concentration of 50 ppm, which is 1.74 times higher than that of the CuO/TiO 2 sensor. In addition, the prepared sensor presents a fast response/recovery time (230 s/60 s) to CO, and has excellent selectivity and long-term stability. Finally, a multi-concentration CO alarm system was constructed through a reasonable circuit design. It is shown that the CuO/TiO 2 /N-MWCNTs-based sensor can achieve high-precision CO detection, which can provide a new idea for the detection of dissolved CO gas in the oil of oil-immersed transformers.
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CHEMOSPHERE
·
2023
·
IF 8.8
Jian Sun,Huayi Qu,Waseem Ali,Yan Chen,Tao Wang,Yonggang Ma,Yan Yuan,Jianhong Gu,Jianchun Bian,Zongping Liu,Hui Zou
Microplastics (MPs) and cadmium (Cd) are important environmental pollutants, that damage the liver. However, the effect and mechanism of combined Cd and MPs exposure on liver fibrosis are still largely unknown. In this study investigated, Cd + MPs exposure increased superoxide anion production and promoted extracellular ATP release compared with exposure to Cd or MPs individually. Cd + MPs increased inflammatory cell infiltration , activated the P2X7-NLRP3 signaling pathway, and promoted inflammatory factor release. Cd + MPs aggravated Cd- or MPs-induced liver fibrosis and induced liver inflammation. In AML12/HSC-T6 cell in vitro poisoning model, exposure of AML12 cells to Cd + MPs increased the opening of connexin hemichannels and promoted extracellular ATP release. Treatment of HSC-T6 cells with the supernatant of AML12 cells exposed to Cd + MPs significantly promoted HSC-T6 cell activation. Treatment of HSC-T6 cells with different concentrations of ATP produced similar results. TAT-Gap19TFA, an inhibitor of connexin hemichannels, significantly inhibited the ATP release and activation of Cd + MPs-treated HSC-T6 cells. Finally, the expression of the ATP receptor P2X7 was silenced in HSC-T6 cells, which significantly inhibited their activation. In conclusion, exposure to Cd + MPs promoted liver fibrosis through the ATP-P2X7 pathway and synergistically affected liver inflammation and fibrosis.
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