Acta Pharmaceutica Sinica B
·
2024
·
IF 14.7
Jinhu Liu,Han Yang,Xiao Sang,Tong Gao,Zipeng Zhang,Shunli Fu,Huizhen Yang,Lili Chang,Xiaoqing Liu,Shuang Liang,Shijun Yuan,Suyun Wei,Yuxin Yang,Xiaoxin Yan,Xinke Zhang,Weiwei Mu,Yongjun Liu,Na Zhang
Cytopharmaceutical based on macrophages is a breakthrough in the field of targeted drug delivery. However, it remains a challenge to localize and control drug release while retaining macrophage activity and exerting its immunotherapeutic effect. Herein, a localized light-triggered release macrophage cytopharmaceutical (USIP@M) was proposed, which could utilize the tumor targeting and immunotherapy effects of macrophages to reverse the immune suppression of tumor microenvironment (TME). Amphiphilic block copolymers with ultraviolet (UV)-responsive o -nitrobenzyl groups were synthesized and co-loaded with sorafenib (SF), IMD-0354 (IMD), and upconverting nanoparticles (UCNPs), which were then taken up by macrophages, and the targeted delivery of drugs was realized by using the tumor tropism of macrophages. UCNPs converted near-infrared light with strong penetrability and high safety into UV light, which promoted the photoresponsive depolymerization of block copolymers and production of exosomes from USIP@M, accelerated drug efflux and maintained the activity of macrophages. IMD simultaneously polarized carrier macrophages and tumor-associated macrophages to exert the antitumor effect of macrophages, enhance T cell immunity, and alleviate the immunosuppressive state of TME. Synergistically with the chemotherapeutic effect of SF, it could effectively kill tumors. In conclusion, based on the localized light-triggered release strategy, this study constructed a novel macrophage cytopharmaceutical that could localize and control drug release while retaining the activity of macrophages and exerting its immunotherapeutic effect, which could effectively treat solid tumors.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Wenqian Cao,Yumeng Qi,Ying Zhang,Ruixue Guo,Ruijuan Qu,Zunyao Wang
Photolysis is the main pathway for the degradation of persistent organic pollutants (POPs). Most investigations, however, have been limited to the ultraviolet or visible region, and the reaction mechanism of infrared (IR) light is still unclear. In this study, the photodegradation of o,p' -dichlorodiphenyltrichloroethanes ( o,p' -DDT) on the silica (SiO 2 )/air interface under different irradiation light sources was systematically investigated. Interestingly, for the first time, effective degradation of o,p' -DDT under IR light irradiation was observed, which was ascribed to the anti-Stokes Raman scattering process of SiO 2 . Moreover, desert sands could also serve as a vector for the photodegradation of o,p' -DDT. The lower removal efficiency of desert sands compared to pure SiO 2 was a combined effect of differences in Fe 3+ component and SiO 2 content. It is worth noting that direct photodegradation plays a dominant role in the photodegradation of o,p' -DDT on SiO 2 . Besides, indirect photodegradation resulted mainly from •OH (25.0%), O 2 • − (6.9%), and 1 O 2 (5.6%) generated in the reaction system. In addition to hydroxylation and dechlorination products, the formation of four novel silicon-based products was observed, which resulted from the direct reaction of silyl radicals with o,p' -DDT. This study revealed that the specific Raman scattering effect of SiO 2 played a vital role in the self-purification process of POPs upon SiO 2 -based environmental matrices. The light-mediated decontamination system upon SiO 2 constructed in this study could provide critical information for addressing POPs contamination on sands.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Hailong Tang,Yongqing Ma,Ganhong Zheng,Chuhong Zhu,Meiling Wang,Yilin Lu,Xiao Sun
Photocatalytic CH 4 conversion to CH 3 OH under mild conditions is undoubtedly an efficient strategy to realize CH 4 upgrading. In this work, in-situ formed highly reactive Fe IV =O complex with a bound Cl axial ligand was detected at ambient temperature and its contribution to CH 4 photoxidation to CH 3 OH was deeply investigated. Under optimized experimental condition, a high CH 3 OH yield of 3026.1 mmol mol Fe −1 (6.76 mmol g cat −1 h −1 ) with selectivity of 73.6 % was obtained during 8 h. Isotope labeling mass spectroscopy experiments manifested that O 2 was the only source of oxygen in products. The formation of Cl-(H 2 O) 4 Fe IV O complex was confirmed using low-temperature electron spin resonance spectroscopy and cryogenic Raman spectroscopy (ν(Fe O) = 828 cm −1 ). Through density functional theory (DFT) calculation, we showed that the Cl axial ligand acts as an “electron reservoir” during CH 4 conversion, i.e., electron acceptor during the process of CH 4 oxidation to CH 3 OH, while electron donor in CH 3 OH desorption. This not only lowered C-H cleavage energy, but also facilitated CH 3 OH desoption and inhibited overoxidation. As far as we know, Cl-(H 2 O) 4 Fe IV O is the first detected Fe IV O complex generated directly from O 2 and Fe 3+ at ambient temperature.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Riguang Cheng,Zhaoyu Liu,Pantrangi Manasa,Zhongxian Zhao,Hongge Pan,Fen Xu,Lixian Sun,Federico Rosei
The inherent thermodynamic stability and slow kinetics of LiAlH₄ pose significant challenges for its practical application in hydrogen storage. This study addresses these limitations by introducing nanoflower-structured layered double oxides (Co₃O₄@CoNi-LDO) as a performance-enhancing catalyst. The Co₃O₄@CoNi-LDO was synthesized through a hydrothermal process followed by calcination and subsequently incorporated into LiAlH₄ via mechanical ball milling. Experimental results demonstrate that the addition of 7 wt% Co₃O₄@CoNi-LDO substantially improves the hydrogen desorption properties of LiAlH₄. The hydrogen release temperatures for the two-step desorption process are reduced to 85.1 °C and 177.0 °C, respectively, with a total hydrogen release of approximately 6.87 wt% below 300 °C. Moreover, the activation energy of the two desorption steps is lowered by 20.0% and 46.3% compared to pristine LiAlH₄. The modified material also exhibits superior rehydrogenation performance, absorbing approximately 0.64 wt% hydrogen within 5 h-markedly better than pristine LiAlH₄. Mechanistic studies reveal that the in-situ formation of catalytically active species, such as Al₁₃Co₄ and Al₀.₉Ni₄.₂₂, anchored on the LiAlH₄ matrix, plays a pivotal role in facilitating hydrogen transfer. These catalytic sites effectively reduce the energy barriers for hydrogen desorption, enhancing the kinetics of the process. This work highlights the potential of Co₃O₄@CoNi-LDO nanoflowers as a highly effective catalyst for improving the hydrogen storage capabilities of LiAlH₄, paving the way for its application in advanced energy storage systems.
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ACS Central Science
·
2024
·
IF 12.7
Xiangfeng Meng,Yue Zhou,Lei Xu,Limu Hu,Changjiang Wang,Xiao Tian,Xiang Zhang,Yi Hao,Bo Cheng,Jing Ma,Lei Wang,Jialin Liu,Ran Xie
Glycosylation plays a pivotal role in the intricate landscape of human cholangiocarcinoma (CCA), actively participating in key pathophysiological processes driving tumor progression. Among the various glycosylation modifications, O-linked β-N-acetyl-glucosamine modification (O-GlcNAcylation) emerges as a dynamic regulator influencing diverse tumor-associated biological activities. In this study, we employed a state-of-the-art chemical proteomic approach to analyze intact glycopeptides, unveiling the critical role of O-GlcNAcylation in orchestrating Keratin 18 (K18) and its interplay with tricarboxylic acid (TCA) cycle enzymes, specifically isocitrate dehydrogenases (IDHs), to propel CCA progression. Our findings shed light on the mechanistic intricacies of O-GlcNAcylation, revealing that site-specific modification of K18 on Ser 30 serves as a stabilizing factor, amplifying the expression of cell cycle checkpoints. This molecular event intricately fosters cell cycle progression and augments cellular growth in CCA. Notably, the interaction between O-GlcNAcylated K18 and IDHs orchestrates metabolic reprogramming by down-regulating citrate and isocitrate levels while elevating α-ketoglutarate (α-KG). These metabolic shifts further contribute to the overall tumorigenic potential of CCA. Our study thus expands the current understanding of protein O-GlcNAcylation and introduces a new layer of complexity to post-translational control over metabolism and tumorigenesis.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Ruyi Zhong,Zisheng Zhang,Huqiang Yi,Lei Zeng,Chao Tang,Limin Huang,Meng Gu
Visible-light photocatalytic hydrogen evolution is a key step towards utilizing solar energy. Here we constructed covalently bonded oxidized graphitic C 3 N 4 /TiO 2 (O-g-C 3 N 4 /TiO 2 ) heterostructure with high surface area via an in-situ solvothermal synthetic strategy. The edge-anchoring of two-dimensional (2D) TiO 2 on 2D O-g-C 3 N 4 was evidenced by the HAADF-STEM EDS mapping, EELS and XPS analysis. Density functional theory computations suggest strong affinity between TiO 2 and O-g-C 3 N 4 2D structures through N O Ti covalent bonding, which drastically enhances the synergetic effect of the light absorption of O-g-C 3 N 4 and high surface area of TiO 2 . The as-formed heterojunction can remarkably boost the visible-light photocatalytic activity for H 2 evolution by 6.1 times compared to physical mixture of TiO 2 nanosheets (NS) and O-g-C 3 N 4 .
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DALTON TRANSACTIONS
·
2017
·Vol. 47
·期 1
·180-189
·
IF 4.029
Dandan Yang,Jie Dong,Baiquan Wang
A series of new pincer-type tridentate o-aryloxide-N-heterocyclic carbene nickel complexes Ni1–Ni3 were synthesized, and the molecular structure of Ni3 was confirmed by X-ray crystallography. In comparison with the above tridentate complexes, the bidentate bis(aryloxide-NHC) nickel complex Ni4 was also synthesized. On activation with either Et2AlCl or Me2AlCl, all nickel complexes showed low activity toward norbornene (NB) homopolymerization. Surprisingly, Ni1–Ni3 catalysts exhibited moderate to high activity toward the homopolymerization (up to 3.21 × 106 g PNB (mol of Ni)−1 h−1) and copolymerization of norbornene with 1-octene (up to 1.39 × 105 g polymer (mol of Ni)−1 h−1) with B(C6F5)3 as the cocatalyst even at 100 °C, showing that tridentate nickel catalysts have high thermal stability. Notably, the tridentate Ni1–Ni3 complexes showed better activities than the corresponding bidentate bis(aryloxide-NHC) nickel complex Ni4. The obtained poly(NB-co-1-octene)s were confirmed to be vinyl-addition copolymers, which exhibited high 1-octene insertion ratio (9%–17%), good thermal stability (Td > 400 °C), high molecular weight (up to 105), and narrow molecular weight distribution (PDI ≤ 1.91).
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Chemical Engineering and Processing-Process Intensification
·
2017
·
IF 2.234
Xiaoming Luo,Juhang Cao,Haipeng Yan,Haiyang Gong,Haoran Yin,Limin He
The separation characteristics of W/O emulsion were investigated under ultrasonic standing wave field in this paper. The effects of the irradiation time, acoustic intensity, frequency, oil viscosity, and oil-water interfacial tension on the separation characteristics of emulsion were studied in details. It was proved that there existed an optimal irradiation time, acoustic intensity and oil-water interfacial tension to achieve the maximum separation efficiency in ultrasonic treatment process. Excessive long irradiation time had little effect on improving the dehydration rate of emulsion but rather increased unnecessary processing time. Excessive high acoustic intensity caused the occurrence of acoustic cavitation phenomenon. The acoustic cavitation would cause the aggregated droplets to be dispersed by oscillating bubbles or even emulsified again by high speed micro jets. The acoustic cavitation threshold is effectively and accurately obtained by a spectral analysis method. The micro acoustic streaming which resulted from the attenuation of acoustic energy occurred with the increase of frequency. It sheared the aggregated droplets, destroyed the stable droplets banding and reduced the separation efficiency of emulsion. The excess surfactant adsorbed on the oil-water interface resulted in the increase of the interfacial film strength, which hindered the coalescence process of droplets and reduced the separation efficiency.
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INFLAMMOPHARMACOLOGY
·
2018
·Vol. 27
·期 5
·969-974
·
IF 3.304
Zhao Mingyi,Zhou Peng,Yu Jun,James Asenso,Xiao Feng,Wang Chun,Wei Wei
Paeoniflorin-6′-O-benzene sulfonate (code: CP-25) is a novel ester derivative of paeoniflorin (Pae). Compared to Pae, CP-25 has higher lipid solubility, bioavailability and better bioactivity. However, the tissue distribution and excretion of CP-25 still remain unknown. The LC–MS method was applied to investigate the tissue distribution and excretion of CP-25 in rats. As such, 50 mg/kg of CP-25 and Pae were administered to rats in multiple doses via an oral route. CP-25 and Pae were distributed widely and rapidly in all the tested tissues. Compared with Pae, the concentrations of CP-25 were almost increased evidently in most tissues. The highest CP-25 level was found in the liver (1476.33 ± 535.20 ng/g, male; 1970.38 ± 177.21 ng/g, female) at 3 h, and a high concentration of CP-25 was detected in male and female intestine, synovium, muscle, lung, and brain. Following a single oral dose of 50 mg/kg of CP-25 in rats, the total excretion of CP-25 was merely 21.8% (18.40, 3.19 and 0.22% for feces, bile and urine, respectively) in males; and was approximately 21.3% (14.04, 7.16 and 0.14% for feces, bile and urine, respectively) in females. The results indicated that the CP-25 concentration was higher in major tissues than Pae; CP-25 was primarily excreted through the feces; and there were gender-related differences in the tissue distribution and excretion.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Han Xu,Qin Yang,Mingjiao Tian,Yaruo Zhao,Dong Guo,Zeyu Jiang,Yanfei Jian,Yadi Wang,Fan Dang,Chunli Ai,Jialei Wan,Reem Albilali,Chi He
Revealing the mechanism behind active oxygen species in chlorinated volatile organic compounds (CVOC) destruction is crucial but challenging. Herein, we designed a chromium-substituted titanium bimetal catalyst with strengthened element interaction, exhibiting remarkable ability to activate oxygen and destroy intermediates. Encapsulated chromium species triple the electron transfer speed (Cr → TiO 2 ), converting 90 % of vinyl chloride at 244 °C. The constructed Cr 6 + −O−Ti 3+ structure distorts TiO 2 lattice, generating defects that promote oxygen species activation. In-situ technologies and DFT calculations demonstrate that vinyl chloride adsorbed at Cr 6+ =O sites is oxidized by lattice oxygen, forming C O species, while surface oxygen activates in a cyclic process, promoting the *CH 2 CH to *CH 2 CHO and CH 2 CO. The constructed Cr-O-Ti structure breaks the rate-limiting step of *CH 2 CHO to CH 2 CO process, accelerating the formation of *CH 3 CO and further promoting the deep oxidation process (*CHO + *CO). This work presents new findings towards CVOC highly efficient purification, showcasing significant application potential.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Lin Lin,Houzhi Fang,Changzhu Li,Jinming Dai,Metab Alharbi,Haiying Cui
The main objective of this study is to investigate the impact and mechanism of soy lecithin incorporation into the gelatin-cinnamaldehyde emulsion, focusing on how it influences emulsion stability during the electrospinning process. In this work, a cinnamaldehyde/gelatin/soy lecithin (CGS) fiber membrane with excellent antibacterial properties was successfully created. The addition of soy lecithin improves the stability of the emulsion and improves the loading performance and fiber morphology of the CGS fiber membrane. Fourier Transform infrared spectroscopy (FTIR) and urea addition confirmed that soy lecithin may strengthen the interface structure of gelatin in the oil and water phases through hydrogen bonds, thus enhancing the stability of the emulsion in electrospinning. The application tests also revealed that the CGS fiber membrane effectively preserved the sensory quality of beef. This study indicates that the vector construction method can extend the utilization of cinnamaldehyde in food industry.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2011
·
IF 2.089
Baimei Yang,Hui Wan,Guofeng Guan
Isobaric binary vapor–liquid equilibrium (VLE) data for 1-butanol + ethylbenzene, or o-, or m-, or p-xylene and isobaric quinary VLE data for 1-butanol + ethylbenzene + o-xylene + m-xylene + p-xylene are measured at 101.33 kPa using a modified Rose cell with circulation of both phases. The four binary systems of 1-butanol + ethylbenzene, or o-, or m-, or p-xylene exhibit minimum boiling azeotropes, and the composition of the azeotropes are reported. The VLE data for the four binary systems are checked to meet rigorous thermodynamic consistency by Herington method and the point-to-point test of the Fredenslund method. The nonideality in vapor phase of the measured binary systems is analyzed through calculating fugacity coefficients. Combined with the Hayden–O'Connell (HOC) equation, the VLE data for 1-butanol + ethylbenzene, or o-, or m-, or p-xylene are well-correlated by the nonrandom two-liquid (NRTL), universal quasichemical activity coefficient (UNIQUAC), and Wilson equations. The NRTL model parameters obtained from correlation are used to predict the VLE data of the quinary system. According to the average absolute deviation values, the obtained quinary predicted values are in good agreement with the experimental values.
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危险品化学品经营许可证（带存储）