Nanoscale
·
2021
·Vol. 13
·期 30
·12966-12978
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IF 7.79
Jie Yu,Xidong He,Zigui Wang,Yupeng Wang,Sha Liu,Xiaoyuan Li,Yubin Huang
Immune checkpoint blockade (ICB) therapy in combination with immunogenic death (ICD) triggered by photothermal therapy (PTT) and oxaliplatin (OXA) treatment was expected to elicit both innate and adaptive immune responses for tumor control and metastasis prevention. In this study, a photothermal agent (IR780), a folic acid (FA) linked oxaliplatin (OXA) prodrug, and PD-L1 inhibitors (BMS-1) were integrated into a liposomal system. The FA tumor-targeting and enhanced permeability and retention (EPR) effect of the liposomal system prolonged circulating times and increased accumulation in tumors, resulting in an enhanced photothermal effect and less systemic toxicity. In addition, PTT and OXA had a considerable synergistic effect in the induction of a combined ICD. The PD-1/PD-L1 checkpoint, which is a negative immune regulatory mechanism, could be blocked by the thermosensitive released BMS-1. Finally, ICD was harnessed to synergize with a small molecule PD-L1 inhibitor for activation of the immune system in the treatment of tumor relapse and metastasis.
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RSC Advances
·
2020
·Vol. 11
·期 1
·48-56
·
IF 3.119
Yingjie Hu,Yuxin Mei,Baining Lin,Xuhong Du,Fan Xu,Huasheng Xie,Kang Wang,Yonghua Zhou
The one-pot synthesis of methyl isobutyl ketone (MIBK) and methyl isobutyl methanol (MIBC) from acetone and hydrogen is a typical cascade reaction comprised of aldol condensation-dehydration-hydrogenation. Pd loss and aggregation during long term operation are typical problems in industrial application. In this paper, an active and stable catalyst was achieved with defective UiO-66 as a support for Pd, which was synthesized with the ratio 15 : 1 of ZrOCl2·8H2O to ZrCl4 as Zr-precursors. The resultant Pd catalyst remained active for at least 1000 h with a MIBK + MIBC selectivity of 84.87–93.09% and acetone conversion of 45.26–53.22% in a continuous trickle-bed reactor. Besides the increased Brønsted acid amount generated by the defect sites was favorable for the activity, the cavity confinement in the UiO-66 (R = 15 : 1) structure also efficiently prevented Pd loss and aggregation during the long term run. The contrast of the characterization of the fresh and used Pd/UiO-66 (R = 15 : 1) indicated that the deactivation of the catalyst was attributed to carbonaceous accumulation on the catalyst surface, which could be easily regenerated by calcination. This work supplied a new alternative for the design and utilization of industrial catalysts for MIBK and MIBC synthesis.
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Antibiotics-Basel
·
2022
·Vol. 11
·期 11
·1660
·
IF 5.222
Yan Wang,Lanyu Liu,Qiping Wu,Qiufen Yin,Feifan Xie
Background: The pharmacokinetic/pharmacodynamic (PK/PD) index of carbapenems that best correlates with in vivo antimicrobial activity is percent time of dosing interval in which free drug concentration remains above MIC (%fT > MIC), while the magnitudes of the PK/PD index of carbapenems remains undefined in critically ill sepsis patients.Methods: A sepsis rat model was first developed by comparing the survival outcomes after intraperitoneal injection of different inoculum size (1–10 × 107CFU) ofPseudomonas aeruginosaATCC9027 (MIC = 0.125 mg/L) in neutropenic rats. The PK characteristics of the model drug meropenem in the developed sepsis rat model was then evaluated, and PK modeling and simulation was applied to design meropenem dosing regimens attaining various PD targets (40%fT > MIC, 100%fT > MIC, and 100%fT > 4 × MIC). The microbiological response and survival outcomes for different meropenem treatment regimens were investigated in the rat sepsis model (n= 12 for each group).Results: The optimal inoculum for the rat sepsis model was 1 × 107CFU ofPseudomonas aeruginosaATCC9027. A one-compartment model with first-order absorption best described the PK of meropenem in sepsis rats. Pronounced survival prolongation and lower hazard risk were observed in the treatment groups of 50 or 75 mg/kg/q2.4h (100%fT > MIC) and 75 mg/kg/q2h (100%fT > 4 × MIC) compared to the 75 mg/kg/q6h (40%fT > MIC) group, while meropenem groups with PD targets of 100%fT > MIC and 100%fT > 4 × MIC showed comparable survival curves. Microbiological response for different PD targets is inconclusive due to irregular bacterial counts in blood samples.Conclusions: The PD target of 40%fT > MIC is suboptimal for sepsis rats, and the aggressive 100%fT > 4 × MIC target does not provide a survival benefit against the target of 100%fT > MIC.Keywords:pharmacokinetics;PK/PD;survival;meropenem;sepsis rat model
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Nano Today
·
2022
·
IF 18.962
Di Liu,Hongliang He,Fei Kong,Yixiang Cao,Fengchao Zang,Ming Ma,Ning Gu,Yu Zhang
Currently, multimodal synergistic nanoplatform emerges as an important cancer therapy paradigm, however, multimodal synergistic theranostic nanoplatform remains to be developed. Herein, using the mouse model of breast cancer, a versatile multimodal synergistic theranostic nanoplatform is rationally designed and synthesized for enhancing chemodynamic therapy (CDT), overcoming immunosuppression within tumor microenvironment , and inhibiting metastasis as well as tracking tumor. To fulfill our design, a composite Fe/Mn magnetic nanoparticle is first synthesized by loading with Fe 3 O 4 and BMS-202 (PD-L1 inhibitor) within a poly(lactide-co-glycolide)-based nanoparticle core, which are further modified with in situ synthesis of MnO 2 layer. Then, the composite metal-organic nanoparticle is coated with two targeting moieties hyaluronic acid (HA) and AMD3100 (CXCR4 antagonist), respectively, to achieve the multimodal synergistic theranostic nanoplatform ( [email protected] +AMD). With surface targeting modification, [email protected] +AMD exhibits enhanced tumor accumulation, where it effectively consumes endogenous glutathione to generate Mn 2+ allowing for the enhanced CDT effect, alleviates tumor hypoxia by O 2 generation and reverses the tumor immunosuppression. [email protected] +AMD blocks CXCR4 receptor on cancer cells, thus suppressing the CXCR4-mediated cancer metastasis and invasion. Additionally, [email protected] +AMD would synchronously be achieving tumor tracking by T 1 -T 2 dual-mode magnetic resonance imaging. Collectively, this strategy holds a novel multimodal synergistic theranostics for effective cancer management.
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CHEMICAL PAPERS
·
2023
·Vol. 77
·期 11
·6637-6646
·
IF 2.2
Chen Lei,Li Rongxin,Li Yuanlong,Shu Qijiang,Yang Tao
The reduced graphene oxide aerogel modified by 4-chlorophenyl sulfoxide was obtained by a simple self-assemble process under the basic reduction-oxide condition, then freeze-dried for future using. The prepared aerogel was shortly named 4CS-rGO, which was characterized by Fourier transform infrared spectroscopy, Raman spectroscopy, scanning electron microscope, et al. 1 mg of 4CS-rGO composite was used as an adsorbent to adsorb Pd(II) and Pt(IV) in 1.0 mL 40 mM Britton-Robinson buffer solution with various pH. The adsorption efficiency of Pd(II) increased with the increase in pH, whereas the hydrolysis of Pd(II) happened at pH 13, and the maximum adsorption efficiency of Pd(II) was 91.82% at pH 12, which was mainly driven by electrostatic attraction. Besides, the adsorption behavior of the 4CS-rGO composite for Pt(IV) was explored to evaluate the possibility to isolate Pd(II) and Pt(IV) ions by using aerogel. We found that, quite interestingly, hydrogen bond, hydrophobic interaction and van der Waals force can strongly conquer electrostatic repulsion driven Pt(IV) ions adsorption behavior at pH 5, and Pt(IV) ions displaced by cationic surfactant. Moreover, a tighter Pt(IV) ions adsorption behavior than Pd(II) ions was observed while we adsorb them respectively with/without 4-chlorophenyl sulfoxide modified the graphene, while branched TBAB was easier and more effectively replaced the adsorbed Pt(IV) ions than strained CTAB.
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Molecular Catalysis
·
2023
·
IF 4.6
Jia Li,Jianfeng Zheng,Xingmin Liu,Zhanggen Huang
Metal additives can greatly improve the catalytic oxidation of photocatalysts for degrading volatile organic compounds (VOCs) including formaldehyde. Different type metal, including Pd, Cu and Na, were doped in TiO 2 (B) nanosheets with oxygen vacancy, and the degradation rate of HCHO were evaluated using the above catalysts. A series of theoretical and experimental studies on these modified TiO 2 (B) photocatalysts were carried out. The presence of O v leads to the appearance of impurity levels under the conduction band of TiO 2 (B), which could enhance the absorption in the visible spectral range by reducing the band gap and inhibiting the recombination of photo-induced charges. TiO 2 (B) with oxygen vacancies and doped with Na is used as a photocatalyst for degrading HCHO, and the removal rate up to 80% within 50 min. It is quite important to match the bandgap structure of photocatalysts and redox potential of O 2 /•O 2 − . Doping of excessive metals is detrimental to the separation and transfer of photogenerated charges. The intermediates and mechanism of photocatalytic oxidation of HCHO were investigated by in situ DRIFTS.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Man Yuan,Renzi Yang,Shuoyun Wei,Xiwei Hu,Dan Xu,Jin Yang,Zhengping Dong
Porous organic polymers (POPs) containing nitrogenous substituents have potential practical applications as heterogeneous catalysts based upon controlled porous structure and surface-anchored noble metal nanoparticles (NMNPs). In this work we prepared a POP material from piperazine and cyanuric chloride starting materials (PC-POP). The PC-POP material contains numerous triazinyl moieties, thus rendering the pores hydrophobic. Subsequently, by means of a novel reverse double-solvent approach (RDSA), microdroplets of Pd(AcO) 2 /CH 2 Cl 2 were introduced into the hydrophobic pores of PC-POP in an aqueous environment; Pd(II) was rapidly reduced by NaBH 4 to form ultra-fine Pd NPs and confined within the pores of PC-POP at high dispersity. The extensive porosity and dispersity of the Pd NPs made the active sites readily accessible, and led to efficient mass transfer. Thus, Pd@PC-POP exhibits superior catalytic performance in catalytic reduction of various nitroarenes. Furthermore, Pd@PC-POP has excellent recyclability, without significant loss of activity nor leaching of Pd active sites during 10 successive reaction cycles. This work points to a practical and cost-effective approach to preparation of POP materials, and also for confining ultra-fine NMNPs in POPs for use as catalysts.
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Journal of Materials Chemistry B
·
2018
·Vol. 7
·期 2
·233-239
·
IF 4.776
Wenchi Zhang,Xin Li,Xuechao Xu,Yanfang He,Fengxian Qiu,Jianming Pan,Xiangheng Niu
In this work, we report a novel naked-eye and fluorescent dual-readout glucose sensing platform based on the bifunctional peroxidase mimicking and ON–OFF fluorescence of Pd nanoparticle-decorated graphitic C3N4 nanosheets (PdNPs/g-C3N4). The PdNPs/g-C3N4 hybrid not only exhibited a strong peroxidase-like activity to catalyze colorless o-phenylenediamine (OPD) into its yellow product OPDox in the presence of H2O2, but it also acted as a turn-off fluorescent sensor for the assembly of the generated OPDox on g-C3N4. When coupled with glucose oxidase (GOx), the platform could provide both visual and fluorescent responses for glucose specifically. Under optimal conditions, the platform was able to detect the target at concentrations as low as 50 μM and 0.4 μM in the linear ranges of 50–2000 μM and 1–1000 μM with the naked eye and a fluorometer, respectively. The developed platform integrates the equipment-free merit of naked-eye observation with the excellent performance of fluorometric analysis well, providing a new and powerful tool for both rough assessment and accurate detection of glucose in diabetes management and other applications.
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JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Meng Wang,Xiaoxu Wang,Bo Feng,Yuanhua Li,Xinchen Han,Zijie Lan,Huajun Gu,Huamin Sun,Meng Shi,Hexing Li,Hui Li
Acquisition of chiral amines is a very important item in scientific research. Chemoenzymatic catalyst combination of Pd nanoparticles supported on the external surface of the ethylenediamine-functionalized MIL-101 ( [email protected] ) with layered cross-linked enzyme aggregates of Candida antarctica lipase B (CALB-CLEAs) was established for the first time. This combination served as an ultra-efficient chemoenzymatic catalyst system for one-pot dynamic kinetic resolution (DKR) of rac -1-phenylethylamine leading to optically pure product (>99% ee value) with almost full conversion and excellent selectivity (>99%) without the aid of any additive. Significantly, aliphatic amines can be also efficiently converted to enantiomerically pure products, making this robust and heterogeneous combination one of the most powerful chemoenzymatic platforms for microwave-assisted one-pot DKR of amines available up to now.
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JOURNAL OF MATERIALS SCIENCE
·
2018
·Vol. 53
·期 24
·16263-16275
·
IF 2.993
Li Jiali,Kong Xianggui,Jiang Meihong,Lei Xiaodong
Up to now, although tremendous effort has been made in exploring Pd-based catalysts for the Suzuki–Miyaura coupling reactions, there is still much room to enhance its catalytic performance by synthesis catalyst with define-designed and tailored structure. Herein, a new kind of Pd-based structured catalyst with hierarchical hollow structure (Pd/Co(OH) 2 /Cu(OH) 2 /copper foam) has been successfully synthesized by three facile steps. As framework, the hierarchical hollow nanoarray structure of Co(OH) 2 /Cu(OH) 2 /copper foam is fabricated by immersion and electrolytic deposition methods. Uniformly dispersed Pd nanoparticles with a narrow size distribution (1.5 ± 0.2 nm) are anchored on the surface of the hierarchical nanotube array through an in situ spontaneous redox reaction between Co(OH) 2 and PdCl 4 2− without any surfactant at room temperature. Compared with other synthesis approaches, it just takes less than 1 h for the whole fabrication process in our strategy, exhibiting very high efficiency. In order to evaluate the catalytic performance of the as-prepared structured catalyst, 16 kinds of reagents were chosen as substrates for Suzuki–Miyaura coupling reaction, exhibiting excellent activity and reusability under mild conditions. We hope this simple and efficient method will open a new strategy to design and prepare structured catalysts.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2018
·
IF 5.667
Wenchi Zhang,Xiangheng Niu,Xin Li,Yanfang He,Hongwei Song,Yinxian Peng,Jianming Pan,Fengxian Qiu,Hongli Zhao,Minbo Lan
In analytical science, it is always of great scientific and practical significances to explore convenient, rapid, and reliable methods/devices to trace the H 2 O 2 level in various matrices. Herein, we fabricated a ready-to-use paper-based chemosensor by using mesoporous carbon-dispersed Pd nanoparticles (Pd NPs/meso-C) as a promising peroxidase mimic for the visual determination of H 2 O 2 . Thanks to the large exposed surface of the meso-C support and the highly dispersed active Pd NPs, the synthesized Pd NPs/meso-C exhibited favorable catalytic performance to trigger the chromogenic reaction of colorless TMB to blue TMBox mediated by H 2 O 2 , providing a K cat of 326.67 s −1 for H 2 O 2 and 0.55 s −1 for TMB, larger than the bare Pd NPs and even comparable to the activity of natural horse radish peroxidase. As demonstrated, this principle could be employed to colorimetrically detect H 2 O 2 in the linear scope of 5–300 μM. By simply immobilizing the Pd NPs/meso-C mimic and the TMB substrate onto a common filter paper, ready-to-use paper-based sensors were further prepared. By combining these test strips with a smartphone and an easy-to-access color-scanning APP together, the integrated platform could be used for the quantitative analysis of H 2 O 2 with advantages of simple operation, fast response, low cost, and good selectivity and repeatability. Furthermore, reliable sensing of the target in milk matrices suggested great promise of the integrated platform in practical applications.
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IET Nanobiotechnology
·
2018
·Vol. 12
·期 4
·441-445
·
IF 2.059
Xiaojie Song,Xianyang Shi,Mi Yang
Biosynthesised nanocomposites have attracted growing interests attributed to their ‘green’ synthesis nature in recent years. Shewanella oneidensis MR-1, a dissimilatory metal-reducing bacterium, was used to reduce palladium (II) nitrate to palladium (0) nanoparticles (Pd NPs) under anaerobic conditions, resulting in the in situ formation of Pd NPs immobilised on TiO 2 nanotubes (TNTs) (Pd/TNTs nanocomposites). The Pd/TNTs nanocomposites were characterised by transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, energy dispersive X-ray, and electron spin resonance, respectively. The results indicated that Pd NPs are successfully grown on the TNTs without aggregation. Photocatalytic degradation of methylene blue (MB) by Pd/TNTs nanocomposites under simulated sunlight was also investigated. Pd/TNTs nanocomposites had photocatalytic efficiency superior to that of single TiO 2 nanomaterials. The photocatalytic activity of Pd/TNTs nanocomposites can be enhanced by S. oneidensis MR-1. The results showed that after only 10 min, the degradation ratio of MB reached 98.7% by Pd/TNTs nanocomposites when simultaneously assisted with S. oneidensis MR-1.
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