Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Lin Hu,Xian-Yong Wei,Mei-Ling Xu,Yu-Hong Kang,Xian-Hou Guo,Feng-Bin Zhang,Zhi-Min Zong,Hong-Cun Bai
The selective hydrodeoxygenation (HDO) of lignin-derived bio-oil still meets the great challenges due to its complex oxygenated organic component. In this research, first time, Pd-based zeolite catalysts were prepared by the modified deposition-precipitation (DP) method for the HDO conversion of guaiacol. Notably, for the same Si/Al ratio of zeolite, Pd 2% /Hβ catalyst showed the higher catalytic activity on the HDO of guaiacol than that Pd 2% /M and Pd 2% /HZSM-5 catalyst, which mainly originated from the synergetic effect between metal nanoparticles size and acid sites of catalyst. As one of typical phenolic monomers , guaiacol can be converted into high yield of hydrocarbons under the condition of 220 °C, 3 MPa H 2 , and 4 h in n -hexane over Pd 2% /Hβ (DP) catalyst. This highly active catalyst exhibited the good recyclability in the HDO conversion of guaiacol. In addition, other typical phenolic monomers can be converted into high yield of hydrocarbons over this highly active catalyst. Considering this, after HDO upgrading, real lignin oil (RLO) can be converted into high yield of hydrocarbons with the carbon number (CN) in range of C7-C15. This work highlighted that the depolymerization monomers from lignin can be further upgraded by this high active catalyst through HDO to obtain jet hydrocarbons fuel .
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EUROPEAN JOURNAL OF PHARMACEUTICAL SCIENCES
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2021
·
IF 4.384
Min Zhang,Zhou Fang,Haitao Zhang,Mingxiao Cui,Mingfu Wang,Kehai Liu
In order to reverse tumor immunosuppressive microenvironment and improve antitumor immune effect based on immune checkpoint blocking, a mannose-modified liposome-based CpG ODNs and PD-L1 antagonistic peptides (P) co-delivery system (HA/M-Lipo CpG-P) was constructed, in which hyaluronic acid (HA) coating was supposed to improve the systemic circulation stability and thereby promote its accumulation in tumor tissues. When the HA/M-Lipo CpG-P complexes enter the tumor tissues, HA will be hydrolyzed under the action of hyaluronidase, exposing P peptides. Then, P peptides linked by octapeptides that can be cleaved by matrix metalloproteinases (MMPs) are released into tumor tissues under the action of MMPs, exerting a blocking effect in the PD-1/PD-L1 pathway. The M-Lipo CpG complexes can recognize macrophage surface mannose receptors through its surface modified mannose molecules, and promote the intracellular delivery of CpG ODNs, thereby activating macrophages. The results showed that HA/M-Lipo CpG-P complexes successfully reversed M2-type macrophages in tumor microenvironment (TME) to M1, thereby activating anti-tumor related immune cells and inhibiting tumor growth. Moreover, the HA/M-Lipo CpG-P complexes showed a better tumor inhibitory effect than the HA/M-Lipo CpG or the HA/M-Lipo-P (monotherapy) treatment groups. Overall, HA/M-Lipo CpG-P complexes provide a promising co-delivery strategy for targeting tumors to improve the antitumor effect based on immune checkpoint blockade.
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高影响因子
Frontiers in Oncology
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2021
·
IF 6.244
Yang Jianru,Jia Yang,Wang Bing,Yang Shengrong,Du Kun,Luo Yujie,Li Yunhe,Zhu Bing
Background: The effects of up-regulated CircCHST15 on lung cancer remained unclear. In this study, the role of CircCHST15 in lung cancer was investigated.Methods: Dual-luciferase reporter verified the bioinformatics prediction that CircCHST15 targeted miR-155-5p and miR-194-5p. The correlation between CircCHST15 and PD-L1 was analyzed by Pearson analysis. CCK-8 and colony formation was performed to determine the viability and proliferation of lung cancer cells. After the lung cancer (subcutaneous-xenotransplant) model was established in mice, the T cell subtype and related cytokines in mouse tumor tissues were detected by flow cytometry and ELISA. Moreover, the expressions of CircCHST15, miR-155-5p, miR-194-5p, immune-related, and proliferation-related factors of the lung cancer cells or mice tumor tissues were detected by immunohistochemistry, RT-qPCR, or Western blot.Results: CircCHST15 and PD-L1 were high-expressed in lung cancer, and the two was positively correlated. CircCHST15 targeted miR-155-5p and miR-194-5p, the later further targeted PD-L1. Lung cancer cell viability and proliferation were increased by miR-155-5p and inhibited by miR-194-5p. CircCHST15 located in the cytoplasm promoted tumor growth, down-regulated the expressions of miR-155-5p and miR-194-5p, and up-regulated the expressions of PD-L1, Ki-67, PCNA, CCL17, CCL22, IFN-γ, TNF-β, and IL-10. Also, CircCHST15 decreased the CD8+ cells in mouse blood and tumor, but increased the Tregs in mouse tumor. PD-L1 inhibitor showed an opposite effect to CircCHST15 on mouse tumors.Conclusion: CircCHST15 sponged miR-155-5p and miR-194-5p to promote the PD-L1-mediated immune escape of lung cancer cells.
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RSC Advances
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2020
·Vol. 11
·期 1
·48-56
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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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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Xiqiang Tian,Muhammad Zahid,Wang Sun,Yujun Zhu
TiO 2 with different morphology as supports can lead to different surface properties and catalytic activities of catalysts. Herein, we reported a novel facile evaporation-induced assisted hydrothermal approach to synthesize three-dimensional hierarchical structure TiO 2 assembled from needle flakes by using Brij-35 as the morphology-directing agent. The morphology of the prepared TiO 2 from flower-like (TiO 2 -FT), sea urchin-like (TiO 2 -SUT), to ball-like (TiO 2 -BT), as well as the size of needle flakes, were controlled by adjusting the amount of Brij-35. These TiO 2 supported palladium catalysts were facilely prepared using a green bio-reductive method with Catalpa Fruit extract as reducing agent, where they showed remarkable catalytic activity in selective hydrogenation of 4-nitrophenol by sodium borohydride. Especially, 1 wt%Pd/TiO 2 -SUT with sea urchin-like exhibited higher reaction rate constant (1.44 min −1 ) than 1 wt%Pd/TiO 2 -FT (1.08 min −1 ) and 1 wt%Pd/TiO 2 -BT (0.72 min −1 ). Furthermore, XRD, N 2 adsorption–desorption, SEM, TEM, CO-FTIR, XPS and CO chemisorption measurements were performed to study the effects of different surface morphologies on the surface properties of catalysts. It reveals that the high catalytic performance of 1 wt%Pd/TiO 2 -SUT can be attributed to its specific hierarchical structure and much higher surface area, improving the uniform dispersion of Pd nanoparticles on the support to expose extra active surface Pd atoms (Pd 0 species) over 1 wt%Pd/TiO 2 -SUT.
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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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JOURNAL OF CATALYSIS
·
2019
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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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Catalysts
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2019
·Vol. 9
·期 4
·387
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IF 3.444
Bei Wang,Liu Tao,Yu Cheng,Fang Yang,Yuguang Jin,Chunmei Zhou,Hao Yu,Yanhui Yang
The direct alcohol fuel cell is a kind of power generation device that directly converts the chemical energy of small molecule alcohols into electric energy. In this paper, the electro-oxidation behaviors of some typical alcohols (methanol, ethanol, ethylene glycol, n-propanol, 2-propanol, and glycerol) over Pt, Pd, and Au electrodes were investigated in acidic, neutral, and alkaline media, respectively. By analyzing the activity information from a cyclic voltammetry (CV) method and some dynamic tests, several regularities were revealed in those electro-oxidation behaviors. Firstly, alkaline media is the best for the electro-oxidation of all these alcohols over Pt, Pd, and Au catalysts. Secondly, the hydrogen bond donation abilities (HBD) of different alcohols were found have a great relationship with the catalytic performance. In alkaline media, on Pt electrodes, the solute HBD is positively correlated with the ease of electrooxidation within the scope of this experiment. Contrarily, it is negatively correlated on Pd and Au electrodes. Additionally, for Pt catalysts in acidic and neutral media, the relationship becomes negative again as the HBD increases. Finally, the alcohol’s molecular structure properties were found to have a remarkably influence on the activity of different catalysts. Over the Pt electrode in alkaline media, the activation energy of methanol oxidation is 44.1 KJ/mol, and is obviously lower than the oxidation of other alcohols. Under similar conditions, the lowest activation energy was measured in the oxidation of n-propanol (14.4 KJ/mol) over the Pd electrode, and in the oxidation of glycerol (42.2 KJ/mol) over the Au electrode. Totally, among all these electrodes, Pt electrodes showed the best activities on the oxidation of C1 alcohol, Pd electrodes were more active on the oxidation of C2-3 monobasic alcohols, and Au electrodes were more active on the oxidation of polybasic alcohols.Keywords:DAFCs;electro-oxidation;gold;palladium;platinum
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JOURNAL OF MATERIALS SCIENCE
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2018
·Vol. 53
·期 24
·16263-16275
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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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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 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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SEPARATION SCIENCE AND TECHNOLOGY
·
2018
·
IF 1.2
Yan Yan,Qi Wang,Zeyang Xiang,Yanzhao Yang
A reasonable project was presented for the extraction and separation of Pt(IV), Pd(II), Ru(III), and Rh(III) from the mixed imidazolium-based ionic liquids (ILs) [C6mim]Cl, [C6mim][NTf2], and [C6mim][DDTC]. Pt(IV) was first separated from other three platinum group metals with a mixture of [C6mim]Cl and [C6mim][NTf2]. Then, separation of Pd(II) and Ru(III) from Rh(III) was realized by changing the concentration of [C6mim][DDTC]. Back-extraction of Pt(IV), Pd(II), and Ru(III) from loaded hydrophobic phase and the recovery of Rh(III) in aqueous phase were also investigated. Mechanisms between Pd(II)/Ru(III) and [C6mim][DDTC] were further explored using ultraviolet spectrophotometry (UV-Vis), infrared spectrophotometry (FTIR), the method of continuous variations, ab initio quantum chemical studies, and X-ray crystallographic analysis. The results afford more directions for extracting and separating metals by introducing devisable functionalized group into ILs.
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