RSC Advances
·
2026
·Vol. 16
·期 2
·1202-1211
·
IF 4.6
Qiuyun Huang,Shiyu Liu,Weihua Shen,Yunjin Fang
For the carbonylation of methyl nitrite (MN) to dimethyl carbonate (DMC), a series of Ce(x)-UiO-66 were synthesized and utilized as supports for Pd/Ce(x)-UiO-66 catalysts. The characteristics of the carriers were investigated using XRD, SEM, TG, NH3-TPD and BET analyses. The results showed that doping cerium in the UiO-66 significantly enhanced the catalytic activity by improving the surface area, acidity and CO adsorption of the catalysts. Ce(0.1)-UiO-66, with the highest thermal stability (547.26 °C), presented the highest catalytic stability in DMC synthesis. It was proven that the damage of CO and the migration of Pd atoms occurred due to the replacement of ligands and metal clusters, which led to catalytic deactivation.
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CNS Neuroscience & Therapeutics
·
2026
·Vol. 32
·期 2
·e70787
·
IF 6.6
Shengnan Xiao,Lianmei Liu,Xuemei Qin,Lei Xu,Zhenyu Li,Zhi Chai
Cycloastragenol derivatives regulate the TLR4/NF‐κB/TERT signaling pathway and tyrosine metabolism, breaking the vicious cycle of “inflammation‐aging” and improving symptoms of Parkinson's disease. This study provides direction for the application of natural products in the development of PD drugs.
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MOLECULES
·
2023
·Vol. 28
·期 3
·922
·
IF 4.6
Pengcheng Li,Jingjing Zhu,Hongyu Zhang,Lan Wang,Shulin Wang,Mengting Zhang,Jianping Wu,Lirong Yang,Gang Xu
Chiral amines are essential components for many pharmaceuticals and agrochemicals. However, the difficulty in obtaining enantiomerically pure amines limits their application. In this study, hollow amorphous ZIF-90 (HamZIF-90) materials were prepared by template engraving, and chemical–enzyme coupling catalysts (HamZIF-90@Pd@CALB) were constructed for the chiral resolution of 1-phenylethylamine. Different from conventional materials, HamZIF-90 had tunable hollow structures by altering its central node zinc ion concentrations, and the embedded hydrogel template gave it more pore structures, which facilitated the loading of enzyme molecules and Pd nanoparticles (NPs). The establishment of the coupling catalysts shortened the mass transfer distance of the reactant molecules between the metal nanoparticles and the enzyme catalyst in the dynamic kinetic resolution (DKR) reaction, resulting in 98% conversion of 1-phenylethylamine and 93% selectivity of Sel.R-amide. The proposal of this idea provided a good idea for future tailor-made MOFs loaded with chemical and enzyme coupled catalyst.Keywords:hollow amorphous;HamZIF-90@Pd@CALB;DKR;1-phenylethylamine
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CHEMOSPHERE
·
2023
·
IF 8.8
Sini Lv,Fengzhen Zheng,Zeyu Wang,Luyao Dai,Huan Liu,Dzmitry Hrynshpan,Tatsiana Savitskaya,Jun Chen
The high hydrophobicity of n -hexane is the main reason why it is difficult to be removed biologically. In this study, the effects of bamboo-charcoal modified by bimetallic Fe/Pd (BBC) on n -hexane biodegradation by Pseudomonas mendocina NX-1 (PM) was investigated. The n- hexane removal efficiency was increased in the presence of BC. The highest n- hexane removal efficiency at 90.0% was achieved at 0.05 g L −1 BCE and 3 g L −1 NH 4 + under pH 7.7 and 35 °C. Additionally, protein content (45.9 μg mL −1 ) and negative cell surface zeta potential (−26.4 mV) were increased during biodegradation process, with PM-BBC being 43.1 μg mL −1 and 19.1 mV. Bacterial growth was improved and maximum cell surface hydrophobicity was obtained after 20 h, which was 59.4% higher than the control with PM-BBC (37.7%) or PM (16.1%), showing biodegradation products of 1-butanol and acetic acid. The results indicate that BBC improved n- hexane biodegradation efficiency by promoting bacterial growth, reducing cell zeta potential, exposing hydrophobic proteins, and increasing cell surface hydrophobicity of bacterial strain NX-1. This investigation suggests that BBC-enhanced biodegradation can be promising to treat n- hexane-containing gas.
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International Journal of Minerals Metallurgy and Materials
·
2023
·Vol. 30
·期 5
·877-885
·
IF 4.8
Wang Junlian,Liu Lu,Xu Wen,Liu Hui,Xu Guodong,Huang Kun,Yu Fengshan,Huang Guoyong
Platinum group metals (PGMs), especially Pd, Pt, and Rh, have drawn great attention due to their unique features. Direct separation of Pd and Pt from highly acidic automobile catalyst leach liquors is disturbed by various factors. This work investigates the effect of various parameters including the acidity, extractant concentration, phase ratio A/O, and diluents on the Pd and Pt extraction and their stripping behaviors. The results show that the Pd and Pt are successfully separated from simulated leach liquor of spent automobile catalysts with monothio-Cyanex 272 and trioctylamine (TOA). Monothio-Cyanex 272 shows strong extractability and specific selectivity for Pd, and only one single stage is needed to recover more than 99.9% of Pd, leaving behind all the Pt, Rh, and base metals of Fe, Mg, Ce, Ni, Cu, and Co in the raffinate. The loaded Pd is efficiently stripped by acidic thiourea solutions. TOA shows strong extractability for Pt and Fe at acidity of 6 mol·L −1 HCl. More than 99.9% of Pt and all of the Fe are extracted into the organic phase after two stages of countercurrent extraction. Diluted HCl easily scrubs the loaded base metals (Fe, Cu, and Co). The loaded Pt is efficiently stripped by 1.0 mol·L −1 thiourea and 0.05–0.1 mol·L −1 NaOH solutions. Monothio-Cyanex 272 and TOA can realize the separation of Pd and Pt from highly acidic leach liquor of spent automobile catalysts.
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JOURNAL OF MATERIALS SCIENCE
·
2022
·Vol. 58
·期 1
·170-185
·
IF 4.682
Zang Yu,Gao Shan,Jing Boyu,Sun Hong,Wang Jianjun,Liu Jiao,Miao Fengjuan,Xu Liang
Four kinds of conjugated microporous polymers (CMPs) with imine structures were synthesized by a Sonogashira coupling reaction followed by a postreaction between aldehydes and amines. Palladium nanoparticles (Pd NPs) were successfully supported on the CMPs to prepare Pd/CMP heterogeneous catalysts and were used to catalyze the Suzuki–Miyaura coupling reaction. The number of aromatic nuclei and nitrogen atoms in the CMPs highly affects Pd loading. In the Suzuki–Miyaura coupling reaction, the Pd/CMP with good Pd NPs dispersibility and appropriate Pd content (Pd/CMP-NA) exhibited the highest catalytic efficiency with 100% conversion and 95.4% yield which can be used for many substrates. The Pd/CMP-NA heterogeneous catalyst was easy to recover and still exhibited good catalytic efficiency after 5 cycles. To further understand the catalytic mechanism of Pd/CMP-NA on the Suzuki–Miyaura coupling reaction, we proposed a rational catalytic cycle. This paper provides an idea for the structural design of CMPs used for Suzuki–Miyaura catalytic reaction.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Yaya Fang,Weiwei Lu,Peng Xu,Kaisheng Yao,Jun Zhang,Xuefeng Wei,Shuge Peng,Kunpeng Sun
In this work, we propose a plasmon-mediated method to activate oxygen for oxidizing benzyl alcohols to aldehydes. First, hollow Ag@Pd core–shell nanoparticles were prepared and characterized and afterward explored for selective oxidation of benzyl alcohols under visible light illumination. Then, electron paramagnetic resonance analysis and spectroscopic measurements suggested that the main active species responsible for the selective oxidation was 1O2, which was subsequently proved to be generated from the transformation of superoxide radicals •O2–. The light illumination and the presence of a Pd shell were the prerequisites for the successful generation of •O2– and 1O2. Furthermore, the wavelength-dependent performance of Ag@Pd verified the plasmon-mediated nature of these core–shell-type nanocatalysts. Finally, a plausible mechanism of plasmonic activation of oxygen and selective oxidation of benzyl alcohols on Ag@Pd was proposed. Our research opens a green and sustainable way to activate molecular O2 into 1O2 for selective oxidation.
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Frontiers in Oncology
·
2022
·
IF 5.738
Da-Lai Xu,Yuan-Qing He,Bin Xiao,Yuan Si,Jian Shi,Xue-Ang Liu,Lei Tian,Qian Ren,Ya-Song Wu,Yi Zhu
Pancreatic ductal adenocarcinoma (PDAC) is a highly aggressive and lethal malignancy with a limited response to current therapies. Novel and effective treatment is urgently needed. Herein, a chimeric antigen receptor (CAR)-NK92 cell line, with an interleukin (IL)-15Rα-sushi/IL-15 complex and a Programmed cell death-1(PD1) signal inverter was constructed and named SP (
S
ushi-IL15-
P
D1). We showed that CAR expression enabled SP cells to proliferate independently of IL-2 and became more resistant to nutrition starvation-induced apoptosis. Meanwhile, SP cells were more effective than NK92 in PDAC cell killing assays in vitro and in vivo, and there was a positive correlation between the killing capability of SP cells and PD-L1 expression in pancreatic cancer cells. Based on the synergistic and comprehensive effects of the special CAR structure, the adhesion, responsiveness, degranulation efficiency, targeted delivery of cytotoxic granule content, and cytotoxicity of SP cells were significantly stronger than those of NK92. In conclusion, the SP cell line is a promising adoptive immunotherapy cell line and has potential value as an adjuvant treatment for pancreatic cancer, especially in patients with high PD-L1 expression.Keywords: pancreatic ductal adenocarcinoma, Chimeric antigen receptor (CAR), IL-15, IL-15Rα-sushi, programmed cell death ligand 1 (PD-L1), adoptive immunotherapy
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MICROCHEMICAL JOURNAL
·
2022
·
IF 5.304
Jilan Qi,Xiaolei Zhang,Qiangyan Zhang,Ying Xue,Fei Meng,Yuanhua Liu,Gongjun Yang
In this work, a “signal on” electrochemiluminescence (ECL) strategy was proposed to detect Apolipoprotein-A1 (Apo-A1), a common tumor biomarker for bladder cancer. The tris(2,2′-bipyridyl)-ruthenium(II) [Ru(bpy) 3 2+ ] was used as luminophor captured by three-dimensional (3D) zinc oxalate metal–organic frameworks (MOFs), which constructed as the ECL nanoprobe (Ru-MOF) for detecting Apo-A1. Meanwhile, L-cysteine (L-Cys) as the co-reactant was connected to the [email protected] core–shell nanostructure through Au-S bond, which was directly modified on the glassy carbon electrode (GCE) to significantly reduce the electron transfer distance between the luminophor and co-reactant. The ECL intensity was “signal on” when the ECL probe of Ru-MOF was linked to the electrode by the immunoreaction of antigen–antibody. Based on these principles, the quantitative relationship between the concentration of Apo-A1 and the ECL intensity was obtained in the range of 1.00 fg·mL −1 to 1.00 ng·mL −1 with a linear coefficient of 0.9968. The proposed ECL immunosensor showed some great advantages, such as simplification, rapidity, stability and selectivity. It was also successfully applied for the determination of Apo-A1 in real serum and urine samples with the recovery of 98.0% ∼ 115.0% (RSD < 5.2%). To sum up, a “signal on” ECL immunosensor was successfully constructed for Apo-A1 detection, and it may facilitate the diagnosis of bladder cancer in clinic.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Xiaoying Qi,Xiang Gong,Na Ye,Zhao Jiang,Tao Fang
Direct methanol and formic acid fuel cells attracted extensive attention with high specific energy and low operating temperature. The efficient electrocatalyst was one of the important factors to limit their commercial applications. Here, the nitrides-modified Pd/C catalysts (Pd–NbN/C, Pd–Mo 2 N/C, Pd-VN/C and Pd-BN/C) were prepared using sodium citrate as a reducing agent in ethylene glycol solution. The mass activities followed the trend of Pd–NbN/C > Pd–Mo 2 N/C > Pd-VN/C > Pd-BN/C > Pd/C, where Pd–NbN/C exhibited the highest mass activity (4052.19 A g Pd −1 ) for MOR, 19.2 times that of the commercial Pd/C (210.53 A g Pd −1 ). Electrochemical measurements (LSV, Tafel, EIS, CA) indicated that the addition of nitrides increased the charge-transfer kinetics, reaction rate and CO tolerance of catalysts for MOR in alkaline media . The rate-determining step was CO ads oxidation process . Combined the structural analysis (HRTEM, XRD , XPS , ICP) with electrochemical results, the enhanced catalytic performance was ascribed to that higher ECSAs and the charge transfer between Pd and nitrides, leading to the negative shift of the d-band center towards the Fermi level . The linear correlations were found for the d-band center VS the mass activities and the onset potential of CO oxidation VS the d-band center, indicating that the activity and anti-CO poisoning ability could be enhanced by controlling the d-band structure of catalysts for MOR. Furthermore, the higher mass activity for FAOR in acidic media suggested that nitrides-modified Pd/C may be the promising bi-functional materials.
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Advanced Science
·
2022
·Vol. 9
·期 27
·2202744
·
IF 17.521
Songtao Dong,Yuan Zhang,Xiangnan Guo,Chuang Zhang,Zhaomeng Wang,Jiang Yu,Yubo Liu,Chang Li,Yuting Hu,Bingjun Sun,Mengchi Sun,Haotian Zhang,Defang Ouyang,Zhonggui He,Yongjun Wang
Spatiotemporal delivery of nanoparticles (NPs) at the “cellular level” is critical for nanomedicine, which is expected to deliver as much cytotoxic drug into cancer cells as possible when NPs accumulate in tumors. However, macrophages and cancer-associated fibroblasts (CAFs) that are present within tumors limit the efficiency of spatiotemporal delivery. To overcome this limitation, glutathion pulse therapy is designed to promote reduction-sensitive Larotaxel (LTX) prodrug NPs to escape the phagocytosis of macrophages and penetrate through the stromal barrier established by CAFs in the murine triple negative breast cancer model. This therapy improves the penetration of NPs in tumor tissues as well as the accumulation of LTX in cancer cells, and remodels the immunosuppressive microenvironment to synergize PD-1 blockade therapy. More importantly, a method is established that can directly observe the biodistribution of NPs between different cells in vivo to accurately quantify the target drugs accumulated in these cells, thereby advancing the spatiotemporal delivery research of NPs at the “cellular level.”
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APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Longyu Xu,Shuya Hua,Jing Zhou,Yiqi Xu,Chunshan Lu,Feng Feng,Jia Zhao,Xiaoliang Xu,Qingtao Wang,Qunfeng Zhang,Xiaonian Li
Semi-hydrogenation of acetylene is one of the most promising methods to eliminate acetylene from ethylene / acetylene mixtures to avoid Ziegler−Natta polymerization catalysts being poisoned. Given that acetylene is always over-hydrogenated on conventional palladium-based catalyst, it is of great importance to facilitate the desorption of ethylene to enhance the ethylene selectivity. Herein, we report a simple method to anchor Pd by unsaturated penta-coordinated aluminum (Al 3+ penta ) on Al 2 O 3 (meso-Al 2 O 3 ). Characterized by 27 Al-NMR, XRD, HR-TEM, CO chemisorption and XPS, Pd/meso-Al 2 O 3 catalyst had a highly dispersion and unique electronic property of Pd, thus exhibiting a high ethylene selectivity (~83%) while the acetylene conversion is > 99%. Besides, the agglomeration of Pd is suppressed by the metal-support interaction (MSI) between Pd and meso-Al 2 O 3 support. Therefore, the preparation method of the catalyst is relatively simple and has certain commercial application prospects.
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