Applied Catalysis O: Open
·
2024
·
IF 0
Zhe Zhang,Weiting Xiao,Yufei He,Dianqing Li,Xiaodong Zhao
During the manufacture of Al 2 O 3 , sulfate would be inevitably introduced when aluminum sulfate is used as raw material, but its effect has received little attention. In this work, Al 2 O 3 supports with different sulfate content were synthesized and used to prepare Pd/Al 2 O 3 catalyst. Sulfates in all samples exist as surface sulfate, and would be partially removed during the preparation process. Sulfate existing in Al 2 O 3 supports had little impact on the electric structure of Pd, but would partially block pores and also consume surface hydroxyl groups. As a result, higher sulfate content in support would lead to lower Pd dispersion in catalysts and slower reaction rate towards the hydrogenation of amyl-anthraquinone.
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DOI
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2017
·
IF 4.233
Wenhao Dong,Yipeng Ren,Zhixue Bai,Jun Jiao,Yuan Chen,Bingkai Han,Qiang Chen
An innovative epinephrine sensor was fabricated by integrating tetrahexahedral (THH) Au-Pd core–shell nanocrystals on reduced graphene oxide (rGO) nanosheets . Furthermore, the nanocomposites combined the large specific areas of rGO with the high-index facets and excellent electrocatalytic activity of the THH Au-Pd nanocrystals, and the nanocomposites were an essential adapter for detecting epinephrine. In the present work, transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR) and X-ray diffraction (XRD) were used to identify and characterize these unique nanocomposites, and the results revealed that a unique THH Au-Pd/rGO core–shell nanostructure was synthesized successfully. To further explore the electrochemical behaviors of these nanomaterials at a GC electrode, we applied cyclic voltammetry (CV), differential pulse voltammetry (DPV) and amperometry to study the conductivity and electrocatalytic activity of the proposed sensor, and the results suggested that the sensor based on Au-Pd/rGO presented a lower limit of detection (0.0012 μM at a signal to noise ratio of 3), wide linear detection range (0.001 µM to 1000 µM), and extraordinary selectivity and reproducibility. Moreover, the data showed that the sensor possessed good stability and acceptable accuracy to detect epinephrine in human serum samples. In summary, this work is not only a potential way to manufacture various nonenzymatic sensors but also a significant contribution to further studies in catalysis, cell fuel cells and other relevant applications.
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DOI
高影响因子
ACS Omega
·
2021
·
IF 3.512
Lin-Xi Wan,Shi-Xing Miao,Zhen-Xiang He,Xiaohuan Li,Xian-Li Zhou,Feng Gao
Palladium/BuAd2P efficiently catalyzed the direct α-arylation of ketone in the anti-Alzheimer’s disease drug donepezil, leading to 15 aryldonepezil analogues exhibiting high selective inhibition of acetylcholinesterase (AChE). The cell-based assays revealed that the 3-methylpridinyl analogue (12) shows significantly lower toxicity compared to donepezil and remarkable neuroprotective activity against H2O2-induced damage in SH-SY5Y cells. Docking results of compound 12 also interpreted the possible mechanism of the selective inhibition between AChE and butyrylcholinesterase (BuChE).
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DOI
高影响因子
TETRAHEDRON
·
2024
·
IF 2.1
Zixu Li,Fei Wang,Kai Ma,Chao Fang,Qiang Jia,Changhu Chu
Aryl triflate is a type of facile and readily available compounds, which could be used as an alternative substrate for Suzuki cross coupling. In this manuscript, a novel ppm-Pd-Fe/C catalyst has been developed by reduction of palladium acetate and iron trichloride with aqueous hydrazine in situ and supported on activated charcoal. In combined with Sphos, and metal zinc as additives, this catalyst, with 300 ppm palladium loading, could be applied in the Suzuki cross coupling between aryl triflates with aryl neopentylglycolboronates.
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高影响因子
BIOSENSORS & BIOELECTRONICS
·
2017
·
IF 7.78
Yujie Yu,Chao Yu,Yazhen Niu,Jun Chen,Yilin Zhao,Yuchan Zhang,Rufei Gao,Junlin He
We designed an amplified detection strategy for the sensitive determination of lead ions (Pb 2+ ) based on a target-triggered nuclear acid cleavage of Pb 2+ -specific DNAzyme as a selectivity interface combined with Pd-Pt alloys modified Fe-MOFs (Fe-MOFs/PdPt NPs) hybrids acting as the signal tag. Streptavidin modified reduced graphene oxide-tetraethylene pentamine-gold nanoparticles (rGO-TEPA-Au) served as a sensor platform for immobilizing more DNAzyme. In the presence of Pb 2+ , the substrate DNA strand can be specifically cleaved at the ribonucleotide site by DNAzyme to produce a new single-DNA on the interface. Then, the hairpin DNA with hybrid strand matched by its complement to the single-DNA was employed to modify the Fe-MOFs/PdPt NPs bioconjugates for signal amplification . Fe-MOFs/PdPt NPs catalyze hydrogen peroxide (H 2 O 2 ) to produce the electrochemical signal which was recorded by chronoamperometry . Benefiting from the Pb 2+ -dependent DNAzyme, the proposed method can selectively detect Pb 2+ in the presence of other metal ions . The newly designed biosensor exhibited a good linear relationship ranging from 0.005 to 1000 nmol L −1 with a low detection limit of 2 pM (S/N = 3) for Pb 2+ . This Pb 2+ -dependent DNAzyme based ultrasensitive biosensor showed high sensitivity and selectivity, providing potential application for Pb 2+ detection in naturally contaminated sewage and spiked drinking water samples.
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高影响因子
Catalysts
·
2019
·Vol. 9
·期 2
·114
·
IF 3.444
Ke Yu,Yan Lin,Jinchen Fan,Qiaoxia Li,Penghui Shi,Qunjie Xu,Yulin Min
Ethanol oxidation reaction (EOR) is an important electrode reaction in ethanol fuel cells. However, there are many problems with commercial ethanol oxidation electrocatalysts today, such as poor durability, poor anti-CO poisoning ability, and low selectivity for C–C bond cleavage. Therefore, it is very meaningful to develop a high-performance EOR catalyst. Herein, we designed ternary N, S, and P-doped hollow carbon spheres (C–N,P,S) from polyphosphazene (PCCP) as Pd supports for EOR. Using SiO2spheres as the templates, the PCCP was first coated on the surfaces of SiO2spheres by in situ polymerization. Through high-temperature pyrolysis and hydrofluoric acid-etching, the hollow PCCP has a large surface area and porous structure. After loading Pd nanoparticles (NPs), the Pd/C–N, P, S catalysts with Pd NPs decorated on the surfaces of C–N, P, S can achieve a high mass peak current density of 1686 mA mgPd−1, which was 2.8 times greater than that of Pd/C. Meanwhile, the Pd/C–N, P, S catalyst also shows a better stability than that of Pd/C after a durability test of 3600s.
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高影响因子
HELVETICA CHIMICA ACTA
·
2023
·Vol. 106
·期 5
·e202200203
·
IF 1.8
Peng Liu,Xin Zhang,Yuan-Yuan Huang,Geng-Wei Liu,Chen-Jie Li,Pin-Mei Yan,Ye-Yan Qin,Rong Guo,Si-Qi Wu,Yun-Yun Zeng,Peng-Bin Pan,Yuan-Gen Yao
High active Pd-based catalyst with low loading capacity for CO oxidative coupling with methyl nitrite (MN) to dimethyl oxalate (DMO) has aroused great interest in the large-scale production of DMO for the next hydrogenation to bring forth ethylene glycol (EG). Here, spinel composite oxide support, namely MgAl 2 O 4 , had been prepared through three different methods: solid combustion method (MAO-SC), hydrothermal method (MAO-HT) and co-precipitation method (MAO-CP), and further Pd nanoparticles were anchored to the surface of MgAl 2 O 4 through a simple wetness impregnation method. In the CO direct esterification to DMO reaction, the Pd/MAO-SC catalyst, which used MgAl 2 O 4 support prepared by solid combustion method, exhibited the highest intrinsic activity with Turnover frequency (TOF) value of 2.39 s −1 and DMO weight space-time yield (956.8 g⋅kg cat −1 ⋅h −1 ) with 44.1 % CO conversion and 97.8 % DMO selectivity, and showed negligible attenuation of activity during the process of continuous reaction for 100 h. The characterization results confirmed that abundant oxygen defect sites occurred in MAO-SC synthesized by combustion method not only can help to anchor the Pd nanoparticles with appropriate size and dispersion, but also can promote the interfacial electron transfer from MgAl 2 O 4 support to Pd nanoparticles, thus significantly enhancing the metal-support interaction (MSI) and providing more CO bridge-adsorption sites that is favorable for the CO oxidative coupling with MN to DMO reaction.
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高影响因子
BIORESOURCE TECHNOLOGY
·
2021
·
IF 9.642
Zeyu Wang,Luyao Dai,Jiachao Yao,Tianjiao Guo,Dzmitry Hrynsphan,Savitskaya Tatsiana,Jun Chen
Aiming at the accumulation of NO 2 − -N and N 2 O during denitrification process, this work focused to improve the denitrification performance by Pd-Fe embedded multi-walled carbon nanotubes (MWCNTs). The main conclusions were as follows: 30 mg/L Pd-Fe/MWCNTs have shown an excellent promotion on denitrification (completely TN removal at 36 h). Meanwhile, enzyme activity results indicated that the generation of NO 2 − -N, NH 4 + -N by Pd-Fe/MWCNTs led the occur of short-cut denitrification by increasing 203.9% the nitrite reductase activity. Furthermore, electrochemical results and index correlation analysis confirmed that the electron exchange capacity (1.401 mmol eg −1 ) of Pd-Fe/MWCNTs was positively related to nitrite reductase activity, indicating its crucial role in electron transport activity (0.46 μg O 2 /(protein·min) at 24 h) during denitrification process by Pd-Fe/MWCNTs played a role of chemical reductant and redox mediator.
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Qi Ge,Haitao Yu,Li Zhang,Shujing Ni,Wenjin Wu,Han Yang,Jiakang Liu,Kun Huang
In this study, a facile method was developed to synthesize honeycomb-like nitrogen-doped porous carbon nanospheres encapsulated ultrafine Pd nanoparticles (Pd/H-NPCNs) by a combination of one-step Friedel-Crafts reaction between carbazole and benzylamine monomers and subsequent in-situ impregnation-pyrolysis reduction strategy. The obtained Pd/H-NPCNs are further treated with H 2 O 2 to remove carbon layer from the surface of metal to produce Pd/H-NPCNs-H 2 O 2 catalyst. Owing to the high surface area, hierarchically porous structure and special honeycomb-like morphology, the Pd/H-NPCNs-H 2 O 2 catalyst shows the excellent catalytic performance in the selective hydrogenation of cinnamaldehyde (CAL) under mild reaction conditions and water as a green solvent.
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高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 22
·期 11
·6222-6230
·
IF 3.43
Xiao Yan,Yafei Luo,Wei Liu,Li Liang,Ya Gan,Zhongzhu Chen,Zhigang Xu,Hua Wan,Dianyong Tang,Hubing Shi,Jianping Hu
Unveiling the reaction mechanism is significant for developing high-performance catalysts. In this paper, a series of precisely controlled PdxM147−x (M = Cu, Pt, Au, Rh, Ru) dendrimer encapsulated nanoparticles (DENs) has been successfully synthesized. The mechanisms of PdxM147−x as catalysts for Suzuki cross-coupling reactions were investigated by combining experimental and theoretical methods. The experimental results indicate that Pd74Cu73 DEN shows similar activity to Pd147 DEN and excellent substrate adaptability under mild reaction conditions. Moreover, the Cu component can play an important role in tuning the catalytic activity of PdxCu147−x DEN. Density functional theory (DFT) calculations illustrate that the similar activities of the Pd147 and Pd74Cu73 DENs originate from the comparable energy barriers of the rate-determining steps. The partial density of states (PDOS) and electron density differences demonstrate that Cu decreases the intensities of the valence orbitals of the top and edge Pd atoms and weakens orbital interactions between the intermediates and Pd74Cu73 DEN, leading to low desorption energies of the products. This work can provide a promising strategy to reduce the cost of Pd catalysts in Suzuki cross-coupling reactions.
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产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2024
·
IF 3.7
Junbo Feng,Junyan Wu,Dongdong Yan,Yadong Zhang
Porous silica nano-flowers (KCC-1) immobilized Pt-Pd alloy NPs (Pt-Pd/KCC-1) with different mass ratios of Pd and Pt were successfully prepared by a facile in situ one-step reduction, using hydrazinium hydroxide as a reducing agent. The as-synthesized silica nanospheres possess radial fibers with a distance of 15nm, exhibiting a high specific surface area (443.56 m 2 ·g –1 ). Meanwhile, the obtained Pt-Pd alloy NPs are uniformly dispersed on the silica surface with a metallic particle size of 4–6 nm, which exist as metallic Pd and Pt on the surface of monodisperse KCC-1, showing the transfer of electrons from Pd to Pt. The as-synthesized 2.5%Pt-2.5%Pd/KCC-1 exhibited excellent catalytic activity and stability for the continuous dehydrogenation of 2-methoxycyclohexanol to prepare guaiacol. Compared with Pt or Pd single metal supported catalysts, the obtained 2.5%Pt-2.5%Pd/KCC-1 shows 97.2% conversion rate of 2-methoxycyclohexanol and 76.8% selectivity for guaiacol, which attributed to the significant synergistic effect of bimetallic Pt-Pd alloy NPs. Furthermore, turn over frequency value of the obtained 2.5%Pt-2.5%Pd/KCC-1 NPs achieved 4.36 s –1 , showing higher catalytic efficiency than other two monometallic catalysts. Reaction pathways of dehydro-aromatization of 2-methoxycyclohexanol over the obtained catalyst are proposed. Consequently, the obtained 2.5%Pt-2.5%Pd/KCC-1 NPs prove their potential in the dehydrogenation of 2-methoxycyclohexanol, while the kinetics and mechanistic study of the dehydrogenation reaction over the catalyst in a continuous fixed-bed reactor may provide valuable information for the development of green, outstanding and powerful synthetic pathway of guaiacol.
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高影响因子
Acta Biomaterialia
·
2025
·
IF 9.6
Yue Hu,Xi He,Ping Chen,Xiao-Li Tian,Rong Wang,Xiangrong Song,Xiao-Qi Yu,Ji Zhang
mRNA-based protein replacement therapy has become one of the most widely applied forms of mRNA therapy, with lipid nanoparticles (LNPs) being extensively studied as efficient delivery platforms for mRNA. However, existing LNPs tend to accumulate in the liver or kidneys after intravenous injection, highlighting the need to develop vectors capable of targeting specific organs. In this study, we synthesized a small library of ionizable lipids and identified PPz-2R 1 as a promising candidate, exhibiting lung-targeting capabilities, high mRNA transfection efficiency, and good stability through structure-activity relationship studies. In an in situ lung cancer model with PTEN deletion, precise delivery of PTEN mRNA to the lungs restored the cancer-suppressing function of the PTEN protein and successfully alleviated the immunosuppressive tumor microenvironment in the lungs by modulating immune cell activity and cytokine levels. Additionally, the upregulation of PD-L1 expression at the tumor site was triggered. Building on this, in vivo treatment with PTEN mRNA combined with anti-PD-1 therapy was tested in tumor-bearing mice. The results demonstrated that the combined treatment strategy effectively overcame immune escape, promoted T cell infiltration, improved survival rates over 60 days, and significantly inhibited tumor growth. Furthermore, the combination treatment was more effective than either therapy alone. This study presents an effective and practical strategy for the targeted treatment of lung diseases and relevant combination therapies. Statement of significance Lipid nanoparticles (LNPs) have been extensively studied as efficient delivery vectors for mRNA. However, it remains essential to develop vectors that can specifically target distinct organs. In this study, we designed and synthesized a series of piperazine-containing ionizable lipids and their analogues, which were initially explored as lung-targeting vectors for PTEN mRNA delivery. Through screening in both in vitro and in vivo experiments, we found that the leading LNPs-assisted PTEN mRNA-mediated protein supplementation therapy effectively downregulated Treg expression and activated immune cells, thereby reversing the immunosuppressive tumor microenvironment in a mouse model of lung cancer. Furthermore, when combined with anti-PD-1-mediated immunotherapy, the combination therapy exhibited the strongest tumor growth inhibition. This approach offers a novel strategy for the targeted treatment of lung diseases and associated combination therapies.
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PubMed
高影响因子
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