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
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2023
·Vol. 27
·期 10
·2737-2750
·
IF 2.5
Chen DePing,Li Mengjue,Chen Ying,Shao Zhenyi,Wei Yanhong,Xian Yong,Liu Xi Chuan,Ying XianJun
The development of economically viable anode catalysts for the alcohol oxidation reaction (AOR) has been a long-standing challenge in direct alcohol fuel cells (DAFCs). A series of Pd–Ag nanoparticles embedded in mesoporous carbon were fabricated in this study using a green approach that did not require the use of a surfactant, which exhibited better catalytic properties for AOR. Experiments and DFT calculations reveal that the d-band center of Pd is influenced by both strain and ligand effects, with the ligand effect predominating. The electrochemical studies demonstrated that the composite-optimized Pd–Ag alloy at a Pd/Ag molar ratio of 1:1 was the highest in terms of ethanol oxidation (EOR) and ethylene glycol oxidation (EGOR) catalytic activity. The mass activities of Pd 1 Ag 1 /MC for EOR and EGOR were 7921 mA mg −1 and 11,520 mA mg −1 , respectively, which were 3.77 and 5.3 fold greater than Pd/C. The impressive performance of Pd 1 Ag 1 /MC catalyst could be attributed to the vital roles of the unique mesoporous structure of carbon sphere with abundant self-doping defect and the boosting effect of Ag (benefit from optimized d-band electronic structure and bi-functional mechanism). The present simple method of synthesizing low-cost, easy-to-use, and high-performance catalysts contributes to the exploration of the large-scale practical applications of direct alkaline alcohol fuel cells.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Fangxu Shi,Fuxin Liang,Yulin Wei,Junyan Wu,Sai Huang,Honglei Wang,Zhi Wang,Guopu Shi
The hydrogenation-catalyzed synthesis of mirabellone, a drug for the treatment of overactive bladder (OAB), faces the challenge of catalytic efficiency and selectivity regulation of its core intermediate. In this study, we propose an innovative strategy for constructing a Pd/B-Al 2 O 3 composite catalytic system on a foam ceramic substrate using the impregnation method, and systematically investigate the modulation mechanism of different boron doping ratios on the catalyst's performance. Experimental and density functional theory studies demonstrate that the incorporation of boron synergistically enhances surface adsorption of reaction intermediates, facilitates the efficient reduction of PdO, and precisely modulates the distribution of acidic sites, thereby establishing a catalytic environment more favorable for the selective reduction of nitro groups. This catalyst, characterized by its unique three-dimensional pore structure and the interface synergistic effect resulting from boron modification, enables a uniform distribution of catalytically active centers and enhances the efficiency of reaction mass transfer. Through the optimization of process parameters, the yield of the target product was significantly improved, providing an innovative technological path for the preparation of the key intermediate of mirabilon.
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Zhiliang Ma,Chao Xie,YueZhou Wei,Xiangbiao Yin,Caiwu Luo,Shunyan Ning,Qiang Wu,Tianjiao Jiang
The efficient separation and recovery of palladium (Pd) from high-level liquid waste (HLLW) are critical for promoting resource sustainability and advancing the nuclear fuel cycle. In this study, a novel silica-based sorbent (HT-paPBI@SiO 2 ) enriched with nitrogen adsorption sites was synthesized via a polymerization–vacuum impregnation–high-temperature optimization strategy to address the challenges of Pd(II) recovery in highly acidic and ionically complex environments. HT‑paPBI@SiO 2 was systematically characterized using SEM, EDS, TG‑DSC, BET, and FT‑IR analyses, which confirmed its rigid framework, abundant porosity, high loading efficiency, and excellent thermal stability. Static batch adsorption experiments demonstrated that HT‑paPBI@SiO 2 efficiently adsorbs Pd(II) over a broad acidity range (0.1–9 M HNO 3 ). In simulated HLLW at 6 M HNO 3 , the material exhibited outstanding selectivity ( SF Pd/other metal ions > 1.05 × 10 3 ) and a high saturation adsorption capacity of 128.2 ± 1.8 mg/g. Furthermore, the adsorption kinetics fit well with a pseudo‑second‑order model, while the equilibrium data conform to the Langmuir isotherm and van’t Hoff thermodynamic models, indicating a spontaneous, endothermic, monolayer chemical adsorption process. Furthermore, dynamic adsorption experiments successfully achieved the selective recovery of Pd(II) from simulated HLLW, highlighting the potential of HT-paPBI@SiO 2 for industrial-scale applications. Mechanistic investigations, supported by FT-IR, XPS, and DFT calculations, revealed that the benzene ring in paPBI was oxidized to a quinone structure under high-temperature treatment. The electron-rich regions resulting from the interaction of the C=O group in quinone with the C=N − C moiety in imidazole enhance the affinity for Pd(II). This interaction facilitates the coordination of nitrogen and oxygen atoms with Pd(II), while NO 3 − ions coordinate to balance the charge.
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产品关联
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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
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
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
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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高影响因子
ACS Catalysis
·
2019
·
IF 12.221
Xueping Qin,Lulu Zhang,Gui-Liang Xu,Shangqian Zhu,Qi Wang,Meng Gu,Xiaoyi Zhang,Chengjun Sun,Perla B. Balbuena,Khalil Amine,Minhua Shao
Improving the reaction kinetics of hydrogen evolution and oxidation reactions (HER/HOR) in alkaline media is critical to promote the development of alkaline fuel cells and electrolyzers. Here, we prepared Pd3Ru alloy nanocatalysts with Ru segregated on the surfaces, forming adatoms and clusters. This structure dramatically lowered the overpotential of Pd toward HER in 1 M KOH by 104 mV at 10 mA cm–2. The HER activity was even higher than that of Pt (6 mV improvement at 10 mA cm–2). Theoretical simulation results revealed that Ru adatoms/clusters on the surface could weaken the hydrogen-binding energy and promote the OH adsorption, consequently lowering the reaction barrier of the rate-determining step in HER. Our findings are of significance for clarifying the role of Ru in bimetallic catalysts and rational design of more active catalysts for HER/HOR.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Xin-Hao Shen,Feng Liu,Qin-Qin Chen,Ying Gao,Xiao-Wen Wang,Xin Liu
The efficient degradation of emerging pollutants in water, represented by CBZ, is receiving increasing attention from all sectors of society. Although advanced oxidation reactions represented by Fenton reaction can efficiently degrade emerging pollutants, the problem of iron sludge that comes with it is hindering the further promotion of this technology. Herein, UiO-66(Zr)-2OH material was synthesized by hydrothermal method and loaded with Pd 0 NPs on the surface of the material by in situ reduction. The MOFs-H 2 -Accelerated Catalytic Fenton system was constructed by accelerating the regeneration of Fe(II) in the system by activating the [H] produced by H 2 introduced into the system at room temperature and pressure. Within 180 min, the removal of the target pollutant CZB could reach more than 99 % under the condition of only 25 µmol of Fe(II) and 25 mmol of H 2 O 2 .
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高影响因子
危险品化学品经营许可证（带存储）