JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2019
·
IF 6.361
Yi Liu,Xiao-Chen Ma,Gang-Gang Chang,Shan-Chao Ke,Tao Xia,Zhi-Yi Hu,Xiao-Yu Yang
The development of a suitable catalytic system in the single catalyst has always been the pursuit for synthetic chemists in order to perform the traditional stepwise reactions in one-pot mode. In this work, an ultra-stable bifunctional catalyst of Pd@MIL-101-SO 3 H was successfully constructed and applied in the one-pot oxidation-acetalization reaction whose products have been widely utilized as fuel additives , perfumes, pharmaceuticals and polymer chemistry . The excellent catalytic performance (>99% yields), on the one hand, can be ascribed to the synergistic effects of Pd NPs with both Lewis and Bronsted acid encapsulated within a sulfonated MIL-101(Cr). On the other hand, the exceptionally high capacity of water adsorption in MIL-101(Cr) could promote the equilibrium movement via interrupting the reversible process. More importantly, Pd@MIL-101-SO 3 H is recyclable and can be reused for at least 8 times without sacrificing its catalytic activities. As far as we know, this is the first time that a water adsorption enhanced equilibrium movement of reversible reaction by porous catalyst to achieve high yields has been realized in Pd@MIL-101-SO 3 H, which may provide an absolutely new and efficient strategy especially for designing reaction-oriented catalysts.
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SPECTROCHIMICA ACTA PART B-ATOMIC SPECTROSCOPY
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2014
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IF 3.15
Xiaolan Liu,Man He,Beibei Chen,Bin Hu
A novel method based on on-line polymer monolithic capillary microextraction (CME)-inductively coupled plasma mass spectrometry (ICP-MS) was developed for the determination of trace Au and Pd in biological samples. For this purpose, poly(glycidyl methacrylate-ethylene dimethacrylate) monolith was prepared and functionalized with mercapto groups. The prepared monolith exhibited good selectivity to Au and Pd, and good resistance to strong acid with a long life span. Factors affecting the extraction efficiency of CME, such as sample acidity, sample flow rate , eluent conditions and coexisting ion interference were investigated in detail. Under the optimal conditions, the limits of detection (LODs, 3σ) were 5.9 ng L − 1 for Au and 8.3 ng L − 1 for Pd, and the relative standard deviations (RSDs, c = 50 ng L −1 , n = 7) were 6.5% for Au and 1.1% for Pd, respectively. The developed method was successfully applied to the determination of Au and Pd in human urine and serum samples with the recovery in the range of 84–118% for spiked samples. The developed on-line polymer monolithic CME-ICP-MS method has the advantages of rapidity, simplicity, low sample/reagent consumption, high sensitivity and is suitable for the determination of trace Au and Pd in biological samples with limited amount available and complex matrix.
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INORGANICA CHIMICA ACTA
·
2024
·
IF 2.7
Jie Cao,Gang Xiong,Zhixiong Luo,Qiuyan Huang,Wenyan Zhou,Ileana Dragutan,Valerian Dragutan,Yaguang Sun,Fu Ding
An amide functionlized bidentate NHC-Pd complex was successfully prepared by a facile solvothermal methodology from a bridged bis-benzimidazolium chloride and K 2 PdCl 4. The new bidentate NHC-Pd complex has been effectively applied as catalyst in Suzuki-Miyaura cross-coupling reactions of aryl halides with arylboronic acids in distilled water (yields up to 99.0%). The bridged bis-benzimidazolium ligand from the Pd complex, bearing the amide functional groups on the nitrogen atom, showed to distinctly influence the electronic and steric effects on the catalytic process. The potential of application of the new NHC-Pd catalyst in diverse C C bond forming processes, working under environmentally friendly conditions, is further outlined.
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Nanoscale
·
2018
·Vol. 10
·期 26
·12487-12496
·
IF 7.233
Haichao Duan,Yu Yang,Jianhua Lü,Changli Lü
Well-dispersed ultrafine palladium nanoparticles supported by reduced graphene oxide functionalized with catechol-terminated thermo-responsive block copolymer (PdNPs@BPrGO) were successfully constructed for highly efficient heterogeneous catalytic reduction. We first synthesized a novel temperature-responsive episulfide-containing double-hydrophilic diblock copolymer, poly(poly(ethylene glycol) methyl ether methacrylate-co-2,3-epithiopropyl methacrylate)-block-poly(N-isopropylacrylamide) (P(PEGMA-co-ETMA)-b-PNIPAM), through a reversible addition–fragmentation chain transfer (RAFT) polymerization utilizing a chain-transfer agent with a catechol unit as the end group. The obtained block copolymers can be facilely anchored to the surface of GO via mussel-inspired chemistry. The PdNPs were loaded on GO decorated with block copolymer brushes (BPrGO) as a support via the in situ reduction of palladium precursors with the episulfide ligands of the block copolymer as a stabilizer. The resulting PdNPs@BPrGO nanohybrid catalyst had good water dispersibility and stability. Furthermore, a low dosage of PdNPs@BPrGO catalyst exhibited excellent catalytic performance in the reduction of methylene blue and nitrophenols. The performance was attributed to the ability of PdNPs@BPrGO to facilitate the diffusion of reactants compared to PdNPs@GO without polymer modification. PdNPs@BPrGO also possessed an interesting temperature-responsive catalytic property due to the reversible “coil-to-globule” phase transition behaviour of PNIPAM blocks onto the surface of catalyst. The PdNPs@BPrGO catalyst was successfully recovered and reused five times without any detectible loss in catalytic activity, demonstrating its great potential in a wide range of industrial catalytic applications.
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Russian Journal of Physical Chemistry A
·
2022
·Vol. 96
·期 9
·1944-1950
·
IF 0.791
Zhang Yuanyang,Bao Kun,Wang Xuchao,Wang Linqi
Abstract A series of Ru and Ru–Pd supported samples on deep desulfurization, especially thiophene-like compounds, were prepared by wet impregnation method. It indicated that the suitable Ru content on the support could be 1.5 wt % (Ru(1.5)/Al 2 O 3 ) under used experimental conditions. The effects of Pd on Ru(1.5)/Al 2 O 3 sample showed that the suitable content of Pd was probably 0.3 wt % (Ru(1.5)–Pd(0.3)/Al 2 O 3 ), and its breakthrough sulfur capacity could be reached to 1.244 g S /kg Cat . XPS and SEM characterization over fresh and used samples of Ru(1.5)–Pd(0.3)/Al 2 O 3 indicated that it had good stable structure. Furthermore, it indicated that the adsorption isotherm model of Freundlich equation was well fitted the experimental data ( R 2 = 0.989) and the parameters of Freundlich equation were obtained by linear regression.
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ELECTROCHIMICA ACTA
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2018
·
IF 5.116
Dong Li,Tianyi Sun,Lu Wang,Na Wang
To improve the electro-catalytic degradation efficiency of the cathode in electrochemical advanced oxidation processes , MnO 2 modified Nano-graphite (MnO 2 /Nano-G) and Pd loaded Foam-Ni (Foam-Ni/Pd) composites were prepared by the chemical redox and electro-deposition methods, respectively, and a two-layer type MnO 2 /Nano-G|Foam-Ni/Pd composite cathode was prepared with the chitosan as a binder. The composites were characterized by X-ray diffraction, scanning electrons microscopy and X-ray photoelectron spectroscopy. Results showed that the mix-crystal structural MnO 2 (α-MnO 2 and γ-MnO 2 ) nanorods with length of 80–200 nm and width of 20–50 nm were uniformly loaded on the Nano-G surface, and the three-dimensional Pd° metal trees/crystals were tightly deposited on the Foam-Ni substrate. The as-prepared cathode was applied to the electro-catalytic degradation of phenol wastewater, and the reaction parameters were optimized. Compared with MnO 2 /Nano-G|Foam-Ni and Nano-G|Foam-Ni cathodes, the degradation efficiency of phenol by MnO 2 /Nano-G|Foam-Ni/Pd cathode was significantly improved. The removal efficiencies of phenol and total organic carbon (TOC) by MnO 2 /Nano-G|Foam-Ni/Pd cathode reached 98.7% and 85.3% after 120 min electrolysis under oxygen aeration condition, respectively. The optimal reaction parameters were current density of 39 mA cm −2 , electrolyte (Na 2 SO 4 ) concentration of 0.1 mol L −1 , electrode distance of 4 cm and initial pH of 7. By determining the variations of H 2 O 2 and OH content in the cathode chamber, it was found that Pd metal crystals improved the reduction of O 2 to H 2 O 2 and MnO 2 nanorods accelerated the dissociation of H 2 O 2 to OH, producing more H 2 O 2 and OH to oxidize phenol and eliminate TOC in wastewater. The results in this study provide useful information for the control of refractory organic pollutants with electrochemical advanced oxidation in wastewater treatment .
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HELVETICA CHIMICA ACTA
·
2022
·Vol. 105
·期 6
·e202200017
·
IF 2.201
Geng-Wei Liu,Peng-Bin Pan,Xin Zhang,Yuan-Yuan Huang,Peng Liu,Ye-Yan Qin,Yuan-Gen Yao
Zinc titanate (ZnTiO 3 ) has recently been applied in various areas for its unique properties. Herein, through tuning the phase structures of ZnTiO 3 support, we synthesized two different Pd-based catalysts for CO oxidative coupling to DMO and further investigated their structure-activity relationships for the first time. The results indicated that the strong metal-support interaction between the cubic phase ZnTiO 3 and Pd species leads to an enriched Pd electronic density and promotes the bridged CO adsorption. As a result, the as-synthesized catalyst with cubic phase ZnTiO 3 performed a turnover frequency (TOF) of 339.3 min −1 , which was much higher than the hexagonal one (226.3 min −1 ).
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Materials Science & Engineering C-Materials for Biological Applications
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2019
·
IF 4.959
Cong Zhang,Jujie Ren,Yifei Xing,Min Cui,Na Li,Peng Liu,Xiaofang Wen,Meng Li
In this work, PdNPs@ZnO-Co 3 O 4 was synthesized via the facile oxidation treatment of bimetallic ZnCo-zeolitic-imidazolate-framework (ZnCo-ZIF) followed by in situ chemical reduction of PdNPs on the surface of the nanocrystals. After combined with MWCNTs, the PdNPs@ZnO-Co 3 O 4 -MWCNTs nanocomposites were formed, which were then exploited as novel electrode materials to construct the non-enzyme electrochemical sensors for high-sensitivity detection of tanshinol. Due to the high catalytic activity of multi-metallic PdNPs@ZnO-Co 3 O 4 , and the excellent charge transfer property between imidazole groups of the ligands in MOFs and MWCNTs, the obtained sensor exhibited high sensitivity for tanshinol detection under optimum experimental conditions. The sensor shows two well linear relationship between the current and tanshinol concentration in the range of 0.002–0.69 mM (R 2 = 0.989) and 0.69–3.75 mM (R 2 = 0.994) with the corresponding sensitivity of 59.16 μA mM − 1 and 19.08 μA mM − 1 . And the limit of detection (LOD) was calculated to be 0.019 μM (S/N = 3). Furthermore, with the advantages of good repeatability, stability and selectivity, the fabricated sensor can be successfully applied to measurement of tanshinol in real medicinal liquids samples. Our results would accelerate the applications of MOFs in electrochemical field and provide insights into design of multifunctional non-enzyme sensing materials for various applications in biocatalysis, bioanalysis and drug testing.
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Journal of Cleaner Production
·
2020
·
IF 7.246
Hao Yin,Jie Zhao,Yuqi Li,Liulian Huang,Hui Zhang,Lihui Chen
A multifunctional and flexible Pd decorated Polydopamine-SiO 2 /PVA electrospun nanofiber membrane was developed by a facile, green, one-step reduction and fixation strategy for simultaneously removal of multiple pollutants from water. Pd NPs were reduced in a mild and green environment with the deposition of dopamine, avoiding secondary pollution of water. The in situ reduced Pd NPs were evenly distributed and firmly immobilized on the nanofiber membrane, effectively avoids the aggregation, thereby greatly improving the catalytic activity . After a single filtration, the developed membrane can simultaneously remove oils, organic chemicals and dyes from water with a high flux (up to 8000 L m −2 ·h −1 ). The removal efficiency for organic chemicals and oils can reach to 99.9% and the degradation efficiency for dyes (e.g., MB and CR) are also very high, up to 99%. More interestingly, the membrane showed robust mechanical properties and corrosion resistance , that can be used in acidic, alkaline, salty and even hot water environment. Besides, the membrane can be reused for at least 10 separation cycles without a significant reduction in separation efficiency, demonstrating excellent reusability and stability.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Qunfeng Chen,Daobin Tang,Qi Zhang,Zhiyuan Tang,Longlong Ma,Xinghua Zhang
Electron-metal support interactions (EMSI), which can tailor the microenvironment through electron transfer and coordination structure design, are an effective strategy to augment the intrinsic catalytic activity of catalysts. However, it remains challenging to establish the interfacial structure and interfacial electron configuration of catalysts to precisely regulate and enhance EMSI. In this work, the spatially defective sites and specific electronic states of Pd-UiO-66 were modified by in-situ constructing a W-O-Zr interface to strengthen the EMSI between Pd nanoparticles (Pd NPs) and UiO-66 support via implanting W into the defective Pd-UiO-66, realizing the effective hydrodeoxygenation (HDO) of vanillin (VAN) at room temperature (RT). The as-prepared catalyst Pd-UiO-66–0.24 W achieved > 99 % conversion of VAN and > 99 % yield of 2-methoxy-4-methylphenol (MMP) within 12 h, which surpassed the previous reports. The DFT analysis revealed that the narrow band-gap energy between Pd-UiO-66–0.24 W and H 2 molecule, along with the σ or π coordination adsorption between p and d orbitals of the implanted W and O in C=O, facilitated the activation of the H 2 molecules and reactant molecules. In addition, the constructed electron-deficient W-O-Zr interfacial sites provided more acidic sites that favor the cleavage of C-O bonds, promoting the HDO process of VAN. This work provides important insights into the modulation of EMSI, structural defects and acidic sites of metal–organic frameworks (MOFs)-based catalysts for efficient HDO of lignin-derived oxygenated compounds.
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BIOSENSORS & BIOELECTRONICS
·
2025
·
IF 10.5
Yingjing Fan,Weilun Pan,Qi Xiu,Yue Qiao,Peng Zhang,Tong Liao,Junjie Feng,Chengtao Nie,Shuai Chu,Ningcen Li,Xiuhua Wu,Lei Zheng,Zhen Cai,Bo Li
Tumor immunotherapy has significantly improved cancer treatment, yet immune checkpoint inhibitors only benefit a subset of patients. A critical challenge is non-invasive detection of tumor PD-L1 mRNA, a key biomarker that dynamically reflects PD-L1 expression and correlates with therapeutic outcomes. Current methods are hindered by the instability of circulating mRNA and the need for invasive tissue biopsies. Herein, we introduce the Cationic LIposome capsulated CRISPR-Cas13a Kit (CLICK) for in-situ detection of circulating PD-L1 mRNA in extracellular vesicles (EVs). CLICK achieves direct target identification in 10 μL plasma within 2 hours without EV purification or RNA extraction, demonstrating a detection limit of 10 3 EVs/mL for PD-L1 mRNA. By integrating membrane fusion-mediated CRISPR delivery with nanoflow cytometry, CLICK resolves PD-L1 mRNA (+) EV subpopulations at single-vesicle resolution, revealing heterogeneous distributions. Clinically validated in 53 immunotherapy patients, CLICK accurately stratifies progressive disease (PD) from stable disease (SD) patients (AUC = 0.8236; 95% CI: 0.7054–0.9417; p= 0.0006) based on PD-L1 mRNA (+) EV percentages. This work establishes a rapid, blood-based paradigm for therapy response monitoring, advancing liquid biopsy through precise EV RNA characterization.
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JOURNAL OF EXPERIMENTAL & CLINICAL CANCER RESEARCH
·
2025
·Vol. 44
·期 1
·321
·
IF 12.8
Lei Yu,Bai Yaowei,Bai Xiatong,Sun Bo,Zhu Licheng,Wu Wenlong,Su Yang,Zhang Hongsen,Wang Yingliang,Zheng Chuansheng
Background and aims Radiofrequency ablation (RFA) is an effective treatment for hepatocellular carcinoma (HCC), but incomplete ablation and recurrence of residual tumors remain significant challenges, partly due to local inflammation and elevated COX-2 levels in the tumor microenvironment. This study aims to investigate the potential of combining celecoxib, a COX-2 inhibitor, with anti-PD-1 monoclonal antibody (αPD-1) to enhance anti-tumor efficacy and activate immune responses. Methods In vitro, ELISA was used to assess the effects of radiofrequency heat treatment and celecoxib on PGE 2 secretion by Hepa1-6 cells. Scanning electron microscopy, flow cytometry, and CCK-8 assays were employed to evaluate the function and cytotoxic activity of NK92 cells against Hepa1-6 cells. In vivo, orthotopic HCC mice were divided into five groups to evaluate tumor volume, pathology, and survival. The role of celecoxib in the COX-2/PGE 2 /NK cell axis and its impact on NK cell immune function were investigated. Results In vitro experiments showed that celecoxib reversed PGE 2 -mediated suppression of NK cell function and cytotoxic activity against HCC cells by inhibiting PGE 2 secretion. In vivo, orthotopic HCC mice treated with celecoxib and αPD-1 exhibited significantly reduced tumor volumes, attenuated the infiltration and activation of NK cells, and prolonged survival compared to control groups. The combination therapy also demonstrated a notable abscopal-like effect, inhibiting metastatic tumor growth and activating systemic immunity. Conclusions Taken together, these findings suggest that celecoxib combined with αPD-1 represents a promising strategy for treating residual HCC after RFA, with enhanced anti-tumor effects and good safety. Graphical abstract
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