Materials Advances
·
2023
·Vol. 4
·期 4
·1135-1145
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IF 5
Dongcang Sun,Changtong Song,Xianhong Zhang,Dong Chen,Yuhong Ma,Wantai Yang
An ultrafiltration (UF) membrane was prepared using a blend of poly(vinyl chloride) (PVC) and low molecular weight poly(vinyl chloride-co-maleic acid monoamide) (PVMA), demonstrating a significantly improved filtration flux. For example, the water flux of the membrane fabricated with PVMA/PVC (50/50 wt%/wt%) was boosted to 691.67 L m−2 h−1vs. 64.66 L m−2 h−1 for the pure PVC membrane, while the porosity of the UF membranes was 88.6% vs. 74.7%, respectively. Employing immobilized palladium nanoparticles as a catalyst, the Pd-PVMA/PVC membrane offered an efficiency as high as 99.0%, which remained greater than 97.0% over three cycles at a filtration flux of 208.75 L m−2 h−1 for the degradation of 4-nitrophenol (4-NP). The catalytic reaction exhibited first-order kinetics and the apparent kinetic reaction constant was as high as 2.65 × 10−3 s−1 at a relatively low Pd nanoparticle loading. In this study, we developed a simple method to prepare PVC UF membranes with high water flux and efficiency for the removal of 4-NP by coupling the catalytic and separation processes.
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高影响因子
JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Jinlong Li,Huiyuan Liu,Weiqi Zhang,Qian Xu,Sae Youn Lee,Narayanamoorthy Bhuvanendran,Huaneng Su
The catalyst layer (CL) is the only electrochemical reaction site in proton exchange membrane fuel cells (PEMFCs), decisive in their performance. Herein, a mild and simplified strategy is implemented into the in-situ growth of Pt–Pd alloy catalysts on the gas diffusion layer (GDL) as the CLs for PEMFCs. Pt/C is used as the nucleation site to assist the in-situ growth of the Pt–Pd CL. The as-prepared Pt–Pd CL behaves as a multi rhombic-pyramidal structure, which are evenly distributed on the GDL surface. The effect of the Pt/Pd atomic ratio on the electrocatalytic activity is investigated through a single-cell performance test, and the optimal atomic ratio is determined to be 1/2, which exhibits excellent cell performance and low activation polarization loss. Meanwhile, the single-cell test results reveal that Pt 1 Pd 2 CL reaches optimal performance at a loading of 0.122 mg cm −2 (∼0.06 mg Pt cm −2 ), with a peak Pt-specific power density of 14.23 W mg −1 (6.81 W mg −1 in PtPd), approximately 3.96 times that of a commercial Pt/C CL (0.2 mg Pt cm −2 ). Furthermore, Pt 1 Pd 2 CL shows significantly better stability than the commercial Pt/C CL, indicating that the in-situ preparation of the Pt-based CL has an excellent prospect for the commercial development of PEMFCs.
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Coatings
·
2023
·Vol. 13
·期 8
·1400
·
IF 3.4
Yuyan Peng,Li Jiang,Yifan Li,Xiaoping Yu
Soluble programmed death-ligand 1 (sPD-L1) levels vary widely among different stages of tumor development, so the direct quantification of sPD-L1 as a cancer biomarker is useful in cancer diagnosis, prognosis and therapeutic assessment. There is an urgent need for an sPD-L1 detection method with a broad detection range and high sensitivity for monitoring cancer progression and evaluating the effectiveness of immunotherapy in real time. Herein, we have reported an enzyme-free, label-free surface plasmon resonance imaging (SPRi) sensor based on an aptamer/sPD-L1/anti–PD-L1 sandwich structure with gold nanoparticle (AuNP) signal enhancement for the ultrasensitive quantitative measurement of sPD-L1 for the first time. The gold chip of the SPRi sensing platform was modified by DNA aptamers, sPD-L1 was specifically adsorbed on the surface of a DNA aptamer-modified gold chip and then coupled with anti–PD-L1. Thus, the detection of sPD-L1 at different concentrations was realized through the formation of an aptamer/sPD-L1/anti–PD-L1 sandwich structure. We also enhanced the SPR signal via AuNPs to further improve sensor sensitivity. The SPRi sensor is able to measure sPD-L1 within a linear range of 50 pM–10 nM and 100 fM–50 pM, and the minimum detection limit is 19 fM. The sensor is designed to be widely applicable, with better accuracy and reliability for more application scenarios. The prepared SPRi sensor shows great potential in improving the sensitivity of detecting sPD-L1. The proposed method demonstrates the excellent performance of the SPRi sensor and provides a possibility for the establishment of effective clinical assay methods in the future.Keywords:programmed death-ligand 1;surface sandwich assay;DNA aptamer/antibody bioreceptor pair;surface plasmon resonance;tumor biomarker
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CATALYSIS LETTERS
·
2022
·Vol. 153
·期 8
·2517-2526
·
IF 2.936
Wu Jindong,Zuo Jianliang,Liu Kuiliang,Lin Jing,Liu Zili
Designing a stable, efficient, highly selective, and low-cost dehydrogenation catalyst, using formic acid to produce hydrogen energy, is challenging even today. This paper reports a facile preparation method of constructing Pd–Co alloy-composite catalyst for hydrogen production using formic acid by heterogeneous catalyst decomposition. The results demonstrate that introducing a nonprecious cobalt metal could significantly reduce precious palladium metal usage. Moreover, the particle size reduces from 13.50 nm (without Co) to 3.4 nm (with Co). More importantly, the Pd 2+ amount in the catalyst affect the catalytic decomposition of formic acid to produce hydrogen. Additionally, Pd 0.9 Co 0.1 /C 650 exhibits excellent catalytic activity and cyclic catalytic stability and it is one of the best non-precious metal doped Pd-based catalysts. The development of a synthetic method with the addition of nonprecious metal in this paper opens up a new avenue for cheap and efficient catalysts for application scenarios of hydrogen production. H 2 production by formic acid dehydrogenation. Graphical abstract
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Journal of Materials Chemistry B
·
2022
·Vol. 10
·期 34
·6532-6545
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IF 7.571
Zhe Tang,Israt Ali,Yike Hou,Ozioma Udochukwu Akakuru,Quan Zhang,Asim Mushtaq,Han Zhang,Yuguang Lu,Xuehua Ma,Jian Ge,M. Zubair Iqbal,Xiangdong Kong
Nanotheranostic agents based on plasmonic nanostructures with their resonance wavelengths located in the second near-infrared window (NIR-II) have gained significant attention in profound tumor photothermal therapy. However, the modulation of localized surface plasmon resonance of gold nanomaterials from the first near-infrared (NIR-I) window to the NIR-II window is still challenging. The structures and compositions of the plasmonic nanomaterials have demonstrated promising characteristics in controlling the optical properties of plasmonic nanostructures. Here, gold nanorod (Au NR) coated with an ultrathin palladium (Pd) shell was developed for tumor-targeted NIR-II photothermal-augmented nanocatalytic therapy through the combination of compositional manipulation and structural evolution strategies. These Au@Pd core–shell hybrid NRs (HNRs) were functionalized with biocompatible chitosan (CS) to acquire lower toxicity and higher stability in physiological systems. Further, Au@Pd–CS HNRs were endowed with an excellent targeting ability by conjugating with folic acid (FA). The as-synthesized Au@Pd–CS–FA HNRs show efficient and complete photothermal ablation of tumor cells upon 1064 nm laser irradiation. The remarkable photothermal conversion efficiency of 69.0% was achieved, which is superior to many reported photothermal agents activated in the NIR-II region. Excitingly, Au@Pd–CS–FA HNRs have peroxidase and catalase activities, simultaneously producing ˙OH for catalytic therapy and O2 for relieving tumor hypoxia and photodynamic therapy. Additionally, in vivo tumor photothermal therapy was carried out, where the biocompatible Au@Pd–CS–FA HNRs penetrate intensely into the tumor cells and consequently show remarkable therapeutic effects. The idea about plasmonic modulation behind the bimetallic core–shell nanostructure in this report can be extended to construct new classes of metal-based nanotheranostic agents with dual-modal combined therapy as an alternative to traditional chemotherapy.
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PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Xin-Xin Fu,Jian-Peng Li,Zhuo-Qian Li,Yan Liu,Chen-Xiao Feng,Hai-Yang Wang,Zhi-Peng Zhao,Qiao-Yun Liu,Zhong-Yi Liu,Zhi-Kun Peng
Biomass is a promising renewable carbon resource, and bio-based platform molecules such as furan derivatives play an important role in the green manufacturing of high value-added chemicals. Of these, the conversion of 2-methylfuran (2-MF) to 3-acetyl-1-propanol (3-AP) over a bifunctional catalyst has attracted significant interest. However, bifunctional catalysts prepared by traditional method suffer from poor catalytic performance and limited stability due to the agglomeration of metal NPs. Here, Pd@HZSM-5, in which Pd NPs were encapsulated in HZSM-5 in situ showed improved stability and 3-AP yield. The highest yield of 3-AP (90.6%) to date was obtained with a nearly 100% conversion of 2-MF. The catalytic performance over a series of Pd@Zeolite confirms the superiority of the encapsulation effect, which is ascribed to the optimal adjustment of metal/acid balance. The Pd@HZSM-5 catalyst displayed excellent stability due to the encapsulation structure, which restricts the Pd NPs agglomeration. The highest yield of 3-AP was obtained at a high concentration of 2-MF (60%), which implies a promising strategy for the green industrial manufacture of 3-AP. This work reports a new bifunctional catalytic system for the green synthesis of 3-AP from 2-MF, thus stimulating the downstream biomass market.
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JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Chunhua Wang,Xiang Li,Ying-Ya Liu,Anjie Wang,Qiang Sheng,Chen-Xi Zhang
The hydrodesulfurization (HDS) of dibenzothiophene (DBT) was studied over a series of Pd catalysts supported on Zr-based metal-organic frameworks, UiO-66 and its amino-functionalized analogues (UiO-66-xNH 2 , where x represents the molar ratio of 2-amino-1,4-benzenedicarboxylic acid/1,4-benzenedicarboxylic acid) to gain an insight into metal-support interactions. Pd/UiO-66 behaved better than a Pd/γ-Al 2 O 3 catalyst and a Pd/MCM-41 catalyst. The presence of amino groups showed minor negative influence on the conversion of DBT but significantly affected the activities and selectivities of different reaction pathways. With the increase in the content of amino groups, the direct desulfurization (DDS) pathway activity of the Pd/UiO-66-xNH 2 catalysts increased, while their hydrogenation pathway activity decreased. This provides an approach for the regulation of the pathway selectivities of Pd HDS catalysts. Based on kinetic analysis and characterization results, we propose that the amino groups affect the HDS performance of Pd/UiO-66 mainly by affecting the adsorption of reacting molecules on metal particles.
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BIOSENSORS & BIOELECTRONICS
·
2023
·
IF 12.6
Zhijun Lin,Mengyao Liu,Wei Xing,Feng-Hua Wang,Hongxia Zhang,Xiao-Li Wei,Hans Schmitthenner,Xi Xie,Xiaojun Xia,Jiang Yang
Sensitive and accurate biomarker-driven assay guidance has been widely adopted to identify responsive patients for immune checkpoint blockade (ICB) therapy to impede disease progression and extend survival. However, most current assays are invasive, requiring surgical pathology specimens and only informing monochronic information. Here, we report a multiplexed enhanced fluorescence microarray immunoassay (eFMIA) based on a nanostructured gold nanoisland substrate (AuNIS), which macroscopically amplifies near-infrared fluorescence (NIRF) of a structurally symmetric IRDye78 fluorophore by over two orders of magnitude of 202.6-fold. Aided by non-contact piezo-driven micro-dispensing (PDMD), eFMIA simultaneously and semi-quantitatively detected intracellular and secreted programmed death-ligand 1 (PD-L1) and intercellular adhesion molecule-1 (ICAM-1) in human nasopharyngeal carcinoma (NPC) cells. The assay performance was superior to fluorescence immunoassays (FIA) and enzyme-linked immunosorbent assays (ELISA), with lower detection limits. Using eFMIA, we found significantly differential levels of soluble PD-L1 (sPD-L1) and sICAM-1 in the sera of 28 cancer patients, with different clinical outcomes following anti-PD-1 ICB therapy. With a well-characterized mechanism, the high-performance plasmonic multiplexed assay with the composite biomarkers may be a valuable tool to assist clinicians with decision-making and patient stratification to afford predictive ICB therapy responses.
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CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2021
·
IF 3.739
Muhammad Sohail Bashir
Developing new strategies for fabrication of porous materials with tunable morphology which have fewer environmental impacts is highly desired. Herein, conventional precipitation polymerization of polyurea (PU) synthesis is converted to interfacial polymerization via simple microfluidics and hierarchically porous and uniform PU microspheres (PPM) are prepared by the reaction of toluene diisocyanate and water, eliminating the use of toxic amines and organic solvents. The morphology and porosity of PPM are probed. The size of PPM is controlled by changing the diameter of flow channels of microfluidic device and their pore size and porosity are tuned by optimizing the polymerization conditions. Moreover, palladium (Pd) is immobilized on PPM by impregnation and subsequent reduction approach to get Pd@PPM. The hybrid composite, Pd@PPM, is used for catalytic reduction of toxic Cr 6+ to benign Cr 3+ by formic acid as a reductant along with sodium format as a promoter in aqueous system. Pd@PPM exhibited high catalytic activity and good stability for Cr 6+ reduction and their large size with high uniformity eased their recovery to reuse them in subsequent Cr 6+ reduction. Porous PU with controllable shape and morphology are rarely available. This work therefore provides new strategy to synthesis PPM with controllable porous morphology and their use as an effective support for catalysis.
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JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS
·
2023
·
IF 3.4
Jia Sun,Rong Li,Jingya Zhang,Yong Huang,Yuan Lu,Chunhua Liu,Yongjun Li,Ting Liu
Shenxiong glucose injection (SGI) containing a water extract from the roots of Danshen and Ligustrazine hydrochloride, is the main drug used for the prevention and treatment of acute myocardial ischemia (AMI) in China. Based on the characteristics of drug clinical applications, this study aims to uncover the compatibility mechanism of SGI by investigating pharmacokinetic (PK) and pharmacodynamic (PD) differences between Danshen glucose injection (DGI), Ligustrazine glucose injection (LGI) and SGI groups after multiple dosing during the pathological state from the perspective of metabolic enzymes. Compared to the LGI group, the absorption (C max ) and exposure (AUC) of ligustrazine increased significantly, and the protein expression of CYP1A2, CYP2C11 and CYP3A2 in the SGI group decreased significantly. Furthermore, the PK and PD experimental data for Danshen and ligustrazine in AMI rats were fitted to obtain a PK-PD binding model with three components. PK-PD parameter analysis showed that in the SGI group the IC50 values of ligustrazine and danshensu on AST, CK-MB, cTn-I and the IC 50 values of rosmarinic acid on AST and CK-MB were lower than the DGI or LGI group. It is speculated that Danshen inhibited CYP1A2, CYP2C11 and CYP3A2 mediating the metabolism of ligustrazine and decreased the expression of these three isozymes, which further affected the in vivo process of ligustrazine. Moreover, the combination of Danshen and ligustrazine could have better regulating effect on AST, CK-MB and cTn-I. This preliminary study has provided a scientific basis for understanding the compatibility mechanism of SGI from the viewpoint of the regulation of CYP enzymes in the PK-PD model.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hao Chen,Xuexian Wu,Danni Liu,Chunyi Ye,Lingui Huang,Xin Long,Lei Wang,Jiujun Zhang,Jing-Li Luo,Xian-Zhu Fu
Energy-saving electrolytic hydrogen production could be realized by replacing sluggish oxygen evolution reaction (OER) with ethanol oxidation reaction (EOR). However, it's challenging to obtain high-performance electrocatalysts with excellent activity (close to the theoretical potential for EOR), superior production selectivity, and stability (anti-poisoning during EOR). In this study, a C@Ni-Pd bifunctional catalyst is fabricated towards EOR and hydrogen evolution with high activity, selectivity, and stability. The potential of EOR over the C@Ni-Pd catalyst is reduced by 1.072 V relative to OER at 100 mA cm −2 . In the water–ethanol co-electrolysis device, the onset potential is as low as 0.4 V, and the current density reaches 100 mA cm −2 at 0.95 V. The power consumption of device is still lower than the water electrolysis theory at high current density. High-selective acetate could be co-produced with hydrogen while without CO 2 emission over C@Ni-Pd bifunctional catalysts. DFT and in-situ Raman spectroscopy results indicate that the highly-active Pd sites endow significant energy-saving hydrogen production effect. The high selectivity is derived from the abundant OH* on the surface of Ni, which promotes the conversion of *CH 3 CO adsorbed on Pd to *CH 3 COOH. This study provides a new straight to design high-performance electrocatalysts for energy-saving co-generation of pure hydrogen and value-added chemicals from organic fuels and water while without CO 2 emissions.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2023
·
IF 3.8
Sheng Wan,Rong Xie,Jianhong Fan,Kewen Tang
Gold (Au) and palladium (Pd) play an increasing role in the production and human life, therefore, it is of great significance to study their recovery. A 5,11,17,23-tetra-ethylthio-25,26,27,28-tetra-hydroxyl thiacalix[4]arene (TCAET) was synthesized specifically for the capture of Au(Ⅲ) and Pd(Ⅱ) from HCl medium by liquid–liquid extraction. In a 0.1 mol·L –1 HCl medium, the transfer of Au(Ⅲ) and Pd(Ⅱ) from the aqueous phase to the organic phase was highly efficient, with a transfer ratio of 100% for Au(Ⅲ) and 98% for Pd(Ⅱ). Furthermore, the extraction equilibrium time for Au(Ⅲ) was just 5 min. Job's method data demonstrated that TCAET formed complexes with Au(III) and Pd(II) in a ratio of 2:3 and 1:1, respectively, during the extraction process. TCAET showed high selectivity toward Pd(II) and Au(III) over other competing metal ions. Moreover, both Au(Ⅲ) and Pd(II) could be successfully stripped from the loaded organic phases with a 1.0 mol·L –1 thiourea in 0.5 mol·L –1 HCl and 0.5 mol·L –1 thiourea in 0.5 mol·L –1 HCl, respectively. Results obtained from five consecutive extraction-stripping cycles showed good reusability of TCAET toward Au(Ⅲ) and Pd(Ⅱ) recovery. The conclusion can provide a certain reference for thiacalixarene in the recovery of precious metal species.
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