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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CATALYSIS COMMUNICATIONS
·
2023
·
IF 3.7
Cuicui Wu,Pan Feng,Xuan Guo,Yunming Fang
Due to complex chemical mechanism of sesquiterpene synthases, amorpha-4, 11-diene (AD) from microbial fermentation contained isomeride β-farnesene (FA) with similar boiling point. For purifying AD, FA was converted to biofuel-valued squalene (SQ) with high boiling point using solid Pd catalysts. (NHT)OS-Pd catalysts resulted in FA conversion of >99.9% and SQ selectivity of >99.0% at 80 °C for 5 h. Moreover, this catalyst exhibited great stability and recycling performance. When (NHT)OS-Pd was applied to AD mixture, almost FA was converted to SQ and AD remained in the pre-reaction state. As SQ had a higher boiling point, AD was easily distilled out.
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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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高影响因子
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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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Hongyuan Wu,Mohib Ullah,Lin Jiang,Jue Wang,Baihe Sun,Jun Gao,He Lv,Zhuo Liu,Keying Shi
The two-dimensional (2D) g-C 3 N 4 nanosheets have been widely recognized for their great potential in gas sensing. However, the disadvantages brought by layer stacking of two-dimensional nanosheets also seriously affect their performance and application. In this paper, three-dimensional hydrangea-like Pd-ZIF-67/g-C 3 N 4 was prepared for the detection of nitrogen dioxide gas at room temperature via a simple hydrothermal method . The Pd-ZIF-67/g-C 3 N 4 gas sensor exhibited excellent sensing properties with highest sensing response (23.8–100 ppm), ultrafast response speed (0.5 s) and lowest limit of detection (10 ppb) at room temperature. Moreover, it also manifests excellent reversibility and durability, optimal stability and commendable selectivity towards NO 2 gas. This excellent performance is due to the three-dimensional spatial configuration, synergistic effect and catalytic action of Pd . In general, the constructed structure and the proposed design strategy have a certain promoting role in promoting the creation of high performance gas sensors with three-dimensional heterogeneous structures based on two-dimensional nanosheets .
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Mengran Lou,Ruiying Wang,Jie Zhang,Xincun Tang,Luxiang Wang,Yong Guo,Dianzeng Jia,Hongli Shi,Lili Yang,Xingchao Wang,Zhipeng Sun,Tao Wang,Yudai Huang
Development of a Pd-based catalyst with highly active and durable properties for formic acid oxidation reaction at the anode remains an important matter of interest in the research community. Herein, we have designed novel coal-based carbon fibers (Coal-CFs) with dicyandiamide (DCD) as nitrogen (N) source, triphenylphosphine (TPP) as phosphorus (P) source dual-doped to support Pd catalysts (Pd/NP-Coal-CFs(DCD/TPP)), which exhibit superior catalytic performance toward formic acid oxidation reaction. Mass activity of formic acid oxidation of Pd/NP-Coal-CFs(DCD/TPP) catalyst is 536.6 mA·mg–1Pd, which is 2.5 times higher than that of Pd/Coal-CFs catalyst. The higher specific surface areas, exclusive electron transport path, and the high synergistic interaction of N and P are the favorable phenomena for catalytic performance. The addition of coal not only increases the abundant defects sites but also makes the utilization of coal with high added value. This N and P dual-doped catalyst inspires an idea for promoting applications in practical fuel cells.
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ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Bin Wang,Tie-yan Chang,Xiang Gong,Zhao Jiang,Sen Yang,Yu-sheng Chen,Tao Fang
The unsatisfactory performance of dehydrogenation catalysts has been the bottleneck for liquid organic hydrogen carrier (LOHC) development. After systematic experiments, the Au/Pd core/shell catalysts were screened from a series of Pd–M (M = Au, Ag, Ru, Rh) combinations for dehydrogenation of dodecahydro-N-ethylcarbazole (12H-NEC) through a one-pot wet chemical synthesis. The ratio of Pd to Au is also within the scope of the experiment, and it was found that the catalytic activity was following the order of Au1Pd1.3 > Au1Pd2 > Au1Pd1 > Ru1Pd1.3 > Au1Pd0.7 > Rh1Pd1.3 > Ag1Pd1.3 supported on rGO for the dehydrogenation process. Au1Pd1.3/rGO greatly improves the efficiency of the dehydrogenation reaction, specifically; while maintaining selectivity and conversion rate of 100%, the reaction time was shortened by 43% compared to the monometallic Pd/rGO catalyst with the highest activity we prepared before, and compared to the best performing bimetallic catalyst in the literature, the optimal reaction time in this work was reduced by 71% when the hydrogen storage requirements of the US DOE (Department of Energy) are met. A cycle performance experiment was performed to verify its excellent catalytic stability. Further catalyst characterization also proves that it has good morphology and stability. A kinetics calculation was carried out to obtain fundamental reaction parameters.
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ACS Omega
·
2018
·
IF 0
Tingting Cheng,Jian Chen,Aofei Cai,Jian Wang,Haiyan Liu,Yuandong Hu,Xiaojun Bao,Pei Yuan
A series of silica supported Pd (Pd/SiO2) catalysts were prepared in various HCl concentrations (CHCl) of the impregnation solution with different electrostatic interactions between Pd precursor and support, and their catalytic properties were evaluated by the selective hydrogenation of nitrile butadiene rubber (NBR). The results show that with the CHCl increasing from 0.1 to 5 M, the particle size of Pd nanoparticles dramatically decreases from 24.2 to 5.1 nm and stabilizes at ∼5 nm when CHCl is higher than 2 M. Using the catalysts prepared with a high CHCl (>2 M), an excellent hydrogenation degree (HD) of ∼94% with 100% selectivity to C═C can be acquired under mild conditions. Interestingly, the HD could be remarkably increased from 65 to 92% by increasing only CCl– from 0.1 to 2 M with the addition of NaCl while keeping CH+ at 0.1 M. This is because PdCl42– is the predominant existing form of precursor at high CCl–, which has a strong electrostatic attraction with the positively charged support favorable for the formation of small-sized Pd nanoparticles over silica. Notably, Pd leaching behavior during the hydrogenation reaction is closely related to CH+, and the higher the CH+, the less Pd residues are detected in the hydrogenated NBR. Our contribution is to provide a facile strategy to synthesize effective and stable Pd/SiO2 catalysts via adjusting the electrostatic interaction, which exhibits a high activity and selectivity for NBR hydrogenation.
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ANALYTICA CHIMICA ACTA
·
2018
·
IF 5.123
Maoqiang Chi,Yun Zhu,Liwei Jing,Ce Wang,Xiaofeng Lu
Over the past few years, nanomaterials-based enzymatic mimics have attracted tremendous attention due to their excellent catalytic activity and environmental stability. In this work, ternary MoS 2 -polypyrrole (PPy)-Pd nanotubes have been prepared through a hydrothermal reaction and in situ redox polymerization process between pyrrole monomer and Na 2 PdCl 4 . The prepared MoS 2 -PPy-Pd nanotubes exhibited a higher peroxidase-like catalytic activity than individual MoS 2 , MoS 2 -PPy, PPy-Pd and MoS 2 -Pd nanocomposites due to the synergistic catalytic effect between the three components. The catalytic kinetic of MoS 2 -PPy-Pd nanotubes follows Michaelis-Menten behaviors, exhibiting a good affinity to both 3,3′,5,5′-tetramethylbenzidine (TMB) and H 2 O 2 substrates. On the basis of high peroxidase-like catalytic efficiency of the MoS 2 -PPy-Pd nanotubes, a simple and convenient colorimetric strategy for the rapid and sensitive detection of l -cysteine with a detection limit of 0.08 μM has been developed. In addition, a high selectivity towards the detection of l -cysteine is achieved. This work present an opportunity of the prepared ternary MoS 2 -PPy-Pd nanotubes for promising potential applications in biosensing, environmental monitoring, and medical diagnostics.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2018
·
IF 3.779
Junhua Li,Jianbo Jiang,Dan Zhao,Zhifeng Xu,Mengqin Liu,Peihong Deng,Xing Liu,Chunming Yang,Dong Qian,Haobin Xie
In this work, Pd-decorated N-doped reduced graphene oxide (Pd/N-RGO) was successfully synthesized by a simple wet-chemical method without using any capping agent and stabilizer . The synthesized Pd/N-RGO composite has been carefully characterized by various techniques. The X-ray photoelectron spectra provide the evidence of successful incorporation of N into the N-RGO sheets, while the presence of Pd nanoparticles with the sizes of 5–20 nm on the N-RGO sheets was confirmed by the transmission electron microscopy . By integrating the advantages of the large surface area of N-RGO sheets and good electron transfer efficiency of Pd nanoparticles, the Pd/N-RGO-based sensor shows an improved electrocatalytic activity toward the estradiol oxidation . Therefore, the Pd/N-RGO composite can be used as an effective sensing platform for the non-enzymatic detection of estradiol. It also demonstrates that the fabricated sensor has two linear concentration ranges (0.1–2 and 2–400 μM) and a low detection limit (1.8 nM) for the estradiol detection. Finally, the resulting sensor was successfully used to detect estradiol in some real samples and the satisfactory recoveries of 96.0–103.9% were obtained. The prepared Pd/N-RGO composite with more distinct merits including simple manufacture, preferable reproducibility and long-term stability can be a promising candidate for the advanced electrode material in sensing applications.
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Small
·
2018
·Vol. 14
·期 33
·1801812
·
IF 9.598
Kai Gu,Xueting Pan,Weiwei Wang,Junjie Ma,Yun Sun,Hailong Yang,Heyun Shen,Zhijun Huang,Huiyu Liu
Loading novel metal nanosheets onto nanosheet support can improve their catalytic performance, but the morphological incompatibility makes it difficult to construct a well-contacted interface, which is of particular interest in supported catalysts. Herein, Pd nanosheets (Pd NSs) are supported onto graphitic carbon nitride nanosheets (CNNSs) with intimate face-to-face contact through an in situ growth method. This method overcomes the limitations of the morphological incompatibility and ensures the intimate interfacial contact between Pd NSs and CNNSs. The nitrogen-rich nature of CNNSs endows Pd NSs with abundant anchoring sites, which optimizes the electronic structure and improves the chemical and morphological stability of Pd NSs. The supported Pd NSs demonstrate high dispersion and exhibit largely enhanced activity toward the reduction of 4-nitrophenol. The concentration-normalized rate constant is up to 3052 min −1 g −1 L, which is 5.4 times higher than that obtained by unsupported Pd NSs. No obvious deactivation is observed after six runs of the recycling experiments. It is believed that the supported novel metal nanosheets with the intimately contacted interface may show promising applications in catalysis.
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CRYSTENGCOMM
·
2017
·Vol. 19
·期 37
·5565-5575
·
IF 3.474
Hui-Ze Wang,Bo Chen,Deng-Yuan Hao,Xin-Peng Miao,Dan Zhao,Ning Zhang
Pursuing a general and feasible method to construct precious metal (PM) nanostructures bounded by high-index facets (HIFs) is highly desirable for both academic and industrial interests in promising metal materials. Herein, attempts to employ modified galvanic replacement processes between MClxy− (M = Pt, Pd or Au) PM precursors and sacrificed templates of Ag nanocubic particles with deliberately introduced high [Cl−] (concentration of Cl−) were investigated to gain more acceptable HIF PM nanostructures. Typically, the Pt–Ag system was chosen as a representative system and monitored by the comprehensive characterizations of UV-vis, XRD, XPS and TEM to illuminate the evolution of the corresponding particles. It was demonstrated that the deliberately introduced Cl− at a certain concentration ([Cl−] was not lower than 1.5 M) could play dual roles in the kinetic evolution of the particles: one was dramatically lowering the etching speed to confine the reaction to the surface layers of the Ag substrates, and the other was facilitating the anisotropic etching process along the PVP-protected Ag surface through the Nernst–Einstein diffusion influence on PtCl42−, which in turn led to the formation of concave nanocubic particles with Pt-highly-dispersed [hk0] high-index surfaces (combined by the [210], [410] and [510] atomic terraces) on the Ag templates. The efficiencies of the method were further confirmed by constructing similar Pd- or Au-highly-dispersed high-index surfaces on Ag templates, suggesting that the method is a novel and general strategy to directly construct PM-based high-index surfaces with high PM dispersion in bimetallic nanostructures, which could be referenced as a solution to obtain superior precious metal materials possessing both unique HIF surface configuration and cost-saving competitiveness for advanced applications.
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