RSC Advances
·
2021
·Vol. 11
·期 53
·33202-33207
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IF 3.361
Wen Wen,Zhongping Li,Xu Wang,Xiaoyan Du,Guangming Wen,Li Li
Metal nanoclusters (NCs) have recently emerged as a novel class of luminescent nanomaterials and held significant potential in analytical chemistry. In this work, novel polyethyleneimine stabilized palladium nanoclusters (PEI–Pd NCs) were synthesized by chemical reduction at 60 °C for 6 h, and used as a fluorescent nanosensor for the detection of oxytetracycline (OTC). The spectral characteristics, surface structure and morphology of the Pd NCs were studied. The selectivity and stability of the nanosensor were also investigated. The experimental results showed that the Pd NCs had good biocompatibility, stability and photobleaching resistance in aqueous solution. The fluorescence quenching effect showed a good linear relationship with the degree of fluorescence quenching of Pd NCs and OTC in the range of 25–440 nM, with a correlation coefficient of 0.99. The limit of detection (LOD) of the proposed nanosensor for OTC was calculated to be 22 nM. The mechanism of determination was thought to be an inner filter effect (IFE) between OTC and Pd NCs. Based on this, we have established a new nanosensing analysis method for detecting OTC.
研究领域:
分析化学
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纳米材料科学
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DOI
高影响因子
ELECTROCHIMICA ACTA
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2018
·
IF 5.116
Yimin Zhang,Youhai Cao,Dong Chen,Penglei Cui,Jun Yang
The use of Ionic Liquids (ILs) to enhance the electrocatalytic activity of metal nanoparticles has garnered sustained research interest. However, current strategies involving ionic liquids do not exploit their use and advantages in chemical synthesis of metal nanoparticles. Herein, we demonstrate a straightforward method, which combines the advantages of ILs in nanoparticle synthesis with the potentials of ILs in electrocatalysis , for the synthesis of Pd nanoclusters for electrochemical oxidation of formaldehyde. This method relies on the use of 1-(2′-aminoethyl)-3-methyl-imidazolum tetrafluoroborate ionic liquid as stabilizers to directly generate Pd nanoclusters with average sizes of 1.8 ± 0.3 nm in a reaction medium consisting of water and methanol at room temperature . The electrochemical measurements prove that the ionic liquid-assisted Pd nanoclusters have mass-normalized activity approximately 7 times than that of commercial Pd/C catalysts for the oxidation of formaldehyde.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 22
·9248-9254
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IF 3.288
Xiaoyan Du,Wenxia Dong,Zhongping Li,Guangming Wen,Meng Liu,Xiujun Fan
Tetracycline (TC) is considered one of the most widely used antibiotic medicines, and ranks the second highest in global production and usage among all antibiotics. In this study, palladium nanoclusters (Pd NCs) have been successfully synthesized using polyvinylpirrolidone (PVP) as a capping agent and an ultrasensitive photoluminescent nanosensor for TC, and was first constructed based on an internal filtration effect causing fluorescence quenching of Pd NCs. The as-synthesized Pd NCs have high fluorescence intensity, good stability at extreme pH, high ionic strength, and excellent stability in light (under UV irradiation), and its fluorescence quantum yield (QY) was up to 5.9%. The fluorescence ratio of I/I0 linearly decreases with the increase in the concentrations of TC in the range from 0 nM to 220 nM in an aqueous buffer with the detection limit of 0.03 nM. The ultrasensitive detection of TC was also successfully realized in the spiked samples of honey with good recoveries. The advantages of this method include simplicity, rapidity, high sensitivity, high selectivity and cost efficiency.
研究领域:
分析化学
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环境科学
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药学
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产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 46
·21265-21276
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IF 3.5
Zhang Kewen,Fan Benwei,Wang Shidong,Zhang Hongwei,Liu Qunhong,Bao Xiaojun,Yuan Pei
Heterogeneous hydrogenation is an effective way to improve the performance of unsaturated polymers, but the preparation of supported catalysts with high metal dispersion and stability remains challenging. Herein, we synthesize a SiO 2 -based support wrapping with carbon nitride on the surface (CN x @SiO 2 ) via the thermal polycondensation of melamine, on which Pd nanoclusters with highly exposed active sites are formed and stably anchored via the strong interaction between N and Pd. The thermal temperature affects the properties of CN x , which further modulates the electronic and structural state of Pd nanoclusters. The Pd/CN x @SiO 2 -500 catalyst, prepared at 500 °C with an optimal CN x structure ( g -C 3 N 4 ) and high nitrogen content, features highly dispersed and electron-rich Pd nanoclusters (1.3 nm). This catalyst exhibits a hydrogenation activity of 98.0% for nitrile rubber, with a selectivity of 100% for C=C bonds. This work provides a facile method to prepare Pd catalysts with high activity and stability, paving the way for the upgrading of unsaturated polymers via hydrogenation. Graphical abstract
研究领域:
催化化学
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材料科学
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高分子化学
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DOI
高影响因子
CATALYSIS LETTERS
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2021
·Vol. 151
·期 9
·2537-2546
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IF 3.186
Zhang Qianqian,Zheng Shanshan,Zhang Jinli,Li Wei,Fu Yan
NADH, composed of metal binding, charged and redox groups, acts as a “three-in-one” template to construct peroxidase mimicking Pd nanoclusters (NCs). The physicochemical properties of Pd NCs are highly dependent upon the molar ratio of [NADH]/[Na 2 PdCl 4 ], thereby contributing to distinct peroxidase mimicking activities. The ultrasmall Pd nanozyme that contains 30% metallic Pd 0 species, exhibits the K m of 0.063 mM toward TMB and 80.8 mM toward H 2 O 2 . Notably, addition of heparin enables the enhancement of its peroxidase-like activity in neutral media. A colorimetric assay was well-established at pH 6 for quantitatively monitoring heparin in aqueous solution and biological fluid. The linear response lies in the range of 0.5–25 µg mL −1 , with the limit of detection of 1.1 ng mL −1 . This work paves a promising pathway to manufacture highly active enzyme mimetics with desirable physicochemical properties. Graphic Abstract
研究领域:
生物化学
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纳米医学
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分析化学
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产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
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2017
·Vol. 23
·期 72
·18187-18192
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IF 5.317
Jishi Chen,Liren Liu,Xu Liu,Lingwen Liao,Shengli Zhuang,Shiming Zhou,Jinlong Yang,Zhikun Wu
Graphical Double-crown Pd 4 (PET) 8 and Pd 5 (PET) 10 were successfully doped with gold through two Au atoms replacing one Pd atom with the other double-crown structure essentially unchanged. Au 4 Pd 2 (PET) 8 is the smallest chiral bimetal nanoclusters so far and it bears chirality originating from not only the helixed Au 4 Pd 2 S 8 framework but also unanimous R or S configuration of sulfur atoms in the enantiomer. Double-crown Ni, Pd, or Pt nanoclusters have attracted extensive interests due to their aesthetic structure and intriguing properties. However, their doping by other metals remains unknown until now. Herein, Pd 4 (PET) 8 and Pd 5 (PET) 10 (PET: SCH 2 CH 2 Ph) were successfully doped with gold and the doped nanoclusters were characterized by using multiple techniques such as mass spectrometry and X-ray crystallography. It is revealed that in the doping not one but two gold atoms replace one Pd with the other double-crown structure essentially unchanged, and the gold-doping results in the blue-shift of the maximum visible absorption, the increase of optical energy gap and the reduction of anti-aromaticity of monometal Pd nanoclusters. Importantly, it is found that Au 4 Pd 2 (PET) 8 nanocluster bears chirality originating from not only the helixed Au 4 Pd 2 S 8 framework, but also unanimous R or S configuration of sulfur atoms in the enantiomer. For the latter chirality origin, it was not previously reported or proposed. Au 4 Pd 2 (PET) 8 reported here also represents the smallest chiral bimetal nanocluster so far to the best of our knowledge. This work advances one step toward both the tailoring of group 10 metal nanoclusters by doping and the understanding of chirality origin for metal nanoclusters.
研究领域:
材料化学
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纳米科学
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产品关联
DOI
PubMed
高影响因子
Inorganic Chemistry Frontiers
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2018
·Vol. 5
·期 11
·2948-2954
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IF 5.106
Yuanxin Du,Ji Xiang,Kun Ni,Yapei Yun,Guodong Sun,Xiaoyou Yuan,Hongting Sheng,Yanwu Zhu,Manzhou Zhu
Atomically precise nanoclusters (NCs) have been widely used as catalysts in many reactions to investigate the structure–activity relationship due to their ultrasmall sizes, well-defined structures and precise compositions, especially bimetallic NCs can further promote the catalytic activity by the synergistic effects of heteroatoms. For electrocatalytic hydrogen evolution reaction (HER) catalysts, a common method to improve the performance is coupling with a nano-metal, but the origin of the enhancement is still unclear due to the diversity and complexity of the nanometal supported composites. Here, we take MoS2 (a star HER electrocatalyst) as an example, to report a strategy to boost the activity and give insight into the activity enhancement of it by combining with bimetallic atomically precise NCs. The crystal structure of this new NC is determined by X-ray crystallography, and its precise composition is identified as Au2Pd6S4(PPh3)4(C6H4F2S)6 (Au2Pd6 for short). The Au2Pd6/MoS2 show significantly improved HER activity and robust durability compared to the single component Pd3 or Au2/MoS2 and bare MoS2. This is attributed to the appropriate adsorption behavior of H atoms on Au2Pd6/MoS2 and the electronic interactions between NCs and MoS2, according to the combination of experiment and theory. This study presents a new strategy to improve the electrocatalytic activity of 2D materials such as MoS2 and sheds light on the origin of the promotion effects at the atomic level.
研究领域:
材料科学
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催化化学
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能源化学
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产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2021
·
IF 5.097
Ying Li,Shujuan Li,Min Bao,Linqun Zhang,Carlo Carraro,Roya Maboudian,Anran Liu,Wei Wei,Yuanjian Zhang,Songqin Liu
Nanomaterials possessing intrinsic enzyme-mimetic activity are becoming an important topic of current research. However, their enzyme-mimetic activity is limited by the particle size of the nanomaterials. In this study, Pd nanoclusters with an average size of 1.4 nm are synthesized by using a metal organic framework, zeolitic imidazolate framework-8 (ZIF-8), as a matrix via an impregnation-reaction method. By virtue of the confined channels of ZIF-8 and the strong chemical interaction between the Pd nanoclusters and ZIF-8 framework, the Pd nanoclusters show a high dispersity and stability. The obtained Pd@ZIF-8 is proven to have enhanced intrinsic peroxidase-like activity, showing Michaelis–Menten constants (Km) as high as 0.13 mM for 3,3′,5,5′-tetramethylbenzidine and 14.02 mM for hydrogen peroxide. Colorimetric testing and electron spin resonance spectra reveal that radicals are generated during the catalytic process of peroxidase-like Pd@ZIF-8 toward H2O2. With the addition of glucose or cholesterol oxidase, the Pd@ZIF-8 can be utilized to construct a highly selective and sensitive fluorescent sensor for glucose and cholesterol, exhibiting a detection limit of 0.10 and 0.092 μΜ, respectively. Additionally, the proposed fluorescent platform exhibits the capability to detect glucose and cholesterol in serum samples with satisfactory recovery, indicating potential application prospects in biochemical analysis.
研究领域:
材料科学
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生物化学
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医学诊断
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产品关联
DOI
高影响因子
Journal of Materials Chemistry B
·
2018
·Vol. 6
·期 36
·5795-5801
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IF 4.776
Xuemei Yin,Linlin Liang,Peini Zhao,Feifei Lan,Lina Zhang,Shenguang Ge,Jinghua Yu
MicroRNAs (miRNAs) are a class of significant biomarkers; however, it is still a huge challenge to express them accurately. Herein, a fluorescent/colorimetric dual-model biosensor based upon the quenching effect of graphitic carbon nitride on palladium nanoclusters (Pd NCs) on the platform of a microfluidic paper-based analytical device was built for the detection of miRNAs. On the one hand, Pd NCs could catalyze a chromogenic reaction so that preliminary detection was achieved by the naked eye. On the other hand, the fluorescence analysis combined with nucleic acid cycle signal amplification was required to get precise result and the detection limit is 3 fM, which was superior to the previous method. What's more, this biosensor could be designed to detect other miRNAs via changing the corresponding aptamer sequences. Therefore, the as-constructed biosensor supplies a versatile platform to conduct point-of-care detection of miRNAs with outstanding performance.
研究领域:
生物化学
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分子诊断
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纳米技术
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医学检测
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2018
·
IF 6.945
Yuanyuan Ji,Ye Ying,Xiaoyu Guo,Yiping Wu,Ying Wen,Haifeng Yang
The Palladium/polydopamine (Pd/PDA) litchi-like nanoclusters are synthesized via a two-step route. The resultant product is characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and the electrochemical properties were evaluated by cyclic voltammetry (CV) and chronoamperometry . Notably, the as-prepared litchi-like Pd/PDA nanoclusters show superior catalytic properties for methanol electro-oxidation in an alkaline medium due to unique Pd dots adhered at PDA surface providing a large electrochemically active surface area (ECSA). Additionally, the high concentration of oxygen functional groups on PDA is essential to the removal of carbonaceous species from the adjacent at the Pd sites. This PDA-based straightforward synthesis strategy offers a new pathway for developing highly active electrocatalysts with aid of special organic polymer .
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2023
·
IF 13.1
Zhongying Fang,Ziwei Zhang,Shemsu Ligani Fereja,Jinhan Guo,Xinjie Tong,Yue Zheng,Rupeng Liu,Xiaolong Liang,Leting Zhang,Zongjun Li,Wei Chen
Direct formic acid fuel cell (DFAFC) is an important research project in clean energy field. However, commercialization of DFAFC is still largely limited by the available catalysts with unsatisfied activity, durability and cost for formic acid electrooxidation (FAEO). Using Pt- and Pd-based nanoclusters as electrocatalysts is a particularly promising strategy to solve the above problem, but two attendant problems need to be solved firstly. (I) The controllable synthesis of practicable and stable sub-2 nm clusters remains challenging. (II) The catalyzing mechanism of sub-2 nm metal clusters for FAEO has not yet completely understood. Herein, different from traditional solution synthesis, by designing a novel supporting material containing electron-rich and electron-deficient functional groups, size- and dispersion-controllable synthesis of ∼1 nm PtPd nanoclusters is realized by an electrochemical process. The electrocatalytic properties and reaction mechanism of the PtPd nanoclusters for the FAEO were studied by different electrochemical techniques, in-situ fourier transform infrared (FTIR) spectra and density functional theory (DFT) calculations. The tiny PtPd nanoclusters have much higher catalytic activity and durability than commercial Pt/C, Pd/C and 3.5 nm PtPd nanoparticles. The present study shows that the metal-reactant interaction plays a decisive role in determining the catalytic activity and cluster-support interaction plays a decisive role in enhancing the durability of electrocatalyst. The ratio and arrangement of Pt and Pd atoms on the surface of 1 nm PtPd cluster as well as the overall valence state, d-band center and specific surface area make them exhibit different catalytic performance and reaction mechanism from nanoparticle catalysts. In addition, in situ FTIR and DFT calculations showed that on the surface of PtPd clusters, the generation of CO 2 through trans-COOH intermediate is the most optimal reaction pathway for the FAEO.
研究领域:
材料科学
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能源化学
·
电催化
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2020
·
IF 7.888
Haiping Li,Tianxing Yang,Yiwei Jiang,Shuai Chen,Yufei He,Junting Feng,Dianqing Li
A feasible method for spontaneous in situ reductions on layered double hydroxides (LDHs) to prepare supported catalysts with Pd sub-nanoparticles is proposed. In this process, the reductive sites for the Pd 2+ are introduced into the LDHs laminates in a highly dispersed distribution, and a series of reductive supports (such as CoAl-LDHs, CoNiFe-LDHs, FeAl-LDHs) are prepared. The obtained reductive support is directly used to reduce Pd precursor without the addition of a reducing agent. HRTEM images show that metallic Pd is successfully reduced and evenly distributed on the support. Moreover, hexadecyl trimethyl ammonium chloride (CTAC) is introduced to improve the dispersion of Pd. HAADF-STEM results illustrate that metallic Pd particles are prepared in the form of a sub-nanometer size. XPS analysis show that Co and Pd species undergo a redox reaction and have an electronic interaction with CTAC. The factors affecting the nucleation and growth of Pd sub-nanoparticles in CTAC-modified support spontaneous in-situ redox are also discussed. The obtained Pd MI /CoAl-LDHs (prepared by modified support spontaneous in situ redox method (MI)) is applied to the selective oxidation of benzyl alcohol. It is found that the selectivity is 91% at a conversion of 92%, and turnover frequency (TOF) of Pd MI /CoAl-LDHs is 2.2 times higher than that of Pd D /MgAl-LDHs prepared by the common dipping method. Furthermore, Pd MI /CoAl-LDHs shows excellent stability in 5 times reusability and 150 h use, demonstrating the Oswald ripening of Pd particles can be effectively prevented.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）