Small
·
2019
·Vol. 16
·期 4
·1904964
·
IF 10.856
Zelin Chen,Yunwei Liu,Chang Liu,Jinfeng Zhang,Yanan Chen,Wenbin Hu,Yida Deng
The development of new type electrocatalysts with promising activity and antipoisoning ability is of great importance for electrocatalysis on alcohol oxidation. In this work, Pd nanowire (PdNW)/CuO x heterogeneous catalysts with different types of Pd O Cu interfaces (Pd/amorphous or crystalline CuO x ) are prepared via a two-step hydrothermal strategy followed by an air plasma treatment. Their interface-dependent performance on methanol and ethanol oxidation reaction (MOR and EOR) is clearly observed. The as-prepared PdNW/crystalline CuO x catalyst with 17.2 at% of Cu on the PdNW surface exhibits better MOR and EOR activity and stability, compared with that of PdNW/amorphous CuO x and pristine PdNW catalysts. Significantly, both the cycling tests and the chronoamperometric measurements reveal that the PdNW/crystalline CuO x catalyst yields excellent tolerance toward the possible intermediates including formaldehyde, formic acid, potassium carbonate, and carbon monoxide generated during the MOR process. The detailed analysis of their chemical state reveals that the enhanced activity and antipoison ability of the PdNW/crystalline CuO x catalyst originates from the electron-deficient Pd δ+ active sites which gradually turn into Pd 5 O 4 species during the MOR catalysis. The Pd 5 O 4 species can likely be stabilized by moderate crystalline CuO x decorated on the surface of PdNW due to the strong Pd O Cu interaction.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
NANOTECHNOLOGY
·
2023
·Vol. 34
·期 35
·355402
·
IF 3.5
Qian Liu,Seng Dong,Yuanzhe Wang,Weiyi Jia,Xi Chen,Faming Gao,Yatao Wang
Fuel cells, as the alternative to fossil energy, have engaged widespread attention by reason of the high conversion efficiency from the chemical energy to the electric energy combined with low pollution emissions. The cathodic ORR catalysts with excellent performance and cost-effectiveness are the dominant point towards the massive development of fuel cells. Here, our group select the Pd NWs as the template and construct the Pd@PtRuNi core–shell bilayer nanostructure to expand platinum atom utilization. Pd@PtRuNi bilayer core–shell NWs unfold elevated mass activity of 1.62\,{\rm{A}}\,{{\rm{mg}}}_{{\rm{metal}}}^{-1} at 0.9 V versus RHE in alkaline media, 2.03- and 6.23-fold of pristine Pd NWs and benchmark commercial Pt/C, respectively. Meanwhile, the cyclic stability tests reveal the excellent durability of Pd@PtRuNi NWs, whose mass activity is only 13.58% degradation after accelerated durability tests. The catalytic activity and durability towards ORR are better than the U.S. 2025 DOE target (0.44\,{\rm{A}}\,{{\rm{mg}}}_{{\rm{pt}}}^{-1} and less than 40% activity attenuation at 0.9 V after 30 000 potential cycles). The elevated catalytic properties can be traceable to the synergism between the ligand effect of Ni and Ru and one-dimensional structure superiority, which optimizes the electronic structure of active sites, promotes the charge transfer and restrains the agglomeration and detachment.
研究领域:
材料科学
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能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Zhen He,Qiaohui Duan,Chengming Wang,Lingwen Liao
A highly active surface can endow the electrocatalysts with extraordinary catalytic performances. However, it remains challenging to tailor the atomic packing characteristics and thus the physical and chemical characteristics of the electrocatalysts . Herein, penta-twinned Pd nanowires (NWs) with abundant high-energy atomic steps (i.e., stepped Pd) are synthesized by seeded synthesis on Pd NWs enclosed by (1 0 0) facets. Benefiting from the catalytically active atomic steps, such as [ n (1 0 0) × m (1 1 1)] on the surface, the resultant stepped Pd NWs can work as an effective electrocatalyst for the ethanol oxidation reaction (EOR) and ethylene glycol oxidation reaction (EGOR), which are essential anode reactions in direct alcohol fuel cells (DAFCs). Compared with commercial Pd/C, the Pd nanowires bound by (1 0 0) facets and atomic steps both display enhanced catalytic activity and stability towards the EOR and EGOR. Importantly, the mass activities of the stepped Pd NWs toward the EOR and EGOR are 6.38 and 7.98 A mg Pd −1 , which are 3.1 and 2.6 times those of Pd NWs enclosed by (1 0 0) facets, respectively. Besides, our synthetic strategy also enables the formation of bimetallic Pd-Cu nanowires with abundant atomic steps. This work not only demonstrates a simple yet effective strategy to obtain mono- or bi-metallic nanowires with abundant atomic steps, but also highlights the significant role of atomic steps for boosting the activity of electrocatalysts.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMISTRY OF MATERIALS
·
2014
·
IF 8.535
Na Lu,Wei Chen,Guoyong Fang,Bi Chen,Keqin Yang,Yun Yang,Zhencai Wang,Shaoming Huang,Yadong Li
We report that 5-fold twinned nanowires and single twinned right bipyramids of Pd with high yields can be selectively synthesized in a hydrophilic system with the assistance of acetonitrile and ethanol, respectively. The controlled synthesis is based on an idea that small organic molecules (SOMs) that can attract halide ions via electrostatic interactions of different strengths could well adjust their activity to tune the etching degree of O2/halides for protecting the twinned Pd crystal nucleus. We consider that relatively stronger interaction between acetonitrile and halide ions for the formation of nanowires is due to the existence of three C–Hδ+ bonds induced by the electron-withdrawing CN group of CH3CN, which is confirmed by an as-called iodine starch test, 1H nuclear magnetic resonance spectra, and theoretical calculations. On the basis of this finding, we then have successfully expanded SOMs to other molecules, including acetone, 1,4-dioxane, and 1,3,5-trioxane, which have a function similar to that of acetonitrile for the production of Pd nanowires, and 2-propanol, which has a function similar to that of ethanol for the fabrication of right bipyramids. Although nanowires and bipyramids are both mainly bound by {001} planes, nanowires show better catalytic performance toward the reduction of 4-nitrophenol, indicating that more twin boundaries could offer more active catalytic sites. This work not only provides new information to decrease the degree of etching of O2/halides for controlling twin structure of noble metals but also supports the idea that creating a twin structure is good for enhancing catalytic activity.
研究领域:
材料科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2016
·
IF 7.145
Maoqiang Chi,Guangdi Nie,Yanzhou Jiang,Zezhou Yang,Zhen Zhang,Ce Wang,Xiaofeng Lu
Here, we report a simple one-step procedure to fabricate coaxial Te@poly(3,4-ethylenedioxythiophene) (PEDOT) nanocables via a self-assembly redox polymerization between 3,4-ethylenedioxythiophene monomer and the oxidant of sodium tellurite without the assistance of any templates and surfactants. The as-synthesized Te@PEDOT coaxial nanocables have diameters of center cores in the range of 5–10 nm, and the size of the outer shell from several nanometers to 15 nm. More interestingly, the as-prepared Te@PEDOT nanocables can be converted to Pd@PEDOT nanocables via a galvanic replacement reaction. The center core of the Pd nanowire exhibits a high crystallinity. The application of the synthesized Pd@PEDOT nanocables as peroxidase-like catalysts for the colorimetric detection of H2O2 is reported. The synergistic effect between the Pd nanowire and electrically conducting PEDOT enhances the catalytic activity toward the oxidation of the peroxidase substrate 3,3′,5,5′-tetramethylbenzidine in the presence of H2O2. A detection limit toward H2O2 is as low as 4.83 μM, and a linear range from 10 to 100 μM has been achieved. This work offers a potential versatile route for the fabrication of cable-like nanocomposites with conducting polymers and other active components, which display great promise in applications such as catalysis, nanoelectronic devices, and energy storage and conversion.
研究领域:
材料科学
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生物催化
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纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Biology-Basel
·
2024
·Vol. 13
·期 12
·960
·
IF 3.6
Kuo Yang,Jueyu Wang,Ying Zhang,Daizong Cui,Min Zhao
Simple SummaryThis study proposed a new method for extractingE. coliflagella, which served as a template for synthesizing palladium (Pd) nanowires. By improving the flagella extraction process, we successfully produced Pd nanowires with better structure and function, which could have important applications in technology and medicine. Traditional methods often led to impurities that interfered with nanomaterial synthesis, but our method provided a cleaner and more efficient way of producing high-quality nanowires. UsingE. coliflagella as a template offered environmental benefits, as it eliminated the need for toxic chemicals and reduced energy consumption. This eco-friendly approach was also safer and more reliable for practical applications. Our research also showed how the functional groups on the flagella surface helped form strong bonds with metals, improving the nanowire formation process. This study highlighted the potential of using biological templates for nanomaterial synthesis, contributing to the development of greener and more efficient technologies.In recent years, the use of bacterial flagella as biomimetic templates has gained increasing attention in nanomaterial synthesis due to their unique structural and functional properties. In this study, we optimized the flagella extraction method and achieved a high concentration of flagella solution. Flagella were isolated fromEscherichia coli. Surface characterization revealed that the flagella had abundant functional groups, such as amino and carboxyl groups, which can serve as nucleation sites for the controlled nucleation and growth of metal nanomaterials. Using bacterial flagella as a template, we synthesized one-dimensional palladium nanowires (Fla-Pd NWs). The results of morphological and phase analyses showed that the synthesized palladium nanoparticles were uniformly and densely distributed on the surface of the flagella. Moreover, the Fla-Pd nanowires exhibited superior electrocatalytic activity, which was applied to develop an electrochemical biosensor. This biosensor was used to detect the early breast cancer biomarker microRNA-21 and exhibited a linear range of 0.66–1.98 µmol/L and a detection limit of 0.78 µmol/L. The method demonstrated high selectivity and reusability, making it a promising strategy for early cancer diagnosis.
研究领域:
纳米材料
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生物医学工程
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癌症诊断
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Tao Chen,Manli Wang,Donghang Hu,Qianlin Ju,Kaige Zhao,Liang Fu,Zelin Chen,Xiaolong Yu,Changjiu Li
The mainstream electrocatalysts for direct ethanol fuel cells (DEFCs) are Pt- or Pd-based nanomaterials, which are severely hampered by CO intermediate poisoning and the relatively low selectivity of the C1 pathway in anodic ethanol oxidation reaction (EOR), thereby impeding the efficiency enhancement and practical application of DEFCs. Herein, we report a Pt-decorated amorphous PdS nanowire [denoted as a-Pd(S)NWs/Pt] catalyst with abundant crystalline/amorphous heterogeneous interfacial active sites for alkaline EOR. The a-Pd(S)NWs/Pt was demonstrated a superior EOR mass activity of 6.16 A·mgPd+Pt–1, which is 22.81 times over that of commercial Pt/C (0.27 A·mgPt–1) and 34.22 times over that of commercial Pd/C (0.18 A·mgPd–1). Additionally, the a-Pd(S)NWs/Pt exhibited considerable stability, significantly enhanced resistance to CO poisoning and enhanced selectivity for the EOR C1 pathway. Density functional theory calculations and experimental results further revealed that the optimized COads and OHads binding energies due to the decoration of Pt nanoclusters can be responsible for the enhanced CO resistance and C1 selectivity of a-Pd(S)NWs/Pt. Furthermore, benefiting from its optimized electronic configuration at the interfacial active sites and the appropriate intermediate adsorption capacity, the a-Pd(S)NWs/Pt electrocatalyst was successfully extended to the electrocatalytic methanol and ethylene glycol oxidation reaction systems.
研究领域:
材料科学
·
电化学
·
催化
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产品关联
DOI
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2020
·Vol. 412
·期 25
·6849-6858
·
IF 3.637
Li Zhi,Qian Weina,Guo Hui,Song Xiao,Yan Hao,Jin Ruyi,Zheng Jianbin
In this study, novel Pd nanowire networks (PdNW) grown on three-dimensional polyaniline hydrogel (3D-PANI) were prepared via a facile one-step electrodeposition approach at a constant potential of − 0.2 V and further utilized as an electrochemical sensing material for sensitive determination of glucose in alkaline medium. Compared with the sensor based on Pd nanofilm (PdNF)/3D-PANI prepared by electrodeposition at − 0.9 V, the sensor based on PdNW/3D-PANI presented substantially enhanced electrocatalytic activity towards glucose oxidation, with an excellent sensitivity of 146.6 μA mM −1 cm −2 , a linear range from 5.0 to 9800 μM, and a low detection limit of 0.7 μM and was, therefore, demonstrated to be available for the determination of glucose in human serum. These findings are likely attributed to the combination of advantages of both PdNW and 3D-PANI, which outperformed most other Pd-based non-enzymatic glucose sensors reported earlier. Moreover, this non-enzymatic electrochemical sensor based on PdNW/3D-PANI may serve as an alternative tool for the assay of glucose and possibly other biomolecules.
Graphical abstract
研究领域:
分析化学
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生物医学工程
·
材料科学
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产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Mengxiao Zhong,Maoqiang Chi,Fuqiu Ma,Yun Zhu,Ce Wang,Xiaofeng Lu
In recent years, a significant challenge in material science has been to fabricate novel functional nanomaterials to mimic the function of natural enzymatic systems. Herein, ternary polyaniline (PANi)–MnO2–Pd nanowires (NWs) are synthesized through a two-step redox reaction process. The prepared PANi–MnO2–Pd NWs were explored to exhibit dual responsive enzyme-like efficiencies, e.g., peroxidase and oxidase-like activities. With the assistance of H2O2, the obtained ternary PANi–MnO2–Pd NWs were able to oxidize the typical peroxidase substrate of 3,3′,5,5′-tetramethylbenzidine (TMB) to yield the oxidized TMB with a blue color, exhibiting a much better peroxidase-like activity than the synthesized PANi–MnO2 NWs alone and Pd nanoparticles owing to the interfacial electron transfer effect among the components. In addition, in the absence of H2O2, the prepared PANi–MnO2–Pd NWs could also oxidize TMB to display an excellent oxidase-like activity. Based on the dual responsive enzyme-like characteristic of the obtained ternary PANi–MnO2–Pd NWs, a rapid and applicative colorimetric way to sensitively determine l-cysteine and ascorbic acid (AA) has been developed. The limits of detection based on the two systems were estimated to be as low as 118 and 34 nM, respectively. We believe that the prepared ternary PANi–MnO2–Pd NWs with both peroxidase and oxidase-like activities will show broad potential applications in bioscience and bioengineering.
研究领域:
材料科学
·
生物传感器
·
生物工程
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2019
·
IF 6.35
Shuzhen Lv,Kangyao Zhang,Ling Zhu,Dianping Tang,Reinhard Niessner,Dietmar Knopp
With the introduction of gas-based contactless electrochemical biosensors lies the prospects of separating the sensing interface from the bioassembly platform, enhancing stability, and exploring signal transduction mechanism, all intimately linking to development of immunoassay. Herein, we report on a H2-based electrochemical biosensor whose signals derived from the chemical signal transduction between a H2 and Pd nanowires@ZIF-67 (ZIF: Zeolitic Imidazolate Frameworks) bilayered sensing interface for immunoassay. Dendritic Pt nanoparticles (DPNs) conjugated on the detection antibody were introduced on the interface of a magnetic microsphere according to an immune sandwich assembly between the antigen and antibody. H2 as a bridge originates from DPNs catalyzing NH3BH3 and links biological signals to electrical signals by reacting with Pd nanowires. Nevertheless, the response of Pd nanowires being extremely effected by O2 in air due to the competitive adsorption on the surface of Pd nanostructures as well as the reaction between chemisorbed O (Pd–O) and adsorbed dihydrogen lead to a decrease in H absorption into PdHx and poor sensing responses under low target concentration. Porous ZIF-67 (window aperture 0.331 nm) as a molecular sieve self-assembling on the surface of the Pd nanowires film could easily permeate H2 (kinetic diameter of 0.289 nm), while interferential O2 (kinetic diameter of 0.346 nm) has difficultly passing through the ZIF-67 layer to contact Pd nanowires and achieves a response of a lower concentration target as well as faster response rate. Under optimal conditions, H2-based electrochemical biosensors exhibit great response toward target alpha-fetoprotein (AFP) within a dynamic working range of 0.1–50 ng mL–1 at a detection limit of 0.04 ng mL–1. Our strategy provides a reusable sensing interface, high specificity, and acceptable accuracy for the immunoassay. In addition, it also expands a promising platform for application as a molecular sieve in electrochemical biosensors.
研究领域:
生物传感器
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纳米技术
·
分析化学
·
材料科学
·
生物医学工程
✓ 已验证
DOI
PubMed
高影响因子
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