RSC Advances
·
2016
·Vol. 6
·期 31
·25877-25881
·
IF 3.289
Ling Li,Mingkun Wang,Ning Cui,Yuedi Ding,Qingling Feng,Wenming Zhang,Xiaowei Li
Incorporation of nanophase ceria into the cathode catalyst Pt/C was used as alternative cathode catalysts for the oxygen reduction reaction in an air-cathode single-chamber microbial fuel cell (SCMFC) for the first time. Electrochemical results reveal that the ceria doped Pt/C catalysts exhibited a higher catalytic performance than the pure Pt/C catalyst. The highest voltage of 580 mV and the maximum power density of 840 ± 24 mW m−2 were achieved from the 3 wt% CeO2 doped Pt/C cathode, which was larger than that of the pure Pt/C cathode.
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JOURNAL OF CATALYSIS
·
2016
·
IF 7.354
Bao Zhang,Jun Li,Yuying Gao,Ruifeng Chong,Zhiliang Wang,Lin Guo,Xianwen Zhang,Can Li
Photocatalytic oxidation reactions provide a promising strategy for green synthesis of fine chemicals. However, the low photocatalytic efficiency and selectivity are the main obstacles. Herein, we report the ultrathin Bi 2 MoO 6 nanoplates with thickness of ∼17 nm which exhibit a superior performance in alcohol oxidation to corresponding aldehyde using O 2 under visible light irradiation, achieving ca. 29 times enhancement of activity compared with Bi 2 MoO 6 synthesized from traditional hydrothermal method (thickness of ∼250 nm). When Pt nanoparticles as cocatalyst are loaded on the surface of the ultrathin Bi 2 MoO 6 nanoplates, the photocatalytic performance is further enhanced. The remarkable enhancement of activity is attributed to the ultrathin 2D geometry of Bi 2 MoO 6 nanoplates, promoting the charge-separation efficiency and affording abundant catalytically active sites. The excellent selectivity of photocatalytic oxidation of benzyl alcohol on the ultrathin Bi 2 MoO 6 is attributed to the different adsorption behaviors of benzyl alcohol and benzaldehyde. This study could also provide an efficient strategy for improving the photocatalytic performance by rational fabrication of two-dimensional semiconductor materials for organic synthesis.
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MICROCHIMICA ACTA
·
2016
·Vol. 184
·期 2
·423-429
·
IF 4.831
Jiao Lei,Mu Zonggang,Miao Luyang,Du Wenwen,Wei Qin,Li He
A dual enhancing strategy has been employed to develop a sandwich type of electrochemical immunoassay for the prostate specific antigen (PSA). The signal is enhanced by using Pt-Cu hierarchical trigonal bipyramid nanoframes (HTBNFs) and a composite consisting of Fe 3 O 4 nanoparticles and reduced graphene oxide in polydopamine that serve to capture the primary antibody (Ab1). This nanocomposite shows better electrical conductivity than Fe 3 O 4 and reduced graphene oxide (RGO), respectively, alone. The Pt-Cu HTBNFs were used to label the secondary antibody (Ab2) and act as tags for signal amplification by virtue of their outstanding electrochemical reduction activity towards H 2 O 2 . At a working potential of +0.1 V (vs. SCE), the interference by dissolved oxygen can be avoided. This immunoassay is highly sensitive, with a linear range that extends from 0.1 pg⋅mL −1 to 5 ng⋅mL −1 and an ultralow detection limit of 0.03 pg⋅mL −1 .
Schematic of the dual amplification strategy in the immunosensor for the prostate specific antigen (PSA) that is based on the use of a first antibody (Ab 1 ) conjugated to a Fe 3 O 4 -reduced graphene oxide nanocomposite (Fe 3 O 4 -RGO), and of Pt-Cu trigonal bipyramid nanoframes as a label for the second antibody (Ab 2 ).
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ANALYTICA CHIMICA ACTA
·
2016
·
IF 4.712
Long Wu,Wenmin Yin,Kun Tang,Dian Li,Kang Shao,Yunpeng Zuo,Jing Ma,Jiawei Liu,Heyou Han
A new electrochemical method has been proposed for the simultaneous determination of butylated hydroxyanisole (BHA) and propyl gallate (PG) in food matrices based on enzymatic biosensors . Spiny Au-Pt nanotubes (SAP NTs) was first synthesized and demonstrated to exhibit intrinsic peroxidase and catalase-like activity. The structure of SAP NTs provides large surface area and favorable medium for electron transfer , on which HRP were immobilized and acted as enzymatic biosensor for the simultaneous detection of BHA and PG. The results revealed that BHA and PG both have well-defined oxidation waves with peak potentials of 624 and 655 mV, respectively. Under the optimal conditions, the method behaved satisfactory analytical performance towards BHA and PG with a wide linear range of 0.3–50 mg L −1 and 0.1–100 mg L −1 , as well as a detection limit of 0.046 mg L −1 and 0.024 mg L −1 (3σ/slope), respectively. Besides, the proposed method exhibits good sensitivity, stability and reproducibility, providing an alternative to fabricate electrode and construct sensitive biosensors.
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PubMed
高影响因子
TALANTA
·
2016
·
IF 4.035
Shan Shan Miao,Mei Sheng Wu,Li Ya Ma,Xiao Jing He,Hong Yang
A novel and highly sensitive electrochemiluminescence (ECL) biosensing system was designed and developed for individual detection of different organophosphorous pesticides (OPs) in food samples. Bimetallic Pt-Au nanoparticles were electrodeposited on multi-walled carbon nanotubes (MWNTs)-modified glass carbon electrode (GCE) to increase the surface area of electrode and ECL signals of luminol. Biocomposites of enzymes from acetylcholinesterase and choline oxidase (AChE and ChOx) were immobilized onto the electrode surface to produce massive hydrogen peroxides (H 2 O 2 ), thus amplifying ECL signals. Based on the dual-amplification effects of nanoparticles and H 2 O 2 produced by enzymatic reactions , the proposed biosensor exhibits highly sensitivity. The proposed biosensing approach was then used for detecting OPs by inhibition of OPs on AChE. Under optimized experimental conditions, the ECL intensity decreased accordingly with the increase in concentration of OPs, and the inhibition rates of OPs were proportional to their concentrations in the range of 0.1–50 nmol L −1 for malathion , methyl parathion and chlorpyrifos, with detection limit of 0.16 nmol L −1 , 0.09 nmol L −1 and 0.08 nmol L −1 , respectively. The linearity range of the biosensor for pesticide dufulin varied from 50 to 500 nmol L −1 , with the detection limit of 29.7 nmol L −1 . The resulting biosensor was further validated by assessment of OPs residues in cabbage, which showed a fine applicability for the detection of OPs in the realistic sample.
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高影响因子
Nanoscale
·
2017
·Vol. 9
·期 31
·11077-11084
·
IF 7.367
Yalin Xiong,Yanling Ma,Junjie Li,Jingbo Huang,Yucong Yan,Hui Zhang,Jianbo Wu,Deren Yang
Bimetallic nanocrystals with a branched shape have received great interest as catalysts due to their unique structures and fascinating properties. However, the conventional synthetic approaches based on the island growth mode often lead to the dendritic nanostructures with inhomogeneous and uncontrolled branches. Here precise control over the number of branches has been realized in the deposition of Pt on Pd seeds through the Stranski–Krastanov growth mechanism. Based on such a growth mode, Pd@Pt core–shell hexapods and octapods have been generated by a seeded growth with Pd octahedra and cubes as the seeds, respectively. We found that Pt atoms are initially deposited on the side faces of Pd seeds through a layer-by-layer epitaxial growth in the presence of oleylamine (OAm), leading to a local strain focused at their corners. These strain-concentrated sites promote the subsequent island growth of Pt atoms at the corners of the Pd seeds, resulting in the Pd@Pt core–shell hexapods or octapods. Both the Pd@Pt core–shell hexapods and octapods exhibit the substantially enhanced catalytic properties in terms of activity and stability towards a methanol oxidation reaction (MOR) relative to the commercial Pt/C. Specifically, the Pd@Pt core–shell hexapods show the highest specific (1.97 mA cm−2) activity and mass activity (0.52 mA μgPt−1) for the MOR, which are 5.8 and 2.6 times higher than those of the commercial Pt/C, respectively. This enhancement can probably be attributed to their unique structures and the synergistic effect between Pt and Pd.
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Nanoscale
·
2017
·Vol. 9
·期 28
·10138-10144
·
IF 7.367
Binbin Jiang,Fan Liao,Yuyang Sun,Yafei Cheng,Mingwang Shao
Cost-effective catalysts for electrocatalytic water splitting play a key role in the renewable energy research. Although Pt has been regarded as the best catalyst, its wide applications have been impeded by its high cost and scarce natural abundance. Therefore, decreasing the Pt usage for electrocatalyst design is significant toward the hydrogen evolution reaction (HER). Herein, flower-like Pt nanocrystals were loaded on the surface of nitrogen-doped graphene using Si nanowires as the sacrificial template. The experimental results showed that the optimal Pt nanocrystals/N-doped graphene with superior HER activity and excellent stability only has a low Pt loading of 5.0 wt%. It is noted that the HER mass activity of the Pt nanocrystals/N-doped graphene is 5 fold higher than that of the 20.0 wt% Pt/C commercial catalyst. This optimal catalyst also achieved a low Tafel slope (28.0 mV dec−1), large apparent exchange current density (0.989 mA cm−2) and high turnover frequency (2.05 s−1). This work may provide an effective avenue for developing highly efficient electrochemical catalysts for the HER.
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RSC Advances
·
2017
·Vol. 7
·期 34
·21145-21152
·
IF 3.108
Bingfeng Chen,Fengbo Li,Guoqing Yuan
Selective hydrodeoxygenation of 5-hydroxy-2(5H)-furanone (HFO) derived from furfural oxidation to γ-butyrolactone (GBL) provides a sustainable alternative to the petroleum-based process for γ-butyrolactone production. Furfural is first converted to HFO through selective photocatalytic oxidation by using air oxygen as the oxidant (yield: 85.0%). HFO is further converted to GBL through hydrodeoxygenation over noble-metal nanoparticles on mesoporous Nb–Zr mixed oxides. The conversion of HFO to GBL involves two reactions: hydrogenation catalyzed by active metal and dehydration over mesoporous solid acids. The catalytic properties of M/Nb–Zr mixed oxides (M = Pt, Ir, Ru, Rh and Pd) are related to the composition of support and active metal. The incorporation of zirconia into matrixes improves the thermal stability of mesoporous mixed oxides and increases the amounts of surface acid, which contributes to its catalytic selectivity to GBL. Pt/Nb5Zr5-550 exhibited the best catalytic performances with 97.3% selectivity of GBL at full conversion. The excellent performance can be correlated with the cooperative effect between active metal species and acid sites. The Pt-solid acid bifunctional catalysts show superior catalytic performance compared with conventional catalysts, such as Pt/H-ZSM-5, Pt/C, Rh/C or Pd/C. An overall GBL yield of 82.7% from furfural was obtained.
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Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 19
·9233-9240
·
IF 8.867
Jun Jiang,Han Gao,Shu Lu,Xing Zhang,Chu-Ya Wang,Wei-Kang Wang,Han-Qing Yu
Fabrication of non-Pt high-performance oxygen reduction reaction (ORR) catalysts is essential for the application of fuel cells. In this work, monodisperse bimetallic Ni–Pd core–shell nanoparticles (NPs) with tunable shell compositions and contents were synthesized by using a modified one-pot colloidal approach and characterized. Also, the core shell structure dependence of their ORR performance without the interruption of an intermetallic phase was explored. The core–shell structured catalysts (Ni@Pd3/C NPs) exhibited a robust ORR activity and stability with a high onset potential of 0.99 V, a half-wave potential of 0.87 V and an average electron transfer number of 3.91 in 0.1 M HClO4. Furthermore, a high onset potential of 0.98 V, a half-wave potential of 0.86 V and an average electron transfer number of 3.98 were achieved in 0.1 M KOH. These results are comparable to those of the commercially available Pt/C catalysts. Moreover, the catalysts also maintained a good long-term cycling stability in both acidic and alkaline electrolytes. Thus, this work demonstrates that the ORR performance of the Ni–Pd alloy could be boosted through constructing the core–shell structure with a Pd-enriched surface and the Ni–Pd model alloy could be further applied to assess the role of the Pd-based core–shell structure in other electrochemical catalytic reactions.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2017
·
IF 5.401
Long Wu,Wenmin Yin,Xuecai Tan,Pan Wang,Fan Ding,Huan Zhang,Biru Wang,Weiyun Zhang,Heyou Han
It is attractive but remains challenging to develop nanomaterials-based methods to realize the colorimetric detection of ultratrace biological analytes. In this work, an HAuCl 4 -H 2 O 2 system was developed for the visual detection of intracellular hydrogen peroxide (H 2 O 2 ) based on the Au-Pt/SiO 2 sensing platform. Owing to their excellent intrinsic peroxidase-like activity, Au-Pt/SiO 2 nanospheres were introduced to catalyze the decomposition of H 2 O 2 and then directly reduce HAuCl 4 into gold nanoparticles (Au NPs) for the naked-eye detection. The produced Au NPs behaved color variations from light purple to wine red as H 2 O 2 concentration increased. Under the optimal conditions, this strategy showed excellent sensitivity for H 2 O 2 with a detection limit of 0.1 nM by naked-eye readout and 0.1 pM by UV–vis spectrometer (S/N = 3), as well as acceptable selectivity for H 2 O 2 , which could meet the demand for the detection of H 2 O 2 in biological systems. The method was further validated by the determination of H 2 O 2 in HeLa cells with low cellular cytotoxicity. Thus, this strategy would provide simple and sensitive detection of H 2 O 2 in biological systems, revealing the potential application in clinical, biological and environmental researches.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Jiang-Hao Lu,Ze Li,Di Zhang,Lu-Hang Song,Xiao-Yan Cai,Liang Mao,Zhi-Qiang Liu,Zhi-Jie Wang,Xiu-Quan Gu,Guo-Dong Yuan
The nano/microstructuring of silicon (Si) via chemical methods has garnered significant attention due to its excellent light-trapping capabilities across a wide spectral range. Current research has predominantly focused on the synthesis of pyramidal-shaped microtextures, which enable two reflections on the surface, while largely overlooking the superior light-trapping potential of inverted pyramid silicon (SiIP) microtextures, which theoretically allow for three reflections. Moreover, there has been limited investigation into the application of inverted pyramid black silicon for solar-driven hydrogen evolution. This study reports the synthesis of uniformly arranged inverted pyramid-textured black silicon using the copper-assisted chemical etching (Cu-ACE) method to enhance the efficiency of solar-driven water splitting for hydrogen production. The formation mechanism and the influence of copper-localized surface plasmon resonance (Cu-LSPR) from Cu nanoparticle (NP) byproducts on photoelectrochemical (PEC) activity were systematically analyzed. To reduce sidewall defects and minimize photogenerated carrier recombination, the surface of the SiIP was treated with tetramethylammonium hydroxide (TMAH). A vertical PN junction was developed through ion implantation to reduce the external bias of the SiIP. Additionally, a uniform TiO₂ antireflective layer was deposited via atomic layer deposition (ALD), reducing the average reflectance of the SiIP-T 4 to 5.78 % over the 300–1100 nm wavelength range. MoSₓ and Pt NPs were electrodeposited to improve the fill factor and enhance HER kinetics. With optimized catalyst loading, the n + p-SiIP-T 4 /TiO₂/Pt 80 mC electrode achieved a photocurrent density of 8.0 mA cm −2 at 0 V vs. RHE, an applied bias photon-to-current efficiency (ABPE) of 0.93 % at 0.24 V vs. RHE, and a double-layer capacitance (Cdl) of 91 μF cm −2 . The onset potential (Von) was positively shifted by ∼1.13 V to 0.49 V vs. RHE compared to a SiIP photocathode, and the photocathode operated continuously at 0 V vs. RHE for 27 h in an acidic electrolyte. These results demonstrate that SiIP has significant potential for PEC hydrogen evolution, with further performance optimization achievable through structural and surface engineering.
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Energy & Environmental Science
·
2024
·Vol. 17
·期 14
·5227-5240
·
IF 32.4
Changle Yue,Chao Feng,Guangxun Sun,Na Liu,Haoyuan Hao,Wenjing Bao,Xiaowei Zhang,Fengyue Sun,Cong Zhang,Jiahui Bi,Yan Zhou,Hsiao-Chien Chen,Yuan Pan,Daofeng Sun,Yukun Lu
Tuning and stabilizing the chemical microenvironment of Pt-based single-atom catalysts is a major challenge in promoting an electrocatalytic hydrogen evolution reaction (HER). Herein, we constructed a hierarchical stabilization system of Pt single-atoms via defect substitution using the polyoxometalate (POM) (NH4)4[ZnMo6O24H6] (ZnMo6) as a template. The well-defined structure of ZnMo6 led to precise local Zn sublimation during the formation of Mo2C, which was converted from the Mo6 ring in situ. The localized defect provides a well-defined Mo(C)–Pt–N coordination environment to trap Pt single-atoms. The obtained single-atom catalyst (PtSA@Mo2C@NC) exhibited a superior and stable electrochemical HER performance with an unprecedented mass activity of 75.21 A mgPt−1 in 0.5 M H2SO4. In-depth theoretical calculation analysis revealed that Mo(C)–Pt–N coordination provides a moderated charge state and low d-band center of the Pt site, thus significantly promoting proton adsorption and H2 desorption. This work demonstrates a promising single-atom stabilization strategy for constructing high-performance HER electrocatalysts through the precise modulation of a three-dimensional chemical environment.
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