ELECTROANALYSIS
·
2015
·Vol. 28
·期 2
·304-311
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IF 2.138
Bingxin Wang,Cui Ye,Xia Zhong,Yaqin Chai,Shihong Chen,Ruo Yuan
A new electrochemical biosensor was developed for organophosphorus pesticides (OPs) and huperzine-A (hupA) detection based on Pd wormlike nanochains/graphitic carbon nitride (Pd WLNCs/g-C 3 N 4 ) nanocomposites and acetylcholinesterase (AChE). The morphologies and components of the nanocomposites were analyzed by transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). The Pd WLNCs/g-C 3 N 4 nanocomposites could effectively immobilize enzymes and promote the signal amplification. Under the optimum condition, the proposed biosensor displayed well performance. The linear response ranges for the determination of OPs and hupA were 1.00 nM to 14.96 µM and 3.89 nM to 20.80 µM, respectively. The corresponding detection limits were 0.33 nM and 1.30 nM (S/N=3). Meanwhile, the biosensor owned good reproducibility and stability, and could also be applied to analyze practical samples, which would be a new hopeful method for pesticide analysis.
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BIOSENSORS & BIOELECTRONICS
·
2015
·
IF 6.409
Qian Zhou,Youxiu Lin,Yuping Lin,Qiaohua Wei,Guonan Chen,Dianping Tang
In this work, a sensitive and specific electrochemical biosensor for lead ion (Pb 2+ ) detection was developed by coupling with synergetic catalysis of porous Au–Pd bimetallic nanoparticles and hemin/G-quadruplex-based DNAzyme. In the presence of target Pb 2+ , the substrate strand was cleaved and the enzyme strand was released. Subsequently, G-rich DNA-labeled Au–Pd bimetallic nanoparticle was linked with the released enzyme strand through the helper DNA . Upon addition of hemin , a large number of hemin/G-quadruplex-based DNAzyme molecules were formed on the electrode to serve as nicotinamide adenine dinucleotide hydrogen (NADH) oxidase and peroxidase mimics. DNAzyme could catalyzed the reduction of H 2 O 2 , generated from NADH in the presence of O 2 , to produce an electrochemical signal when using thionine as the electron mediator. Introduction of porors Au–Pd bimetallic nanoparticles could enhance the detectable signal and cause the increase in the sensitivity. Experimental results showed that the variations (∆ I ) in the cathodic peak currents of the biosensor were linearly dependent on target Pb 2+ concentrations from 1.0 pM to 100 nM with a detection limit (LOD) of 0.34 pM. The excellent performance of the sensing platform indicated its promising prospect as a valuable tool for simple and cost-effective Pb 2+ detection in practical application.
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APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Xueliang Cui,Yunfeng Zheng,Meng Tian,Zhengping Dong
A novel yolk–shell-structured material (Fe 3 O 4 @γ-AlOOH-YSMs) with hierarchical γ-AlOOH flakes as the mesoporous shell and Fe 3 O 4 nanoparticles (NPs) in the hollow core was prepared by using Fe 3 O 4 @SiO 2 NPs as the seeds as well as NaAlO 2 and urea as the precursor. The prepared Fe 3 O 4 @γ-AlOOH-YSMs were used as a catalyst support for fabricating a Pd/Fe 3 O 4 @γ-AlOOH-YSMs nanocatalyst with no obvious aggregation of the Pd NPs. The Pd/Fe 3 O 4 @γ-AlOOH-YSMs nanocatalyst was utilized for the catalytic reduction of the widely used and highly toxic 4-nitrophenol, rhodamine B, methylene blue, and methyl orange; and showed excellent catalytic activity as compared with other noble-metal-based catalysts. Furthermore, the Pd/Fe 3 O 4 @γ-AlOOH-YSMs nanocatalyst also can be easily separated from the reaction mixture and reused for at least ten times without any obvious decrease in the catalytic activity, indicating its reusability and stability.
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APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Shuaishuai Ding,Chunhua Zhang,Yefei Liu,Hong Jiang,Rizhi Chen
Highly efficient Pd@CN catalysts for selective hydrogenation of phenol to cyclohexanone in water were successfully fabricated by loading Pd nanoparticles (NPs) in N-doped carbons (CN) derived from ZIF-67 with dicyandiamide (DICY) as the additional nitrogen source. For comparison, polyvinylpyrrolidone (PVP) was also used as the additional nitrogen source during the ZIF-67 synthesis. The results showed that the PVP and DICY had significantly different impacts on the microstructures of as-obtained CN materials and the catalytic performance of Pd@CN catalysts in the phenol hydrogenation. The addition of DICY had the positive promotion effect on the surface area of the obtained CN materials. Moreover, the introduction of DICY could increase the nitrogen content of CN and then prevent the re-oxidation of Pd NPs during air contact, resulting in higher Pd 0 ratio. In comparison with PVP, the DICY was more suitable as the additional nitrogen source for the formation of CN and Pd@CN (Pd@CN D , Pd@CN P ). The Pd@CN D exhibited superior catalytic activity as compared to Pd@CN P (phenol conversion 96.9% vs. 67.4%). More importantly, the as-prepared Pd@CN D catalyst could be reused for four times without catalytic performance reduction. The work would aid the development of Pd@CN catalysts with superior catalytic properties.
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CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Shuang Zheng,Pengyong Yang,Fumin Zhang,De-Li Chen,Weidong Zhu
Pd nanoparticles encaged within an amine-functionalized metal-organic framework (MOF), Pd@NH 2 -UiO-66, was successfully prepared via one pot direct construction of the MOF framework, cooperative in situ metal precursor incorporation followed by on-site moderate reduction process. Because of its abundant of nanocages accessible through small pore windows, as well as excellent coordination capability of metal ions sites from the amine groups within the NH 2 -UiO-66 matrix, the Pd nanoparticles were homogeneously confined within its cavities. Intriguingly, the prepared Pd@NH 2 -UiO-66 exhibits a high catalytic activity and exclusive selectivity in the liquid-phase hydrogenation of 2,3,5-trimethylbenzoquinone (TMBQ) to 2,3,5-trimethylhydroquinone (TMHQ), a key vitamin-E intermediate in a short period under relatively mild reaction conditions. Additionally, this catalyst was recycled up to 8 times without significant loss in both activity and selectivity. Furthermore, reaction mechanism was investigated using dispersion corrected density functional theory calculations, suggesting that the superior performance of Pd@NH 2 -UiO-66 could be ascribed to the cooperation between the Pd nanoparticle and the amine-functionalized UiO-66. This MOF-based composite shows great potential as heterogeneous catalyst for the catalytic hydrogenation reactions due to its high stability, excellent catalytic properties, and simple preparation.
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DALTON TRANSACTIONS
·
2017
·Vol. 46
·期 22
·7210-7218
·
IF 4.029
Wenhui Liu,Qi Wang,Yan Zheng,Shubin Wang,Yan Yan,Yanzhao Yang
In this study, a method of one-step separation and recycling of high purity Pd(II) and Pt(IV) using an ionic liquid, 1-butyl-3-benzimidazolium bromate ([HBBIm]Br), was investigated. The effects of [HBBIm]Br concentration, initial metal concentration, and loading capacity of [HBBIm]Br were examined in detail. It was observed that [HBBIm]Br was a very effective extractant for selectively extracting Pd(II) and precipitating Pt(IV). Through selectively extracting Pd(II) and precipitating Pt(IV), each metal with high purity was separately obtained from mixed Pd(II) and Pt(IV) multi-metal solution. The method of one-step separation of Pd(II) and Pt(IV) is simple and convenient. The anion exchange mechanism between [HBBIm]Br and Pt(IV) was proven through Job's method and FTIR and 1H NMR spectroscopies. The coordination mechanism between [HBBIm]Br and Pd(II) was demonstrated via single X-ray diffraction and was found to be robust and distinct, as supported by the ab initio quantum-chemical studies. The crystals of the [PdBr2 ·2BBIm] complex were formed first. Moreover, the influence of the concentrations of hydrochloric acid, sodium chloride, and sodium nitrate on the precipitation of Pt(IV) and extraction of Pd(II) was studied herein. It was found that only the concentration of H+ could inhibit the separation of Pt(IV) because H+ could attract the anion PtCl62−; thus, the exchange (anion exchange mechanism) between the anions PtCl62− and Br− was prevented. However, both the concentration of H+ and Cl− can obviously inhibit the extraction of Pd(II) because H+ and Cl− are the reaction products and increasing their concentration can inhibit the progress of the reaction (coordination mechanism).
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RSC Advances
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2017
·Vol. 7
·期 4
·1947-1955
·
IF 3.108
Xin Ran,Long Yang,Qing Qu,Shunling Li,Ying Chen,Limei Zuo,Lei Li
In this work, ultrasmall Pd–Pt bimetallic nanoclusters with a uniform size of 2.0 nm monodispersed on β-cyclodextrin functionalized reduced graphene oxide (β-CD-RGO) were successfully prepared in aqueous solution at room temperature within 30 min without the need for any organic solvent or high temperature. The integration of β-CD and RGO was responsible for the formation of the monodispersed 2.0 nm Pd–Pt bimetallic nanoclusters. Inspired by the monodisperse, ultrasmall, and pristine properties of the Pd–Pt clusters, the Pd–Pt@β-CD-RGO nanohybrid displayed enhanced activity for methanol and ethanol oxidation in alkaline media in comparison with the commercial Pd/C catalysts. This facile and simple method is of significance for the preparation of bimetallic nanocatalysts with high catalytic activity on suitable supporting materials.
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SOLID STATE SCIENCES
·
2017
·
IF 1.811
Chi Him A. Tsang,D.Y.C. Leung
Fabrication of electrocatalyst for direct glucose fuel cell (DGFC) operation involves destructive preparation methods with the use of stabilizer like binder, which may cause activity depreciation. Binder-free electrocatalytic electrode becomes a possible solution to the above problem. Binder-free bimetallic Pd-Pt loaded graphene aerogel on nickel foam plates with different Pd/Pt ratios (1:2.32, 1:1.62, and 1:0.98) are successfully fabricated through a green one-step mild reduction process producing a Pd-Pt/GO/nickel form plate (NFP) composite. Anode with the binder-free electrocatalysts exhibit a strong activity in a batch type DGFC unit under room temperature. The effects of glucose and KOH concentrations, and the Pd/Pt ratios of the electrocatalyst on the DGFC performance are also studied. Maximum power density output of 1.25 mW cm −2 is recorded with 0.5 M glucose/3 M KOH as the anodic fuel, and Pd 1 Pt 0.98 /GA/NFP as catalyst, which is the highest obtained so far among other types of electrocatalyst.
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ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Hui Xiong,Xinyi Hu,Xiaoying Qi,Zhao Jiang
It is essential to design and produce stable, high-activity, and low-cost anode catalysts for direct methanol fuel cells (DMFCs). To improve the efficiency of the methanol oxidation reaction (MOR) in alkaline media, a series of PdM-NbN/C (M=Co, Ni, Cu) bi-component catalysts were synthesized by introducing various oxyphilic metals. Electrochemical evaluations show that the presence of Ni and Co significantly enhances catalytic activity, charge transfer kinetics, CO tolerance, and long-term stability compared to Pd-NbN/C. Among these, PdNi-NbN/C exhibits the highest mass activity of 4806.67 A·g Pd −1 , the lowest onset potential and charge transfer resistance, as determined from electrochemical testing. The rate-determining step (RDS) is identified as the CO ads oxidation reaction. Characterization analysis confirms that the second oxyphilic metals primarily optimize the Pd electronic structure and modulate the interaction between Pd and NbN, making a favorable shift in the d-band centers. Additionally, Ni and Co elements tend to form hydroxides in higher proportions, which aids in the removal of CO ads and accelerates the RDS. The electronic interactions between Pd, Ni, and NbN species are key to the enhanced catalytic performance for MOR. Pd nanoparticles in the electron-deficient condition may aid in the activation of methanol and its intermediates, as indicated by the linear relationship between the mass activities and d-band centers. This work offers important information for the logical design of efficient anode catalysts for DMFCs.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Xuping Li,Yanwei Li,Xingtang Xu,Xiaohua Wang,Guang Sun,Bo Zhang,Yan Wang,Jianliang Cao
Metal oxide semiconductor (MOS)-based hydrogen (H 2 ) sensor that can work at room or near room temperature has attracted an increasing concern owing to its potential application in hydrogen storage and utilization. Herein, a co-sensitization strategy by La doping and Pd decoration is proposed to realize the detection of H 2 at near room temperature (50 °C) on In 2 O 3 porous nanotubes (PNTs). The In 2 O 3 PNTs were prepared via a solvothermal method and then sequentially doped with La 3+ and decorated with Pd nanoparticles via an immersion, freeze-drying and calcination route and a chemical reduction method, respectively. The results of gas-sensing measurements indicated that after a compositional evolution from In 2 O 3 to La-doped In 2 O 3 (La-In 2 O 3 ) and Pd-decorated La-In 2 O 3 (Pd/La-In 2 O 3 ), the fabricated H 2 sensor showed a higher sensitivity at lower operating temperature. At a near room temperature of 50 °C, the response of the best Pd/La-In 2 O 3 sensor to 50 ppm H 2 was as high as 8.34, increasing about 4.85, 1.20 and 1.15 folds compared to the In 2 O 3 (1.72 at 160 °C), La-In 2 O 3 (6.97 at 150 °C) and Pd/In 2 O 3 (7.24 at 80 °C) sensors, respectively. The sensitization effects and mechanism of La dopant and Pd modifier as well as their synergistic effects were discussed in detail.
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Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Jun Zhang,Tiantian Peng,Lanyu Luo,Weimin Wu,Xinlan Xu,Boyu Liu,Lingying Jiang,Shi-Yu Lu,Meng Jin
Maximizing reaction kinetics of Pd catalysts for oxygen reduction reaction (ORR) while minimizing CO poisoning during methanol oxidation reaction (MOR) remains a key challenge for advancing direct methanol fuel cells (DMFCs). Herein, we synthesize an anatase/rutile TiO2 homojunction (A/R-TiO₂) through energy band alignment and oxygen vacancies engineering, providing support for Pd nanoparticles to decipher the strong correlation between this unique structure and the electrocatalytic properties of Pd/A/R-TiO₂ catalysts. Combined experimental results and theoretical calculations demonstrate that the near perfect energy band alignment and abundant oxygen vacancies in A/R-TiO₂ not only accelerate electron transfer to Pd surface, thereby maximizing reaction kinetics and catalytic efficiency, while optimize the electronic structure of Pd active sites to reduce adsorption energy of key intermediates (*OH, *CH2OH, *CO) during ORR and MOR. Consequently, the Pd/A/R-TiO₂ catalyst delivers remarkably positive E1/2 of 0.929 V and enhanced mass activity of 4.27 A mgPd-1 at 0.85 V for ORR, respectively nearly 13 and 27 times greater than those of Pt/C and Pd/C catalysts commercially available at present. The Pd/A/R-TiO₂ catalyst displays high selectivity for an effective four-electron transfer pathway, a lower H2O2 yield (1.66%), and excellent methanol crossover tolerance. Importantly, the catalyst demonstrates exceptional stability, exhibiting minimal activity decay and negligible structural degradation after 10000 cycles. Furthermore, the as-synthesized catalyst achieves superior MOR activity (4.10 A mg-1 and 8.85 A cm-2) and enhanced CO tolerance, surpassing commercial Pt/C and Pd/C catalysts. These bifunctional catalysts thus hold strong potential for large-scale and industry-orientated use of DMFCs.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Jinxu Zhang,Fusheng Yang,Tao Fang,Bin Wang,Qingyuan Yang,Zhen Wu,Zaoxiao Zhang
The N-ethylcarbazole/dodecahydro-N-ethylcarbazole system, which offers advantages such as excellent hydrogen storage capacity, good reversibility, and reliable safety, is recognized as a potential candidate for hydrogen storage. However, the inefficient dehydrogenation by existing catalysts limits the commercial application of the system. In this work, CTAB was used as the soft template to increase the specific surface area of CeO 2 supports, and further the active metals were formed upon them through various reduction methods. A series of Pd/CeO 2 catalysts were thus prepared, among which Pd/CeO 2 –C6 adopted a composite strategy of using CTAB as the template to increase the specific surface area of CeO 2 and enhancing the dispersion of Pd through ultrasound assisted reduction, showed the best catalytic dehydrogenation performance for 12H-NEC. After 7 h of reaction at 453 K, the conversion rate of 12H-NEC reached 100 % with 97.24 % of hydrogen released. Combining BET, HRTEM, XPS, CO-pulse chemisorption and other characterization analyses, it was found that the incorporation of CTAB effectively enhanced both the specific surface area and oxygen vacancy concentration of CeO 2 , while ultrasound assisted reduction enabled a small particle size and good dispersion of metal Pd on the support. The strong synergetic effects of support and active metal in Pd/CeO 2 –C6 catalyst largely accounts for its good catalytic performance. This work offers valuable insights and guidance for the development of efficient dehydrogenation catalysts for 12H-NEC.
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