ACS Catalysis
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2015
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IF 9.312
Kui Shen,Liang Chen,Jilan Long,Wei Zhong,Yingwei Li
Although MOFs supporting noble metal nanoparticles (NPs) have been widely used in heterogeneous catalysis, they are still limited in catalytic efficiency on a per-noble-metal-atom basis. Here we developed a MOFs-templated strategy to non-noble metal @noble metal core–shell nanocatalysts, which could far surpass the traditional MOFs supporting noble NPs in catalytic properties, by using MOFs-derived metal NPs as sacrificial templates to reduce noble metal ions via galvanic replacement reaction. As a model system, Co@Pd core–shell NPs embedded in the N-doped carbon matrix (Co@Pd/NC) were synthesized with an average size of ca. 9.4 nm and a ultrathin Pd shell by using ZIF-67 and Pd(NO3)2 as the precursor and Pd source, respectively. The highly exposed Pd atom on Co nanoparticles made it an attractive catalyst with high efficiency. When being used in the hydrogenation of nitrobenzene, the Co@Pd/NC exhibited an unprecedented high activity over Pd-based catalysts, yielding 98% conversion after 45 min reaction, which was far more active than the pristine ZIF-67 and MIL-101 supporting Pd NPs (with 40% and 3% conversion after 90 min reaction, respectively) under identical conditions, suggesting its overwhelmingly better performance than MOFs supporting noble NPs. We anticipated that this strategy would form the basis for developing a new class of MOF-templated core–shell nanocatalyst with potential applications in numerous catalytic reactions.
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ACS Applied Materials & Interfaces
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2016
·
IF 7.145
Kai Cai,Yuxiang Liao,Huan Zhang,Jiawei Liu,Zhicheng Lu,Zhao Huang,Shengli Chen,Heyou Han
Here, we, for the first time, synthesized Pd nanotubes covered by high-density Au-islands, in which abundant exposed Pd–Au heterojunction interfaces are present and the content of element Au can be easily controlled. The optimized nanostructures show remarkably enhanced activity for catalyzing different alcohols in alkaline media than commercial Pd/C. The mass activity is 9.66, 1.83, and 4.60 A mgmetal–1 toward the electrooxidation of ethanol, glycerol, and ethylene glycol in alkaline media, which is about 6, 4, and 7 times that of Pd/C, respectively. Additionally, a model was proposed to explain the relationship between the structure and the catalytic activity.
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NEW JOURNAL OF CHEMISTRY
·
2017
·Vol. 41
·期 10
·4014-4021
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IF 3.269
Fuchong Li,Yansheng Liu,Tianqiong Ma,Dianhong Xu,Xu Li,Guangbi Gong
Palladium nanoparticles (NPs) were applied for the hydrodechlorination of chlorophenols in contaminated water using H2 as a clean and sustainable reductant. In this study, a high-efficiency Pd-based catalyst (Pd/Fe3O4@C) was facilely synthesized and applied for the reduction of 4-nitrophenol and hydrodechlorination of 4-chlorophenol in an aqueous solution. Compared with most Pd-based catalysts, the Pd/Fe3O4@C nanocatalyst exhibits a higher catalytic performance. The well-dispersed Pd NPs were modified on the spherical carbon surface through coordination chemical bond. The superparamagnetic character of the Fe3O4 core enabled the Pd/Fe3O4@C nanocatalyst to be very easily separated and recovered from the reaction mixture. Thus, the nanocatalyst can be repeatedly used without significant weight loss. The high catalytic activity of the Pd/Fe3O4@C nanocatalyst indicates that noble metal nanoparticles supported on magnetic carbon sphere materials could act as promising catalysts and have potential applications in numerous Pd-based catalytic reactions.
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JOURNAL OF THE ENERGY INSTITUTE
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2016
·
IF 1
Nan Li,Wei-Yan Xia,Chang-Wei Xu,Shuang Chen
This study investigated Pt/C and Pd/C catalysts promoted by Au for glycerol electrooxidation in alkaline medium . The results show that addition of Au can significantly promote the catalytic activity and stability of Pt/C and Pd/C for glycerol electrooxidation. The catalysts with a weight ratio of 4:1 for Pt to Au and Pd to Au show the best performance for glycerol electrooxidation and the PtAu(wt 4:1)/C shows a better performance than the PdAu(wt 4:1)/C. Glycerol electrooxidation on the PdAu(wt 4:1)/C has a better stability than that on the Pt/C. The results show that the PdAu(wt 4:1)/C can give a better discharge performance than the Pt/C in a direct glycerol fuel cell. Electrooxidation of pre-adsorbed CO has been used to explain the results.
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Catalysts
·
2016
·Vol. 6
·期 7
·100
·
IF 2.964
Chi Zhang,Wenrong Cao,Hongye Cheng,Lifang Chen,Zhiwen Qi
The size of metal particles is an important factor to determine the performance of the supported metal catalysts. In this work, we report subnanometer Pd clusters supported on zirconia by the microwave-assisted hydrothermal method. The presence of subnanometer Pd clusters on the zirconia surface was confirmed by two-dimensional Gaussian-function fits of the aberration-corrected high-angle annual dark-field images. These subnanometer Pd catalysts exhibit high catalytic performance for the hydrogenation of biomass-derived succinic acid to γ-butyrolactone in water and avoid the formation of overhydrogenated products, such as 1,4-butanediol and tetrahydrofuran. The catalyst with an ultra-low Pd loading of 0.2 wt. % demonstrated high selectivity (95%) for γ-butyrolactone using water as a solvent at 473 K and 10 MPa. Moreover, it can be reused at least six times without the loss of catalytic activity, illustrating high performance of the small Pd clusters.Keywords:succinic acid hydrogenation;aqueous phase;subnanometer;Pd catalyst
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ULTRASONICS SONOCHEMISTRY
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2016
·
IF 4.556
Ling-Xia Zuo,Li-Ping Jiang,Jun-Jie Zhu
For the alkaline fuel cell cathode reaction, it is very essential to develop novel catalysts with superior catalytic properties. Here, we report the synthesis of highly active and stable MoS 2 /Pd composites for the oxygen reduction reaction (ORR), via a simple, eco-friendly sonochemical method. The bulk MoS 2 was first transformed into single and few layers MoS 2 nanosheets through ultrasonic exfoliation. Then the exfoliated MoS 2 nanosheets served as supporting materials for the nucleation and further in-situ growth of Pd nanoparticles to form MoS 2 /Pd composites via ultrasonic irradiation. Cyclic voltammetry and rotating disk voltammetry measurements demonstrate that as-prepared MoS 2 /Pd composites which provides a direct four-electron pathway for the ORR, have better electrocatalytic activity , long-term operation stability than commercial Pt/C catalyst. We expect that the present work would provide a promising strategy for the development of efficient oxygen reduction electrocatalyst . In addition, this study can also be extended to the preparation of other hybrid with desirable morphologies and functions.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2016
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IF 2.822
Fen-Ying Kong,Yu Luo,Jin-Wei Zhang,Jing-Yi Wang,Wei-Wei Li,Wei Wang
In this work, we successfully prepared well-defined bimetallic alloyed Pt-Pd nanocubes (NCs) supported on reduced graphene oxide nanosheets (rGO-Pt-Pd NCs). Pt-Pd NCs were uniformly dispersed on rGO by hydrothermal treatment of preformed Pt-Pd NCs and GO in alkaline media. The detailed morphology, crystal structure and composition were well characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). Furthermore, with the special structure of Pt-Pd NCs and the synergetic effects of Pt, Pd and rGO, the rGO-Pt-Pd NCs modified electrode exhibited excellent electrocatalytic performance in the sensing of chloramphenicol (CAP). The linear covered the range of 0.2–30 μM and the detection limit reached 0.1 μM (S/N = 3). The modified electrode also displayed good stability, high reproducibility and satisfactory selectivity.
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BIOSENSORS & BIOELECTRONICS
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2015
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IF 6.409
Xiang Zhu,Tingting Liu,Hongli Zhao,Libo Shi,Xiaoqing Li,Minbo Lan
Considering the critical roles of superoxide anion (O 2 ∙− ) in pathological conditions, it is of great urgency to establish a reliable and durable approach for real-time determination of O 2 ∙− . In this study, we propose a porous Pt–Pd decorated superoxide dismutase (SOD) sensor for qualitative and quantitative detection O 2 ∙− . The developed biosensor exhibits a fast, selective and linear amperometric response upon O 2 ∙− in the concentration scope of 16 to 1536 μM ( R 2 =0.9941), with a detection limit of 0.13 μM (S/N=3) and a low Michaelis–Menten constant of 1.37 μM which indicating a high enzymatic activity and affinity to O 2 ∙− . Inspiringly, the proposed sensor possesses an ultrahigh sensitivity of 1270 μA mM −1 cm −2 . In addition, SOD/porous Pt–Pd sensor exhibits excellent anti-interference property, reproducibility and long-term storage stability. Beyond our expectation, the trace level of O 2 ∙− released from living cells has also been successfully captured. These satisfactory results are mainly ascribed to (1) the porous interface with larger surface area and more active sites to provide a biocompatible environment for SOD (2) the specific biocatalysis of SOD towards O 2 ∙− and (3) porous Pt–Pd nanomaterials fastening the electron transfer . The superior electrochemical performance makes SOD/porous Pt–Pd sensor a promising candidate for monitoring the dynamic changes of O 2 ∙− in vivo .
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RSC Advances
·
2017
·Vol. 7
·期 59
·36923-36928
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IF 3.108
Yueyue Yin,Yong Yang,Liangzhu Zhang,Yongsheng Li,Zhiyuan Li,Weiwei Lei,Yunfeng Ma,Zhengren Huang
Here, we report a facile synthesis of Pd/Au nano-dogbones (NDBs) by loading massive Pd nanoparticles on the two ends of Au nanorods (NRs) via a seed-mediated method. The as-prepared samples were investigated by using TEM, elemental analysis, UV-vis and FDTD simulation. The photocatalytic activity of Pd/Au NDBs was assessed by dehydrogenation of formic acid under visible-to-NIR light irradiation. The Pd/Au NDBs shows much higher enhanced reaction activity compared with samples with core–shell structure due to the increased electron and hole pair separation and total catalytic sites. More importantly, the introduction of Au NRs broadens the photoresponse range and improves the utilization of sunlight efficiently. This finding provides a rational approach to improve photocatalytic performance by forming dogbone structures via integrating plasmonic metals and conventional catalysts.
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2016
·Vol. 21
·期 2
·391-401
·
IF 2.327
Peng Meiling,Xu Wei,Cui Weihao,Wang Tao,Wang Sheng
This study reports the synthesis of octahedral Pd-Pt bimetallic alloy nanocrystals through a facile, one-pot, templateless, and seedless hydrothermal method in the presence of glucose and hexadecyl trimethyl ammonium bromide. The morphologies, compositions, and structures of the Pd-Pt nanocrystals were fully characterized by various physical techniques, thereby demonstrating their highly alloying octahedral nanostructures. The formation or growth mechanism of the Pd-Pt bimetallic alloy nanocrystals was explored and is discussed here based on the experimental observations. In addition, the synthesized Pd-Pt nanocrystals were applied to the methanol oxidation reaction (MOR) in alkaline media, which proved that the as-prepared catalysts exhibit enhanced electrocatalytic activity for MOR. Pd 1 Pt 3 exhibited the best stability and durability, and its mass activity was 3.4 and 5.2 times greater than those of Pt black and Pd black catalysts, respectively. The facile synthetic process and excellent catalytic performance of the as-prepared catalysts demonstrate that they have the potential to be used in direct methanol fuel cell techniques.
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ACS Sustainable Chemistry & Engineering
·
2016
·
IF 5.267
Yanbing Wang,Kai Yu,Da Lei,Wei Si,Yajun Feng,Lan-Lan Lou,Shuangxi Liu
An environmentally benign and homogeneous base-free route for 5-hydroxymethyl-2-furfural (HMF) aerobic oxidation to 2,5-furandicarboxylic acid (FDCA) in water was reported using Mg–Al–CO3 hydrotalcite-supported Pd nanoparticles (xPd/HT-n) as catalyst. The influences of the Mg/Al molar ratio of hydrotalcite and Pd loading amount on the catalytic performance of these catalysts were originally systematically investigated. These catalysts exhibited excellent catalytic activity and FDCA selectivity in the HMF oxidation, especially for 2%Pd/HT-5 and 2%Pd/HT-6; >99.9% FDCA yields were achieved for 8 h under ambient pressure and homogeneous base-free conditions. The remarkably improved catalytic performance could be attributed to the suitable basicity of the Mg–Al–CO3 hydrotalcite and the abundant OH– groups on the surface of hydrotalcite. The plausible reaction mechanism was proposed based on the results of a series of controlled experiments. Furthermore, these catalysts were quite stable and could be reused at least five times without obvious loss in reaction activity.
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CHEMICAL ENGINEERING JOURNAL
·
2016
·
IF 5.31
Hao Feng,Xun Zhu,Rong Chen,Qiang Liao,Jian Liu,Lin Li
In this study, a gas-liquid-solid microreactor with the polydopamine functionalized surface coated by highly-active palladium nanocatalysts using the electroless deposition was successfully developed for hydrogenation of nitrobenzene. Experimental results showed that in the 40-h continuous operation, the developed microreactor exhibited rather high average nitrobenzene conversion more than 97% under various inlet nitrobenzene concentrations from 30 to 90 mM. Besides, the effect of the gas and liquid flow rates on the aniline concentration and nitrobenzene conversion was also studied. It was found that for a given liquid flow rate, the increase of the gas flow rate led to an increase in both the aniline concentration and nitrobenzene conversion as a result of more hydrogen supplied. Further increasing the gas flow rate caused no change of them due to excess supplied hydrogen. There existed a minimum gas flow rate to acquire the complete conversion of nitrobenzene. Similarly, for a given gas flow rate, increasing the liquid flow rate did not change the aniline concentration and nitrobenzene conversion due to sufficient supply of hydrogen. Once the supplied hydrogen became insufficient at high liquid flow rate, both the aniline concentration and nitrobenzene conversion were decreased. Based on these results, the excess ratios were achieved under different conditions. It was found that the excess ratio decreased with the increase of the liquid flow rate and inlet nitrobenzene concentration as a result of the enhanced mass transport. The obtained results in this work are beneficial for optimizing the gas-liquid-solid microreactor operation.
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