Nanoscale
·
2020
·Vol. 13
·期 6
·3528-3542
·
IF 6.895
Yaxing Liu,Weiyin Li,Guizhe Zhao,Gang Qin,Yuexia Li,Yaqing Liu
The lack of direct insight into the microstructural evolution of catalytic materials under electrochemical polarization has inhibited the development of heterogeneous catalysts. By investigating a typical Au@Pd core–shell nanostructure, the present study discloses the microstructural evolution of heterogeneous catalytic materials during the methanol electrooxidation reaction (MOR). The electrocatalytic activity of the as-prepared Au@Pd_core–shell nanoparticles continuously increased during the first 100 successive voltammetry cycles of the MOR. Microstructural characterization studies revealed that during the MOR, an Au/Pd mixed bimetallic shell was formed by the self-driven microstructural evolution of the Au@Pd_core–shell nanoparticles. Both the experimental and calculation results indicated that the Au/Pd mixed bimetallic shell reduced the binding strength of OH− and CO on the catalyst surface. The exposed Au atoms in the shell region also produced large-scale reactive ˙OH radicals that facilitated the oxidative removal of the adsorbed carbonaceous species from the adjacent Pd active sites.
研究领域:
催化
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电化学
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纳米材料
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Zhuo Zong,Kebin Xu,Dongliang Li,Zhenghua Tang,Wei He,Zhen Liu,Xiufang Wang,Yong Tian
Bimetallic core-shell nanostructures have been gaining considerable research attentions recently, mainly thanks to their versatile applications in many fields, including catalysis, electrocatalysis, electronic, sensing and so on. Herein, we demonstrate a peptide templated Au@Pd core-shell structure for both oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER). By employing peptide sequence FlgA3 as surface capping agent, core-shell structure with Pd nanoparticles coated on the surface of Au nanoparticles were prepared. The Au@Pd core-shell structures demonstrated effective electrocatalytic activities toward both ORR and HER, whereas the catalytic activity was optimized by tuning the Pd-to-Au ratio. Among a series of samples tested, we discovered that the Au@Pd 1.0 sample exhibited the best ORR activity, superior to that of Pt/C and Pd/C, while its HER activity was also among the finest, close to that of Pt/C and Pd/C. The Au@Pd 1.0 sample also exhibited remarkable stability beyond Pt/C and Pd/C in both ORR and HER. Such intriguing electrocatalytic performances are attributed to the core-shell structure induced lattice strain. The results offer reliable pathway for designing peptide templated core-shell bimetallic nanostructures as dual or multiple functional electrocatalysts with excellent electrocatalytic activities and longevity.
研究领域:
材料科学
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电化学
·
生物材料
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 14
·10352-10357
·
IF 3.84
Zhen Sun,Qingshan Zhao,Guanghui Zhang,Yang Li,Guoliang Zhang,Fengbao Zhang,Xiaobin Fan
Au–Pd bimetallic nanoparticles (NPs) with core–shell structures have been successfully anchored on chemical exfoliated MoS2 (Au–Pd/MoS2) through a facile co-reduction method at room temperature. The Au–Pd/MoS2 hybrids were characterized by X-ray diffraction (XRD), scanning electronic microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), energy dispersive X-ray spectroscopy (EDX) and X-ray photoelectron spectroscopy (XPS). The pristine MoS2 nanosheets exhibit some peroxidase-like activity for the oxidation of 3,3,5,5-tetramethylbenzidine (TMB), and their catalytic activity is significantly enhanced by the deposition of Au–Pd NPs. A systematic study revealed that Au–Pd NPs with a mass ratio of 1 : 2 on MoS2 (Au1.0Pd2.0/MoS2) showed the highest catalytic activity compared with other counterparts. This excellent performance of the Au1.0Pd2.0/MoS2 hybrids should be ascribed to not only the intrinsic catalytic activity of MoS2, but also the complicated metal–metal and metal–support interactions.
研究领域:
材料科学
·
生物化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2023
·Vol. 13
·期 4
·643
·
IF 3.9
Minming Bao,Yuxi Liu,Jiguang Deng,Lin Jing,Zhiquan Hou,Zhiwei Wang,Lu Wei,Xiaohui Yu,Hongxing Dai
The development of efficient and stable catalysts is of great importance for the elimination of volatile organic pollutants (VOCs). In this work, AuPdxnanoparticles (NPs) were loaded on TiO2through the electrostatic adsorption approach to generate theyAuPdx/TiO2(i.e., 0.35AuPd0.46/TiO2, 0.34AuPd2.09/TiO2, and 0.37AuPd2.72/TiO2;xandyare Pd/Au molar ratio and AuPdxloading, respectively;x= 0.46–2.72; andy= 0.34–0.37 wt%) catalysts, and their catalytic activities for the oxidation of ethyl acetate were determined. The results showed that the 0.37AuPd2.72/TiO2sample exhibited the best activity (T50%= 217 °C andT90%= 239 °C at SV = 40,000 mL/(g h),Ea= 37 kJ/mol, specific reaction rate at 220 °C = 113.8 µmol/(gPds), and turnover frequency (TOFNoble metal) at 220 °C = 109.7 × 10−3s−1). The high catalytic performance of the 0.37AuPd2.72/TiO2sample was attributed to the good dispersion of AuPd2.72NPs, the strong redox ability, the large ethyl acetate adsorption capacity, and the strong interaction between AuPdxand TiO2. Acetaldehyde, ethanol, and acetic acid are the main intermediates in the oxidation of ethyl acetate, and the loading of AuPdxNPs effectively reduces the formation of the toxic by-product acetaldehyde. The oxidation of ethyl acetate over the 0.34AuPd2.09/TiO2sample might occur via the pathway of ethyl acetate → ethanol → acetic acid → acetate → CO2and H2O. We believe that the obtained results may provide a useful idea for the design of bimetallic catalysts under industrial conditions and for understanding the VOCs oxidation mechanisms.Keywords:supported Au–Pd nanocatalyst;ethyl acetate oxidation;strong electrostatic adsorption;sulfur dioxide resistance;reaction mechanism
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Qiang Zhou,Xinyu Wang,Tao Xing,Mingqing Wang,Mingbo Wu,Wenting Wu
Hydrogen peroxide (H 2 O 2 ) is widely used as an oxidant for photocatalytic oxidation of methane to value-added chemicals under mild conditions, but suffers from low utilization efficiency. Herein, we propose a comprehensive strategy for the proper amount of hydroxyl radicals (•OH) generation from H 2 O 2 by regulating the Pd/Au molar ratios and the total Au-Pd contents loaded on In 2 O 3 . For the photocatalytic oxidation of methane at ambient temperature, the yield and selectivity of CH 3 OH over the optimized 1.0% AuPd 0.5 /In 2 O 3 catalyst were as high as 2187.0 μmol g −1 h −1 and 94.0% respectively, exceeding most reported literatures. Mechanism investigations revealed that the formation of Au-Pd alloys may contribute to the homolytic cleavage of H 2 O 2 into •OH radicals and improve the selectivity of •OH generation. This work provides some guidance for the delicate design of photocatalysts to manipulate selective H 2 O 2 activation and efficient photocatalytic methane oxidation.
研究领域:
化学
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催化
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Xiaoliang Li,Jiangjiang Feng,Michal Perdjon,Rena Oh,Wei Zhao,Xiaoyang Huang,Shusen Liu
Au-Pd bimetallic nanoparticles immobilized on series of CeO 2 supports with different morphologies, e.g. , rod, cube, and polyhedrons were prepared through the deposition-precipitation method with a consequent investigation on their catalytic performances for benzyl alcohol oxidation in the absence of solvent. The experimental results exhibited that the morphology of CeO 2 has a markedly impact on the catalytic performance of Au-Pd/CeO 2 . In which Au-Pd supported on CeO 2 rod could achieve higher benzyl alcohol conversion than that supported on CeO 2 polyhedrons and CeO 2 cube, however, CeO 2 cube supported Au-Pd showed the highest selectivity towards the production of benzaldehyde. ICP-AES, XRD, Raman, N 2 -BET, TEM, HAADF-STEM, and XPS were conducted to characterize the catalysts. The results revealed that the excellent behavior of Au-Pd/CeO 2 -rod in benzyl alcohol oxidation was closely related with the smaller size of CeO 2 particle, the higher concentration of oxygen defects in support and the higher number of Ce 3+ and Pd 2+ species on the catalyst surface. The present study on the morphologies of CeO 2 support in solvent-free benzyl alcohol oxidation would offer a notable approach for the future catalyst design.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 10
·1-13
·
IF 5.3
Guo Liang,Zhou Shijin,Xue Jinyan,Liu Zenghui,Xu Shuqing,He Zhangxu,Yang Huaixia
A sandwich electrochemical sensor was fabricated based on multi-walled carbon nanotubes/ordered mesoporous carbon/AuNP (MWCNTs/CMK-3/AuNP) nanocomposites and porous core–shell nanoparticles Au@PdNPs to achieve rapid and sensitive detection of AFB 1 in complex matrices. MWCNTs/CMK-3/AuNP nanocomposite, which was prepared by self-assembly method, served as a substrate material to increase the aptamer loading and improve the conductivity and electrocatalytic activity of the electrode for the first signal amplification. Then, Au@PdNPs, which were synthesized by one-pot aqueous phase method, were applied as nanocarriers loaded with plenty of capture probe antibody (Ab) and signal molecule toluidine blue (Tb) to form the Au@PdNPs-Ab-Tb bioconjugates for secondary signal amplification. The sensing system could still significantly improve the signal output intensity even in the presence of ultra-low concentration target compound due to the dual signal amplification of MWCNTs/CMK-3/AuNP nanocomposites and Au@PdNPs-Ab-Tb. The method exhibited high selectivity, low detection limit (9.13 fg/mL), and strong stability to differentiate AFB 1 from other mycotoxins. Furthermore, the sensor has been successfully applied to the quantitative determination of AFB 1 in corn, malt, and six herbs, which has potential applications in food safety, quality control, and environmental monitoring. Graphical Abstract
研究领域:
分析化学
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食品安全
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环境监测
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
BIOELECTROCHEMISTRY
·
2020
·
IF 4.722
Qingshan Yang,Ping Wang,Enhui Ma,Haoxuan Yu,Kaiwei Zhou,Chunyuan Tang,Jie Ren,Yueyun Li,Qing Liu,Yunhui Dong
In this work, a sandwich-type electrochemical immunosensor was fabricated to the effective detection of hepatitis B surface antigen (HBsAg). The designed electrochemical immunosensor was based on Au core and Pd shell nanodendrites loaded on amino functionalized molybdenum dioxide nanosheets (Au@Pd NDS/NH 2 –MoO 2 NSs) as the secondary antibody (Ab 2 ) label and silver nanoparticles were loaded by electrodeposited (D-Ag NPs) on the surface of electrode as the platform. Because of the synergistic effect and abundant catalytic activity sites provided by surface dendrite structure, Au@Pd NDs were more effective than single gold and palladium nanoparticles in catalytic reduction of hydrogen peroxide (H 2 O 2 ). MoO 2 had the good catalytic capacity for reduction of H 2 O 2 and favourable electrical conductivity . Hence, the obtained Au@Pd NDS/NH 2 –MoO 2 NSs were more effective than Au@Pd NDs and NH 2 –MoO 2 NSs in catalytic reduction of hydrogen peroxide attribute to a synergistic effect. Also, Ag NPs with admirable electrical conductivity and biocompatibility were used as sensing platforms and primary antibodies (Ab 1 ) carriers, which can accelerate the electron transfer and improve the sensitivity of the immunosensor. Here, the proposed electrochemical immunosensor offered a wide linear interval from 10 fg mL −1 to 100 ng mL −1 and the lower limit of detection of 3.3 fg mL −1 (S/N = 3) for detection of HBsAg under optimal experimental conditions. Furthermore, the accuracy of the actual serum sample analysis was satisfactory, which showed that the electrochemical immunosensor possessed a good application prospect in clinical detection.
研究领域:
生物医学工程
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Zhe Wang,Jiangjiang Feng,Xiaoliang Li,Rena Oh,Dongdong Shi,Ouardia Akdim,Ming Xia,Liang Zhao,Xiaoyang Huang,Guojie Zhang
TiO 2 nanocrystals with controlled facets have been extensively investigated due to their excellent photocatalytic performance in sustainable and green energy field. However, the applications in thermal catalysis without applying UV irradiation are comparably less and the identification of their intrinsic roles, especially the different catalytic behaviors of each crystal facet, remains not fully recognized. In this study, bimetallic AuPd nanoparticles supported on anatase TiO 2 nanosheets exposing {0 0 1} facets or TiO 2 nanospindles exposing {1 0 1} as a catalyst were prepared by sol-immobilization method and used for solvent-free benzyl alcohol oxidation . The experimental results indicated that the exposed facet of the support has a significant effect on the catalytic performance. AuPd/TiO 2 -001 catalyst exhibited a higher benzyl alcohol conversion than that of the AuPd/TiO 2 -101. Meanwhile, all the prepared AuPd/TiO 2 catalysts were characterized by XRD , ICP-AES, XPS, BET, TEM, and HRTEM . The results revealed that the higher number of oxygen vacancies in TiO 2 -sheets with the exposed {0 0 1} facets of higher surface energy could be responsible for the observed enhancement in the catalytic performance of benzyl alcohol oxidation. The present study displays that it is plausible to enhance the catalytic performance for the benzyl alcohol oxidation by tailoring the exposed facet of the TiO 2 as a catalyst support.
研究领域:
催化
·
材料科学
·
化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROCHIMICA ACTA
·
2010
·Vol. 168
·期 3
·347-354
·
IF 2.648
Qian Ping,Ai Shiyun,Yin Huanshun,Li Jinhuan
Au-Pd bimetallic nanoparticles were prepared in the presence of an amine-terminated dendrimer of a fourth generation poly(amidoamine) type. A biosensor was fabricated by immobilizing dsDNA on a thin layer of a dendrimer-encapsulated bimetallic nanoparticles (Au-Pd) in a chitosan composite on a glassy carbon electrode. The biosensor was evaluated by square wave voltammetry for the determination of the oxidative damage of immobilized DNA and the antioxidant capacity of sericin. The biosensor is shown to be suitable for the rapid detection of DNA damage and the assessment of the antioxidant capacity of sericin.
研究领域:
生物分析化学
·
纳米生物技术
·
分子毒理学
·
食品与药物分析
·
生物传感技术
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2017
·
IF 4.233
Wenhao Dong,Yipeng Ren,Zhixue Bai,Jun Jiao,Yuan Chen,Bingkai Han,Qiang Chen
An innovative epinephrine sensor was fabricated by integrating tetrahexahedral (THH) Au-Pd core–shell nanocrystals on reduced graphene oxide (rGO) nanosheets . Furthermore, the nanocomposites combined the large specific areas of rGO with the high-index facets and excellent electrocatalytic activity of the THH Au-Pd nanocrystals, and the nanocomposites were an essential adapter for detecting epinephrine. In the present work, transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR) and X-ray diffraction (XRD) were used to identify and characterize these unique nanocomposites, and the results revealed that a unique THH Au-Pd/rGO core–shell nanostructure was synthesized successfully. To further explore the electrochemical behaviors of these nanomaterials at a GC electrode, we applied cyclic voltammetry (CV), differential pulse voltammetry (DPV) and amperometry to study the conductivity and electrocatalytic activity of the proposed sensor, and the results suggested that the sensor based on Au-Pd/rGO presented a lower limit of detection (0.0012 μM at a signal to noise ratio of 3), wide linear detection range (0.001 µM to 1000 µM), and extraordinary selectivity and reproducibility. Moreover, the data showed that the sensor possessed good stability and acceptable accuracy to detect epinephrine in human serum samples. In summary, this work is not only a potential way to manufacture various nonenzymatic sensors but also a significant contribution to further studies in catalysis, cell fuel cells and other relevant applications.
研究领域:
材料科学
·
分析化学
·
生物医学工程
✓ 已验证
DOI
高影响因子
Catalysts
·
2023
·Vol. 13
·期 2
·435
·
IF 3.9
Yiran Liu,Yao Chen,Wen Guan,Yu Cao,Fang Wang,Yunlei Zhang
Aerobic oxidation of bio-sourced 2,5-bis(hydroxymethyl)furan (BHMF) to 2, 5-furandicarboxylic acid (FDCA), a renewable and green alternative to petroleum-derived terephthalic acid (TPA), is of great significance in green chemicals production. Herein, hierarchical porous bowl-like nitrogen-rich (nitrated) carbon-supported bimetallic Au-Pd nanocatalysts (AumPdn/ N-BNxC) with different nitrogen content and bimetal nanoparticle sizes were developed and employed for the highly efficient aerobic oxidation of BHMF to FDCA in sodium carbonate aqueous solution. The reaction pathway for catalytic oxidation of BHMF went through the steps of BHMF→HMF→HMFCA→FFCA→FDCA. Kinetics studies showed that the activation energies of BHMF, HMF, HMFCA, and FFCA were 58.1 kJ·moL−1, 39.1 kJ·moL−1, 129.2 kJ·moL−1, and 56.3 kJ·moL−1, respectively, indicating that the oxidation of intermediate HMFCA to FFCA was the rate-determining step. ESR tests proved that the active species was a superoxide radical. Owing to the synergy between the nitrogen-rich carbon support and bimetallic Au-Pd nanoparticles, the Au1Pd1/N-BN2C nanocatalysts exhibited BHMF conversion of 100% and FDCA yield of 95.8% under optimal reaction conditions. Furthermore, the nanocatalysts showed good stability and reusability. This work provides a versatile strategy for the design of heterogeneous catalysts for the highly efficient production of FDCA from BHMF.Keywords:2,5-bis(hydroxymethyl)furan;2,5-furandicarboxylic acid;aerobic oxidation;nitrogen-doped carbon;bimetallic Au-Pd nanoparticles
研究领域:
绿色化学
·
催化化学
·
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）