ChemCatChem
·
2019
·Vol. 11
·期 6
·1779-1788
·
IF 4.495
Wei Zhang,Ziqiang Xiao,Jiajun Wang,Wenqin Fu,Rong Tan,Donghong Yin
Graphical Alloys of Catalysis ! Synergistic effect in Au−Pd alloy catalysts enhanced selective aerobic oxidation of alcohols using air at atmospheric pressure in water. A series of bimetallic Au−Pd alloy nanoparticles (NPs) with varied Au/Pd molar ratios was supported on Gamma-alumina (γ-Al 2 O 3 ) surface through the co-impregnation-reduction method using HAuCl 4 and PdCl 2 as metal precursors. Characterization results suggested the high dispersion of Au−Pd alloy NPs, as well as the interplay between the two compositions. Benefitting from the synergistic effects of Au−Pd alloying, the bimetallic Au-Pd x @γ-Al 2 O 3 catalysts were highly efficient for selective aerobic oxidation of various alcohols either aromatic or aliphatic in water using air at atmospheric pressure as a sole oxidant without the need for any cocatalyst. Quantitative yields of corresponding aldehydes or ketones were achieved over Au-Pd 1.2 @γ-Al 2 O 3 within 2 h, whereas pure Au@γ-Al 2 O 3 or Pd@γ-Al 2 O 3 was far less efficient. More importantly, the “alloying effect” appeared to stabilize the bimetallic NPs against aggregation and poisoning, which made the Au-Pd x @γ-Al 2 O 3 more stable and reusable in the aerobic oxidation of alcohols.
研究领域:
化学
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催化材料科学
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产品关联
DOI
高影响因子
ANALYST
·
2022
·Vol. 147
·期 24
·5655-5662
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IF 5.227
Ying Zhou,Ruichun Li,Guomei Zhang,Yan Zhang,Caihong Zhang,Shaomin Shuang
Metal–organic frameworks (MOFs) have emerged as interesting nanomaterials owing to their large surface area, high porosity, tunable pore architecture and easy functionalization. However, an inferior electrical conductivity hinders their application in electrochemical sensing. In this paper, gold–palladium alloy/UiO-66-NH2/graphene (AuPd/UiO-66-NH2/GN) composites were synthesized by loading alloys on the surfaces of MOFs and then attaching them to the graphene surface. The addition of metal nanoparticles and graphene enhanced the electron transfer ability of MOFs. Then, composites were used to modify a glassy carbon electrode (GCE) to construct a sensitive dopamine (DA) electrochemical sensor. The developed sensor manifested two linear relationships in lower concentration ranges and in higher concentration ranges with a 0.21 × 10−6 mol L−1 low detection limit (3σ/k) under optimal conditions. The results certified that the constructed sensor had high selectivity, excellent reproducibility and good stability, and had been used successfully for DA detection in actual human serum samples.
研究领域:
材料科学
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分析化学
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生物医学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Inorganic Chemistry Frontiers
·
2018
·Vol. 5
·期 11
·2948-2954
·
IF 5.106
Yuanxin Du,Ji Xiang,Kun Ni,Yapei Yun,Guodong Sun,Xiaoyou Yuan,Hongting Sheng,Yanwu Zhu,Manzhou Zhu
Atomically precise nanoclusters (NCs) have been widely used as catalysts in many reactions to investigate the structure–activity relationship due to their ultrasmall sizes, well-defined structures and precise compositions, especially bimetallic NCs can further promote the catalytic activity by the synergistic effects of heteroatoms. For electrocatalytic hydrogen evolution reaction (HER) catalysts, a common method to improve the performance is coupling with a nano-metal, but the origin of the enhancement is still unclear due to the diversity and complexity of the nanometal supported composites. Here, we take MoS2 (a star HER electrocatalyst) as an example, to report a strategy to boost the activity and give insight into the activity enhancement of it by combining with bimetallic atomically precise NCs. The crystal structure of this new NC is determined by X-ray crystallography, and its precise composition is identified as Au2Pd6S4(PPh3)4(C6H4F2S)6 (Au2Pd6 for short). The Au2Pd6/MoS2 show significantly improved HER activity and robust durability compared to the single component Pd3 or Au2/MoS2 and bare MoS2. This is attributed to the appropriate adsorption behavior of H atoms on Au2Pd6/MoS2 and the electronic interactions between NCs and MoS2, according to the combination of experiment and theory. This study presents a new strategy to improve the electrocatalytic activity of 2D materials such as MoS2 and sheds light on the origin of the promotion effects at the atomic level.
研究领域:
材料科学
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催化化学
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能源化学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Jin Wang,Peina Zhang,Yujiao Xiahou,Dayang Wang,Haibing Xia,Helmuth Möhwald
The present work introduces a new way to prepare Au–Pd alloy nanowire networks (NWNs) via deposition of Pd atoms onto Au nanowires in reaction media at room temperature without the aid of additional reducing agents. Thanks to their excellent colloidal stability in water as well as in ethanol, the resulting NWNs can be utilized to produce composite thin films with Nafion (perfluorinated sulfonic acid) with dimensions above dozens of square centimeters by means of solution casting on the glass substrate. Most importantly, these films can be easily transferred onto different solid substrates by lift-off technology. Moreover, the resulting Au–Pd alloy NWNs can also be easily and thoroughly loaded into macroscopic carbon fiber cloth (CFC). Both the Au–Pd alloy NWN/Nafion composite film and the Au–Pd alloy NWN-loaded CFC can be used as flexible electrodes for electrocatalysis of ethanol oxidation, with electrocatalytic performance at different distorted states superior by 2 orders of magnitude to those reported in the literature (e.g., commercial Pd/C catalysts and Pd-based nanostructured catalysts). This work opens new possibilities for the large-scale manufacturing of electrodes for fuel cells.
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
Nature Communications
·
2024
·Vol. 15
·期 1
·1-18
·
IF 14.7
Meng Xiangqin,Fan Huizhen,Chen Lei,He Jiuyang,Hong Chaoyi,Xie Jiaying,Hou Yinyin,Wang Kaidi,Gao Xingfa,Gao Lizeng,Yan Xiyun,Fan Kelong
Developing strategies that emulate the killing mechanism of neutrophils, which involves the enzymatic cascade of superoxide dismutase (SOD) and myeloperoxidase (MPO), shows potential as a viable approach for cancer therapy. Nonetheless, utilizing natural enzymes as therapeutics is hindered by various challenges. While nanozymes have emerged for cancer treatment, developing SOD-MPO cascade in one nanozyme remains a challenge. Here, we develop nanozymes possessing both SOD- and MPO-like activities through alloying Au and Pd, which exhibits the highest cascade activity when the ratio of Au and Pd is 1:3, attributing to the high d-band center and adsorption energy for superoxide anions, as determined through theoretical calculations. The Au 1 Pd 3 alloy nanozymes exhibit excellent tumor therapeutic performance and safety in female tumor-bearing mice, with safety attributed to their tumor-specific killing ability and renal clearance ability caused by ultrasmall size. Together, this work develops ultrasmall AuPd alloy nanozymes that mimic neutrophil enzymatic cascades for catalytic treatment of tumors.
研究领域:
生物医学工程
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肿瘤学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2019
·
IF 6.361
Yanan Liu,Hui Zhou,Tiantian Yin,Youcong Gong,Guanglong Yuan,Lanmei Chen,Jie Liu
At present, autophagic dysfunction has been considered to be involved in the pathogenesis of Alzheimer’s disease (AD). Thus, the activation of autophagy provides a potential means of eliminating the intracellular amyloid-β (Aβ) and slows down the neurotoxicity induced by Aβ. Here, we synthesize a Quercetin (Qu) modified polysorbate 80 (P-80)-coated AuPd core-shell structure. Our results indicate that Concave cubic Qu@P-80@AuPd can activate autophagy of SH-SY5Y cells, promote the fusion of autophagosomes and lysosomes, accelerate the clearance of Aβ, and protect SH-SY5Y cells from Aβ-induced cytotoxicity damage. Furthermore, Concave cubic Qu@P-80@AuPd also has good biocompatibility and high blood-brain barrier (BBB) permeability. Therefore, we anticipate that Concave cubic Qu@P-80@AuPd will be used as a potential autophagy inducer to treat AD.
研究领域:
神经生物学
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纳米医学
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药理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CRYSTENGCOMM
·
2023
·Vol. 25
·期 25
·3655-3661
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IF 3.1
Ningkang Qian,Degong Ding,Liang Ji,Junjie Li,Hui Zhang,Deren Yang
Lattice engineering is a powerful strategy not only to optimize electrocatalytic performances, but also to deepen the understanding of electrocatalytic mechanisms. Lattice engineering can be effectively achieved in core–shell nanocrystals owing to the lattice mismatch of heterostructures. Herein, we constructed three kinds of icosahedra consisting of Au73Pd27@Pt, Au66Pd34@Pt and Pd@Pt core–(interlayer)–shell by a seed-mediated method. The introduction of an ultrathin Pd interlayer in the Au66Pd34@Pt icosahedra enables us to separately identify the strain effect and ligand effect. The specific activities towards the EOR of these icosahedra are in the sequence Au73Pd27@Pt > Au66Pd34@Pt > Pd@Pt, indicating that both the ligand effect and strain effect caused by Au can enhance the activity of Pt towards the EOR. The in situ FTIR studies confirm that the EOR processes on these icosahedra are all dominated by the C2 pathway, and hence we ascribe the enhancements of EOR activities to the faster kinetics of the C2 pathway by producing acetate or acetaldehyde.
研究领域:
材料科学
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电催化
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale Research Letters
·
2019
·Vol. 14
·期 1
·1-9
·
IF 3.159
Li Xiaoliang,Feng Jiangjiang,Sun Jia,Wang Zhe,Zhao Wei
TiO 2 (P25)-supported Au-Pd bimetal nanoparticles displayed excellent performance in the solvent-free benzyl alcohol catalytic oxidation. However, little research attention has been paid to investigate the effects of TiO 2 form on the catalytic activity of Au-Pd/TiO 2 . In the present research, rutile, brookite, and anatase TiO 2 were successfully synthesized and subsequently applied as the carrier to load Au-Pd nanoparticles by the deposition-precipitation method. The experimental results indicated that the benzyl alcohol conversion employing the rutile TiO 2 -supported Au-Pd catalyst is higher than the conversion of anatase and brookite TiO 2 -loaded Au-Pd catalysts. However, the Au-Pd/TiO 2 -rutile displayed the lowest and highest selectivity toward benzaldehyde and toluene, respectively. ICP-AES, XRD, XPS, and TEM were conducted to characterize these catalysts. The corresponding experimental results revealed that the excellent performance of Au-Pd/TiO 2 -rutile catalyst was attributed to both the smaller Au-Pd nanoparticle size distribution and the higher concentrations of O α and Pd 2+ species on the catalyst surface. In the recycle experiments, the Au-Pd/TiO 2 -rutile catalyst displayed lower reaction stability compared with the Au-Pd/TiO 2 -anatase and Au-Pd/TiO 2 -brookite, which might be due to the coverage of larger amount of aldehyde products on the surface.
研究领域:
化学
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材料科学
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DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2025
·
IF 3.7
Yuanming Feng,Yunpeng Bi,Yifei Wang,Fang Yang,Guangxing Yang,Yuguang Jin,Xiaoyue Wan,Yihu Dai,Yanhui Yang,Dan Yang,Chunmei Zhou
Graphical Supported AuPd alloy, Au@Pd core-shell, Au−Pd Janus particle and Au+Pd mixture catalysts with different configurations were prepared to selectively oxidize GLY toward DHA, in which AuPd/CNT catalyst with the strongest interaction between the Au and Pd atoms afforded the superior catalytic performance. Gold/palladium binary catalysts have been widely used to the selective oxidation of glycerol to produce value-added chemicals. However, the essential effect of the structure of Au/Pd binary catalysts on the catalytic performance has not been elucidated yet. In this work, Au, Pd, AuPd alloy, Au@Pd core-shell, and Au−Pd Janus nanoparticle catalysts prepared by sol-immobilization and photochemical deposition methods were employed to the selective oxidation of glycerol toward dihydroxyacetone (DHA). The results showed that the activation of glycerol and oxygen molecule was significantly promoted with the appropriate interaction between Au and Pd atoms. That was, the turnover frequency of glycerol and DHA generation rate over the alloyed AuPd nanoparticles were remarkably higher than those of Au@Pd core-shell and Au−Pd Janus nanoparticle catalysts. It was due to the synergistic effect of Pd and Au atoms remarkably promoted the electron transfer from Pd to Au, resulting in increasing the activity of the exposed Au sites, and moderately inhibiting the activity of the exposed Pd sites, which benefited to generate DHA rapidly. After optimizing, up to 61 % yield of DHA was achieved at 87 % glycerol conversion over the alloyed AuPd catalyst.
研究领域:
化学工程
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Tianhang Liu,Kaisheng Yao,Hang Li,Qi Wang,Tianhang Han,Aozhou Wang,Haili Zhao,Weiwei Lu
Developing a simple, environmentally friendly, and mild method to one-step prepare bimetallic nanoframes is pretty important but still technically challenging. In this paper, a simple and easy-to-operate ionic liquid (IL)-regulated protocol is proposed to fabricate Au–Pd superbranched trigonal nanoframes (STNFs) in water at room temperature. In the aqueous solution containing precursors (Na2PdCl4 and HAuCl4) and a reducing agent (ascorbic acid), a common IL 1-octyl-3-methylimidazolium chloride ([C8mim]Cl) was used to guide the anisotropic growth and construction of Au–Pd STNFs, brightly showing green and energy-saving characteristics. Au–Pd STNFs take shape as unique two-dimensional (2D) trigonal frameworks containing multilevel orderly branches. It is found that [C8mim]Cl is crucial to the formation of Au–Pd STNFs. Owing to the unique structures, high specific surface areas, large freestanding sizes, and probably electronic effects between Au and Pd, Au–Pd STNFs-1 exhibit dramatically enhanced catalytic activity, selectivity, durability, and convenience for recycling in the 4-nitrostyrene hydrogenation reaction. Specifically, 4-nitrostyrene can be converted completely only within 5.0 min at 25 °C under atmospheric pressure, and the selectivity toward 4-nitroethylbenzene is as high as 100% and maintains good performance after five cycles. It is expected that well-constructed Au–Pd STNFs also display advanced potential in other applications.
研究领域:
材料科学
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催化化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Qiuxiang Wang,Junlin Cai,Yu Sun,Weizhen Chen,Hongpu Huang,Shupeng Wang,Luhong Fu,Shuifen Xie
Three-dimensional (3D) porous heterogeneous metallic nanomaterials hold remarkable competitiveness in electrocatalytic fields due to their flexible porous structure and the electronic effect between heteroatoms, but challenges in synthesis still remain. Here, we design a facile stepwise reduction method to successfully synthesize urchin-like Au/Pd nanobranches (NBs). In a one-pot synthesis, small Au nanoparticles were initially generated. Later, numerous Pd nanotwigs were epitaxially grown and interlaced on the Au seeds to create unique channels, forming an Au-core/Pd-branches structure eventually. The as-prepared Au/Pd NBs exhibit greatly improved activity and stability for alkaline oxygen reduction reaction (ORR) electrocatalysis compared to the commercial Pt/C, with mass activity (1.4 A mg–1) and specific activity (2.4 mA cm–2) increased by 8.8 and 8.9 times, respectively. The excellent ORR performances of Au/Pd NBs are mainly attributed to the optimized electronic structure, improved utilization of surface active sites, and accelerated mass and charge transfer, which derives from the strong ligand effect, as well as the abundant porous channels of the Au/Pd NBs structure. The controllable design and synthesis of 3D porous Pd-based nanomaterials sheds light on a gigantic potential for ORR electrocatalysis.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Kaisheng Yao,Tianjin Li,Chenchen Zhao,Weiwei Lu,Shuang Zhao,Jianji Wang
Conceiving a simple, green, and mild one-pot route to grow and construct anisotropic bimetallic 3D architectures with multilevel structures and promising functions is highly desirable and technically important in many applications. Herein, a facile ionic liquid-modulated strategy is presented for the preparation of hyperbranched Au3Pd1 bimetallic nanodendrites (NDs) in aqueous solution at room temperature. To implement this protocol, HAuCl4 and Na2PdCl4 are used as precursors and ascorbic acid as a reductant, and a common ionic liquid 1-butyl-3-methylimidazolium chloride ([C4mim]Cl) is utilized to direct the anisotropic growth of 3D Au3Pd1 NDs, which exhibits an eco-friendly feature. It is shown that the alloy Au3Pd1 NDs possess multilevel architectures, that is, primary 3D large flowers (with diameters of about 2.5–4.0 μm), secondary 2D leaves, tertiary symmetric branches, and quaternary symmetric petals. A series of factors influencing morphologies and properties of the products are investigated, and the results indicate that both [C4mim]Cl and Au/Pd atomic ratios are crucial to the formation of 3D Au3Pd1 NDs. Owing to the well-defined morphology and probable electronic effects between Au and Pd, the 3D Au3Pd1 NDs display high catalytic selectivity and good durability toward stepwise hydrogenation of 4-nitrophenylacetylene with a 100% conversion and 99.5% selectivity to 4-nitrostyrene in the first step and then 100% conversion from 4-nitrostyrene and 96.7% selectivity to 4-nitroethylbenzene in the second step. It is believed that the well-defined 3D Au3Pd1 NDs would also exhibit promising applications in other catalysis and eletrocatalysis applications.
研究领域:
材料科学
·
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）