ACS Applied Materials & Interfaces
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2020
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IF 8.758
Jin Li,Ying Song,Yanna Wang,Hui Zhang
A series of hierarchical nanosheet array-like Co–Al layered double hydroxides (LDHs)/reduced graphene oxide (rGO) hybrid supported ultrafine PdCu nanocluster (NC) catalysts m-PdCux/LDHs/rGO (x: Cu/Pd molar ratio of 1.5, 3.0, and 5.5; m: Pd loadings of ∼0.80, 0.40, 0.11, and 0.01 wt %) were assembled via an ultrasonic-assisted NaBH4 reduction–sol immobilization strategy. The as-obtained catalysts display ultrafine PdCu alloy NCs with sizes of ∼0.9–1.8 nm finely tuned by both Cu/Pd ratios and Pd loadings and mainly distributed on the edge sites of LDH nanosheets and part of LDHs–rGO junctions upon the unique hierarchical nanosheet array-like structure. Three catalysts 0.85-PdCu1.5/LDHs/rGO, 0.83-PdCu3.0/LDHs/rGO, and 0.80-PdCu5.5/LDHs/rGO exhibit excellent Heck reactivity for iodobenzene with styrene, of which the 0.83-PdCu3.0/LDHs/rGO shows the highest activity, much higher than Pd/LDHs/rGO and single LDHs or GO supported PdCu3.0 catalysts, attributed to the ultrafine PdCu3.0 NCs, the largest electron density of the Pd0 center, and the strongest PdCu3.0 NCs–LDHs–rGO three-phase synergistic effect. The lowest Pd-loading sample 0.01-PdCu3.0/LDHs/rGO shows an unprecedented turnover frequency of 210 000 h–1 (Pd dosage: 2 × 10–5 mol %) with the highest value so far, excellent adaptability for substrates, and reusability. The present work provides a versatile method for designing hierarchically structured ultrafine Pd–M alloy NC catalysts for varied catalysis processes.
研究领域:
催化化学
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材料科学
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纳米技术
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产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
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2018
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IF 0
Yanfang He,Xiangheng Niu,Longhua Li,Xin Li,Wenchi Zhang,Hongli Zhao,Minbo Lan,Jianming Pan,Xifeng Zhang
Nanomaterials with enzyme-like characteristics (nanozymes) are an emerging alternative of traditional bioenzymes that holds great promise in a variety of fields. The activity and efficiency of most current nanozymes, however, are lower than those of natural enzymes, which will inevitably hinder their wider applications. Thus, the development of new nanozymes with favorable catalytic properties is urgently desired. In this work, we reported a coral-structured bimetallic PdCu nanozyme that exhibited enhanced peroxidase activity and efficiency. The coral-like nanozyme fabricated by a microwave-assisted wet-chemical method was composed of assembled PdCu branches. In a comparison with pure Pd, the bimetallic PdCu had an enhanced ability to catalyze the reaction of colorless tetramethylbenzidine (TMB) to its blue oxide (TMBox) in the presence of hydrogen peroxide (H2O2). X-ray photoelectron spectroscopy and theoretical calculation indicated that the insertion of Cu atoms into the Pd lattice would increase the Pd0 proportion and decrease the adsorption difficulty of H2O2, both of which finally resulted in improvements in the catalytic activity and efficiency. It was further found that thiocyanate (SCN–) could inhibit the color reaction by decreasing the activity of PdCu selectively. On the basis of this principle, SCN– in the much wider range of 0.001–100 μM could be detected, along with a limit of detection down to 1 nM.
研究领域:
材料科学
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生物化学
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分析化学
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产品关联
DOI
BIOSENSORS & BIOELECTRONICS
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2015
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IF 6.409
Dan Wu,Xiang Ren,Lihua Hu,Dawei Fan,Yang Zheng,Qin Wei
A highly sensitive electrochemical adenosine aptasensor was fabricated by covalently immobilizing 3′-NH 2 -terminated capture probe (SSDNA1) and thionine (TH) on Au–GS modified glassy carbon electrode. 3′-SH-terminated adenosine aptamer (SSDNA2) was adsorbed onto palladium/copper alloyed supported on MWCNTs ( [email protected] )-conjugated multiple bienzymes, glucose oxidase (GOx), and horseradish peroxidase (HRP) (SSDNA2/ [email protected] /HRP/GOx). Then, it was immobilized onto the electrode surface through the hybridization between the adenosine aptamer and the capture probe. The signal was amplified based on the gradual electrocatalytic reduction of GOx-generated hydrogen peroxide by the multiple HRP through the mediating ability of the loaded multiple TH. However, the peak current of TH decreased in the presence of adenosine because the interaction between adenosine and its aptamer made SSDNA2/ [email protected] /HRP/GOx release from the modified electrode . Various experimental parameters have been optimized for the detection of adenosine and tests for selectivity , reproducibility and stability have also been performed. Under the optimal condition, the proposed aptasensor displayed a wide linear range (10–400 nM) with the low detection limit (2.5 nM), which has been applied in human serum samples with satisfactory results. Thus, the combination of Au–GS as a sensor platform and [email protected] /HRP/GOx as labels can be a promising amplification strategy for highly sensitive adenosine detection.
研究领域:
生物传感器
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分析化学
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医学检测
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Bin Wang,Tie-yan Chang,Zhao Jiang,Jin-jia Wei,Tao Fang
The unsatisfactory performance with high precious metal dosage of dehydrogenation catalysts has been the bottleneck for the development of liquid organic hydrogen carrier (LOHC). The most representative dodecahydro- N -ethylcarbazole in LOHC also faces the same problem. Here, we report a series of bimetallic PdCu catalysts with different ratios supported on reduced graphene oxide prepared by a facile one-pot synthesis method. The most cost-effective Pd 1.2 Cu/rGO catalyst with the lowest amount of precious metals in the catalysts reported for dehydrogenation of dodecahydro- N -ethylcarbazole was selected from a series of samples, while maintaining the catalytic activity and selectivity to the final product of N-ethylcarbazole as the Pd/rGO catalyst with the highest activity in recently reported studies. At the same time, the change of Pd and Cu content and the effect of preparation temperature on dehydrogenation performance were also studied, and the corresponding reaction kinetics were revealed. In combination with various characterization methods of catalyst, the relationship between structure and properties of PdCu NPs was explored in depth. The average particle size and electron transfer between Pd and Cu were identified as the key factors affecting the catalytic activity.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
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2021
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IF 6.901
Na Ye,Yanxin Bai,Zhao Jiang,Tao Fang
For the first time, PdCu/TaN C catalyst with a special core-shell structure is assembled, which exhibits high catalytic performance for methanol oxidation reaction (MOR) in alkaline medium (1326.95 A g Pd −1 ) and formic acid oxidation reaction (FAOR) in acidic medium (1052.63 A g Pd −1 ), 6.3 and 4.9 times those of the commercial Pd/C, respectively. According to the results of Tafel, Electrochemical Impedance Spectroscopy (EIS), CO stripping and chronoamperometry (CA), it is revealed that the reaction kinetics, anti-CO poisoning ability and stability of PdCu/TaN C for MOR and FAOR are all enhanced significantly. Density Functional Theory (DFT) calculations also indicate that the adsorption intensity of CO is weakened and the binding intensity of OH is enhanced on the Pd 3 Cu 1 /TaN(001) surface, which are beneficial to the removal of adsorbed CO and enhancement of the anti-CO poisoning ability. Combined with the characterization analysis and theoretical calculations, the good catalytic performance of PdCu/TaN C for MOR and FAOR can be attributed to the unique electronic structure and morphology from the effective interface, geometric effects and proper d-band center.
研究领域:
电化学
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催化材料
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理论计算
✓ 已验证
DOI
高影响因子
ChemElectroChem
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2020
·Vol. 7
·期 12
·2614-2620
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IF 4.154
Qingfeng Zhang,Fan Li,Lina Lin,Jiaheng Peng,Wencong Zhang,Wenlong Chen,Qian Xiang,Fenglei Shi,Wen Shang,Peng Tao,Chengyi Song,Rong Huang,Hong Zhu,Tao Deng,Jianbo Wu
Graphical Shape the future : PdCu intermetallic cubes and spheres are synthesized to investigate the facet dependence on the oxygen reduction reaction and peroxide reduction. The cubes show large improvements in mass activity towards both reactions, compared with the spheres. DFT calculation uncovers that the dominant {100} faces of the cubes offer more appropriate oxygen adsorption and are thermodynamically favorable for peroxide reduction compared to the surface of spheres. Palladium-based nanocatalysts have the potential to replace platinum-based catalysts for fuel-cell reactions in alkaline electrolytes, especially PdCu intermetallic nanoparticles with high electrochemical activity and stability. However, unlike the synthetic methods for obtaining the nanoparticles, the effect of PdCu shape on the performance is relatively less well studied. Here, we demonstrate the facet dependence of PdCu intermetallics on the oxygen reduction reaction (ORR) and peroxide reduction, and reveal that the {100} dominant PdCu cubes have a much higher ORR mass activity and specific activity than spheres at 0.9 V vs. RHE, which is four and five times that of commercial Pd/C and Pt/C catalysts, respectively, and show only a 31.7 % decay after 30 000 cycles in the stability test. Moreover, cubic PdCu nanoparticles show higher peroxide electroreduction activity than Pd cubes and PdCu spheres. Density functional theory (DFT) calculation reveals that the huge difference originates from the reduction in oxygen adsorption energy and energy barrier of peroxide decomposition on the ordered {100} PdCu surface. Given the relationship between the shape and electrochemical performance, this study will contribute to further research on electrocatalytic improvements of catalysts in alkaline environments.
研究领域:
材料科学
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电化学
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催化
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Small
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2024
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IF 13
Saima Ashraf,Yanyan Liu,Shuling Liu,Sehrish Mehdi,Huanhuan Zhang,Ruofan Shen,Xianji Guo,Xianli Wu,Jianchun Jiang,Yongfeng Wang,Baojun Li
Palladium-based catalysts are remarkable in endorsing hydrogen (H 2 ) generation through formic acid (HCOOH, FA) dehydrogenation under near-ambient conditions. Hydrogen energy efficiency depends on high-performance catalyst design. In this study, Pd-Cu nanoalloy catalysts with mutable atomic ratios are successfully fabricated on TiO 2 nanosheets (TiO 2 -NSs).The synergistic electronic interactions between Palladium (Pd) and copper (Cu) are revealed through a density of states (DOS) analysis of alloy supported over a mixed valence state of Ti linked to oxygen vacancies (Vo) in TiO 2 -NSs, Enhanced adsorption of target molecules reveals novel active sites for Formic acid dehydrogenation (FAD), with O─H bond cleavage via HCOO formate intermediate preceding C─H and C─O bond cleavage. Experimental and theoretical research demonstrates that the Pd-Cu/TiO 2 -NSs (3:7) catalyst d electron redistribution and d-band center shift lower the activation energy for O─H bond cleavage, exhibit superior H 2 production than pure Pd and Cu, increasing Pd electron density due to synergistic effects from reactive crystal facets, defects, and strong metal support interactions (SMSI), lowering the activation energy for HCOOH dissociation step, generating carbon dioxide (CO 2 ) and H 2 with a unprecedented high turnover frequency (TOF) of 6268 mol H2 .h −1 .molPd −1 at 303K with activation energy ( E a ) of 15 KJ mol −1 . This attempt models an efficient HCOOH-to-hydrogen catalyst.
研究领域:
催化
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材料科学
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化学工程
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能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Yuhong Li,Yujun Cheng,Yutian Huang,Pengcheng Zhao,Junjie Fei,Yixi Xie
Glyphosate (Gly), as a widely used broad-spectrum herbicide, may lead to soil and water pollution due to its persistence in the environment. Herein, the co-reduction method was employed to anchor bimetallic PdCu onto the Ni and nitrogen-doped 3D Flower-like Carbon Materials (Ni@NC), creating a composite material (PdCu/Ni@NC) with high specific surface area and good catalytic performance. This composite was used to modify screen-printed electrodes (SPE) to develop a portable and efficient Gly detection platform. In the presence of Cl⁻, the copper active sites convert to CuCl, achieving signal amplification. Upon the addition of Gly, a competitive reaction between Cu and Gly converts CuCl into a Cu-Gly complex, resulting in a sharp decrease in the electrochemical signal. This signal drop is used to detect Gly. The bimetallic PdCu nanoparticles (NPs) endowed the sensing platform with better stability and electrochemical performance due to their synergistic effect, and their stability was simply verified by Density functional theory (DFT). The sensor demonstrates a linear detection range spanning from 1 × 10⁻¹ ³ to 1 × 10⁻⁵ M, with a limit of detection (LOD) of 3.72 × 10⁻¹ ⁴ M. The sensor demonstrated a recovery rate of 95.9 % to 104.5 % in actual samples such as water and soil, indicating its potential for practical application.
研究领域:
环境科学
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分析化学
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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
Materials Research Express
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2024
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IF 1.8
Wende Fan,Yulin Xie,Yinyuan Zhang,Xiaoju Li,Chunxia Li
Combined chemodynamic/photothermal therapy has great potential in tumor treatment. However, the presence of excessive glutathione (GSH) in the tumor microenvironment (TME) can attenuate its therapeutic effect, and other components in the TME have not been fully utilized as well. In this article, we designed a noble metal nanozyme called PdCu@BSA, which can be used for the combined chemodynamic therapy (CDT) and photothermal therapy (PTT) of tumor. In detail, PdCu@BSA has three different types of enzyme-like activities. Its catalase (CAT)-like activity can degrade extra H2O2 in the TME to create O2 and relieve the hypoxic situation. The glutathione oxidase (GSHox)-like activity can consume high level of GSH in the TME to reduce the consumption of reactive oxygen species (ROS). Peroxidase (POD)-like activity catalyzes H2O2 to form strong oxidized ·OH. The above enzyme-like activities enhance the effectiveness of CDT. Besides, PdCu@BSA has good photothermal effect and can be used for PTT when exposed to 1064 nm laser. Therefore, based on multiple enzyme-like activities and photothermal effects, PdCu@BSA can be employed for synergistic tumor therapy, resulting in good therapeutic outcome.
研究领域:
纳米技术
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癌症治疗
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生物医学工程
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材料科学
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生物化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2019
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IF 6.361
Tongxin Song,Fei Gao,Liujun Jin,Yangping Zhang,Cheng Wang,Shujin Li,Chunyan Chen,Yukou Du
At present, although a large number of palladium-based nanowire electrocatalysts have been prepared, there are few reports on nanowires containing rich metal oxides . Herein, porous PdCu alloy nanowires and PdCu-SnO 2 nanowires were prepared by using a galvanic displacement synthesis method. Due to their one-dimensional structure, rough surfaces with non-homogeneous edges, electronic effect, and the advanced PdCu/SnO 2 interface of the as-synthesized PdCu-SnO 2 nanowire catalysts, they exhibited a mass activity of 7770.0 mA mg −1 towards ethanol oxidation , which was 7.6-fold higher than that of Pd/C catalysts (1025.0 mA mg −1 ). In addition, they behaved strong durability upon chronoamperometry and continuous cyclic voltammetry tests. The electrochemical measurements demonstrated that SnO 2 was introduced into the PdCu/SnO 2 interface, which promoted the oxidation of ethanol at a lower potential and accelerated the oxidation of Pd-CO ads via SnO 2 -OH ads to regenerate the active sites. This research highlights the significance of introducing metal oxides into the nanostructure interface, and the performance of Pd-containing catalysts towards ethanol oxidation reaction was greatly improved.
研究领域:
材料科学
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电化学
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催化反应
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Ziyi Li,Xiaolong Zhu,Jiamu Xiao,Wei Lu,Donglin Gan,Jian Shen,Xuefeng Jiang,Mingqian Wang
The misuse of antibiotics exacerbates the problems of bacterial resistance, rendering antibiotic treatment ineffective and, in severe cases, posing life-threatening risks. Therefore, the development of novel antimicrobial materials and their clinical applications have garnered significant attention from healthcare professionals. Bimetallic nanozymes hold significant potential for treating clinical bacterial infections, owing to their superior antimicrobial activity and excellent biocompatibility. In this study, PdZn and PdCu bimetallic nanozymes with folded structures were synthesized using a one-step hydrothermal method. Their photothermal and peroxidase-like catalytic activities were compared, and the underlying causes of the variations in their catalytic performance were analyzed through computational studies. Additionally, the antimicrobial efficacy and wound-healing potential of these two nanozymes were evaluated. Experimental results demonstrated that PdCu exhibited superior catalytic performance compared to PdZn, which aligned with density functional theory calculations confirming its enhanced catalytic ability. In vitro antimicrobial experiments have successfully demonstrated that PdZn and PdCu can effectively inhibit the survival of Escherichia coli and Staphylococcus aureus down to less than 2 % by utilising the synergistic effect of photo-thermal catalysis at 980 nm near-infrared laser. Antibacterial experiments in vivo demonstrated that PdZn and PdCu nanozymes could promote wound healing and slow down the inflammatory response. PdCu exhibited a superior ability to promote wound healing compared with PdZn. PdCu + H 2 O 2 + NIR and PdZn + H 2 O 2 + NIR decreased the trauma area to 9.37 % and 6.04 % respectively, whereas the control group decreased it to only 41.21 %. Overall, this study further explores the potential of Pd-based nanozymes for biological applications and provides guidance for the synthesis of highly efficient Pd-based 2D nanobiomaterials.
研究领域:
生物医学
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材料科学
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纳米医学
✓ 已验证
产品关联
DOI
高影响因子
ACS Materials Au
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2022
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IF 0
Qingsong Luo,Hai Wang,Liang Wang,Feng-Shou Xiao
Selective hydrogenation of acetylene to ethylene is an industrially important process to purify the raw ethylene stream for producing high-grade polyethylene. The supported Pd catalyst exhibits superior activity for acetylene hydrogenation but suffers from poor ethylene selectivity because of the easy overhydrogenation to produce ethane. Here, we report that the PdCu alloy nanoparticles within siliceous zeolite crystals effectively tuned Pd-catalyzed overhydrogenation into semihydrogenation. This catalyst displayed an ethylene selectivity of 92.9% with a full conversion of acetylene. Mechanism studies reveal that the zeolite fixation stabilized the alloyed structure, where the electron-enriched Pd surface benefits the rapid ethylene desorption to hinder the deep hydrogenation. This work provides an efficient strategy for a rational design of bimetallic metal catalysts for selective hydrogenations.
研究领域:
催化化学
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材料科学
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纳米技术
✓ 已验证
DOI
危险品化学品经营许可证（带存储）