CATALYSIS LETTERS
·
2019
·Vol. 150
·期 4
·1011-1019
·
IF 2.372
Huang Pingquan,Zeng Xiaoyan,Du Fan,Zhang Lei,Peng Xinwen
Abstract Novel thiol functionalized xylose hydrochar microspheres supported palladium nanoparticles (C–SH–Pd) were synthesized by gentle heating of palladium (II) acetate and thiol functionalized xylose hydrochar (C–SH) in ethanol. The as-prepared C–SH–Pd exhibited high catalytic activity towards Suzuki reactions with a yield of high up to 100%. Moreover, it could be reused for at least five times without heavily loss of the catalytic activity. The amount of palladium entrapped on C-SH microspheres was measured by AAS and found to be 1.42 mmol/g. Leaching studies showed that the filtrate contained less than 0.2 ppm Pd. Due to the superior catalytic performance and stability of the C–SH–Pd catalyst, it can be exploited in other cross coupling reactions in the long run. Graphic Abstract
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
Biomaterials Science
·
2022
·Vol. 10
·期 23
·6804-6817
·
IF 7.59
Guiyin Li,Wenzhan Li,Shengnan Li,Xinhao Li,Xiaoqing Yao,Wen Xue,Jintao Liang,Jiejing Chen,Zhide Zhou
Glypican-3 (GPC3) is a membrane-associated proteoglycan that is specifically upregulated in hepatocellular carcinoma (HCC) and has become one of the most promising biomarkers closely related to the occurrence and development of HCC. In this work, platinum@palladium nanoparticles decorated with hemin-reduced graphene oxide (H-rGO-Pt@Pd NPs) were used not only as a support for GPC3 aptamer (GPC3Apt) immobilization, but also as a new redox nanoprobe in electrochemical analysis for the determination of GPC3. The electrochemical aptasensor involved a reaction cell with a three-electrode system, and the differential pulse voltammetry (DPV) technique was adopted. In the presence of GPC3, the formed GPC3Apt–GPC3 complexes had stable structures and were cleaved from the electrode surface, leading to more electroactive H-rGO-Pt@Pd NPs repelling freely from the GPC3Apt/H-rGO-Pt@Pd NPs and thus to the increase of the oxidation peak current of hemin in H-rGO-Pt@Pd NPs. Under optimal conditions and a working voltage of +700 mV (vs. Ag/AgCl), the label-free electrochemical GPC3 aptasensor showed superior performance with a wider concentration linear range (0.001–10.0 μg mL−1), a lower limit of detection (LOD) (0.181 ng mL−1, S/N = 3), a higher sensitivity (0.0446 μA μM−1 cm−2) and good selectivity. Furthermore, the fabricated aptasensor was applied to GPC3 determination in human serum samples with satisfactory recoveries of 94.3%–119% and RSDs of 0.15%–5.78%. The current work provides a flexible approach for the rapid and sensitive analysis of GPC3 and has a broad application prospect in the diagnosis of HCC.
研究领域:
生物医学工程
·
分析化学
·
肿瘤学
✓ 已验证
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 20
·6732-6741
·
IF 6.119
Yafeng Chen,Guimin Jiang,Xiangzhi Cui,Zuotai Zhang,Xinmei Hou
Eliminating indoor formaldehyde (HCHO) pollution at room temperature is highly needed to improve the environment while saving energy. Herein, Pd/CeO2 catalysts with different morphologies of the CeO2 support were employed to investigate their performance for HCHO oxidation. The Pd/CeO2 nanocube (Pd/CeO2-C) catalyst exhibited excellent catalytic activity compared to commercial CeO2 and CeO2 nanorods. HCHO can be completely converted into CO2 and H2O over the Pd/CeO2-C (0.64 wt% Pd) catalyst at a weight hourly space velocity of 36 000 mL g−1 h−1 at room temperature. Multiple characterization results confirmed that the strong interfacial interaction between Pd and the CeO2-C support guarantees a high percentage of metallic Pd on the CeO2-C surface and its high dispersion, which is crucial for the oxidation of formaldehyde at low temperature. The in situ diffuse reflectance infrared Fourier transform results indicated that CO, formate and dioxymethylene species are the main intermediates over the Pd/CeO2-C catalyst, and the active O species is responsible for their decomposition and oxidation. This work may promote the practical application of high performance Pd-based catalysts for indoor HCHO purification and related catalytic processes.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2019
·Vol. 166
·期 4
·F264
·
IF 3.12
Yuxia Pan,Maomao Tu,Xiaoqin Shi,Qi Zhang,Xiaoyu Guo,Mengzhu Li,Yiping Wu,Ye Ying,Ying Wen,Haifeng Yang
The direct methanol fuel cell calls for designing various highly active catalysts containing less platinum, still keeping with reasonable stability. In this work, through controlling reaction system under acidic media (pH = 1), ∼3 nm PtPd nanoparticles are dispersed onto the TiO2 support (3PtPd/TiO2) via a facile one-pot hydrothermal route. In comparison with that of homemade Pt/TiO2 and commercial Pt black catalysts, as-synthesized 3PtPd/TiO2 shows a better performance for directly electrochemical catalysis of methanol and simultaneously exhibits high ability against poison from carbon oxide species. Clearly, the optimized usage of anatase TiO2 not only enhances catalytic activity due to the metal-support interactions but also improves long durability, which could be attributed to the OH existing at the surfaces of TiO2 and Pd.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Min Song,Ming Chen,Chang Zhang,Jingjing Zhang,Wei Liu,Xiao Huang,Jingwen Li,Guang Feng,Deli Wang
The atomic ensemble effect will affect the catalysis on catalyst surfaces and determine the selectivity of multielectron reactions, which is an effective potential strategy to modulate the oxygen reduction reaction (ORR) selectivity for hydrogen peroxide (H2O2) production. Here, we reported the investigation of the ensemble effect on Pt/Pd chalcogenides for the two-electron ORR. A series of Pt/Pd chalcogenides were synthesized via introducing chalcogens into Pt/Pd, resulting in catalysts with isolated Pt/Pd active site. X-ray adsorption spectroscopy reveals the change of the electronic structure. Their ORR selectivity transformed from a four-electron process to a two-electron one, which was attributed to the isolated active sites changing the adsorption mode and the tunable electronic property weakening the adsorption energy. Density functional theory calculations revealed that Pt/Pd chalcogenides possessed a lower binding energy of OOH* and inhibited the breakage of the O–O bond, and PtSe2/C with an optimal adsorption energy of OOH* showed 91% selectivity toward H2O2 production. This work provides a design principle for synthesizing highly selective Pt group catalysts for H2O2 production.
研究领域:
催化化学
·
材料科学
·
理论计算
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2017
·Vol. 164
·期 12
·F1241
·
IF 3.259
Xin Li,Xiangheng Niu,Wenchi Zhang,Qingang Xiong,Yanfang He,Jianming Pan,Tao Zhang,Fengxian Qiu
Exploring advanced electrocatalysts to accelerate the sluggish methanol oxidation reaction (MOR) in the anode of direct methanol fuel cells is a promising route to alleviate the current challenges of fossil fuel exhaustion and environmental pollution. Herein, we develop capping-free PdCo alloys with a coral-like structure and use them as potential electrocatalysts to promote the MOR in alkaline media. A facile microwave-assisted wet chemical approach was established to prepare the unique PdCo architectures, in which no capping agent was employed. Through regulating the precursor ([PdCl4]2− and Co2+) proportion, the ratio of bimetals could be expediently tailored. HRTEM, SAED, XRD and XPS verified the formation of PdCo alloys with different Co abundances on surface. It was found that, together with morphology and crystallinity, the electrocatalytic activities of PdCo materials toward methanol oxidation were highly dependent on their compositions. Among synthesized PdCo structures, the best Pd56Co44 with a moderate Co enrichment on the alloy surface exhibited a mass activity dramatically 11.4 times higher than the pure Pd counterpart. This impressive activity of Pd56Co44 synergistically originated from the bifunctional effects and the electronic interactions between Pd and Co. In addition, the good performance durability of bimetallic PdCo was also demonstrated.
研究领域:
材料科学
·
电化学
·
能源转换与存储
✓ 已验证
DOI
高影响因子
PARTICLE & PARTICLE SYSTEMS CHARACTERIZATION
·
2017
·Vol. 35
·期 5
·1700377
·
IF 4.474
Yaping Li,Qiaoxi Liu,Jianbo Jin,Wei Ye,Canyu Hu,Shanwei Hu,Zeming Qi,Ran Long,Li Song,Junfa Zhu,Yujie Xiong
The heterogeneous nanocatalyst based on palladium (Pd) is one of the most preferable choices for catalytic hydrogenation reactions as the adsorption and dissociation of hydrogen molecules (H 2 ) are almost spontaneous on Pd surface to form the adsorbed H atoms (H ad ). However, in terms of alkyne semihydrogenation, it remains a grand challenge to optimize both the activity and selectivity of reactions using bare Pd catalysts as the case is largely complicated by the excessive H ad produced from rapid H 2 dissociation and the strong Pd-H binding. In this communication, a well-designed model is developed for seeking a selective semihydrogenation catalyst based on surface lattice engineering. In the proposed model, the ultrathin atomic layer of AuPd shell is grown on the Au nanocubes. The Au nanocubes provide specific facets as substrates for hosting catalytic sites, which can also provide information for further lattice engineering design. While Pd atoms are the active centers for hydrogenation reactions in the nanostructures, alloying Pd atoms with Au in the shells can significantly alter the binding of H ad to metals. As such, the activity and selectivity in catalytic alkyne semihydrogenation can be substantially maneuvered by tailoring the atomic arrangement of Pd and Au on surface. As a proof of concept, the Au@AuPd nanocatalyst with a surface Pd/Au ratio of 1:4 achieves a 98.9% semihydrogenation selectivity with a conversion of 98.2% in the 2-methyl-3-butyn-2-ol (MBY) hydrogenation reaction.
研究领域:
材料科学
·
催化化学
·
纳米技术
✓ 已验证
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2017
·
IF 4.95
Dandan Song,Yan Li,Xiong Lu,Muxue Sun,Hui Liu,Guangming Yu,Faming Gao
A highly sensitive acetylcholinesterase (AChE) electrochemical biosensor for the quantitative determination of organophosphate pesticides (OPs) in vegetables and fruits based on palladium-copper nanowires (Pd-Cu NWs) was reported. AChE immobilized on the modified electrode could catalyze hydrolysis of acetylthiocholine chloride (ATCl), generating an irreversible oxidation peak. When exposed to the OPs, the activity of the AChE was inhibited and the current significantly decreased. The detection mechanism is based on the inhibition of AChE. The Pd-Cu NWs not only provide a large active surface area (0.268 ± 0.01) cm 2 for the immobilization of AChE, which was approximately 3.8 times higher than the bare glass carbon electrode, but also exhibit excellent electro-catalytic activity and remarkable electron mobility . The biosensor modified with Pd-Cu NWs displayed a good affinity to ATCl and catalyzed hydrolysis of ATCl, with a low Michaelis–Menten constant ( K M ) of 50.56 μM. Under optimized conditions, the AChE-Cs/Pd-Cu NWs/GCE biosensor detected malathion with wide linear ranges of 5–1000 ppt and 500–3000 ppb, and the low detection limit was 1.5 ppt (4.5 pM). In addition, the OPs biosensor has been applied to the analysis of malathion in commercial vegetable and fruit samples, with excellent recoveries in the range of 98.5%–113.5%. This work provides a simple, sensitive and effective platform for biosensors and exhibits future potential in practical application for the OPs assay.
研究领域:
分析化学
·
环境科学
·
生物技术
✓ 已验证
DOI
高影响因子
JOURNAL OF POLYMERS AND THE ENVIRONMENT
·
2023
·Vol. 31
·期 12
·5261-5271
·
IF 5.3
Li Yuqi,Zhang Hui,Lin Xiaoying,Gong Lingzhu,Shi Ronghui
Water pollution caused by dyeing wastewater discharge, organic chemical reagent leakage and frequent oil spill incidents has aroused widespread international concern. Various methods have been proposed to remove single pollutant from wastewater. However, it is still a challenging task to develop advanced materials that can simultaneously and effectively remove various pollutants from wastewater. In this study, we successfully fabricated a novel multifunctional Pd-decorated alginate/nanofibrillated cellulose (Pd@ALG/NFC) aerogel through a facile and green in-situ reduction, followed by solution-aerogel conversion strategy. The as-prepared Pd@ALG/NFC aerogel exhibited superior catalytic activity toward methylene blue (MB) with a high degradation efficiency above 99% and excellent underwater superoleophobicity with OCA > 150° for various oils. It enabled rapid degradation of MB and efficient separation of different kinds of organic pollutants and oils from water by gravity, with an efficiency exceeding 98.3% and a water flux above 120.5 L·m − 2 ·min − 1 . Moreover, the aerogel is compressible, shape stable and recyclable. These features make the hybrid aerogel a promising candidate for multi-pollutants wastewater treatment.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2024
·
IF 3.7
Junzhe Xu,Shuang Liu,Lin Li,Xian Qin,Ruixin Qu,Jinguo Wang,Di Liu,Gaixia Wei
We synthesized CN11, a carbon nitride material rich in sp 3 hybrid graphitic nitrogen (sp 3 -N), employing a facile oxalic acid-assisted melamine molecular assembly strategy. CN11 promoted the formation of Pd nanoparticles (NPs) predominantly exposing {2 0 0} facets, termed Pd/CN11-2. This facet-specific configuration significantly boosted hydrogen adsorption, leading to notable improvements in catalytic activity. Compared to Pd/XC-72-2 and Pd/g-C 3 N 4 -2, Pd/CN11-2 exhibited a remarkable two-fold and nineteen-fold increase in catalytic yield for hydrazo compound hydrogenation, respectively. Pd/CN11-2 also demonstrated robust performance across a range of reaction conditions, maintaining excellent yield. This study emphasizes the critical role of tailored support structures in controlling Pd NPs facets, thereby enhancing hydrogenation efficiency. It provides valuable insights for advancing the industrial application of Pd-based catalysts, underscoring the importance of strategic support modulation for optimizing catalytic performance.
研究领域:
催化化学
·
材料科学
·
纳米催化
·
有机合成
·
工业催化
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2015
·
IF 3.313
Lan Yang,Wei Luo,Gongzhen Cheng
Monodisperse trimetallic CoAgPd alloy nanoparticles (NPs) were synthesized by a controlled co-reduction of cobalt (II) acetylacetonate , silver nitrate and palladium acetylacetonate in oleylamine at 90 °C using 2-methylpyridine borane as the reducing agents. This is the first time using amine borane as the reducing agent to synthesize non-noble metal contained monodisperse trimetallic alloy NPs at relatively low temperature. The 2.8 nm monodisperse CoAgPd NPs were further assembled on graphene by a simple solution-phase self-assembly method, and tested for catalytic dehydrogenation of formic acid at room temperature . Unexpectedly, the introducing of small amount of cobalt can significantly enhance the catalytic activity and selectivity.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 10
·期 1
·266-287
·
IF 12.732
Na Ye,Pengcheng Zhao,Xiaoying Qi,Wenchao Sheng,Zhao Jiang,Tao Fang
Core–shell like PdSn–TaN(tantalum nitride)/C catalysts with tunable oxophilicity were prepared through a surfactant-free solvothermal method. Optimized Pd1Sn3–TaN/C exhibited good activity (3293.46 A gPd−1, 15.6 times that of commercial Pd/C), stability and tolerance to COad-like species towards the methanol oxidation reaction (MOR) in alkaline media, which can be ascribed to the interfacial structures and bi-functional effects. Briefly, the core–shell like structure can provide an effective Pd–TaN/C interface related to the large ECSA, and the introduction of Sn can further synergistically modulate the interfacial electronic structures, thereby significantly promoting the MOR performances, as revealed by HRTEM, XPS and electrochemical results. Furthermore, in situ ATR-SEIRAS (attenuated total reflection-surface enhanced infrared absorption spectroscopy) measurements displayed that PdSn–TaN/C went through the dual-channel pathways including a large amount of HCOOad and a small amount of COad towards MOR in alkaline medium, which is different from the single COad pathway on commercial Pd/C. Density functional theory (DFT) calculations indicated that the coadsorption intensity and amount of OH provided a chance for CO conversion into CO2 on Pd4–SnO2/TaN(001). Compared to Pd(111), the CO binding energy was evidently reduced on Pd4–SnO2/TaN(001). Meanwhile, Pd1Sn3–TaN/C also showed high mass activity towards the formic acid oxidation reaction (FAOR) in acidic media, which further confirmed that Pd1Sn3–TaN/C may be a promising bi-functional electrocatalyst with high efficiency.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）