Journal of Saudi Chemical Society
·
2016
·
IF 1.978
Xiaomeng Xia,Xi Gao,Junhui Xu,Chuanfeng Hu,Xinhua Peng
A feasible palladium-catalyzed Wacker oxidation system has been developed, which is characterized by not adding ligand and using hydrogen peroxide as the sole oxidant. Compared with the traditional Wacker system, the described method offers a facile and environment-friendly choice using the green oxidant, and can be applied to more complex substrates.
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高影响因子
RSC Advances
·
2016
·Vol. 6
·期 92
·89157-89166
·
IF 3.289
Zhen Liu,Baoyang Lu,Yansha Gao,Taotao Yang,Ruirui Yue,Jingkun Xu,Lei Gao
In this study, bimetallic Pd–Au/PEDOT/graphene (Pd–Au/PEDOT/rGO) nanocomposites were facilely prepared in an aqueous medium by a one-pot method. In addition to the Pd–Au/PEDOT nanoparticles, dendritic bimetallic Pd–Au nanoclusters were also obtained in the composites, which were verified by transmission electron microscopy and element analysis mapping characterization. The morphology of the nanocomposites was greatly influenced by the molar ratio of the added metal salt precursors. X-ray photoelectron spectroscopy and X-ray diffraction analyses indicated the presence of synergism and electron exchange between the Pd–Au bimetallic nanostructures, which play an important role in the enhancement of the electrocatalytic activity of the composite toward the oxidation of caffeic acid (CA). Under optimized conditions, the Pd–Au/PEDOT/rGO modified glassy carbon electrode showed a wide linear range of 0.001–55 μM and a low detection limit of 0.37 nM (S/N = 3) for CA detection. These results provide valuable insight on the development of novel modified electrodes based on bimetallic graphene nanocomposites for high performance electrochemical sensors.
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Catalysis Science & Technology
·
2022
·Vol. 12
·期 8
·2519-2530
·
IF 6.177
Lixue Qi,Jiajun Dai,Yichen Liao,Jian Tian,Daohua Sun
The low olefin selectivity of Pd-based catalysts is a long-term challenge for the selective hydrogenation of 1,3-butadiene. Hybrid Pd/metal–organic framework (MOF) catalysts may help tackle this problem as they can stabilize Pd nanoparticles and regulate their electronic property. Herein, both surface-supported Pd/ZIF-67 and encapsulated Pd@ZIF-67 catalysts were prepared to explore the synergy between Pd and ZIF-67 and the structure–performance relationship of the catalysts. SEM and TEM reveal the different spatial positions of Pd on the two catalysts. Interestingly, encapsulated Pd@ZIF-67 shows excellent catalytic performance in the 40 h test, with a conversion of 100% and a butene selectivity of 98%, outperforming the surface-supported Pd/ZIF-67 catalyst. XPS, CO-IR and DFT calculations indicate that the encapsulated structure promotes the synergistic interaction between the ZIF-67 and Pd sites. Furthermore, in situ DRIFTS of 1-butene reveals that the enhanced synergistic interaction weakens the adsorption of 1-butene on the catalyst surface while inhibiting its isomerization and further hydrogenation. The presented strategy together with the mechanistic results clarify the relationship between the structure and the synergistic interaction and provide a promising approach for the application of synergistic interactions in hydrogenation catalysts.
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BIOMATERIALS
·
2023
·
IF 14
Yuquan Li,Junxu Yang,Xiaoming Chen,Hao Hu,Nihan Lan,Jinmin Zhao,Li Zheng
Mitochondrial reactive oxygen species (mROS) play a crucial role in the process of osteoarthritis (OA), which may be a promising target for therapy of OA. In this study, novel mitochondrial-targeting and SOD-mimic Mn 3 O 4 @PDA@Pd-SS31 nanozymes with near-infrared (NIR) responsiveness and synergistic cascade to scavenge mROS were designed for the therapy of OA. Results showed that the nanozymes accelerated the release of Pd and Mn 3 O 4 under NIR irradiation, exhibiting enhanced activities of SOD and CAT mimic enzymes with reversed mitochondrial dysfunction and promoted mitophagy to effectively scavenge mROS from chondrocytes, modulate the microenvironment of oxidative stress, and eventually inhibit the inflammatory response. Nanozymes were excreted in vivo through intestinal metabolic pathway and had good biocompatibility, effectively reducing the inflammatory response and relieving articular cartilage degeneration in OA joints, with a reduction of 93.7 % and 93.8 % in OARSCI scores for 4 and 8 weeks respectively. Thus, this study demonstrated that the mitochondria targeting and NIR responsive Mn 3 O 4 @PDA@Pd-SS31 nanozymes could efficiently scavenge mROS, repair damaged mitochondrial function and promote cartilage regeneration, which are promising for the treatment of OA in clinical applications.
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PubMed
高影响因子
ChemCatChem
·
2019
·Vol. 12
·期 5
·1376-1384
·
IF 4.495
Wen-Di Guo,Lei Liu,Shu-Qing Yang,Xiao-Chao Chen,Yong Lu,Giang VO-Thanh,Ye Liu
Graphical Synergetic catalysis : The one-pot tandem bis-alkoxycarbonylation of alkynes was accomplished over the bi-functional catalytic system containing Xantphos-modified Pd-complex and Lewis super-acid of Al(OTf) 3 . Via the synergetic catalysis, the involved Xantphos-modified Pd-complex was responsible for the activation of CO and the alkynes through coordination to Pd-center while Al(OTf) 3 was in charge of the activation of the alcohol to facilitate the formation of [Pd−H] + active species. Tandem bis-alkoxycarbonylation of alkynes allows for the preparation of 2-substituted succinates from alkynes and nucleophile alcohol via two successive alkoxycarbonylation with advantages of 100 % atomic economy and simplified one-pot operation. Herein, the one-pot tandem bis-alkoxycarbonylation of alkynes was accomplished over the bi-functional catalytic system containing Xantphos-modified Pd-complex and Lewis super-acid of Al(OTf) 3 . It was found that, via the synergetic catalysis, the involved Xantphos-modified Pd-complex was responsible for the activation of CO and the alkynes through coordination to Pd-center while Al(OTf) 3 was in charge of the activation of the alcohol to facilitate the formation of [Pd−H] + active species. The in situ high-pressure FT-IR analysis, coupled with 1 H/ 13 C NMR spectral characterizations, confirmed that the introduced Al(OTf) 3 with intensive oxophilicity (via acid-base pair interaction) was able to activate nucleophilic MeOH to be a reliable proton-donor ( i. e . hydride-source) to warrant the formation and stability of [Pd−H] + species upon the oxidation of Pd 0 by H + (Pd 0 +H + →[Pd II −H] + ). Over the developed bi-functional catalytic system, the yields of the target diesters were obtained in the range of 36∼86 % in this sequence with the wide substrate scope.
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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.
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JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Fengxia Tong,Jing Wang,Min Lv,Xiaolei Bao,Wen Xie,Xizhuang Liang,Zhaoke Zheng
Hybrid plasmonic nanostructures exhibit strong interactions with incident light, providing new opportunities for activating the C–H bond in formic acid (HCOOH) for H 2 production. However, it remains a challenge to effectively exciting and extracting plasmonic energy into reactants. Herein, we report a facile strategy to boosting energy transfer by amplifying local electromagnetic field and elucidate plasmon-induced bond activation mechanism at single-particle level. Snowflake-like Pd-Au superstructures (Pd-Au SSs) were chemically synthesized through the selective growth of ordered perpendicular Pd nanoarrays on Au nanostars. Pd-Au SSs possess self-constructed hotspots and high surface-to-volume ratio, enabling efficient energy transfer. The obtained structures exhibited a turnover frequency (TOF) of 15,943 h −1 for H 2 production under plasmon excitation. Furthermore, in situ single-particle analysis showed that the photoluminescence (PL) density of individual Pd-Au SSs was reduced when immersed in HCOOH, which potentially implies that dehydrogenation process might involve indirect energy transfer through charge carriers and direct energy transfer by metal-adsorbate electronic states. Theoretical and experimental analyses revealed that the enhanced local electromagnetic field, which allows high rates of direct resonant transfer of charge from plasmonic nanostructures to the adsorbed molecules, makes significant contributions to C–H bond activation and H 2 production. This work not only provide valuable insights into plasmon-enhanced catalytic processes at single-particle level, but also establish a universal framework for designing novel high-performance multicomponent plasmonic nanostructures with precise geometries.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Yongqing Wang,Zhiqiang Lan,Hong Fu,Haizhen Liu,Jin Guo
MgTM/ZIF-67 nanocomposites were prepared by the deposition-reduction method using ZIF-67, MgCl 2 , and TMCl x (TM = Ni, Cu, Pd, Nb) as raw materials. The dehydrogenation activation energies of MgTM/ZIF-67 (TM = Ni, Cu, Pd, Nb) nanocomposites were calculated to be 115.4 kJ mol −1 H 2 , 115.7 kJ mol −1 H 2 , 113.6 kJ mol −1 H 2 , and 75.8 kJ mol −1 H 2 , respectively; hence, the MgNb/ZIF-67 nanocomposite manifested the best comprehensive hydrogen storage performance. The hydrogen storage capacity of the MgNb/ZIF-67 nanocomposite was hardly attenuated after the 100th hydrogen absorption-desorption cycle. The dehydrogenated enthalpies of MgH 2 and CoMg 2 H 5 in MgNb/ZIF-67 hydride were calculated to be 72.4 kJ mol −1 H 2 and 81.0 kJ mol −1 H 2 , respectively, which were lower than those of additive-free MgH 2 and Mg/ZIF-67. The improved hydrogen storage properties of MgNb/ZIF-67 can be ascribed to the CoMg 2 –Mg(Nb) core-shell structure and the catalytic effects of NbH and niobium oxide nanocrystals .
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高影响因子
CHEMICAL PHYSICS LETTERS
·
2018
·
IF 1.686
Fangchen Zhen,Maofei Ran,Wei Chu,Chengfa Jiang,Wenjing Sun
Pd-Fe 3 O 4 hybrid nanostructures were prepared using a simple one-pot hydrothermal method. The prepared materials were characterized by Fourier transform-infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, transmission electron microscopy, inductively coupled plasma, N 2 adsorption-desorption, and vibrating sample magnetometry. This self-assembled nanosystem acted as an efficient magnetically recyclable noble metal-based multi-functional nanocatalyst. It showed excellent catalytic activity and stability for the Heck reaction of iodobenzene and styrene under mild conditions. The methods used to prepare the Pd-Fe 3 O 4 catalysts were simple and low-cost, which will be useful for the large-scale development and application of a magnetically recoverable Pd catalyst.
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高影响因子
RARE METALS
·
2020
·Vol. 39
·期 12
·1473-1482
·
IF 2.161
Feng Shao-Ping,Huang Kun
Abstract Separation of palladium (Pd) and platinum (Pt) by solvent extraction is difficult because of their extremely similar physicochemical properties. Development of new extractants with a high extraction efficiency and excellent separation selectivity is the primary focus for enhancing the separation of Pd and Pt by solvent extraction. In this study, a new extractant, 2-((2-methoxyethyl)thio)-1H-benzimidazole (MOBI), which contains N, S, and O atoms, was synthesized and used to separate Pd(II) and Pt(IV) from a hydrochloric acid aqueous solution. The experimental results revealed that Pd(II) and Pt(IV) were effectively separated under the optimal conditions: MOBI concentration of 0.005 mol·L −1 , HCl concentration of 0.2 mol·L −1 , organic/aqueous (O/A) phase ratio of 1.0, and contact time of 15 min. The separation coefficient between Pd(II) and Pt(IV) was 1246.40, which indicates that MOBI has a higher selectivity for Pd(II) than Pt(IV). In addition, the mechanism of coordination between Pd(II) and MOBI was demonstrated through the slope method, Fourier transform infrared spectroscopy (FTIR), hydrogen-1 nuclear magnetic resonance spectroscopy ( 1 H NMR), and carbon-13 nuclear magnetic resonance spectroscopy ( 13 C NMR). The results revealed that MOBI could coordinate with Pd(II) via the N atom in the benzimidazole ring of MOBI molecules to form [Pd(MOBI) 2 Cl 2 ] (O) . Graphic abstract
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ANTIMICROBIAL AGENTS AND CHEMOTHERAPY
·
2024
·Vol. 68
·期 3
·
IF 4.1
Xiaonan Zhang,Yan Wang,Sanwang Li,Feifan Xie,Hanxi Yi
Bacterial infections, including those caused by Pseudomonas aeruginosa, often lead to sepsis, necessitating effective antibiotic treatment like carbapenems. The key pharmacokinetic/pharmacodynamic (PK/PD) index correlated to carbapenem efficacy is the fraction time of unbound plasma concentration above the minimum inhibitory concentration (MIC) of the pathogen (%fT > MIC). While multiple targets exist, determining the most effective one for critically ill patients remains a matter of debate. This study evaluated meropenem’s bactericidal potency and its ability to combat drug resistance in Pseudomonas aeruginosa under three representative PK/PD targets: 40% fT > MIC, 100% fT > MIC, and 100% fT > 4× MIC. The hollow fiber infection model (HFIM) was constructed, validated, and subsequently inoculated with a substantial Pseudomonas aeruginosa load (1 × 108 CFU/mL). Different meropenem regimens were administered to achieve the specified PK/PD targets. At specified intervals, samples were collected from the HFIM system and subjected to centrifugation. The resulting supernatant was utilized to determine drug concentrations, while the precipitates were used to track changes in both total and drug-resistant bacterial populations over time by the spread plate method. The HFIM accurately reproduced meropenem’s pharmacokinetics in critically ill patients. All three PK/PD target groups exhibited a rapid bactericidal response within 6 h of the initial treatment. However, the 40% fT > MIC and 100% fT > MIC groups subsequently showed bacterial resurgence and resistance, whereas the 100% fT > 4× MIC group displayed sustained bactericidal activity with no evidence of drug resistance. The HFIM system revealed that maintaining 100% fT > 4× MIC offers a desirable microbiological response for critically ill patients, demonstrating strong bactericidal capacity and effective prevention of drug resistance.
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PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Fu Li,Jingnan Yang,Xiaomei Zhou,Fei Han,Qian Huo,Qingxin Guan,Wei Li
Converting CO 2 to ethanol through photothermal catalysis faces significant challenges due to it involves multi-electron reduction and kinetically sluggish C-C coupling process. Here, copper and a minor quantity of palladium are encapsulated within the cage of UiO-66 using a dual-solvent-sonication method to form ultrafine Cu 2 O/Cu-Pd clusters. The Cu-Cu 2 O serves as an electron center to enhance CO 2 uptake and activation, while the incorporation of Pd accelerates H 2 activation. Due to differences in electronegativity , electrons tend to transfer from Cu to Pd, which reduces the electrostatic repulsion between intermediates and facilitates the coupling of *CO and *CHO. The photothermal ethanol yield of Cu 6 Pd@UiO-66 reached 1077.69 μmol·g cat –1 ·mL –1 with a selectivity of 94.62%, representing an 11.64-fold increase over the non-illumination, and a 3.11-fold enhancement compared with Cu 6 @UiO-66. This study offers evidence supporting the promotion of C-C coupling through an asymmetric electron distribution , potentially advancing the conversion of CO 2 to liquid products.
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