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Catalysts · 2021 ·Vol. 11 ·期 4 ·522 · IF 4.146

Palladium Particles Modified by Mixed-Frequency Square-Wave Potential Treatment to Enhance Electrocatalytic Performance for Formic Acid Oxidation

Fangchao Li,Bin Liu,Yuanhao Shen,Jie Liu,Cheng Zhong,Wenbin Hu

Palladium catalysts have attracted widespread attention as advanced electrocatalysts for the formic acid oxidation (FAO) due to their excellent electrocatalytic activity and relatively high abundance. At present, electrodeposition methods have been widely developed to prepare small-sized and highly-dispersed Pd electrocatalysts. However, the customary use of surfactants would introduce heterogeneous impurities, which requires complicated removal processes. In this work, we reported a two-step electrochemical method that employed square-wave potential treatment (SWPT) to modify electrodeposited Pd particles without the use of capping agents. Under the SWPT with a mixed frequency, Pd particles show significantly reduced size and more dispersed distribution, exhibiting a high mass activity of 1.43 A mg−1toward FAO, which is 4.6 times higher than the counterpart of commercial Pd/C. The increase in electrocatalytic activity of FAO is attributed to the highly developed surface of palladium particles uniformly distributed over the support surface.Keywords:Pd nanoparticles;formic acid oxidation;electrocatalysis;square-wave potential treatment

CAS / MDL: 7440-05-3
研究领域: 化学 · 材料科学
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APPLIED ORGANOMETALLIC CHEMISTRY · 2017 ·Vol. 31 ·期 12 ·e3889 · IF 2.319

Pd nanoparticles supported on CeO2 as efficient catalyst for hydrogen generation from formaldehyde solution at room temperature

Tao Feng,Ranxiao Tang,Ningzhao Shang,Cheng Feng,Shutao Gao,Chun Wang

A facile and efficient method for facilitating hydrogen generation from formaldehyde aqueous solution was developed using Pd nanoparticles supported on CeO 2 (Pd/CeO 2 ) as the catalyst. The prepared Pd/CeO 2 catalyst exhibited 100% H 2 selectivity and excellent catalytic activity for formaldehyde dehydrogenation with the initial rate of 2089 ml min −1 g Pd −1 at room temperature and atmospheric pressure without any extra additive. The prepared catalyst was stable and reusable, and its catalytic activity kept almost unchanged after it was reused for the fifth run. Therefore, it is considered that this Pd/CeO 2 based hydrogen generation system may serve as an alternative hydrogen supply candidate for practical application.

研究领域: 化学 · 能源材料科学
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APPLIED SURFACE SCIENCE · 2017 · IF 3.387

Flower-Like ZnO-Assisted One-Pot Encapsulation of Noble Metal Nanoparticles Supported Catalysts with ZIFs

Lu Lin,Haiou Liu,Xiongfu Zhang

Rational design of efficient approaches to fabricate MOFs-coated core-shell composites is promising but challenging. We report here the encapsulation of Pd nanoparticles (Pd NPs) supported flower-like ZnO (F-ZnO) microspheres with ZIF-8 shell through a facile strategy, in which the formation and immobilization of Pd NPs on F-ZnO supports and the subsequent growth of ZIF-8 shells over them are effectively integrated into one-pot synthetic route. Importantly, the utilization of ZnO both as support of Pd NPs and Zn 2+ source of ZIF-8 is favorable for the implement of one-pot synthesis, due to its functions in anchoring Pd NPs and inducing ZIF-8 formation. Further insights into the morphological influence of zinc oxide particles on the resulting materials indicate that the flower-like microspheres with 2D nanosheets as subunits also benefit the coating of Pd NPs supported cores with ZIF-8, resulting in a well-defined core-shell catalyst. The achieved catalyst deliveries remarkable performance in terms of selectivity, anti-poisoning and recyclability in the liquid hydrogenations of alkenes.

研究领域: 材料科学 · 催化化学
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RSC Advances · 2014 ·Vol. 4 ·期 108 ·63048-63054 · IF 3.708

Plasma synthesis of oxidized graphene foam supporting Pd nanoparticles as a new catalyst for one-pot synthesis of dibenzyls

Liang Ren,Fan Yang,Chunxia Wang,Yongfeng Li,Hailing Liu,Zhiqiang Tu,Liqiang Zhang,Zhichang Liu,Jinsen Gao,Chunming Xu

We have developed an environmentally-friendly method for the synthesis of Pd nanoparticle (Pd NPs) decorated different graphene supports, and the morphology and structure of the hybrids are characterized by transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy and elemental mappings. Four hybrid materials based on graphene foam (GF), oxidized graphene foam (OGF), graphene oxide (GO) and reduced graphene oxide (RGO) have been used to catalyze Heck coupling reactions, and the effect of support on the activity of the hybrid material has been studied. Our results have revealed that Pd NP decorated OGF (Pd/OGF) is the most active catalyst, showing better performance than the commercial Pd/C catalyst. More importantly, the Pd/OGF catalyst has been successfully used for one-pot synthesis of dibenzyls with different aryl bromides and olefins, which has simplified the separation and purification process and realized a green organic synthesis process.

研究领域: 材料科学 · 催化化学 · 环境科学
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GREEN CHEMISTRY · 2022 ·Vol. 24 ·期 4 ·1570-1577 · IF 11.034

Phosphoric acid-modified commercial kieselguhr supported palladium nanoparticles as efficient catalysts for low-temperature hydrodeoxygenation of lignin derivatives in water

Ruixue Yangcheng,Jiansu Ran,Zhaohui Liu,Yuntong Cui,Jianjian Wang

Efficient production of high value-added chemicals and biofuels via low-temperature chemoselective HDO of lignin derivatives in water is still a challenge. Here, we construct a low-cost, active and stable Pd/PCE catalyst using phosphoric acid-modified commercial Celite (PCE) as the support, and this catalyst exhibits excellent activity in low-temperature HDO of vanillin as well as other lignin derivatives in water. The superior catalytic performance is due to the presence of P species on the surface of Pd/PCE, accelerating the selective conversion of the intermediate into the final product. Detailed experimental and mechanistic studies reveal that the rapid conversion of the intermediate to the final product proceeds via a free-radical process in an interfacial microenvironment created by intimate interacting between the P species and Pd NPs. The insights of this work provide a new low-cost catalytic system for efficient production of valuable chemicals and future biofuels from lignin derivatives.

研究领域: 化学工程 · 催化科学
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Particuology · 2024 · IF 4.1

Room-temperature hydrogen adsorption in Pd nanoparticle decorated UiO-66-NH2 via spillover

Jingchuan Wang,Junhong Luo,Yong Yao,Jiangfeng Song,Yan Shi

To improve room-temperature hydrogen storage, palladium (Pd) nanoparticles were innovatively decorated by carbon bridge onto the amino-group functioned Zr-terephthalate metal-organic framework (MOF) UiO-66 to reduce the diffusion energy barrier and then improve the hydrogen spillover effect. Powder X-ray diffraction shows broad Pd peak and retained UiO-66-NH 2 integrity after Pd decoration. The hydrogen uptake capacity show that UiO-66-NH 2 -Pd exhibits best hydrogen storage performance than UiO-66-NH 2 and pristine UiO-66. The hydrogen up taken in Pd decorated UiO-66 (UiO-66-NH 2 -1Pd) was close to 4 wt% under 20 MPa at room temperature. Density functional theory (DFT) calculations show that hydrogen adsorption energy of UiO-66-NH 2 -Pd was −0.5897 eV, which was much lower than that of UiO-66-NH 2 (−0.3716 eV) and UiO-66 (−0.2975 eV). Ultimately, Pd decorated NH 2 group functioned UiO-66 enable improve storage capacities through hydrogen spillover under ambient conditions which could satisfy the demand for sustainable energy, especially for the long-term storage energy media.

研究领域: 材料科学 · 能源科学
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CHEMISTRY-A EUROPEAN JOURNAL · 2024 · IF 3.9

Hollow UiO-66-NH2 encapsulated Pd catalysts for highly selective hydrogenation of furfural to furfuryl alcohol

Bo Zhao,Yao Yao,Kexin Huang,Jiaxin Li,Minjie Chen,Chao Liu,Hongjian Xu,Xinyu Zhao,Ganggang Chang

The selective hydrogenation of furfural (FFA) to furfuryl alcohol (FA) is regarded as attractive transformation to achieve the sustainable synthesis of value-added chemicals from biomass resources. However, the conventional supported catalysts are significantly restricted by their narrow pore size, ununiform dispersion and easy leaching or aggregation of catalytic sites. Herein, we designed hollow UiO-66-NH2 as the support to encapsulate Pd nanoparticles (Pd@H-UiO-66-NH2) to achieve the highly active and selective conversion of FFA to FA. Benefiting from the void-confinement effect and substrate enrichment of hollow structure, as well as the surface wrinkles, the as-prepared catalyst Pd@H-UiO-66-NH2 exhibited 96.8 % conversion of FFA with satisfactory selectivity reaching up to 92.4 % at 80 °C, 0.5 MPa H2 in isopropanol solvent within 6 h. More importantly, as-prepared Pd@H-UiO-66-NH2 catalyst exhibited excellent long-term stability, as well as good universality toward a series of hydrogenation of unsaturated hydrocarbons.

研究领域: 化学工程 · 催化材料科学
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Nanomaterials · 2019 ·Vol. 9 ·期 7 ·1009 · IF 4.034

Highly Efficient Catalytic Performances of Nitro Compounds and Morin via Self-Assembled MXene-Pd Nanocomposites Synthesized through Self-Reduction Strategy

Juanjuan Yin,Lun Zhang,Tifeng Jiao,Guodong Zou,Zhenhua Bai,Yan Chen,Qingrui Zhang,Meirong Xia,Qiuming Peng

With development of the society, the problem of environmental pollution is becoming more and more serious. There is the urgent need to develop a new type of sustainable green material for degradable pollutants. However, the conventional preparation method is limited by conditions such as cumbersome operation, high energy consumption, and high pollution. Here, a simple method named self-reduction has been proposed, to synthesize highly efficient catalytic nitro compounds and morin self-assembled MXene-Pd nanocomposites. Palladium nanoparticles were grown in situ on MXene nanosheets to form MXene@PdNPs. MXene@PdNPs composites with different reaction times were prepared by adjusting the reduction reaction time. In particular, MXene@PdNPs20 exhibited a high catalytic effect on 4-NP and 2-NA, and the first-order rate constants of the catalysis were 0.180 s−1and 0.089 s−1, respectively. It should be noted that after eight consecutive catalytic cycles, the conversion to catalyze 4-NP was still greater than 94%, and the conversion to catalyze 2-NA was still greater than 91.8%. Therefore, the research of self-assembled MXene@PdNPs nanocomposites has important potential value for environmental management and sustainable development of human health, and provides new clues for the future research of MXene-based new catalyst materials.Keywords:nanocomposites;catalyst;MXene;self-reduction;palladium nanoparticles

研究领域: 环境科学 · 材料科学
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Journal of CO2 Utilization · 2019 · IF 5.189

The synergistic effect of Pd NPs and UiO-66 for enhanced activity of carbon dioxide methanation

Haoxi Jiang,Qiang Gao,Shutian Wang,Yifei Chen,Minhua Zhang

Carbon dioxide methanation is of great importance for both environment and energy because of the reduction of carbon dioxide emissions and the utilization of carbon source. In this work, UiO-66 was employed as the support for palladium nanoparticles via a sol-gel method to enhance the activity of CO 2 methanation. The physical-chemical properties of as-prepared catalysts were characterized using N 2 adsorption-desorption, X-ray diffraction (XRD), transmission electron microscope (TEM), temperature programmed desorption (TPD), temperature programmed reduction (TPR), thermo-gravimetric analysis (TGA), Fourier-transform infrared (FTIR) spectroscopy and X-ray photoelectron spectroscopy (XPS). It was found that there was a synergistic effect between UiO-66 and supported Pd. CO 2 could be activated in UiO-66 via its Zr 6 O 4 (OH) 4 nods, while H 2 molecules were dissociated at Pd for further hydrogenation of activated CO 2 . As a result, the catalyst with a Pd loading of 6 wt.% exhibited a high activity with 56.0% of CO 2 conversion and 97.3% of CH 4 selectivity, corresponding to a STY of 856 g·h −1 ·kg cat −1 at 4 MPa and 340 °C.

研究领域: 环境科学 · 能源化学
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Molecular Catalysis · 2021 · IF 5.062

Pd nanoparticles supported on amine-functionalized SBA-15 for the selective hydrogenation of phenol

Huafan Li,Tiantian She,Guofeng Chen,Menghua Sun,Libo Niu,Guoyi Bai

In this paper, a stable Pd/NH 2 -SBA-15 catalyst was prepared by an ammonia evaporation method using amino-functionalized SBA-15 as support. Pd/NH 2 -SBA-15 showed excellent catalytic performance in the selective hydrogenation of phenol to produce cyclohexanone. Furthermore, this Pd/NH 2 -SBA-15 catalyst kept the conversion of phenol and selectivity of cyclohexanone both over 90 % even after 10 runs, much better than Pd/SBA-15 and the previously reported Pd-based catalysts, demonstrating the benefit of amine functionalization on the activity of supported Pd nanoparticles. TEM and XPS results indicate that small Pd particles were highly dispersed on the NH 2 -SBA-15 support and a stronger interaction occurred between the active Pd particles and the amine functionalized SBA-15 support, which could effectively inhibit the agglomeration of the active Pd particles during the reaction and then improve the stability of this catalyst.

CAS / MDL: 919-30-2
研究领域: 催化化学 · 材料科学
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JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL · 2015 · IF 3.615

Hydrodechlorination of chlorophenols catalyzed by SiO2/Pd@m-SiO2 core-shell structured catalyst

Yansheng Liu,Bo Qiao,Xinlin Li,Xuanduong Le,Wei Zhang,Jiantai Ma

Palladium metal nanoparticles have been applied to hydrodechlorination of chlorophenols in contaminated water using H 2 as a clean and sustainable reductant. However, there are two major challenges to widespread technology adoption which are the activity loss caused by nanoparticle aggregation and the difficulty of nanoparticle recovery. In this study, a synthesis of a core-shell structured catalyst with encapsulated Pd nanoparticles has been given and whose catalytic activity has been tested in hydrodechlorination of chlorophenols under 1   atm H 2 at room temperature. The catalyst material consists of a nonporous silica core decorated with Pd nanoparticles that are further encapsulated within an ordered mesoporous silica shell. Well-defined mesopores (2.4   nm) provide a physical barrier to prevent Pd nanoparticle (∼10   nm) movement, aggregation and detachment from the support into water. Compared with some supported Pd catalysts such as Pd/AC and Pd/Al 2 O 3, SiO 2 /Pd@m-SiO 2 exhibits higher catalytic performance. After 5 times of recycling, catalytic activity of SiO 2 /Pd@m-SiO 2 reduces slightly and this result confirms the good recyclability of SiO 2 /Pd@m-SiO 2 . The function of the mesoporous shell, preventing aggregation of active nanoparticles, suggests a promising general strategy of using metal nanoparticle catalysts for water purification and related aqueous-phase applications.

研究领域: 环境科学 · 材料科学
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Reaction Kinetics Mechanisms and Catalysis · 2018 ·Vol. 126 ·期 1 ·463-476 · IF 1.515

Fabrication of Pd@N-doped porous carbon-TiO2 as a highly efficient catalyst for the selective hydrogenation of phenol to cyclohexanone in water

Zhang Jiuxuan,Liu Yefei,Jiang Hong,Chen Rizhi

A highly efficient catalyst with the structure of semiconductor–metal heterojunction for phenol hydrogenation in water was fabricated by loading the Pd nanoparticles on the N-doped porous carbon-TiO 2 (CN-TiO 2 ) materials, which was synthesized via the one-step carbonization of TiO 2 -contained ZIF-67. The microstructures of the as-prepared Pd@CN-TiO 2 catalysts were investigated in detail and the catalytic properties were tested by the phenol hydrogenation under mild conditions. With increasing TiO 2 amount, the charge transfer and specific surface area of Pd@CN-TiO 2 initially increase and then reduce, thereby the catalytic performance show a similar regular pattern. The as-fabricated Pd@CN-TiO 2 exhibits a superior catalytic performance than the Pd nanoparticles supported on TiO 2 or CN separately, owing to their synergistic effect. When the parameters affecting the catalytic efficiency are optimized, the conversion of phenol and selectivity for cyclohexanone can even achieve 98% in pairs with a higher reaction rate of 0.45 mmol h −1 . Furthermore, the Pd@CN-TiO 2 shows stable performance in the recycling experiments.

CAS / MDL: 10026-22-9
研究领域: 材料科学 · 催化化学
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