Catalysis Science & Technology
·
2023
·Vol. 13
·期 17
·5058-5070
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IF 5
Zihan Lv,Zeng Hong,Chao Qian,Shaodong Zhou
Pt–Pd alloy nano-catalysts supported on TiO2 were developed to enable efficient light-induced photocatalytic N-alkylation of amines with alcohols. Various techniques such as BET, XRD, XPS, HRTEM, UV-vis DRS, and PL analysis were utilized to characterize the catalysts. The photocatalytic mechanism was discussed based on observation as well as theoretical calculation. It was found that Pt serves as a hydrogen shuttle, extracting hydrogen from alcohols to Pd for subsequent hydrogenation on the Pd site. By changing the Pd/Pt ratio, it is feasible to tune the reaction rates of methanol dehydrogenation and imine hydrogenation simultaneously, resulting in an efficient N-alkylation reaction. As a result, the optimum catalyst Pd1Pt1/TiO2 exhibits excellent catalytic performance which is superior to the previously reported ones in terms of both the catalytic efficiency and the production capacity.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Yalin Yu,Zhihao Dong,Ling Tan,Nannan He,Rong Tang,Fang Jiang,Huan Chen
Diminishing the size of metal nanostructures can significantly improve the performance of catalysts. However, the self-aggregation of small particles is still an insurmountable obstacle, resulting in the unfavorable stability and recyclability. Herein, we designed and fabricated the Pd-CeO 2-x -NC catalyst though an accurate deposition strategy to downsize the Pd particle to sub-nanometer level and enhance its running stability. The CeO 2-x nanoclusters were firstly dispersed on the nitrogen-doped carbon nanosheets. Further, the active Pd sub-nanoclusters were accurately scattered on the surface of CeO 2-x ascribing to the strong metal-support interaction (SMSI) between Pd and CeO 2-x , which was beneficial to promote the catalytic activity. Subsequently, the high oxidation state Pd n + species were formed due to the electron transfer from Pd to CeO 2-x caused by the SMSI effect. Strikingly, the HER performance of Pd-CeO 2-x -NC was surprisingly correlated with the ratio of Pd n + , suggesting Pd n + acted as the dominant active species. Besides, the SMSI effect stabilized the valence state of active Pd n + species and prevented the sub-nanometer Pd clusters from aggregation, which played a vital role for the enhanced stability of the hybrid catalyst. This synthetic process described here is contributed to prepare various nanostructured catalysts with satisfactory stability through the direct targeting strategy.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Shuqian Xie,Lu Deng,Hui Huang,Jie Yuan,Jingkun Xu,Ruirui Yue
Herein, a ternary-nanocomposite Pd-polypyrrole/nitrogen-doped graphene (Pd-PPy/NGE) has been prepared facilely by the one-pot method. In simple terms, PPy was in-situ polymerized on the surface of NGE with PdCl 4 2- as the oxidant, and simultaneously Pd nanopaticles were loaded on the surface of PPy or embedded in PPy particles. The obtained Pd-PPy/NGE nanocomposite exhibits promising electrocatalytic properties toward the oxidation reaction of alcohols in alkaline medium. Especially, the optimized Pd-PPy/NGE (1:50) catalyst possesses mass activity of 2176.7, 1192.7 and 498.9 mA mg Pd -1 toward ethylene glycol , methanol and ethanol electrooxidation , respectively, which are 4.3, 6.7 and 2.9 times of those for commercial Pd/C catalyst. Moreover, the Pd-PPy/NGE (1:50) also shows higher anti-poisoning ability and operating stability than the Pd/C catalyst. The promising electrocatalytic performance of the Pd-PPy/NGE (1:50) for alcohols oxidation can be ascribed to the well dispersion of Pd nanoparticles , the porous and stable three dimentional structure of the composite, and the synergistic effect between different components. The structural randomness of the conducting polymer and the potential synergistic effect between the metal nanoparticles and various supports would provide broad development space for these composites as electrocatalysts in direct alcohol fuel cell .
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zareen Zuhra,Shafqat Ali,Sajjad Ali,Hu Xu,Rongzhen Wu,Yuanyuan Tang
Designing materials for selective recovery of precious metals is a critical challenge in response to recent outbreaks of electronic wastes owing to economic and environmental concerns. We introduced high-performance hybrid materials (MCNTs) comprising of six-amino groups based on hexaaminobenzene metal-organic framework (HAB-MOF) and carbon nano-tube (CNT) sponge for selective recovery of Au(III) and Pd(II). Among all MOFs ever reported in the literature, the particular synthesized 30-MCNT (30 mg HAB-MOF on CNT sponge) exhibited the highest adsorption capacity ( q e ) of 1832 mg/g (45 °C, pH 3.0) for Au(III) and 1651 mg/g (45 °C, pH 1.0) for Pd(II), which can be regarded as a benchmark in the MOF family. The highly selective nature of 30-MCNT was examined in the presence of ten different metal ions and the results showed that the Au(III)/Pd(II) adsorption efficiency was decreased by only 5–10%. Moreover, the Au(III) and Pd(II) recovery was maintained ∼ 100% from the initial solution with metal concentration of 200 mg/L. The superior performance was mainly attributed to the role of abundant amino groups in the hybrid framework, developing several types of interactions with Au(III) and Pd(II) ions such as hydrogen bonding, electrostatic interactions, acid-base affinity and π-π inner sphere complexation. Furthermore, the remarkably high surface area and robust chemical and mechanical stability of CNT-sponge provided an exceptional support for impregnation of HAB-MOF to avail greater active sites and easier handpicked recycle. Density functional theory (DFT) simulation and X-ray photoelectron spectroscopy (XPS) studies were employed to explore the interaction mechanisms during the adsorption processes. Owing to facile and environment-friendly synthesis, excellent recovery and recycling, the material can be possibly considered for industrial application in precious metal recovery.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2021
·Vol. 37
·期 6
·1296-1300
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IF 1.307
Rong Xin,Lu Xiuli,Lu Tongbu
T he fabrication of highly active and easily recyclable Pd-based catalyst is meaningful for their practical application. Herein, a Pd-based dip-catalyst(Pd@Pyr-GDY) is fabricated on graphdiyne(Pyr-GDY) grown on copper foam, and applied in the reduction of nitroarenes. Specially, the as-formed Pd@Pyr-GDY shows good catalytic performance toward the reduction of 4-nitrophenol(4-NP) to 4-aminophenol(4-AP) by NaBH 4 with a rate constant k value of 3.84 min −1 , which is 12-fold higher than that of the commercial Pd/C. More importantly, Pd@Pyr-GDY could be easily and rapidly recovery from the reaction medium and no distinct inactivation was found after six cycles of the reaction. This work presents an easy way to design an efficient and easily recyclable Pd-based catalyst for practical use.
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FUEL
·
2018
·
IF 4.908
Yanyan Lei,Wenzhi Li,Qingchuan Liu,Qizhao Lin,Xusheng Zheng,Qifu Huang,Shengnan Guan,Xinhua Wang,Chengxin Wang,Fengyu Li
The catalytic efficiency of CeO 2 carriers and the catalytic properties of palladium (Pd) nanocrystals loaded on different morphology CeO 2 carrier were studied for lean methane (CH 4 ) combustion. The catalytic activity of simple CeO 2 carriers was ranked in the order of rod-CeO 2 (r-CeO 2 ) > cube-CeO 2 (c-CeO 2 ) > octahedral-CeO 2 (o-CeO 2 ). After the Pd species was loaded on CeO 2 , 90% of CH 4 was converted at 348 °C catalyzed by Pd/octahedral-CeO 2 (Pd/o-CeO 2 ) with (1 1 1) crystal faces, which had much higher catalytic activity comparing with Pd loaded on c-CeO 2 with (1 0 0) crystal faces and r-CeO 2 with (1 1 0) and (1 0 0) crystal faces. The results of XRD , HRTEM , EDS , H 2 -TPR, XPS and elemental mapping showed that the Pd species in the form of Pd 0 and PdO were highly dispersed on surface of all CeO 2 carriers. Most importantly, quasi In-situ XPS results convinced that Ce 3+ /Ce 4+ ion pairs played an important role in the catalytic combustion of low-concentration methane by adsorbing or releasing oxygen. Compared with r-CeO 2 and c-CeO 2 , the concentration of Ce 3+ on the surface of o-CeO 2 carrier was greatly increased when the Pd species were present, which indirectly reflected that the concentration of oxygen vacancies on the carrier surface also increased. Consequently, the high catalytic activity of Pd/o-CeO 2 is not only related to the high dispersion of Pd 0 and PdO species on the surface of the catalyst, but also closely related to the synergistic interaction between Pd species and (1 1 1) specific faces of o-CeO 2 exposing.
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ACS Catalysis
·
2022
·
IF 13.7
Pengfei Han,Cheng Tang,Sarina Sarina,Eric R. Waclawik,Aijun Du,Steven E. Bottle,Yanfen Fang,Yingping Huang,Kun Li,Huai-Yong Zhu
Research on visible-light photocatalysts of metal nanoparticles (NPs) has focused on increasing the reactant conversion by light-excited charges (electrons and positively charged holes). However, light irradiation can accelerate catalysis by other mechanisms. Here, we report that 650 nm wavelength irradiation of 0.75 W·cm–2 significantly increases nitrile yield of ammoxidation of primary aromatic alcohols with an ammonium salt over supported Pd NPs at 80 °C in air. We found that the desorption of the nitrile product from the catalyst is the rate-determining step; the irradiation promotes not only alcohol oxidation and subsequent aldehyde cyanation over the Pd NPs but also the nitrile desorption selectively via resonance energy transfer to achieve a high nitrile yield. This new mechanism provides a knob for the exquisite control of catalytic reaction pathways for ecofriendly synthesis.
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EUROPEAN POLYMER JOURNAL
·
2023
·
IF 6
Jiayi Wang,Yicen Ge,Yue Wang,Rui Sun,Xiao Yang,Haodan Xue,Xiaoyan Ma,Jinyu Liu,Keling Hu
Pd nanoparticles (NPs) supported by micelles formed with poly(2-(dimethylamino)ethyl methacrylate)- b -poly(lauryl methacrylate) (Pd/PDMAEMA- b -PLMA) were prepared and employed as catalyst in the Suzuki-Miyaura cross-coupling reaction of aryl bromides with arylboronic acids in water. Most reactions proceeded with high efficiency at room temperature with only 0.05 mol% Pd loading in the absence of ligands, which afforded the desired functionalized biaryls in 73–98 % yields after 24 h. After reaction, Pd/PDMAEMA- b -PLMA retained in the aqueous phase was easily separated from the insoluble biaryl product and could be further reused two times without significant loss in catalytic efficiency. Characterization of the catalyst disclosed that sub-2 nm Pd NPs were embedded in the hydrophilic corona of polymeric micelles that served as nanoreactors in water.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Liqin Kong,Feng Hong,Peng Luan,Yiping Chen,Yaoze Feng,Ming Zhu
The development of biosensors capable of assessing umami intensity has elicited significant attention. However, the detection range of these biosensors is constrained by the sensing components and strategies used. In this study, we introduce a novel competitive, ultra-high-sensitivity electrochemical impedance biosensor by utilizing composite nanomaterials and T1R1 as a composite signal probe. Pd/Cu-TCPP(Fe) had a substantial surface area, effectively enhancing the loading capacity of the T1R1 and thus augmenting the biosensor's recognition precision. Furthermore, the Pd/Cu-TCPP(Fe) elevated peroxidase-like activity catalyzed the formation of insoluble precipitates of 4-CN, resulting in cascaded amplification of the impedance signal. The remarkable catalytic activity of the composite signal probe endowed the biosensor with exceptional analytical performance, featuring a detection limit of 0.86 pg/mL and a linear detection range spanning from 10 to 10000 pg/mL. Successful application of the biosensor for umami substance detection in fish was also demonstrated, signifying its substantial potential in food-flavor evaluation.
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ACS Applied Energy Materials
·
2023
·
IF 6.4
Rui Chen,Ying-Ying Wang,Xia Jiang,Ming-Hao Ji,Hao-Yan Shi,Hai-Long Wang,Yan-Xin Chen,Can-Zhong Lu
This article describes a photocatalytic (PC) hydrogen evolution technology that utilizes Pd/LaCoO3/PCN nanocomposites. In the preparation process, a narrow band gap pure LaCoO3 phase was obtained using a template method, which was subsequently combined with Pd-NPs loaded with pCN to form a Z-scheme heterojunction. The formation of this heterojunction resulted in a material with improved charge transfer characteristics and electron well performance. Under visible light irradiation, the composite material demonstrated a higher PC hydrogen evolution activity, resulting in a H2 yield of 40.2 μmol g–1 h–1. This yield represents a 259 times improvement over pure pCN materials, respectively. Furthermore, in the presence of a sacrificial agent, triethanolamine (TEOA), the production of H2 increased compared to methanol, likely due to the more vital binding ability of the amine-containing pCN to TEOA. Finally, the study found that Pd/LaCoO3/PCN nanocomposites displayed excellent stability and reusability during three continuous cycles. These results suggest that this material may become an efficient and sustainable technology for solar fuel production.
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SOLID STATE SCIENCES
·
2023
·
IF 3.5
Yinghua Lan,Xuejing Wang,Yanmei Chen,Juan Xu,Yanhui Zhang
The synergistic effect of heavy metal ions and organic pollutants can enhance the photocatalytic performance and provides a new idea for environmental governance, so it has important research value. In this work, we prepared Pd–TiO 2 composites by ascorbic acid reduction method, and obtained the crystal structure, morphology and surface state information of the composites through a series of characterizations, which verified the successful preparation of the composites. It was used for simultaneous photocatalytic removal of bisphenol A (BPA) and Cr(Ⅵ), and it was found that the photocatalytic removal efficiency was significantly improved compared to their individual removal. This can be attributed to the synergistic effect between BPA and Cr(Ⅵ), where they enhance the separation efficiency of photogenerated electron-hole pairs and prolong the lifetime of photogenerated carriers. In addition, the effects of BPA concentration and Cr(Ⅵ) concentration on photocatalytic removal efficiency were also investigated. The mechanism of photocatalytic degradation of BPA by Cr(Ⅵ) coupling system was discussed by changing the experimental conditions, it is proved that the photocatalytic products of BPA can improve the removal efficiency of Cr(Ⅵ).
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APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Qian Wang,Limei Sheng,Xuan Guo,Rong Chen,Chengjie Zhou,Fu Yang
Dynamic kinetic resolution (DKR) of chiral amines with enzyme and noble metal has been widely concerned in chemistry, biology and pharmacy fields. While the synergistic effect and long-term stability of enzyme-noble metal in catalysts remain challenging. In this paper, several functional polymers were designed and employed as the carrier of lipase and palladium (Pd) for one-pot DKR of α-phenethylamine. By modulating the multisite weak force (MSWF) of the polymers on the active centers, the optically pure product with high conversion (>99%) and ee (>99%) were obtained and the designed catalyst Pd@PE-2OH_CalB showed superior stability to other commercial catalysts, such as Pd/C and Novozym 435. Additionally, the heterogeneous chemoenzymatic catalysts could be easily recovered and recycled up to seven times without sacrificing efficiency. Further investigation revealed that the enhanced catalytic performance depended on MSWF formed by the abundant ionic sites, functional groups, and lots of hydrogen bonds of poly(ionic liquid)s.
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