ACS Catalysis
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2022
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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
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2023
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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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ACS Applied Energy Materials
·
2023
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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
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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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RSC Advances
·
2023
·Vol. 13
·期 39
·27283-27291
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IF 3.9
Ying Shen,Hongyuan Wu,Xia Luo,Haizhi Zhang,Liming Cheng
In addition to size, shape and morphology, enzyme–mimetic property could be efficiently regulated by controlling composition, forming complexes or hybrids, and surface modification. Herein, Pd nanoparticles with an average diameter of 2.52 nm were decorated on ultrathin 2D copper(II)-porphyrin derived metal–organic framework (MOF) nanosheets by a simple reduction method for catalytic activity regulation. In comparison with other nanozymes, the as-synthesized Pd modified 2D MOF hybrid nanosheets (Pd@Cu-TCPP(Fe)) presented excellent peroxidase–mimic activity, exhibiting an even superior catalytic ability towards H2O2 with a Michaelis–Menten constant as low as 2.33 mM. Based on a cascade reaction between glucose oxidase and Pd@Cu-TCPP(Fe), a colorimetric method for the detection of glucose was established and validated with a wide linear range (0.2–8.0 mM), good recovery (89.5–94.2%) and nice reproducibility (3.65%). All these features guaranteed its excellent ability for glucose determination in human cerebrospinal fluids. This study could offer a valuable reference for constructing novel optical biosensors.
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Journal of Environmental Chemical Engineering
·
2023
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IF 7.7
Juan Miao,Jingmin Wang,Zhen Lv,Xiaoying Feng,Ning Zhang,Xinquan Zhou,Hang Xu,Xuefeng Wei,Shuge Peng
A nitrogen-doped carbon-anchored single atom Pd (SA-Pd/NC) electrocatalyst was prepared by pyrolysis of Pd-doped zeolite imidazolite framework (ZIF) precursors. The SA-Pd/NC catalyst was characterized by high-resolution transmission electron microscopy , aberration-corrected high-angle annular dark field scanning transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy and Raman spectrometry and applied in the degradation of 2,4-dichlorophenol (2,4-DCP). We demonstrate that the SA-Pd/NC catalyst has dual functions, with both electrocatalytic hydrodechlorination (ECH) activity and in situ heterogeneous electro-Fenton (hetero-EF) activity even at low current density. The ECH process was the main pathway of 2,4-DCP degradation without oxygen aeration. Under aerobic conditions , hetero-EF coupling with ECH occurred simultaneously on the SA-Pd/NC cathode, i.e., the dechlorination product phenol was oxidatively degraded with the reactive oxygen species produced on the electrode. The degradation rate of 2,4-DCP and TOC removal rate reached 95.1% and 37.6%, respectively, with a current density of 2.5 mA cm −2 and an initial pH of 3.0. This work provides the design of bifunctional single-atom catalysts for 2,4-DCP degradation, including dechlorination and mineralization.
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APPLIED CATALYSIS A-GENERAL
·
2023
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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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FOOD CHEMISTRY
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2023
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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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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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CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Yi-Bai Sun,Miao Ni,Chen Chi,Dong-Rui Yang,Xue-Lu Chen,Qi Qi,Jian Li,Xing-Hua Xia
The development of efficient catalysts with low energy consumption has always been a key issue for sustainable hydrogen energy. Here, we report a catalyst comprising a single atomic Pd layer deposited on Au nanorods (ML-Pd@Au NRs) that shows a super-high HER activity and ultra-low overpotential under localized surface plasmon resonance condition. The Au NR plays triple determining roles in HER performance via adjusting the electronic structure and lattice strain of Pd that effectively reduces the adsorption energy of H-adatoms, eliminating the penetration of H adatoms in multilayer Pd crystal that decreases the H adatoms diffusion kinetics, and providing high energetic hot charge carriers under near-IR light irradiation that decreases the activation energy and onset potential of HER. The single atomic Pd layer on Au NRs ensures the hot electron transfer as the main dissipation pathway of the plasmonic hot charge carriers for HER. Thus, under near-IR light irradiation, HER on ML-Pd@Au NRs occurs with a high mass activity of 17.47 mA mg −1 at 100 mV and a very low overpotential of 13 mV at 10 mA cm −2 , which are superior to the commercial Pd/C and commercial Pt/C catalysts under the same conditions.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Xin Song,Fangjun Shao,Zijiang Zhao,Xiaonian Li,Zhongzhe Wei,Jianguo Wang
Precise regulation of reaction selectivity at high conversions is the key to non-terminated alkyne semi-hydrogenation. Herein, a support modification strategy was employed to incorporate trace amounts of Mg elements into alumina support. The modified support loaded Pd catalyst optimized the activity and selectivity of the non-terminated alkyne semi-hydrogenation reaction. The TEM and XRD characterization of the catalysts demonstrated the entry of Mg elements into the Al 2 O 3 lattice to achieve the modification of the support. For the 2-butyne-1-ol semi-hydrogenation reaction, the Pd 0.5 /Mg 1 @Al 2 O 3 catalyst showed 99 % conversion and 97 % selectivity of the cis product at hydrogen pressure of 0.1 MPa and 25 °C. The introduced Mg element changed the electronic structure of Pd nanoparticles in the catalyst. The precise regulation of the 2-butyne-1-ol semi-hydrogenation reaction was achieved by adjusting the ratio of Pd 0 to Pd 2+ using the synergistic effect of Pd 0 and Pd 2+ .
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Deng Wang,Jin Liu,Jiangbo Xi,Jizhou Jiang,Zhengwu Bai
Efficient catalyst with enhanced activity and high stability is important for chemical industry. Active species, support as well as their interaction play key roles on catalytic performance for supported heterogeneous catalysts . In this work, Pd Fe dual-metal nanoparticles (NPs) were anchored and confined in an interface of double-layered carbon nanotubes/nitrogen-doped carbon (CNT/NC) support to obtain a dual-metal CNT/PdFe/NC catalyst. The microstructure and composition of CNT/PdFe/NC catalyst were systematically characterized by transmission electron microscopy (TEM), X-ray photoelectron spectrometry (XPS), inductively coupled plasma mass spectrometry (ICP-MS), X-ray diffraction (XRD) and surface area analysis. Benefiting from the catalytically active tubular CNT/NC support, uniformly dispersed Pd Fe dual-metal NPs and unique confined structure, the CNT/PdFe/NC catalyst exhibited excellent catalytic activity for nitroarenes reduction reaction. The catalytic activity of the Pd Fe dual-metal NPs was much better than that of monometal counterparts (CNT/Pd/NC and CNT/Fe/NC), showing an enhanced synergetic effect. The catalytic turnover frequency (TOF) of the CNT/PdFe/NC catalyst amounted to 70.36 min −1 toward 4-nitrophenol (4-NP) reduction reaction, being superior to previously reported noblemetal-based catalysts. Furthermore, this catalyst also exhibited an excellent stability and reusability due to the intrinsic confined structure. This work provides valuable insights to rationally design and develop an efficient dual-metal catalyst.
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