Journal of Chemistry
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2018
·
IF 1.726
Zou Bin,Chen Xueshan,Xia Jiaojiao,Zhou Cunshan
Conversion of HMF into FDCA was carried out by a simple and green process based on alkaline ionic liquid (IL) modified Pd/C catalyst (Pd/C-OH−). Alkaline ionic liquids were chosen to optimize Pd/C catalyst for special hydrophilicity and hydrophobicity, redox stability, and unique dissolving abilities for polar compounds. The Pd/C-OH− catalyst was successfully prepared and characterized by SEM, XRD, TG, FT-IR, and CO2-TPD technologies. Loading of alkaline ionic liquid on the surface of Pd/C was 2.54 mmol·g−1. The catalyst showed excellent catalytic activity in the HMF oxidation after optimization of reaction temperature, reaction time, catalyst amount, and solvent. Supported alkaline ionic liquid (IL) could be a substitute and promotion for homogeneous base (NaOH). Under optimal reaction conditions, high HMF conversion of 100% and FDCA yield of 82.39% were achieved over Pd/C-OH− catalyst in water at 373 K for 24 h.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
·
IF 11.698
Yazhi Yin,Bing Hu,Xinliang Li,Xiaohai Zhou,Xinlin Hong,Guoliang Liu
Direct CO 2 hydrogenation to methanol provides a means of CO 2 fixation and a way of hydrogen storage in a more energy-dense and transportable form. Pd-ZnO catalysts can be active for this reaction, but their activities are strongly associated with the preparation methods which influence the dispersion and stability of Pd nanoparticle. Here we report a novel fabrication of highly effective PdZn alloy catalysts derived from Pd@zeolitic imidazolate framework (ZIF-8) for the hydrogenation of CO 2 . The confinement of subnanometric Pd particles in the pore framework of ZIF-8 facilitates the formation of Pd-ZnO interfaces with strong-metal-support-interaction (SMSI) after a simple pyrolysis under air condition. The porous texture and high surface area of ZnO ensures a high dispersion of Pd nanoparticles. Different pyrolysis temperatures were studied in catalysis and the highest methanol yield reached 0.65 g g cat −1 h −1 at 270 °C, 4.5 MPa, with a TOF of 972 h −1 , over a PdZn catalyst prepared at 400 °C. Such excellent activity has ranked the top reported values over advanced Pd-based catalysts under comparable conditions. The crucial factors for such high methanol yield are the formation of small-sized PdZn alloy particles after H 2 reduction and abundant surface oxygen defects on ZnO. The SMSI between PdZn and ZnO also ensures a long term stability of our PdZn catalysts. At last, we propose the active site that was strongly associated with methanol formation is a PdZn alloy rather than metallic Pd.
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CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Rongrong Li,Wubing Yao,Yanxian Jin,Wenping Jia,Xiaoying Chen,Jingjing Chen,Jianli Zheng,Yuan Hu,Deman Han,Jia Zhao
Hydrocinnamaldehyde (HCAL) is a crucial intermediate in the manufacture of perfumes and pharmaceuticals, but highly selective hydrogenation of cinnamaldehyde (CALD) to hydrocinnamaldehyde with a good conversion rate is a challenging. We report that the incorporation of Ag into Pd-based catalysts promotes their catalytic activity and HCAL selectivity (HCAL selectivity of 98.6% with >99.9% CALD conversion for Pd-0.3Ag/MCM-41) for CALD hydrogenation compared to those of catalysts with no Ag, e.g., HCAL selectivity of 84.5% for Pd/MCM-41and 77.3% for Pd/AC (activated carbon). The Pd-0.3Ag/MCM-41 catalyst shows an outstanding stability during five cycles of use. The excellent performance of the Pd-0.3Ag/MCM-41 catalyst in CALD hydrogenation is due to the ultra-small size of the Pd nanoparticles (Pd-Ag alloy, a geometric and electronic modification of Pd).
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NEW JOURNAL OF CHEMISTRY
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2017
·Vol. 41
·期 21
·13036-13042
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IF 3.269
Fenfen Lu,Yan Xu,Xia Jiang,Yang Liu,Jiale Huang,Daohua Sun
Low temperature 1,3-butadiene hydrogenation over biosynthesized Pd/γ-Al2O3 catalysts annealed under different atmospheres (H2 and air) was compared in a fixed bed reactor, and the catalysts were prepared using a facile sol-immobilization method. The structural properties of the Pd/γ-Al2O3 catalysts in relation to their activities in 1,3-butadiene hydrogenation were investigated by X-ray photoelectron spectroscopy, X-ray diffraction, hydrogen temperature-programmed reduction, thermogravimetry, transmission electron microscopy, CO chemisorption measurement techniques and Fourier transform infrared spectroscopy. The results of characterization revealed that the calcination atmosphere (H2 and air) exhibited a remarkable impact on the chemical state of Pd species and catalytic activity, and the coexistence of the metallic state and oxidation state of Pd was a key factor for higher catalytic activity and butene selectivity, while the catalyst with the existence of the metallic state only (H2–Pd/γ-Al2O3) showed lower butene selectivity, and the catalyst with the oxidation state alone (air–Pd/γ-Al2O3) hardly showed any activity in 1,3-butadiene hydrogenation. Therefore, the chemical state of Pd played an important role in the 1,3-butadiene hydrogenation reaction.
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Nanoscale Research Letters
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2017
·Vol. 12
·期 1
·1-8
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IF 2.833
Zhang Jingyi,Feng Anni,Bai Jie,Tan Zhibing,Shao Wenyao,Yang Yang,Hong Wenjing,Xiao Zongyuan
The synergetic effect of alloy and morphology of nanocatalysts play critical roles towards ethanol electrooxidation. In this work, we developed a novel electrocatalyst fabricated by one-pot synthesis of hierarchical flower-like palladium (Pd)-copper (Cu) alloy nanocatalysts supported on reduced graphene oxide (Pd-Cu (F) /RGO) for direct ethanol fuel cells. The structures of the catalysts were characterized by using scanning electron microscopy (SEM), transmission electron microscope (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectrometer (XPS). The as-synthesized Pd-Cu (F) /RGO nanocatalyst was found to exhibit higher electrocatalytic performances towards ethanol electrooxidation reaction in alkaline medium in contrast with RGO-supported Pd nanocatalyst and commercial Pd black catalyst in alkaline electrolyte, which could be attributed to the formation of alloy and the morphology of nanoparticles. The high performance of nanocatalyst reveals the great potential of the structure design of the supporting materials for the future fabrication of nanocatalysts.
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JOURNAL OF THE AMERICAN OIL CHEMISTS SOCIETY
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2017
·Vol. 94
·期 12
·1481-1489
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IF 1.421
Senan Ahmed M.,Zhang Sicheng,Qin Shuhao,Chen Zhuqi,Yin Guochuan
With the rapid depletion of fossil resources, the exploitation of biomass to partly replace fossil resources as the source of carbon in the chemical industry constitutes a promising alternative for the near future. This work introduces catalytic transformation of vegetable oil, i.e., methyl linoleate, to its conjugated esters by a simple Pd(OAc) 2 /Sc(OTf) 3 catalyst, which has extensive applications in industry. It was found that adding non-redox metal ions like Sc(III) to a simple Pd(OAc) 2 catalyst can effectively improve its isomerization activity in toluene/ t -BuOH solvent, whereas Pd(OAc) 2 alone is inactive. Preliminary mechanistic investigations together with previous studies suggested that the in situ-generated heterobimetallic Pd(II)/Sc(III) dimer serves as the key species for methyl linoleate isomerization, and the reaction proceeds by [1,3]-hydrogen shift mechanism involving a formal Pd(II)/Pd(IV) cycle.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Keming Zhang,Xiaohe Tian,Zhe Xu,Haishan Huan,Rui Zhang,Xiaoting Feng,Qingnan Wang,Yanting Tang,Chenlu Liu,Shaofei Wang
Membrane-based gas separation offers notable energy efficiency benefits for hydrogen purification, yet it is often hindered by the inherent trade-off between permeability and selectivity. To address this challenge, a novel mixed matrix membrane (MMM) design is presented to boost H 2 separation performance via continuous hydrogen spillover mechanisms for the first time. The MMM incorporates a palladium-functionalized ZIF-67 gel (Pd@ZIF-67 gel) network into a polymer of intrinsic microporosity (PIM-1) matrix. The ZIF-67 gel network serves as a uniform dispersion medium for palladium nanoparticles (Pd NPs), thereby generating a multitude of active sites. These exposed sites, in conjunction with the microporous structure of ZIF-67, facilitate hydrogen dissociation and establish a continuous hydrogen spillover pathway throughout the membrane. This synergistic MMM design leads to substantial improvements in both hydrogen transport and selectivity. At an optimal loading of 28 wt% Pd@ZIF-67 gel, the MMMs exhibit a H 2 permeability of 3620 Barrer and a remarkable 417% enhancement in H 2 /CH 4 selectivity (24.9), surpassing the 2008 upper bound. This approach paves the way for the development of advanced materials tailored for gas separation applications.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2015
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IF 3.313
Yan Yang,Wei Wang,Fengxia Wang,Yanqin Liu,Dan Chai,Ziqiang Lei
In this study, a novel Pd-(NiFe) x -(NiFeO) y /C catalyst is fabricated by supporting Pd on partially oxidized nickel–iron alloy. Because of the promotion effect between nickel–iron alloy and nickel–iron oxide towards Pd, the catalyst exhibits excellent electrocatalytic performance for ethylene glycol oxidation . Specifically, it has much larger electrochemically active surface area, better electrocatalytic activity and durability compared to Pd/C counterpart. After all, this strategy is well suited to synthesize other metal alloys and oxides synergistically promoting Pd electrocatalysts for direct ethylene glycol fuel cells.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2017
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IF 2.843
Chuang Li,Guangyue Xu,Xiaohao Liu,Ying Zhang,Yao Fu
Tetrahydrofurfuryl alcohol (THFAL), as a green industrial solvent, can be obtained directly from biomass-derived furfural with 100% conversion and 100% yield over a hydroxyapatite-supported Pd catalyst (Pd-HAP) under relatively mild conditions (40 °C, 1 MPa H2, and 3 h) in 2-propanol. At room temperature and reacting for 8 h, the yield of THFAL was more than 99%. By capturing the intermediates, two pathways were proposed as follows: (1) Furfural was partially hydrogenated to furfuryl alcohol, and then, furfuryl alcohol was further hydrogenated to THFAL. (2) Furfural and 2-propanol first formed 2-(isopropoxymethyl)furan (2-IPMF) via etherification, and then, 2-IPMF was ultimately converted to THFAL. The Pd-HAP catalyst was characterized by various techniques including XRD, SEM, TEM, HAADF-STEM, XPS, and ICP-AAS. The results revealed that the outstanding catalytic performance of Pd-HAP was attributed to the quasicoordination effect between Pd and HAP, which not only contributed to highly dispersed and stable Pd nanoclusters but also led to better activation of hydrogen. The recyclability of the Pd-HAP catalyst was also investigated and proved its stability in the conversion of furfural and high selectivity toward THFAL.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2016
·Vol. 30
·期 8
·680-683
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IF 2.452
Lulu Wang,Minxin Yang,Xiaochong Liu,He Song,Lu Han,Wenyi Chu,Zhizhong Sun
A bidentate-chelation assistant palladium-catalyzed direct C-H cyanation of picolinamides with TMSCN is described. The reaction of various derivatives gave the corresponding cyanated products in moderate to good yields under mild conditions. In addition, the cyanated product could transform into some valuable functional groups in good yields. Copyright © 2016 John Wiley & Sons, Ltd.
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PLoS One
·
2017
·Vol. 12
·期 3
·e0174589
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IF 2.806
Guofu Huang,Mianmian Wang,Yongyou Hu,Sihao Lv,Changfang Li
In this study, two kinds of cellulose derivatives (polyanionic cellulose (PAC) and hydroxypropylmethyl cellulose (HPMC)) were selected as stabilizers of Pd/Fe nanoparticles (NPs) to investigate their influences on the debromination performances of 2,2',4,4'-tretrabromodiphenyl ether (BDE47). Field emission scanning electron microscope (FE-SEM) images revealed that the cellulose-stabilized Pd/Fe NPs were smaller and more uniform than the bare-Pd/Fe NPs. X-ray diffractometer (XRD) and X-ray photoelectron spectroscopy (XPS) results suggested that cellulose coatings found on Pd/Fe NPs surfaces featured some antioxidation abilities, which followed the order of HPMC < PAC. Sedimentation tests demonstrated that the stabilizing power of PAC for Pd/Fe NPs was higher than that of HPMC. Fourier transfer infrared spectrometer (FTIR) results indicated that PAC molecules were bound to the Pd/Fe NPs surfaces by polar covalent bonds and hydrogen bonds, while HPMC molecules interacted with the nanoparticles by hydrogen bonds. Batch debromination test for BDE47 demonstrated that the catalytic debromination rate with cellulose-stabilized Pd/Fe NPs was higher than that with bare-Pd/Fe NPs during reaction period of 15 min. Overall, this study indicated that both celluloses are beneficial to forming smaller, more regular, stable and antioxidative Pd/Fe NPs, leading to higher debromination reactivity for BDE47 compared with the bare-Pd/Fe NPs. Therefore Pd/Fe NPs can be utilized as a promising remediation technology for the contaminated groundwater and soils.
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RSC Advances
·
2016
·Vol. 6
·期 74
·70424-70432
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IF 3.289
Ran Ji,Shangru Zhai,Wei Zheng,Zuoyi Xiao,Qingda An,Feng Zhang
Towards the aerobic oxidation of alcohols, palladium nanoparticle immobilized mesoporous catalysts have been extensively investigated; however, the preparation of efficient catalytic materials without using complexing moieties remains a challenge. Herein, a simple yet effective concept that directly utilizes inorganic ZrSBA-15, a mild acidic framework, as a supporting matrix for Pd NPs was applied. The catalysts were fully characterized using X-ray diffraction, N2 adsorption–desorption isotherms, Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy and transmission electron microscopy. It was demonstrated that, on the basis of these characterization results, active Pd NPs had been successfully loaded onto the porous framework of ordered ZrSBA-15. More significantly, the method of preparation was also attributed to the catalytic properties of the resultant sample, in which the interactions between Pd species and acidic framework were improved, leading to a uniform dispersion and enhanced stabilization of Pd particles. Meanwhile, Pd/ZrSBA-15 catalysts exhibited expected activity in the aerobic oxidation of benzyl alcohol with at least 95% conversion and 99% selectivity for benzaldehyde. Moreover, the oxidation reaction could be performed smoothly under solvent- and base-free conditions, and the catalyst was recycled several times with negligible loss in selectivity and conversion.
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