INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Guangyue Xu,Chuang Li,Tianyu Deng,Chenguang Wang,Ying Zhang,Yao Fu
The conversion of levulinic acid (LA) to γ-valerolactone (GVL) is one of the most important reactions from biomass-derived platform chemicals to value-added chemicals. In this work, bimetallic PdRu/TiO2 catalyst compared to monometallic Ru/TiO2 was designed for the conversion of LA to GVL at ambient H2 pressure. The highly dispersed Pd affected the reaction by two antagonistic effects: (I) increasing the reaction rate by promoting the activation of H2; (II) decreasing the reaction rate by lowering the activation ability of carbonyl group over Ru. The kinetic analysis refined by H2 concentration showed much lower apparent activation energy over 0.2Pd1Ru/TiO2 than that over Ru/TiO2. Finally, the catalysts were evaluated by both GVL productivity and catalyst cost to show increasing benefit of Pd addition at lower H2 pressure. This study offers both theoretical foundation and application instructions for high efficiency conversion of LA to GVL under mild conditions, especially ambient H2 pressure.
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Science Advances
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2020
·Vol. 6
·期 6
·
IF 13.117
Zecong Xiao,Zhenwei Su,Shisong Han,Jinsheng Huang,Liteng Lin,Xintao Shuai
The response to programmed cell death protein-1 (PD-1)/programmed death ligand-1 (PD-L1) blockade in cancer immunotherapy is limited because of multiple immune evasion mechanisms. Here, a previously unknown strategy is proposed to synergize the nuclear factor κB (NF-κB) inhibition and PD-1 blockade for antitumor immunotherapy. A dual pH-sensitive nanocarrier loading curcumin (CUR) and anti–PD-1 monoclonal antibody (aPD-1) may bind to circulating PD-1+ T cells and then follow their infiltration into the tumor. Furthermore, the nanodrug bound to PD-1+ T cells may be released in the tumor microenvironment, leaving aPD-1 to block PD-1 on T cells and generating a CUR-encapsulated cationic nanodrug that can be easily taken up by tumor cells/tumor associated macrophages (TAMs). Thus, not only the antitumor T cells mediate efficient CUR delivery to tumor but also the efficient CUR delivery promotes the tumor infiltration of antitumor T cells, thereby resulting in effective activation of antitumor immunity.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Ze Yin,Minguang Han,Zhao Hu,Li Feng,Yongze Liu,Ziwen Du,Liqiu Zhang
For efficient usage of visible light, Pd loading graphitic carbon nitride (Pd/g-C 3 N 4 ) hybrids were synthesized and peroxymonosulfate (PMS) was accompanied to improve the photoactivities of Pd/g-C 3 N 4 . The photocatalytic system consisting of Pd/g-C 3 N 4 , PMS and visible light (Pd/g-C 3 N 4 -PMS-Vis) exhibited higher bezafibrate (BZF) removal efficiency than Pd/g-C 3 N 4 -PMS, Pd/g-C 3 N 4 -Vis, g-C 3 N 4 -PMS, g-C 3 N 4 -Vis, and g-C 3 N 4 -PMS-Vis systems, which can be ascribed to the electron transfer from Pd/g-C 3 N 4 to PMS. Density functional theory (DFT) calculation proved that the chemical bond interaction forming between Pd and g-C 3 N 4 inspired the electron excitation, separation and transportation. Meanwhile, Pd particles with local surface plasma resonance (LSPR) phenomenon could also enhance the visible light adsorption. Notably, the photocurrent response of Pd/g-C 3 N 4 was significantly improved with PMS, demonstrating the photoinduced electrons on Pd/g-C 3 N 4 are capable to immigrate to PMS. The added PMS can perform as electron acceptors, thus favoring the quantum efficiency of photoinduced charge carriers to form SO 4 − . The BZF degradation mechanism was clarified by the addition of different scavengers and the major reaction active species were hydroxyl radicals (OH ) and sulfate radical (SO 4 − ). Four possible pathways in the degradation of BZF were also put forward via LC-MS/MS analysis (R-oxy substituent, oxidation dichlorination, OH-addition and oxidation deaminization). In the 2%Pd/g-C 3 N 4 -PMS-Vis system, an obvious decrease of genetic toxicity was observed because of the high removal efficiency and final low concentration of BZF. The results of this research underlined great prospective of Pd/g-C 3 N 4 catalysts and provided a potential approach to photocatalytically remedy the polluted water by micropollutants.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Min Shao,Muhan Chen,Mei Fan,Guoting Luo,Ci Jin,Zhangjie Huang
In this study, based on a cyano-functionalized ionic liquid, 1-nitrile-1-octylpyrrole bromide ([C 8 Y 3 Pr]Br), a [C 8 Y 3 Pr]Br/cyclohexane/tributyl phosphate (TBP)/NaCl microemulsion system was constructed and used for the extraction of Pd(II) and preparation of Pd nanoparticles from multimetal solutions. The key extraction parameters including vibration time, [C 8 Y 3 Pr]Br concentration, phase ratio ( R W/O ), and HCl concentration were evaluated. Compared with other ionic-liquid microemulsion systems, the cyano-functionalized ionic liquid [C 8 Y 3 Pr]Br microemulsion system showed excellent extraction performance for Pd(II). Almost all Pd(II) was extracted (>98.0%) from a multimetal solution using the microemulsion system, while the separation factors ( β Pd/M ) of [C 8 Y 3 Pr]Br-based microemulsions for Pd(II) with Cu 2+ , Fe 3+ , Ni 2+ , Zn 2+ , Co 2+ , and Mg 2+ exceeded 1.0 × 10 3 . The mechanism extracting Pd(II) using [C 8 Y 3 Pr]Br was confirmed to be an anion-exchange reaction via Job’s method, spectral analysis (UV, FTIR), and DFT calculations. Alcohols and hydrazine hydrate were used as demulsifiers, and Pd nanoparticles were directly obtained from the microemulsion phase. The Pd nanoparticles were identified by TEM, XPS, and XRD analyses. The chemical structures of extracted species based on the microemulsion system and the mechanism of demulsification of alcohols were studied. Thus, an effective new process was developed in this study for the direct preparation of Pd nanoparticles from mixed metal solutions via solvent extraction.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
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IF 5.816
Bin Qu,Ye Tao,Lan Yang,Yihui Liu
Transition metal phosphide based orange-like Pd@Co@P nanoparticles supported on reduced graphene oxide (Pd@Co@P/rGO) have been synthesized by a one-pot co-reduction at room temperature using methylamine borane (MeAB) as the reducing agent. The prepared Pd@Co@P/rGO nanoparticles were characterized by powder X-ray diffraction (XRD), transmission electron microscope (TEM), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FT-IR), selected area electron diffraction (SAED) and confocal Raman microscopy (Raman). Compared with Pd/rGO and Pd@Co/rGO, the Pd@Co@P/rGO catalyst has higher catalytic activity for the hydrolytic production of ammonia borane (AB) with the turnover frequency value (TOF) of 127.57 min −1 and the activation energy of 39.05 kJ mol −1 . This excellent catalytic performance may be caused by the orange-like structure and good dispersion of Pd@Co@P/rGO nanoparticles, and the synergistic electron interactions between palladium , cobalt, and phosphorus.
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APPLIED CATALYSIS A-GENERAL
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2021
·
IF 5.706
Jiaorong Yan,Li Wang,Yun Guo,Yanglong Guo,Qiguang Dai,Wangcheng Zhan
Cobalt-doped alumina nanosheets were prepared by dynamic hydrothermal method, and then the precious metal Ru or Pd was loaded and investigated for catalytic combustion of propane. Cobalt doping imparted the prominent redox ability to irreducible alumina nanosheets with superior thermal stability and established the strong metal-support interaction and easy activation of gaseous oxygen. Comparative investigation between Ru and Pd supported on Co-doped Al 2 O 3 nanosheets suggested that Ru based catalysts presented a higher activity and water-resistance while the preferable sintering-resistance and oxygen-tolerance were observed on Pd based catalysts. Unexpectedly, the Pd/CoANS-800 catalysts exhibited a re-dispersion of PdO x at high temperature and re-activation for propane oxidation . Ru based catalysts were more tolerant to Cl species from the metal precursor, and the presence of H 2 O could accelerate the removal of the residual Cl species from the catalyst surface especially Pd based catalysts, which led to the promotion of catalytic activity.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Jingjing Zhu,Huaqiang Chen,Lan Wang,Engang Fu,Jianping Wu,Qilei Zhang,Lirong Yang,Gang Xu
A composite hollow mesoporous MIL-101@Pd@ZIF-8-30min (HM-MIL@Pd@ZIF-30min) nanocatalyst with hollow core and stable shell was developed in this study. Hollow mesoporous MIL-101(HM-MIL) was hydrothermally synthesized and employed as the supports of Pd nanoparticles by adopting a facile HM-MIL-template strategy to make ZIF-8 crystals uniformly overgrew on HM-MIL-101@Pd microcrystal cores. The obtained core-shell catalyst possessed hollow mesoporous structure, and the shell layer of ZIF-8 had additional advantages of abundant Lewis basic sites for heterogeneous racemization reaction. Compared with unmodified HM-MIL@Pd and solid MIL-101(Cr)@Pd@ZIF-8 (S-MIL@Pd@ZIF-8), HM-MIL@Pd@ZIF-8-30min had higher racemic chemical activity (conv. 99%) and selectivity (sel. R-amide 94%) in one-pot dynamic kinetic resolution (DKR) reaction system of rac -1-phenethylamine. The catalyst showed excellent stability, and the conversion and selectivity reached 95% and 93% respectively after ten catalytic cycles.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2019
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IF 5.589
Zeyu Wang,Cong Chen,Huan Liu,Dzmitry Hrynshpan,Tatsiana Savitskaya,Jianmeng Chen,Jun Chen
The microbial reduction of nitrate in the presence of nanoscale zero-valent iron (nZVI) was evaluated to assess the feasibility of employing nZVI for biological denitrification treatment. The effect of modified nZVI on the growth, metabolism, and denitrification performance of Alcaligenes sp. TB under aerobic conditions was studied. Results showed that Alcaligenes sp. TB with nZVI/Pd had 31.5% increase in nitrate removal and 18.1% decrease in nitrite accumulation within 28 h. nZVI/Pd exhibited less inhibition on the cell growth (OD 600 = 0.725), NADH/NAD + ratio (86% of control), and electron transfer system activity (68.5% of control). In addition, nZVI/Pd decreased the membrane fluidity by increasing the trans/cis isomerization ratio (317.7% of control) to enhance the resistance of nZVI. This study underlines the effects of nZVI/Pd on membrane susceptibility via membrane fatty acid transformation during denitrification and suggests the influence of engineered nanomaterials on denitrification.
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PubMed
高影响因子
Nanomaterials
·
2019
·Vol. 9
·期 12
·1698
·
IF 4.034
Yanliang Yang,Dongsheng Deng,Dong Sui,Yanfu Xie,Dongmi Li,Ying Duan
The hydrogenation of furan ring in the biomass-derived furans is of great importance for the conversion of biomass to valuable chemicals. Fabrication of high activity and selectivity catalyst for this hydrogenation under mild conditions was one of the focuses of this research. In this manuscript, UiO-66-v, in which vinyl bonded to the benzene ring, was first prepared. Then, the uniformly distributed vinyl was used as the reductant for the preparation of Pd/UiO-66-v. The catalyst was characterized by X-ray diffraction, thermogravimetric, N2physical adsorption/desorption, X-ray photoelectron spectroscopy, scanning electron microscope, transmission electron microscopy, energy dispersive spectrometer elemental mappings, and inductively coupled plasma atomic emission spectroscopy to find the Pd/UiO-66-v had a narrow palladium nanoparticles size of 3–5 nm and maintained the structure and thermal stability of UiO-66-v. The Pd/UiO-66-v was used for the hydrogenation of furfuryl alcohol to tetrahydrofurfuryl alcohol in water. 99% conversion of furfuryl alcohol was obtained with 90% selectivity to tetrahydrofurfuryl alcohol after reacted at 0.5 MPa H2, 303 K for 12 h. The Pd/UiO-66-v was proved to be effective for the hydrogenation of furan ring in furans and could be used for at least five times.Keywords:furfuryl alcohol;hydrogenation;tetrahydrofurfuryl alcohol;Pd/UiO-66-v;water solvent
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高影响因子
ChemCatChem
·
2019
·Vol. 11
·期 9
·2362-2369
·
IF 4.495
Xue Zhao,Yunfan Fu,Chen Yao,Shuran Xu,Yu Shen,Qiong Ding,Wenjing Liu,Haibo Zhang,Xiaohai Zhou
Graphical A closo case : In situ preparation of ultrafine Pd and Pt nanoparticles on dodecahydro-closo-dodecaborate organic polymers for high efficiency catalytic hydrolytic dehydrogenation of ammonia borane. Using in situ reduction strategy by combining organic frameworks and ultrafine Pd and Pt nanoparticles (Pd−NPs and Pt−NPs) to synthesize composites with tunable morphology and high dispersion has attracted extensive attentions in fabrication of composite nanomaterials. Herein, on the new kind of substrate, BOPs@Pd and BOPs@Pt nano materials have been successfully fabricated via in situ reduction of Na 2 PdCl 4 and H 2 PtCl 6 triggered by reducibility of organic boron polymers (BOPs). The final products are obtained by loading Pd−NPs and Pt−NPs with ultra-small size and high dispersion without any tedious chemical modification or additional additives. These materials show high catalytic activity and recyclability in the hydrolysis dehydrogenation of ammonia borane (AB).
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高影响因子
Small
·
2019
·Vol. 15
·期 14
·1900050
·
IF 10.856
Ting Su,Zhong Lin Wang,Zhiwei Wang
It is demonstrated that the redox reaction behaviors of Pd nanoparticles in HAuCl 4 solutions can be substantially modified by the introduction of hexadecyl trimethyl ammonium bromide (CTAB) agents through systematic liquid cell transmission electron microscopy (LCTEM) investigations. The gradual dissolution of Pd nanoparticles is observed when HAuCl 4 solution is pumped into liquid flow cells, the etching characteristics of which are depended on both HAuCl 4 concentrations and incident electron doses. In comparison, with the presence of CTAB agents, the dominated phenomenon appears to be the precipitation of Au species and incorporation onto the surface of Pd seeds. It is also observed that the rapid growth of Au on Pd seeds occurs by loading Pd and HAuCl 4 solutions into static liquid cells. The resultant Au shells exhibit rather sparse structural configurations and are formed possibly by homogeneous nucleation/coalescence of Au species as well as monomer attachments. The observed Au-shell growth instead of Pd dissolution is attributed to the presence of the residual regents, which may be also responsible for the initially already existing small Au adsorptions at the corner/edge sites of Pd seeds. The study provides a useful reference for the convenient fabrication of complex nanostructures and functional nanomaterials in a controllable way.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Xiang Li,Fuping Dong,Lihua Zhang,Qinqin Xu,Xianyi Zhu,Songmiao Liang,Lijie Hu,Haibo Xie
The design and fabrication of functional hydrogel materials for environmental catalysis is a frontier topic both in fields of material science and catalysis. In this study, a new cellulosic hydrogel anchoring 1,1,3,3-tetramethyl guanidinium–based ionic liquids moiety (CHI) was firstly prepared by simply adding bicyclic anhydrides into newly developed 1,1,3,3-tetramethyl guanidine/DMSO/CO 2 solvent system for cellulose. The presence and amount of bicyclic anhydrides as a cross linker was proved to be an important factor for the hydrogel formation. And then, Pd nanoparticles (NPs)@CHI composites were fabricated by the reduction of the absorbed Pd(II) ions on CHI using NaBH 4 as reducing agent. The samples were characterized by techniques of 1 H NMR, 13 C NMR, FT-IR, SEM, TEM, EDX, XPS, XRD and ICP-OES analysis. It was identified that the CHI presented good immobilization capacity of Pd NPs, and the achieved Pd NPs@CHI composite had high catalytic activity and excellent reusability for the reduction of 4-nitrophenol in water. The activation parameters of the reduction reaction of 4-nitrophenol catalyzed by Pd NPs@CHI using NaBH 4 were calculated as Ea = 10.8 kJ mol −1 , ΔH # = 8.1 kJ mol −1 and ΔS # = −234.8 J mol −1 K −1 .
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