ChemElectroChem
·
2018
·Vol. 5
·期 24
·3901-3905
·
IF 4.446
Wen-Tao Kuang,Ze-Li Jiang,Hui Li,Jing-Xuan Zhang,Lin-Nan Zhou,Yong-Jun Li
Graphical Bond breaking and bond making : Au/Pd 63 Pt 37 nanowires are prepared in a one-pot, two-step synthesis. The tri-metallic nanowires are an excellent bi-functional catalyst, capable of electrochemically catalyzing ethanol oxidation (C−C bond breaking) to output electric energy and chemically catalyzing Suzuki coupling (C−C bond formation) to produce new materials. Tri-metallic nanowire catalysts combine the synergistic effect of multiple metals with the geometrical effect of nanowires, exhibiting better catalytic performance than composition-equivalent nanospherical catalysts. However, tri-metallic nanowires are not easily produced directly because of the participation of multiple precursors and the difficulty of selecting capping agents. Herein, we develop a one-pot, two-step synthetic strategy, producing tri-metallic Au/PdPt core/shell nanowires. Moreover, the PdPt shell is an alloy composed of nanoparticles, and its Pd : Pt atomic ratio is easily adjusted by controlling reaction time. The formation of Au/PdPt nanowires is attributed to the initial formation of Au/Pd core/shell nanowire and subsequent galvanic replacement between Pd shell and PtCl 6 2− . As-prepared Au/PdPt nanowires show composition- and structure-dependent catalytic activity and durability for the electrooxidation of methanol and ethanol, and the Suzuki coupling reaction. Optimized Au/Pd 63 Pt 37 nanowire, due to its proper Pd : Pt atomic ratio and porosity of the PdPt shell, exhibits excellent catalytic activity and durability towards methanol and ethanol electrooxidation, ∼18 and 11 times in the specific activity better than that of commercial state-of-the-art Pt/C catalyst, respectively. Moreover, Au/Pd 63 Pt 37 nanowire shows the superior catalytic performance in Suzuki coupling reaction, ∼96 % at yield, far better than commercial state-of-the-art Pd/C catalyst.
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Molecular Catalysis
·
2019
·
IF 2.938
Xinli Tong,Zhenya Zhang,Yiqi Gao,Yue Zhang,Linhao Yu,Yongdan Li
A novel carbon-chain increasing valorization of furfural (FUR), a cheap bio-based platform compound, has been successfully performed via the catalytic oxidative condensation process with mono-dispersed palladium oxide catalyst. For the reaction of furfural, n-propanol and O 2 , the PdO@TiO 2 exhibited a prominent catalytic activity in which a 77.8% conversion of FUR with 89.2% selectivity of 3-(furan-2-yl)-2-methylacrylaldehyde was obtained. Based on the XRD, SEM, TEM, HRTEM, XPS, and UV–vis results of catalysts, it was concluded that high activity is associated with particle size, uniform distribution of palladium oxide and surface area of the support. Moreover, the recycling experiments confirmed that mono-dispersed palladium oxide catalyst was stable, in which it still kept a good catalytic performance after being recycled for five times. This provided a new route for the selective transformation of the hemicellulose-derived platform compounds.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2019
·
IF 3.131
Rui Sun,Fangfang Ren,Dong Wang,Yufeng Yao,Zhenghao Fei,Huiwen Wang,Zongtang Liu,Rong Xing,Yukou Du
Design of high performance and low cost electrocatalysts for the oxidation of small organic molecules remains a great challenge for the practical application of direct fuel cells. Herein, a novel composite catalyst composed of PdAu nanoparticles (NPs) uniformly dispersed on the polydopamine functionalized MWCNTs (PDA-MWCNTs) has been synthesized. TEM images indicate that MWCNTs are successfully coated by PDA, and the as-prepared PdAu NPs are homogeneously dispersed on the PDA functional MWCNTs with smaller sizes than those on pristine MWCNTs. Electrochemical tests reveal that PDA-MWCNTs is a promising catalyst carrier for direct ethylene glycol fuel cell (DEGFC), and the PdAu(1:1)/PDA-MWCNTs catalyst displays the highest peak current density among all catalysts towards ethylene glycol oxidation reaction (EGOR) in alkaline medium, with mass activity of 1540.3 mA mg Pd −1 , which is 1.5, 2.6, 9.8, 13.4 and 2.0 times greater than those of PdAu(1:3)/PDA-MWCNTs, PdAu(3:1)/PDA-MWCNTs, Pd/PDA-MWCNTs, Pd/MWCNTs and commercial Pd/C catalysts, respectively. In addition, PdAu(1:1)/PDA-MWCNTs catalyst also exhibits the best stability. These findings are valuable for the development of advanced Pd-based catalysts, which will help promote the industrialization of direct fuel cell.
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BIORESOURCE TECHNOLOGY
·
2019
·
IF 6.669
Da Wang,Guangci Li,Chuanhui Zhang,Zhong Wang,Xuebing Li
Ni nanoparticles inlaid in lignin-derived carbon constructing the “inlaid type” Ni/C-I was reported to improve stability and adjust metal-support interaction of lignin hydrogenolysis catalyst. The Ni/C-I was further heat treated in air to prepare Ni/C-R so as to re-expose the blocked active sites by carbon species. A lot of characterization techniques were carried out to confirm the “inlaid structure” of the catalysts. The lignin depolymerization results demonstrated that the Ni/C-R had better catalytic performance than traditional “supported type” Ni/C, 23.3% aromatic monomer yield and 82.4% bio-oil yield were achieved. Moreover, the mechanism studies with lignin model compound revealed that Ni/C-R had better bond breaking ability than Ni/C, even C C bond could be cleaved. The electron effect could be responsible for that, since the electrons could transfer from Ni 0 to carbon support for Ni/C-R, which could improve the bond breaking ability.
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高影响因子
JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Juan Du,Jiaren Zhang,Yong Sun,Wenlong Jia,Zhihao Si,He Gao,Xing Tang,Xianhai Zeng,Tingzhou Lei,Shijie Liu,Lu Lin
Catalytic transfer hydrogenation (CTH) of bio-derived furfural (FF) to furfuryl alcohol (FFA) was performed using the physically mixed CuO-Pd/C as catalyst and formic acid (FA) as hydrogen donor. The evolution investigation of Cu showed the precursor CuO firstly dissolved into Cu 2+ by FA and then formed coordination polymer-copper(II), which uniformly dispersed in reaction solution of 1, 4-dioxane. Subsequently the Cu 2+ was in-situ reduced and Cu-Pd alloys formed simultaneously. The in-situ prepared nano Cu-Pd/C catalyst exhibited the best performance with a complete FF conversion and FFA selectivity of 98.1%. Reaction conditions test suggested that the FFA selectivity was greatly dependent on the Cu content. The underlying mechanism revealed that the Pd in Cu-Pd alloys mainly promoted the FF conversion by enhancing hydrogen adsorption, while the nano Cu for increasing FFA selectivity; the Cu-Pd alloys functioned in synergistic way. Leaching and recycling tests demonstrated an excellent stability of the Cu-Pd/C catalyst.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2018
·
IF 3.235
Yan Zhang,Lingqian Kong,Hongmei Du,Jinsheng Zhao,Yu Xie
Three novel donor-accept type electrochromic polymers with very low band gap, namely PMFTTP, PMFBTTP and PMFMOTTP, were prepared via electrochemical polymerization , employing 2,3-bis(5-methylfuran-2-yl)thieno[3,4- b ]pyrazine as the acceptor units and thiophene , butylthiophen and methoxythiophen as the donor units, respectively. All the polymers were comparatively studied by cyclic voltammetry (CV), scanning electron micrographs (SEM), UV–vis-NIR spectroscopy and colorimetry . The results revealed that PMFTTP and PMFBTTP showed obvious color change from green color to brown in the oxidation process , while PMFMOTTP exhibited color change from brick red to dark gray. And the three polymers possessed very low optical band gaps in the following order: PMFTTP (1.23 eV) > PMFBTTP (0.88 eV) > PMFMOTTP (0.74 eV), which demonstrated the different election-donating ability of thiophene or its derivatives. The electrochromic kinetic investigations manifested that the polymers presented satisfactory optical contrasts (ΔT%) in the near infrared region (NIR), which were 35%, 67% and 60% for PMFTTP, PMFBTTP and PMFMOTTP, respectively. Moreover, the polymers also displayed short switching times (lower than 1 s at any wavelengths), high coloration efficiencies (around about 200 cm 2 /C) and outstanding robust stabilities, suggesting the probability of being the promising candidates for the electrochromic devices. In summary, the above positive results, especially the neutral green color and the very low band gap, had important theoretical significance for the application and development of electrochromic polymers.
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ACS Applied Bio Materials
·
2018
·
IF 0
Lantao Liu,Nan Li,Meijun Chen,Hailin Yang,Qian Tang,Chengbin Gong
The phototoxicity of UV light limits the application of conventional azobenzene-based photoresponsive molecularly imprinted polymers in the biomedical field. This paper reports a tetra-ortho-methoxy-substituted azobenzene, N-(4-((4-amino-2,6-dimethoxyphenyl)diazenyl)-3,5-dimethoxyphenyl)methacrylamide (ADDDM), whose photoswitching is induced by all visible-light irradiation (440 nm for trans form to cis form and 630 nm for cis form to trans form) in N,N-dimethylformamide and tetrahydrofuran (1:9, v/v). Using ADDDM as the monomer, a visible-light-responsive surface molecularly imprinted polymer (VSMIP) on silica microspheres was fabricated for acyclovir (ACV). VSMIP showed a higher drug loading capacity, better specificity, faster drug release rate, and faster photoisomerization rate constant to ACV than the corresponding visible-light-responsive surface molecularly nonimprinted polymer (VSNIP). The selectivity of VSMIP to ACV and competing materials (ganciclovir and triacetylganciclovir) was examined by ultraviolet–visible spectroscopy, and the VSMIP showed excellent specificity of recognition toward ACV. The VSMIP can realize a visible-light-triggered (440/630 nm) release and uptake of ACV through chicken skin tissue (1 mm in thickness).
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DRUG METABOLISM AND DISPOSITION
·
2018
·Vol. 46
·期 4
·442-450
·
IF 3.64
Huimin Zhao,Siyuan Li,Zixin Yang,Ying Peng,Xiaohui Chen,Jiang Zheng
Erlotinib (ELT), a tyrosine kinase inhibitor, is widely used for the treatment of nonsmall cell lung cancer in clinic. Unfortunately, severe drug-induced liver injury and other adverse effects occurred during the treatment. Meanwhile, ELT has been reported to be a mechanism-based inactivator of cytochrome P450(CYPs) 3A4 and 3A5. The objectives of this study were to identify ketene intermediate of ELT and investigate the association of the acetylenic bioactivation with the enzyme inactivation caused by ELT. A ketene intermediate was detected in human microsomal incubations of ELT, using 4-bromobenzylamine as a trapping agent. CYPs 3A4 and 3A5 mainly contributed to the bioactivation of ELT. Microsomal incubation study showed that the ketene intermediate covalently modified the enzyme protein at lysine residues and destroyed the structure of heme. The vinyl and ethyl analogs of ELT showed minor enzyme inhibitory effect (less than 20%), whereas ELT inactivated more than 60% of the enzyme. The present study provided a novel bioactivation pathway of ELT and facilitated the understanding of the mechanisms of ELT-induced mechanism-based enzyme inactivation and liver injury.
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高影响因子
EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
·
2018
·
IF 4.816
Liangfeng Huang,Gaofei Wei,Xiaoqi Sun,Yali Jiang,Zeqian Huang,Yanjuan Huang,Yifeng Shen,Xiaoyu Xu,Yunhui Liao,Chunshun Zhao
Therapeutic effects of photodynamic therapy (PDT) are limited by the selectivity of photosensitizer (PS). Herein, a novel tumor-targeted drug-PS conjugate (Gan-ZnPc) which integrated with zinc phthalocyanine (ZnPc) and Ganetespib has been developed. ZnPc is a promising PS with remarkable photosensitization ability. Ganetespib is a heat shock protein 90 (Hsp90) inhibitor with preferential tumor selectivity and conjugated to ZnPc as a tumor-targeted ligand. The multifunctional small molecule conjugate, Gan-ZnPc, could be bound to extracellular Hsp90 and then selectively internalized into the tumor cells, followed by the generation of abundant intracellular reactive oxygen species (ROS) upon irradiation. Besides, Gan-ZnPc can arrest cell proliferation and induce apoptosis by the inhibition of Hsp90. Herein, with combination of the inhibition of Hsp90 and the generation of cytotoxic ROS, Gan-ZnPc implements tumor selectivity, concentrated PDT and chemotherapy in a synergistic manner, which results in highly effective anti-tumor activity in vitro and in vivo.
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RSC Advances
·
2015
·Vol. 5
·期 50
·40227-40235
·
IF 3.84
Fangyuan Yi,Fugui Xu,Yong Gao,Huaming Li,Daoyong Chen
In this study, the preparation of styrene/divinylbenzene-based macrocellular polymers of high internal phase emulsions (polyHIPEs) with interconnected open-cell structure as well as their application as support for Pd nanoparticles are presented. Firstly, water in oil high internal phase emulsions (HIPEs) were generated by adding the water stepwise to the oil phase (styrene and divinylbenzene) containing Janus polymer nanoparticles that consist of a linear poly(methyl methacrylate) “tail” and a cross-linked poly(4-vinylpyridine) “head”. The generated water in oil HIPEs stabilized solely by Janus polymer nanoparticles were then converted to polyHIPEs foams by polymerizing the external continuous oil phase, followed by the extraction with methanol and the drying under the reduced press. Scanning electron microscopy observation revealed that the as-produced macrocellular polyHIPEs were foam structure with closed and/or partially open-cells. Partial cells covered by a thin polymer film were peeled off during the post-treatment. Some key factors influencing the polyHIPEs morphologies, including emulsifier particles content, the mole ratio of styrene to divinylbenzene and the internal phase volume fraction were investigated, and macrocellular polyHIPEs with interconnected open-cell morphologies could be achieved under optimal conditions. Benefited from the strong interaction between the emulsifier particles embedded in the polyHIPEs and H2PdCl4 precursor, Pd nanoparticles were facilely supported in situ within the macrocellular polyHIPEs without any functional monomers or post-functionalization requirement. The obtained Pd@macrocellular polymer hybrid foams were then applied for the heterogeneous Suzuki–Miyaura carbon–carbon coupling reactions between iodobenzene and benzeneboronic acid, and a high catalytic activity with a good recyclability were demonstrated.
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APPLIED ENERGY
·
2014
·
IF 5.261
Jinxing Long,Ying Xu,Tiejun Wang,Zhengqiu Yuan,Riyang Shu,Qi Zhang,Longlong Ma
Serious char formation caused by the repolymerization of unsaturated decomposition products is a considerable challenge for current lignin utilization. Here, a novel and efficient base-catalyzed depolymerization and in situ hydrogenolysis process for lignin decomposition and char elimination was proposed using the synergic catalyst of NaOH coordinated with Ru/C. In which, lignin was first depolymerized to phenolic monomer and its oligomer, and then the oligomer was further converted to more stable aliphatic alcohols simultaneously. The results showed that more than 92.5% of lignin was converted, giving 12.69% phenolic monomer, 6.12% aliphatic alcohol and less than 14.03% residual solid. This residual solid selectivity was far lower than it from the single catalyst condition. Furthermore, the products were analyzed using GC–MS, GPC, HPLC–MS and 1 H NMR. The synergistic effect between depolymerization and hydrogenolysis was also investigated through comparative analysis of the feedstock, products, and the recovered lignin.
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RSC Advances
·
2014
·Vol. 4
·期 108
·63048-63054
·
IF 3.708
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.
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