INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Huifang Liu,Jianyu Han,Qitian Huang,Hongwei Shen,Lijun Lei,Zhipeng Huang,Zhixin Zhang,Zongbao K. Zhao,Feng Wang
Catalytic hydrotreating of renewable oils is a promising way to get diesel alkanes, with the use of microbial lipids further facilitating scalable production of green diesel. The core issue of triglyceride hydrodeoxygenation (HDO) research is still to develop efficient catalysts under mild reaction conditions. Herein, we demonstrate that the heteropolyacid (HPA)-modified SiO2 supported Pd catalysts showed high activity for the HDO reaction of methyl stearate and soybean oil to diesel alkanes (C15∼C18, >90 wt % at 200 °C). Characterizations show that the Brønsted acid sites introduced by grafting heteropolyacid on SiO2 and metal sites of small Pd particles contribute to the high HDO activity of this bifunctional catalyst. Additionally, lipids produced by Rhodosporidium toruloides Y4 from glucose or corn stover were also transformed to about 75 wt % of diesel-range alkane products. This integration of microbial lipid production with chemical catalysis should facilitate the engineering of green diesel production from lignocellulosic biomass.
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DOI
高影响因子
ACS Catalysis
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2020
·
IF 12.35
Qiang Deng,Rui Gao,Xiang Li,Jun Wang,Zheling Zeng,Ji-Jun Zou,Shuguang Deng
Upgrading furanic aldehydes (such as furfural or 5-hydroxymethyl furfural) to cyclopentanone compounds (such as cyclopentanone or 3-hydroxymethyl cyclopentanone) is of great significance for the synthesis of high-value chemicals and biomass utilization. Developing an efficient reduced metal/acidic support with Lewis acidity is the key to facilitating the carbonyl hydrogenation and hydrolysis steps in the hydrogenative ring-rearrangement reaction. Herein, three pure Lewis acidic pyrochlore supports of the form A2B2O7 (La2Sn2O7, Y2Sn2O7, and Y2(Sn0.7Ce0.3)2O7-δ) with the same crystal structures and different metals are synthesized. The Lewis acidity and the surface properties of the pyrochlore can be tuned by inserting different kinds of A and B site metals. After impregnation, Pd nanoparticles with appropriate particle sizes are uniformly loaded on the surface of pyrochlore. For the reaction of the furanic aldehydes, all of these pyrochlore-based catalysts exhibit hydrogenation and hydrolysis rates that are both faster than those of traditional support-based catalysts due to the oxygen vacancy and pure Lewis acidity of the support. Among these pyrochlore-based catalysts, Pd/Y2Sn2O7 exhibits activity and selectivity that are higher than those of Pd/La2Sn2O7. Moreover, the Y2Sn2O7-based catalyst partially substituted by Ce3+ ions at the B site is more efficient, with the highest cyclopentanone yield and 3-hydroxymethyl cyclopentanone yield of 95.0% and 92.5%, respectively. Furthermore, the catalyst can still maintain an effective activity and stability after 4 runs. This study not only presents an efficient biobased route for the production of cyclopentanone compounds but also focuses on the acid catalytic performance of pyrochlore based on its pure Lewis acidity.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2018
·Vol. 42
·期 11
·9324-9331
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IF 3.201
Jie Li,Saisai Cheng,Tianxing Du,Ningzhao Shang,Shutao Gao,Cheng Feng,Chun Wang,Zhi Wang
In this work, a porous g-C3N4 nanosheets/reduced graphene oxide (rGO) composite was synthesized via the hydrothermal co-assembly of GO and g-C3N4 nanosheets (g-C3N4 NS). Compared with g-C3N4 NS, rGO and bulk g-C3N4/rGO, the g-C3N4 NS/rGO supported Pd nanocatalyst displayed a remarkable catalytic activity for the hydrogenation of alkenes with formic acid and formates as the hydrogen source at atmospheric pressure. Among all the as-prepared Pd-g-C3N4 NS/rGO catalysts, the optimized Pd-g-C3N4 NS/rGO20 exhibited the highest turnover frequency of 133 mol mol−1 Pd h−1, which is among the highest value reported in documents. 99% conversion and 99% selectivity were achieved after 30 min reaction at 30 °C for the hydrogenation of nitrobenzene. In addition, Pd-g-C3N4 NS/rGO20 exhibited an excellently high stability after five successive cycles without significant loss of its catalytic activity.
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高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 19
·9545-9553
·
IF 11.301
Tianhang Gu,Wei Teng,Nan Bai,Zehan Chen,Jianwei Fan,Wei-xian Zhang,Dongyuan Zhao
Bimetals have attracted considerable attention as electrocatalysts towards selective reduction of nitrate to benign dinitrogen. Design of highly efficient and stable bimetallic catalysts by taking the effects of both active sites increasing and synergistic composition into account is of paramount importance but still a grand challenge. Herein we report novel bimetallic Pd–Cu nanoparticles (NPs) incorporated in porous N-doped carbon octahedra prepared by a spatial confinement strategy of in situ pyrolysis of metal–organic frameworks with the assistance of polyvinyl pyrrolidone (PVP) as electrocatalysts achieving targeted denitrification. Pd–Cu NPs exhibit superior dispersity with a N-doped matrix and are strongly dependent on the variation of PVP, Pd precursor and pyrolysis temperature. The material shows high efficiency (∼97.1%) for the reduction of nitrate from 100 to 2.9 mg NO3−-N L−1 (well below drinking water standards of 10 mg NO3−-N L−1), and especially the selectivity over 83% for benign N2 at neutral pH within 24 h. Encapsulated and well-dispersed Pd–Cu NPs and doped N in the carbonaceous matrix synergistically enhance the interfacial electron transfer for transformation of NO3−-N(V). Porous structures endow the catalyst with outstanding stability after eight cycles and over a wide pH of 4–10. More importantly, the nanocatalyst performs well with real contaminated water (selectivity of 91% for nitrogen) in laboratory batch reactors. This nanocatalyst shows promise in wastewater treatment and environmental remediation due to the spatial confinement strategy and introduction of heterogeneous atoms.
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CATALYSIS LETTERS
·
2021
·Vol. 152
·期 4
·1160-1169
·
IF 3.186
Cheng Lin,Cao Liumei,Ren Hao,Guo Qiaoqiao,Deng Huifang,Li Yiming
The construction of a multifunctional catalyst for multistep sequential\tandem reactions at the molecular level faces a formidable challenge. Multivariate (MTV)-MOFs can provide a facile and tunable platform for rationally designing such multifunctional catalysts via grafting different catalytic groups on the bridging ligands. However, the related investigations are still limited. Here, Pd(II) and l -proline are metalated and decorated to organic linkers, respectively, to build a MTV-MOF, which is then successfully applied to sequential Suzuki Coupling/asymmetric Aldol reactions with satisfied coupling performance (yields up to 99%) and good enantioselectivities ( ee anti up to 98%). Inductively coupled plasma optical emission spectrometer (ICP-OES) measurements of the supernatant and hot leaching test suggest the heterogeneous nature of the catalyst. Macrosubstrate tests verify that the reaction occurs inside the pores of the MOF. The heterogeneous catalyst can maintain structural stability and catalytic activity within three cycles. Graphic Abstract Versatile Pd(II) and l -proline were metalated and decorated, respectively, into stable UiO-67 to construct bifunctional and heterogeneous multivariate MOF catalyst, which displayed efficient and recyclable catalytic activity in sequential Suzuki Coupling/asymmetric Aldol reactions.
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高影响因子
Inorganic Chemistry Frontiers
·
2021
·Vol. 8
·期 9
·2280-2287
·
IF 6.569
Yangyang Ren,Chuanliang Li,Baosong Li,Fan Gao,Xinghua Zhang,Xiaojing Yang,Lanlan Li,Zunming Lu,Xiaofei Yu
Here, PtPd nanoframes were prepared by etching Pd@PdPt core–shell rhombic dodecahedrals (RDs) with Fe3+ provided by iron chloride hexahydrate (FeCl3·6H2O). Based on the experimental results, PtPd nanoframes were formed due to the etching of Pd cores. In terms of catalytic performance, the measured specific activity and mass activity of PtPd nanoframes were 1.11 mA cm−2 and 840.38 mA mg−1, respectively, which were much higher than those of Pd@PdPt core–shell RDs, Pt black and Pt/C, suggesting the preeminent activity of PtPd nanoframes. Meanwhile, PtPd nanoframes showed better stability compared with Pd@PdPt core–shell RDs, Pt black and Pt/C. The strengthened catalytic properties may be caused by the larger surface area owing to the novel structure and the strong electronic interaction between Pt and Pd.
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CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Riyang Shu,Ying Xu,Longlong Ma,Qi Zhang,Chao Wang,Ying Chen
Many effective methods have been proposed to achieve lignin depolymerization, while controllable product distribution is still hard to realize. Herein, an efficient lignin hydrogenolysis process with controllable product distribution was put forward using Pd/C catalyst cooperated with metal chloride. Results showed that lignin produced a high amount of guaiacols in the presence of ZnCl 2 , while a high amount of phenols in the presence of CrCl 3 . Guaiacylglycerol-β-guaiacyl ether was used as the model compound to carry out the mechanistic investigation. A synergetic catalysis effect between Pd/C and metal chloride was exhibited in this process. And the Lewis acidity was an important factor to determine the product distribution. With the synergetic catalysis of Pd/C and metal chloride, the dissociation energy of β-O-4 bond was reduced significantly, which made the cleavage easier to realize. The phenolic monomer product of guaiacols was produced in the initial stage. Then CrCl 3 catalyst with strong Lewis acidity could further promote the occurrence of demethoxylation and alkylation, converting the guaiacols into phenols. This work figures out the mechanism of product control in the hydrogenolysis process and displays a clear potential for the controllable valorization of lignin.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Hui Chen,Jie He,Jinsheng Sun
The production of cyclohexanone, of industrial importance, is at a distance to environment friendly and efficiency. As a solution, a mild sustainable catalytic hydrogenation is presented herein, of phenol into cyclohexanone on Pd/C with potassium formate the hydrogen donor under open atmosphere. Some important reaction conditions, such as temperature, reaction time, catalyst, amount of potassium formate, etc. were investigated and analyzed. The positive growth was found to accelerate the conversion rate of phenol while reducing cyclohexanone selectivity by weakening the protection of phosphotungstic acid. Phosphotungstic acid was confirmed to be the co-catalyst exhibiting the highest activity under given conditions. Based on experiments, we have made reasonable assumptions about the reaction mechanism, while the reaction kinetics proves high reaction rates within a wide temperature range, indicating the reaction to be quick process. Furthermore, the good reusability and recyclability of Pd/C catalyst is verified to benefit future industrial applications.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Wenhui Zou,Yingcen Liu,Caicheng Song,Hua Lin,He Huang,Wanyue Ye,Rongwen Lu,Shufen Zhang
A series of PdO@MCM-41-x was in situ synthesized by a facile one-pot method, and their catalytic performance for dehydrogenation of formic acid was investigated. The PdO nanoparticles were immobilized in MCM-41 channel with small size of 2.2–2.5 nm due to the confinement of mesoporous silica . The initial turnover frequency (TOF) of as-prepared catalyst can reach 1096 h −1 at 323 K with 100% hydrogen selectivity. The hydrogen production activity was better than that of catalyst priorly reduced by hydrogen because of the gradual reduction of PdO nanoparticles and generation of fresh Pd(0) during the formic acid dehydrogenation process, which was confirmed by XPS characterization and catalytic system monitoring. It provides a new way for the preparation of simple and efficient catalysts for hydrogen production , which has great application potential.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2025
·
IF 4.1
Zikang Hou,Baogang Zhang,Xia Li,Yuanjie Liang
Tailoring a highly active interlayer in Pd electrodes is critical for determining electrode performance and stability. In this study, an active Cu-porphyrin interlayer is electrodeposited onto the sponge nickel (SN) skeleton. The modified sponge nickel is subsequently used to support Pd particles and fabricate an effective Pd/Cu-P/SN composite electrode. Compared with the initial Pd/SN electrode, the increase in dechlorination efficiency is 3.59 times for the Pd/Cu-P/SN electrode. Furthermore, substantial improvements in both mass activity and current efficiency are achieved, with respective increases of approximately 14.2-fold and 4.2-fold relative to the untreated electrode. These significant enhancements are ascribed to the well-designed active Cu-porphyrin interphase. Specifically, the Cu-porphyrin interlayer on the SN skeleton provides an enlarged specific surface area, thus accommodating a greater dispersion of Pd particles. Additionally, the confinement of Pd particles on Cu-porphyrin regions leads to the establishment of Pd Cu interfaces, and this interfacial intimacy expedites the evolution of active hydrogen, leading to a high electrocatalytic removal rate even at an elevated 4-chlorophenol concentration. The Pd/Cu-P/SN composite electrode presented here shows a great application potential for the electrocatalytic treatment of organic chlorophenol wastewater, which also paves a new avenue for enhancing electrode properties through rational introducing of metal-porphyrin interphase.
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产品关联
DOI
高影响因子
BIOMATERIALS
·
2025
·
IF 12.9
Zhanxue Xu,Xinrui Yang,Xingyu Lu,Dandan Su,Yidan Wang,Huixing Wu,Zhenhua Zhang,Changrui Long,Liqian Su,Yanyu Wang,Hongbo Chen,Shijian Xiang,Benjie Zhou
Combination therapies for melanoma face challenges due to asynchronous drug delivery and associated toxicity, underscoring the need for advanced delivery systems. While immune checkpoint inhibitors (ICIs) enhance T cell activity, optimal cytotoxic responses require efficient antigen presentation by mature dendritic cells (DCs), which are often functionally impaired in the tumor microenvironment. Thus, effective treatment requires coordinated T cell activation, DC-mediated priming, and direct tumor suppression. Herein, wild Glycyrrhiza uralensis Fisch roots-derived nanovesicles (GC NV) are demonstrated to be effective inhibitors of melanoma proliferation. The vesicles exert this activity through the intracellular delivery of encapsulated miRNA (miR2916) and bioactive molecules (isoliquiritigenin), with this capacity for intracellular delivery extending to the STING agonist DMXAA. We also demonstrate how chemical modification can be used to install PD-L1 antibodies on the membrane surface of these GC NV, imbuing these vesicles with selectivity for tumor cells. Combining DMXAA encapsulation with surface-displayed PD-L1 antibodies creates vesicles (GP@DMX NV) that both promote DCs maturation and elicit CD8 + T cell response. Our multifunctional GP@DMX NV reverse the immunosuppressive microenvironment of melanoma and significantly enhance the immunotherapeutic potential of immune checkpoints.
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DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Xinyi Hu,Xiaoying Qi,Hui Xiong,Jiale Dou,Linsen Li,Ming Ma,Riguang Zhang,Zhao Jiang
Direct methanol fuel cells (DMFCs) have gained widespread attention as environmentally friendly energy conversion devices, but the commercialization process still faces many challenges. Among these factors, low catalytic performance and high noble metal content of anode electrocatalysts limits the commercial applications. Based on the oxidation process of CO ads in the rate-limiting step of alkaline methanol oxidation reaction (MOR), a strategy to accurately regulate the oxygen content of the catalyst was proposed by controlling calcination temperature of transition metal nitride. A series of Pd-MoO x N y /C catalysts were designed and constructed. The results showed that Pd-MoO x N y /C-2 obtained after calcination at 400 °C showed the highest catalytic activity (3218.75 A·g Pd −1 ), kinetic and CO toxicity resistance for MOR. The structural characterizations showed that the nanoparticle size and dispersion of Pd, the surface oxidation degree and oxygen doping ratio of the catalysts significantly changed the electronic structures and surface element composition, altered the d-band centers, which promoted the activation of methanol molecules and intermediates. In a word, catalytic performance for MOR may be precisely controlled by directly controlling the composition and structure of the catalyst surfaces.
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高影响因子
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