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Pd-Ni nanoparticles supported on titanium oxide as effective catalysts for Suzuki-Miyaura coupling reactions

Dongxu Han, Zhiguo Zhang, Zongbi Bao, Huabin Xing, Qilong Ren

《化学科学与工程前沿（英文）》 2018年 第12卷 第1期   页码 24-31 doi: 10.1007/s11705-017-1669-4

摘要： We have successfully prepared a series of Pd-Ni/TiO catalysts by a one-step impregnation-reduction method. Among these catalysts with different compositions of Ni and Pd, the one with the Ni:Pd ratio of 2.95 showed the best activity. Small monodispersed Pd-Ni bimetallic nanoparticles were loaded on the surface of titanium oxide nanopowder as confirmed with TEM and EDS mapping. The XPS analysis demonstrated that Pd exists as 31% Pd(II) species and 69% Pd(0) species and all nickel is Ni(II). The prepared Pd-Ni/TiO exhibited enhanced catalytic activity compared to an equal amount of Pd/TiO for Suzuki-Miyaura reactions together with excellent applicability and reusability.

关键词： Pd-Ni bimetallic nanoparticles     nanocatalysis     Suzuki-Miyaura reaction     titanium oxide    

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Ultrafine Fe-modulated Ni nanoparticles embedded within nitrogen-doped carbon from Zr-MOFs-confined conversion

《化学科学与工程前沿（英文）》 2022年 第16卷 第7期   页码 1114-1124 doi: 10.1007/s11705-021-2087-1

摘要： Improvement of the low-cost transition metal electrocatalyst used in sluggish oxygen evolution reaction is a significant but challenging problem. In this study, ultrafine Fe-modulated Ni nanoparticles embedded in a porous Ni-doped carbon matrix were produced by the pyrolysis of zirconium metal-organic-frameworks, in which 2,2′-bipyridine-5,5′-dicarboxylate operating as a ligand can coordinate with Ni2+ and Fe3+. This strategy allows formation of Fe-modulated Ni nanoparticles with a uniform dimension of about 2 nm which can be ascribed to the spatial blocking effect of ZrO2. This unique catalyst displays an efficient oxygen evolution reaction electrocatalytic activity with a low overpotential of 372 mV at 10 mA·cm–2 and a small Tafel slope of 84.4 mV·dec–1 in alkaline media. More importantly, it shows superior durability and structural stability after 43 h in a chronoamperometry test. Meanwhile, it shows excellent cycling stability during 4000 cyclic voltammetry cycles. This research offers a new insight into the construction of uniform nanoscale transition metals and their alloys as highly efficient and durable electrocatalysts.

关键词： metal-organic framework     pyrolysis     ultrafine     Fe-modulated Ni nanoparticles     oxygen evolution reaction    

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Room-temperature hydrogenation of halogenated nitrobenzenes over metal–organic-framework-derived ultra-dispersed Ni

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1782-1792 doi: 10.1007/s11705-022-2220-9

摘要： Ultra-dispersed Ni nanoparticles (7.5 nm) on nitrogen-doped carbon nanoneedles (Ni@NCNs) were prepared by simple pyrolysis of Ni-based metal–organic-framework for selective hydrogenation of halogenated nitrobenzenes to corresponding anilines. Two different crystallization methods (stirring and static) were compared and the optimal pyrolysis temperature was explored. Ni@NCNs were systematically characterized by wide analytical techniques. In the hydrogenation of p-chloronitrobenzene, Ni@NCNs-600 (pyrolyzed at 600 °C) exhibited extraordinarily high performance with 77.9 h–1 catalytic productivity and > 99% p-chloroaniline selectivity at full p-chloronitrobenzene conversion under mild conditions (90 °C, 1.5 MPa H2), showing obvious superiority compared with reported Ni-based catalysts. Notably, the reaction smoothly proceeded at room temperature with full conversion and > 99% selectivity. Moreover, Ni@NCNs-600 afforded good tolerance to various nitroarenes substituted by sensitive groups (halogen, nitrile, keto, carboxylic, etc.), and could be easily recycled by magnetic separation and reused for 5 times without deactivation. The adsorption tests showed that the preferential adsorption of –NO2 on the catalyst can restrain the dehalogenation of p-chloronitrobenzene, thus achieving high p-chloroaniline selectivity. While the high activity can be attributed to high Ni dispersion, special morphology, and rich pore structure of the catalyst.

关键词： halogenated nitrobenzenes     room-temperature hydrogenation     Ni nanoparticles     nitrogen-doped carbon nanoneedles     metal–organic-framework    

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Bamboo-like -doped carbon nanotubes encapsulating M(Co, Fe)-Ni alloy for electrochemical production of

《化学科学与工程前沿（英文）》 2022年 第16卷 第4期   页码 498-510 doi: 10.1007/s11705-021-2082-6

摘要： The electrochemical conversion of CO2-H2O into CO-H2 using renewable energy is a promising technique for clean syngas production. Low-cost electrocatalysts to produce tunable syngas with a potential-independent CO/H2 ratio are highly desired. Herein, a series of N-doped carbon nanotubes encapsulating binary alloy nanoparticles (MxNi-NCNT, M= Fe, Co) were successfully fabricated through the co-pyrolysis of melamine and metal precursors. The MxNi-NCNT samples exhibited bamboo-like nanotubular structures with a large specific surface area and high degree of graphitization. Their electrocatalytic performance for syngas production can be tuned by changing the alloy compositions and modifying the electronic structure of the carbon nanotube through the encapsulated metal nanoparticles. Consequently, syngas with a wide range of CO/H2 ratios, from 0.5:1 to 3.4:1, can be produced on MxNi-NCNT. More importantly, stable CO/H2 ratios of 2:1 and 1.5:1, corresponding to the ratio to produce biofuels by syngas fermentation, could be realized on Co1Ni-NCNT and Co2Ni-NCNT, respectively, over a potential window of –0.8 to –1.2 V versus the reversible hydrogen electrode. Our work provides an approach to develop low-cost and potential-independent electrocatalysts to effectively produce syngas with an adjustable CO/H2 ratio from electrochemical CO2 reduction.

关键词： electrochemical reduction of CO2     syngas     N-doped carbon nanotubes     encapsulated alloy nanoparticles     CO/H2 ratio    

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Translocation and biotoxicity of metal (oxide) nanoparticles in the wetland-plant system

《环境科学与工程前沿（英文）》 2021年 第15卷 第6期 doi: 10.1007/s11783-021-1432-4

摘要：

• Aquatic plants are more likely to absorb TiO2 NPs that are beneficial to them.

关键词： Constructed wetlands     Aquatic plants     Nanoparticles     Physiological activity     Biomass    

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Enhanced 4-chlorophenol biodegradation by integrating FeO nanoparticles into an anaerobic reactor: Long-term

《环境科学与工程前沿（英文）》 2022年 第16卷 第8期 doi: 10.1007/s11783-022-1519-6

摘要：

• 4-chlorophenol biodegradation could be enhanced in Fe2O3 coupled anaerobic system.

关键词： Dechlorination     Fe2O3 nanoparticles     Electron transfer     Microbial community    

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Gold nanoparticles/single-stranded DNA-reduced graphene oxide nanocomposites based electrochemical biosensor

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1572-1582 doi: 10.1007/s11705-021-2112-4

摘要： High density and uniform distribution of the gold nanoparticles functionalized single-stranded DNA modified reduced graphene oxide nanocomposites were obtained by non-covalent interaction. The positive gold nanoparticles prepared by phase inversion method exhibited good dimensional homogeneity and dispersibility, which could readily combine with single-stranded DNA modified reduced graphene oxide nanocomposites by electrostatic interactions. The modification of single-stranded DNA endowed the reduced graphene oxide with favorable biocompatibility and provided the preferable surface with negative charge for further assembling of gold nanoparticles to obtain gold nanoparticles/single-stranded DNA modified reduced graphene oxide nanocomposites with better conductivity, larger specific surface area, biocompatibility and electrocatalytic characteristics. The as-prepared nanocomposites were applied as substrates for the construction of cholesterol oxidase modified electrode and well realized the direct electron transfer between the enzyme and electrode. The modified gold nanoparticles could further catalyze the products of cholesterol oxidation catalyzed by cholesterol oxidase, which was beneficial to the enzyme-catalyzed reaction. The as-fabricated bioelectrode exhibited excellent electrocatalytic performance for the cholesterol with a linear range of 7.5‒280.5 μmol·L‒1, a low detection limit of 2.1 μmol·L‒1, good stability and reproducibility. Moreover, the electrochemical biosensor showed good selectivity and acceptable accuracy for the detection of cholesterol in human serum samples.

关键词： reduced graphene oxide     gold nanoparticles     electrochemical biosensor     cholesterol oxidase     cholesterol    

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polymeric substances from activated sludge on the aggregation kinetics of silver and silver sulfide nanoparticles

《环境科学与工程前沿（英文）》 2022年 第16卷 第2期 doi: 10.1007/s11783-021-1450-2

摘要：

• The NPs aggregation in the electrolyte solution is consistent with the DLVO theory.

关键词： Silver nanoparticles     Silver sulfide nanoparticles     Extracellular polymeric substances     Aggregation kinetics     Influence mechanisms    

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The cooperation effect of Ni and Pt in the hydrogenation of acetic acid

《化学科学与工程前沿（英文）》 2022年 第16卷 第3期   页码 397-407 doi: 10.1007/s11705-021-2076-4

摘要： The catalytic hydrogenation of carboxylic acid to alcohols is one of the important strategies for the conversion of biomass. Herein, a series of Ni-doped PtSn catalysts were prepared, characterized and studied in the hydrogenation of acetic acid. The Ni dopant has a strong interaction with Pt, which promotes the hydrogen adsorption, providing an activated hydrogen-rich environment for the hydrogenation. Meanwhile, the presence of Ni also improves the Pt dispersion, giving more accessible active sites for hydrogen activation. The cooperation of Pt and Ni significantly promotes the catalytic activity of the hydrogenation of acetic acid to ethanol. As a result, the catalyst with 0.1% Ni exhibits the best reaction activity, and its space time yield is twice as that of the PtSn/SiO2 catalyst. It provides a meaningful instruction on the catalyst design for the carboxylic acid hydrogenation.

关键词： acetic acid     ethanol     hydrogenation     Pt     Ni     cooperation effect    

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Size and shape effects of MnFeO nanoparticles as catalysts for reductive degradation of dye pollutants

《环境科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 108-171 doi: 10.1007/s11783-021-1396-4

摘要： The magnetic nanoparticles that are easy to recycle have tremendous potential as a suitable catalyst for environmental toxic dye pollutant degradation. Rationally engineering shapes and tailoring the size of nanocatalysts are regarded as an effective manner for enhancing performances. Herein, we successfully synthesized three kinds of MnFe2O4 NPs with distinctive sizes and shapes as catalysts for reductive degradation of methylene blue, rhodamine 6G, rhodamine B, and methylene orange. It was found that the catalytic activities were dependent on the size and shape of the MnFe2O4 NPs and highly related to the surface-to-volume ratio and atom arrangements. Besides, all these nanocatalysts exhibit selectivity to different organic dyes, which is beneficial for their practical application in dye pollutant treatment. Furthermore, the MnFe2O4 NPs could be readily recovered by a magnet and reused more than ten times without appreciable loss of activity. The size and shape effects of MnFe2O4 nanoparticles demonstrated in this work not only accelerate further understanding the nature of nanocatalysts but also contribute to the precise design of nanoparticles catalyst for pollutant degradation.

关键词： Dye degradation     MnFe2O4 nanoparticles     Size and shape-control    

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Functional magnetic nanoparticles for facile viable but nonculturable bacteria separation and purification

Chunming Wang, Huirong Lin, Chengsong Ye

《环境科学与工程前沿（英文）》 2016年 第10卷 第6期 doi: 10.1007/s11783-016-0874-6

摘要： The functional surface-modified MNPs were capable of capture with high efficiency. After induced to VBNC state by chlorination, cells could be separated by MNPs with an additional incubation process. This study provides a facile and economic method for VBNC cell enrichment and purification. GRAPHIC ABSTRACT Viable But Nonculturable (VBNC) Bacteria, which represent a unique population of microorganisms in drinking water systems, have become a potential threat to human health. Current studies on VBNC cells usually fail to obtain pure VBNC state bacteria, which may lead to inaccurate results. We therefore introduce a novel method of VBNC cell separation and purification in this paper. PAH-coated magnetic nanoparticles (MNPs) were synthesized and found to be capable of capturing and releasing bacterial cells with high efficiency. With the aid of an additional incubation step, VBNC cells were easily isolated and purified from normal bacteria using functional MNPs. Our method represents a new technique that can be utilized in studies of VBNCs.

关键词： Drinking water biosafety     VBNC     Nanoparticles     Magnetic separation and purification    

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Size-controlled green synthesis of silver nanoparticles assisted by L-cysteine

Wenchao Zhang,Lin Zhang,Yan Sun

《化学科学与工程前沿（英文）》 2015年 第9卷 第4期   页码 494-500 doi: 10.1007/s11705-015-1527-1

摘要： A green and size-controlled synthesis of silver nanoparticles (Ag NPs) in aqueous solution with the assistance of L-cysteine is presented. The size of Ag NPs decreases with the increase of L-cysteine concentration, and thus can be controlled by adjusting L-cysteine concentration. TEM analysis shows that Ag NPs with an average size of 3 nm can be produced in the presence of 1.0 mmol/L L-cysteine, about one sixth of the size of Ag NPs obtained in the absence of L-cysteine (17 nm). The as-synthesized silver colloidal solution is stable and can be stored at room temperature for at least two months without any precipitation. This L-cysteine assisted method is simple, feasible and efficient, and would facilitate the production and application of Ag NPs.

关键词： nanoparticles     silver     L-cysteine     size distribution     synthesis    

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Catalytic decomposition of low level ozone with gold nanoparticles supported on activated carbon

Pengyi ZHANG , Bo ZHANG , Rui SHI ,

《环境科学与工程前沿（英文）》 2009年 第3卷 第3期   页码 281-288 doi: 10.1007/s11783-009-0032-5

摘要： Highly dispersed gold nanoparticles were supported on coal-based activated carbon (AC) by a sol immobilization method and were used to investigate their catalytic activity for low-level ozone decomposition at ambient temperature. Nitrogen adsorption-desorption, scanning electron microscope (SEM), and X-ray photoelectron spectroscopy (XPS) were used to characterize the catalysts before and after ozone decomposition. The results showed that the supported gold nanoparticles prepared with microwave heating were much smaller and more uniformly dispersed on the activated carbon than those prepared with traditional conduction heating, exhibiting higher catalytic activity for ozone decomposition. The pH values of gold precursor solution significantly influenced the catalytic activity of supported gold for ozone decomposition, and the best pH value was 8. In the case of space velocity of 120000h, inlet ozone concentration of 50mg/m, and relative humidity of 45%, the Au/AC catalyst maintained the ozone removal ratio at 90.7% after 2500min. After being used for ozone decomposition, the surface carbon of the catalyst was partly oxidized and the oxygen content increased accordingly, while its specific surface area and pore volume only decreased a little. Ozone was mainly catalytically decomposed by the gold nanoparticles supported on the activated carbon.

关键词： ozone decomposition     activated carbon     gold nanoparticles     catalysis     sodium citrate     microwave    

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Ecotoxicological effect of zinc oxide nanoparticles on soil microorganisms

Zhaoyi SHEN,Zhuo CHEN,Zhen HOU,Tingting LI,Xiaoxia LU

《环境科学与工程前沿（英文）》 2015年 第9卷 第5期   页码 912-918 doi: 10.1007/s11783-015-0789-7

摘要： The widespread production and use of zinc oxide nanoparticles (ZnO-NPs) in recent years have posed potential threat to the ecosystem. This study aimed to investigate the ecotoxicological effect of ZnO-NPs on soil microorganisms using laboratory microcosm test. Respiration, ammonification, dehydrogenase (DH) activity, and fluorescent diacetate hydrolase (FDAH) activity were used as ecotoxicological parameters. The results showed that in the neutral soil treated with 1 mg ZnO-NPs per g soil (fresh, neutral), ammonification was significantly inhibited during the study period of three months, but the inhibition rate decreased over increasing time. Inhibition in respiration was observed in the first month of the test. In various ZnO-NPs treatments (1 mg, 5 mg, and 10 mg ZnO-NPs per g soil), DH activity and FDAH activity were inhibited during the study period of one month. For both enzyme activities, there were positive dose–response relationships between the concentration of ZnO-NPs and the inhibition rates, but the curves changed over time due to changes of ZnO-NPs toxicity. Soil type affected the toxicity of ZnO-NPs in soil. The toxicity was highest in the acid soil, followed by the neutral soil. The toxicity was relatively low in the alkaline soil. The toxicity was not accounted for by the Zn released from the ZnO-NPs. Direct interaction of ZnO-NPs with biologic targets might be one of the reasons. The adverse effect of ZnO-NPs on soil microorganisms in neutral and acid soils is worthy of attention.

关键词： zinc oxide nanoparticles (ZnO-NPs)     soil microorganisms     respiration     ammonification     dehydrogenase (DH) activity     fluorescent diacetate hydrolase (FDAH) activity    

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VITHM1 mediated green synthesis of silver nanoparticles: Mechanism and biological applications

Mani Abirami, Krishnan Kannabiran

《化学科学与工程前沿（英文）》 2016年 第10卷 第4期   页码 542-551 doi: 10.1007/s11705-016-1599-6

摘要： We present the microbial green synthesis of silver nanoparticles (NPs) by VITHM1 strain (MTCC No. 12465). The secondary metabolites in the cell free supernatant of this bacterium when incubated with 1 mmol/L AgNO , mediated the biological synthesis of AgNPs. The synthesized AgNPs were characterized by UV-visible spectrum, X-ray diffraction (XRD), atomic force microscope, scanning electron microscopy equipped with energy dispersive spectroscopy, transmission electron microscopy, FT-IR spectroscopy, dynamic light scattering and zeta potential. They were highly stable and, spherical in shape with the average size of 30?50 nm. The secondary metabolites involved in the formation of AgNPs were identified gas chromatography-mass spectrography. The 3D structure of the unit cell of the synthesized AgNPs was determined using XRD data base. The synthesized AgNPs exhibited significant antibacterial activity against tested bacterial pathogens, and did not show haemolysis on human red blood cells. This green synthesis could provide a new platform to explore and use AgNPs as antibacterial therapeutic agents.

关键词： Streptomyces ghanaensis VITHM1     nanoparticles     3D structure     antibacterial activity    

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标题 作者 时间 类型 操作

Pd-Ni nanoparticles supported on titanium oxide as effective catalysts for Suzuki-Miyaura coupling reactions

Dongxu Han, Zhiguo Zhang, Zongbi Bao, Huabin Xing, Qilong Ren

期刊论文

Ultrafine Fe-modulated Ni nanoparticles embedded within nitrogen-doped carbon from Zr-MOFs-confined conversion

期刊论文

Room-temperature hydrogenation of halogenated nitrobenzenes over metal–organic-framework-derived ultra-dispersed Ni

期刊论文

Bamboo-like -doped carbon nanotubes encapsulating M(Co, Fe)-Ni alloy for electrochemical production of

期刊论文

Translocation and biotoxicity of metal (oxide) nanoparticles in the wetland-plant system

期刊论文

Enhanced 4-chlorophenol biodegradation by integrating FeO nanoparticles into an anaerobic reactor: Long-term

期刊论文

Gold nanoparticles/single-stranded DNA-reduced graphene oxide nanocomposites based electrochemical biosensor

期刊论文

polymeric substances from activated sludge on the aggregation kinetics of silver and silver sulfide nanoparticles

期刊论文

The cooperation effect of Ni and Pt in the hydrogenation of acetic acid

期刊论文

Size and shape effects of MnFeO nanoparticles as catalysts for reductive degradation of dye pollutants

期刊论文

Functional magnetic nanoparticles for facile viable but nonculturable bacteria separation and purification

Chunming Wang, Huirong Lin, Chengsong Ye

期刊论文

Size-controlled green synthesis of silver nanoparticles assisted by L-cysteine

Wenchao Zhang,Lin Zhang,Yan Sun

期刊论文

Catalytic decomposition of low level ozone with gold nanoparticles supported on activated carbon

Pengyi ZHANG , Bo ZHANG , Rui SHI ,

期刊论文

Ecotoxicological effect of zinc oxide nanoparticles on soil microorganisms

Zhaoyi SHEN,Zhuo CHEN,Zhen HOU,Tingting LI,Xiaoxia LU

期刊论文

VITHM1 mediated green synthesis of silver nanoparticles: Mechanism and biological applications

Mani Abirami, Krishnan Kannabiran

期刊论文