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Conversion of CO into CO by high active and stable PdNi nanoparticles supported on a metal-organic framework

《化学科学与工程前沿（英文）》 2022年 第16卷 第7期   页码 1139-1148 doi: 10.1007/s11705-021-2111-5

摘要： The solubility of Pd(NO3)2 in water is moderate whereas it is completely soluble in diluted HNO3 solution. Pd/MIL-101(Cr) and Pd/MIL-101-NH2(Cr) were synthesized by aqueous solution of Pd(NO3)2 and Pd(NO3)2 solution in dilute HNO3 and used for CO oxidation reaction. The catalysts synthesized with Pd(NO3)2 solution in dilute HNO3 showed lower activity. The aqueous solution of Pd(NO3)2 was used for synthesis of mono-metal Ni, Pd and bimetallic PdNi nanoparticles with various molar ratios supported on MOF. Pd70Ni30/MIL-101(Cr) catalyst showed higher activity than monometallic counterparts and Pd+ Ni physical mixture due to the strong synergistic effect of PdNi nanoparticles, high distribution of PdNi nanoparticles, and lower dissociation and desorption barriers. Comparison of the catalysts synthesized by MIL-101(Cr) and MIL-101-NH2(Cr) as the supports of metals showed that Pd/MIL-101-NH2(Cr) outperforms Pd/MIL-101-(Cr) because of the higher electron density of Pd resulting from the electron donor ability of the NH2 functional group. However, the same activities were observed for Pd70Ni30/MIL-101(Cr) and Pd70Ni30/MIL-101-NH2(Cr), which is due to a less uniform distribution of Pd nanoparticles in Pd70Ni30/MIL-101-NH2(Cr) originated from amorphization of MIL-101-NH2(Cr) structure during the reduction process. In contrast, Pd70Ni30/MIL-101(Cr) revealed the stable structure and activity during reduction and CO oxidation for a long time.

关键词： CO oxidation     heterogeneous catalysis     metal-organic framework     NH2 functional group     PdNi    

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Bamboo-like -doped carbon nanotubes encapsulating M(Co, Fe)-Ni alloy for electrochemical production ofsyngas with potential-independent CO/H ratios

《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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Theoretical and experimental study on the fluidity performance of hard-to-fluidize carbon nanotubes-based CO2

《化学科学与工程前沿（英文）》 2022年 第16卷 第10期   页码 1460-1475 doi: 10.1007/s11705-022-2159-x

摘要： Carbon nanotubes-based materials have been identified as promising sorbents for efficient CO2 capture in fluidized beds, suffering from insufficient contact with CO2 for the high-level CO2 capture capacity. This study focuses on promoting the fluidizability of hard-to-fluidize pure and synthesized silica-coated amine-functionalized carbon nanotubes. The novel synthesized sorbent presents a superior sorption capacity of about 25 times higher than pure carbon nanotubes during 5 consecutive adsorption/regeneration cycles. The low-cost fluidizable-SiO2 nanoparticles are used as assistant material to improve the fluidity of carbon nanotubes-based sorbents. Results reveal that a minimum amount of 7.5 and 5 wt% SiO2 nanoparticles are required to achieve an agglomerate particulate fluidization behavior for pure and synthesized carbon nanotubes, respectively. Pure carbon nanotubes + 7.5 wt% SiO2 and synthesized carbon nanotubes + 5 wt% SiO2 indicates an agglomerate particulate fluidization characteristic, including the high-level bed expansion ratio, low minimum fluidization velocity (1.5 and 1.6 cm·s–1), high Richardson−Zakin index (5.2 and 5.3 > 5), and low Π value (83.2 and 84.8 < 100, respectively). Chemical modification of carbon nanotubes causes not only enhanced CO 2 uptake capacity but also decreases the required amount of silica additive to reach a homogeneous fluidization behavior for synthesized carbon nanotubes sorbent.

关键词： CO2 capture     CNT-based sorbents     fluidization     SiO2 nanoparticles     fluidized bed reactors    

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Effect of TiO

Navid Azizi, Mojgan Isanejad, Toraj Mohammadi, Reza M. Behbahani

《化学科学与工程前沿（英文）》 2019年 第13卷 第3期   页码 517-530 doi: 10.1007/s11705-018-1781-0

摘要： Membranes have attracted much attention as economical methods for industrial chemical processes. The effects of the titanium dioxide nanoparticle load on the morphology and CO /CH separation performance of poly (ether-block-amide) (PEBAX-1657) mixed matrix membranes (MMMs) were investigated from pressures of 3–12 bar and temperatures of 30°C–60°C. The PEBAX membranes were characterized by scanning electron microscopy, Fourier transform infrared spectroscopy, X-ray diffraction, thermal gravimetric analysis, atomic force microscopy and tensile strength analysis. The incorporation of TiO nanoparticles into the polymeric MMMs improved the CO /CH gas separation performance (both the permeability and selectivity) of the membranes. The CO permeability and ideal CO /CH selectivity values of the nanocomposite membrane loaded with 8 wt-% TiO were 172.32 Barrer and 24.79, respectively whereas those of the neat membrane were 129.87 Barrer and 21.39, respectively.

关键词： mixed matrix membrane     TiO2 nanoparticles     PEBAX-1657     CO2/CH4 separation    

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Cobalt-nanoparticle catalysts derived from zeolitic imidazolate framework@MXene composites for efficient oxidative self-coupling of benzylamines

《化学科学与工程前沿（英文）》 2023年 第18卷 第1期 doi: 10.1007/s11705-023-2378-9

摘要： In this study, we synthesize a catalyst comprising cobalt nanoparticles supported on MXene by pyrolyzing a composite in a N2 environment. Specifically, the composite comprises a bimetallic Zn/Co zeolitic imidazole framework grown in situ on the outer surface of MXene. The catalytic efficiency of the catalyst is tested for the self-coupling of 4-methoxybenzylamine to produce value-added imine, where atmospheric oxygen (1 atm) is used as the oxidant. Based on the results, the catalyst displayed impressive catalytic activity, achieving 95.4% yield of the desired imine at 383 K for 8 h. Furthermore, the catalyst showed recyclability and tolerance toward benzylamine substrates with various functional groups. The outstanding performance of the catalyst is primarily attributed to the synergetic catalytic effect between the cobalt nanoparticles and MXene support, while also benefiting from the three-dimensional porous structure. Additionally, a preliminary investigation of potential reaction mechanisms is conducted.

关键词： MXene     sacrificial template     oxidative self-coupling     Co nanoparticles     imine    

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“Charging” the cigarette butt: heteroatomic porous carbon nanosheets with edge-induced topological defects for enhanced oxygen evolution performance

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1755-1764 doi: 10.1007/s11705-023-2318-8

摘要： Owing to the complexity of electron transfer pathways, the sluggish oxygen evolution reaction process is defined as the bottleneck for the practical application of Zn–air batteries. In this effort, metal nanoparticles (Co, Ni, Fe, etc.) encapsulated within nitrogen-doped carbon materials with abundant edge sites were synthesized by one-step pyrolysis treatment using cigarette butts as raw materials, which can drastically accelerate the overall rate of oxygen evolution reaction by facilitating the adsorption of oxygenated intermediates by the edge-induced topological defects. The prepared catalyst of nitrogen-doped carbon porous nanosheets loaded with Co nanoparticles (Co@NC-500) exhibits enhanced catalytic activity toward oxygen evolution reaction, with a low overpotential of 350 mV at the current density of 10 mA·cm–2. Furthermore, the Zn–air battery assembled with Co@NC-500 catalyst demonstrates a desirable performance affording an open-circuit potential of 1.336 V and power density of 33.6 mW·cm–2, indicating considerable practical application potential.

关键词： oxygen evolution reaction     porous carbon nanosheets     Co nanoparticles     edge-induced topological defects     Zn–air batteries    

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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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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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标题 作者 时间 类型 操作

Conversion of CO into CO by high active and stable PdNi nanoparticles supported on a metal-organic framework

期刊论文

Bamboo-like -doped carbon nanotubes encapsulating M(Co, Fe)-Ni alloy for electrochemical production ofsyngas with potential-independent CO/H ratios

期刊论文

Theoretical and experimental study on the fluidity performance of hard-to-fluidize carbon nanotubes-based CO2

期刊论文

Effect of TiO

Navid Azizi, Mojgan Isanejad, Toraj Mohammadi, Reza M. Behbahani

期刊论文

Cobalt-nanoparticle catalysts derived from zeolitic imidazolate framework@MXene composites for efficient oxidative self-coupling of benzylamines

期刊论文

“Charging” the cigarette butt: heteroatomic porous carbon nanosheets with edge-induced topological defects for enhanced oxygen evolution performance

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

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