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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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Catalytic activity of noble metal nanoparticles toward hydrodechlorination: influence of catalyst electronic

Man ZHANG,Feng HE,Dongye ZHAO

《环境科学与工程前沿（英文）》 2015年 第9卷 第5期   页码 888-896 doi: 10.1007/s11783-015-0774-1

摘要： In this study, stabilized Pd, Pt and Au nanoparticles were successfully prepared in aqueous phase using sodium carboxymethyl cellulose (CMC) as a capping agent. These metal nanoparticles were then tested for catalytic hydrodechlorination toward two classes of organochlorinated compounds (vinyl polychlorides including trichloroethylene (TCE), tetrachloroethylene (PCE), and alkyl polychlorides including 1,1,1-trichloroethane (1,1,1-TCA), and 1,1,1,2-tetrachloroethane (1,1,1,2-TeCA)) to determine the rate-limiting steps and to explore the reaction mechanisms. The surface area normalized reaction rate constant, , showed a systematic dependence on the electronic structure (the density of states at the Fermi level) of the metals, suggesting that adsorption of organochlorinated reactants on the metal catalyst surfaces is the rate-limiting step for catalytic hydrodechlorination. Hydrodechlorination rates of 1,1,1-TCA and 1,1,1,2-TeCA agreed with the bond strength of the first (weakest) dissociated C-Cl bond, suggesting that C-Cl bond cleavage, which is the first step for dissociative adsorption of the alkyl polychlorides, controlled the catalytic hydrodechlorination rate. However, hydrodechlorination rates of TCE and PCE correlated with the adsorption energies of their molecular (non-dissociative) adsorption on the noble metals rather than with the first C-Cl bond strength, suggesting that molecular adsorption governs the reaction rate for hydrodechlorination of the vinyl polychlorides.

关键词： catalytic hydrodechlorination     electronic structure     metal nanoparticles     reaction mechanisms    

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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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Recent advances in gold-metal oxide core-shell nanoparticles: Synthesis, characterization, and their

Michelle Lukosi,Huiyuan Zhu,Sheng Dai

《化学科学与工程前沿（英文）》 2016年 第10卷 第1期   页码 39-56 doi: 10.1007/s11705-015-1551-1

摘要： Heterogeneous catalysis with core-shell structures has been a large area of focus for many years. This paper reviews the most recent work and research in core-shell catalysts utilizing noble metals, specifically gold, as the core within a metal oxide shell. The advantage of the core-shell structure lies in its capacity to retain catalytic activity under thermal and mechanical stress, which is a pivotal consideration when synthesizing any catalyst. This framework is particularly useful for gold nanoparticles in protecting them from sintering so that they retain their size, structure, and most importantly their catalytic efficiency. The different methods of synthesizing such a structure have been compiled into three categories: seed-mediated growth, post selective oxidation treatment, and one-pot chemical synthesis. The selective oxidation of carbon monoxide and reduction of nitrogen containing compounds, such as nitrophenol and nitrostyrene, have been studied over the past few years to evaluate the functionality and stability of the core-shell catalysts. Different factors that could influence the catalyst’s performance are the size, structure, choice of metal oxide shell and noble metal core and thereby the interfacial synergy and lattice mismatch between the core and shell. In addition, the morphology of the shell also plays a critical role, including its porosity, density, and thickness. This review covers the synthesis and characterization of gold-metal oxide core-shell structures, as well as how they are utilized as catalysts for carbon monoxide (CO) oxidation and selective reduction of nitrogen-containing compounds.

关键词： core-shell     characterization     core-shell structure     Different     stability    

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Nexus between polymer support and metal oxide nanoparticles in hybrid nanosorbent materials (HNMs) for

Ryan C. SMITH,Jinze LI,Surapol PADUNGTHON,Arup K. SENGUPTA

《环境科学与工程前沿（英文）》 2015年 第9卷 第5期   页码 929-938 doi: 10.1007/s11783-015-0795-9

摘要： Metal oxide nanoparticles like hydrated ferric oxide (HFO) or hydrated zirconium oxide (HZrO) are excellent sorbents for environmentally significant ligands like phosphate, arsenic, or fluoride, present at trace concentrations. Since the sorption capacity is surface dependent for HFO and HZrO, nanoscale sizes offer significant enhancement in performance. However, due to their miniscule sizes, low attrition resistance, and poor durability they are unable to be used in typical plug-flow column setups. Meanwhile ion exchange resins, which have no specific affinity toward anionic ligands, are durable and chemically stable. By impregnating metal oxide nanoparticles inside a polymer support, with or without functional groups, a hybrid nanosorbent material (HNM) can be prepared. A HNM is durable, mechanically strong, and chemically stable. The functional groups of the polymeric support will affect the overall removal efficiency of the ligands exerted by the Donnan Membrane Effect. For example, the removal of arsenic by HFO or the removal of fluoride by HZrO is enhanced by using anion exchange resins. The HNM can be precisely tuned to remove one type of contaminant over another type. Also, the physical morphology of the support material, spherical bead versus ion exchange fiber, has a significant effect on kinetics of sorption and desorption. HNMs also possess dual sorption sites and are capable of removing multiple contaminants, namely, arsenate and perchlorate, concurrently.

关键词： ion exchange     sorption     arsenic     perchlorate     fluoride    

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Influence of surface modified mixed metal oxide nanoparticles on the electrochemical and mechanical properties

《化学科学与工程前沿（英文）》 2023年 第17卷 第1期   页码 1-14 doi: 10.1007/s11705-022-2176-9

摘要： Newly synthesized functional nanoparticles, 3-amino-1,2,4-triazole (ATA)/SiO2–TiO2 were introduced to the polyurethane (PU) matrix. Electrochemical techniques were used to investigate the barrier properties of the synthesized PU–ATA/SiO2–TiO2 nanocomposite coated steel specimen. In natural seawater, electrochemical impedance spectroscopy experiments indicated outstanding protective behaviour for the PU–ATA/SiO2–TiO2 coated steel. The coating resistance (Rcoat) of PU–ATA/SiO2–TiO2 was determined to be 2956.90 kΩ·cm–2. The Rcoat of the PU–ATA/SiO2–TiO2 nanocomposite coating was found to be over 50% higher than the PU coating. The current measured along the scratched surface of the PU–ATA/SiO2–TiO2 coating was found to be very low (1.65 nA). The enhanced ATA/SiO2–TiO2 nanoparticles inhibited the entry of electrolytes into the coating interface, as revealed by scanning electron microscopy/energy dispersive X-ray spectroscopy and X-ray diffraction analysis of the degradation products. Water contact angle testing validated the hydrophobic nature of the PU–ATA/SiO2–TiO2 coating (θ = 115.4°). When the concentration of ATA/SiO2−TiO2 nanoparticles was 2 wt %, dynamic mechanical analysis revealed better mechanical properties. Therefore, the newly synthesised PU–ATA/SiO2–TiO2 nanocomposite provided excellent barrier and mechanical properties due to the addition of ATA/SiO2–TiO2 nanoparticles to the polyurethane, which inhibited material degradation and aided in the prolongation of the coated steel’s life.

关键词： SiO2/TiO2 nanoparticle     nanocomposite coatings     dynamic mechanical analysis     electrochemical techniques     corrosion     colloids and interfaces    

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(Super)paramagnetic nanoparticles as platform materials for environmental applications: From synthesis

Wenlu Li, John D. Fortner

《环境科学与工程前沿（英文）》 2020年 第14卷 第5期 doi: 10.1007/s11783-020-1256-7

摘要： • The fabrication of monodisperse, (super)paramagnetic nanoparticles is summarized. • Monolayer and bilayer surface coating structures are described. • Mono/bilayer coated nanoparticles showed high sorption capacities for U, As, and Cr. Over the past few decades, engineered, (super)paramagnetic nanoparticles have drawn extensive research attention for a broad range of applications based on their tunable size and shape, surface chemistries, and magnetic properties. This review summaries our recent work on the synthesis, surface modification, and environmental application of (super)paramagnetic nanoparticles. By utilizing high-temperature thermo-decomposition methods, first, we have broadly demonstrated the synthesis of highly monodispersed, (super)paramagnetic nanoparticles, via the pyrolysis of metal carboxylate salts in an organic phase. Highly uniform magnetic nanoparticles with various size, composition, and shape can be precisely tuned by controlled reaction parameters, such as the initial precursors, heating rate, final reaction temperature, reaction time, and the additives. These materials can be further rendered water stable via functionalization with surface mono/bi-layer coating structure using a series of tunable ionic/non-ionic surfactants. Finally, we have demonstrated platform potential of these materials for heavy metal ions sensing, sorption, and separation from the aqueous phase.

关键词： Superparamagnetic nanoparticles     Surface functionalization     Environmental sensing     Heavy metal ion sorption    

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Application of metal oxides-based nanofluids in PV/T systems: a review

《能源前沿（英文）》 2022年 第16卷 第3期   页码 397-428 doi: 10.1007/s11708-021-0758-8

摘要： Having the wide application of metal oxides in energy technologies, in recent years, many researchers tried to increase the performance of the PV/T system by using metal oxide-based nanofluids (NFs) as coolants or optical filters or both at the same time. This paper summarizes recent research activities on various metal oxides (Al2O3, TiO2, SiO2, Fe3O4, CuO, ZnO, MgO)-based NFs performance in the PV/T system regarding different significant parameters, e.g., thermal conductivity, volume fraction, mass flowrate, electrical, thermal and overall efficiency, etc. By conducting a comparative study among the metal oxide-based NFs, Al2O3/SiO2-water NFs are mostly used to achieve maximum performance. The Al2O3-water NF has a prominent heat transfer feature with a maximum electrical efficiency of 17%, and a maximum temperature reduction of PV module of up to 36.9°C can be achieved by using the Al2O3-water NF as a coolant. Additionally, studies suggest that the PV cell’s efficiency of up to 30% can be enhanced by using a solar tracking system. Besides, TiO2-water NFs have been proved to have the highest thermal efficiency of 86% in the PV/T system, but TiO2 nanoparticles could be hazardous for human health. As a spectral filter, SiO2-water NF at a size of 5 nm and a volume fraction of 2% seems to be very favorable for PV/T systems. Studies show that the combined use of NFs as coolants and spectral filters in the PV/T system could provide a higher overall efficiency at a cheaper rate. Finally, the opportunities and challenges of using NFs in PV/T systems are also discussed.

关键词： metal oxide     nanofluids (NFs)     nanoparticles (NPs)     optical filter     PV/T systems     solar energy    

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Copper nanoparticles/polyaniline-derived mesoporous carbon electrocatalysts for hydrazine oxidation

Tao Zhang, Tewodros Asefa

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 329-338 doi: 10.1007/s11705-018-1741-8

摘要：

Copper nanoparticles-decorated polyaniline-derived mesoporous carbon that can serve as noble metal-free electrocatalyst for the hydrazine oxidation reaction (HzOR) is synthesized via a facile synthetic route. The material exhibits excellent electrocatalytic activity toward HzOR with low overpotential and high current density. The material also remains stable during the electrocatalytic reaction for long time. Its good electrocatalytic performance makes this material a promising alternative to conventional noble metal-based catalysts (e.g., Pt) that are commonly used in HzOR-based fuel cells.

关键词： copper nanoparticles     mesoporous carbon     noble metal-free electrocatalyst     hydrazine oxidation reaction     polyaniline    

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Cystine-assisted accumulation of gold nanoparticles on ZnO to construct a sensitive surface-enhanced

《化学科学与工程前沿（英文）》 2023年 第17卷 第1期   页码 15-23 doi: 10.1007/s11705-022-2177-8

摘要： Recently, various semiconductor/metal composites have been developed to fabricate surface-enhanced Raman spectroscopy substrates. However, low metal loading on semiconductors is still a challenge. In this study, cystine was introduced to increase the accumulation of gold nanoparticles on zinc oxide, owing to the biomineralization property of cystine. Morphological analysis revealed that the obtained ZnO/Au/cystine composite not only had a higher metal loading but also formed a porous structure, which is beneficial for Raman performance. Compared with ZnO/Au, the ZnO/Au/cystine substrate displayed a 40-fold enhancement in the Raman signal and a lower limit of detection (10–11 mol·L−1) in the detection of rhodamine 6G. Moreover, the substrate has favorable homogeneity and stability. Finally, ZnO/Au/cystine displayed excellent performance toward crystal violet and methylene blue in a test based on river water samples. This study provided a promising method to fabricate sensitive semiconductor/noble metal-based surface-enhanced Raman spectroscopy substrates for Raman detection.

关键词： biomineralization     cystine     semiconductor/metal composite     SERS detection     Raman detection    

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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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Micro-sized hydrothermal carbon supporting metal oxide nanoparticles as efficient catalyst for mono-dehydration

Cheng PAN, Chao FAN, Wanqin WANG, Teng LONG, Benhua HUANG, Donghua ZHANG, Peigen SU, Aqun ZHENG, Yang SUN

《能源前沿（英文）》 2022年 第16卷 第5期   页码 822-839 doi: 10.1007/s11708-020-0677-0

摘要： Most known catalytic dehydration of sugar alcohols such as D-sorbitol and D-mannitol can only produce di-dehydrated forms as major product, but mono-dehydrated products are also useful chemicals. Moreover, both di- and mono-dehydration demand a high temperature (150°C or higher), which deserves further attentions. To improve the mono-dehydration efficiency, a series of metal-containing hydrothermal carbonaceous materials (HTC) are prepared as catalyst in this work. Characterization reveals that the composition of preparative solution has a key influence on the morphology of HTC. In transformation of D-sorbitol, all HTC catalysts show low conversions in water regardless of temperature, but much better outputs are obtained in ethanol, especially at a higher temperature. When D-mannitol is selected as substrate, moderate to high conversions are obtained in both water and ethanol. On the other hand, high mono-dehydration selectivity is obtained for both sugar alcohols by using all catalysts. The origin of mono-dehydration selectivity and role of carbon component in catalysis are discussed in association with calculations. This study provides an efficient, mild, eco-friendly, and cost-effective system for mono-dehydration of sugar alcohols, which means a lot to development in new detergents or other fine chemicals.

关键词： hydrothermal carbon     morphology     catalyst     mono-dehydration     sugar alcohol    

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

《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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Sulfur-deficient CoNi2S4 nanoparticles-anchored porous carbon nanofibers as bifunctional

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1707-1717 doi: 10.1007/s11705-023-2308-x

摘要： Water electrolysis technology is considered to be one of the most promising means to produce hydrogen. Herein, aiming at the problems of high overpotential and slow kinetics in water splitting, N-doped porous carbon nanofibers-coupled CoNi2S4 nanoparticles are prepared as bifunctional electrocatalyst. In the strategy, NaCl is used as the template to prepare porous carbon nanofibers with a large surface area, and sulfur vacancies are created to modulate the electronic structure of CoNi2S4. Electron spin resonance confirms the formation of abundant sulfur vacancies, which largely reduce the bandgap of CoNi2S4 from 1.68 to 0.52 eV. The narrowed bandgap is conducive to the migration of valence electrons and decreases the charge transfer resistance for electrocatalytic reaction. Moreover, the uniform distribution of CoNi2S4 nanoparticles on carbon nanofibers can prevent the aggregation and facilitate the exposure of electrochemical active sites. Therefore, the composite catalyst exhibits low overpotentials of 340 mV@100 mA·cm–2 for oxygen evolution reaction and 380 mV@100 mA·cm–2 for hydrogen evolution reaction. The assembled electrolyzer requires 1.64 V to achieve 10 mA·cm–2 for overall water-splitting with good long-term stability. The excellent performance results from the synergistic effect of porous structures, sulfur deficiency, nitrogen doping, and the well-dispersed active component.

关键词： nanoparticle     sulfur vacancy     porous carbon nanofiber     transition metal sulfides     electrolysis    

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SERS nanoprobes for bio-application

Han-Wen Cheng,Jin Luo,Chuan-Jian Zhong

《化学科学与工程前沿（英文）》 2015年 第9卷 第4期   页码 428-441 doi: 10.1007/s11705-015-1536-0

摘要： The ability to tune the size, shape, composition and surface properties impart nanoparticles with the desired functions for bio-application. This article highlights some of the recent examples in the exploration of metal (e.g., gold and silver) nanoparticles, especially those with magnetic properties and bio-conjugated structures, as theranostic nanoprobes. Such nanoprobes exhibit tunable optical, spectroscopic, magnetic, and electrical properties for signal amplifications. Examples discussed in this article will focus on the nanoproble-enhanced colorimetric detection and surface enhanced Raman scattering (SERS) detection of biomarkers or biomolecules such as proteins and DNAs. The understanding of factors controlling the biomolecular interactions is essential for the design of SERS nanoprobes with theranostic functions.

关键词： surface-enhanced Raman scattering     functional nanoprobes     bio-conjugation     metal nanoparticles     magnetic properties     theranostic materials    

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标题 作者 时间 类型 操作

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

期刊论文

Catalytic activity of noble metal nanoparticles toward hydrodechlorination: influence of catalyst electronic

Man ZHANG,Feng HE,Dongye ZHAO

期刊论文

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

期刊论文

Recent advances in gold-metal oxide core-shell nanoparticles: Synthesis, characterization, and their

Michelle Lukosi,Huiyuan Zhu,Sheng Dai

期刊论文

Nexus between polymer support and metal oxide nanoparticles in hybrid nanosorbent materials (HNMs) for

Ryan C. SMITH,Jinze LI,Surapol PADUNGTHON,Arup K. SENGUPTA

期刊论文

Influence of surface modified mixed metal oxide nanoparticles on the electrochemical and mechanical properties

期刊论文

(Super)paramagnetic nanoparticles as platform materials for environmental applications: From synthesis

Wenlu Li, John D. Fortner

期刊论文

Application of metal oxides-based nanofluids in PV/T systems: a review

期刊论文

Copper nanoparticles/polyaniline-derived mesoporous carbon electrocatalysts for hydrazine oxidation

Tao Zhang, Tewodros Asefa

期刊论文

Cystine-assisted accumulation of gold nanoparticles on ZnO to construct a sensitive surface-enhanced

期刊论文

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

期刊论文

Micro-sized hydrothermal carbon supporting metal oxide nanoparticles as efficient catalyst for mono-dehydration

Cheng PAN, Chao FAN, Wanqin WANG, Teng LONG, Benhua HUANG, Donghua ZHANG, Peigen SU, Aqun ZHENG, Yang SUN

期刊论文

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

期刊论文

Sulfur-deficient CoNi2S4 nanoparticles-anchored porous carbon nanofibers as bifunctional

期刊论文

SERS nanoprobes for bio-application

Han-Wen Cheng,Jin Luo,Chuan-Jian Zhong

期刊论文