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Scaling up of cluster beam deposition technology for catalysis application

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1360-1379 doi: 10.1007/s11705-021-2101-7

摘要： Many research works have demonstrated that the combination of atomically precise cluster deposition and theoretical calculations is able to address fundamental aspects of size-effects, cluster-support interactions, and reaction mechanisms of cluster materials. Although the wet chemistry method has been widely used to synthesize nanoparticles, the gas-phase synthesis and size-selected strategy was the only method to prepare supported metal clusters with precise numbers of atoms for a long time. However, the low throughput of the physical synthesis method has severely constrained its wider adoption for catalysis applications. In this review, we introduce the latest progress on three types of cluster source which have the most promising potential for scale-up, including sputtering gas aggregation source, pulsed microplasma cluster source, and matrix assembly cluster source. While the sputtering gas aggregation source is leading ahead with a production rate of ~20 mg·h–1, the pulsed microplasma source has the smallest physical dimensions which makes it possible to compact multiple such devices into a small volume for multiplied production rate. The matrix assembly source has the shortest development history, but already show an impressive deposition rate of ~10 mg·h–1. At the end of the review, the possible routes for further throughput scale-up are envisaged.

关键词： nanoparticle     cluster     cluster beam deposition     magnetron sputtering     heterogeneous catalysis    

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The energy-environment nexus: aerosol science and technology enabling solutions

Pratim BISWAS, Wei-Ning WANG, Woo-Jin AN

《环境科学与工程前沿（英文）》 2011年 第5卷 第3期   页码 299-312 doi: 10.1007/s11783-011-0351-1

摘要： Energy issues are important and consumption is slated to increase across the globe in the future. The energy-environment nexus is very important as strategies to meet future energy demand are developed. To ensure sustainable growth and development, it is essential that energy production is environmentally benign. There are two temporal issues—one that is immediate, and needs to address the environmental compliance of energy generation from fossil fuel sources; and second that is the need to develop newer alternate and more sustainable approaches in the future. Aerosol science and technology is an enabling discipline that addresses the energy issue over both these time scales. The paper is a review of aspects of aerosol science and engineering that helps address carbon neutrality of fossil fuels. Advanced materials to meet these challenges are discussed. Future approaches to effective harvesting of sunlight that are enabled by aerosol studies are discussed.

关键词： energy-environment nexus     aerosol science and technology     fossil fuels     carbon dioxide conversion     solar energy     nanoparticle technology    

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Performance of iron-air battery with iron nanoparticle-encapsulated C–N composite electrode

《能源前沿（英文）》 doi: 10.1007/s11708-023-0913-5

摘要： Highly efficient and stable iron electrodes are of great significant to the development of iron-air battery (IAB). In this paper, iron nanoparticle-encapsulated C–N composite (NanoFe@CN) was synthesized by pyrolysis using polyaniline as the C–N source. Electrochemical performance of the NanoFe@CN in different electrolytes (alkaline, neutral, and quasi-neutral) was investigated via cyclic voltammetry (CV). The IAB was assembled with NanoFe@CN as the anode and IrO2 + Pt/C as the cathode. The effects of different discharging/charging current densities and electrolytes on the battery performance were also studied. Neutral K2SO4 electrolyte can effectively suppress the passivation of iron electrode, and the battery showed a good cycling stability during 180 charging/discharging cycles. Compared to the pure nano-iron (NanoFe) battery, the NanoFe@CN battery has a more stable cycling stability either in KOH or NH4Cl + KCl electrolyte.

关键词： energy storage and conversion     metallic composites     nanocomposites     iron-air battery     iron anode    

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Effect of noble metal nanoparticle size on C–N bond cleavage performance in hydrodenitrogenation: a study

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 1986-2000 doi: 10.1007/s11705-023-2337-5

摘要： Breakage of the C–N bond is a structure sensitive process, and the catalyst size significantly affects its activity. On the active metal nanoparticle scale, the role of catalyst size in C–N bond cleavage has not been clearly elucidated. So, Ru catalysts with variable nanoparticle sizes were obtained by modulating the reduction temperature, and the catalytic activity was evaluated using 1,2,3,4-tetrahydroquinoline and o-propylaniline with different C–N bond hybridization patterns as reactants. Results showed a 13 times higher reaction rate for sp3-hybridized C–N bond cleavage than sp2-hybridized C–N bond cleavage, while the reaction rate tended to increase first and then decrease as the catalyst nanoparticle size increased. Different concentrations of terrace, step, and corner sites were found in different sizes of Ru nanoparticles. The relationship between catalytic site variation and C–N bond cleavage activity was further investigated by calculating the turnover frequency values for each site. This analysis indicates that the variation of different sites on the catalyst is the intrinsic factor of the size dependence of C–N bond cleavage activity, and the step atoms are the active sites for the C–N bond cleavage. When Ru nanoparticles are smaller than 1.9 nm, they have a strong adsorption effect on the reactants, which will affect the catalytic performance of the Ru catalyst. Furthermore, these findings were also confirmed on other metallic Pd/Pt catalysts. The role of step sites in C–N bond cleavage was proposed using the density function theory calculations. The reactants have stronger adsorption energies on the step atoms, and step atoms have d-band center nearer to the Fermi level. In this case, the interaction with the reactant is stronger, which is beneficial for activating the C–N bond of the reactant.

关键词： sp3/sp2-hybridized C–N bond     noble metal nanoparticle     catalytic active site     turnover frequency     DFT    

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Iron oxide nanoparticle-based theranostics for cancer imaging and therapy

Xiaoqing REN,Hongwei CHEN,Victor YANG,Duxin SUN

《化学科学与工程前沿（英文）》 2014年 第8卷 第3期   页码 253-264 doi: 10.1007/s11705-014-1425-y

摘要： Theranostic platform, which is equipped with both diagnostic and therapeutic functions, is a promising approach in cancer treatment. From various nanotheranostics studied, iron oxide nanoparticles have advantages since IONPs have good biocompatibility and spatial imaging capability. This review is focused on the IONP-based nanotheranostics for cancer imaging and treatment. The most recent progress for applications of IONP nanotheranostics is summarized, which includes IONP-based diagnosis, magnetic resonance imaging (MRI), multimodal imaging, chemotherapy, hyperthermal therapy, photodynamic therapy, and gene delivery. Future perspectives and challenges are also outlined for the potential development of IONP based theranostics in clinical use.

关键词： theranostics     iron oxide nanoparticles     MRI     drug delivery     photothermal therapy     photodynamic therapy    

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Nanoparticle-enhanced coolants in machining: mechanism, application, and prospects

《机械工程前沿（英文）》 2023年 第18卷 第4期 doi: 10.1007/s11465-023-0769-8

摘要： Nanoparticle-enhanced coolants (NPECs) are increasingly used in minimum quantity lubrication (MQL) machining as a green lubricant to replace conventional cutting fluids to meet the urgent need for carbon emissions and achieve sustainable manufacturing. However, the thermophysical properties of NPEC during processing remain unclear, making it difficult to provide precise guidance and selection principles for industrial applications. Therefore, this paper reviews the action mechanism, processing properties, and future development directions of NPEC. First, the laws of influence of nano-enhanced phases and base fluids on the processing performance are revealed, and the dispersion stabilization mechanism of NPEC in the preparation process is elaborated. Then, the unique molecular structure and physical properties of NPECs are combined to elucidate their unique mechanisms of heat transfer, penetration, and anti-friction effects. Furthermore, the effect of NPECs is investigated on the basis of their excellent lubricating and cooling properties by comprehensively and quantitatively evaluating the material removal characteristics during machining in turning, milling, and grinding applications. Results showed that turning of Ti‒6Al‒4V with multi-walled carbon nanotube NPECs with a volume fraction of 0.2% resulted in a 34% reduction in tool wear, an average decrease in cutting force of 28%, and a 7% decrease in surface roughness Ra, compared with the conventional flood process. Finally, research gaps and future directions for further applications of NPECs in the industry are presented.

关键词： nanoparticle-enhanced coolant     minimum quantity lubrication     biolubricant     thermophysical properties     turning     milling     grinding    

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Cobalt nanoparticle decorated N-doped carbons derived from a cobalt covalent organic framework for oxygen

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1550-1560 doi: 10.1007/s11705-021-2104-4

摘要： The low cost and highly efficient construction of electrocatalysts has attracted significant attention owing to the use of clean and sustainable energy technologies. In this work, cobalt nanoparticle decorated N-doped carbons (Co@NC) are synthesized by the pyrolysis of a cobalt covalent organic framework under an inert atmosphere. The Co@NC demonstrates improved electrocatalytic capabilities compared to N-doped carbon without the addition of Co nanoparticles, indicating the important role of cobalt. The well-dispersed active sites (Co-Nx) and the synergistic effect between the carbon matrix and Co nanoparticles greatly enhance the electrocatalytic activity for the oxygen reduction reaction. In addition, the Co content has a significant effect on the catalytic activity. The resulting Co@NC-0.86 exhibits a superb electrocatalytic activity for the oxygen reduction reaction in an alkaline electrolyte in terms of the onset potential (0.90 V), half-wave potential (0.80 V) and the limiting current density (4.84 mA·cm–2), and a high selectivity, as well as a strong methanol tolerance and superior durability, these results are comparable to those of the Pt/C catalyst. Furthermore, the superior bifunctional activity of Co@NC-0.86 was also confirmed in a home-built Zn-air battery, signifying the possibility for application in electrode materials and in current energy conversion and storage devices.

关键词： cobalt embedment     N-doped carbons     covalent organic framework     oxygen reduction     Zn-air battery    

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Cobalt-nanoparticle catalysts derived from zeolitic imidazolate framework@MXene composites for efficient

《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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A review on the application of nanofluids in enhanced oil recovery

《化学科学与工程前沿（英文）》 2022年 第16卷 第8期   页码 1165-1197 doi: 10.1007/s11705-021-2120-4

摘要： Enhanced oil recovery (EOR) has been widely used to recover residual oil after the primary or secondary oil recovery processes. Compared to conventional methods, chemical EOR has demonstrated high oil recovery and low operational costs. Nanofluids have received extensive attention owing to their advantages of low cost, high oil recovery, and wide applicability. In recent years, nanofluids have been widely used in EOR processes. Moreover, several studies have focused on the role of nanofluids in the nanofluid EOR (N-EOR) process. However, the mechanisms related to N-EOR are unclear, and several of the mechanisms established are chaotic and contradictory. This review was conducted by considering heavy oil molecules/particle/surface micromechanics; nanofluid-assisted EOR methods; multiscale, multiphase pore/core displacement experiments; and multiphase flow fluid-solid coupling simulations. Nanofluids can alter the wettability of minerals (particle/surface micromechanics), oil/water interfacial tension (heavy oil molecules/water micromechanics), and structural disjoining pressure (heavy oil molecules/particle/surface micromechanics). They can also cause viscosity reduction (micromechanics of heavy oil molecules). Nanofoam technology, nanoemulsion technology, and injected fluids were used during the EOR process. The mechanism of N-EOR is based on the nanoparticle adsorption effect. Nanoparticles can be adsorbed on mineral surfaces and alter the wettability of minerals from oil-wet to water-wet conditions. Nanoparticles can also be adsorbed on the oil/water surface, which alters the oil/water interfacial tension, resulting in the formation of emulsions. Asphaltenes are also adsorbed on the surface of nanoparticles, which reduces the asphaltene content in heavy oil, resulting in a decrease in the viscosity of oil, which helps in oil recovery. In previous studies, most researchers only focused on the results, and the nanoparticle adsorption properties have been ignored. This review presents the relationship between the adsorption properties of nanoparticles and the N-EOR mechanisms. The nanofluid behaviour during a multiphase core displacement process is also discussed, and the corresponding simulation is analysed. Finally, potential mechanisms and future directions of N-EOR are proposed. The findings of this study can further the understanding of N-EOR mechanisms from the perspective of heavy oil molecules/particle/surface micromechanics, as well as clarify the role of nanofluids in multiphase core displacement experiments and simulations. This review also presents limitations and bottlenecks, guiding researchers to develop methods to synthesise novel nanoparticles and conduct further research.

关键词： nanofluid     EOR mechanism     nanoparticle adsorption     interface property     internal property    

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Floret-like Fe–N nanoparticle-embedded porous carbon superstructures from a Fe-covalent triazine polymer

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 525-535 doi: 10.1007/s11705-022-2232-5

摘要： Fe–Nx nanoparticles-embedded porous carbons with a desirable superstructure have attracted immense attention as promising catalysts for electrochemical oxygen reduction reaction. Herein, we employed Fe-coordinated covalent triazine polymer for the fabrication of Fe–Nx nanoparticle-embedded porous carbon nanoflorets (Fe/N@CNFs) employing a hypersaline-confinement-conversion strategy. Presence of tailored N types within the covalent triazine polymer interwork in high proportions contributes to the generation of Fe/N coordination and subsequent Fe–Nx nanoparticles. Owing to the utilization of NaCl crystals, the resultant Fe/N@CNF-800 which was generated by pyrolysis at 800 °C showed nanoflower structure and large specific surface area, which remarkably suppressed the agglomeration of high catalytic active sites. As expect, the Fe/N@CNF-800 exhibited unexpected oxygen reduction reaction catalytic performance with an ultrahigh half-wave potential (0.89 V vs. reversible hydrogen electrode), a dominant 4e– transfer approach and great cycle stability (> 92% after 100000 s). As a demonstration, the Fe/N-PCNF-800-assembled zinc–air battery delivered a high open circuit voltage of 1.51 V, a maximum peak power density of 164 mW·cm–2, as well as eminent rate performance, surpassing those of commercial Pt/C. This contribution offers a valuable avenue to exploit efficient metal nanoparticles-based carbon catalysts towards energy-related electrocatalytic reactions and beyond.

关键词： Fe–Nx nanoparticles     hypersaline-confinement conversion     floret-like carbon     covalent triazine polymers     oxygen reduction reaction    

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Decoration of CdMoO micron polyhedron with Pt nanoparticle and their enhanced photocatalytic performance

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 1949-1961 doi: 10.1007/s11705-023-2360-6

摘要： This study aimed to prepare and apply a novel Pt/CdMoO4 composite photocatalyst for photocatalytic N2 fixation and tetracycline degradation. The Pt/CdMoO4 composite was subjected to comprehensive investigation on the morphology, structure, optical properties, and photoelectric chemical properties. The results demonstrate the dispersion of Pt nanoparticles on the CdMoO4 surface. Close contact between CdMoO4 and Pt was observed, resulting in the formation of a heterojunction structure at their contact region. Density functional theory calculation and Mott-Schottky analysis revealed that Pt possesses a higher work function value than CdMoO4, resulting in electron drift from CdMoO4 to Pt and the formation of a Schottky barrier. The presence of this barrier increases the separation efficiency of electron-hole pairs, thereby improving the performance of the Pt/CdMoO4 composite in photocatalysis. When exposed to simulated sunlight, the optimal Pt/CdMoO4 catalyst displayed a photocatalytic nitrogen fixation rate of 443.7 μmol·L‒1·g‒1·h‒1, which is 3.2 times higher than that of pure CdMoO4. In addition, the composite also exhibited excellent performance in tetracycline degradation, with hole and superoxide species identified as the primary reactive species. These findings offer practical insights into designing and synthesizing efficient photocatalysts for photocatalytic nitrogen fixation and antibiotics removal.

关键词： photocatalytic N2 fixation     Pt/CdMoO4     tetracycline degradation     Schottky barrier    

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A Pt-Bi bimetallic nanoparticle catalyst for direct electro-oxidation of formic acid in fuel cells

Shu-Hong LI, Yue ZHAO, Jian CHU, Wen-Wei LI, Han-Qing YU, Gang LIU, Yang-Chao TIAN

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 388-394 doi: 10.1007/s11783-012-0475-y

摘要： Direct formic acid fuel cells are a promising portable power-generating device, and the development of efficient anodic catalysts is essential for such a fuel cell. In this work Pt-Bi nanoparticles supported on micro-fabricated gold wire array substrate were synthesized using an electrochemical deposition method for formic acid oxidation in fuel cells. The surface morphology and element components of the Pt-Bi/Au nanoparticles were characterized, and the catalytic activities of the three Pt-Bi/Au nanoparticle electrodes with different Pt/Bi ratios for formic acid oxidation were evaluated. It was found that Pt Bi /Au had a much higher catalytic activity than Pt Bi /Au and Pt Bi /Au, and Pt Bi /Au exhibited a current density of 2.7 mA·cm , which was 27-times greater than that of Pt/Au. The electro-catalytic activity of the Pt-Bi/Au electrode for formic acid oxidation increased with the increasing Bi content, suggesting that it would be possible to achieve an efficient formic acid oxidation on the low Pt-loading. Therefore, the Pt-Bi/Au electrode offers a promising catalyst with a high activity for direct oxidation of formic acid in fuel cells.

关键词： catalyst     electrochemical deposition     formic acid oxidation     fuel cell     gold wire array     microfabrication    

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Dynamic changes of protein corona compositions on the surface of zinc oxide nanoparticle in cell culture

Vo-Van Giau, Yoon-Hee Park, Kyu-Hwan Shim, Sang-Wook Son, Seong-Soo A. An

《化学科学与工程前沿（英文）》 2019年 第13卷 第1期   页码 90-97 doi: 10.1007/s11705-018-1766-z

摘要：

The potential applications of nanomaterials used in nanomedicine as ingredients in drug delivery systems and in other products continue to expand. When nanomaterials are introduced into physiological environments and driven by energetics, they readily associate proteins forming a protein corona (PC) on their surface. This PC could result in an alteration of the nanomaterial’s surface characteristics, affecting their interaction with cells due to conformational changes in adsorbed protein molecules. However, our current understanding of nanobiological interactions is still very limited. Utilizing a liquid chromatography–mass spectroscopy/mass spectroscopy technology and a Cytoscape plugin (ClueGO) approach, we examined the composition of the PC for a set of zinc oxide nanoparticles (ZnONP) from cell culture media typically and further analyzed the biological interaction of identified proteins, respectively. In total, 36 and 33 common proteins were investigated as being bound to ZnONP at 5 min and 60 min, respectively. These proteins were further analyzed with ClueGO, a Cytoscape plugin, which provided gene ontology and the biological interaction processes of identified proteins. Proteins bound to the surface of nanoparticles that may modify the structure, therefore the function of the adsorbed protein could be consequently affect the complicated biological processes.

关键词： ZnONPs     nanoparticles     protein corona     ClueGO    

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Effects of iron oxide nanoparticles on phenotype and metabolite changes in hemp clones ( L.)

《环境科学与工程前沿（英文）》 2022年 第16卷 第10期 doi: 10.1007/s11783-022-1569-9

摘要：

● Fe3O4 NPs increased the biomass and chlorophyll content of hemp clones.

关键词： Fe3O4 nanoparticle     Hemp     Growth enhancement     THC     Metabolite    

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Temporal evolution of charged and neutral nanoparticle concentrations during atmospheric new particle

E. Rohan Jayaratne, Buddhi Pushpawela, Lidia Morawska

《环境科学与工程前沿（英文）》 2016年 第10卷 第5期 doi: 10.1007/s11783-016-0862-x

摘要： Over 100 new particle formation events were studied. In 50 events, charged and neutral particles were not formed at the same time. In 42 of these events the charged particles formed before the neutral particles. Their subsequent growth rates were not determined by the particle charge. The result suggests that ion induced nucleation plays a role in particle formation. Time series of nanoparticle number concentration during new particle formation (NPF) events in the urban environment of Brisbane, Australia, showed that the formation of charged particles often occurred before that of neutral particles. We monitored 241 days during the calendar year 2012 over which NPF events were observed on 108 days. We studied the times at which the charged and neutral particle concentrations in the size range 1.8–3.2 nm reached their peak values and found that they were clearly different in 50 events with the peak neutral particle concentration lagging behind the charged particle concentration during 42 of these events with a mean time lag of 24±12 min. While the charged particles were more likely to form before the neutral particles, once formed, the growth rate of the particles did not depend on their charge. While ion-induced nucleation is not the dominant mechanism of NPF in the atmosphere, our observations suggest that the presence of ions in the atmosphere plays a role that cannot be ignored.

关键词： Charged particles     Cluster ions     Secondary particles     Environmental pollution    

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标题 作者 时间 类型 操作

Scaling up of cluster beam deposition technology for catalysis application

期刊论文

The energy-environment nexus: aerosol science and technology enabling solutions

Pratim BISWAS, Wei-Ning WANG, Woo-Jin AN

期刊论文

Performance of iron-air battery with iron nanoparticle-encapsulated C–N composite electrode

期刊论文

Effect of noble metal nanoparticle size on C–N bond cleavage performance in hydrodenitrogenation: a study

期刊论文

Iron oxide nanoparticle-based theranostics for cancer imaging and therapy

Xiaoqing REN,Hongwei CHEN,Victor YANG,Duxin SUN

期刊论文

Nanoparticle-enhanced coolants in machining: mechanism, application, and prospects

期刊论文

Cobalt nanoparticle decorated N-doped carbons derived from a cobalt covalent organic framework for oxygen

期刊论文

Cobalt-nanoparticle catalysts derived from zeolitic imidazolate framework@MXene composites for efficient

期刊论文

A review on the application of nanofluids in enhanced oil recovery

期刊论文

Floret-like Fe–N nanoparticle-embedded porous carbon superstructures from a Fe-covalent triazine polymer

期刊论文

Decoration of CdMoO micron polyhedron with Pt nanoparticle and their enhanced photocatalytic performance

期刊论文

A Pt-Bi bimetallic nanoparticle catalyst for direct electro-oxidation of formic acid in fuel cells

Shu-Hong LI, Yue ZHAO, Jian CHU, Wen-Wei LI, Han-Qing YU, Gang LIU, Yang-Chao TIAN

期刊论文

Dynamic changes of protein corona compositions on the surface of zinc oxide nanoparticle in cell culture

Vo-Van Giau, Yoon-Hee Park, Kyu-Hwan Shim, Sang-Wook Son, Seong-Soo A. An

期刊论文

Effects of iron oxide nanoparticles on phenotype and metabolite changes in hemp clones ( L.)

期刊论文

Temporal evolution of charged and neutral nanoparticle concentrations during atmospheric new particle

E. Rohan Jayaratne, Buddhi Pushpawela, Lidia Morawska

期刊论文