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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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Hollow carbon spheres and their noble metal-free hybrids in catalysis

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1380-1407 doi: 10.1007/s11705-021-2097-z

摘要： Hollow carbon spheres have garnered great interest owing to their high surface area, large surface-to-volume ratio and reduced transmission lengths. Herein, we overview hollow carbon sphere-based materials and their noble metal-free hybrids in catalysis. Firstly, we summarize the key fabrication techniques for various kinds of hollow carbon spheres, with a particular emphasis on controlling pore structure and surface morphology, and then heterogeneous doping as well as their metal-free/containing hybrids are presented; next, possible applications for non-noble metal/hollow carbon sphere hybrids in the area of energy-related catalysis, including oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, water splitting, rechargeable Zn-air batteries and pollutant degradation are discussed; finally, we introduce the various challenges and opportunities offered by hollow carbon spheres from the perspective of synthesis and catalysis.

关键词： hollow carbon spheres     functionalization     noble metal-free     catalysis    

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Shape/size controlling syntheses, properties and applications of two-dimensional noble metal nanocrystals

Baozhen An,Mingjie Li,Jialin Wang,Chaoxu Li

《化学科学与工程前沿（英文）》 2016年 第10卷 第3期   页码 360-382 doi: 10.1007/s11705-016-1576-0

摘要： Two dimensional (2D) nanocrystals of noble metals (e.g., Au, Ag, Pt) often have unique structural and environmental properties which make them useful for applications in electronics, optics, sensors and biomedicines. In recent years, there has been a focus on discovering the fundamental mechanisms which govern the synthesis of the diverse geometries of these 2D metal nanocrystals (e.g., shapes, thickness, and lateral sizes). This has resulted in being able to better control the properties of these 2D structures for specific applications. In this review, a brief historical survey of the intrinsic anisotropic properties and quantum size effects of 2D noble metal nanocrystals is given and then a summary of synthetic approaches to control their shapes and sizes is presented. The unique properties and fascinating applications of these nanocrystals are also discussed.

关键词： two-dimension     noble metal     nanocrystal     surface plasmon     controllable synthesis    

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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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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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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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Zinc modification of Ni-Ti as efficient NiZnTi catalysts with both geometric and electronic improvements for hydrogenation of nitroaromatics

《化学科学与工程前沿（英文）》 2022年 第16卷 第4期   页码 461-474 doi: 10.1007/s11705-021-2072-8

摘要： The catalytic hydrogenation of nitroaromatics is an environmentally friendly technology for aniline production, and it is crucial to develop noble-metal-free catalysts that can achieve chemoselective hydrogenation of nitroaromatics under mild reaction conditions. In this work, zinc-modified Ni-Ti catalysts (NixZnyTi1) were fabricated and applied for the hydrogenation of nitroaromatics hydrogenation. It was found that the introduction of zinc effectively increases the surface Ni density, enhances the electronic effect, and improves the interaction between Ni and TiO2, resulting in smaller Ni particle size, more oxygen vacancies, higher dispersion and greater concentration of Ni on the catalyst surface. Furthermore, the electron-rich Niδ– obtained by electron transfer from Zn and Ti to Ni effectively adsorbs and dissociates hydrogen. The results reveal that NixZnyTi1 (Ni0.5Zn0.5Ti1) shows excellent catalytic performance under mild conditions (70 °C and 6 bar). These findings provide a rational strategy for the development of highly active non-noble-metal hydrogenation catalysts.

关键词： bimetal strategy     oxygen vacancy     non-noble metal catalyst     hydrogenation     aromatic nitro compounds    

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Noble-metal-free cobalt hydroxide nanosheets for efficient electrocatalytic oxidation

Jie Lan, Daizong Qi, Jie Song, Peng Liu, Yi Liu, Yun-Xiang Pan

《化学科学与工程前沿（英文）》 2020年 第14卷 第6期   页码 948-955 doi: 10.1007/s11705-020-1920-2

摘要： Cobalt hydroxide has been emerging as a promising catalyst for the electrocatalytic oxidation reactions, including the oxygen evolution reaction (OER) and glucose oxidation reaction (GOR). Herein, we prepared cobalt hydroxide nanoparticles (CoHP) and cobalt hydroxide nanosheets (CoHS) on nickel foam. In the electrocatalytic OER, CoHS shows an overpotential of 306 mV at a current density of 10 mA·cm . This is enhanced as compared with that of CoHP (367 mV at 10 mA·cm ). In addition, CoHS also exhibits an improved performance in the electrocatalytic GOR. The improved electrocatalytic performance of CoHS could be due to the higher ability of the two-dimensional nanosheets on CoHS in electron transfer. These results are useful for fabricating efficient catalysts for electrocatalytic oxidation reactions.

关键词： electrocatalytic oxidation     cobalt hydroxide     nanosheet     water     glucose    

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Fischer-Tropsch synthesis by reduced graphene oxide nanosheets supported cobalt catalysts: Role of support and metalnanoparticle size on catalyst activity and products selectivity

Hasan Oliaei Torshizi, Ali Nakhaei Pour, Ali Mohammadi, Yahya Zamani, Seyed Mehdi Kamali Shahri

《化学科学与工程前沿（英文）》 2021年 第15卷 第2期   页码 299-309 doi: 10.1007/s11705-020-1925-x

摘要： In this paper, a series of cobalt catalysts supported on reduced graphene oxide (rGO) nanosheets with the loading of 5, 15 and 30 wt-% were provided by the impregnation method. The activity of the prepared catalysts is evaluated in the Fischer-Tropsch synthesis (FTS). The prepared catalysts were carefully characterized by nitrogen adsorption-desorption, hydrogen chemisorption, X-ray diffraction, Fourier transform infrared spectroscopy, Raman spectroscopy, temperature programmed reduction, transmission electron microscopy, and field emission scanning electron microscopy techniques to confirm that cobalt particles were greatly dispersed on the rGO nanosheets. The results showed that with increasing the cobalt loading on the rGO support, the carbon defects are increased and as a consequence, the reduction of cobalt is decreased. The FTS activity results showed that the cobalt-time yield and turnover frequency passed from a maximum for catalyst with the Co average particle size of 15 nm due to the synergetic effect of cobalt reducibility and particle size. The products selectivity results indicated that the methane selectivity decreases, whereas the C selectivity raises with the increasing of the cobalt particle size, which can be explained by chain propagation in the primary chain growth reactions.

关键词： cobalt catalyst     cobalt particle size     Fischer-Tropsch synthesis     reduced graphene oxide     supported catalyst    

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Hydro-pyrolysis of lignocellulosic biomass over alumina supported Platinum, Mo

Songbo He, Jeffrey Boom, Rolf van der Gaast, K. Seshan

《化学科学与工程前沿（英文）》 2018年 第12卷 第1期   页码 155-161 doi: 10.1007/s11705-017-1655-x

摘要： In-line hydro-treatment of bio-oil vapor from fast pyrolysis of lignocellulosic biomass (hydro-pyrolysis of biomass) is studied as a method of upgrading the liquefied bio-oil for a possible precursor to green fuels. The nobel metal (Pt) and non-noble metal catalysts (Mo C and WC) were compared at 500 °C and atmospheric pressure which are same as the reaction conditions for fast pyrolysis of biomass. Results indicated that under the pyrolysis conditions, the major components, such as acids and carbonyls, of the fast pyrolysis bio-oil can be completely and partially hydrogenated to form hydrocarbons, an ideal fossil fuel blend, in the hydro-treated bio-oil. The carbide catalysts perform equally well as the Pt catalyst regarding to the aliphatic and aromatic hydrocarbon formation (ca. 60%), showing the feasibility of using the cheap non-noble catalysts for hydro-pyrolysis of biomass.

关键词： bio-oil     pyrolysis     hydro-deoxygenation (HDO)     non-noble metal catalysts     hydro-treatment    

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高压下铜-氢化合物体系的结构研究 Article

Jack Binns, Miriam Peña-Alvarez, Mary-Ellen Donnelly, Eugene Gregoryanz,Ross T. Howie, Philip Dalladay-Simpson

《工程（英文）》 2019年 第5卷 第3期   页码 505-509 doi: 10.1016/j.eng.2019.03.001

摘要：

理论和实验研究都表明，极端高压条件下氢气和众多金属或非金属所构成的二元体系化合物的物理性质显著增强，这使得含氢二元体系成为高压科学领域的重要研究对象。尽管氢气的化学性质活泼，但一些贵金属（如铜、银、金）依旧很难在常温常压下与氢气反应生成相应的金属氢化物，截至目前，没有任何贵金属与氢的摩尔比大于1的稳定化合物被报道。在本研究中，我们通过结合原位激光加热，在金刚石对顶砧压腔中通过氢气和金属铜单质反应成功合成了铜-氢二元化合物。通过对X射线衍射数据进行分析，我们探究了从常压到最高50 GPa压力范围内铜-氢体系的相行为和稳定性。该实验证实了前期理论预测的三个铜-氢化合物相：γ0-CuH0.15、γ1-CuH0.5和ε-Cu2H。更值得一提的是，该研究还通过对金刚石对顶砧腔体内部样品进行激光加热，合成了目前已知的室温下最高氢含量和稳定性的贵金属氢化物γ2-CuH0.65。该项研究加深了人们对于过渡金属-氢化合物体系的认知，同时，通过该实验合成的氢化物由于具有很高的含氢量，有望被设计成理想的储氢材料。

关键词： 高压     储氢材料     贵金属化学    

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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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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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Sulfur-deficient CoNi2S4 nanoparticles-anchored porous carbon nanofibers as bifunctional electrocatalyst for overall water splitting

《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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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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标题 作者 时间 类型 操作

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

期刊论文

Hollow carbon spheres and their noble metal-free hybrids in catalysis

期刊论文

Shape/size controlling syntheses, properties and applications of two-dimensional noble metal nanocrystals

Baozhen An,Mingjie Li,Jialin Wang,Chaoxu Li

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

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

Tao Zhang, Tewodros Asefa

期刊论文

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

期刊论文

Zinc modification of Ni-Ti as efficient NiZnTi catalysts with both geometric and electronic improvements for hydrogenation of nitroaromatics

期刊论文

Noble-metal-free cobalt hydroxide nanosheets for efficient electrocatalytic oxidation

Jie Lan, Daizong Qi, Jie Song, Peng Liu, Yi Liu, Yun-Xiang Pan

期刊论文

Fischer-Tropsch synthesis by reduced graphene oxide nanosheets supported cobalt catalysts: Role of support and metalnanoparticle size on catalyst activity and products selectivity

Hasan Oliaei Torshizi, Ali Nakhaei Pour, Ali Mohammadi, Yahya Zamani, Seyed Mehdi Kamali Shahri

期刊论文

Hydro-pyrolysis of lignocellulosic biomass over alumina supported Platinum, Mo

Songbo He, Jeffrey Boom, Rolf van der Gaast, K. Seshan

期刊论文

高压下铜-氢化合物体系的结构研究

Jack Binns, Miriam Peña-Alvarez, Mary-Ellen Donnelly, Eugene Gregoryanz,Ross T. Howie, Philip Dalladay-Simpson

期刊论文

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

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

Sulfur-deficient CoNi2S4 nanoparticles-anchored porous carbon nanofibers as bifunctional electrocatalyst for overall water splitting

期刊论文

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

期刊论文