Development of Continuous Apparatus using Microreactor for Production of Nanoparticles in Supercritical Water

超临界水中微反应器连续生产纳米颗粒装置的开发

• 批准号: 15360416
• 负责人: ARAI Kunio
• 金额: $ 9.28万
• 依托单位: Tohoku University
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (B)
• 财政年份: 2003
• 资助国家: 日本
• 起止时间: 2003 至 2005
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-15360416/
• 关键词: Supercritical water; Hydrothermal synthesis; Metal Oxides; Nanoparticles; Microreactor; Solubility; Flow-through apparatus; ナノサイズ微粒子

Over the past ten years, a flow-through hydrothermal synthesis method with microreactor for continuous production of metal oxides have been established for forming micro or nano size metal oxide fine particles in subcritical and supercritical water. This method promises to heat starting solutions rapidly to the given temperature and to control reaction time exactly. When water in its near-critical or supercritical state is used, the hydrothermal reaction rate and metal oxide solubility can be controlled by changing temperature and pressure since the reaction solvent properties are strongly dependent on the conditions in these regions. Therefore, this method has great potential for producing nano-size metal oxide fine particles. There are many reports for producing nanoparticle by this method. However, there is no report that the controllability of the particle size is discussed on the basis of metal oxide solubility and supersaturation. In this work, to develop this method as a generic … More technology for producing nanocrystals we focus on the quantitative clarification of experimental conditions for producing single nano-sized metal oxide particles by this method and also its crystallinity on the basis of estimated metal oxide solubilities.We carried out hydrothermal synthesis of metal oxides (AlO(OH), CuO, Fe2O3, NiO, ZrO2) nanoparticles from metal nitrates aqueous solution at 673 K and 30 MPa by this method. Particle size, phase and crystallinity of the obtained particles were characterized by TEM, XRD and TG, respectively. Effect of the difference of the metals in starting materials on particle size, conversion and crystallinity was analyzed on the basis of supersaturation, which was evaluated by estimated metal oxide solubilities. The result suggests that supersaturation should be set to higher than 104 in this method to obtain particles in single nanoscale. Further, crystallinity of the obtained particles was evaluated as weight loss through TG analysis. In addition that longer reaction time increased the crystallinity, it was found that smaller supersaturation also increased the crystallinity. This result can be explained that large supersaturation lead to include water molecule on the way to formation of particles. Less

在过去的十年中，已经建立了用于连续生产金属氧化物的具有微反应器的流通式水热合成方法，用于在亚临界和超临界水中形成微米或纳米尺寸的金属氧化物细颗粒。该方法保证了快速加热起始溶液到给定温度，并精确控制反应时间。当使用处于其近临界或超临界状态的水时，水热反应速率和金属氧化物溶解度可以通过改变温度和压力来控制，因为反应溶剂性质强烈地依赖于这些区域中的条件。因此，该方法具有制备纳米尺寸金属氧化物细颗粒的巨大潜力。用这种方法制备纳米粒子已有许多报道。然而，没有报道基于金属氧化物溶解度和过饱和度来讨论粒度的可控性。在这项工作中，开发这种方法作为一个通用的 ...更多信息 在此基础上，利用水热法在673 K、30 MPa条件下从金属硝酸盐水溶液中合成了AlO（OH）、CuO、Fe_2O_3、NiO、ZrO_2等金属氧化物纳米粒子。采用TEM、XRD和TG等手段对产物的粒径、物相和结晶度进行了表征。在过饱和度的基础上分析了起始原料中金属的差异对粒径、转化率和结晶度的影响，所述过饱和度通过估计的金属氧化物溶解度来评估。结果表明，在该方法中，过饱和度应设置为高于104，以获得单一纳米级的颗粒。此外，通过TG分析评价所得颗粒的结晶性作为重量损失。此外，较长的反应时间增加结晶度，它被发现，较小的过饱和度也增加结晶度。这一结果可以解释为大的过饱和度导致在颗粒形成的过程中包含水分子。少

项目成果

流通式超臨界水熱合成法によるナノ粒子設計

使用流通式超临界水热合成法设计纳米粒子

• 发表时间: 2005
• 期刊: Journal of the Society of Inorganic Materials, Japan 12
• 作者: H.Uchida;Y.Kojima;M.Matsuoka;Masayoshi Mizutani;水谷 正義;水谷 正義;Masayoshi Mizutani;Kiwamu Sue;陶究
• 通讯作者: 陶究

Design of Nanoparticles in Supercritical Water using Flow-through Hydrothermal Synthesis Method

采用流通式水热合成法设计超临界水中的纳米颗粒

• 发表时间: 2005
• 期刊: Journal of the Society of Inorganic Materials, Japan 12
• 作者: Kiwamu Sue;Kiwamu Sue;Kiwamu Sue;陶 究;Kiwamu Sue;Kiwamu Sue
• 通讯作者: Kiwamu Sue

Continuous production of nickel fine particles by hydrogen reduction in near-critical water

近临界水中氢还原连续生产镍细颗粒

• 发表时间: 2004
• 期刊: Industrial and Engineering Chemistry Research 43・9
• 作者: Y.Yamasaki;A.Kariyasaki;A.Ousaka;S.Morooka;Kiwamu Sue
• 通讯作者: Kiwamu Sue

Kiwamu Sue: "Continuous production of nickel fine particles by hydrogen reduction in near-critical water"Industrial and Engineering Chemistry Research. (accepted). (2004)

Kiwamu Sue：“在近临界水中通过氢还原连续生产镍细颗粒”工业与工程化学研究。

Hydrothermal synthesis of zinc oxide crystals in homogeneous mixture of carbon dioxide, hydrogen, and water

在二氧化碳、氢气和水的均匀混合物中水热合成氧化锌晶体

• 发表时间: 2004
• 期刊: Chemistry Letters 33・6
• 作者: Kiwamu Sue;Kiwamu Sue;Kiwamu Sue;陶 究;Kiwamu Sue;Kiwamu Sue;Kiwamu Sue;Kiwamu Sue;Kiwamu Sue;Kiwamu Sue
• 通讯作者: Kiwamu Sue