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Solid- state reduction of silica nanoparticles via oxygen abstraction from SiO4 units by polyolefins under mechanical stressing

机译：通过机械应力下聚烯烃通过来自SiO4单元的氧抽取的硅纳米粒子的固态减少

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摘要

Metal oxides with an oxidation number lower than the highest often exhibit attractive functional properties. However, conventional chemical or thermal reduction of the stable oxides is often laborious and cannot be stopped at an appropriate level of reduction. Therefore, we here try to explore non-conventional reduction processes in a solid-state without external heating. Unique features of reduction processes of SiO2 toward suboxides, SiOx (1 x 2), were made possible by milling fumed silica nanoparticles with polyolefins (POL), i.e., polypropylene (PP) or polyethylene (PE) and a fluorine-containing one, polyvinylidene difluoride (PVDF). We mainly examined the electronic and coordination states of Si by Si2p XPS spectra and Si-29 MAS NMR, respectively. They significantly differ from a similar commercial product obtained via a thermal route. Judging from the chemical shift of Si-29 MAS NMR as a criterion of the degree of reduction of SiO2, the function of POL as a reductant is in the order PP approximate to PE PVDF. Since the present solid-state reaction is free from the formation of unstable gaseous SiO as an intermediate, the products are free from the Si component in a Q(0) state close to that of metallic Si. From these results we conclude that the present silicon suboxides obtained by co-milling silica with POL are closer to those defined as a random bonding model of SiO, than a random mixture model, the former being unachievable by a thermal process. The main mechanism of the present solid-state reduction is the oxygen abstraction from the SiO4 units by the polarized POL, with its simultaneous oxidative decomposition up to the state of carbon. The reaction process is simple and scalable so that it may offer a new affordable fabrication method of silicon suboxides.
机译：氧化数低于最高的金属氧化物通常表现出有吸引力的功能性。然而，常规的氧化物的常规化学或热还原通常艰苦，并且不能在适当的还原水平下停止。因此，我们在这里尝试在没有外部加热的情况下在固态中探索非传统的减少过程。通过用聚烯烃（POL），即聚丙烯（PP）或聚乙烯（PE）和含氟1，通过研磨气相二氧化硅纳米粒子，使得SiO 2朝向二氧化物，SiO 3，SiOx（1 x 2）的独特特征。 ，聚偏二氟化乙烯（PVDF）。我们主要通过Si2P XPS Spectra和Si-29 Mas NMR分别检查了SI的电子和协调状态。它们与通过热途径获得的类似商业产品显着不同。从Si-29 Mas NMR的化学转向判断作为SiO2的减少程度的标准，作为还原剂的POR的功能是PP近似于PE＆GT的顺序。 PVDF。由于本发明的固态反应没有形成不稳定的气态SiO作为中间体，因此产物不含Q（0）状态的Si组分，接近金属Si。从这些结果，我们得出结论，通过将二氧化硅与Pol共铣二氧化硅获得的本硅氧化硅均更越接近SiO的随机粘合模型，而前者通过热过程不可成熟。本发明的固态减少的主要机制是偏振炎的SiO4单元的氧气抽象，其同时氧化分解直至碳的状态。反应过程简单且可伸缩，使得它可以提供一种新的实惠的硅氧化硅制造方法。

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  • 来源
    《RSC Advances》 |2018年第63期|共7页
  • 作者

    Senna Mamoru; Noda Hirotaka; Xin Yunzi; Hasegawa Hiroki; Takai Chika; Shirai Takashi; Fuji Masayoshi;

  • 作者单位

    Keio Univ Fac Sci &

    Technol Yokohama Kanagawa Japan;

    Nagoya Inst Technol Adv Ceram Res Ctr Tajimi Japan;

    Nagoya Inst Technol Adv Ceram Res Ctr Tajimi Japan;

    Nagoya Inst Technol Adv Ceram Res Ctr Tajimi Japan;

    Nagoya Inst Technol Adv Ceram Res Ctr Tajimi Japan;

    Nagoya Inst Technol Adv Ceram Res Ctr Tajimi Japan;

    Nagoya Inst Technol Adv Ceram Res Ctr Tajimi Japan;

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  • 正文语种 eng
  • 中图分类 化学;
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