机械诱导自蔓延反应(MSRs)瞬时制备二元金属瑀:评估粒度、体积模量、试剂熔化温差和热力学常数对点火时间的影响†。

Matej Baláž, Róbert Džunda, Radovan Bureš, Tibor Sopčák and Tamás Csanádi
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引用次数: 0

摘要

机械诱导的自推进反应(MSRs)提供了以超快方式获得所需产物的可能性,因此具有成本和能源效率高的特点。在这项工作中,通过在行星式球磨机中对金属和助熔剂的混合物进行不到 10 分钟的处理,证明了这一方法适用于 10 种二元金属卤化物(CdS、CdSe、In2S3、NiS、NiSe、PbS、PbSe SnSe、ZnS 和 ZnSe)。首次报道了镍基系统的 MSR 过程。所研究的金属与硒的反应要比与硫的反应快得多(镍除外)。通过 X 射线衍射对研磨罐内气体压力的现场监测和随后的现场监测,证明 MSR 成功发生。回收产物的晶体尺寸通常在 40-260 纳米之间。所有反应都是在空气环境中进行的,因此不需要惰性气体的存在。我们努力将观察到的点火时间与前驱体的粒度、熔化温度、体积模量和热力学参数(ΔH/Cp 和 ΔG)联系起来。虽然热力学参数在这里似乎并不起重要作用,但反应金属的粒度和体积模量很可能会影响 MSR 的点火时间。也就是说,较高的延展性(较低的体积模量)和较细的颗粒似乎会缩短 MSR 点火前的活化期。这项研究为进一步研究金属卤化物的 MSR 奠定了基础,因为它普遍评估了不同体系在固定研磨条件下更多参数对 MSR 过程的影响。所提出的合成途径也是一种改进,它通过显示在一分钟范围内达到某些所需产物的可能性,减少了时间和能量,比传统的渐进反应快得多,并进一步强调了机械化学的环境友好特性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Mechanically induced self-propagating reactions (MSRs) to instantly prepare binary metal chalcogenides: assessing the influence of particle size, bulk modulus, reagents melting temperature difference and thermodynamic constants on the ignition time†

Mechanically induced self-propagating reactions (MSRs) to instantly prepare binary metal chalcogenides: assessing the influence of particle size, bulk modulus, reagents melting temperature difference and thermodynamic constants on the ignition time†

Mechanically induced self-propagating reactions (MSRs) offer the possibility to obtain desired products in an ultrafast and thus cost- and energy-efficient manner. In this work, this is demonstrated for ten binary metal chalcogenides (CdS, CdSe, In2S3, NiS, NiSe, PbS, PbSe SnSe, ZnS and ZnSe) by processing mixtures of metals and chalcogens in a planetary ball mill for less than 10 minutes. The MSR process for Ni-based systems is reported for the first time. The studied metals reacted much faster with selenium than with sulfur (with the exception of Ni). The successful MSR occurrence was evidenced by an abrupt increase of gas pressure in the milling jar monitored in situ and subsequently ex situ by X-ray diffraction. The crystallite size of the as-received products was usually in the range 40–260 nm. All the reactions were performed in an air atmosphere, and thus the presence of an inert gas was not necessary. An effort was made to correlate the observed ignition times with the particle size of the precursors, their melting temperature, bulk modulus and thermodynamic parameters (ΔH/Cp and ΔG). While the thermodynamics does not seem to play an important role here, the particle size and bulk modulus of the reacting metal most probably influence the ignition time of MSRs. Namely, higher ductility (low bulk modulus) and finer particles seem to shorten the activation period before the MSR ignition. This study forms a cornerstone for further research in MSRs of metal chalcogenides because it universally assesses the influence of more parameters on the MSR course under fixed milling conditions for different systems. The proposed synthetic pathway also represents an improvement by reducing both time and energy by showing the possibility to reach some of the desired products within a minute-range, being much faster than a classical gradual reaction and further underlines the environmentally benign character of mechanochemistry.

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