美国宾夕法尼亚州立大学Raymond E. Schaak团队开发了一种同时多离子交换途径合成高熵金属硫化物纳米粒子的策略。相关研究成果于2021年1月6日发表在国际知名学术期刊《美国化学会志》。

高熵材料含有大量随机分布的元素，具有独特的催化、电化学和力学性能。随机化元素的高构型熵驱动高熵材料的形成；因此，通常需要高温和淬火来稳定它们。正因为如此，高熵材料的胶体纳米粒子很难合成，尽管它们具有理想的高比表面积和溶液分散性，但仍然很少见。

该文中，研究人员开发了同时多阳离子交换作为一种替代低温途径来制备高熵材料的胶体纳米粒子。Cu1.8S纳米粒子与Zn2+、Co2+、In3+和Ga3+的亚化学计量混合物反应生成高熵金属硫化物Zn0.25Co0.22Cu0.28In0.16Ga0.11S纳米粒子。Zn0.25Co0.22Cu0.28In0.16Ga0.11S纳米粒子具有热稳定性，使用较少阳离子的交换反应不会产生高熵相。胶体纳米粒子阳离子交换作为一个合成平台的使用提供了熵和焓驱动力，除了结构熵之外，还能够在溶液可及温度下形成高熵相。

附：英文原文

Title: Simultaneous Multication Exchange Pathway to High-Entropy Metal Sulfide Nanoparticles

Author: Connor R. McCormick, Raymond E. Schaak

Issue&Volume: January 6, 2021

Abstract: High entropy materials, which contain a large number of randomly distributed elements, have unique catalytic, electrochemical, and mechanical properties. The high configurational entropy of the randomized elements drives the formation of high entropy materials; therefore, high temperatures and quenching are typically required to stabilize them. Because of this, colloidal nanoparticles of high entropy materials are difficult to synthesize and remain rare, despite their desirable high surface areas and solution dispersibilities. Here, we introduce simultaneous multication exchange as an alternative low-temperature pathway to colloidal nanoparticles of high entropy materials. Roxbyite Cu1.8S nanoparticles react with a substoichiometric mixture of Zn2+, Co2+, In3+, and Ga3+ to produce nanoparticles of the high entropy metal sulfide Zn0.25Co0.22Cu0.28In0.16Ga0.11S. The Zn0.25Co0.22Cu0.28In0.16Ga0.11S nanoparticles are thermally stable, and exchange reactions using fewer cations do not produce the high entropy phase. The use of colloidal nanoparticle cation exchange as a synthetic platform provides both entropic and enthalpic driving forces that, in addition to configurational entropy, enable the formation of high entropy phases at solution-accessible temperatures.

DOI: 10.1021/jacs.0c11384

Source: https://pubs.acs.org/doi/10.1021/jacs.0c11384