Degradation Chemistry and Kinetic Stabilization of Magnetic CrI3

化学 碘化物 反应速率常数 水解 降级(电信) 无定形固体 甲酸 无机化学 光化学 化学工程 动力学 有机化学 电信 物理 量子力学 计算机科学 工程类
作者
Taiming Zhang,Magdalena Grzeszczyk,Jing Li,Wei Yu,Haomin Xu,Peng He,Li‐Ming Yang,Zhizhan Qiu,Huihui Lin,Huimin Yang,Jian Zeng,Tao Sun,Zejun Li,Jishan Wu,Ming Lin,Kian Ping Loh,Chenliang Su,Kostya S. Novoselov,Alexandra Carvalho,Maciej Koperski,Jiong Lu
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:144 (12): 5295-5303 被引量:22
标识
DOI:10.1021/jacs.1c08906
摘要

The discovery of the intrinsic magnetic order in single-layer chromium trihalides (CrX3, X = I, Br, and Cl) has drawn intensive interest due to their potential application in spintronic devices. However, the notorious environmental instability of this class of materials under ambient conditions renders their device fabrication and practical application extremely challenging. Here, we performed a systematic investigation of the degradation chemistry of chromium iodide (CrI3), the most studied among CrX3 families, via a joint spectroscopic and microscopic analysis of the structural and composition evolution of bulk and exfoliated nanoflakes in different environments. Unlike other air-sensitive 2D materials, CrI3 undergoes a pseudo-first-order hydrolysis in the presence of pure water toward the formation of amorphous Cr(OH)3 and hydrogen iodide (HI) with a rate constant of kI = 0.63 day-1 without light. In contrast, a faster pseudo-first-order surface oxidation of CrI3 occurs in a pure O2 environment, generating CrO3 and I2 with a large rate constant of kCr = 4.2 day-1. Both hydrolysis and surface oxidation of CrI3 can be accelerated via light irradiation, resulting in its ultrafast degradation in air. The new chemical insights obtained allow for the design of an effective stabilization strategy for CrI3 with preserved optical and magnetic properties. The use of organic acid solvents (e.g., formic acid) as reversible capping agents ensures that CrI3 nanoflakes remain stable beyond 1 month due to the effective suppression of both hydrolysis and oxidation of CrI3.
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