化学物理
相间
原子单位
氧化还原
材料科学
相(物质)
金属
单斜晶系
分子动力学
化学反应
纳米尺度
微观结构
动力学(音乐)
化学
化学工程
结晶学
纳米技术
计算化学
物理
晶体结构
生物化学
遗传学
有机化学
量子力学
声学
工程类
冶金
生物
作者
Xianhu Sun,Dazhuan Wu,Wissam A. Saidi,Wenhui Zhu,Wei-Chang Yang,Stephen D. House,Meng Li,Renu Sharma,Judith C. Yang,Guangwen Zhou
出处
期刊:Small
[Wiley]
日期:2023-11-08
标识
DOI:10.1002/smll.202305746
摘要
Redox-induced interconversions of metal oxidation states typically result in multiple phase boundaries that separate chemically and structurally distinct oxides and suboxides. Directly probing such multi-interfacial reactions is challenging because of the difficulty in simultaneously resolving the multiple reaction fronts at the atomic scale. Using the example of CuO reduction in H2 gas, a reaction pathway of CuO → monoclinic m-Cu4 O3 → Cu2 O is demonstrated and identifies interfacial reaction fronts at the atomic scale, where the Cu2 O/m-Cu4 O3 interface shows a diffuse-type interfacial transformation; while the lateral flow of interfacial ledges appears to control the m-Cu4 O3 /CuO transformation. Together with atomistic modeling, it is shown that such a multi-interface transformation results from the surface-reaction-induced formation of oxygen vacancies that diffuse into deeper atomic layers, thereby resulting in the formation of the lower oxides of Cu2 O and m-Cu4 O3 , and activate the interfacial transformations. These results demonstrate the lively dynamics at the reaction fronts of the multiple interfaces and have substantial implications for controlling the microstructure and interphase boundaries by coupling the interplay between the surface reaction dynamics and the resulting mass transport and phase evolution in the subsurface and bulk.
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