In situ atomic-scale imaging of the metal/oxide interfacial transformation.
In situ atomic-scale imaging of the metal/oxide interfacial transformation.
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金属/氧化物界面转变的原位原子尺度成像。
DOI：
10.1038/s41467-017-00371-4
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发表时间：
2017-08-21
影响因子：
16.6
通讯作者：
Zhou G
中科院分区：
文献类型：
--
作者：
Zou L;Li J;Zakharov D;Stach EA;Zhou G
由于金属/氧化物界面的埋藏特性，直接探测其结构动力学一直是一个重大挑战。利用环境透射电子显微镜，研究了Cu氧化过程中Cu2O/Cu界面的原位形成，并探讨了H2气体还原过程中界面转变和晶粒旋转的原子机制。Cu2O→Cu相变首先沿Cu2O/Cu界面逐层发生。Cu2O/Cu界面上氧空位的积累导致界面附近Cu2O晶格的坍塌，导致Cu2O/Cu界面倾斜并伴随Cu2O岛旋转。这些结果提供了关于负载氧化物氧化还原反应的前所未有的微观细节，这与需要在母体氧化物和还原相之间形成新的界面的大块或分离氧化物的还原有根本的不同。金属/氧化物界面在非均相催化和氧化还原反应中起着重要作用，但其埋藏性质使其难以研究。在这里，作者使用环境透射电子显微镜来探测Cu2O/Cu界面发生氧化还原反应时的原子水平转变。
Directly probing structure dynamics at metal/oxide interfaces has been a major challenge due to their buried nature. Using environmental transmission electron microscopy, here we report observations of the in-place formation of Cu2O/Cu interfaces via the oxidation of Cu, and subsequently probe the atomic mechanisms by which interfacial transformation and grain rotation occur at the interfaces during reduction in an H2 gas environment. The Cu2O→Cu transformation is observed to occur initially along the Cu2O/Cu interface in a layer-by-layer manner. The accumulation of oxygen vacancies at the Cu2O/Cu interface drives the collapse of the Cu2O lattice near the interface region, which results in a tilted Cu2O/Cu interface with concomitant Cu2O island rotation. These results provide unprecedented microscopic detail regarding the redox reactions of supported oxides, which differs fundamentally from the reduction of bulk or isolated oxides that requires the formation of new interfaces between the parent oxide and the reduced phase. Metal/oxide interfaces play an important role in heterogeneous catalysis and redox reactions, but their buried nature makes them difficult to study. Here, the authors use environmental transmission electron microscopy to probe the atomic-level transformations at Cu2O/Cu interfaces as they undergo redox reactions.
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影响因子：
15
作者：
LaGrow, Alec P.;Ward, Michael R.;Boyes, Edward D.
通讯作者：
Boyes, Edward D.
影响因子：
3.7
作者：
MONKHORST, HJ;PACK, JD
通讯作者：
PACK, JD
影响因子：
--
作者：
Dalverny, A. -L.;Filhol, J. -S.;Doublet, M. -L.
通讯作者：
Doublet, M. -L.
影响因子：
6
作者：
Hashibon, Adham;Elsaesser, Christian
通讯作者：
Elsaesser, Christian
影响因子：
3.7
作者：
Li, Liang;Liu, Qianqian;Zhou, Guangwen
通讯作者：
Zhou, Guangwen