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In Situ Monitoring of H2-Induced Nonstoichiometry in Cu2O
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2022-06-14 , DOI: 10.1021/acs.jpclett.2c00988
Jianyu Wang 1 , Chaoran Li 1 , Yaguang Zhu 1 , Jorge Anibal Boscoboinik 2 , Guangwen Zhou 1
Affiliation  

Using ambient-pressure X-ray photoelectron spectroscopy and Auger electron spectroscopy to monitor the reduction of Cu2O in H2, we identify the formation of an intermediate, oxygen-deficient Cu2O phase and its progressive inward growth into the deeper region of the oxide. Complemented by atomistic modeling, we show that the oxygen-deficient Cu2O formation occurs via molecular H2 adsorption at the Cu2O surface, which results in the loss of lattice oxygen from the formation of H2O molecules that desorb spontaneously from the oxide surface. The resulting oxygen-deficient Cu2O is a stable intermediate that persists before the Cu2O is fully reduced to metallic Cu. The oxygen vacancy-induced charge of the coordinating Cu atoms results in a satellite feature in Cu LMM, which can be used as a fingerprint to identify nonstoichiometry in oxides and local charge transfer induced by the nonstoichiometry.

中文翻译:

Cu2O 中 H2 诱导非化学计量的原位监测

使用环境压力 X 射线光电子能谱和俄歇电子能谱来监测H 2中 Cu 2 O 的还原,我们确定了中间缺氧 Cu 2 O 相的形成及其逐渐向内生长到更深的区域。氧化物。辅以原子模型,我们表明缺氧 Cu 2 O 的形成是通过在 Cu 2 O 表面的分子 H 2吸附发生的,这导致晶格氧因 H 2 O 分子的形成而损失,而 H 2 O 分子会自发解吸。氧化物表面。所得的缺氧 Cu 2 O 是一种稳定的中间体,在 Cu 之前持续存在2 O 完全还原为金属Cu。配位铜原子的氧空位诱导电荷导致铜 LMM 中的卫星特征,可用作指纹来识别氧化物中的非化学计量和由非化学计量引起的局部电荷转移。
更新日期:2022-06-14
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