Oxygen Vacancy-Induced Novel Low-Temperature Water Splitting Reactions on FeO(111) Monolayer-Thick Film

Oxygen Vacancy-Induced Novel Low-Temperature Water Splitting Reactions on FeO(111) Monolayer-Thick Film
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DOI:
10.1021/jp307104a
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发表时间:
2012-10
影响因子:
3.7
通讯作者:
Lingshun Xu;Zongfang Wu;Wenhua Zhang;Yuekang Jin;Qing Yuan;Yunsheng Ma;Weixin Huang
Lingshun Xu;Zongfang Wu;Wenhua Zhang;Yuekang Jin;Qing Yuan;Yunsheng Ma;Weixin Huang
中科院分区:
化学3区
文献类型:
--
作者:
Lingshun Xu;Zongfang Wu;Wenhua Zhang;Yuekang Jin;Qing Yuan;Yunsheng Ma;Weixin Huang

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利用XPS、UPS和TDS研究了Pt(111)表面FeO(111)单分子膜、Pt(111)表面FeO(111)单分子岛和Pt(111)表面含氧空位的FeO(111)单分子膜在110 K下的水化学吸附和反应。水在化学计量比的FeO(111)单层膜上发生可逆的分子吸附。在Pt(111)上的化学计量的FeO(111)单层厚的岛上,水在FeO(111)-Pt(111)界面的配位不饱和的Fe(II)位点处解离,形成OH,遵循H2O + FeCUS + FeO → FeH 2 O-OwH + FeOH,其中Ow表示从H2O解离出O。在加热时,在高于500 K时发生H2析出。在具有氧空位的FeO(111)单层膜上,水解离并分子化学吸附,形成H(a)、OH和H2O(a)的混合吸附层,其吸附顺序为H2O + Fe-O空位+ FeO → FeOwH + FeOH和H2O +2Fe-O空位→ FeOwH + H(a)-Fe-O空位。在加热时,除了高温H2释放之外,额外的H2解吸...
We have used XPS, UPS, and TDS to comparatively study water chemisorption and reaction on stoichiometric FeO(111) monolayer-thick film on Pt(111), stoichiometric FeO(111) monolayer-thick islands on Pt(111), and FeO(111) monolayer-thick films with oxygen vacancies on Pt(111) at 110 K. On stoichiometric FeO(111) monolayer-thick film, water undergoes reversible molecular adsorption. On stoichiometric FeO(111) monolayer-thick islands on Pt(111), water dissociates at coordination-unsaturated Fe(II) sites of the FeO(111)–Pt(111) interface to form OH following H2O + FeCUS + FeO → FeCUS–OwH + FeOH in which Ow means O from H2O. Upon heating, H2 evolution occurs above 500 K. On FeO(111) monolayer-thick films with oxygen vacancies, water dissociates and molecularly chemisorbs to form a mixed adsorbate layer of H(a), OH, and H2O(a) following both H2O + Fe–Ovacancy + FeO → FeOwH + FeOH and H2O + 2 Fe–Ovacancy → FeOwH + H(a)–Fe–Ovacancy. Upon heating, besides the high-temperature H2 evolution, additional H2 desorption ...