吸附
催化作用
活动站点
反应机理
化学
Atom(片上系统)
密度泛函理论
反应中间体
化学吸附
计算化学
物理化学
材料科学
结晶学
有机化学
计算机科学
嵌入式系统
作者
Bei Li,Jiaqi Li,Yi Rong,Yaxuan Tian,Jing Li,Xingchen Liu,Qinglan Hao,Botao Teng
标识
DOI:10.1016/j.apsusc.2022.153832
摘要
OH adsorbs at the active site of the coordinatively unsaturated surface Sn with electron accumulation on CaSnO 3 and form H 2 O 2 . • Three methods were used to calculate the surface energies of CaSnO 3 (1 2 1) • O 4 (Sn) surface is most stable among 17 terminations of CaSnO 3 (1 2 1) • The uncoordinated Sn atom is the active site for OH adsorption and H 2 O 2 formation. • Two practical ways to develop 2e-WOR catalyst with high performance were proposed. The two-electron water oxidation reaction (2e-WOR) is an eco-friendly process to produce H 2 O 2 , which attracts much attention due to its low cost and high safety. CaSnO 3 is a potential industrial catalyst for 2e-WOR reaction with high performance. However, the surface structure and active site of CaSnO 3 , as well as H 2 O 2 formation mechanism, are still unknown due to its complex structure and limitation of characterization technique in resolution of surface fine structure and intermediates. To solve this difficult problem, the authors systematically investigated the surface structures of CaSnO 3 and the adsorption and reaction behaviors of H 2 O, OH and H 2 O 2 on CaSnO 3 by density functional theory method. The present work indicated that the O4(Sn) surface with 5-coordinated Sn is the most stable termination of CaSnO 3 (1 2 1) by comparing the surface energies of 17 terminations of CaSnO 3 (1 2 1); OH strongly chemisorbs at the top site of Sn on CaSnO 3 (1 2 1) and can diffuse on surface with the free energy barrier of 0.68 ∼ 1.07 eV; the coordination unsaturated Sn atom is the active site for OH adsorption and H 2 O 2 formation. According to the deep understanding of the mechanism of the 2e-WOR reaction to H 2 O 2 on CaSnO 3 , two practical ways were proposed to design and develop 2e-WOR catalysts with high performance.
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