In this study, CeO_x with different exposed facets was prepared to investigate their potential effect on activating the peroxone reaction (H₂O₂/O₃) and breaking through the restriction of solution pH on peroxone. By controlling the concentration of hydroxide, cube CeO_x with a (100) facet, rod CeO_x with a (110) facet and octahedron CeO_x with a (111) facet were prepared by the hydrothermal precipitation method, and they all promoted heterogeneous peroxone for oxalic acid (OA) under acidic conditions. The catalytic activity of CeO_x was highly related to their surface oxygen vacancies (OVs) and the interfacial electron transfer process. Both experiments and theoretical calculations showed that CeO_x with different exposed facets activated peroxone in different ways and (111) CeO_x possessed better activity than (100) or (110) CeO_x. The low efficiencies of (100) and (110) CeO_x were due to their inefficient use of H₂O₂ to reduce surface Ce⁴⁺ and their large energy gap to generate surface peroxide (OVs-OOH). (111) CeO_x was stable with surface-adsorbed H₂O₂, and the rich electrons at OVs could be donated to H₂O₂ and generate OVs-OOH, which then triggered O₃ decomposition into hydroxyl radical (˙OH) and superoxide radical (˙O₂⁻). These electron migration processes depended on the electron-donating ability of the OVs rather than solution pH, therefore, still greater amounts of reactive species were generated under acidic conditions. The flexibility of the (111) CeO_x/H₂O₂/O₃ process was further investigated for removing 20 kinds of pharmaceuticals. The synergy effect of (111) CeO_x/O₃ and H₂O₂ varied with the structure of the pharmaceuticals.

中文翻译：

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揭示 CeOx 上 H2O2、O3 和氧空位之间的多面依赖性行为以及酸性条件下过氧酮反应的促进

在本研究中，制备了具有不同暴露面的CeO _x以研究它们对激活过氧酮反应 (H ₂ O ₂ /O ₃ ) 和突破溶液 pH 对过氧酮的限制的潜在影响。通过控制氢氧化物的浓度，水热沉淀法制备了具有（100）面的立方CeO _x、具有（110）面的棒状CeO _x和具有（111）面的八面体CeO _x，它们均促进了异质过氧酮用于酸性条件下的草酸 (OA)。CeO _x的催化活性与它们的表面氧空位（OV）和界面电子转移过程高度相关。实验和理论计算均表明，具有不同暴露面的CeO _x以不同方式激活过氧酮，并且（111）CeO _x比（100）或（110）CeO _x具有更好的活性。(100) 和(110) CeO _x的低效率是由于它们低效地使用H ₂ O ₂来还原表面Ce ⁴⁺以及它们产生表面过氧化物(OVs-OOH)的大能隙。(111) CeO _x与表面吸附的 H ₂ O ₂稳定，OVs 处的富电子可以捐赠给 H₂ O ₂并生成OVs-OOH，然后触发O ₃分解为羟基自由基(˙OH)和超氧自由基(˙O ₂ ⁻ )。这些电子迁移过程取决于 OV 的给电子能力，而不是溶液的 pH 值，因此，在酸性条件下会产生更多的活性物质。进一步研究了（111）CeO _x /H ₂ O ₂ /O ₃工艺去除20种药物的灵活性。(111) CeO _x /O ₃与H ₂ O ₂的协同效应 因药物结构而异。