Reactivity loss by intermediates aggregation and water vapor inhibition are two major and longstanding challenges for the noble-metal-based catalysts in oxygenated volatile organic compounds (OVOCs) oxidation. Herein, the core-shell Pd@CoO Janus sites are creatively designed and stabilized over the HSAPO-34 support. Quasi XPS spectra reveal that the strong interactions in Pd@CoO Janus sites promote the charge redistribution and electron back-donation through Pd-O-Co coordination. Therefore, abundant positively charged Pd sites are formed and oxygen species transformation is facilitated, which significantly promote the low-temperature efficiency of acetone oxidation. Furthermore, the Pd@CoO/HSAPO-34 catalyst facilitates HO molecules dissociation and produce reactive OH and OH species, which considerably promotes the rapid decomposition of aldehyde intermediate via attacked CHO* group, ensuring low-temperature oxidation of acetone. This work provides valuable guidance to develop specific catalysts with functional active sites for rationally utilizing HO molecules to improve low-temperature performance and modulate reaction pathways during OVOCs oxidation.

中文翻译：

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通过促进核壳 Pd@CoO Janus 上的 H2O 解离来促进中间体转化，以实现丙酮的有效氧化


中间体聚集导致的反应性损失和水蒸气抑制是含氧挥发性有机化合物 (OVOC) 氧化中贵金属基催化剂面临的两个主要且长期存在的挑战。在此，核壳 Pd@CoO Janus 位点经过创造性设计并在 HSAPO-34 支持上稳定。准XPS谱表明，Pd@CoO Janus位点的强相互作用通过Pd-O-Co配位促进电荷重新分布和电子回馈。因此，形成了丰富的带正电的Pd位点，促进了氧物质的转化，从而显着提高了丙酮氧化的低温效率。此外，Pd@CoO/HSAPO-34催化剂促进H2O分子解离并产生活性OH和OH物种，这通过攻击CHO*基团显着促进醛中间体的快速分解，确保丙酮的低温氧化。这项工作为开发具有功能活性位点的特定催化剂提供了宝贵的指导，以合理利用 H2O 分子来提高低温性能并调节 OVOC 氧化过程中的反应途径。