驱动纳米材料尺寸依赖表面化学活性的一般电子原理
The general electronic principle driving size-dependent surface chemical activities of nanomaterials
摘要：
尺寸可以广泛地影响纳米材料在化学吸附、催化、表面效应等方面的表面化学活性（SCA），但其潜在的电子性质一直是个谜。我们报告了一个一般的电子原理，驱动器的大小依赖SCA的起源相结合的实验探测和理论建模。以H_2O_2在TiO_2上的化学吸附为模型反应，通过实验揭示了表面化学相互作用的中心电子过程在于表面原子轨道从能带态到表面配位键的竞争性重新分配.通过定义轨道势，一个网站依赖的固有电子特性，决定表面活动，我们进一步建立了一个数学模型，揭示了结构因素如何与SCA相关的物理本质，特别是大小的作用。我们发现尺寸效应的电子本质在于它与轨道势的负相关以及对其他结构因素如缺陷和配位数的放大效应。
英文摘要：
Size can widely affect the surface chemical activities (SCAs) of nanomaterials in chemisorption, catalysis, surface effects, etc., but the underlying electronic nature has long remained mysterious. We report a general electronic principle that drives the origin of size-dependent SCAs by combining experimental probing and theoretical modeling. Using the chemisorption of H2O2 on TiO2 as a model reaction, we experimentally reveal that the central electronic process of surface chemical interactions lies in the competitive redistribution of surface atomic orbitals from energy band states into surface coordination bonds. By defining orbital potential, a site-dependent intrinsic electronic property that determines surface activities, we further establish a mathematical model to uncover the physical nature of how structural factors correlate to SCAs, particularly the roles of size. We discover that the electronic nature of size effect lies in its inverse correlation to orbital potential and amplification effect on other structural factors like defects and coordination numbers.
机构、总结、中文摘要均由AI分析而来，可能存在错误，请以论文正文为准。
