Catalyst Design Based on Morphology- and Environment-Dependent Adsorption on Metal Nanoparticles
Catalyst Design Based on Morphology- and Environment-Dependent Adsorption on Metal Nanoparticles
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DOI：
10.1021/acscatal.5b01696
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发表时间：
2015-09
期刊：
影响因子：
12.9
通讯作者：
Michael G. Taylor;N. Austin;Chrysanthos E. Gounaris;Giannis Mpourmpakis
中科院分区：
文献类型：
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作者：
Michael G. Taylor;N. Austin;Chrysanthos E. Gounaris;Giannis Mpourmpakis
了解金属-吸附物的相互作用是控制和提高金属纳米颗粒（NPs）在能源和生物医学应用领域功能的关键。然而，吸附取决于NP的形态特征，例如它们的大小和形状，反过来，NP的形态取决于化学环境（吸附剂的存在）。在这项工作中，我们引入了一种新的、可计算的框架，它能够捕捉作为NP大小和形状的函数的吸附趋势，包括化学环境对NP形态的影响。我们的方法在催化领域进行了测试，特别是在金（Au）上的CO氧化行为，这是一种高度结构敏感的反应。我们的研究结果表明，实验观察到的CO氧化活性与Au NPs上的平均CO吸附（结合）能之间存在很强的相关性，从而可以作为NP形态的函数来预测催化行为。我们证明了Au NP大小起着关键作用……
Understanding metal–adsorbate interactions is key to controlling and improving the functionality of metal nanoparticles (NPs) in energy and biomedical application areas. However, adsorption is dependent on the morphological characteristics of the NPs, such as their size and shape, and in turn, the NP morphology is dependent on the chemical environment (presence of adsorbates). In this work, we introduce a novel and computationally tractable framework that is able to capture adsorption trends as a function of NP size and shape, including the impact of chemical environment on NP morphology. Our methodology is tested in the area of catalysis and specifically on the CO oxidation behavior on gold (Au), a highly structure-sensitive reaction. Our results reveal a strong correlation between the experimentally observed CO oxidation activity and the average CO adsorption (binding) energy on Au NPs enabling catalytic behavior prediction as a function of NP morphology. We demonstrate that the Au NP size plays a pivot...