Structure–Property–Performance Relationships of Cuprous Oxide Nanostructures for Dielectric Mie Resonance-Enhanced Photocatalysis
Structure–Property–Performance Relationships of Cuprous Oxide Nanostructures for Dielectric Mie Resonance-Enhanced Photocatalysis
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DOI：
10.1021/acscatal.2c00977
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发表时间：
2022-06
期刊：
影响因子：
12.9
通讯作者：
Ravi Teja A. Tirumala;Sunil Gyawali;Aaron Wheeler;S. Ramakrishnan;R. Sooriyagoda;Farshid Mohammadparast;Nishant Khatri;Susheng Tan;A. Kalkan;Alan D Bristow;M. Andiappan
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文献类型：
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作者：
Ravi Teja A. Tirumala;Sunil Gyawali;Aaron Wheeler;S. Ramakrishnan;R. Sooriyagoda;Farshid Mohammadparast;Nishant Khatri;Susheng Tan;A. Kalkan;Alan D Bristow;M. Andiappan
纳米金属氧化物如Cu2O、CeO2、α-Fe2O3和TiO2光催化可有效地将太阳能转化为化学能和修复污染。在这篇文章中，我们报道了一种新的方法，介电Mie共振增强光催化，以提高金属氧化物光催化剂的催化活性。具体地说，我们证明了具有介电Mie共振的Cu2O纳米结构比没有介电Mie共振的Cu2O纳米结构表现出高出一个数量级的光催化速率。我们的时域有限差分(FDTD)模拟和实验结果预测了光催化速率与Cu2O纳米球和纳米立方体的尺寸之间的火山型关系。利用瞬时吸收测量，我们发现在表现出较高光催化速率的Cu2O纳米结构中，与介电Mie共振介导的电荷载流子产生相关的相干电子过程占主导地位。虽然我们在实验中仅用Cu2O纳米粒子演示了介电Mie共振增强光催化，但基于我们的FDTD模拟，我们预计其他金属氧化物光催化剂也可以达到同样的效果，包括CeO2，α-Fe2O3和TiO2.
Nanostructured metal oxides, such as Cu2O, CeO2, α-Fe2O3, and TiO2, can efficiently mediate photocatalysis for solar-to-chemical energy conversion and pollution remediation. In this contribution, we report a novel approach, dielectric Mie resonance-enhanced photocatalysis, to enhance the catalytic activity of metal oxide photocatalysts. Specifically, we demonstrate that Cu2O nanostructures exhibiting dielectric Mie resonances can exhibit up to an order of magnitude higher photocatalytic rate as compared with Cu2O nanostructures not exhibiting dielectric Mie resonances. Our finite-difference time-domain (FDTD) simulation and experimental results predict a volcano-type relationship between the photocatalytic rate and the size of Cu2O nanospheres and nanocubes. Using transient absorption measurements, we reveal that a coherent electronic process associated with dielectric Mie resonance-mediated charge carrier generation is dominant in Cu2O nanostructures that exhibit higher photocatalytic rates. Although we experimentally demonstrate dielectric Mie resonance-enhanced photocatalysis with only Cu2O nanoparticles here, based on our FDTD simulations, we anticipate the same can be achieved with other metal oxide photocatalysts, including CeO2, α-Fe2O3, and TiO2.