Predictive Removal of Interfacial Defect-Induced Trap States between Titanium Dioxide Nanoparticles via Sub-Monolayer Zirconium Coating.
Predictive Removal of Interfacial Defect-Induced Trap States between Titanium Dioxide Nanoparticles via Sub-Monolayer Zirconium Coating.
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DOI：
10.1021/acs.jpcc.2c06927
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发表时间：
2023-01-12
影响因子：
3.7
通讯作者：
Douthwaite, Richard E.
中科院分区：
文献类型：
--
作者：
Debgupta, Joyashish;Lari, Leonardo;Isaacs, Mark;Carey, John;McKenna, Keith P.;Lazarov, Vlado K.;Chechik, Victor;Douthwaite, Richard E.
第一性原理模拟的TiO 2表面和它们的界面接触表明，缺陷引起的陷阱状态的带隙内产生的固有的结构扭曲，这些可以通过修改与Zr（IV）离子进行校正。这些预测的实验测试已经进行了使用改性的Zr前体的范围内，其特征在于使用结构和光谱方法的nanocrystals。连续波电子顺磁共振（EPR）光谱显示，在光照下，纳米粒子-纳米粒子界面空穴陷阱状态占主导地位，这是显着减少后，优化Zr掺杂。这些材料的纳米多孔膜的制造和使用电化学方法的电荷注入表明，Zr掺杂也导致在这些纳米晶系统中改善的电子导电性和迁移率。这里描述的减少界面缺陷的浓度的简单方法可以具有更广泛的应用，以提高并入金属氧化物粉末和膜的系统的效率，包括光催化剂、光催化剂、燃料电池和相关的能量应用。
First principles modeling of anatase TiO2 surfaces and their interfacial contacts shows that defect-induced trap states within the band gap arise from intrinsic structural distortions, and these can be corrected by modification with Zr(IV) ions. Experimental testing of these predictions has been undertaken using anatase nanocrystals modified with a range of Zr precursors and characterized using structural and spectroscopic methods. Continuous-wave electron paramagnetic resonance (EPR) spectroscopy revealed that under illumination, nanoparticle–nanoparticle interfacial hole trap states dominate, which are significantly reduced after optimizing the Zr doping. Fabrication of nanoporous films of these materials and charge injection using electrochemical methods shows that Zr doping also leads to improved electron conductivity and mobility in these nanocrystalline systems. The simple methodology described here to reduce the concentration of interfacial defects may have wider application to improving the efficiency of systems incorporating metal oxide powders and films including photocatalysts, photovoltaics, fuel cells, and related energy applications.
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