兴奋剂
催化作用
锐钛矿
材料科学
掺杂剂
氧气
密度泛函理论
物理化学
光催化
计算化学
化学
有机化学
光电子学
作者
Muhammed Fasil Puthiyaparambath,Raghu Chatanathodi
出处
期刊:Physical Review Materials
[American Physical Society]
日期:2023-11-08
卷期号:7 (11)
被引量:3
标识
DOI:10.1103/physrevmaterials.7.115801
摘要
${\mathrm{TiO}}_{2}$ has wide applications in catalysis and photocatalysis and is an attractive alternative to Pt or Pt-based catalysts due to its abundance, low cost, and nontoxicity. However, it does not display any worthwhile catalytic activity as far as the oxygen reduction reaction (ORR) is concerned. Attempts have been made to improve the activity of ${\mathrm{TiO}}_{2}$ by doping and creating defects on the surface. Nb-doped ${\mathrm{TiO}}_{2}$ is experimentally found to have good conductivity and electrochemical activity for low-Nb concentrations. This paper presents a systematic modeling study of how Nb doping influences the ORR activity of anatase ${\mathrm{TiO}}_{2}$ using plane-wave density-functional theory method. We elucidate the probable dopant sites, the effect of Nb doping on the oxygen binding capability at active sites, the favored reaction pathway, and the transition state. We find a remarkable enhancement in the capability of ${\mathrm{TiO}}_{2}$ to catalyze ORR upon doping with Nb. We have also modeled the effect of solvation on the binding of oxygen and other reaction intermediates, using a model where water molecules are added as a monolayer over Nb-doped ${\mathrm{TiO}}_{2}$. Solvation introduces additional hydrogen bonding, which improves the binding of intermediates to the active site and lowers activation barriers. Our model for ORR in Nb-doped ${\mathrm{TiO}}_{2}$ agrees with recent experimental results on the same.
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