Scholarlink

<p>Transition metal-doped CeO<sub>2</sub> catalysts exhibit great potentials for the selective catalytic reduction (SCR) of nitrogen oxide (NO<sub><i>x</i></sub>) with NH<sub>3</sub> (NH<sub>3</sub>-SCR). However, traditional research mainly relies on a lot of experiments to find out effective catalysts, which wastes a lot of time and resources. Screening out effective CeO<sub>2</sub>-based catalysts for low-temperature NH<sub>3</sub>-SCR via density functional theory (DFT) calculations is crucial for the rational design and synthesis of efficient catalysts. Herein, transition metal (M = Co, Cr, Cu, Fe, Mn, Mo, Nb, Ni, Ta, Ti, V, and W)-doped CeO<sub>2</sub> catalysts were screened out via accelerated DFT calculations for NH<sub>3</sub>-SCR of nitric-oxide (NO) using three theoretical terms; (i) an adsorption energy of NH<sub>3</sub>, (ii) an adsorption energy of NO, and (iii) the reaction energies between NO with O<sub>2</sub> and lattice oxygen. The theoretically predicted trend in catalytic performance is as follows: CeO<sub>2</sub>-Mn, -Cu, -Mo &gt; CeO<sub>2</sub>-Fe, -Co, -Ni, -V, -Cr &gt; CeO<sub>2</sub>-W, -Ti &gt; CeO<sub>2</sub>-Nb, -Ta. The theoretical prediction was well verified via experimental NH<sub>3</sub>-SCR activity of NO at low temperatures (90–300&#xa0;°C), demonstrating CeO<sub>2</sub>-Mo as efficient NH<sub>3</sub>-SCR catalyst across a broad temperature range. Temperature-programmed desorption of NH<sub>3</sub> and in situ diffuse reflectance infrared Fourier transforms spectroscopy further indicated that metal doping significantly enhanced the NH<sub>3</sub> adsorption capacity and strength of CeO<sub>2</sub> in the medium- to low-temperature range. Consequently, accelerated DFT calculations provide a useful tool with great potentials for predicting the catalytic performance. </p> Graphical abstract <p></p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Computational screening-aided design of transition metal-doped CeO2 as NH3-SCR catalysts

  • 期刊论文

  • 发表日期：

    2025年6月30日

查看全文
  • Bo-Yu Wu,
  • Zhuo-Shen Huang,
  • Dan-Feng Zhao,
  • Fa-Jie Hu,
  • Bao-Xiang Peng,
  • Ning Pu,
  • Shen-Gen Zhang,
  • Xiu-Bing Huang

摘要

Transition metal-doped CeO2 catalysts exhibit great potentials for the selective catalytic reduction (SCR) of nitrogen oxide (NOx) with NH3 (NH3-SCR). However, traditional research mainly relies on a lot of experiments to find out effective catalysts, which wastes a lot of time and resources. Screening out effective CeO2-based catalysts for low-temperature NH3-SCR via density functional theory (DFT) calculations is crucial for the rational design and synthesis of efficient catalysts. Herein, transition metal (M = Co, Cr, Cu, Fe, Mn, Mo, Nb, Ni, Ta, Ti, V, and W)-doped CeO2 catalysts were screened out via accelerated DFT calculations for NH3-SCR of nitric-oxide (NO) using three theoretical terms; (i) an adsorption energy of NH3, (ii) an adsorption energy of NO, and (iii) the reaction energies between NO with O2 and lattice oxygen. The theoretically predicted trend in catalytic performance is as follows: CeO2-Mn, -Cu, -Mo > CeO2-Fe, -Co, -Ni, -V, -Cr > CeO2-W, -Ti > CeO2-Nb, -Ta. The theoretical prediction was well verified via experimental NH3-SCR activity of NO at low temperatures (90–300 °C), demonstrating CeO2-Mo as efficient NH3-SCR catalyst across a broad temperature range. Temperature-programmed desorption of NH3 and in situ diffuse reflectance infrared Fourier transforms spectroscopy further indicated that metal doping significantly enhanced the NH3 adsorption capacity and strength of CeO2 in the medium- to low-temperature range. Consequently, accelerated DFT calculations provide a useful tool with great potentials for predicting the catalytic performance.

Graphical abstract