<p>Photocatalytic CO<sub>2</sub> reduction to ethanol has practical value and represents a promising route toward carbon neutrality. However, there are great challenges to realizing CO<sub>2</sub>-to-ethanol conversion to date. In this work, a photocatalyst PPU/CdS, composed of a Zr-MOF UiO-66-NH<sub>2</sub> decorated with PdPt alloy nanoparticles and coupled with CdS photosensitizer, was developed, achieving a remarkable ethanol production rate of 182.6 µmol g<sup>−1</sup> h<sup>−1</sup>, which is superior to most of the reported systems. <i>In situ</i> infrared spectroscopy and theoretical calculations revealed the origin of the high performance: the detection of *OCCO intermediate ensures that *CO species undergoes further coupling, rather than releases as CO in the conventional pathway, because of the low energy barrier of 1.17 eV for the coupling step on PPU/CdS. Meanwhile, the presence of Pt greatly accelerates electron transfer, resulting in a significantly higher ethanol production for PPU/CdS compared to the P+PU/CdS catalyst, in which the Pd and Pt NPs exist individually.</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

Synergistic bimetallic nanoparticle-MOF photocatalyst for ethanol production via carbon dioxide reduction

  • Xiang-Yu Lu,
  • Qiang Zhou,
  • Kai-Yang Zhang,
  • Jing-Shan Fan,
  • Feng Gong,
  • Wei-Yin Sun

摘要

Photocatalytic CO2 reduction to ethanol has practical value and represents a promising route toward carbon neutrality. However, there are great challenges to realizing CO2-to-ethanol conversion to date. In this work, a photocatalyst PPU/CdS, composed of a Zr-MOF UiO-66-NH2 decorated with PdPt alloy nanoparticles and coupled with CdS photosensitizer, was developed, achieving a remarkable ethanol production rate of 182.6 µmol g−1 h−1, which is superior to most of the reported systems. In situ infrared spectroscopy and theoretical calculations revealed the origin of the high performance: the detection of *OCCO intermediate ensures that *CO species undergoes further coupling, rather than releases as CO in the conventional pathway, because of the low energy barrier of 1.17 eV for the coupling step on PPU/CdS. Meanwhile, the presence of Pt greatly accelerates electron transfer, resulting in a significantly higher ethanol production for PPU/CdS compared to the P+PU/CdS catalyst, in which the Pd and Pt NPs exist individually.