Scholarlink

<p>Controlling the intrinsic activity and long-term stability of active sites is essential to advance the formulation of catalysts. The hydrogenation of CO<sub>2</sub> to methanol over indium oxide (In<sub>2</sub>O<sub>3</sub>) is believed to proceed at oxygen vacancies (V<sub>O</sub><sup>∙∙</sup>) formed in situ. Here, we study how the structural dynamics of <i>c</i>-In<sub>2</sub>O<sub>3</sub> are altered through doping with Sn or Zr, affecting the local structure, catalytic activity, and stability. We find that V<sub>O</sub><sup>∙∙</sup> sites in Sn-doped <i>c</i>-In<sub>2</sub>O<sub>3</sub> are unreactive towards their replenishment by CO<sub>2</sub>, leading to catalyst deactivation by the formation of In<sup>0</sup> and Sn<sup>0</sup>. Conversely, V<sub>O</sub><sup>∙∙</sup> sites in Zr-doped <i>c</i>-In<sub>2</sub>O<sub>3</sub> show a high reactivity towards CO<sub>2</sub>, translating into a high catalytic activity and stability against over-reduction-induced deactivation. The diverging properties originate from the distinct defect dynamics in these two materials. The balance between V<sub>O</sub><sup>∙∙</sup> formation and its replenishment during CO<sub>2</sub> hydrogenation is the key characteristic for both activity and stability of In<sub>2</sub>O<sub>3</sub>-based catalysts.</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

Dopant-controlled oxygen vacancy dynamics define CO2-to-methanol catalysis on In2O3

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年5月14日

查看全文
  • Matthias Becker,
  • Margareth S. Baidun,
  • Annelies Landuyt,
  • Agnieszka Kierzkowska,
  • Felix Donat,
  • Alexander A. Kolganov,
  • Evgeny A. Pidko,
  • Paula M. Abdala,
  • Alexey Fedorov,
  • Christoph R. Müller

摘要

Controlling the intrinsic activity and long-term stability of active sites is essential to advance the formulation of catalysts. The hydrogenation of CO2 to methanol over indium oxide (In2O3) is believed to proceed at oxygen vacancies (VO∙∙) formed in situ. Here, we study how the structural dynamics of c-In2O3 are altered through doping with Sn or Zr, affecting the local structure, catalytic activity, and stability. We find that VO∙∙ sites in Sn-doped c-In2O3 are unreactive towards their replenishment by CO2, leading to catalyst deactivation by the formation of In0 and Sn0. Conversely, VO∙∙ sites in Zr-doped c-In2O3 show a high reactivity towards CO2, translating into a high catalytic activity and stability against over-reduction-induced deactivation. The diverging properties originate from the distinct defect dynamics in these two materials. The balance between VO∙∙ formation and its replenishment during CO2 hydrogenation is the key characteristic for both activity and stability of In2O3-based catalysts.