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<p>Ligand modification of Cu catalysts has emerged as a promising strategy to enhance activity and stability in acetylene hydrochlorination. However, the limited availability of primary coordinating heteroatoms hinders precise engineering of the Cu active site microenvironment. Herein, a secondary coordination sphere modulation strategy was developed using various substituted hydrocarbon groups in the ligands. The local microenvironment around the Cu active sites was precisely tuned, leading to the Cu<sup>+</sup> ratio of freshly prepared catalysts and reactive activity revealing a linear correlation, and the C<sub>2</sub>H<sub>2</sub> adsorption energy exhibiting a distinct volcano plot correlation with catalytic activity. Among these catalysts, Cu-MMTB/AC exhibited the highest activity, achieving an acetylene conversion of 88.5% under the reaction conditions (T = 180 °C, gas hourly space velocity (GHSV) (C<sub>2</sub>H<sub>2</sub>) = 180 h<sup>−1</sup>, and <i>V</i>(HCl): <i>V</i>(C<sub>2</sub>H<sub>2</sub>) = 1.2). Moreover, <sup>1#</sup>Cu<sub>3</sub>-MMTB<sub>1</sub> exhibits advantages in both intermediate formation and HCl activation processes along the reaction pathway. This strategy offers a new avenue for designing high-performance Cu catalysts and promoting the use of mercury-free industrial catalysts.</p>

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Modulating the secondary coordination sphere of the Cu site for boosting acetylene hydrochlorination

  • 期刊论文

  • 发表日期：

    2025年7月1日

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  • Dingqiang Feng,
  • Linfeng Li,
  • Yunsheng Dai,
  • Wei Li,
  • Jinli Zhang,
  • Bao Wang,
  • Jiangjiexing Wu

摘要

Ligand modification of Cu catalysts has emerged as a promising strategy to enhance activity and stability in acetylene hydrochlorination. However, the limited availability of primary coordinating heteroatoms hinders precise engineering of the Cu active site microenvironment. Herein, a secondary coordination sphere modulation strategy was developed using various substituted hydrocarbon groups in the ligands. The local microenvironment around the Cu active sites was precisely tuned, leading to the Cu+ ratio of freshly prepared catalysts and reactive activity revealing a linear correlation, and the C2H2 adsorption energy exhibiting a distinct volcano plot correlation with catalytic activity. Among these catalysts, Cu-MMTB/AC exhibited the highest activity, achieving an acetylene conversion of 88.5% under the reaction conditions (T = 180 °C, gas hourly space velocity (GHSV) (C2H2) = 180 h−1, and V(HCl): V(C2H2) = 1.2). Moreover, 1#Cu3-MMTB1 exhibits advantages in both intermediate formation and HCl activation processes along the reaction pathway. This strategy offers a new avenue for designing high-performance Cu catalysts and promoting the use of mercury-free industrial catalysts.