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<p>The ammoximation of cyclohexanone using a Ti‑zeolite/H<sub>2</sub>O<sub>2</sub> system, coupled with a Beckmann rearrangement, is now commercially employed to produce ε‑caprolactam—a critical precursor for the synthesis of Nylon 6. The in situ generation of H<sub>2</sub>O<sub>2</sub> integrated with the titanosilicate-catalysed ammoximation of cyclohexanone can eliminate the need for transportation and storage of concentrated H<sub>2</sub>O<sub>2</sub>, mitigating the economic and environmental costs associated with its production via the conventional anthraquinone process. Here we present a titanium-mordenite‑confined low-Pd-loaded catalyst with subnanometric Pd clusters within specific pores, enabling direct cyclohexanone ammoximation with H<sub>2</sub> and O<sub>2</sub>. With only 0.055 wt% Pd, this catalyst maintains exceptional stability for over 4,020 h of continuous ammoximation with H<sub>2</sub> and O<sub>2</sub>, achieving 99% oxime selectivity even in H<sub>2</sub>O. Our work contributes to the development of an alternative ammoximation route that minimizes precious-metal usage, reducing reliance on both organic solvents and H<sub>2</sub>O<sub>2</sub>, and paves the way towards a more eco-efficient process for ε-caprolactam production.</p><p></p>

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Titanium mordenite-confined low-loaded Pd for efficient oxime production with H2 and O2

  • 期刊论文

  • 发表日期：

    2026年1月8日

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  • Zhipeng Wan,
  • Qingjie Zeng,
  • Zhuoya Dong,
  • Yue Ma,
  • Jicong Yan,
  • Xiang Wang,
  • Chengwei Zhai,
  • Haoyi Lin,
  • Mingbin Gao,
  • Jiangwei Zhang,
  • Yanhang Ma,
  • Hao Xu,
  • Lansun Zheng,
  • Peng Wu

摘要

The ammoximation of cyclohexanone using a Ti‑zeolite/H2O2 system, coupled with a Beckmann rearrangement, is now commercially employed to produce ε‑caprolactam—a critical precursor for the synthesis of Nylon 6. The in situ generation of H2O2 integrated with the titanosilicate-catalysed ammoximation of cyclohexanone can eliminate the need for transportation and storage of concentrated H2O2, mitigating the economic and environmental costs associated with its production via the conventional anthraquinone process. Here we present a titanium-mordenite‑confined low-Pd-loaded catalyst with subnanometric Pd clusters within specific pores, enabling direct cyclohexanone ammoximation with H2 and O2. With only 0.055 wt% Pd, this catalyst maintains exceptional stability for over 4,020 h of continuous ammoximation with H2 and O2, achieving 99% oxime selectivity even in H2O. Our work contributes to the development of an alternative ammoximation route that minimizes precious-metal usage, reducing reliance on both organic solvents and H2O2, and paves the way towards a more eco-efficient process for ε-caprolactam production.