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<p>Macroporous adsorption resin (MR) offers numerous advantages, including a large specific surface area, good tolerance to organic solvents as well as low cost, thus making it an excellent carrier for immobilized catalysts. For the first time, Pd single atoms were immobilized onto MR as a highly active heterogeneous racemization catalyst (a single-atom catalyst), coupling with the immobilized lipase CHIRALZYME IM-100. This combination has led to the development of a highly efficient and cost-effective dynamic kinetic resolution (DKR) protocol. In the DKR of phenylethylamine, a 100% amide yield and 100% enantiomeric excess (ee) were achieved under zero gauge pressure of hydrogen at 60 ℃. Furthermore, the yield remained at 87.6% at 5&#xa0;h after the 7th cycle. According to the comparison of a simple data group EP, this racemization catalyst demonstrates the highest activity among several Pd-based racemization catalysts reported in the literature. With <i>R</i><sup>2</sup> of 0.9991 and <i>p</i>-value of &lt; 0.0001, a model was established to correlate amide yield with Pd-MR dosage, reaction time, and the concentration of Na₂PdCl₄ solution in adsorption. Through response surface methodology (RSM) optimization, the optimal loading ratio of palladium to enzyme was determined, effectively reducing palladium usage.</p>

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A Chemoenzymatic DKR Protocol with Pd Single Atoms as Racemization Catalyst

  • 期刊论文

  • 发表日期：

    2026年3月30日

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  • Xiaoying Zhang,
  • Xin Gao,
  • Shifang Xu,
  • Yunlong Zhang,
  • Shiyang Wen,
  • Junhong Liu,
  • Fanye Wang,
  • Yuanyuan Zhang

摘要

Macroporous adsorption resin (MR) offers numerous advantages, including a large specific surface area, good tolerance to organic solvents as well as low cost, thus making it an excellent carrier for immobilized catalysts. For the first time, Pd single atoms were immobilized onto MR as a highly active heterogeneous racemization catalyst (a single-atom catalyst), coupling with the immobilized lipase CHIRALZYME IM-100. This combination has led to the development of a highly efficient and cost-effective dynamic kinetic resolution (DKR) protocol. In the DKR of phenylethylamine, a 100% amide yield and 100% enantiomeric excess (ee) were achieved under zero gauge pressure of hydrogen at 60 ℃. Furthermore, the yield remained at 87.6% at 5 h after the 7th cycle. According to the comparison of a simple data group EP, this racemization catalyst demonstrates the highest activity among several Pd-based racemization catalysts reported in the literature. With R2 of 0.9991 and p-value of < 0.0001, a model was established to correlate amide yield with Pd-MR dosage, reaction time, and the concentration of Na₂PdCl₄ solution in adsorption. Through response surface methodology (RSM) optimization, the optimal loading ratio of palladium to enzyme was determined, effectively reducing palladium usage.