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<p>Enzyme compartmentalization is a ubiquitous biochemical mechanism that nature uses to perform simultaneous but chemically incompatible metabolic processes in physically separated environments. However, it is a substantial challenge in homogeneous catalysis to spatially confine specific reaction components to prevent undesired pathways. Here we exploit the concept of compartmentalized enantioselective energy transfer catalysis by integrating artificial triplet photoenzymes and tailored triplet quenchers. The confined protein cavity was genetically encoded with a photosensitizer for enantioselective [2 + 2] photocycloaddition of 1-naphthol derivatives, while the outer bulk solution was modified with strategically introduced quenchers to inhibit the racemic background reaction induced by direct excitation, a fundamental challenge in asymmetric photocatalysis. This study not only expands the repertoire of artificial photoenzymes but also introduces a distinctive biocatalytic approach for precisely controlling reaction processes with spatial resolution, a capability that is usually unattainable in traditional chemocatalysis.</p><p></p>

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Enantioselective energy transfer catalysis compartmentalized by triplet photoenzymes

  • 期刊论文

  • 发表日期：

    2025年10月24日

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  • Xinjie Yang,
  • Juan Guo,
  • Junyi Qian,
  • Jianjian Huang,
  • Juan Shi,
  • Miao Jiang,
  • Junshuai Zhang,
  • Tengfei Pang,
  • Ningning Sun,
  • Yu Fu,
  • Weining Zhao,
  • Guojiao Wu,
  • Xi Chen,
  • Yuzhou Wu,
  • Fangrui Zhong

摘要

Enzyme compartmentalization is a ubiquitous biochemical mechanism that nature uses to perform simultaneous but chemically incompatible metabolic processes in physically separated environments. However, it is a substantial challenge in homogeneous catalysis to spatially confine specific reaction components to prevent undesired pathways. Here we exploit the concept of compartmentalized enantioselective energy transfer catalysis by integrating artificial triplet photoenzymes and tailored triplet quenchers. The confined protein cavity was genetically encoded with a photosensitizer for enantioselective [2 + 2] photocycloaddition of 1-naphthol derivatives, while the outer bulk solution was modified with strategically introduced quenchers to inhibit the racemic background reaction induced by direct excitation, a fundamental challenge in asymmetric photocatalysis. This study not only expands the repertoire of artificial photoenzymes but also introduces a distinctive biocatalytic approach for precisely controlling reaction processes with spatial resolution, a capability that is usually unattainable in traditional chemocatalysis.