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<p>Photo-redox catalysis has emerged as a new generation of biochemical protocols in proximity labeling, noninvasive therapy, ultrafast activation. However, the well-developed photocatalysts cannot simultaneously possess low-energy absorption and high excited potentials to initiate photochemical reactions. Herein, we develop new Ru-PCs as bio-photocatalyst exhibiting both green-light absorption and high <i>E</i><sub><i>red</i></sub><i>*</i>. Ru-PCs cooperatively function with natural coenzyme riboflavin (RF) via an integrated proton-coupled electron transfer (PCET) process to in situ transform Ru-PCs with two distinct ligands and consecutively mediate redox between phenol substrates, excited photocatalysts and oxygen. One quaternized (Qn) ligand keeps the metal-to-ligand-charge-transfer (MLCT) and the other carbonylated (Cb) ligand reserves a proton transfer site. Irradiating RuQnCb bio-photocatalyst leads to a highly selective neolignan oxidative intermolecular cross-coupling reaction of [4 + 2] cyclization of two phenol modules in diluted serum. Photo-modification of proteins has been accomplished within several seconds green light irradiation in a 97 % yield, without non-target conjugations to natural groups.</p>

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Coenzyme-functionalized photo-redox catalysis for low-energy click labeling

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月14日

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  • Kui Xiao,
  • Ni-Yuan Zhang,
  • Ke-Ting Zhou,
  • Jia-Long Chen,
  • Zhuan Wen,
  • Yu Xia,
  • Hao Wang,
  • Chen-Ho Tung,
  • Li-Zhu Wu

摘要

Photo-redox catalysis has emerged as a new generation of biochemical protocols in proximity labeling, noninvasive therapy, ultrafast activation. However, the well-developed photocatalysts cannot simultaneously possess low-energy absorption and high excited potentials to initiate photochemical reactions. Herein, we develop new Ru-PCs as bio-photocatalyst exhibiting both green-light absorption and high Ered*. Ru-PCs cooperatively function with natural coenzyme riboflavin (RF) via an integrated proton-coupled electron transfer (PCET) process to in situ transform Ru-PCs with two distinct ligands and consecutively mediate redox between phenol substrates, excited photocatalysts and oxygen. One quaternized (Qn) ligand keeps the metal-to-ligand-charge-transfer (MLCT) and the other carbonylated (Cb) ligand reserves a proton transfer site. Irradiating RuQnCb bio-photocatalyst leads to a highly selective neolignan oxidative intermolecular cross-coupling reaction of [4 + 2] cyclization of two phenol modules in diluted serum. Photo-modification of proteins has been accomplished within several seconds green light irradiation in a 97 % yield, without non-target conjugations to natural groups.