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Harvard Medical School / UC Berkeley

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Adv. Mater., Jul 04 2025, | https://doi.org/10.1002/adma.202418134 Photoinduced Plasmon Electron Transfer-based Bioorthogonal Cleavage Reaction for Precision Tumor Therapy

Subin Yu ^1,2, Dohyub Jang^3,4, Haeun Kang ¹, Heejun Lee ⁵, Jihye Park ⁵, Honghwan Choi ³, Wen-Tse Huang ⁶, Minju Kim ¹, Kyungwha Chung^2,7, Dong June Ahn^4,6, Ru-Shi Liu⁸, Joonho Bang ^5,9, Sehoon Kim ^3,10, Luke P. Lee ^1,2,7, Dong Ha Kim^{1,11,12,13,14}

¹Department of Chemistry and Nanoscience, Ewha Womans University, Seoul, 03760, Republic of Korea.
²Harvard Institute of Medicine, Harvard Medical School, Harvard University, Brigham and Women's Hospital, Boston, MA, 02115, USA.
³Chemical and Biological Integrative Research Center, Korea Institute of Science and Technology, 5 Hwarang-ro 14-Gil, Seongbuk-gu, Seoul, 02792, Republic of Korea.
⁴Department of Biomicrosystem Technology, Korea University, Seoul, 136-701, Republic of Korea.
⁵Department of Materials Engineering and Convergence Technology, Gyeongsang National University, Jinju, 52828, Republic of Korea.
⁶Department of Chemical and Biological Engineering, Korea University, Seoul, 02841, Republic of Korea.
⁷Institute of Quantum Biophysics, Department of Biophysics, Sungkyunkwan University, Suwon, 16419, Republic of Korea.
⁸Department of Chemistry, National Taiwan University, Taipei, 106, Taiwan.
⁹School of Materials Science and Engineering, Gyeongsang National University, Jinju, 52828, Republic of Korea.
¹⁰KU-KIST Graduate School of Converging Science and Technology, Korea University, Seoul, 02841, Republic of Korea.
¹¹Basic Sciences Research Institute (Priority Research Institute), Ewha Womans University, 52, Ewhayeodae-gil, Seodaemun-gu, Seoul, 03760, Republic of Korea.
¹²Nanobio∙Energy Materials Center (National Research Facilities and Equipment Center), Ewha Womans University, 52, Ewhayeodae-gil, Seodaemun-gu, Seoul, 03760, Republic of Korea.
¹³College of Medicine, Ewha Womans University, 25, Magokdong-ro 2-gil, Gangseo-gu, Seoul, 07804, Republic of Korea.
¹⁴Gradutate Program in Innovative Biomaterials Convergence, Ewha Womans University, 52 Ewhayeodae-gil, Seodaemun-gu, Seoul, 03760, Republic of Korea.

S.U. and D.J. contributed equally to this work.
Corresponding Authors: Ru-Shi Liu, Joonho Bang, Sehoon Kim, Luke P. Lee, Dong Ha Kim

Abstract

Photocatalytic reactions have been harnessed to develop advanced medical solutions for transformative cancer therapy. However, their limited catalytic activities within biological environments must be enhanced to maximize their potential in practical applications. Here, a spatiotemporally controllable photocatalytic cancer therapy is reported through the photoinduced plasmon electron transfer (PiPET)-based biorthogonal cleavage reaction of a pro-photosensitizer, allyl carbamate-conjugated methylene blue (MB). The electron transfer in Pd-conjugated Au nanobipyramids is examined to improve catalytic activity by simulating the energy differences between the desorbed and adsorbed states, bond distances, and charge densities with and without excess electrons. A significantly enhanced release of allyl carbamate-conjugated methylene blue is achieved by ninefold and demonstrated precise spatiotemporal control of the bioorthogonal reaction in vivo. Both in vitro and in vivo studies reveal the remarkable tumor-suppressing capability of the bioorthogonal system, which is attributed to the photothermal and PiPET effects, coupled with the prevention of leuko-MB formation. The PiPET-based bioorthogonal cleavage reaction can offer an innovative solution for precise tumor therapy using spatiotemporal phototherapeutic strategies.

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