Journal
SMALL METHODS
Volume 4, Issue 7, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smtd.202000013
Keywords
electron-donating; hypoxic tumor; intersystem crossing; O-2(center dot-) photogeneration; type I photodynamic therapy
Funding
- National Natural Science Foundation of China [61525402, 61775095, 51703187]
- Jiangsu Provincial key research and development plan [BE2017741]
- Jiangsu Province Policy Guidance Plan [BZ2019014]
- Six talent peak innovation team in Jiangsu Province [TD-SWYY-009]
- Jiangsu Provincial Graduated Training Innovation Project [KYCX19_0862]
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Tumor hypoxia severely impedes the therapeutic efficacy of type II photodynamic therapy (PDT) depending on singlet oxygen (O-1(2)) generation. To combat hypoxic tumors, herein, a new approach is devised to boost superoxide radical (O-2(center dot-)) photogeneration for type I PDT. Heavy atoms are introduced onto aza-BODIPY molecules (iodine substituted butoxy-aza-BODIPY, IBAB) to promote their intersystem-crossing (ISC) ability. Meanwhile, methoxy-poly(ethylene glycol)-b-poly(2-(diisopropylamino) ethyl methacrylate) (mPEG-PPDA) with enhanced electron-donating efficiency is employed as a coating matrix to encapsulate IBAB, thereby obtaining amphiphilic aza-BODIPY nanoplatforms (PPIAB NPs). Under irradiation, triplet-state IBAB in PPIAB NPs is efficiently generated from singlet state favored by the elevated ISC ability. The electron-rich environment provided by mPEG-PPDA can donate triplet-state IBAB with one electron to form charge-separated-state IBAB, which in turn transfers electron to O-2 for O-2(center dot-) production. Significantly, owing to recyclable O-2 generated by disproportionation or Harber-Weiss/Fenton reaction, prominent O-2(center dot-) is generated by PPIAB NPs even in a severe hypoxic environment (2% O-2), enabling superior therapeutic efficacy (96.2% tumor-inhibition rate) over NPs not following this strategy. Thus, the proof-of-concept design of ISC-enhanced and electron-rich polymer encapsulating PPIAB NPs illuminates the path to preparing O-2(center dot-) photogenerator for hypoxic cancer treatment.
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