Energy band tunable piezoelectric nanozyme heterojunction toward cancer synergistic catalytic therapy.

Abstract

Piezoelectric catalytic therapy (PCT) based on piezoelectric semiconductors provides a new approach for cancer therapy. Various researches have explored the construction of heterojunction structures with nanozymes to strengthen PCT effect via accelerating electron transfer kinetics and synergistic nanozyme catalysis therapy (NCT). However, limited by the fixed energy band structure of nanozymes, the selectable piezoelectric semiconductors and nanozymes with matched energy levels are few. In this work, Cu2+ engineered nanozyme MIL-100 (Fe) was self-assembled on the surface of piezoelectric material BaTiO3 (BTO) to obtain BaTiO3@MIL-100 (Fe, Cu) (BTO@Fe-Cu) nanoparticles (NPs) with flexible heterojunction types, which presented synergetic NCT and PCT effect. Theoretical calculations revealed that Cu2+ introduced a new 3d orbital in the Fe-O structure, which altered the charge transfer pathways and enhanced the dual-enzyme activity of MIL-100 (Fe). Lattice distortion further modulated the valence band gap and transformed the heterostructure from type-Ⅰ to type-S for high electron-hole separation efficiency. BTO@Fe-Cu NPs fundamentally intensified the efficiency of NCT and PCT, which synergistically activated the ferroptosis/cuproptosis pathways. Moreover, scRNA-seq analysis indicated treatment-associated changes in immune-cell composition and transcriptional states. Together with the immunophenotyping results, these findings supported the potential of the piezoelectric nanozyme for the immunosuppressive tumor microenvironment (TME) regulation.

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