TY - JOUR
T1 - Multiple therapeutic mechanisms of pyrrolic N-rich g-C3N4 nanosheets with enzyme-like function in the tumor microenvironment
AU - Song, Shanshan
AU - Yang, Miao
AU - He, Fei
AU - Zhang, Xiao
AU - Gao, Yijun
AU - An, Baichao
AU - Ding, He
AU - Gai, Shili
AU - Yang, Piaoping
N1 - Funding Information:
Financial support from the National Natural Science Foundation of China (NSFC51972075 and 22275045), Natural Science Foundation of Shandong Province (ZR2019ZD29), and the Fundamental Research funds for the Central Universities are greatly acknowledged.
Publisher Copyright:
© 2023 Elsevier Inc.
PY - 2023/11/15
Y1 - 2023/11/15
N2 - Nanozyme-based synergistic catalytic therapies for tumors have attracted extensive research attention. However, the unsatisfactory efficiency and negative impact of the tumor microenvironment (TME) hinder its clinical applications. In this study, we provide an easy method to prepare transition metals loaded onto pyrrolic nitrogen-rich g-C3N4 (PN-g-C3N4) for forming metal-N4 sites. This N-rich material effectively transfers electrons from g-C3N4 to metal-N4 sites, promotes the oxidation–reduction reaction of metals with different valence states, and improves material reusability. Under TME conditions, copper ions loaded onto PN-g-C3N4 (Cu-PN-g-C3N4, CPC) can produce ·OH through a Fenton-like reaction for tumor inhibition. This Fenton-like reaction and tumor cell inhibition can be improved further by a photodynamic effect caused by light irradiation. We introduced upconversion nanoparticles (UCNPs) into CPC to obtain nano-enzymes (UCNPs@Cu-PN-g-C3N4, UCPC) for effectively penetrating the tissue, which emits light corresponding to the UV absorption region of CPC when excited with 980 nm near-infrared (NIR) light. The nanoplatform can reduce H2O2 concentration upon exposure to NIR light; this induces an increase in dissolved oxygen content and produces a higher supply of reactive oxygen species (ROS) for destroying tumor cells. Owing to the narrow bandgap (1.92 eV) of UCPC under 980 light irradiation, even under the condition of hypoxia, the excited electrons in the conduction band can reduce insoluble O2 through a single electron transfer process, thus effectively generating O2•–. Nanoenzyme materials with catalase properties produce three types of ROS (·OH, O2•– and 1O2) when realizing chemodynamic and photodynamic therapies. An excellent therapeutic effect was established by killing cells in vitro and the tumor-inhibiting effect in vivo, proving that the prepared nanoenzymes have an effective therapeutic effect and that the endogenous synergistic treatment of multiple treatment technologies can be realized.
AB - Nanozyme-based synergistic catalytic therapies for tumors have attracted extensive research attention. However, the unsatisfactory efficiency and negative impact of the tumor microenvironment (TME) hinder its clinical applications. In this study, we provide an easy method to prepare transition metals loaded onto pyrrolic nitrogen-rich g-C3N4 (PN-g-C3N4) for forming metal-N4 sites. This N-rich material effectively transfers electrons from g-C3N4 to metal-N4 sites, promotes the oxidation–reduction reaction of metals with different valence states, and improves material reusability. Under TME conditions, copper ions loaded onto PN-g-C3N4 (Cu-PN-g-C3N4, CPC) can produce ·OH through a Fenton-like reaction for tumor inhibition. This Fenton-like reaction and tumor cell inhibition can be improved further by a photodynamic effect caused by light irradiation. We introduced upconversion nanoparticles (UCNPs) into CPC to obtain nano-enzymes (UCNPs@Cu-PN-g-C3N4, UCPC) for effectively penetrating the tissue, which emits light corresponding to the UV absorption region of CPC when excited with 980 nm near-infrared (NIR) light. The nanoplatform can reduce H2O2 concentration upon exposure to NIR light; this induces an increase in dissolved oxygen content and produces a higher supply of reactive oxygen species (ROS) for destroying tumor cells. Owing to the narrow bandgap (1.92 eV) of UCPC under 980 light irradiation, even under the condition of hypoxia, the excited electrons in the conduction band can reduce insoluble O2 through a single electron transfer process, thus effectively generating O2•–. Nanoenzyme materials with catalase properties produce three types of ROS (·OH, O2•– and 1O2) when realizing chemodynamic and photodynamic therapies. An excellent therapeutic effect was established by killing cells in vitro and the tumor-inhibiting effect in vivo, proving that the prepared nanoenzymes have an effective therapeutic effect and that the endogenous synergistic treatment of multiple treatment technologies can be realized.
KW - Catalase-like nanozymes
KW - Photodynamic therapy
KW - Tumor catalytic therapy
KW - Tumor microenvironment-adjusted
UR - http://www.scopus.com/inward/record.url?scp=85165234390&partnerID=8YFLogxK
U2 - 10.1016/j.jcis.2023.06.177
DO - 10.1016/j.jcis.2023.06.177
M3 - Journal article
C2 - 37473473
AN - SCOPUS:85165234390
SN - 0021-9797
VL - 650
SP - 1125
EP - 1137
JO - Journal of Colloid and Interface Science
JF - Journal of Colloid and Interface Science
ER -