Biomimetically constructing a hypoxia-activated programmable phototheranostics at the molecular level

Zhang, Hang; Wu, Jiahui; Xue, Hao‐Zong; Zhang, Ruijing; Yang, Zi‐Shu; Gao, Song; Zhang, Junlong

doi:10.1039/d2sc02554j

Cited by 10 publications

(3 citation statements)

References 73 publications

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“…In comparison to control complex 57 , 56 produces dioxygen 6.8 times faster. The reaction occurs in PBS buffer at a pH of 7.4 In a following work, 56 has been combined with a photosensitizer to construct a programmable phototheranostics [81] …”

Section: Endohedral Group Acts As a Ligandmentioning

confidence: 99%

Reactions in Endohedral Functionalized Cages

Otte

2023

Eur J Org Chem

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The introduction of enhanced functionalization is a key aspect in the current design of cage chemistry. At the moment, several approaches are intensively investigated. The synthesis of cage compounds that display endohedral functionalization plays a key role among them. Here, the studies of reactions that occur in endohedral‐functionalized cage compounds is reviewed. After an introduction in current trends in cage‐chemistry the discussion of reactions in endohedral‐cage compounds is divided into three sections. These are: 1) Endohedral groups that are by themselves functional, 2) endohedral groups that can bind to a transition‐metal complex and 3) endohedral groups that can bind by themselves to a metal. The article closes with an outlook on additional current developments in the field of endohedral‐functionalized cage‐compounds, which may contribute in the future towards reactivity in cage compounds.

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Section: Endohedral Group Acts As a Ligandmentioning

confidence: 99%

Reactions in Endohedral Functionalized Cages

Otte

2023

Eur J Org Chem

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“…Introducing a metal center into an organic ligand framework via metal coordination offers an attractive means of designing PSs by allowing access to metal-centered excited states and reactivity. − Recent work from our laboratory ,, revealed that appropriately designed Ni(II) complexes can function as photothermal agents whose excited state energies can be dissipated via thermally accessible radiationless relaxation mechanisms, arising from their small d–d ligand-field splittings . Separate studies of Ni(II) complexes as metalloenzyme catalysts − led us to consider the possibility of using them to catalyze Fenton-like reactions intracellularly, thus reprograming the TME to be less immunosuppressive.…”

Section: Introductionmentioning

confidence: 99%

Nickel(II) Phototheranostics: A Case Study in Photoactivated H₂O₂-Enhanced Immunotherapy

Zhang,

Xu,

Yao

et al. 2023

J. Am. Chem. Soc.

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Phototheranostics have emerged as a promising subset of cancer theranostics owing to their potential to provide precise photoinduced diagnoses and therapeutic outcomes. However, the design of phototheranostics remains challenging due to the nature of tumors and their microenvironment, including limitations to the oxygen supply, high rates of recurrence and metastasis, and the immunosuppressive state of cancer cells.Here we report a dual-functional oxygen-independent phototheranostic agent, Ni-2, rationally designed to provide a near-infrared (NIR) photoactivated thermal-and hydroxyl radical (•OH)-enhanced photoimmunotherapeutic anticancer response. Under 880 nm laser irradiation, Ni-2 exhibited high photostability and excellent photoacoustic and photothermal effects with a photothermal conversion efficacy of 58.0%, as well as novel photoredox features that allowed the catalytic conversion of H 2 O 2 to •OH upon photooxidation of Ni(II) to Ni(III). As a multifunctional photoagent, Ni-2 was found not only to inhibit tumor growth in a CT26 tumor-bearing mouse model but also to activate an immune response via a combination of photothermal-and H 2 O 2 -induced effects. When combined with an antiprogrammed death-ligand 1 (aPD-L1), Ni-2 treatment allowed for the suppression of distant tumor growth and cancer metastasis. Collectively, the present results provide support for the proposition that Ni-2 or its analogues could emerge as useful tools for photoimmunotherapy. They also highlight the potential of appropriately designed 3d transition metal complexes as "all-inone" phototheranostics.

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“…In recent decades, photodynamic therapy (PDT) has received considerable attention for cancer treatment due to its ability to enhance cancer treatment through the generation of reactive oxygen species (ROS) upon light irradiation [1][2][3][4][5]. The photosensitizers (PSs) that are closely related to the effectiveness of PDT are especially critical [6][7][8][9]. When exposed to white light or laser, PSs can undergo type-II photochemical reactions to generate singlet oxygens ( 1 O 2 , energy transfer) or type-I reactions to generate toxic radicals (O 2…”

Section: Introductionmentioning

confidence: 99%

Precise ligand engineering of Ir(III)‐based photosensitizer with aggregation‐induced emission for image‐guided photodynamic therapy

Tong,

Liu,

Huang

et al. 2023

Luminescence

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Photodynamic therapy (PDT), which relies on the production of reactive oxygen species (ROS) induced by a photosensitizer to kill cancer cells, has become a non‐invasive approach to combat cancer. However, the conventional aggregation‐caused quenching effect, as well as the low ROS generation ability of photosensitizers, restrict their biological applications. In this work, a new Ir(III) complex with a dendritic ligand has been strategically designed and synthesized by ingenious modification of the ancillary ligand of a reported Ir(III) complex (Ir‐1). The extended π‐conjugation and multiple aromatic donor moieties endow the resulting complex Ir‐2 with obvious aggregation‐induced emission (AIE) activity and bathochromic emission. In in vitro experiments, importantly, Ir‐2 nanoparticles exhibit the excellent photoinduced ROS generation capabilities of O2•− and 1O2, as well as excellent biocompatibility and the lipid droplets (LDs) targeting feature. This study would provide useful guidance to design efficient Ir(III)‐based photosensitizers used in biological applications in the future.

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Biomimetically constructing a hypoxia-activated programmable phototheranostics at the molecular level

Abstract: A programmable strategy at the molecular level to modulate the ratio of a catalyst and photosensitizer to maximize the collaborative efficiency of anti-angiogenesis and PDT.

Cited by 10 publications

References 73 publications

Reactions in Endohedral Functionalized Cages

Reactions in Endohedral Functionalized Cages

Nickel(II) Phototheranostics: A Case Study in Photoactivated H₂O₂-Enhanced Immunotherapy

Precise ligand engineering of Ir(III)‐based photosensitizer with aggregation‐induced emission for image‐guided photodynamic therapy

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Biomimetically constructing a hypoxia-activated programmable phototheranostics at the molecular level

Abstract: A programmable strategy at the molecular level to modulate the ratio of a catalyst and photosensitizer to maximize the collaborative efficiency of anti-angiogenesis and PDT.

Cited by 10 publications

References 73 publications

Reactions in Endohedral Functionalized Cages

Reactions in Endohedral Functionalized Cages

Nickel(II) Phototheranostics: A Case Study in Photoactivated H2O2-Enhanced Immunotherapy

Precise ligand engineering of Ir(III)‐based photosensitizer with aggregation‐induced emission for image‐guided photodynamic therapy

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Nickel(II) Phototheranostics: A Case Study in Photoactivated H₂O₂-Enhanced Immunotherapy