Dual Regulation of Energy/Electron Transfer in MOF@COP Heterojunctions through Ingenious Molecular Engineering for Enhanced Sonodynamic Cancer Therapy

IF 9.6 1区化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Materials Letters Pub Date : 2024-08-20 DOI:10.1021/acsmaterialslett.4c01035

Jiwei Wang, Sainan Liu, Qi Meng, Zhendong Liu, Wenying Zhang, Jia Tan, Binbin Ding, Ping’an Ma, Jun Lin

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Abstract

Sonosensitization-mediated reactive oxygen species generation associated with energy and electron transfer is an essential process of sonodynamic therapy. However, the development of sonosensitizers with both high intersystem crossing (ISC) rates and efficient carrier separation remains greatly challenging. Herein, we present a new scheme to construct a class of heterojunctions (MC-R, R = −H, −OCH₃, −Br) by Zr-based metal–organic framework (NU-901) and porphyrin-based covalent organic polymers (COPs) with different substituents. In this sonocatalytic system, the type-II heterojunction based on NU-901 and COPs can effectively promote the separation of electron–hole pairs, increasing the generation of superoxide anions, while the introduction of substituents (−OCH₃, −Br) can extend the conjugation of COPs by p-π binding and enhance spin–orbit coupling through heavy atom effects, which could regulate the ISC process and improve the quantum yield of singlet oxygen. Remarkably, MC-Br as a representative MC-R exhibits the best tumor inhibition efficiency in vivo.

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通过巧妙的分子工程设计实现 MOF@COP 异质结中能量/电子转移的双重调控，从而增强癌症的声动力疗法

声敏化介导的活性氧生成与能量和电子转移有关，是声动力疗法的重要过程。然而，开发同时具有高系统间穿越（ISC）率和高效载流子分离的声敏化剂仍面临巨大挑战。在此，我们提出了一种新方案，通过锆基金属有机框架（NU-901）和具有不同取代基的卟啉基共价有机聚合物（COPs）来构建一类异质结（MC-R，R = -H、-OCH3、-Br）。在该声催化体系中，基于 NU-901 和 COPs 的 II 型异质结能有效促进电子-空穴对的分离，增加超氧阴离子的生成，而取代基（-OCH3、-Br）的引入能通过 p-π 结合扩展 COPs 的共轭作用，并通过重原子效应增强自旋轨道耦合，从而调节 ISC 过程，提高单线态氧的量子产率。值得注意的是，MC-Br 作为 MC-R 的代表，在体内表现出最佳的肿瘤抑制效率。

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来源期刊

ACS Materials Letters MATERIALS SCIENCE, MULTIDISCIPLINARY-

CiteScore

14.60

自引率

3.50%

发文量

261

期刊介绍： ACS Materials Letters is a journal that publishes high-quality and urgent papers at the forefront of fundamental and applied research in the field of materials science. It aims to bridge the gap between materials and other disciplines such as chemistry, engineering, and biology. The journal encourages multidisciplinary and innovative research that addresses global challenges. Papers submitted to ACS Materials Letters should clearly demonstrate the need for rapid disclosure of key results. The journal is interested in various areas including the design, synthesis, characterization, and evaluation of emerging materials, understanding the relationships between structure, property, and performance, as well as developing materials for applications in energy, environment, biomedical, electronics, and catalysis. The journal has a 2-year impact factor of 11.4 and is dedicated to publishing transformative materials research with fast processing times. The editors and staff of ACS Materials Letters actively participate in major scientific conferences and engage closely with readers and authors. The journal also maintains an active presence on social media to provide authors with greater visibility.