Catechol-Isolated Atomically Dispersed Nanocatalysts for Self-Motivated Cocatalytic Tumor Therapy

Dr. Yuemei Wang, Shuwen Qiu, Dr. Liping Wang, Dr. Penghao Ji, Dr. Yuedong Guo, Heliang Yao, Chenyang Wei, Prof. Minfeng Huo, Prof. Jianlin Shi
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Abstract

Nanocatalytic tumor therapy based on Fenton nanocatalysts has attracted considerable attention because of its therapeutic specificity, enhanced outcomes, and high biocompatibility. Nevertheless, the rate-determining step in Fenton chemistry, which involves the transition of a high-valence metallic center (FeIII) to a Fenton-active low-valence metallic center (FeII), has hindered advances in nanocatalyst-based therapeutics. In this study, we constructed mesoporous single iron atomic nanocatalysts (mSAFe NCs) by employing catechols from dopamine to coordinate and isolate single iron atoms. The catechols also serve as reductive ligands, generating a field-effect-based cocatalytic system that instantly reduces FeIII species to FeII species within the mSAFe NCs. This self-motivated cocatalytic strategy enabled by mSAFe NCs accelerates the kinetics of the Fenton catalytic reaction, resulting in remarkable performance for nanocatalytic tumor therapy both in vitro and in vivo.

Abstract Image

用于自发催化肿瘤治疗的儿茶酚分离型原子分散纳米催化剂
基于芬顿纳米催化剂的纳米催化肿瘤疗法因其治疗特异性、增强疗效和高度生物相容性而备受关注。然而,芬顿化学的速率决定步骤涉及高价金属中心(FeIII)向芬顿活性低价金属中心(FeII)的转变,这阻碍了基于纳米催化剂的治疗方法的发展。在本研究中,我们利用多巴胺中的儿茶酚来配位和分离单个铁原子,从而构建了介孔单铁原子纳米催化剂(mSAFe NCs)。儿茶酚还可作为还原配体,产生一个基于场效应的协同催化系统,在 mSAFe NCs 内瞬间将 FeIII 物种还原为 FeII 物种。这种由 mSAFe NCs 实现的自激协同催化策略加快了芬顿催化反应的动力学过程,从而使纳米催化肿瘤治疗在体外和体内都表现出卓越的性能。
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来源期刊
Angewandte Chemie
Angewandte Chemie 化学科学, 有机化学, 有机合成
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