Bioinspired Copper Single-Atom Catalysts for Tumor Parallel Catalytic Therapy

Bioinspired Copper Single-Atom Catalysts for Tumor Parallel Catalytic Therapy
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DOI:
10.1002/adma.202002246
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发表时间:
2020-07-23
期刊:
影响因子:
29.4
通讯作者:
Shi, Jianlin
Shi, Jianlin
中科院分区:
材料科学1区
文献类型:
--
作者:
Lu, Xiangyu;Gao, Shanshan;Shi, Jianlin

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活性氧(ROS)对细胞内生物分子的氧化形成了基于ROS的肿瘤治疗的基础。然而,目前的治疗方式不能同时催化H(2)O(2)和O(2)产生ROS,从而导致不令人满意的治疗效果。本文报道了一种具有生物启发性的掺杂有单原子铜物种的中空N掺杂碳球(Cu-HNCS),其可以直接催化氧气和过氧化氢分解为ROS,即超氧离子(O-2中心点(-))和羟基自由基(中心点OH),分别在酸性肿瘤微环境中用于在没有外部能量输入的情况下氧化细胞内生物分子,从而导致增强的肿瘤生长抑制作用。值得注意的是,Cu-HNCS中的Cu物质的芬顿反应周转频率比商业Fe(3)O(4)纳米颗粒中的Fe高约5000倍。实验结果和密度泛函理论计算表明,Cu-HNCS的高催化活性来源于单原子铜,计算结果预示了下一代芬顿催化剂的出现.这项工作提供了一个有效的范例,肿瘤平行催化治疗,大大提高治疗效果。
The oxidation of intracellular biomolecules by reactive oxygen species (ROS) forms the basis for ROS-based tumor therapy. However, the current therapeutic modalities cannot catalyze H(2)O(2)and O(2)concurrently for ROS generation, thereby leading to unsatisfactory therapeutic efficacy. Herein, it is reported a bioinspired hollow N-doped carbon sphere doped with a single-atom copper species (Cu-HNCS) that can directly catalyze the decomposition of both oxygen and hydrogen peroxide to ROS, namely superoxide ion (O-2 center dot(-)) and the hydroxyl radical (center dot OH), respectively, in an acidic tumor microenvironment for the oxidation of intracellular biomolecules without external energy input, thus resulting in an enhanced tumor growth inhibitory effect. Notably, the Fenton reaction turnover frequency of Cu species in Cu-HNCS is approximate to 5000 times higher than that of Fe in commercial Fe(3)O(4)nanoparticles. Experimental results and density functional theory calculations reveal that the high catalytic activity of Cu-HNCS originates from the single-atom copper, and the calculation predicts a next-generation Fenton catalyst. This work provides an effective paradigm of tumor parallel catalytic therapy for considerably enhanced therapeutic efficacy.