Lab of Low-Dimensional Materials Chemistry, Key Laboratory for Ultrafine Materials of Ministry of Education, Frontier Science Center of the Materials Biology and Dynamic Chemistry, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, 200237, Shanghai, China.
State Key Laboratory of Chemical Engineering and School of Chemical Engineering, East China University of Science and Technology, 200237, Shanghai, China.
Nat Commun. 2022 Jan 10;13(1):91. doi: 10.1038/s41467-021-27640-7.
Pursuing and developing effective methodologies to construct highly active catalytic sites to maximize the atomic and energy efficiency by material engineering are attractive. Relative to the tremendous researches of carbon-based single atom systems, the construction of bio-applicable single atom materials is still in its infancy. Herein, we propose a facile and general interfacial-confined coordination strategy to construct high-quality single-atom nanotherapeutic agent with Fe single atoms being anchored on defective carbon dots confined in a biocompatible mesoporous silica nanoreactor. Furthermore, the efficient energy conversion capability of silica-based Fe single atoms system has been demonstrated on the basis of the exogenous physical photo irradiation and endogenous biochemical reactive oxygen species stimulus in the confined mesoporous network. More importantly, the highest photothermal conversion efficiency with the mechanism of increased electron density and narrow bandgap of this single atom structure in defective carbon was proposed by the theoretical DFT calculations. The present methodology provides a scientific paradigm to design and develop versatile single atom nanotherapeutics with adjustable metal components and tune the corresponding reactions for safe and efficient tumor therapeutic strategy.
追求和开发有效的方法来构建高效的催化活性位点，通过材料工程最大限度地提高原子和能源效率是吸引人的。相对于基于碳的单原子体系的大量研究，生物可应用的单原子材料的构建仍处于起步阶段。在此，我们提出了一种简便通用的界面受限配位策略，用于构建高质量的单原子纳米治疗剂，其中 Fe 单原子锚定在受限在生物相容性介孔二氧化硅纳米反应器中的缺陷碳点上。此外，基于受限介孔网络中的外源物理光辐照和内源性生化活性氧刺激，证明了基于硅的 Fe 单原子体系的高效能量转换能力。更重要的是，通过理论 DFT 计算提出了这种缺陷碳中单原子结构增加电子密度和窄带隙的机制，从而实现了最高的光热转换效率。本方法为设计和开发具有可调金属成分的多功能单原子纳米治疗剂提供了一种科学范例，并可调节相应反应以实现安全有效的肿瘤治疗策略。
