基于石墨烯独特生物界面效应的功能化载体研究进展

doi:10.6023/A21050238

化学学报 ›› 2021, Vol. 79 ›› Issue (10): 1244-1256.DOI: 10.6023/A21050238 上一篇下一篇

综述

基于石墨烯独特生物界面效应的功能化载体研究进展

岳华^a, 马光辉^a^,^b^,^*()

a 中国科学院过程工程研究所北京 100190
b 中国科学院大学北京 100049

投稿日期:2021-06-03 发布日期:2021-08-09
通讯作者: 马光辉

作者简介:

岳华, 中国科学院过程工程研究所青年研究员. 2012年获中国科学院过程工程研究所博士学位, 研究方向聚焦于纳微粒子生物医药新剂型的理论探索和应用研究. 目前发表SCI论文45篇, 以第一/通讯作者在Nat. Commun.、Sci. Adv.、Adv. Drug Deliver. Rev.等权威期刊发表论文15篇(两篇论文他引超100次), 授权专利4项, 参编书籍2部. 对石墨烯生物学效应的研究工作被评价为“最系统的研究之一”. 被优选为中国科学院青年创新促进会会员, 担任第一届中日颗粒论坛、天然与仿生颗粒论坛学术秘书等. 获中国颗粒学会自然科学奖一等奖(R06)等省部级奖2项.

马光辉, 中国科学院过程工程研究所研究员. 国家杰出青年基金(2001)获得者, 1993年在日本东京农工大学获得工学博士学位, 现任生化工程国家重点实验室主任. 主要研究方向为均一生物微球和微囊的制备及其在生化工程中的应用, 研究和开发用于生化分离、药物载体、免疫佐剂(疫苗递送系统)、细胞培养微载体、酶固定化载体等创新产品. 在Nat. Mater.、Nat. Bio. Eng.、Sci. Adv.、Nat. Commun.、Acc. Chem. Res.、JACS、Adv. Mater.等国际著名学术期刊上发表SCI论文431篇, ESI高被引9篇, 总他引超过10000次. 获中国发明专利授权 80余件、美国等国外专利授权12件, 专利技术和产品在国内外500多家单位得到应用. 获国家技术发明二等奖, 北京市科学技术一等奖, 第三世界青年女研究者奖, 中国化工学会基础研究成果一等奖等省部级一等奖多项.

基金资助:
北京市自然科学基金面上项目(2202056); 国家自然科学基金重点项目(32030062)

Advances in Functionalized Carriers Based on Graphene's Unique Biological Interface Effect

Hua Yue^a, Guanghui Ma^a^,^b()

a Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
b University of Chinese Academy of Sciences, Beijing 100049, China

Received:2021-06-03 Published:2021-08-09
Contact: Guanghui Ma
Supported by:
Beijing Municipal Natural Science Foundation(2202056); Key Program of National Natural Science Foundation of China(32030062)

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摘要/Abstract

二维石墨烯及其衍生物与生物界面的相互作用, 展现出相比于传统维度粒子截然不同的特性, 为功能化医药载体的设计开发提供了潜力策略. 除了优异的电学、热学、光学等性能外, 石墨烯的独特的二维性质, 可以引起细胞更强的应激反应, 包括与细胞膜发生水平摩擦/竖直嵌入/三明治超级结构、选择性被细胞内吞、胞内限域折叠、引发细胞自噬以及隐形活化效应. 基于上述独特界面效应以及理论模拟机制, 对石墨烯进行合理设计, 可在保障安全性的前提下, 满足药物递送、疫苗佐剂、成像传感、光热治疗等需求. 本综述结合课题组近10年在(氧化)石墨烯与生物界面效应、微观作用机理及应用开发方面的系统研究工作, 同时涵盖了国际最新进展, 以期为石墨烯高效、安全体系的设计、构建和应用, 提供理论依据和前瞻性预测.

关键词: 石墨烯, 生物界面效应, 二维载体, 药物递送, 疫苗佐剂

The interaction of two-dimensional graphene and its derivatives with biological interfaces exhibits distinct properties and advantages over traditional dimensional particles, offering potential strategies for the design and development of functionalized pharmaceutical carriers. Apart from the excellent electrical, thermal and optical properties, the two-dimensional structure endows the graphene stronger interactions with cell membranes and then induces obvious cellular response. These responses include the horizontal friction/slant insertion or sandwiched superstructure, selective internalization by phagocytes, folding effect upon the limited intracellular space, autophagy phenomenon and invisible activation. Based on these unique interfacial effects and theoretical simulation mechanisms, rational designs will meet the needs of drug delivery, vaccine carriers, imaging and sensing, and photothermal therapy as well as good biosafety. This review concludes our researches of exploring the biological interface effects, dynamic molecular mechanism, and applications regarding graphene (oxide) in the past 10 years. Meanwhile, it also covers the latest international progress, in order to provide theoretical basis and prospective prediction for the design, construction, and application of efficient and safe graphene systems.

Key words: graphene, biological interface effect, 2D carrier, drug delivery, vaccine adjuvant

引用此文

岳华, 马光辉. 基于石墨烯独特生物界面效应的功能化载体研究进展[J]. 化学学报, 2021, 79(10): 1244-1256.

Hua Yue, Guanghui Ma. Advances in Functionalized Carriers Based on Graphene's Unique Biological Interface Effect[J]. Acta Chimica Sinica, 2021, 79(10): 1244-1256.

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图/表 17

图1. CCK8法(A)以及LIVE/DEAD方法(B、C)检测脱锰前后的GO对细胞活性的影响

Figure 1. CCK8 assay (A) and LIVE/DEAD assay (B, C) showing the effect of GO on cell cytotoxicity. Reprinted with permission from Ref. [14]. Copyright (2012) Elsevier

图2. 腹腔注射GO-PEG(GOP)对小鼠各指标影响

Figure 2. Effects of different peritoneal administration of GOP in different aspect. Reprinted with permission from Ref. [20]. Copyright (2020) Royal Society of Chemistry

图3. 巨噬细胞和非吞噬类细胞对GO的内化情况及机制分析

Figure 3. The GO internalization event and mechanism of macrophages and non-phagocytes after incubation with GO. Reprinted with permission from Ref. [14]. Copyright (2012) Elsevier

图4. GO-磷脂膜三明治结构的实验证据. (A)冷冻电镜图片(左)及3D 重构图(右)(标尺20 nm). (B)嵌入GO后的细胞膜粗糙度. (C) FRAP分析膜磷脂流动性

Figure 4. Experimental evidence of the sandwiched graphene- membrane superstructure. (A) Cyro-TEM images (left) and tomography views (right) of the lipid vesicles in the presence of GO (Scale bars, 20 nm). (B) The roughness index of the cell membrane with embedded GOs. (C) FRAP analysis showing the fluidity of the membrane lipids. From Ref. [24] (Science advances, 5 (2019) eaaw3192). Reprinted with permission from AAAS.

图5. GO的胞内折叠效应(A)及相应细胞因子分泌情况(B)

Figure 5. The intracellular folding effect of GO (A) and cytokine profile (B) of cells. (Reprinted with permission from Ref. [14]. Copyright (2012) Elsevier)

图6. GO表面修饰策略

Figure 6. The strategy of GO surface functionalization

图7. 不同修饰GO对线粒体形态(上)及膜电位(下)的影响

Figure 7. The effect of different modified GO on the mitochondria morphology (Upper panels) and membrane potential (Lower panel). Reprinted with permission from Ref. [30]. Copyright (2015) American Chemical Society

图8. PEG修饰后的不同维度碳材料形貌、细胞因子分泌水平及表面利用度模拟图

Figure 8. Comparison of morphology, cytokine secretion levels, and nano-membrane interaction manner among PEGylated carbon nanomaterials in different dimensions. Reprinted with permission from Ref. [31]. Copyright (2017) Nature Publishing Group

图9. GO与OVA不同残基的接触数(A)、氢键/范德华作用力(B)以及酪氨酸上π-π堆积(C, 上)和谷氨酰胺氢键作用(C, 下)的分子模拟图

Figure 9. Contact number of OVA residues (A), the vdW energy (blue) and hydrogen bond number between OVA and GO (B), and the tyrosine π-π stacking (Upper) and glutamine hydrogen bond (Lower) that interacted with GO (C). Reprinted with permission from Ref. [35]. Copyright (2015) The Royal Society of Chemistry

图10. nGO及nGO-PEG 与细胞膜通过表面摩擦的作用模拟图

Figure 10. Simulations of bare and PEGylated nGO-membrane interactions by face-on configurations. Reprinted with permission from Ref. [31]. Copyright (2017) Nature Publishing Group

图11. GO-PEG激活细胞膜上αvβ8的力传导途径

Figure 11. Schematic diagram of αvβ8 activation through GO-PEG-induced mechanotransduction on the membrane. Reprinted with permission from Ref. [38]. Copyright (2021) WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

图12. 三明治结构模式图(A)及药物分子经2D粒子膜间递送(B)与传统颗粒胞内递送(C)扩散到跨膜受体上的模拟结果

Figure 12. The cartoon illustration of the superstructure of GO inside the cell membrane (A), and the configurations of the drug beads undergoing the intramembrane delivery from a sandwiched GO (B) and the intracellular delivery (C). From Ref. [24] (Science advances, 5 (2019) eaaw3192). Reprinted with permission from AAAS

图13. 三明治结构递送膜受体药物的效果: GO (5 μg/mL)和脂质体载体辅助后药物入膜量的比较(A)、不同药物处理后的乳腺癌MCF-7细胞活性数据(B)以及细胞成像图(红色: 死细胞; 绿色: 活细胞)(C)

Figure 13. The efficacy of delivering membrane-specific drug via the sandwiched superstructure. (A) Analysis of drug entry amount in the cell membrane with the assistant of GO (5 μg/mL) or liposome carrier. (B) Relative cell viability after different drug treatment in breast cancer cell MCF-7. (C) Images of live cell (green)/dead cell (red). From Ref. [24] (Science advances, 5 (2019) eaaw3192). Reprinted with permission from AAAS

图14. 基于二维GO独特性质开发的肿瘤疫苗及其效果

Figure 14. The unique properties of 2D GO and corresponding tumor vaccine efficacy. Reprinted with permission from Ref. [35]. Copyright (2015) The Royal Society of Chemistry

图15. 氧化石墨烯的体外发光性质

Figure 15. Photofluorescence property of the graphene oxide inner the cells. Reprinted with permission from Ref. [14]. Copyright (2012) Elsevier

图16. 可激活荧光探针的构建方案及其对肿瘤部位MMP酶的响应性和特异性

Figure 16. The scheme of the inducible probe and the MMP sensitivity and specificity in the tumor sites. Reprinted with permission from Ref. [58]. Copyright (2013) The Royal Society of Chemistry

图17. 基于石墨烯量子点构建程序性诊疗体系

Figure 17. Construction of GQD-based theranostic agent for programmatically monitoring and treatment. Reprinted with permission from Ref. [66]. Copyright (2017) American Chemical Society

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基于石墨烯独特生物界面效应的功能化载体研究进展

Advances in Functionalized Carriers Based on Graphene's Unique Biological Interface Effect

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