用于纳米催化肿瘤治疗的异核双金属原子催化剂

doi:10.1016/S1872-2067(22)64207-4

催化学报 ›› 2023, Vol. 47: 1-31.DOI: 10.1016/S1872-2067(22)64207-4

• 综述 • 下一篇

用于纳米催化肿瘤治疗的异核双金属原子催化剂

韩璟怡, 管景奇^*()

吉林大学化学学院物理化学研究所, 吉林长春130021

收稿日期:2022-10-30 接受日期:2022-12-01 出版日期:2023-04-18 发布日期:2023-03-20
通讯作者: *电子信箱: guanjq@jlu.edu.cn (管景奇).
基金资助:
国家自然科学基金(22075099);吉林省自然科学基金项目(20220101051Jc);吉林省教育厅(JJKH20220967KJ)

Heteronuclear dual-metal atom catalysts for nanocatalytic tumor therapy

Jingyi Han, Jingqi Guan^*()

Institute of Physical Chemistry, College of Chemistry, Jilin University, Changchun 130021, Jilin, China

Received:2022-10-30 Accepted:2022-12-01 Online:2023-04-18 Published:2023-03-20
Contact: *E-mail: guanjq@jlu.edu.cn (J. Guan).
About author:Jingqi Guan (Jilin University) was invited as a young member of the 6^th Editorial Board of Chin. J. Catal. and the 5^th Editorial Board of Acta Phys.-chim. Sin. Prof. Jingqi Guan received his B.A. degree in 2002 and Ph.D. degree in 2007 from Jilin University. He carried out postdoctoral research in the University of California at Berkeley from 2012 to 2013 and in Dalian Institute of Chemical Physics, Chinese Academy of Sciences from 2014 to 2018. His research interests are in engineering single-atom catalysts and 2D materials for electrocatalysis, renewable energy, and biosensors. He has published more than 180 peer-reviewed papers.
Supported by:
National Natural Science Foundation of China(22075099);Natural Science Foundation of Jilin Province(20220101051Jc);Education Department of Jilin Province(JJKH20220967KJ)

摘要/Abstract

摘要：

癌症是威胁人类健康的重大疾病之一. 目前, 化疗、放疗和手术治疗是三大常规治疗癌症手段, 虽然这些治疗技术成熟, 但都存在不足, 且治疗成本高昂, 并使得患者在治疗过程中承受痛苦. 因此, 开发活性位点丰富、催化效率高、肿瘤组织识别准确的新型抗肿瘤催化材料, 利用有限的治疗资源, 以最低的毒性取得最佳的治疗效果, 成为癌症治疗的研究新前沿. 随着纳米材料的快速发展, 异核双原子催化剂(HDACs)在保留单原子催化剂的最大原子利用率, 活性位点分布均匀, 孤立单原子的不饱和配位环境和有利于电荷转移的电子结构等优点的基础上, 其两种不同金属原子不仅能提供更丰富的反应活性位点, 两者之间还具有独特的协同作用, 可以有效突破单原子催化剂的线性限制并优化活性中间物种的吸附能垒和构型, 显著提高催化活性和选择性从而获得满意的治疗效果, 在纳米催化肿瘤治疗领域展现出巨大的实际应用潜力.

本文对HDACs的表征手段、制备方法及其近年来在纳米催化肿瘤治疗领域的应用进行了系统的综述. 首先简要介绍了原子水平活性位点的各种表征方法, 特别是原位技术, 讨论了它们应用的侧重点, 并比较了各自的优缺点. 其次, 由于反应原子的高表面自由能、难以调控的动力学行为以及与载体的弱结合使得HDACs在合成过程中极不稳定. 一旦异质活性金属原子之间的距离变近, 就不可避免地发生团聚, 从而形成合金或大尺寸的纳米颗粒. 因此, 实现HDACs的精确和可控合成一直是该领域的研究重点. 本文对HDACs的四大主要制备策略即传统的高温热解法、湿式化学双溶剂法、原子层沉积技术和软模板自组装技术进行了系统总结, 并简要介绍了相关催化剂的应用潜力. 再次, 概括性地阐明了HDACs的抗肿瘤治疗机理, 并依据其发挥疗效的机理, 针对性地将近年来应用于抗癌领域的HDACs划分为芬顿/类芬顿反应或其他机制两大类, 并对这两类HDACs进行了详细的介绍. 最后, 探讨了HDACs在抗肿瘤领域可能面临的问题和挑战并展望了未来研究方向和应用前景, 以期为应用于该领域HDACs的研究提供富有价值的借鉴.

关键词: 异核, 双原子催化剂, 肿瘤治疗, 活性氧, 类芬顿反应

Abstract:

Due to excellent catalytic activity and high atomic utilization rate, single atom catalysts (SACs) have become a rising star in the field of nanocatalytic medicine. Heteronuclear dual-atom catalysts (HDACs) retain the advantages of monoatomic catalysts, have more optionally regulated coordination environment, possess favorable synergistic effects between different active sites, and can break through the restriction of adsorption ratio of SACs, making them the most ideal candidates for catalytic tumor therapy. In this review, we first introduce the advanced characterization methods of HDACs. Then, HDACs in different application fields are classified and elaborated according to various preparation strategies. According to the pharmacodynamic mechanisms, the application of HDACs in the field of nanocatalytic tumor therapy is emphatically introduced. Finally, a concise but focused summary and perspective is provided to outline the current challenges and prospects for future development of HDACs for oncology therapy.

Key words: Heteronuclear, Dual-atom catalyst, Tumor therapy, Reactive oxygen, Fenton-like reaction

韩璟怡, 管景奇. 用于纳米催化肿瘤治疗的异核双金属原子催化剂[J]. 催化学报, 2023, 47: 1-31.

Jingyi Han, Jingqi Guan. Heteronuclear dual-metal atom catalysts for nanocatalytic tumor therapy[J]. Chinese Journal of Catalysis, 2023, 47: 1-31.

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图/表 22

Fig. 1. Schematic diagram of adsorption configurations for single and diatomic sites (blue: adsorbed molecules, such as O2 or N2).

Fig. 2. Characterization techniques for SACs.

Table 1 Main characterizations for analyzing DACs.

Method	Purpose	Advantage	Disadvantage	Ref.
Microscopy (TEM, HAADF-STEM)	Direct imaging of metal elements with atomic resolution is used to detect the size and distribution of metal single atoms. The technique also provides relevant local structural information of atomic-level sites on the supporting material.	(1) Since the principle is based on Rutherford scattering, the image is bright enough to allow the observation of thick samples and low contrast samples. (2) Using the strong excitation and high-resolution imaging of the objective lens during the scanning transmission mode, microdiffraction can be achieved, which enables the visual observation of single atoms with 3D structure fixed in the N-doped graphene framework.	(1) It can only provide regional imaging of a specified location, without the ability to observe a wide area. (2) Only the surface of the sample can be characterized, while the morphology and structure of the core material encapsulated in the shell materials with 3D structure cannot be observed.	[114, 128‒131]
XAFS	Used to characterize the local geometric or electronic structure of a sample. It can elucidate the physical distance, coordination state, electronic structure and other highly accurate local information in atomic level.	(1) The overall structure can be determined by accurate in situ characterization of the single bimetallic atoms. (2) It can provide information about the stable adsorption structure and chemical bonding state of single atom on substrate materials. (3) The oxidation state and coordination number of the metal center in the complex can be characterized.	(1) Because X-rays are destructive, they can damage samples during measurements. (2) For XANES, there is the effect of multiple scattering emitted by photoelectrons and Auger electrons. Therefore, it is difficult to determine the identity of the oxidation states and scattering atoms.	[132‒135]
FTIR	By monitoring the adsorption behavior of these highly responsive guest molecules, the dispersion status of atomic-level metal sites in functional carriers was evaluated.	(1) High sensitivity, samples even below 10 nanograms can obtain satisfactory FTIR spectrograms. (2) The sample preparation is simple, and the reflectance spectrum of the opaque sample can be measured directly. (3) In the process of analysis, the original morphology and crystal form of the sample can be maintained without any detriment of the sample.	The analysis of complex mixtures and aqueous solutions is complicated.	[136‒140]
Mössbauer spectroscopy	Used to detect the coordination structure and electronic properties of materials such as oxidation states, spin states, chemical bond properties and other microscopic structure information.	(1) Mössbauer spectroscopy has extremely high energy resolution. (2) Because the Mössbauer effect involves resonant transition, the energy level structure, which depends on the chemical environment of the nuclear determines the shape and spectrum parameters, so it can reflect the change of the chemical environment around the resonant nuclear extremely sensitively. (3) Mössbauer spectroscopy has very little damage to the sample. (4) The test objects can be crystalline, amorphous, powdery or even frozen solutions, and the range of applications is extremely wide.

Table 1 Main characterizations for analyzing DACs.

Method	Purpose	Advantage	Disadvantage	Ref.
Microscopy (TEM, HAADF-STEM)	Direct imaging of metal elements with atomic resolution is used to detect the size and distribution of metal single atoms. The technique also provides relevant local structural information of atomic-level sites on the supporting material.	(1) Since the principle is based on Rutherford scattering, the image is bright enough to allow the observation of thick samples and low contrast samples. (2) Using the strong excitation and high-resolution imaging of the objective lens during the scanning transmission mode, microdiffraction can be achieved, which enables the visual observation of single atoms with 3D structure fixed in the N-doped graphene framework.	(1) It can only provide regional imaging of a specified location, without the ability to observe a wide area. (2) Only the surface of the sample can be characterized, while the morphology and structure of the core material encapsulated in the shell materials with 3D structure cannot be observed.	[114, 128‒131]
XAFS	Used to characterize the local geometric or electronic structure of a sample. It can elucidate the physical distance, coordination state, electronic structure and other highly accurate local information in atomic level.	(1) The overall structure can be determined by accurate in situ characterization of the single bimetallic atoms. (2) It can provide information about the stable adsorption structure and chemical bonding state of single atom on substrate materials. (3) The oxidation state and coordination number of the metal center in the complex can be characterized.	(1) Because X-rays are destructive, they can damage samples during measurements. (2) For XANES, there is the effect of multiple scattering emitted by photoelectrons and Auger electrons. Therefore, it is difficult to determine the identity of the oxidation states and scattering atoms.	[132‒135]
FTIR	By monitoring the adsorption behavior of these highly responsive guest molecules, the dispersion status of atomic-level metal sites in functional carriers was evaluated.	(1) High sensitivity, samples even below 10 nanograms can obtain satisfactory FTIR spectrograms. (2) The sample preparation is simple, and the reflectance spectrum of the opaque sample can be measured directly. (3) In the process of analysis, the original morphology and crystal form of the sample can be maintained without any detriment of the sample.	The analysis of complex mixtures and aqueous solutions is complicated.	[136‒140]
Mössbauer spectroscopy	Used to detect the coordination structure and electronic properties of materials such as oxidation states, spin states, chemical bond properties and other microscopic structure information.	(1) Mössbauer spectroscopy has extremely high energy resolution. (2) Because the Mössbauer effect involves resonant transition, the energy level structure, which depends on the chemical environment of the nuclear determines the shape and spectrum parameters, so it can reflect the change of the chemical environment around the resonant nuclear extremely sensitively. (3) Mössbauer spectroscopy has very little damage to the sample. (4) The test objects can be crystalline, amorphous, powdery or even frozen solutions, and the range of applications is extremely wide.

Fig. 3. (a) Fe-Co dual-site structure. M?ssbauer spectra of Fe,Mn/N-C (b) and Fe,Mn/N-C (c) under room-temperature. (d) Al MAS-NMR spectra. (e) Intensity changes. (f) Photographs of Pt-Al2O3 samples under white light and UV light (365 nm). (a,b) Reproduced with permission [125]. Copyright 2017, American Chemical Society. (c) Reproduced with permission [126]. Copyright 2021, Springer Nature. (d?f) Reproduced with permission [148]. Copyright 2017, Springer Nature.

Fig. 4. Schematic diagrams of the mechanisms of typical high-temperature pyrolysis (a), wet chemical double-solvent (b), Pt ALD mechanism on graphene nanosheets (c) and soft template self-assembly methods (d). (a) Reproduced with permission [163]. Copyright 2021, Royal Society of Chemistry. (b) Reproduced with permission [155]. Copyright 2018, Royal Society of Chemistry. (c) Reproduced with permission [164]. Copyright 2022, Elsevier. (d) Reproduced with permission [165]. Copyright 2022, John Wiley and Sons Ltd.

Fig. 5. (a) Schematic diagram of various construction strategies of MOF-based SACs. HAADF-STEM image of Fe-Mn dual sites (b) and corresponding intensity profiles (c). (d) Fe M?ssbauer spectrum. Fe (e) and Mn (g) K-edge XANES spectra. Fe (f) and Mn (h) Fourier-transform EXAFS spectra. (i) WT of the k2-weighted EXAFS data. (a) Reproduced with permission [28]. Copyright 2020, Royal Society of Chemistry. (b?i) Reproduced with permission [186]. Copyright 2022, Elsevier.

Fig. 6. Schematic diagrams of the synthesis of (Fe,Co)/CNT (a) and the structure of Fe-Co sites (b). HAADF-STEM image (c) and the EELS (d) of the (Fe,Co)/CNT. Various intermediate geometric structures (e) and ORR free energy diagram (dashed line: the traditional 2e? pathway) (f) on (Fe,Co)/CNT. (g) Relationship between ORR activity and ΔGOH*. Co-SAs: Co site of bare Co SAs/N-C). Synthetic illustration (h) and HAADF images (i,j) of A-CoPt-NC. (k) Bimetallic atomic configuration model derived from the (h) region. (l?q) Theoretical calculation results of A-CoPt-NC. (l) ORR free energy diagram of (Co-Pt)@N8V4. Local state densities (m,n) and charge density vertical views (o,p) of (Co-Pt) @N8V4 (m,o) and (Pt-Pt)@N8V4 (n, p). (q) ORR pathway on (Co-Pt)@N8V4. (a?g) Reproduced with permission [187]. Copyright 2018, Royal Society of Chemistry. (h?q) Reproduced with permission [188]. Copyright 2018, American Chemical Society.

Fig. 7. Synthetic illustration of CoPNi-N/C (a) and CoDNi-N/C (b). Change of Bader charge in Co-N/C (c) and Co/Ni-N/C (d). Average electron density difference in plane between Co-N/C (e) and CoXNi-N/C (f) (yellow regions: the electron accumulation, cyan regions: the electron depletion). (g) Synthetic illustration of (Fe,Co)/NC. (h) HAADF-STEM images of (Fe,Co)/N-C (red circles: Fe/Co bimetallic active site). (i) Intensity profiles of corresponding zoomed areas in (h). (j) HRTEM image; XANES spectra (k) of (Fe,Co)/N-C and corresponding Fe EXAFS fitting data (l). (m) The structure of Fe-Co dual sites. (n) ORR intermediate and transition state energies of (Fe,Co)/N-C. (a?f) Reproduced with permission [198]. Copyright 2019, Elsevier. (g?n) Reproduced with permission [125] Copyright 2017, American Chemical Society.

Fig. 8. XANES spectra of Co K-edge (a) and Zn K-edge (c). (b,d) FT EXAFS spectra of corresponding samples. (e) Optimized calculated geometry of the Zn/CoN-C. (f) Optimized adsorption configuration geometry of O2. (g) Possible ORR reaction pathways in acidic environments. (h,i) ORR free energy diagram. Synthetic illustration (j) and HAADF image (k) of (Zn, Co)/NSC. (l) Corresponding intensity profiles. (m) Optimized calculated geometry of the (Zn, Co)/NSC. (n) Optimized adsorption configuration geometry of O2. (o,p) ORR free energy diagrams. (a?i) Reproduced with permission [199] Copyright 2019, John Wiley and Sons Ltd. (j?p) Reproduced with permission [200]. Copyright 2019, Elsevier BV.

Fig. 9. (a) Schematic diagram of the ice-assisted photocatalytic reduction method. (b?j) The geometry structures of different samples. (k) PDOS plots. HAADF-STEM (l) and element maps (m?p) of PtRuSA-CN620. Ru K-edge (q) and Pt L3-edge XANES (r) and FT spectrum of Ru/Pt at (s,t) R and (u,v) k spaces. Reproduced with permission [201]. Copyright 2019, Royal Society of Chemistry.

Fig. 10. (a) Synthetic illustration. (b) HAADF-STEM image. EELS spectrum (c) and corresponding contrast profiles (d) and EELS mapping (e) of (Fe,Co)/N-C. (f) Schematic diagram of the synthesis. HAADF-STEM image (g) and contrast profiles (h) of IrCo-N-C. Charge density diagrams of CoN4 (i) and IrCoN5 (j). XANES spectra (k,l), FT-EXAFS spectra (m,n) and EXAFS fitting curves (o,p) at Co K-edge (k,m,o) and Ir L3-edge (l,n,p). Ir L3-edge WT images for Ir/C (q), Ir-N-C (r), and IrCo-N-C (s). PDOS diagrams of CoN4-O (t) and IrCoN5-O (u). (v) Schematic bond formation of the Co?O bond. (a?e) Reproduced with permission [207]. Copyright 2020, American Chemical Society. (f?v) Reproduced with permission [208]. Copyright 2021, American Chemical Society.

Fig. 11. (a) Schematic diagram of the synthesis of Fe-NiNC. TEM (b,c) and HAADF-STEM (d) images of Fe-NiNC. (e) The Fe-Ni distance measurements. (f,g) XANES spectra. (h,i) FT-EXAFS. Free energy diagrams (j,k) and proposed mechanisms (l,m) for ORR (j,l) and OER (k,m). (a?m) Reproduced with permission [209]. Copyright 2020, Elsevier BV.

Fig. 12. (a) Synthetic illustration of Pt-Ru dimers/NCNTs using ALD technology. (b) HAADF-STEM image. (c) The intensity profile. (d) Distribution histogram of various structure tapes. (e) The ratio of loading Pt and Ru atoms under different ALD temperatures; XANES spectra (f,g,i) and corresponding k2-weighted FT-EXAFS (h,j). (k) Most stable H adsorption configurations. (l) Surface models. (m) Most stable adsorption configurations of OH. (a?j) Reproduced with permission [217]. Copyright 2019, Springer Nature. (k?m) Reproduced with permission [218]. Copyright 2019, American Chemical Society.

Fig. 13. (a) Synthetic illustration of various catalysts. (b) Ligand release curve during the titration. (c) DRIFTS spectra. (d,e) STEM images of Pt-Sn nanocluster. (f,g) Obvious intensity differences between Pt and Sn along the directions of the lines marked in (e). (a?c) Reproduced with permission [219]. Copyright 2022, American Chemical Society. (d?g) Reproduced with permission [220]. Copyright 2022, Wiley-VCH Verlag GmbH & CO. KGaA.

Fig. 14. (a) Synthetic illustration of FeCo-NSC. AFM image and corresponding height profile (b) and HAADF-STEM image (c). (d) The intensity plots of Fe-Co sites. (e,h) XANES spectra. FT-EXAFS spectra (f,i) and corresponding fitting in R space (g,j) of Fe K-edge (e?g) and Co K-edge (h?j) of FeCo-NSC and related samples. (k,l) HAADF-STEM images of the CN-FeNi-P. (m,p) XANES profiles. (n,q) EXAFS spectra FT k3-weighted in R space. (o,r) WT images of Fe K-edge (m?o) and Ni K-edge (p?r) of CN-FeNi-P and related samples. (a?j) Reproduced with permission [221]. Copyright 2022, Elsevier. (k?r) Reproduced with permission [222]. Copyright 2022, Elsevier.

Fig. 15. Schematic diagram of biological consequences of ROS increase. Oncogenic signals in tumor cells stimulate increased ROS production. Endogenous ROS and exogenous DNA damage agents, mitochondrial mutations cause respiratory chain failure and further increase ROS production. The above fault may affect the apoptotic response to anticancer drugs, making cancer cells resistant to the drugs. A surge in cellular ROS causes DNA damage and promotes mutations, which in turn leads to increased drug sensitivity.

Fig. 16. Schematic diagrams of the mechanism of endogenous Fenton response triggered by MSFP (a) and follow-up anti-tumor therapy for MSFP (b). Growth (c) and survival curves (d) of mice 4T1 tumor. (e) Schematic diagram of MSFP catalyzing the formation of ?OH, resulting in the oxidation of TMB (colorless) to oxTMB (blue). (f) Normalized absorbance of MB (C/C0) after 30 min in acidic PBS containing 100 μm H2O2. (g) Michaelis-Menten dynamics. (h) Line Weaver-Burk plotting of MSFP. (a?h) Reproduced with permission [235]. Copyright 2022, John Wiley and Sons Ltd.

Fig. 17. (a?d) Schematic diagram of the synergistic and “division of labor” catalytic mechanisms of FeCo-DIA/NC for “ROS cycling” and concurrent catalytic therapy in tumors. (e?h) DFT simulations of Fenton activity. Proposed reaction mechanisms at the Fe (e) and Co (g) sites. Free energy diagrams of Fenton process at Fe (f) and Co (h) sites. (i) Schematic diagram of in vivo studies. Body weight curve (j), tumor tissue proliferation curve (k) and survival rate (l) of mice during treatments. (m) Digital photographs of the dissected tumor. Reproduced with permission [16]. Copyright 2022, Elsevier.

Fig. 18. (a) The structure of (Fe, Pt)SA-N-C. (b) Fe K-edge EXAFS. (c) Pt L3-edge EXAFS. (d,e) In vivo treatment options. Tumor growth curves (f), weight change curves (g), Photos (h) of corresponding tumor tissue. (i) ESR spectra of BMPO/?OH. (j) Probable Fenton-like reaction mechanisms for attaining ?OH on (Fe,Pt)SA-N-C. (k) H2O2 adsorption models. (l) Free energy diagrams for Fenton-like reaction. Projected density of states of (Fe, Pt)SA-N-C after adsorbing H2O* (m) and H2O2* (n). Reproduced with permission [236]. Copyright 2022, American Chemical Society.

Fig. 19. (a) Schematic diagram of the synthesis of RBC-HNTM-Pt@Au and the efficient treatment of osteomyelitis via SDT mechanism. (b) Photos of the rat surgical site. (c) Routine blood tests after 4 weeks of treatment (n = 3). (d) Photoluminescence spectra. (e) The 1O2 comparison curve detected by 1,3-diphenylisobenzofuran (DPBF) degradation. (f) Ultrasonic current test. (g) Electrochemical impedance spectra. Reproduced with permission [240]. Copyright 2021, American Chemical Society.

Fig. 20. Schematic diagrams of sonocatalytic mechanism (a) and osteomyelitis operation via sonodynamic therapy (b). Charge density difference (c,f) of g-ZnN4, bad charge, O2 activated energy, magnetic moment (d,g), and DOS (e,h) of g-ZnN4 (c?e) and g-ZnN4-MoS2 (f?h). (i) The infected leg wound. (j) Fluorescence intensity statistics of inducible nitric oxide synthase and transforming growth factor-β. (k) Micro-CT analysis of infected legs. Reproduced with permission [241]. Copyright 2022, Wiley-VCH Verlag.

Fig. 21. Schematic diagrams of the synthesis of samples (1?5) (a) and crystal structures of samples (3) and (5) (b). (c) Viability of normal Caco-2 cells treated with samples 1?5 for 72 h after 15 d of inoculation (n ≥ 12). Reproduced with permission [245]. Copyright 2022, MDPI AG.

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用于纳米催化肿瘤治疗的异核双金属原子催化剂

Heteronuclear dual-metal atom catalysts for nanocatalytic tumor therapy

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