Materials Today最新文献_第2页

Topology and curvature effects in the photonics of ring – split ring – cuboid transitions 环形-分裂环形-立方体过渡光子学中的拓扑和曲率效应

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.08.015

Mikhail Bochkarev , Nikolay Solodovchenko , Kirill Samusev , Mikhail Limonov

Topological transitions in various materials are actively being studied, including topological quantum phase transitions, going beyond the Landau theory and the concept of the order parameter. Here we propose the concept of a transition between two structures with different topology using the example of the transition between a flat dielectric ring and a split ring and its further unbending into a rectangular Fabry-Pérot resonator. Experimentally and theoretically, we discovered the lifting of the degeneracy of the CW-CCW photonic modes of the ring and the formation of two families: topological, which acquire an additional phase

π

, equal to the Berry phase in a thin Möbius strip, and ordinary ones, which do not acquire an additional phase. Topological modes arise due to the gradual “cutting” of one antinode of the field by a gap into two antinodes as the angular size of the gap increases from zero to one degree. Thus, using a topological Fabry-Pérot resonator with variable curvature and fixed length, resonant modes with an arbitrary non-integer number of waves are realized and a new generation of resonators is created with the prospect of unique classical and quantum applications.

人们正在积极研究各种材料中的拓扑转变，包括拓扑量子相变，超越了朗道理论和有序参数的概念。在此，我们以平面介质环和分裂环之间的过渡及其进一步弯曲成矩形法布里-佩罗共振器为例，提出了两种不同拓扑结构之间的过渡概念。通过实验和理论，我们发现环的 CW-CCW 光子模式的退行性被解除，并形成了两个系列：拓扑模式和普通模式，前者获得了额外的相位 π，相当于薄莫比乌斯带中的贝里相位，后者则没有获得额外的相位。拓扑模式产生的原因是，当间隙的角度从零增加到一度时，场的一个反节点会被间隙逐渐 "切割 "成两个反节点。因此，利用具有可变曲率和固定长度的拓扑法布里-佩罗共振器，可以实现具有任意非整数波的共振模式，并创造出新一代共振器，具有独特的经典和量子应用前景。

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引用次数: 0

In-situ reconstructed surface/inner-structure synergistic design enabling 4.6 V LiCoO2 cathode for all-solid-state thin-film battery 原位重构表面/内部结构协同设计使全固态薄膜电池的钴酸锂正极电压达到 4.6 V

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.09.011

Jinxu Qiu , Hongliang Li , Yu Zhao , Rongrui Xu , Kaiyuan Wei , Yixiu Cui , Jie Shu , Yanhua Cui

Developing high-voltage LiCoO₂ cathode film is a promising approach to meet high-energy density demands for intelligent microdevices. However, the electrochemical performance of bare LiCoO₂ is compromised beyond 4.55 V due to irreversible phase transitions, cobalt dissolution, and intergranular cracking. Meanwhile, vacuum physical deposition technology and interface compatibility pose challenges to achieving higher capacity integrated into a narrow space. Herein we proposed an in-situ reconstructed surface/inner-structure synergistic modification prototype strategy to achieve a superior high-voltage LiCoO₂ through a facile in-situ magnetron sputtering. This sandwich structure design enables a synergistic effect of internal titanium body-doping and external LiCoPO₄ compact layer to strengthen stability under high voltage. Consequently, the triggered defects and strong PO coordination are substantially beneficial for stabilizing Li⁺ channels, inhibiting Co migration, as well as enhancing diffusion kinetics. Strain field analysis reveals that the mitigated lattice deformation along (104) preferential orientation is beneficial for alleviating volumetric strain even at an operating voltage of up to 4.6 V. Additionally, the induced body and surface atom rearrangement regulates the band structure and reduces oxygen redox activity. Therefore, the as-designed high-voltage LiCoO₂-based all-solid-state thin-film battery achieves superior cycle stability with 75 % capacity retention after 500 cycles at 1 C under 10 °C.

开发高电压钴酸锂阴极薄膜是满足智能微型设备高能量密度需求的一种可行方法。然而，由于不可逆相变、钴溶解和晶间裂纹等原因，裸钴酸锂的电化学性能在 4.55 V 以上会受到影响。同时，真空物理沉积技术和界面兼容性也为在狭窄空间内实现更高的集成容量带来了挑战。在此，我们提出了一种原位重构表面/内部结构协同改性原型策略，以通过简便的原位磁控溅射技术实现卓越的高压钴酸锂。这种三明治结构设计使内部钛体掺杂和外部钴酸锂致密层产生协同效应，从而增强了高压下的稳定性。因此，引发的缺陷和强 PO 配位对稳定 Li+ 通道、抑制 Co 迁移以及增强扩散动力学大有裨益。应变场分析表明，即使在高达 4.6 V 的工作电压下，沿（104）优先取向的晶格变形也能得到缓解，从而有利于减轻体积应变。此外，诱导的体原子和表面原子重排调节了带状结构，降低了氧氧化还原活性。因此，按设计制造的基于钴酸锂的高电压全固态薄膜电池实现了卓越的循环稳定性，在 10 °C、1 C 条件下循环 500 次后容量保持率为 75%。

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引用次数: 0

Engineering defects in graphitic carbon nitride photocatalysts 氮化石墨碳光催化剂中的工程缺陷

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.09.019

Qi Li , Siyu Zhao , Baojiang Jiang , Mietek Jaroniec , Liping Zhang

Graphitic carbon nitride (g-C₃N₄) has emerged as a promising metal-free photocatalyst. However, it continues to face significant challenges in achieving competitive activities both in laboratories and practical applications. Defect engineering is a versatile strategy to refine the intrinsic properties of semiconductor photocatalysts, modulating their electronic structure, charge dynamics and active surface sites. Given rapid advancements in this field, there is an urgent need to overview the progress in engineering of defects in g-C₃N₄, which is essential for a deeper understanding of the activity of this photocatalyst. This review focuses on the synthesis, characterization, and physiochemical properties of defect-engineered g-C₃N₄, including g-C₃N₄ with substitutional dopants, interstitial dopants, vacancies, functional groups and/or structural disorder. It also explores various applications of g-C₃N₄ materials with introduced defects for photocatalytic H₂ evolution, CO₂ reduction, N₂ fixation and organic transformations, along with the mechanisms underlying their performance at the molecular level. Finally, this review article presents a perspective on the design, synthesis and properties of defect-modified g-C₃N₄ photocatalysts.

氮化石墨碳（g-C3N4）已成为一种前景广阔的无金属光催化剂。然而，要在实验室和实际应用中实现具有竞争力的活性，它仍然面临着巨大的挑战。缺陷工程是完善半导体光催化剂内在特性、调节其电子结构、电荷动力学和活性表面位点的一种通用策略。鉴于这一领域的快速发展，迫切需要对 g-C3N4 缺陷工程的进展进行综述，这对于深入了解这种光催化剂的活性至关重要。本综述重点介绍缺陷工程 g-C3N4 的合成、表征和理化性质，包括具有取代掺杂、间隙掺杂、空位、官能团和/或结构紊乱的 g-C3N4。文章还探讨了引入缺陷的 g-C3N4 材料在光催化 H2 演化、CO2 还原、N2 固定和有机物转化方面的各种应用，以及这些材料在分子水平上的性能机理。最后，这篇综述文章对缺陷修饰 g-C3N4 光催化剂的设计、合成和性能进行了展望。

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引用次数: 0

Advancing solid-state sodium batteries: Status quo of sulfide-based solid electrolytes 推进固态钠电池：硫化物固态电解质的现状

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.08.011

Zhendong Yang , Bin Tang , Dehang Ren , Xinyu Yu , Yirong Gao , Yifan Wu , Yongan Yang , Zhongfang Chen , Zhen Zhou

Solid-state sodium batteries are among the most promising candidates for replacing conventional lithium-ion batteries for next-generation electrochemical energy storage systems. Their advantages include abundant Na resources, lower cost, enhanced safety, and high energy density. Central to the development of these batteries is the use of all-solid-state sodium electrolytes, with sulfide-based solid electrolytes emerging as particularly viable due to their high ionic conductivity (on par with liquid electrolytes), favorable interfacial contact with electrodes, and mild preparation conditions. Despite these benefits, several crucial challenges limit the development of sulfide-based solid electrolytes, including a narrow electrochemical stability window, unstable interface between sulfide-based solid electrolytes and electrodes, and the growth of detrimental sodium dendrites. This review examines the fundamental ion transport mechanism in sulfide-based solid electrolytes, discusses the primary challenges and strategic solutions, and separately addresses the critical interfacial issues at the cathode and anode. It also highlights the importance of scaling up these techniques for industrial applications. Finally, this review offers key recommendations for advancing the industrialization and enhancing the energy density of sulfide-based solid-state sodium batteries. Hopefully, solid-state sodium batteries based on sulfide-based solid electrolytes will achieve significant breakthroughs in energy density and industrial scalability in the very near future.

固态钠电池是最有希望取代传统锂离子电池的下一代电化学储能系统。它们的优势包括丰富的钠资源、较低的成本、更高的安全性和高能量密度。开发这些电池的核心是使用全固态钠电解质，其中硫化物基固态电解质因其离子电导率高（与液态电解质相当）、与电极的界面接触良好以及制备条件温和而特别可行。尽管硫化物固态电解质具有这些优点，但其发展仍面临一些关键挑战，包括电化学稳定性窗口狭窄、硫化物固态电解质与电极之间的界面不稳定以及有害的钠枝晶生长。本综述探讨了硫化物固体电解质的基本离子传输机制，讨论了主要挑战和战略解决方案，并分别讨论了阴极和阳极的关键界面问题。综述还强调了扩大这些技术的工业应用规模的重要性。最后，本综述为推进硫化物固态钠电池的工业化和提高能量密度提出了重要建议。希望在不久的将来，基于硫化物固体电解质的固态钠电池能在能量密度和工业可扩展性方面取得重大突破。

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引用次数: 0

Metals beyond tomorrow: Balancing supply, demand, sustainability, substitution, and innovations 未来的金属：平衡供应、需求、可持续性、替代和创新

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.09.007

T. DebRoy , J.W. Elmer

Finite or scarce metal supplies, rising demand, declining ore grades, and prospects of creating a climate-friendly metallurgical industry pose both a challenge and an opportunity to revitalize metals production through sustainable technology, innovations, and informed public policies. The rapid rise in metal consumption, faster than the population growth, challenges both the supply-demand balance and international environmental goals. Depletion of green technology critical metals, with known metal reserves unlikely to last more than half a century, emphasizes the need for increased substitutions, recycling, and reuse efforts. In the past, organized research and serendipity empowered us to innovate manufacturing processes and develop new alloys that fulfilled important societal needs. However, a renewed emphasis on metals research and development is required to meet new and future challenges where the use of critical metals is optimized, and metal sustainability is taken into account. While green technologies offer hope for a cleaner future, scale-up concerns and higher costs of these metals inhibit their widespread use. Current mitigation strategies fall short of Paris Agreement goals, but using advanced high-strength steels could significantly cut total steel usage and greenhouse gas emissions. Ensuring long-term reliance on metals necessitates finding a delicate balance between the challenges facing the metals industry and the multitude of technical and political factors important for their resolution. Engaging and educating the younger generation, particularly Generation Z, policymakers, and industry leaders, is necessary to effectively map out a path forward to revitalize the metals industry.

有限或稀缺的金属供应、不断增长的需求、不断下降的矿石品位，以及创建气候友好型冶金工业的前景，都为通过可持续技术、创新和明智的公共政策振兴金属生产带来了挑战和机遇。金属消费量的快速增长超过了人口的增长速度，这对供需平衡和国际环境目标都提出了挑战。绿色技术的关键金属已经耗尽，已知的金属储量不可能维持半个世纪以上，这就强调了加强替代、回收和再利用工作的必要性。过去，有组织的研究和偶然性使我们能够创新制造工艺，开发新合金，满足重要的社会需求。然而，为了应对新的和未来的挑战，我们需要重新重视金属研发，优化关键金属的使用，并考虑金属的可持续性。虽然绿色技术为更清洁的未来带来了希望，但这些金属的规模化问题和较高的成本阻碍了它们的广泛使用。目前的减排战略无法实现《巴黎协定》的目标，但使用先进的高强度钢可以显著减少钢材的总用量和温室气体排放量。要确保对金属的长期依赖，就必须在金属行业面临的挑战与解决这些挑战的众多重要技术和政治因素之间找到微妙的平衡。让年轻一代（尤其是 Z 世代）、政策制定者和行业领导者参与进来并对他们进行教育，对于有效规划振兴金属行业的前进道路十分必要。

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引用次数: 0

Droplet nanogenerators: Mechanisms, performance, and applications 液滴纳米发电机：机理、性能和应用

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.08.017

Pawantree Promsuwan , Md Al Mahadi Hasan , Suwen Xu , Ya Yang

The need for power technology that improves human life and convenience is driving the demand for increased energy consumption. At present, fossil fuels are the primary source of energy that meets the energy demand of mankind. However, they are also the main cause of environmental pollution. Therefore, it is imperative to develop technology that can harness energy from renewable sources to replace fossil fuels. One promising technology that has gained significant attention is the droplet nanogenerators, which harvest energy from various forms of water. This technology has grown in popularity due to its straightforward design, low fabrication cost, and high output power, which is sufficient to power small electronic devices sustainably. With innovative structures and various fundamental materials, droplet nanogenerators’ performance can be improved, which leads to the expansion of their application areas. This review summarizes recent advancements in droplet nanogenerators, including mechanisms, output performance, and applications. Finally, the challenges and opportunities associated with droplet nanogenerators are briefly discussed.

对改善人类生活和便利性的电力技术的需求，推动了能源消耗的增长。目前，化石燃料是满足人类能源需求的主要能源。然而，化石燃料也是造成环境污染的主要原因。因此，当务之急是开发能够利用可再生能源替代化石燃料的技术。液滴纳米发电机是一项前景广阔的技术，它能从各种形式的水中获取能量，已受到广泛关注。这种技术设计简单、制造成本低、输出功率高，足以为小型电子设备持续供电，因此越来越受欢迎。通过创新结构和各种基础材料，液滴纳米发电机的性能可以得到改善，从而拓展其应用领域。本综述总结了液滴纳米发电机的最新进展，包括机理、输出性能和应用。最后，简要讨论了与液滴纳米发生器相关的挑战和机遇。

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引用次数: 0

Regulating interfacial behavior via reintegration the Helmholtz layer structure towards ultra-stable and wide-temperature-range aqueous zinc ion batteries 通过重新整合赫尔姆霍兹层结构调节界面行为，实现超稳定、宽温程锌离子水电池

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.08.003

Shijia Li , Jingwen Zhao , Xieyu Xu , Jiasen Shen , Kai Zhang , Xue Chen , Kai Wang , Xingxing Jiao , Ziyang Wang , Dinghao Xu , Qianyu Zhang , Yangyang Liu , Ying Bai

Aqueous zinc-ion batteries are recognized as a potential candidate in large-scale energy storage devices. However, parasitic reactions on interfaces have severely limited their further development due to sticky de-solvation process of Zn(H₂O)₆²⁺. Acetylacetone (Hacac) is proposed as a tri-functional additive by altering the solvation structure to address detrimental interface issues. Specifically, the acetyl groups induced by decomposition of Hacac inhibit dendrite growth, by-product aggregation on anode via guiding ordered deposition of zinc ions and suppressing water decomposition in internal Helmholtz plane (IHP). Meanwhile, the acetyl groups remarkably alleviate by-product aggregation and maintain the cathode structure by accelerating zinc ion transfer and inhibiting disintegration of water in IHP. With the addition of 0.5 wt% Hacac, Zn metal maintains a high coulombic efficiency of 99.9 % after 2000 cycles at 10 mA cm⁻² and 1 mAh cm⁻², with superior longevity of 5200 h at 1 mA cm⁻² with 0.5 mAh cm⁻² for Zn|Zn cells. As expected, the assembled Zn|NH₄V₄O₁₀ batteries exhibit an outstanding capacity retention of 90 % up to 22,000 cycles at 10 A/g. As a highly efficient strategy, the reframing of Helmholtz layer structure via electrolyte additive could be broadened to address general interfacial issues in advanced energy storage systems.

锌离子水电池被认为是大规模储能设备的潜在候选者。然而，由于 Zn(H2O)62+ 的粘性脱溶过程，界面上的寄生反应严重限制了其进一步发展。乙酰丙酮（Hacac）作为一种三功能添加剂，通过改变溶解结构来解决有害的界面问题。具体来说，Hacac 分解后产生的乙酰基团通过引导锌离子有序沉积和抑制内部亥姆霍兹平面（IHP）的水分解，抑制了枝晶的生长和阳极上副产物的聚集。同时，乙酰基通过加速锌离子转移和抑制 IHP 中水的分解，显著缓解了副产物的聚集并保持了阴极结构。添加 0.5 wt% Hacac 后，金属锌在 10 mA cm-2 和 1 mAh cm-2 条件下循环 2000 次后仍能保持 99.9 % 的高库仑效率，在 1 mA cm-2 和 0.5 mAh cm-2 条件下，Zn|Zn 电池的寿命可达 5200 小时。正如预期的那样，组装好的 Zn|NH4V4O10 电池在 10 A/g 条件下可循环使用 22,000 次，容量保持率高达 90%。作为一种高效的策略，通过电解质添加剂重构亥姆霍兹层结构可扩展到解决先进储能系统中的一般界面问题。

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引用次数: 0

Recent advances in conducting gels for flexible and stretchable smart electronic devices: A comprehensive review 用于柔性和可拉伸智能电子设备的导电凝胶的最新进展：全面回顾

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.09.001

Bablesh Gupta , Suman Kalyan Samanta , Ranbir Singh

Conducting gels have garnered significant attention due to their distinctive properties, such as unique electrical/thermal conductivity, biocompatibility, flexibility, stretchability, and transparency. These gels adeptly combine the viscoelastic features with the combination of organic, metal, and semiconductor components. Consequently, these gels have become the subject of extensive exploration across various fields, encompassing tactile sensors, power generation systems, actuators, wearable electronics, and biomedical devices. Their potential applications extend beyond these fields to encompass human–machine interfaces, artificial intelligence, and other implementations. This review provides a comprehensive examination of the synthesis methods for various electrically conducting gels, such as hydrogels, organogels, metal–organic gels, and perovskite gels. Furthermore, this study investigates the promising applications of these gels across various fields, focusing on their potential use in energy storage, energy harvesting devices, and advanced sensors. Resolutely, the review outlines both the prospects and challenges in further research endeavors concerning the development and utilization of these remarkable gels for boosting the evolution of cutting-edge mechanically versatile intelligent stretchable skin-like devices.

导电凝胶因其独特的特性，如独特的导电性/导热性、生物相容性、柔韧性、伸展性和透明度，而备受关注。这些凝胶巧妙地将粘弹性特征与有机、金属和半导体成分相结合。因此，这些凝胶已成为各个领域广泛探索的主题，包括触觉传感器、发电系统、致动器、可穿戴电子设备和生物医学设备。它们的潜在应用范围已超出这些领域，包括人机界面、人工智能和其他应用。本综述全面探讨了各种导电凝胶（如水凝胶、有机凝胶、金属有机凝胶和包晶凝胶）的合成方法。此外，本研究还探讨了这些凝胶在各个领域的应用前景，重点关注它们在能量存储、能量收集装置和先进传感器中的潜在用途。本综述坚定地概述了进一步研究的前景和挑战，即开发和利用这些非凡的凝胶来推动尖端机械多功能智能可拉伸类皮肤设备的发展。

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引用次数: 0

Metabolic intervention mitochondria nanomotors breakdown redox homeostasis for boosting oxidative stress-dependent antitumor therapy 代谢干预线粒体纳米马达打破氧化还原平衡，促进氧化应激依赖性抗肿瘤治疗

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.08.019

Xinping Luo , Xincong Li , Shiyu Li , Chenxi Zhou , Jing Li , Zhanwei Zhou , Minjie Sun

Aberrant metabolic balance in malignant tumors shapes defensive redox homeostasis and protected tumor cells from oxidative stress damage, consequently impeding clinical transformation process of oxidative stress-dependent anti-tumor therapies represented by chemodynamic therapy and immunotherapy. Herein, a rational designed mitochondria nanomotor was developed by coating a GSH-responsive functional Pt(IV) prodrug layer DP on magnetic iron oxide nanoparticles (MN), which can thoroughly breakdown redox homeostasis by metabolic intervention strategy. Specifically, DP loading two dichloroacetic acid (DCA) axial ligands was stimuli-responsively reduced into Pt(II) and DCA molecules in highly reductive tumor cells, accompanied with glutathione elimination and oxidative stress counteraction weakening. Subsequently, DCA increased pyruvate influx into the mitochondria by pyruvate dehydrogenase activation and enduringly elevated oxidative phosphorylation level, breaking the tumor redox homeostasis thoroughly, contributing to 7.5-fold amplifying hydrogen peroxide production and sensitizing chemodynamic therapy mediated by MN, finally resulting in inspiring 89.5% tumor suppression rate on triple negative breast cancer model. In short, this work realized comprehensive and sustainable oxidative stress elevation of the intracellular environment by metabolic intervention strategy and provided an ingenious perspective of augmenting oxidative stress-dependent anti-tumor therapies.

恶性肿瘤代谢平衡失调会影响防御性氧化还原平衡，保护肿瘤细胞免受氧化应激损伤，从而阻碍以化学动力疗法和免疫疗法为代表的氧化应激依赖型抗肿瘤疗法的临床转化进程。本文通过在磁性氧化铁纳米粒子（MN）上包覆GSH响应性功能铂(IV)原药层DP，开发了一种合理设计的线粒体纳米马达，可通过代谢干预策略彻底打破氧化还原平衡。具体来说，在高还原性肿瘤细胞中，含有两种二氯乙酸（DCA）轴向配体的DP被刺激性还原成铂(II)和DCA分子，同时谷胱甘肽被消除，氧化应激反应减弱。随后，DCA通过激活丙酮酸脱氢酶增加丙酮酸流入线粒体，并持续升高氧化磷酸化水平，彻底打破了肿瘤的氧化还原平衡，使过氧化氢的产生量增加了7.5倍，对MN介导的化学动力学治疗产生了增敏作用，最终使三阴性乳腺癌模型的抑瘤率达到89.5%。总之，这项工作通过代谢干预策略实现了细胞内环境全面、可持续的氧化应激升高，为增强氧化应激依赖性抗肿瘤疗法提供了一个巧妙的视角。

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引用次数: 0

Light-activated polymeric crosslinked nanocarriers as a checkpoint blockade immunoregulatory platform for synergistic tumor therapy 光活化聚合物交联纳米载体作为检查点阻断免疫调节平台用于肿瘤协同治疗

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.07.012

Yao Yang , Xiaotong Liang , Qimanguli Saiding , Jiachan Lin , Jinyuan Li , Wenyan Wang , Ping Huang , Li Huang , Wenfeng Zeng , Jinhai Huang , Hongzhong Chen , Wei Tao , Xiaowei Zeng

Photodynamic therapy (PDT) can enhance immune checkpoint blockade (ICB) antitumor immunity. However, PDT can significantly exacerbate the hypoxic tumor microenvironment and stimulate tumor neovascularization, promoting tumor invasion and metastasis. Camptothecin can inhibit angiogenesis by down-regulating hypoxia-inducible factor 1α (HIF-1α). Therefore, this study proposed to combine camptothecin with PDT for the first time to alleviate the disadvantage of PDT, and play its dual role of chemotherapy and antiangiogenesis. Here, a light-activated nanocarrier crosslinked the anti-PD-L1, photosensitizer, and camptothecin prodrug mildly with a thioketal bond for checkpoint blockade immunoregulation was designed. Firstly, photosensitizer-induced PDT and immunogenic cell death effect significantly increase T cell infiltration (33.3 % CD8⁺ increase), enhancing ICB antitumor immunity. Secondly, the antiangiogenic effect of camptothecin was beneficial for alleviating hypoxic tumor microenvironment exacerbated by PDT (HIF-1α expression decreased in tumor cells). Thirdly, light-activated release facilitates tumor accumulation (3.22 times) and controlled drug release. Thus, the immune checkpoint blockade combined with PDT and an antiangiogenic therapy of camptothecin creates a positive feedback co-delivery platform that exemplifies cascaded synergistic tumor therapy by checkpoint blockade immunoregulation. Besides, it also introduces a new strategy for combining small molecule drugs with macromolecules like proteins to treat various diseases.

光动力疗法（PDT）可以增强免疫检查点阻断（ICB）的抗肿瘤免疫力。然而，光动力疗法会明显加剧缺氧的肿瘤微环境，刺激肿瘤新生血管，促进肿瘤的侵袭和转移。喜树碱可通过下调缺氧诱导因子1α（HIF-1α）抑制血管生成。因此，本研究首次提出将喜树碱与光动力疗法相结合，以缓解光动力疗法的缺点，发挥其化疗和抗血管生成的双重作用。本文设计了一种将抗PD-L1、光敏剂和喜树碱原药以硫酮键温和交联的光激活纳米载体，用于检查点阻断免疫调节。首先，光敏剂诱导的PDT和免疫原性细胞死亡效应显著增加了T细胞浸润（CD8+增加33.3%），增强了ICB的抗肿瘤免疫力。其次，喜树碱的抗血管生成作用有利于缓解因 PDT 而恶化的缺氧肿瘤微环境（肿瘤细胞中 HIF-1α 的表达减少）。第三，光激活释放有利于肿瘤积聚（3.22 倍）和药物的可控释放。因此，免疫检查点阻断与光动力疗法和喜树碱抗血管生成疗法相结合，创建了一个正反馈联合给药平台，体现了检查点阻断免疫调节的级联协同肿瘤治疗。此外，它还介绍了一种将小分子药物与蛋白质等大分子结合治疗各种疾病的新策略。

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引用次数: 0