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CdS/ZnSe Quantum Dot Assembled Clusters vs. Dot-on-Rod: Charge Separation and Utilization for Efficient Photocatalytic NO3−-to-NH3 Conversion CdS/ZnSe量子点组装簇与点对棒:电荷分离与高效光催化NO3−到nh3转化的利用
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1002/adma.202517410
Yu-Lin Yin, Shu-Lin Meng, Xin-Ling Zhang, Jia-Hao Li, Chen Zhang, Chen-Ho Tung, Li-Zhu Wu
Photocatalytic NO3 reduction with semiconductor nanocrystals has promising prospects for ammonia (NH3) synthesis, which typically relies on broad light absorption, efficient charge separation, and high surface reactivity. Represented herein is, however, contrary to the widely accepted facts that long-lived charge separation favors higher photocatalytic efficiency, i.e. ZnSe@CdS dot-on-rods with better charge separation unexpectedly yield NH3 with much lower efficiency (4.10 mmol h−1 gcat.−1) than CdS/ZnSe assembled clusters (53.85 mmol h−1 gcat.−1). Mechanistic studies reveal that the intimate binding of ZnSe on CdS in dot-on-rods accelerates charge separation by 3 orders of magnitude, while the electron transfer from CdS to NO3 and the hole transfer from ZnSe to 1-phenylethanol proceed at 108 s−1. As a result, the comparable charge transfer rates in the assembled cluster of ZnSe and CdS quantum dots enable effective utilization of separated electrons and holes timely for photocatalytic NO3-to-NH3 reaction, while the imbalance of fast charge separation and slow utilization of electrons and holes in dot-on-rods leads to inferior NH3 yield. The kinetic balance for photocatalytic NO3-to-NH3 reaction offers valuable guidance for orchestrating multi-step photochemical events to realize elegant transformations.
利用半导体纳米晶体光催化还原NO3−合成氨(NH3)具有广阔的光吸收、高效的电荷分离和高的表面反应性。然而,本文所代表的与广泛接受的事实相反,即长时间的电荷分离有利于更高的光催化效率,即ZnSe@CdS具有更好电荷分离的棒上点意外地以低得多的效率(4.10 mmol h−1 gcat)产生NH3。cd /ZnSe组装簇(53.85 mmol h−1 gcat.−1)。机理研究表明,在点对棒中,ZnSe与CdS的紧密结合加速了3个数量级的电荷分离,同时电子从CdS转移到NO3 -和ZnSe到1-苯乙醇的空穴转移以108 s−1的速度进行。结果表明,ZnSe和CdS量子点组装簇中电荷转移速率相当,能够及时有效地利用分离的电子和空穴进行光催化NO3−- NH3反应,而点对棒中电荷快速分离与电子和空穴缓慢利用的不平衡导致NH3产率较低。光催化NO3−到nh3反应的动力学平衡为协调多步光化学事件以实现优雅的转化提供了有价值的指导。
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引用次数: 0
Proton Provision-Conversion-Spillover Cascade Programming on Dual Supported Pt Atoms for Robust Hydrogen Production 双支撑Pt原子上的质子供给-转换-溢出级联规划
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1002/adma.202522479
Mansheng Liao, Yuan Zhang, Qianyi Lin, Kaiming Liang, Yayun Hong, Lei Zhang
Rational proton engineering offers a powerful strategy for enhancing the hydrogen evolution reaction (HER) performance of single-atom catalysts (SACs). Notably, achieving concerted proton management across multiple reaction steps presents a highly efficient approach, yet it remains more challenging to implement than single-step regulation. Here, we propose a domino-type proton provision-conversion-spillover programming for Pt SACs in acidic HER, enabled by ultrathin porous nitrogen-doped carbon (main 1–2 atomic layers, sub-1 nm) encapsulated TiN nanowires with tips as dual-support tip-platform (Pt-NC1@TiN NWs). Experimental and theoretical results demonstrate that this platform triggers tip-distance-spillover domino effects to drive a proton cascade throughout HER. Specifically, NC1@TiN nanotips induce tip-enhanced effect that promotes interfacial proton accessibility. Concurrently, the short-distance Pt/TiN vertical coupling optimizes electronic modulation of unsaturated Pt-N2 sites to enhance their intrinsic activity. Exposed TiN sites function as hydrogen spillover centers to facilitate H2 desorption. Consequently, Pt-NC1@TiN NWs achieve a superior Pt mass activity of 153.5 A/mgPt@-100 mV, surpassing Pt/C by two orders of magnitude. Notably, it reaches 2 A/cm2 at low cell voltage of 1.75 V and sustains stable operation at 1 A/cm2 for 1200 h in proton exchange membrane water electrolyzer (PEMWE). This work indicates the potential of harnessing multi-step domino processes for advanced catalyst design.
合理的质子工程为提高单原子催化剂的析氢反应性能提供了有力的策略。值得注意的是,实现跨多个反应步骤的协调质子管理是一种高效的方法,但实施起来仍然比单步调节更具挑战性。在这里,我们提出了一个多米诺骨式质子供应-转换-溢出编程,用于酸性HER中的Pt SACs,通过超薄多孔氮掺杂碳(主要1-2原子层,sub- 1nm)封装TiN纳米线,尖端作为双支撑尖端平台(Pt-NC1@TiN NWs)实现。实验和理论结果表明,该平台触发尖端距离溢出多米诺骨牌效应,驱动质子级联贯穿HER。具体来说,NC1@TiN纳米尖端诱导了尖端增强效应,促进了界面质子的可及性。同时,短距离Pt/TiN垂直耦合优化了不饱和Pt- n2位点的电子调制,增强了其固有活性。暴露的TiN位点作为氢溢出中心,促进H2的解吸。因此,Pt-NC1@TiN NWs的Pt质量活度达到153.5 a /mgPt@-100 mV,比Pt/C高出两个数量级。值得注意的是,它在1.75 V的低电池电压下达到2 A/cm2,并在质子交换膜水电解槽(PEMWE)中以1 A/cm2稳定运行1200小时。这项工作表明利用多步骤多米诺过程进行先进催化剂设计的潜力。
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引用次数: 0
Bioinspired Engineered Virus-Mimetic Vesicles for Enhanced Cytosolic Delivery of STING Agonists Into Dendritic Cells 生物启发工程病毒模拟囊泡增强STING激动剂进入树突状细胞的胞浆输送
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1002/adma.202520019
Shi-Zhen Geng, Yaru Shi, Jinjin Yang, Yiwen Gao, Zhehao Zhang, Hao Wu, Pan-Miao Liu, Jinjin Shi, Yiling Yang, Jian-Jun Yang
Effective delivery to dendritic cells (DCs) is crucial for the clinical translation of STING agonists, however, current cyclic dinucleotide (CDN) therapies are hindered by inefficient cytosolic delivery and off-target activation-induced T cell exhaustion. Here, a high-fidelity, dengue virus-mimetic platform (CDN@VLP) is engineered to leverage natural tropism for precise cytosolic release in immature DCs. Compared to conventional lipid nanoparticles, CDN@VLP enhances DC-specific uptake by 1.9-fold while reducing non-specific T cell internalization in tumors by 14.8-fold, achieving comparable antitumor efficacy at one-fortieth the dose of free CDN. Systematic screening identifies an optimal VLP subtype that improves targeted accumulation in type 1 conventional DCs (cDC1s)—a subset essential for STING pathway activation—by 2.3-fold and amplifies durable type I interferon responses, resulting in a 12.8-fold increase in IFN-β production. Transcriptomic analysis further reveals that CDN@VLP promotes cDC1 recruitment into tumors by enhancing the secretion of key chemokines (XCL1, CCL4, and CCL5), suggesting an additional mechanism of action. By mimicking viral tropism, the CDN@VLP platform establishes a paradigm for precision STING activation, overcoming the trade-off between potency and specificity in cDC1-targeted immunotherapy.
有效递送到树突状细胞(dc)对于STING激动剂的临床翻译至关重要,然而,目前的环二核苷酸(CDN)治疗受到低效的细胞质递送和脱靶激活诱导的T细胞衰竭的阻碍。在这里,一个高保真度的登革热病毒模拟平台(CDN@VLP)被设计为利用自然趋向性在未成熟的树突状细胞中精确释放细胞质。与传统的脂质纳米颗粒相比,CDN@VLP将dc特异性摄取提高了1.9倍,同时将肿瘤中的非特异性T细胞内化降低了14.8倍,在游离CDN剂量的十分之一下达到相当的抗肿瘤效果。系统筛选确定了一种最佳的VLP亚型,该亚型可将1型常规dc (cDC1s) (STING通路激活所必需的子集)的靶向积累提高2.3倍,并放大持久的I型干扰素反应,从而使IFN-β的产生增加12.8倍。转录组学分析进一步揭示CDN@VLP通过增强关键趋化因子(XCL1、CCL4和CCL5)的分泌来促进cDC1向肿瘤募集,提示了另一种作用机制。通过模仿病毒的趋向性,CDN@VLP平台建立了精确STING激活的范例,克服了cdc1靶向免疫治疗中效力和特异性之间的权衡。
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引用次数: 0
Efficient Non-Invasive Rejuvenation of Spent Lithium Iron Phosphate Batteries Through Controlled Overdischarge. 通过控制过放电实现废旧磷酸铁锂电池的高效无创再生。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1002/adma.202522927
Jinu Song, Yujie Chen, Nianji Zhang, Cancan Peng, Huan Li, Chao Ye, Shi-Zhang Qiao

Recycling lithium iron phosphate (LFP) batteries presents critical economic and environmental challenges because of their low metal value and high energy intensity of conventional metallurgical processes. While direct recycling methods offer a pathway for lithium replenishment, they are often hindered by stringent impurity controls and complex operating conditions that limit scalability. Here, we introduce a controlled overdischarge (COD) protocol as a non-invasive strategy to rejuvenate spent LFP (S-LFP) batteries. COD selectively decomposes the solid-electrolyte interphase, releasing trapped Li+ and reducing Li/Fe antisite defects while simultaneously suppressing copper dissolution. The COD protocol recovers 9.56% of lost capacity and extends lifespan by over 200 cycles. Furthermore, compared to metallurgical recycling, this method markedly lowers greenhouse gas emissions to 168 g kg-1 and energy consumption to 3 MJ kg-1 of feedstock. These findings highlight COD as a sustainable and scalable alternative for S-LFP battery recycling.

磷酸铁锂(LFP)电池由于其低金属价值和传统冶金工艺的高能量强度,对其回收提出了严峻的经济和环境挑战。虽然直接回收方法为锂的补充提供了一条途径,但它们往往受到严格的杂质控制和复杂的操作条件的阻碍,限制了可扩展性。在这里,我们介绍了一种控制过放电(COD)协议,作为一种非侵入性策略来恢复废LFP (S-LFP)电池的活力。COD选择性地分解固体-电解质界面,释放捕获的Li+,减少Li/Fe对位缺陷,同时抑制铜的溶解。COD协议恢复了9.56%的丢失容量,延长了200多个周期的使用寿命。此外,与冶金回收相比,该方法显著降低温室气体排放量至168 g kg-1,能源消耗至3 MJ kg-1。这些发现强调了COD作为S-LFP电池回收的可持续和可扩展的替代方案。
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引用次数: 0
Construction and Microenvironment Regulation of Short Charge Transfer Tunnel at MOF/COF Heterointerfaces for Visible-Light-Driven Hydrogen Evolution MOF/COF异质界面短电荷转移隧道的构建及微环境调控
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1002/adma.202522294
Hanxi Li, Zhi-Gang Li, Xinghao Zhang, Huiye Jiao, Haichao Wang, Zhenhai Fan, Yutong Wang, Yang Li, Jijie Zhang, Xian-He Bu
Raising electron transfer efficiency is a crucial issue in improving photocatalytic productivity. Herein, we propose a strategy for anchoring single atoms and the establishment of a short-distance electron transport pathway. By incorporating nitrogen-containing monodentate ligands into UIO-66-NH2, Pt single atom could be co-anchored by both the nitrogen atom and the vacant Zr-oxo cluster. Subsequently, the Pt-containing UIO was condensed with TpPa-1. Thereby, a molecular-level electron transfer pathway from TpPa to Pt has been established at the heterointerface between TpPa and UIO. By rationally adjusting the positions of the functional groups (-H, -Cl, and -OCH3) in the monodentate ligand, their involvement in the pathway was precisely regulated. They functioned as electron relays when positioned at the ortho-position of the amino group, thereby facilitating the electron delivery. Cl exhibited a more pronounced effect compared to OCH3, UPT-o-Cl achieved the maximum H2 yield of 14.21 mmol g−1 h−1. Mechanism calculations revealed that the groups located along the pathway would regulate the microenvironment of the constructed tunnels, resulting in a higher electron density and enhanced ability to adsorb H intermediates of the Pt sites. This research reports a strategy for precisely regulating the microenvironment adjacent to the active site, providing new insights into enhancing carrier mobility and utilization efficiency.
提高电子传递效率是提高光催化效率的关键问题。在此,我们提出了一种锚定单原子和建立短距离电子传递途径的策略。通过将含氮单齿配体加入到UIO-66-NH2中,Pt单原子可以被氮原子和空的Zr-oxo簇共同锚定。随后,含pt的UIO与tpa -1缩合。因此,在TpPa和UIO之间的异质界面上建立了从TpPa到Pt的分子水平的电子转移途径。通过合理调节单齿配体中官能团(-H、-Cl、-OCH3)的位置,精确调节其参与该通路。当它们位于氨基的邻位时,它们起电子继电器的作用,从而促进电子的传递。与OCH3相比,Cl的作用更明显,UPT-o-Cl的H2产率最高,为14.21 mmol g−1 h−1。机制计算表明,位于通道沿线的基团会调节构建的隧道的微环境,导致更高的电子密度和对Pt位点的H中间体的吸附能力增强。本研究报告了一种精确调节活性位点附近微环境的策略,为提高载体的移动性和利用效率提供了新的见解。
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引用次数: 0
Broadband Excitation of Antiferromagnetic Dynamics by Acoustic Phonons 声子对反铁磁动力学的宽带激励
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1002/adma.202521359
Shixuan Liang, Wenxuan Zhu, Chong Chen, Mingyuan Ma, Weiaqi Du, Lei Han, Yanzhang Cao, Yichen Su, Shihai An, Zhiyuan Zhou, Sulei Fu, Yuyan Wang, Feng Pan, Cheng Song
Excitation of antiferromagnetic dynamics is at the core of ultrafast spintronics. Coherent excitation of antiferromagnetic magnons is typically monochromatic, confined at dispersion intersections between antiferromagnetic magnons and the excitation source. Broadband excitation can be enabled by introducing electron spins in an incoherent manner, albeit accompanied by high energy consumption from Joule heating. Here, we demonstrate a broadband excitation of antiferromagnetic dynamics of 2D antiferromagnet CrSBr without Joule heating, by Rayleigh-type surface acoustic wave (R-SAW). Incoherent magnons are efficiently excited via the angular momentum transfer from acoustic phonons, across a wide range up to the spin-flop field. The collinear alignment between the Néel vector and phonon angular momenta induces strong excitation of magnons with high phonon dissipation, whereas orthogonal alignment suppresses dissipation, as revealed by R-SAW transmission. Our work uncovers a mutual interplay between phonon transport and antiferromagnetic order parameters, offering a broadband, low-loss route to manipulate antiferromagnetic dynamics.
反铁磁动力学的激发是超快自旋电子学的核心。反铁磁磁子的相干激发通常是单色的,局限于反铁磁磁子与激发源之间的色散交叉点。宽带激发可以通过以非相干方式引入电子自旋来实现,尽管伴随着焦耳加热的高能量消耗。本文利用瑞利型表面声波(R-SAW)对二维反铁磁CrSBr进行了无焦耳加热的宽带激励。非相干磁振子通过声子的角动量传递有效地激发,在宽范围内直至自旋翻转场。由R-SAW透射可知,nsamel矢量与声子角动量的共线排列诱导了高声子耗散的强磁振子激发,而正交排列抑制了耗散。我们的工作揭示了声子输运和反铁磁有序参数之间的相互作用,为操纵反铁磁动力学提供了一种宽带、低损耗的途径。
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引用次数: 0
Elemental Selenium Phase-Change Material for Scalable Ultra-Low-Loss Programmable Photonics 用于可扩展超低损耗可编程光子学的硒元素相变材料
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1002/adma.202520056
Wentao Huang, Hu Wang, Shanshan Wang, Menglin Huang, Yuting Sun, Weijun Weng, Zhitang Song, Jiabin Shen, Shiyou Chen, Zengguang Cheng, Peng Zhou
Chalcogenide phase-change photonics has revolutionized reconfigurable optics by enabling nonvolatile light-matter control. While low-loss phase-change materials (PCMs) with near-zero extinction coefficients (k ≈ 0) unlock ideal phase-only modulation, their growing compositional complexity hinders uniform fabrication and switching stability. Here, we introduce an elemental solution: wafer-scale (8-inch) selenium (Se) thin films achieving unprecedented uniformity, full near-infrared transparency, and ultralow losses across the visible range, meanwhile sustaining one million (106) reversible cycles without degradation. First-principles calculations reveal that the giant refractive index switching (Δn ≈ 0.6) stems from the unique fracture-reconfiguration dynamics of Se helical chains. Furthermore, we demonstrate a manufacturable, etch-free platform with laser-reconfigurable patterns for dynamic image generation and Gaussian-vortex beam conversion. By harmonizing atomic simplicity with device-grade scalability, this elemental PCM establishes a new paradigm for high-performance programmable photonics.
硫系相变光子学通过实现非挥发性光物质控制,彻底改变了可重构光学。虽然具有接近零消光系数(k≈0)的低损耗相变材料(pcm)解锁了理想的纯相位调制,但其日益增长的成分复杂性阻碍了均匀制造和开关稳定性。在这里,我们介绍了一种基本解决方案:晶圆级(8英寸)硒(Se)薄膜,具有前所未有的均匀性,完全的近红外透明度,以及在可见光范围内的超低损耗,同时可以维持100万(106)个可逆循环而不会降解。第一线原理计算表明,巨大的折射率转换(Δn≈0.6)源于硒螺旋链独特的断裂-重构动力学。此外,我们展示了一个可制造的、无蚀刻的平台,该平台具有用于动态图像生成和高斯涡旋光束转换的激光可重构模式。通过协调原子简单性和器件级可扩展性,这种元素PCM建立了高性能可编程光子学的新范例。
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引用次数: 0
Solar-Powered Radiation Cooling/Heating for Advanced Thermal Management of Wound 用于伤口高级热管理的太阳能辐射冷却/加热
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1002/adma.202520985
Junyi Lu, Jiayi Mao, Chenyu Zong, Juan Wang, Guangxin Gu, Wenguo Cui
Active heating and cooling techniques are widely used in biological tissue regeneration. However, given the growing emphasis on environmental sustainability, heat exchange without additional energy input is receiving increasing attention. This Perspective examines the influence of temperature on wound healing and explores the potential of passive radiative cooling and passive radiative heating for thermal wound management. The advantages are highlighted, relevant application scenarios outlined, and current challenges identified, with the aim of proposing novel zero-energy wound treatment strategies for the biomedical field.
主动加热和主动冷却技术在生物组织再生中应用广泛。然而,由于日益强调环境的可持续性,无需额外能源投入的热交换正受到越来越多的关注。本展望研究了温度对伤口愈合的影响,并探讨了被动辐射冷却和被动辐射加热在热伤口管理中的潜力。强调了其优势,概述了相关的应用场景,并确定了当前的挑战,旨在为生物医学领域提出新的零能量伤口治疗策略。
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引用次数: 0
Cu+-Driven Ferroionic Structure and Pressure-Tunable Magnetism in Layered Thiophosphate CuVP2S6. 层状硫代磷酸盐CuVP2S6的Cu+驱动铁离子结构和可调压磁性。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1002/adma.202520850
Ruichen Xie, Zhongchong Lin, Yan Cao, Chao Yun, Zhi Zhang, Shaohua Fan, Yuxuan Peng, Xiaobai Ma, Kewei Li, Caijuan Shi, Dong Zhou, Rui Han, Honglin Du, Xiaoxi Liu, Zhaochu Luo, Jinbo Yang, Wenyun Yang

Two-dimensional (2D) van der Waals (vdW) magnets offer a versatile platform to explore fundamental physics and low-dimensional functionalities. Metal thiophosphates (MTPs) with mobile Cu+ ions exhibit a ferroionic state, where polarization arises from ionic redistribution among multiple nearly degenerate sites. CuVP2S6 uniquely combines intrinsic ferromagnetism from the V sublattice with Cu+-driven ferroionic configurational freedom, enabling direct exploration of how ionic dynamics influence magnetic interactions. Herein, high-quality CuVP2S6 single crystals are synthesized, and their structural and physical properties are systematically investigated. Temperature-dependent neutron diffraction elucidates a ferroionic structure with dynamic distributions of copper ions across multiple crystallographic sites. The versatile occupations are driven by local symmetry-controlled orbital interactions between copper ions and surrounding ligands through a second-order Jahn-Teller mechanism. Magnetic measurements identify a ferromagnetic (FM) transition below 3.3 K. The pressure-controlled magnetocrystalline anisotropy and interlayer exchange interactions mediated by Cu+ migration are demonstrated, boosting the Curie temperature remarkably by over 60% and inducing a soft-to-hard FM transition unparalleled within the MTP family. These results demonstrate that ionic configurational freedom provides an efficient route to control magnetism, opening new possibilities for spintronic applications.

二维(2D)范德华(vdW)磁体为探索基础物理和低维功能提供了一个通用的平台。金属硫代磷酸盐(MTPs)具有可移动的Cu+离子表现出铁离子状态,其中极化是由离子在多个近简并位点之间的重新分配引起的。CuVP2S6独特地结合了V亚晶格的固有铁磁性和Cu+驱动的铁离子构型自由,从而可以直接探索离子动力学如何影响磁相互作用。本文合成了高质量的CuVP2S6单晶,并对其结构和物理性质进行了系统的研究。温度相关的中子衍射阐明了铁离子结构与铜离子的动态分布跨越多个晶体的位置。铜离子与周围配体之间的局部对称控制轨道相互作用通过二阶Jahn-Teller机制驱动了多用途占据。磁测量识别铁磁(FM)跃迁低于3.3 K。Cu+迁移介导的压力控制磁晶各向异性和层间交换相互作用,显著提高了居里温度60%以上,并诱导了MTP家族中无与伦比的软-硬FM转变。这些结果表明,离子构型自由提供了控制磁性的有效途径,为自旋电子应用开辟了新的可能性。
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引用次数: 0
Coupling Pt Single-Atoms with Amorphous LDH Nanosheets as a High-Efficiency Sonosensitizer for Sonodynamic Immunotherapy. 铂单原子与非晶LDH纳米片耦合作为声动力免疫治疗的高效声敏剂。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1002/adma.72457
Tao Wang, Tingting Hu, Shibo Wang, Ruimin Xue, Chen Zhao, Boming Liu, Yu Yang, Chaojie Yu, Hai Li, Ruizheng Liang

Sonodynamic therapy (SDT) represents a minimally invasive alternative for cancer treatment. However, its efficacy is constrained by the insufficient reactive oxygen species generation of inorganic sonosensitizers due to wide bandgaps, rapid electron-hole recombination, and insufficient oxygen adsorption/activation. Herein, we report for the first time a novel sonosensitizer constructed by anchoring Pt single-atoms onto amorphous CoMgMo-layered double hydroxide (Pt/a-LDH) for high-efficiency sonodynamic immunotherapy. Through the synergy of defect engineering and single-atom modification, Pt/a-LDH achieves sharp bandgap reduction (from 2.4 to 0.6 eV) and abundant defective environment, dramatically promoting charge separation and inhibiting electron-hole recombination (an inhibition rate of 89.8%). Moreover, the unique 2D structure and hydroxyl coordination environment of LDH yield ultrahigh single-atom loading efficiency and defect density, which significantly promote oxygen adsorption/activation, reduce reaction energy barrier (bond energy from 3.6 to 2.1 eV), and accelerate reaction kinetics. Consequently, Pt/a-LDH achieves a significant enhancement in sonodynamic performance, generating singlet oxygen at 5.3 and 38.2 times that of CoMgMo-LDH and TiO2 sonosensitizer, respectively. In vivo assays demonstrate that polyethylene glycol-modified Pt/a-LDH induces robust immunogenic cell death, activates dendritic cell maturation, stimulates T-cell infiltration, and reprograms the immunosuppressive tumor microenvironment, offering a new paradigm for high-performance sonodynamic immunotherapy.

声动力疗法(SDT)是一种微创的癌症治疗方法。然而,由于带隙宽、电子-空穴复合快、氧吸附/活化不足,无机声敏剂的活性氧生成不足,限制了其效果。在此,我们首次报道了一种新型的声敏剂,它将Pt单原子锚定在无定形comgmo层状双氢氧化物(Pt/a- ldh)上,用于高效的声动力免疫治疗。通过缺陷工程和单原子修饰的协同作用,Pt/a-LDH实现了带隙的大幅缩小(从2.4 eV降至0.6 eV)和丰富的缺陷环境,显著促进了电荷分离,抑制了电子-空穴复合(抑制率为89.8%)。此外,LDH独特的二维结构和羟基配位环境产生了超高的单原子负载效率和缺陷密度,显著促进了氧的吸附/活化,降低了反应能垒(键能从3.6 eV降至2.1 eV),加速了反应动力学。因此,Pt/a- ldh显著提高了声动力性能,产生的单重态氧分别是CoMgMo-LDH和TiO2声敏剂的5.3倍和38.2倍。体内实验表明,聚乙二醇修饰的Pt/a- ldh诱导免疫原性细胞死亡,激活树突状细胞成熟,刺激t细胞浸润,并重新编程免疫抑制肿瘤微环境,为高性能声动力免疫治疗提供了新的范例。
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引用次数: 0
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