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Fast and Trap-Minimized Li Transport via Size-Mismatch-Driven Cation-Ordering Control in Li-Excess Disordered Rocksalt Cathodes. 在Li- excess无序岩盐阴极中通过尺寸错配驱动的阳离子排序控制快速和最小化陷阱Li输运。
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-24 DOI: 10.1021/acsnano.5c22044
Jinho Ahn,Bonyoung Ku,Hyunji Kweon,Hoseok Lee,Hobin Ahn,Myungeun Choi,Myeong Hwan Lee,Moonsu Yoon,Junghyun Choi,Jihyun Hong,Jongsoon Kim
Li-excess cation-disordered rocksalt (DRX) is considered a promising cathode for lithium-ion batteries owing to its high-energy densities. However, short-range cation ordering (SRCO) commonly arises in DRX cathodes due to local electrostatic interactions and size similarities among cations, resulting in Li-trapping and sluggish Li-transport. Here, we propose that the SRCO suppression in the DRX system can be achieved without complex high-entropy composition by simultaneously tuning electrostatic interactions and the cationic size effect. The incorporation of Ti4+ into Li-Nb/Mn DRX, being lower-valent and smaller than Nb5+, weakens high-valence-driven interactions and increases the ionic size mismatch with Li+, thereby promoting Li/TM mixing and energetically disfavoring the SRCO formation. Thus, a low-entropy DRX, Li1.2Nb0.15Mn0.55Ti0.1O2 (LNM-0.1Ti) exhibits significantly enhanced Li+ transport, reduced voltage hysteresis, and improved structural stability compared to Li1.2Nb0.2Mn0.6O2 (LNM) due to disruption of SRCO. LNM-0.1Ti delivers a high capacity of ∼327 mAh g-1 and an energy density of ∼1026 Wh kg-1, outperforming LNM (∼274 mAh g-1, ∼837 Wh kg-1). Notably, the higher-Ti composition, Li1.2Nb0.1Mn0.5Ti0.2O2, exhibits reduced rate capability and energy density compared with LNM-0.1Ti, underscoring the importance of compositional balance in optimizing low-entropy DRX performance. These findings highlight a practical strategy for the development of high-performance DRX cathodes.
锂过量阳离子无序岩盐(DRX)因其高能量密度被认为是锂离子电池极具前景的阴极材料。然而,由于局部静电相互作用和阳离子之间的尺寸相似性,在DRX阴极中通常会出现短程阳离子有序(SRCO),导致锂捕获和锂传输缓慢。在这里,我们提出可以通过同时调整静电相互作用和阳离子尺寸效应来实现DRX系统中SRCO的抑制,而无需复杂的高熵组成。Ti4+在Li- nb /Mn DRX中的掺入比Nb5+价低且体积小,减弱了高价驱动的相互作用,增加了与Li+的离子尺寸失配,从而促进了Li/TM混合,在能量上不利于SRCO的形成。因此,由于SRCO的破坏,低熵DRX, li1.2 nb0.2 mn0.55 ti0.1 o2 (LNM-0.1 ti)与Li1.2Nb0.2Mn0.6O2 (LNM)相比,Li+输运显著增强,电压滞后降低,结构稳定性提高。LNM-0.1 ti的高容量为~ 327 mAh g-1,能量密度为~ 1026 Wh kg-1,优于LNM (~ 274 mAh g-1, ~ 837 Wh kg-1)。值得注意的是,与LNM-0.1Ti相比,高ti成分Li1.2Nb0.1Mn0.5Ti0.2O2表现出较低的速率能力和能量密度,强调了成分平衡对优化低熵DRX性能的重要性。这些发现强调了开发高性能DRX阴极的实用策略。
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引用次数: 0
Multimetallic Pt-Based Alloy Nanowires Library as a Platform for Selective Electrocatalytic Oxidation of Ethylene Glycol. 多金属pt基合金纳米线库作为乙二醇选择性电催化氧化的平台。
IF 16 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-24 Epub Date: 2026-03-08 DOI: 10.1021/acsnano.5c21597
Yaming Liu, Zhenle Hu, Xinrui Zhu, Xinyu Li, Tong Zuo, Yutian Zhao, Guoqiang Liu, Yanting Cheng, Chao Zhi, Jiaguang Meng, Xiang Li, Jingnan Wang, Mingshang Jin

While traditional Pt-based catalysts suffer from inadequate selectivity and stability in electrocatalytic ethylene glycol oxidation reactions, we present a general and scalable synthesis strategy, fabricating a broad multimetallic Pt-based alloy nanowires (NWs) library from binary to quinary. Among these, the PtAgCuRhRu NWs exhibit exceptional performance, with a mass activity ∼8 times higher than that of Pt/C and a Faradaic efficiency for glycolic acid (GA) reaching 93.49%. In the membrane electrode assembly electrolyzer, the catalyst maintained its activity over 140 h with 99% GA selectivity. In situ experimental and theoretical calculations reveal oxygenophilic Rh and Ru promote *OH adsorption, facilitating the conversion of *COCH2OH to GA and the oxidative removal of COads, enhancing activity and stability. Additionally, the high energy barrier for C-C bond cleavage suppresses undesired decomposition due to the introduction of Ag and Cu, leading to superior GA selectivity.

虽然传统的pt基催化剂在电催化乙二醇氧化反应中选择性和稳定性不足,但我们提出了一种通用的、可扩展的合成策略,制造了从二元到五元的广泛的多金属pt基合金纳米线(NWs)库。其中,PtAgCuRhRu NWs表现出优异的性能,其质量活性比Pt/C高~ 8倍,对乙醇酸(GA)的法拉第效率达到93.49%。在膜电极组装电解槽中,催化剂的活性保持在140 h以上,GA选择性达到99%。原位实验和理论计算表明,亲氧性Rh和Ru促进*OH吸附,促进*COCH2OH转化为GA和氧化去除COads,增强活性和稳定性。此外,C-C键的高能量势垒抑制了由于Ag和Cu的引入而导致的不希望的分解,从而导致优越的GA选择性。
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引用次数: 0
Chiral Carbon Dots as Nanoantennas for Amplification of Molecular Chirality. 手性碳点作为纳米天线用于分子手性放大。
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-24 DOI: 10.1021/acsnano.5c22147
Mateusz Pawlak,Aleksandra Wajda,Zofia Rejman,Maciej Roman,Tomasz P Wróbel,Agnieszka Kaczor
We present herein a previously unreported chiroptical phenomenon, leveraging the intrinsic optical nanoscale-originated properties of chiral (l- and d-cysteine derived) carbon dots (C-Dots), specifically, their surface (low-lying electronic excited) states. We show here that these structures generate an exceptional chiroptical response that, furthermore, can be transferred to molecularly chiral entities interacting with C-Dots. In such assemblies, C-Dots behave as nanoantennas, losing their own chiral identity to the advantage of the newly formed chiral (nano)assemblies that show at least 20-times higher intensity of vibrational optical activity compared to the molecular chirality signal. In a conceptual way, the observed phenomenon is similar to surface-enhanced Raman and Raman optical activity (ROA) spectroscopies, in which nanoparticles, in resonance with the incoming light, enhance the electromagnetic field around analyzed molecules, amplifying their Raman or ROA signal. Our findings enable the application of C-Dots as highly efficient chirality nanosensors which, in light of their rich surface chemistry, translates to the broad potential for the development of C-Dots-based nanoprobes with tailored properties as well as for the rational design of next-generation chiral nanomaterials.
我们在此提出了一个以前未报道的手性现象,利用手性(l-和d-半胱氨酸衍生)碳点(C-Dots)固有的光学纳米级性质,特别是它们的表面(低洼电子激发态)。我们在这里表明,这些结构产生了一个特殊的手性反应,而且,可以转移到与C-Dots相互作用的分子手性实体。在这种组合中,C-Dots表现为纳米天线,失去了自己的手性特性,而新形成的手性(纳米)组合的优势在于,与分子手性信号相比,C-Dots表现出至少20倍的振动光学活性强度。从概念上讲,观察到的现象类似于表面增强拉曼和拉曼光学活性(ROA)光谱,其中纳米颗粒与入射光共振,增强被分析分子周围的电磁场,放大其拉曼或ROA信号。我们的研究结果使C-Dots作为高效手性纳米传感器的应用成为可能,鉴于其丰富的表面化学性质,这为开发具有定制性能的基于C-Dots的纳米探针以及合理设计下一代手性纳米材料提供了广阔的潜力。
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引用次数: 0
Digital Immunoassays for Sensitive Quantification of Blood Biomarkers Using Solid-State Nanopores. 使用固体纳米孔对血液生物标志物进行敏感定量的数字免疫分析。
IF 16 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-24 DOI: 10.1021/acsnano.5c16690
Liqun He, Breeana Elliott, Philipp Mensing, Kyle Briggs, Michel Godin, Jonathan Flax, James McGrath, Vincent Tabard-Cossa

Digital immunoassays enable highly sensitive detection of biomolecules, offering absolute quantification rather than relying on bulk signal intensity. We adapt a digital immunoassay scheme for a nanopore sensor, a versatile platform for single-molecule counting. Current nanopore sensors have demonstrated great progress when counting nucleic acids but struggle with proteins due to variability in translocation behavior and limited recognition strategies. While recent advancements have highlighted the promise of nanopore platforms for protein studies, precise quantification remains a challenge. Here, building on previous work, we present a nanopore-based digital immunoassay that employs gold nanoparticle-mediated molecular amplification with a single-molecule readout. This approach translates protein recognition into quantifiable DNA, enabling a precise digital assay. This assay employs a DNA NanoLock probe combined with a paramagnetic bead-based immunocapture, where the target proteins trigger a structural transformation of the NanoLock, converting their presence into a binary DNA-based signal. By incorporating AuNPs carrying hundreds of DNA proxy reporters, we effectively amplify the detectable signal by 2 orders of magnitude, significantly improving sensitivity. We validate the performance of this system by detecting the glial fibrillary acidic protein, a biomarker for traumatic brain injury and neurodegenerative diseases, in plasma samples and demonstrate high femtomolar-level sensitivity (∼40 pg/mL). Using the NanoLock probe, we further mitigate previous challenges, with reduced assay times (hours) and extended dynamic range (3-log). The self-calibrating nature of this digital approach offers robust, reproducible measurements across different nanopores, eliminating interdevice variability.

数字免疫分析能够高度灵敏地检测生物分子,提供绝对定量,而不是依赖于大量信号强度。我们为纳米孔传感器采用了数字免疫分析方案,这是一种用于单分子计数的多功能平台。目前的纳米孔传感器在计算核酸方面已经取得了很大的进步,但由于易位行为的可变性和有限的识别策略,它们在计算蛋白质方面存在困难。虽然最近的进展突出了纳米孔平台用于蛋白质研究的前景,但精确的量化仍然是一个挑战。在此,在先前工作的基础上,我们提出了一种基于纳米孔的数字免疫测定方法,该方法采用金纳米颗粒介导的分子扩增和单分子读数。这种方法将蛋白质识别转化为可量化的DNA,从而实现精确的数字分析。该试验采用DNA NanoLock探针结合基于顺磁珠的免疫捕获,其中靶蛋白触发NanoLock的结构转化,将其存在转化为基于二进制DNA的信号。通过整合携带数百个DNA代理报告基因的aunp,我们有效地将可检测信号放大了2个数量级,显著提高了灵敏度。我们通过检测血浆样本中的神经胶质纤维酸性蛋白(一种创伤性脑损伤和神经退行性疾病的生物标志物)来验证该系统的性能,并显示出高飞摩尔水平的灵敏度(~ 40 pg/mL)。使用NanoLock探针,我们进一步减轻了之前的挑战,减少了分析时间(小时),扩大了动态范围(3-log)。这种数字方法的自校准特性提供了跨不同纳米孔的可靠、可重复的测量,消除了设备间的可变性。
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引用次数: 0
In Situ Electrochemical Construction of CoCu2O Nanoclusters for Efficient Nitrate-to-Ammonia Electroreduction. 硝酸-氨电还原CoCu2O纳米团簇的原位电化学构建
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-23 DOI: 10.1021/acsnano.5c18616
Xu Luo,Jianying Wang,Xinyi Liu,Xiaozhi Xu,Dahui Fang,Yun Zhao,Feng Xie,Zhigang Shao
Designing highly efficient and synergistic electrocatalysts for the electrochemical nitrate reduction reaction (NO3RR) toward ammonia (NH3) is crucial for developing green, sustainable, and scalable pathways for NH3 synthesis. This study used a in situ electrochemical reduction strategy to construct CoCu2O nanoparticles on a CoCuHHTP substrate, successfully fabricating a CoCu2O@CoCuHHTP catalyst. The characterization techniques, including TEM, XRD, XPS, and FTIR, revealed that the CoCuHHTP surface was uniformly decorated with 2-5 nm CoCu2O nanoparticles. Moreover, the partially reduced substrate exposed abundant noncoordi-nated hydroxyl groups, which provided an ideal microenvironment for the adsorption of reaction intermediates and a stable proton transfer. A combination of electrochemical measurements, in situ spectroscopic/mass spectrometric analyses, and DFT calculations was used to elucidate the synergistic catalytic mechanism. CoCu2O acted as an efficient water dissociation center to continuously supply abundant hydrogen adatoms (Had), while the numerous hydroxyl groups in the partially reduced CoCuHHTP substrate stabilized various key nitrogen-containing intermediates (e.g., *NO3, *NO2, *NO, and *NOH) via hydrogen bonding. Consequently, this effectively suppressed the byproduct formation, which significantly reduced the reaction energy barrier and synergistically promoted efficient NH3 generation with high selectivity. DFT calculations further confirmed, at the atomic level, the NO3- adsorption and *NO hydrogenation step, is identified as the rate-determining step, that on the HHTP-modified CoCu2O(111) surface were only 0.54 and 0.55 eV, respectively, which were significantly lower than those on CoCuHHTP (0.98 and 1.16 eV) and pure CoCu2O (0.80 and 0.68 eV). This highlighted the critical role of hydrogen bonding in optimizing the reaction pathway and enhancing the intrinsic activity. Electrochemical performance tests demonstrated that CoCu2O@CoCuHHTP achieved a 1200 μmol h-1 cm-2 NH3 production rate at - 0.6 V (vs RHE), which was 3.5 times higher than that of pristine CoCuHHTP, with up to 97.9% faradaic efficiency for NH3 (FENH3). In a flow electrolyzer coupled with the oxygen evolution reaction, the catalyst operated stably for 1800 h (30 cycles) at 100 mA cm-2 while maintaining an above 80% FENH3, which demonstrated an exceptional catalytic stability and practical application potential.
设计高效、协同的硝酸还原反应(NO3RR)电催化剂是开发绿色、可持续、可扩展的氨合成途径的关键。本研究采用原位电化学还原策略在CoCuHHTP衬底上构建CoCu2O纳米颗粒,成功制备了CoCu2O@CoCuHHTP催化剂。TEM、XRD、XPS、FTIR等表征技术表明,CoCuHHTP表面被2 ~ 5 nm的CoCu2O纳米粒子均匀修饰。此外,部分还原的底物暴露出丰富的非配位羟基,为反应中间体的吸附和稳定的质子转移提供了理想的微环境。电化学测量、原位光谱/质谱分析和DFT计算相结合,阐明了协同催化机理。CoCu2O作为高效的水解离中心,持续提供丰富的附氢原子(Had),而部分还原的CoCuHHTP底物中大量的羟基通过氢键稳定了各种关键含氮中间体(如*NO3、*NO2、*NO和*NOH)。因此,这有效地抑制了副产物的形成,显著降低了反应能垒,协同促进了高选择性高效NH3的生成。DFT计算进一步证实,在原子水平上,NO3-吸附和*NO加氢步骤被确定为速率决定步骤,在htp修饰的CoCu2O(111)表面分别仅为0.54和0.55 eV,显著低于CoCuHHTP(0.98和1.16 eV)和纯CoCu2O(0.80和0.68 eV)。这突出了氢键在优化反应途径和提高内在活性方面的关键作用。电化学性能测试表明,CoCu2O@CoCuHHTP在- 0.6 V (vs RHE)下NH3的产率为1200 μmol h-1 cm-2,是原始CoCuHHTP的3.5倍,NH3 (FENH3)的法拉第效率高达97.9%。实验结果表明,该催化剂在100 mA cm-2条件下稳定运行1800 h(30个循环),同时FENH3含量保持在80%以上,具有优异的催化稳定性和实际应用潜力。
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引用次数: 0
An Engineered Triple-Functional Nanoplatform for Effective Sepsis Therapy via Macrophage-Targeted Polo-like Kinase 1 Inhibition. 通过巨噬细胞靶向polo样激酶1抑制有效治疗败血症的工程三功能纳米平台。
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-23 DOI: 10.1021/acsnano.5c20947
Chuang Yuan,Hongli Li,Yunlong Gao,Rui Zeng,Zichao Luo,Xinyu Yang
Sepsis accounts for 20% of global mortality, largely driven by dysregulated hyperactivation of macrophages that disrupts immune homeostasis. Current anti-inflammatory strategies often compromise pathogen clearance and exacerbate immunosuppression. Precisely targeting hyperactivated macrophages while preserving antimicrobial function represents a promising therapeutic approach. Through high-throughput screening of 390 kinase inhibitors in hyperactivated macrophages, we identified the polo-like kinase 1 (PLK1) inhibitor GSK461364 as a potent modulator of hyperactivation. However, its clinical translation is limited by dose-dependent cytotoxicity and systemic toxicity. To address this, we engineered mannose-functionalized nanoparticles (Nano-PLK1in) for targeted combinatorial delivery of the inhibitor and glutathione to hyperactive macrophages. These nanoparticles significantly enhanced cellular uptake, approximately 2-fold, in both murine and human hyperactivated macrophages. The triple-action Nano-PLK1in platform enables: (i) precision inhibition of the caspase-11 pathway via PLK1 blockade, (ii) reactivation of redox homeostasis through glutathione-mediated mitochondrial protection, and (iii) preservation of antimicrobial capacity without broad immunosuppression. In murine models of sepsis, Nano-PLK1in markedly improved survival by 50% compared to free drug, along with a 41.8% reduction in coagulopathy and a 28.9-54.3% decrease in ALT/creatinine levels reflecting multiorgan protection, and enhanced bacterial clearance. By integrating precision macrophage reprogramming with effective pathogen eradication, our nanoscale engineering strategy surmounts the efficacy-toxicity trade-off of conventional therapies, highlighting its translational promise for sepsis treatment.
脓毒症占全球死亡率的20%,主要由巨噬细胞过度激活失调引起,破坏免疫稳态。目前的抗炎策略往往损害病原体清除和加剧免疫抑制。精确靶向过度活化的巨噬细胞,同时保持抗菌功能是一种很有前途的治疗方法。通过高通量筛选390激酶抑制剂在高活化巨噬细胞中,我们发现polo样激酶1 (PLK1)抑制剂GSK461364是一个有效的高活化调节剂。然而,其临床转化受到剂量依赖性细胞毒性和全身毒性的限制。为了解决这个问题,我们设计了甘露糖功能化纳米颗粒(Nano-PLK1in),用于靶向组合递送抑制剂和谷胱甘肽至过度活跃的巨噬细胞。这些纳米颗粒显著提高了小鼠和人类过度活化的巨噬细胞的细胞摄取,大约是原来的2倍。三作用纳米PLK1平台能够:(i)通过PLK1阻断精确抑制caspase-11途径,(ii)通过谷胱甘肽介导的线粒体保护重新激活氧化还原稳态,以及(iii)在不广泛免疫抑制的情况下保持抗菌能力。在小鼠脓毒症模型中,与游离药物相比,Nano-PLK1in显着提高了50%的生存率,同时凝血功能降低41.8%,ALT/肌酐水平降低28.9-54.3%,反映了多器官保护,并增强了细菌清除率。通过将精确的巨噬细胞重编程与有效的病原体根除相结合,我们的纳米级工程策略超越了传统疗法的疗效-毒性权衡,突出了其在败血症治疗中的转化前景。
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引用次数: 0
Fourier Plane Tomographic Spectroscopy Reveals Orientation-Dependent Multipolar Plasmon Modes in Micrometer-Scale Janus Particles. 傅里叶平面层析光谱揭示了微米尺度Janus粒子中取向相关的多极等离子体模式。
IF 16 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-23 DOI: 10.1021/acsnano.6c01771
Felix H Patzschke, Frank Cichos

Precise control of light-matter interactions is a cornerstone of next-generation technologies, from ultrasensitive biosensing and single-molecule tracking to the development of adaptive metamaterials. While small, symmetric nanostructures are well-understood, micrometer-scale plasmonic Janus particles (pJPs), comprising dielectric cores with thin metallic caps, exhibit complex optical properties due to their asymmetric structure. Despite widespread applications in active matter research, their orientation-dependent scattering properties remain largely unexplored. We introduce Fourier plane tomographic spectroscopy for simultaneous four-dimensional characterization of scattering from individual micrometer-scale particles across wavelength, incident angle, and scattering angle. Combining measurements with finite-element simulations, we identify discrete spectral markers in visible and near-infrared regions that evolve predictably with cap orientation. Spherical-harmonics decomposition reveals that these markers arise from three distinct multipolar modes up to fifth order: axial-propagating transverse-electric, transverse-propagating transverse-electric, and transverse-propagating axial-electric, with retardation-induced splitting. We observe progressive red-shifts and line width narrowing of higher-order resonances, demonstrating curvature's influence on mode dispersion. Orientation-specific scattering patterns exhibit polarization-dependent features enabling optical tracking of particle rotation. Beyond pJPs, this methodology establishes a general framework for characterizing asymmetric nanostructures of diverse material combinations and geometries, offering a toolkit for designing orientation-responsive nanoantennas, reconfigurable metasurfaces, active colloidal systems with tailored light-matter interactions, and high-precision optical tracking of particle rotation.

光-物质相互作用的精确控制是下一代技术的基石,从超灵敏生物传感和单分子跟踪到自适应超材料的开发。虽然人们已经很好地理解了小而对称的纳米结构,但微米尺度的等离子体Janus粒子(pJPs),由带有薄金属帽的电介质芯组成,由于其不对称结构而表现出复杂的光学特性。尽管在活性物质研究中得到了广泛的应用,但它们的定向散射特性仍未得到充分的研究。我们引入傅里叶平面层析光谱来同时表征单个微米尺度粒子在波长、入射角和散射角上的四维散射。结合测量和有限元模拟,我们确定了可见光和近红外区域的离散光谱标记,这些标记可预测地随帽的方向演变。球谐波分解表明,这些标记来自三种不同的多极模式,最高可达五阶:轴向传播横向电、横向传播横向电和横向传播轴向电,并伴有延迟诱导分裂。我们观察到高阶共振的渐进红移和线宽变窄,证明了曲率对模色散的影响。定向散射模式表现出与偏振相关的特征,能够光学跟踪粒子旋转。除了pJPs,该方法还为表征不同材料组合和几何形状的不对称纳米结构建立了一个总体框架,为设计定向响应纳米天线、可重构超表面、具有定制光物质相互作用的活性胶体系统以及粒子旋转的高精度光学跟踪提供了一个工具包。
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引用次数: 0
Engineered Magnetobacterial Microrobots with Tunable Self-Mineralization for Precise Imaging-Guided Photothermal Therapy. 具有可调自矿化的工程磁细菌微机器人用于精确成像引导光热治疗。
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-23 DOI: 10.1021/acsnano.5c19758
Hui Ran,Lishan Zhang,Yicheng Ye,Ning Zhong,Yuanyuan Wang,Bingquan Huang,Yuejun Jiang,Xue Yang,Qiuyun Wei,Hao Tian,Fei Peng,Yingfeng Tu
Micro/nanomotors hold promise for remote manipulation in complex biological environments. However, integrating robust barrier penetration, real-time tracking, and effective theranostics within a motor system remains a formidable translational challenge. Here, we engineer sequential magneto-actuated and optically imageable biohybrid micromotors (BAMs) for precise tumor therapy. BAMs consist of two components, magnetospirillum bacteria (AMB-1), enabling autonomous tumor tropism via hypoxia-driven chemotaxis and magnetic navigation under external fields, and extracellularly biomineralized Ag2S quantum dots, serving as near-infrared (NIR)-II fluorescence imaging agents and photothermal converters. In vivo studies demonstrate that BAMs can migrate to the hypoxic core of the tumors through the synergistic effect of hypoxia-targeting chemotaxis and magnetic actuation, which can be monitored via NIR-II fluorescence imaging. Moreover, as a photothermal therapeutic agent, BAMs effectively induce tumor cell apoptosis and suppress tumor growth through photothermal conversion. This innovative BAMs platform not only overcomes passive diffusion but also provides precise theranostics through integrated magnetic guidance, NIR-II imaging, and photothermal therapy, showcasing the promise of biohybrid systems.
微/纳米马达有望在复杂的生物环境中进行远程操作。然而,在运动系统中整合强大的屏障穿透、实时跟踪和有效的治疗仍然是一个巨大的挑战。在这里,我们设计了顺序磁驱动和光学成像的生物混合微电机(BAMs),用于精确的肿瘤治疗。BAMs由两部分组成,一是磁螺旋藻细菌(AMB-1),它通过缺氧驱动的趋化和磁场导航在外场下实现肿瘤的自主向性;二是细胞外生物矿化Ag2S量子点,作为近红外(NIR)-II荧光显像剂和光热转换器。体内研究表明,BAMs可以通过低氧靶向趋化和磁致动的协同作用迁移到肿瘤的缺氧核心,这可以通过NIR-II荧光成像进行监测。此外,BAMs作为光热治疗剂,通过光热转化有效诱导肿瘤细胞凋亡,抑制肿瘤生长。这种创新的BAMs平台不仅克服了被动扩散,而且通过集成磁引导,NIR-II成像和光热治疗提供精确的治疗,展示了生物混合系统的前景。
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引用次数: 0
Overcoming Passivation-Corrosion Dilemma of Al Current Collector for Aqueous Zn Battery. 克服锌水电池铝集流器钝化-腐蚀难题。
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-23 DOI: 10.1021/acsnano.6c02382
Zixiang Meng,Yuhan Zou,Jiashu Chen,Yongbiao Mu,Yan Li,Yuyuan Wang,Qian Liu,Yuyang Yi,Lin Zeng,Guangping Zheng,Shixue Dou,Jingyu Sun
Al current collectors are widely adopted in nonaqueous batteries because of their low cost, high conductivity, and low density, yet their deployment in aqueous congeners (i.e., Zn-ion batteries) is largely precluded by concurrent issues of surface passivation and electrolyte-driven corrosion. Here, an on-site N-doped carbon-skinned Al current collector (NC@Al) is developed to resolve this longstanding dilemma. Enabled by an ultrafast Joule heating process, elevated temperature carbonization could be completed in seconds without thermally deforming the Al substrate, which renders a dense and continuous double-sided NC overlayer, affording favorable interfacial adhesion. Combined theoretical calculations and experimental diagnostics verify the NC overlayer simultaneously helps suppress the Al passivation-corrosion issue and promote uniform Zn deposition. As a result, symmetric cells based on NC@Al exhibit durable cycling beyond 3500 h at 0.5 mA cm-2/0.25 mAh cm-2. When paired with an iodine cathode, our constructed pouch cells with an active material loading of 25 mg cm-2 sustain stable operation for 1000 cycles under a stringent N/P ratio of 1.77. Technoeconomic analysis further highlights the energy-efficiency advantage of our route in practical manufacturing. This work establishes a strategy for employing commercially available Al current collector materials toward aqueous batteries.
铝集流器由于其低成本、高导电性和低密度而被广泛应用于非水电池中,但由于表面钝化和电解质驱动的腐蚀问题,它们在水电池(即锌离子电池)中的应用在很大程度上被排除在外。在这里,一个现场n掺杂碳皮铝电流收集器(NC@Al)被开发来解决这个长期存在的难题。通过超快焦耳加热工艺,可以在几秒钟内完成高温碳化,而不会使Al衬底发生热变形,从而形成致密连续的双面NC覆层,提供良好的界面附着力。理论计算和实验诊断相结合,验证了NC覆盖层同时有助于抑制Al钝化腐蚀问题和促进均匀Zn沉积。因此,基于NC@Al的对称电池在0.5 mA cm-2/0.25 mAh cm-2下表现出超过3500小时的持久循环。当与碘阴极配对时,我们构建的活性材料负载为25 mg cm-2的袋状电池在严格的N/P比为1.77的条件下可稳定运行1000次。技术经济分析进一步强调了我们的路线在实际制造中的节能优势。这项工作建立了一种将市售铝集流材料用于水性电池的策略。
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引用次数: 0
Wavelength-Tailoring Copper Oxidation States for Tunable Photoelectrochemical Syngas Generation. 波长裁剪铜氧化态用于可调谐的光电化学合成气生成。
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-23 DOI: 10.1021/acsnano.5c21792
Yi-Cheng Wang,Yan Liu,Chenyu Xu,Peng-Fei Sui,Yi Liu,Renfei Feng,Xiaolei Wang,Jing-Li Luo
The photoelectrochemical CO2 reduction reaction (PEC CO2RR) to syngas is of great significance for meeting the needs of the green chemical industry, and controlling the CO/H2 ratio is an important issue. However, the reliance on thin-film semiconductor photocathodes significantly limits the available fabrication methods, and some of the proposed schemes have not been able to precisely tune the CO/H2 ratio by indirectly regulating the electronic structure of active sites. In order to overcome the limitations of traditional fabrication methods, this work proposes a simple photodeposition method for loading Cu2-xTe onto 1% S-doped ZnTe/ZnO to regulate the oxidation state of Cu between +1 and +2 by precisely controlling the deposition light wavelength from violet to red. With shorter deposition light wavelengths, the photon energy increases, leading to a reduced valence state of Cu. As the Cu oxidation state decreases, the band structure of Cu2-xTe-ZnTe can be modulated, with the overall d-band center shifting toward the Fermi level. Besides, the electron density around the Cu active sites increases due to the shorter Cu-Cu bond, resulting in stabilized reaction intermediates and a faster charge transfer process, leading to higher CO selectivity with suppressed hydrogen evolution reaction. As a result, Cu@S-ZnTe/ZnO shows a tunable CO/H2 molar ratio ranging from 0.45 to 1.70 by adjusting the oxidation state of Cu, which can be precisely controlled by simply varying the deposition light wavelength with a specific filter. This demonstrates the great potential of the proposed photodeposition method and the resulting photoelectrocatalyst for practical PEC CO2RR applications.
光电化学CO2还原反应(PEC CO2RR)制合成气对于满足绿色化工的需要具有重要意义,而CO/H2比的控制是其中的一个重要问题。然而,对薄膜半导体光电阴极的依赖极大地限制了可用的制造方法,并且一些提出的方案无法通过间接调节活性位点的电子结构来精确调节CO/H2比。为了克服传统制备方法的局限性,本工作提出了一种简单的光沉积方法,将Cu2-xTe加载到1% s掺杂的ZnTe/ZnO上,通过精确控制沉积光波长从紫到红来调节Cu在+1和+2之间的氧化状态。随着沉积光波长的缩短,光子能量增加,导致Cu的价态降低。随着Cu氧化态的降低,Cu2-xTe-ZnTe的能带结构可以被调制,整个d带中心向费米能级移动。此外,Cu-Cu键的缩短增加了Cu活性位点周围的电子密度,使得反应中间体稳定,电荷转移过程加快,CO选择性提高,析氢反应受到抑制。通过调节Cu的氧化态,Cu@S-ZnTe/ZnO的CO/H2摩尔比可在0.45 ~ 1.70范围内进行调节,而这可以通过改变特定滤光片的沉积光波长来精确控制。这证明了所提出的光沉积方法和由此产生的光电催化剂在实际PEC CO2RR应用中的巨大潜力。
{"title":"Wavelength-Tailoring Copper Oxidation States for Tunable Photoelectrochemical Syngas Generation.","authors":"Yi-Cheng Wang,Yan Liu,Chenyu Xu,Peng-Fei Sui,Yi Liu,Renfei Feng,Xiaolei Wang,Jing-Li Luo","doi":"10.1021/acsnano.5c21792","DOIUrl":"https://doi.org/10.1021/acsnano.5c21792","url":null,"abstract":"The photoelectrochemical CO2 reduction reaction (PEC CO2RR) to syngas is of great significance for meeting the needs of the green chemical industry, and controlling the CO/H2 ratio is an important issue. However, the reliance on thin-film semiconductor photocathodes significantly limits the available fabrication methods, and some of the proposed schemes have not been able to precisely tune the CO/H2 ratio by indirectly regulating the electronic structure of active sites. In order to overcome the limitations of traditional fabrication methods, this work proposes a simple photodeposition method for loading Cu2-xTe onto 1% S-doped ZnTe/ZnO to regulate the oxidation state of Cu between +1 and +2 by precisely controlling the deposition light wavelength from violet to red. With shorter deposition light wavelengths, the photon energy increases, leading to a reduced valence state of Cu. As the Cu oxidation state decreases, the band structure of Cu2-xTe-ZnTe can be modulated, with the overall d-band center shifting toward the Fermi level. Besides, the electron density around the Cu active sites increases due to the shorter Cu-Cu bond, resulting in stabilized reaction intermediates and a faster charge transfer process, leading to higher CO selectivity with suppressed hydrogen evolution reaction. As a result, Cu@S-ZnTe/ZnO shows a tunable CO/H2 molar ratio ranging from 0.45 to 1.70 by adjusting the oxidation state of Cu, which can be precisely controlled by simply varying the deposition light wavelength with a specific filter. This demonstrates the great potential of the proposed photodeposition method and the resulting photoelectrocatalyst for practical PEC CO2RR applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"15 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147495101","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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