Materials Today Nano最新文献_第2页

Manipulation of nitrogen doping levels in SiC nanowires and their negatively correlated microwave absorption properties SiC纳米线中氮掺杂水平的控制及其负相关微波吸收性能

IF 8.2 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today Nano

Pub Date : 2026-01-29 DOI: 10.1016/j.mtnano.2026.100770

Jingwen Deng , Huimin Liu , Qing'an Cui , Bing Liu , Liyuan Han , Jie Pu , Hejun Li , Xuemin Yin

Silicon carbide nanowires (SiCnws) are promising microwave absorbers, yet their performance is limited by a low dielectric constant and a lack of magnetic loss. While doping offers a potential solution, controlling doping levels in SiCnws remains challenging, and its effect on absorption performance is unclear. In this study, we developed a simple chemical vapor deposition (CVD) method to prepare nitrogen-doped SiCnws with tunable nitrogen content on carbon fiber cloth. By adjusting the nitrogen amount, the microstructure and electromagnetic parameters of SiCnws could be regulated, and their effect on the electromagnetic wave absorption ability was further investigated. Surprisingly, the absorption capacity of SiCnws decreased with increasing nitrogen content. Compared to nitrogen-doped SiCnws, undoped SiCnws exhibited the best absorption performance, achieving an effective absorption bandwidth of 4.17 GHz (13.83–18 GHz, 1.30 mm thickness) and a minimum reflection loss of −37.15 dB (1.40 mm thickness). This unexpected trend is attributed to the imbalance between dielectric constant and magnetic permeability caused by small atom doping. This study not only provides a simple method for regulating the nitrogen doping levels in SiCnws but also offers insights for the development of SiCnws-based microwave absorbers.

碳化硅纳米线（SiCnws）是一种很有前途的微波吸收材料，但其性能受到介电常数低和缺乏磁损耗的限制。虽然掺杂提供了一个潜在的解决方案，但控制SiCnws中的掺杂水平仍然具有挑战性，并且其对吸收性能的影响尚不清楚。在这项研究中，我们开发了一种简单的化学气相沉积（CVD）方法，在碳纤维布上制备氮掺杂的SiCnws，其氮含量可调。通过调节氮量，可以调节SiCnws的微观结构和电磁参数，并进一步研究其对电磁波吸收能力的影响。令人惊讶的是，SiCnws的吸收能力随着氮含量的增加而下降。与氮掺杂的SiCnws相比，未掺杂的SiCnws表现出最好的吸收性能，有效吸收带宽为4.17 GHz （13.83-18 GHz， 1.30 mm厚度），最小反射损耗为−37.15 dB （1.40 mm厚度）。这种意想不到的趋势是由于小原子掺杂导致介电常数和磁导率之间的不平衡。该研究不仅为调控SiCnws中氮掺杂水平提供了一种简单的方法，而且为SiCnws基微波吸收剂的开发提供了新的思路。

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引用次数: 0

Smart light-triggered thermo-responsive superwetting CoZn-ZIF decorated PVDF/PNIPAM@GO nanofiber membranes for switchable oil-water emulsion separation 智能光触发热响应超湿CoZn-ZIF修饰PVDF/PNIPAM@GO纳米纤维膜，可切换油水乳液分离

IF 8.2 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today Nano

Pub Date : 2026-01-29 DOI: 10.1016/j.mtnano.2026.100767

Le Yin , Mu Hu , Yajie Liu , Yang You , Yuan Wang , Shaojun Yuan

Efficient separation of oil–water emulsion remains a persistent challenge in wastewater treatment, as conventional membranes often suffer from fouling, poor recyclability, and lack of dynamic control. Here, we report a light-triggered thermo-responsive superwetting nanofiber membrane (PPZ@GO) that combines electrospun PNIPAM/PVDF nanofibers with graphene oxide (GO) and in situ grown bimetallic CoZn–ZIF frameworks. In this hybrid design, PVDF provides mechanical robustness, PNIPAM enables reversible thermo-responsive wettability, GO facilitates rapid photothermal heating, and CoZn–ZIF imparts hierarchical roughness and enhanced interfacial functionality. The optimized [email protected] % membrane exhibits rapid photothermal heating to 48.6 °C within 20 s under simulated solar light, enabling reversible wettability switching between underwater superoleophobicity (light off, below LCST) and under-oil superhydrophobicity (light on, above LCST). This dual-mode response allows on-demand separation of both oil-in-water and water-in-oil emulsions, achieving fluxes above 2000 L m⁻² h⁻¹ and 1000 L m⁻² h⁻¹, respectively, with separation efficiencies exceeding 99 %. The membrane further demonstrates excellent antifouling resistance, mechanical durability, and stable performance across repeated cycles. By integrating photothermal conversion with thermo-responsive switching in a nanofibrous MOF–polymer scaffold, this work provides a versatile strategy for designing smart, energy-efficient membranes, offering broad potential for next-generation oily wastewater remediation and advanced separation technologies.

由于常规膜存在污染、可回收性差、缺乏动态控制等问题，油水乳化液的高效分离一直是污水处理领域面临的挑战。在这里，我们报道了一种光触发热响应超湿纳米纤维膜（PPZ@GO），它将静电纺PNIPAM/PVDF纳米纤维与氧化石墨烯（GO）和原位生长的双金属CoZn-ZIF框架结合在一起。在这种混合设计中，PVDF提供了机械稳健性，PNIPAM提供了可逆的热响应润湿性，GO促进了快速光热加热，而CoZn-ZIF赋予了分层粗糙度和增强的界面功能。优化后的[email protected] %膜在模拟太阳光照下，在20秒内快速光热加热到48.6°C，实现了水下超疏油性（不亮，低于LCST）和油下超疏水性（亮，高于LCST）之间的可逆润湿性切换。这种双模式响应允许按需分离水包油和油包水乳剂，分别实现超过2000 L m−2 h−1和1000 L m−2 h−1的通量，分离效率超过99%。该膜进一步表现出优异的防污性能、机械耐久性和在重复循环中的稳定性能。通过在纳米纤维mof聚合物支架中集成光热转换和热响应开关，这项工作为设计智能、节能膜提供了一种通用策略，为下一代含油废水修复和先进分离技术提供了广阔的潜力。

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引用次数: 0

Fabrication of advanced triboelectric nanogenerators based on freestanding few-layer β-rhombohedral borophene sheets for posture recognition 基于独立少层β-菱形硼罗芬片的先进摩擦电纳米发电机的制造及其姿态识别

IF 8.2 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today Nano

Pub Date : 2026-01-29 DOI: 10.1016/j.mtnano.2026.100769

Fengbo Liao , Yishan Wang , Haojian Lin , Yuehan Liu , Qi An , Jun Wang , Qingyun He , Fengfei Wang , Kai Dong , Ye Li , Fei Liu

The attention state recognition of personnel working in confined environments is very crucial for enhancing the safety of wearable devices. However, there is still a lack of compact and easily integrable posture recognition system to assist in such assessments. In this work, we construct a novel posture acquisition system based on the triboelectric nanogenerator (B@TENG), in which few-layer β-rhombohedral (β-rh.) borophene/Polydimethylsiloxane (B/PDMS) nanocomposite film is used as the enhanced triboelectric layer. In experiments, the output voltage and current of the B/PDMS-based TENG (B@TENG) are significantly improved to be 3.8 and 2.5 times higher than bare PDMS-based TENG with an ultralow borophene content of only 0.4 wt%, surpassing those of many other TENGs with a high-content of other 2D materials. First-principle calculation is used to analyze the improvement mechanism of B@TENG. The simulations show that the enhanced mechanism should be attributed to the differential quantum capacitance effect of few-layer borophene sheets, which can effectively increase the dielectric constant and surface charge density of PDMS-based TENG devices. To accurately achieve the recognition of sitting posture, a device arrays of eight B@TENGs equipped with our self-developed chip are integrated to create a compact sitting-posture acquisition system. Using the CNN-LSTM model, the transition among different sitting postures can be efficiently recognized with an average accuracy over 95 %. Moreover, the B@TENG recognition system can accurately differentiate different posture transition frequencies, which may provide an effective approach for various applications in multimodal attention monitoring systems.

密闭环境中工作人员的注意力状态识别对于提高可穿戴设备的安全性至关重要。然而，目前仍缺乏紧凑且易于集成的姿态识别系统来辅助此类评估。在这项工作中，我们构建了一种基于摩擦电纳米发电机的新型姿态采集系统（B@TENG），该系统使用少层β-菱形（β-rh.）硼苯/聚二甲基硅氧烷（B/PDMS）纳米复合薄膜作为增强摩擦电层。在实验中，B/PDMS-based TENG （B@TENG）的输出电压和电流明显提高，比裸PDMS-based TENG高3.8倍和2.5倍，硼烯含量仅为0.4 wt%，超过了许多其他2D材料含量高的TENG。采用第一性原理计算分析了B@TENG的改进机理。仿真结果表明，这种增强机制应归因于少层硼罗芬片的差分量子电容效应，它可以有效地提高基于pdm的TENG器件的介电常数和表面电荷密度。为了准确地实现坐姿的识别，我们集成了一个8个设备阵列B@TENGs，配备了我们自主研发的芯片，形成了一个紧凑的坐姿采集系统。使用CNN-LSTM模型可以有效识别不同坐姿之间的转换，平均准确率在95%以上。此外，B@TENG识别系统可以准确区分不同的姿势转换频率，为多模态注意力监测系统的各种应用提供了有效的方法。

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引用次数: 0

Recent advances in microstructure engineering for flexible capacitive pressure sensors 柔性电容压力传感器微结构工程研究进展

IF 8.2 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today Nano

Pub Date : 2026-01-27 DOI: 10.1016/j.mtnano.2026.100764

Taiding Xu , Ling Chen , Junhui Ding , Linxian Chen , Ke Zhao , Miao Qi , Lei Xu , Jingxia Qiu , Jun Dong , Sheng Li

Flexible pressure sensors (FPSs) can accurately convert mechanical signals into electrical signals, garnering significant attention for their use in mimicking human skin sensation. Flexible capacitive pressure sensors (FCPSs) are favored among various pressure sensors due to their simple device structure, low power consumption, and high stability. These attributes cause FCPSs to be widely used in wearable devices and machine tactile sensing applications. To better satisfy these demands, it is important to improve the performance of FCPSs in terms of sensitivity, linearity, working range, stability, response time, and recovery time. In recent years, significant efforts have been dedicated to improving sensing performance through the integration of distinctive microstructures within the dielectric and electrode layers. This review introduces the working mechanisms and fabrication strategies of various microstructure configurations in FCPSs. These microstructures are classified into two categories: homogeneous microstructures and non-uniform microstructures. Typical examples include micropyramids, micropillars/microcones, microhemispheres, hybrid/hierarchical structures, sandpaper-based structures, natural plant-derived microstructures, porous structures, and fiber-network structures. The influence of microstructural design on sensor performance is systematically analyzed. Furthermore, potential future developments and key challenges in the advancement of FCPSs are discussed.

柔性压力传感器（FPSs）可以准确地将机械信号转换为电信号，因其在模拟人类皮肤感觉方面的应用而备受关注。柔性电容式压力传感器（fcps）由于其器件结构简单、功耗低、稳定性高等特点，在各种压力传感器中备受青睐。这些特性使得fcps广泛应用于可穿戴设备和机器触觉传感应用。为了更好地满足这些需求，提高fcps在灵敏度、线性度、工作范围、稳定性、响应时间和恢复时间方面的性能是很重要的。近年来，通过在介电层和电极层中集成独特的微结构来提高传感性能已经付出了巨大的努力。本文综述了fcps中各种结构的工作机理和制作策略。这些微观结构可分为两类：均匀微观结构和非均匀微观结构。典型的例子包括微金字塔、微柱/微锥、微半球、混合/分层结构、基于砂纸的结构、天然植物衍生的微观结构、多孔结构和纤维网络结构。系统分析了微结构设计对传感器性能的影响。此外，还讨论了fcps的潜在未来发展和主要挑战。

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引用次数: 0

Study on multi-physical coupling characteristics of ordered porous tungsten oxide films based on oxygen vacancy regulation 基于氧空位调控的有序多孔氧化钨膜多物理耦合特性研究

IF 8.2 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today Nano

Pub Date : 2026-01-25 DOI: 10.1016/j.mtnano.2026.100766

Lingna Jia, Panzhe Hou, Tianen Liu, Aiqi Zhang, Peipei Lu, Lihu Liu, Junmeng Zhang, Huiyuan Sun

A well-ordered WO₃ nanoporous array structure was successfully fabricated on anodized aluminum oxide using direct-current magnetron sputtering technology. The experiment revealed that the sample exhibited significant room-temperature ferromagnetism, resistive switching behavior, and ferroelectricity. Moreover, a strong coupling effect was observed between their ferromagnetism and the electrical properties. Through annealing treatments under various atmospheres, combined with photoluminescence spectroscopy, X-ray photoelectron spectroscopy, and Kelvin probe force microscopy analyses, it was demonstrated that the evolution of these observed properties is closely related to the oxygen vacancies that captured single electrons. These findings provide experimental evidence for the application of wide-bandgap metal oxides in novel multi-physical memory devices, intelligent equipment, and spintronics systems.

采用直流磁控溅射技术，在阳极氧化铝表面成功制备了有序的WO3纳米孔阵列。实验表明，该样品具有明显的室温铁磁性、电阻开关性能和铁电性。此外，它们的铁磁性和电学性质之间存在很强的耦合效应。通过不同气氛下的退火处理，结合光致发光光谱、x射线光电子能谱和开尔文探针力显微镜分析，证明了这些观察到的性能的演变与捕获单电子的氧空位密切相关。这些发现为宽带隙金属氧化物在新型多物理存储器件、智能设备和自旋电子学系统中的应用提供了实验依据。

引用次数: 0

Elucidation dynamics of ZnO and ZrO2 in catalytic CO2 Hydrogenation: An in-situ TEM study 催化CO2加氢过程中ZnO和ZrO2的解析动力学：原位TEM研究

IF 8.2 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today Nano

Pub Date : 2026-01-24 DOI: 10.1016/j.mtnano.2026.100765

Lizhuo Wang , Yasuhiro Sakamoto , Ang Li , Xin Fang , Yuhan Men , Penny Xiao , Paul A. Webley , Xiaodong Han , Jun Huang

Cu/ZnO/ZrO₂ (CZZ) catalysts are widely used in CO₂ hydrogenation to methanol. However, their structural dynamics under reaction conditions and related reaction mechanism remain unclear. In this study, we employed in-situ transmission electron microscopy (TEM) to investigate structural changes in Cu/ZnO/ZrO₂ catalysts under CO₂ and H₂/CO₂ environments at 200 °C and 250 °C. Under CO₂ conditions, coexisting CuO and ZnO phases were observed along with a diminishing crystalline ZrO₂ phase. Under H₂/CO₂ conditions, dynamic formation and evolution of a CuZn alloy phase occurred, accompanied by the reappearance of crystalline ZrO₂ nanoparticles. It is also noted that copper in Cu/ZnO/ZrO₂ is difficult to be completely reduced in a H₂/CO₂ environment, in contrast to un-supported CuO nanoparticles. These results suggest a distinct function of ZrO₂ and ZnO support in the catalyst, which alters the catalytic performance of the CZZ system. The findings of this study provide new insight into the dynamic behavior of CZZ catalysts under actual reaction conditions.

Cu/ZnO/ZrO2 （CZZ）催化剂广泛应用于CO2加氢制甲醇。然而，它们在反应条件下的结构动力学和相关的反应机理尚不清楚。本研究采用原位透射电镜（TEM）研究了Cu/ZnO/ZrO2催化剂在200°C和250°C的CO2和H2/CO2环境下的结构变化。在CO2条件下，CuO相和ZnO相共存，ZrO2相逐渐减少。在H2/CO2条件下，CuZn合金相的动态形成和演化伴随着ZrO2纳米颗粒结晶的重现。研究还发现，Cu/ZnO/ZrO2中的铜在H2/CO2环境中很难被完全还原，而非CuO纳米颗粒。这些结果表明ZrO2和ZnO载体在催化剂中具有明显的作用，从而改变了CZZ体系的催化性能。本研究结果对实际反应条件下CZZ催化剂的动力学行为提供了新的认识。

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引用次数: 0

Hydrothermal growth dynamics of TiO2 nanorods on p-Si: Linking reaction time to structural evolution and optoelectronic device performance p-Si上TiO2纳米棒的水热生长动力学：反应时间与结构演变和光电子器件性能的联系

IF 8.2 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today Nano

Pub Date : 2026-01-23 DOI: 10.1016/j.mtnano.2026.100759

Selcuk Izmirli , Sukru Cavdar

In this study, the structural, morphological, and electrical properties of TiO₂ nanorod (TNR)-based heterojunction devices synthesized on p-Si substrates using the hydrothermal method for different durations were comprehensively investigated. During the production process, reaction kinetics and growth dynamics were also evaluated; ion transport and crystal growth activities were discussed in detail, starting from the nucleation stage. SEM images showed that the lengths of TNR structures produced with hydrothermal reaction times of 1, 2, 3, and 4 h increased from 355 nm to 1.78 μm, while their diameters increased from 30–40 nm to 280–300 nm. XRD analyses revealed that the dominant phase in all samples was rutile TiO₂, and that the growth dynamics occurred in the (101) plane, while growth in the (002) and (110) planes supported the formation of the crystal structure. In the I-V characterization of heterojunction devices produced with TNRs of different thicknesses, devices with thin TNR interfaces stood out with their strong rectification behavior, low ideality factors, and strong photodiode performance. However, with the growth of TNR structures, the diode character was lost. In the photodetector performance metrics of the devices, devices with thin TNR interfaces also exhibited higher photoresponsivity (R_ph) and photosensitivity (S_ph) behavior. Furthermore, these devices offered high detectivity (D∗) even at low light intensities. The results obtained confirm that the hydrothermal production parameters optimized in this study are crucial for TNR morphology.

在本研究中，采用水热法在p-Si衬底上合成了基于TiO2纳米棒（TNR）的异质结器件，并对其结构、形态和电性能进行了全面研究。在生产过程中，对反应动力学和生长动力学进行了评价；从成核阶段开始，详细讨论了离子输运和晶体生长活性。SEM图像显示，经过1、2、3和4 h的水热反应，得到的TNR结构的长度从355 nm增加到1.78 μm，直径从30 ~ 40 nm增加到280 ~ 300 nm。XRD分析表明，所有样品的优势相均为金红石型TiO2，生长动力学发生在（101）平面，而（002）和（110）平面的生长支持晶体结构的形成。在用不同厚度的TNR制作的异质结器件的I-V表征中，具有薄TNR接口的器件以其强整流行为、低理想因数和强光电二极管性能而脱颖而出。然而，随着TNR结构的增长，二极管特性逐渐丧失。在器件的光电探测器性能指标中，具有薄TNR接口的器件也表现出更高的光响应性（Rph）和光敏性（Sph）行为。此外，这些装置即使在低光强下也能提供高探测性（D *）。研究结果证实了本研究优化的热液生产参数对TNR形貌的影响至关重要。

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引用次数: 0

2-Dimensional black phosphorus nanostructures for biomedical applications 生物医学应用的二维黑磷纳米结构

IF 8.2 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today Nano

Pub Date : 2026-01-20 DOI: 10.1016/j.mtnano.2026.100763

Govinakere M. Dhanush , Chitradurga K. Praveen Kumar , K. Pramoda , Hamse Kameshwar Vivek , Yarabahally R. Girish

Two-dimensional black phosphorus (2D-BP), a puckered layered phosphorus nanomaterial, is a promising candidate for various biomedical applications due to its unique physicochemical properties, including good biocompatibility, tunable band gap, high carrier mobility, large surface-to-volume ratio, and excellent biodegradability. BP is a promising candidate for various biomedical applications. Recent research on biomedical fields emphasizes its viable in mitigating bacterial infections, good biocompatibility and promoting wound healing, which are critical challenges in modern medicine, especially in chronic and infected wounds. This review focuses on the latest development of black phosphorus for potential use in Tumor treatment, bioimaging, antibacterial, drug delivery and wound healing applications which we are discussed here. In addition to this we also examine ongoing progress of BP-incorporated composites and targeted delivery systems, and overcome the dominant existing challenges like material stability, cytotoxicity, and scalability. The review concludes with insights into future directions and potential clinical translation.

二维黑磷（2D-BP）是一种皱褶状层状磷纳米材料，具有良好的生物相容性、可调节的带隙、高载流子迁移率、大的表面体积比和优异的生物降解性等独特的物理化学性质，在生物医学领域具有广阔的应用前景。BP是一种很有前途的生物医学应用候选者。近年来生物医学领域的研究强调其在减轻细菌感染、良好的生物相容性和促进伤口愈合方面的可行性，这是现代医学，特别是慢性和感染伤口的关键挑战。本文就黑磷在肿瘤治疗、生物成像、抗菌、给药和伤口愈合等方面的最新研究进展作一综述。除此之外，我们还研究了bp复合材料和靶向递送系统的持续进展，并克服了材料稳定性、细胞毒性和可扩展性等主要挑战。综述总结了对未来发展方向和潜在临床翻译的见解。

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引用次数: 0

Development strategies for sorafenib-based targeted radiotheranostic biomaterials: From targeted delivery to multimodal monitoring 基于索拉非尼的靶向放射治疗生物材料的发展策略：从靶向递送到多模式监测

IF 8.2 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today Nano

Pub Date : 2026-01-18 DOI: 10.1016/j.mtnano.2026.100762

Zijing Li , Luqi Song , Zheyi Shi , Yi Feng , Ran Zhu , Wei Chen , Jiaming Xie

Hepatocellular carcinoma (HCC) is one of the significant threats to human health worldwide, and its conventional treatments have obvious limitations. With the development of nanomedicine, the strategy of integrating multiple therapeutic approaches into a single nanoplatform is expected to lead to more efficient treatment of tumors. This study utilizes the nanomaterial PCN-224 as a carrier, labels it with ¹⁷⁷Lu, and modifies its surface with sorafenib (SOR) to construct an integrated diagnostic and therapeutic nanoplatform. The surface modification of SOR not only functions as targeted therapy (TT), but also enhances the active targeting of the nanoparticles and their accumulation at the tumor site. This in vivo distribution could be monitored by dual-modality imaging using fluorescence imaging and SPECT/CT imaging. The long retention allows ¹⁷⁷Lu-mediated radioisotope therapy (RIT) to continue working inside the tumor, thereby improving the limitations of photodynamic therapy (PDT), where the depth of light penetration is limited. Additionally, all three therapeutic modalities can act as inducers of immunogenic cell death (ICD), thereby further enhancing the therapeutic effects by activating the immune response. In conclusion, this work designs a combined triple therapy of PDT-RIT-TT to treat HCC through the direct killing effect and the indirect effect of ICD, utilizing multiple synergistic effects to improve the shortcomings of single therapy, and shows promising prospects for clinical application.

肝细胞癌（HCC）是全球范围内威胁人类健康的重要疾病之一，其常规治疗方法存在明显局限性。随着纳米医学的发展，将多种治疗方法整合到单一纳米平台的策略有望带来更有效的肿瘤治疗。本研究以纳米材料PCN-224为载体，用177Lu对其进行标记，并用sorafenib （SOR）修饰其表面，构建了一个集成诊断和治疗的纳米平台。SOR的表面修饰不仅具有靶向治疗（TT）的功能，而且增强了纳米颗粒的活性靶向及其在肿瘤部位的蓄积。这种体内分布可以通过荧光成像和SPECT/CT成像的双模成像来监测。长时间的滞留使177lu介导的放射性同位素治疗（RIT）能够在肿瘤内继续工作，从而改善光动力治疗（PDT）的局限性，其中光穿透深度有限。此外，所有三种治疗方式都可以作为免疫原性细胞死亡（ICD）的诱导剂，从而通过激活免疫反应进一步增强治疗效果。综上所述，本工作设计了PDT-RIT-TT三联疗法，通过ICD的直接杀伤作用和间接作用治疗HCC，利用多重协同作用改善单一治疗的不足，具有良好的临床应用前景。

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引用次数: 0

Atomistic insights into the hydrogen poisoning effect in ammonia synthesis over Ru surfaces from dynamic first-principles microkinetic modeling 从动力学第一性原理微动力学模型对Ru表面氨合成中氢中毒效应的原子见解

IF 8.2 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today Nano

Pub Date : 2026-01-17 DOI: 10.1016/j.mtnano.2026.100761

Lu Wang, Bo Yang

Hydrogen poisoning strongly suppresses the activity of Ru-based catalysts for ammonia synthesis, yet its atomistic origin remains unclear. In this study, we systematically investigate the influence of hydrogen coverage on the dynamic kinetics and mechanism of ammonia synthesis across three representative ruthenium, Ru(0001), Ru(10

\overline{1}

1), and Ru-step surface. We find that under hydrogen-poisoning conditions, all investigated surfaces follow an associative reaction mechanism. A notable shift in the reaction pathway and degree of rate control is observed on both the Ru(0001) and Ru-step surfaces as a function of hydrogen coverage, revealing a coverage-dependent evolution of the rate-determining steps. Our results also demonstrate that the Ru-step surface consistently exhibits the highest intrinsic activity. Under hydrogen-rich conditions, this surface achieves a turnover frequency of 1.36 × 10⁻² s⁻¹ and a reaction order with respect to H₂ of −0.25 at 673 K and 1 MPa, in excellent agreement with experimental observations under identical conditions. This quantitative consistency underscores that the hydrogen-covered surface, rather than the clean surface, represents the true catalytic state under working conditions. These findings provide fundamental atomic-scale insights into the origin of hydrogen poisoning and establish a theoretical foundation for the rational design of next-generation Ru-based catalysts.

氢中毒强烈抑制了钌基合成氨催化剂的活性，但其原子起源尚不清楚。在本研究中，我们系统地研究了氢覆盖对三种具有代表性的钌，Ru(0001), Ru（10.1）和Ru-step表面的氨合成动力学和机理的影响。我们发现在氢中毒条件下，所有被研究的表面都遵循缔合反应机制。在Ru（0001）和Ru步表面上观察到反应路径和速率控制程度的显著变化，作为氢覆盖的函数，揭示了速率决定步骤的覆盖依赖演化。我们的结果还表明，Ru-step表面始终表现出最高的固有活性。在富氢条件下，在673 K和1 MPa下，该表面的周转率为1.36 × 10−2 s−1，对H2的反应阶数为−0.25，与相同条件下的实验结果非常吻合。这种定量的一致性强调了氢覆盖的表面，而不是干净的表面，代表了工作条件下的真实催化状态。这些发现为氢中毒的起源提供了基本的原子尺度的见解，并为下一代钌基催化剂的合理设计奠定了理论基础。

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引用次数: 0