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Nontoxic CuInS2/ZnS Colloidal Quantum Dots for White Light-Emitting Diodes 用于白光二极管的无毒CuInS2/ZnS胶体量子点
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-03 DOI: 10.1021/acsnano.5c12714
Xiangda Deng,Wenxin Yang,Tianmin Wu
CuInS2 quantum dots (CIS QDs), with tunable photoluminescence spanning from the visible to near-infrared (NIR) region, hold significant potential for consumer electronics and bioimaging due to their favorable photophysical properties and absence of toxic elements. However, their intrinsic lack of short-wavelength emission has hindered their use in white light-emitting applications. Herein, we report a facile synthesis of zinc–acetate–oleylamine (Zn–Ac–OAm) and oleylamine (OAm)-coencapsulated CIS/ZnS QDs that deliver full-spectrum sunlight-like emissions, characterized by a distinct 455 nm peak and an ultrabroad full width at half-maximum (fwhm) of 241 nm. The Zn–Ac–OAm emitter produces blue-green fluorescence, effectively compensating for the short-wavelength deficiency of the CIS/ZnS QDs. More importantly, strong interactions between Zn–Ac–OAm and CIS/ZnS QDs enable efficient energy transfer within coencapsulated structures. As a proof of concept, white light-emitting diodes (WLEDs) fabricated using these coencapsulated CIS/ZnS QDs exhibit excellent photophysical performance, achieving a high color rendering index (CRI) of 92.1 and external quantum efficiency (EQE) of 7.2%. This coencapsulation strategy, together with the elucidated photophysical mechanisms, provides viable pathways for extending the application of long-wavelength-emitting nanomaterials in next-generation lighting and display technologies.
CuInS2量子点(CIS QDs)具有从可见光到近红外(NIR)区域可调谐的光致发光,由于其良好的光物理特性和不含有毒元素,在消费电子和生物成像领域具有重要的潜力。然而,它们固有的短波长发射不足阻碍了它们在白光发射应用中的应用。在此,我们报道了一个简单的合成锌-乙酸酯-油胺(Zn-Ac-OAm)和油胺(OAm)-共封装CIS/ZnS量子点,提供全光谱类阳光发射,其特点是有一个明显的455nm峰和超宽的半峰宽(fwhm)为241nm。Zn-Ac-OAm发射体产生蓝绿色荧光,有效地补偿了CIS/ZnS量子点的短波长缺陷。更重要的是,Zn-Ac-OAm和CIS/ZnS量子点之间的强相互作用可以在共封装结构内实现有效的能量传递。作为概念验证,使用这些共封装CIS/ZnS量子点制造的白光发光二极管(wled)表现出优异的光物理性能,实现了92.1的高显色指数(CRI)和7.2%的外部量子效率(EQE)。这种共封装策略,连同阐明的光物理机制,为扩展长波发射纳米材料在下一代照明和显示技术中的应用提供了可行的途径。
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引用次数: 0
Enabling Ultrahigh-Power-Density LiMn0.6Fe0.4PO4 Cathodes via Kinetics Limitation Breakthrough and Jahn–Teller Distortion Mitigation 通过突破动力学限制和减小Jahn-Teller畸变实现超高功率密度LiMn0.6Fe0.4PO4阴极
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-02 DOI: 10.1021/acsnano.5c21496
Pengxu Wang, Haifeng Yu, Ling Chen, Yaoguo Fang, Qian Cheng, Hao Jiang, Chunzhong Li
Development of high-power LiMnxFe1-xPO4 (LMFP) cathodes is fundamentally challenged by the interplay between sluggish one-dimensional Li+ diffusion and severe Jahn–Teller distortion. Herein, we propose a synergistic substitution strategy to concurrently tackle these issues. Partial replacement of PO4 tetrahedra by planar BO3 groups creates three-dimensional interconnected Li-ion diffusion networks, while doping Nb5+ into transition-metal sites widens the diffusion channels. This tailored microstructure not only overcomes the intrinsic Li+ diffusion kinetics limitation but also dissipates the mechanical stress arising from high-rate operating conditions, suppressing the Jahn–Teller distortion in MnO6 octahedra by 36%. The optimized LMFP cathode delivers an ultrahigh reversible capacity of 126 mAh g–1 at 10C (about a 3.6-fold improvement over the pristine LMFP) and retains 80.2% of its initial capacity after 2000 cycles at 3C in pouch-type full cells. This work elucidates the critical link between Li+ diffusion kinetics and structural stability, providing an available paradigm for designing high-power, long-life Mn-based cathode materials.
高功率LiMnxFe1-xPO4 (LMFP)阴极的发展从根本上受到了一维Li+扩散缓慢和严重的Jahn-Teller畸变之间相互作用的挑战。在此,我们提出了一种协同替代策略来同时解决这些问题。平面BO3基团部分取代PO4四面体形成三维互联的锂离子扩散网络,而在过渡金属位点掺杂Nb5+则拓宽了扩散通道。这种定制的微观结构不仅克服了固有的Li+扩散动力学限制,而且还消除了高速率操作条件下产生的机械应力,将MnO6八面体的Jahn-Teller畸变抑制了36%。优化后的LMFP阴极在10C下提供了126 mAh g-1的超高可逆容量(比原始LMFP提高了约3.6倍),并且在袋型充满电池中,在3C下循环2000次后仍保持其初始容量的80.2%。这项工作阐明了Li+扩散动力学和结构稳定性之间的关键联系,为设计高功率、长寿命的锰基阴极材料提供了一个可用的范例。
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引用次数: 0
Unravel Electrolyte-Dependent Interphase Structures in Lithium-Sulfurized Polyacrylonitrile Batteries via Cryogenic Transmission Electron Microscopy 通过低温透射电子显微镜揭示锂硫化聚丙烯腈电池中电解质依赖的界面结构
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-02 DOI: 10.1021/acsnano.5c14570
Cheng Zhen, Xianbin Wei, Yuxuan Cui, Xinzhen Lu, Jiashu Chen, Menghao Li, Tingting Zhang, Shaobo Han, Xuming Yang, Meng Danny Gu
The emerging lithium–sulfur batteries using sulfurized polyacrylonitrile cathodes feature exceptional stability and good compatibility with various electrolytes. However, the study of correlating battery performance with electrolytes based on ultrafine interphase structures is nearly blank. This work compares the solid- and cathode-electrolyte interphases (SEI and CEI) formed in five representative electrolytes, from the perspective of ultrafine structures acquired via cryogenic transmission electron microscopy and electron energy loss spectroscopy. The premature battery failure in the baseline ester- and ether-based electrolytes is related to the thick and uneven interphase layers on both the anodes and cathodes, which reflects continuous electrolyte decomposition. The use of film-forming additives brings substantial improvement in cycle stability, which is attributed to an inorganic-rich interphase that blocks electrolyte permeation and further decomposition. However, it comes along with aggregated byproducts on both SEI and CEI. Better stability is delivered in a localized high-concentration electrolyte, which aligns with the compact SEI and CEI layers with condensed inorganic species. Based on our observations and reasoning, the formation of inorganic-rich interphase involves anions or additives, which could serve as a practical guideline for rational electrolyte designing.
采用硫化聚丙烯腈阴极的新型锂硫电池具有优异的稳定性和与各种电解质的良好相容性。然而,基于超细相间结构的电池性能与电解质之间关系的研究几乎是空白。本文从低温透射电镜和电子能量损失能谱获得的超细结构的角度,比较了五种代表性电解质中形成的固体和阴极电解质界面相(SEI和CEI)。在基线酯基和醚基电解质中,电池过早失效与阳极和阴极上厚且不均匀的间相层有关,这反映了电解质的持续分解。成膜添加剂的使用大大提高了循环稳定性,这是由于富含无机的界面相阻止了电解质的渗透和进一步分解。然而,它在SEI和CEI上都伴随着聚合的副产品。在局部高浓度电解质中提供更好的稳定性,这与紧凑的SEI和CEI层与凝聚的无机物质相一致。根据我们的观察和推理,富无机间相的形成涉及阴离子或添加剂,这可以为合理设计电解质提供实用的指导。
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引用次数: 0
Unveiling Spin Transition at Single-Particle Level in Levitating Spin Crossover Nanoparticles 揭示悬浮自旋交叉纳米粒子在单粒子水平的自旋跃迁
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-02 DOI: 10.1021/acsnano.5c18794
Elena Pinilla-Cienfuegos, Lucas Mascaró-Burguera, Ramón Torres-Cavanillas, J. Ignacio Echavarría, Alejandro Regueiro, Eugenio Coronado, Javier Hernandez-Rueda
The ability to control and understand phase transitions of individual nanoscale building blocks is key to advancing the next generation of low-power reconfigurable nanophotonic devices. To address this critical challenge, molecular nanoparticles (NPs) exhibiting spin crossover (SCO) phenomenon are trapped by coupling a quadrupole Paul trap to a multispectral polarization-resolved scattering microscope. This contact-free platform simultaneously confines, optically excites, and monitors the spin transition in Fe(II)–triazole NPs in a pressure-tunable environment, eliminating substrate artifacts. Thus, we demonstrate light-driven manipulation of the spin transition in levitating NPs, enabled by laser heating and free of substrate-induced effects. Using the robust spin bistability near room temperature of our SCO system, we quantify reversible optovolumetric changes of up to 10%, revealing precise switching thresholds at the single-particle level. Independent pressure modulation produces a comparable volume increase, confirming mechanical control over the same bistable transition. These results constitute full real-time control and readout of spin states in levitating SCO NPs, with operating conditions compatible with ultralow-power optical switching, data storage, and nanoscale sensing.
控制和理解单个纳米级构建块的相变的能力是推进下一代低功耗可重构纳米光子器件的关键。为了解决这一关键挑战,通过将四极保罗阱与多光谱偏振分辨散射显微镜耦合来捕获具有自旋交叉(SCO)现象的分子纳米粒子(NPs)。这种无接触平台在压力可调的环境中同时限制、光学激发和监测Fe(II) -三唑NPs中的自旋跃迁,消除了衬底伪像。因此,我们证明了悬浮NPs中自旋跃迁的光驱动操纵,通过激光加热和无衬底诱导效应实现。利用SCO系统在室温附近的鲁棒自旋双稳定性,我们量化了高达10%的可逆光体积变化,揭示了单粒子水平的精确开关阈值。独立的压力调制产生了相当的体积增加,确认了对相同双稳态过渡的机械控制。这些结果构成了悬浮SCO NPs中自旋态的完全实时控制和读出,其操作条件与超低功耗光开关、数据存储和纳米级传感兼容。
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引用次数: 0
Polymer-Derived Amorphous Aluminosilicate Nanomembranes for H2 Purification 聚合物衍生的非晶硅铝纳米膜用于氢气净化
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-02 DOI: 10.1021/acsnano.5c18108
Vinh T. Bui, Amandine Tirino, Ameya Manoj Tandel, Leiqing Hu, Erda Deng, Lingxiang Zhu, Shixian Ha, Won-Il Lee, Kim Kisslinger, Chang-Yong Nam, Haiqing Lin
Aluminosilicate zeolite membranes with robust microporous crystalline structures are attractive for the molecular separation of H2 from light gases, but their large-scale fabrication is complicated and costly, hindering their practical applications. Herein, we present polymer-derived amorphous aluminosilicate nanomembranes that combine the exceptional processability of polymers with the superior gas separation properties of aluminosilicates. Specifically, thin-film composite membranes comprising 150 nm polydimethylsiloxane were first treated with oxygen plasma to generate 10 nm polyorganosilica (POSi) on the surface, which were then subjected to few-cycle atomic layer deposition (ALD) using trimethylaluminum as a metal precursor and water vapor as a coreactant. This scalable two-step process yields few-nanometer amorphous aluminosilicates with strong size-sieving ability. For example, three-cycle ALD treatment of POSi increases H2/CO2 selectivity from 39 to 200 and H2/CH4 selectivity from 190 to 500, while decreasing H2 permeance from 990 to 210 GPU at 150 °C, superior to the state-of-the-art membranes. Rapid and scalable manufacturing of amorphous aluminosilicate nanolayers can also be of interest for catalysis and adsorption applications.
具有坚固的微孔晶体结构的铝硅酸盐沸石膜对从轻气体中分离H2具有吸引力,但其大规模制造复杂且成本高,阻碍了其实际应用。在此,我们提出了聚合物衍生的无定形硅酸铝纳米膜,它结合了聚合物的卓越可加工性和硅酸铝优越的气体分离性能。具体来说,首先用氧等离子体处理含有150纳米聚二甲基硅氧烷的薄膜复合膜,在表面生成10纳米聚有机硅(POSi),然后使用三甲基铝作为金属前驱体,水蒸气作为共反应剂进行少循环原子层沉积(ALD)。这种可扩展的两步工艺生产出具有强粒度筛选能力的非晶硅铝酸盐。例如,三循环ALD处理后,POSi的H2/CO2选择性从39提高到200,H2/CH4选择性从190提高到500,而在150℃下,H2透过率从990降低到210 GPU,优于最先进的膜。快速和可扩展的无定形硅酸铝纳米层的制造也可以用于催化和吸附应用。
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引用次数: 0
Oxygen Self-Sufficient Ir–MnII/III Coordination-Assembled Nanoparticles Evoke Apoptosis and Ferroptosis for Boosting Hypoxic Melanoma Photoimmunotherapy 氧自给自足的Ir-MnII /III配位组装纳米颗粒促进缺氧黑色素瘤光免疫治疗的凋亡和铁凋亡
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-02 DOI: 10.1021/acsnano.5c21399
Zixin Tang,Jun Shu,Ai-Ling Luo,Xianbo Wu,Tao Feng,Hui Chao
Photoimmunotherapy, recognized as the fifth modality of cancer treatment, integrates phototherapy with immunotherapy to enhance therapeutic outcomes. However, its immunomodulatory efficacy is often constrained by the tumor hypoxic microenvironment and single-immunostimulatory mechanisms. To address these challenges, we developed pH-light cascade-responsive nanoparticles (Ir–MnII/IIINPs) via coordination-driven assembly of a two-photon photosensitizer (Ir–OH) and immunoadjuvant Mn ions. Ir–MnII/IIINPs dissociate in the acidic lysosomal environment and activate upon irradiation, alleviating hypoxia via in situ oxygen generation and downregulating hypoxia-inducible factor 1α (HIF-1α) and programmed cell death ligand 1 (PD-L1) to reverse the immunosuppressive microenvironment. Abundant reactive oxygen species (ROS) produced by photodynamic and Fenton-like reactions induce lysosomal membrane permeabilization, facilitating the escape of Ir–OH into mitochondria. This process activates both ferroptosis and mitochondrial apoptosis to trigger immunogenic cell death (ICD). Moreover, mitochondrial damage-induced mtDNA release synergizes with the stimulator of interferon genes (STING) agonist Mn2+ to activate the cyclic guanosine monophosphate-adenosine monophosphate synthase (cGAS) -STING pathway, amplifying antitumor immunity. In a murine orthotopic melanoma model, Ir–MnII/IIINPs effectively reverses the immunosuppressive tumor microenvironment and achieves excellent photoimmunotherapeutic efficacy. This work presents a strategy for pH-light cascade-responsive and immune microenvironment remodeling via photoimmunotherapy, offering a promising direction for developing cancer treatments.
光免疫疗法将光疗法与免疫疗法相结合,以提高治疗效果,被认为是癌症治疗的第五种方式。然而,其免疫调节作用往往受到肿瘤缺氧微环境和单一免疫刺激机制的制约。为了解决这些挑战,我们通过双光子光敏剂(Ir-OH)和免疫佐剂Mn离子的配位驱动组装开发了ph光级联响应纳米颗粒(Ir-MnII /IIINPs)。Ir-MnII /IIINPs在酸性溶酶体环境中解离并在辐照下激活,通过原位产氧缓解缺氧,下调缺氧诱导因子1α (HIF-1α)和程序性细胞死亡配体1 (PD-L1)以逆转免疫抑制微环境。光动力和芬顿样反应产生的大量活性氧(ROS)诱导溶酶体膜渗透,促进Ir-OH逃逸到线粒体中。这一过程激活铁下垂和线粒体凋亡,从而引发免疫原性细胞死亡(ICD)。此外,线粒体损伤诱导的mtDNA释放与干扰素基因刺激剂(STING)激动剂Mn2+协同作用,激活环鸟苷单磷酸-腺苷单磷酸合成酶(cGAS) -STING途径,增强抗肿瘤免疫。在小鼠原位黑色素瘤模型中,Ir-MnII /IIINPs有效逆转了免疫抑制的肿瘤微环境,取得了优异的光免疫治疗效果。本研究提出了一种通过光免疫疗法进行ph -光级反应和免疫微环境重塑的策略,为癌症治疗的发展提供了一个有希望的方向。
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引用次数: 0
Highly Stable and Low-Cost Pure-Silica Zeolite with Narrow 8-Ring Pores: Unlocking Exclusive Carbon Dioxide Recognition from Hydrocarbons 具有窄8环孔的高稳定低成本纯硅沸石:从碳氢化合物中解锁专属二氧化碳识别
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-02 DOI: 10.1021/acsnano.5c19160
Chao Ma, Wenna Zhang, Jing Wang, Chenyang Nie, Xiaohe Wang, Nana Yan, Xiaona Liu, Peng Guo, Zhongmin Liu
The similar molecular sizes and physicochemical properties of carbon dioxide (CO2) and hydrocarbons like methane (CH4), acetylene (C2H2), ethylene (C2H4), and ethane (C2H6) make their separation a major industrial challenge. Here, we develop a low-cost, easily regenerable, pure-silica zeolite adsorbent “Instituto de Tecnología Química-55” (ITQ-55) capable of exclusively recognizing CO2 over these hydrocarbons. Guided by three-dimensional electron diffraction (3D ED) and density functional theory calculations, we identified commercially available and cost-effective diquaternary ammonium compounds as alternative organic structure-directing agents (OSDAs), partially replacing the previously expensive and complex ones for the synthesis of pure-silica ITQ-55. The calcined ITQ-55 features narrow 8-ring pores that enable selective CO2 adsorption while minimizing the uptake of CH4, C2H2, C2H4, and C2H6. Notably, the uptake ratio of CO2/C2H2 is much higher than that of currently reported CO2-selective adsorption materials. Dynamic breakthrough tests reveal that ITQ-55 exhibits excellent separation performance for CO2/C2H2, CO2/CH4, CO2/C2H4, and CO2/C2H6. In addition, the spent ITQ-55 adsorbent can be easily regenerated at 80 °C. Furthermore, theoretical calculations confirm that the separation mechanism of ITQ-55 for CO2/hydrocarbons is a size-exclusion mechanism.
二氧化碳(CO2)与甲烷(CH4)、乙炔(C2H2)、乙烯(C2H4)和乙烷(C2H6)等碳氢化合物的分子大小和物理化学性质相似,这使得它们的分离成为一项重大的工业挑战。在这里,我们开发了一种低成本,易于再生的纯硅沸石吸附剂Instituto de Tecnología Química-55 (ITQ-55),能够专门识别这些碳氢化合物上的二氧化碳。在三维电子衍射(3D ED)和密度泛函数理论计算的指导下,我们确定了商业上可获得且具有成本效益的二季铵化合物作为替代有机结构导向剂(OSDAs),部分取代了以前合成纯硅ITQ-55所需的昂贵且复杂的有机结构导向剂。煅烧的ITQ-55具有狭窄的8环孔,可以选择性地吸附CO2,同时最大限度地减少CH4, C2H2, C2H4和C2H6的吸收。值得注意的是,它对CO2/C2H2的吸收比远远高于目前报道的二氧化碳选择性吸附材料。动态突破试验表明,ITQ-55对CO2/C2H2、CO2/CH4、CO2/C2H4和CO2/C2H6具有优异的分离性能。此外,用过的ITQ-55吸附剂在80℃下可以很容易地再生。此外,理论计算证实了ITQ-55对CO2/烃类的分离机制为粒径排斥机制。
{"title":"Highly Stable and Low-Cost Pure-Silica Zeolite with Narrow 8-Ring Pores: Unlocking Exclusive Carbon Dioxide Recognition from Hydrocarbons","authors":"Chao Ma, Wenna Zhang, Jing Wang, Chenyang Nie, Xiaohe Wang, Nana Yan, Xiaona Liu, Peng Guo, Zhongmin Liu","doi":"10.1021/acsnano.5c19160","DOIUrl":"https://doi.org/10.1021/acsnano.5c19160","url":null,"abstract":"The similar molecular sizes and physicochemical properties of carbon dioxide (CO<sub>2</sub>) and hydrocarbons like methane (CH<sub>4</sub>), acetylene (C<sub>2</sub>H<sub>2</sub>), ethylene (C<sub>2</sub>H<sub>4</sub>), and ethane (C<sub>2</sub>H<sub>6</sub>) make their separation a major industrial challenge. Here, we develop a low-cost, easily regenerable, pure-silica zeolite adsorbent “Instituto de Tecnología Química-55” (ITQ-55) capable of exclusively recognizing CO<sub>2</sub> over these hydrocarbons. Guided by three-dimensional electron diffraction (3D ED) and density functional theory calculations, we identified commercially available and cost-effective diquaternary ammonium compounds as alternative organic structure-directing agents (OSDAs), partially replacing the previously expensive and complex ones for the synthesis of pure-silica ITQ-55. The calcined ITQ-55 features narrow 8-ring pores that enable selective CO<sub>2</sub> adsorption while minimizing the uptake of CH<sub>4</sub>, C<sub>2</sub>H<sub>2</sub>, C<sub>2</sub>H<sub>4</sub>, and C<sub>2</sub>H<sub>6</sub>. Notably, the uptake ratio of CO<sub>2</sub>/C<sub>2</sub>H<sub>2</sub> is much higher than that of currently reported CO<sub>2</sub>-selective adsorption materials. Dynamic breakthrough tests reveal that ITQ-55 exhibits excellent separation performance for CO<sub>2</sub>/C<sub>2</sub>H<sub>2</sub>, CO<sub>2</sub>/CH<sub>4</sub>, CO<sub>2</sub>/C<sub>2</sub>H<sub>4</sub>, and CO<sub>2</sub>/C<sub>2</sub>H<sub>6</sub>. In addition, the spent ITQ-55 adsorbent can be easily regenerated at 80 °C. Furthermore, theoretical calculations confirm that the separation mechanism of ITQ-55 for CO<sub>2</sub>/hydrocarbons is a size-exclusion mechanism.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"8 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097977","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
Boosting Electrocatalytic Ammonia Synthesis via Main-Group Metal Doping and Ionic Liquid Encapsulation in Copper Metal–Organic Frameworks 主基金属掺杂和铜金属有机骨架中离子液体包封促进电催化合成氨
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-02 DOI: 10.1021/acsnano.5c19267
Bo Han, Jie Ding, Man-Fai Ng, Chengyi Liu, Chu Zhang, Cailing Chen, Nan Zhang, Yue Hu, Jing Yan, Beier Jia, Erhai Hu, Mengxin Chen, Zhangliu Tian, Yu Han, Shibo Xi, Chade Lv, Qiang Zhu, Madhavi Srinivasan, Bin Liu, Qingyu Yan
The electrochemical nitrogen reduction reaction (EN2RR) provides a sustainable method for synthesizing ammonia at room temperature, but it is hindered by the low ammonia faradic efficiency (FE) and production yield. Herein, we report an effective EN2RR electrocatalyst: the ionic liquid-encapsulated aluminum copper bimetallic metal–organic framework (IL-AlCu-MOF). Comparisons across pristine Cu-MOF, AlCu-MOF, IL-Cu-MOF, and IL-AlCu-MOF reveal that the combination of Al doping and IL encapsulation can simultaneously promote dinitrogen activation and accelerate proton generation via water dissociation in a neutral electrolyte, which synergistically enhances the yield and selectivity of ammonia in EN2RR. The IL-AlCu-MOF achieves an NH3 yield of 124.7 μg·h–1·mgcat–1 with an FENH3 of 20.3% at −0.3 V (vs reversible hydrogen electrode, RHE) in 0.1 M K2SO4. In situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) measurements indicate improved water dissociation kinetics over that of IL-AlCu-MOF, and differential electrochemical mass spectrometry (DEMS) captures the EN2RR intermediates. Density functional theory (DFT) calculations show that Al doping modulates the Cu electronic structure for enhanced N2 activation, while IL encapsulation strengthens water adsorption at the MOF surface and thus accelerates water dissociation, both of which contribute to boosting the EN2RR performance.
电化学氮还原反应(EN2RR)为常温下合成氨提供了一种可持续的方法,但氨的法相效率(FE)和产率低阻碍了该方法的发展。本文报道了一种有效的EN2RR电催化剂:离子液体封装铝铜双金属金属有机骨架(IL-AlCu-MOF)。通过对原始Cu-MOF、AlCu-MOF、IL-Cu-MOF和IL-AlCu-MOF的比较发现,Al掺杂和IL包封可以同时促进二氮活化,并通过中性电解质中的水解离加速质子生成,从而协同提高EN2RR中氨的产率和选择性。IL-AlCu-MOF在−0.3 V (vs可逆氢电极,RHE)和0.1 M K2SO4条件下,NH3产率为124.7 μg·h-1·mgcat-1, FENH3为20.3%。原位衰减全反射表面增强红外吸收光谱(ATR-SEIRAS)测量表明,与IL-AlCu-MOF相比,水解离动力学有所改善,差分电化学质谱(DEMS)捕获了EN2RR中间体。密度泛函理论(DFT)计算表明,Al掺杂调节Cu电子结构增强N2活化,而IL包封增强MOF表面的水吸附从而加速水解离,两者都有助于提高EN2RR性能。
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引用次数: 0
Interpretable Machine Learning for Solid-State Batteries 固态电池的可解释机器学习
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-02 DOI: 10.1021/acsnano.5c21738
Xinyu Ye, Yaxin Cheng, Xuexia Lan, Yiwei You, Jing Peng, Guojin Liang, Xin Guo, Chenglong Zhao, Ho Seok Park, Yuanmiao Sun, Hui-Ming Cheng
Solid-state batteries (SSBs) have emerged as promising candidates for next-generation energy storage systems due to their high energy density and enhanced safety. In recent years, machine learning (ML) has become a transformative tool in battery research to accelerate the discovery of new materials and predict cycle life. However, the widespread application of ML is hindered by the “black-box” nature of many models, which limits their interpretability and scientific credibility. We propose a structured framework for using ML in SSB research by encompassing five components: (i) solid electrolyte design, (ii) material characterization, (iii) electrode/electrolyte interface optimization, (iv) battery lifetime prediction, and (v) dendrite inhibition. For each component, we identify its specific requirements and recommend appropriate approaches to develop interpretable ML. Finally, we summarize current challenges and propose corresponding suggestions as well as open-source toolchains aimed at transitioning from “black-box” predictions to mechanism-driven design, which will accelerate the development of high-performance SSBs for energy storage.
固态电池(SSBs)因其高能量密度和增强的安全性而成为下一代储能系统的有希望的候选者。近年来,机器学习(ML)已成为电池研究中的变革性工具,可以加速新材料的发现并预测循环寿命。然而,ML的广泛应用受到许多模型的“黑箱”性质的阻碍,这限制了它们的可解释性和科学可信度。我们提出了一个结构化的框架,将ML用于SSB研究,包括五个组成部分:(i)固体电解质设计,(ii)材料表征,(iii)电极/电解质界面优化,(iv)电池寿命预测,(v)枝晶抑制。对于每个组件,我们确定了其具体要求,并推荐了开发可解释ML的适当方法。最后,我们总结了当前的挑战,并提出了相应的建议,以及旨在从“黑箱”预测过渡到机制驱动设计的开源工具链,这将加速高性能储能ssb的开发。
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引用次数: 0
Moiré-Induced Electronic Reconstruction in van der Waals Heterobilayer PtSe2/PtTe2 van der Waals异质层PtSe2/PtTe2中moir<s:1>诱导的电子重构
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-02 DOI: 10.1021/acsnano.5c19273
Yin-Song Liao, Ruei-Yu Wang, Han-Wei Tsai, Guan-Hao Chen, Hsin-Hsien Chan, Hsun-Ting Hsieh, Cheng-Maw Cheng, Chun-Liang Lin, Meng-Kai Lin, Jyh-Pin Chou
van der Waals heterostructures composed of a few atomic layers have attracted significant attention in the condensed matter physics community. Although interlayer bonding is weak, effects such as moiré modulation, charge redistribution, and electronic hybridization can substantially modify the band structure and interlayer coupling. In this work, we investigate heterostructures composed of few-layer PtSe2 and PtTe2 by using first-principles calculations implemented within density functional theory (DFT) and angle-resolved photoemission spectroscopy (ARPES). While both materials are Dirac semimetals in the bulk form, they undergo a transition to semiconducting states in the few-layer limit. These heterostructures allow systematic examination of how dimensional confinement and interfacial interactions influence band structure and interlayer coupling. Our combined ARPES measurements and DFT calculations indicate the presence of electronic hybridization at the interface. The interlayer coupling in PtSe2/PtTe2 is associated with flat-band features and valence-band splitting induced by both inversion symmetry breaking and spin–orbit coupling. Furthermore, the local density of states indicates metallic behavior at the MM site while it remains semiconducting at MX and XX sites with the band gap of 0.40 and 0.25 eV, respectively. Further analysis shows that the electronic hybridization and charge transfer between PtSe2 and PtTe2 are sensitive to the interlayer distance, which is consistent with moiré characteristics. These results highlight how interfacial interactions govern the electronic properties of vdW heterostructures.
由几个原子层组成的范德华异质结构引起了凝聚态物理界的广泛关注。虽然层间键合较弱,但莫尔调制、电荷重分配和电子杂化等效应可以显著地改变能带结构和层间耦合。在这项工作中,我们使用密度泛函理论(DFT)和角分辨光谱学(ARPES)中的第一性原理计算来研究由少层PtSe2和PtTe2组成的异质结构。虽然这两种材料都是大块形式的狄拉克半金属,但它们在几层限制下经历了向半导体状态的过渡。这些异质结构允许系统地检查尺寸限制和界面相互作用如何影响能带结构和层间耦合。我们的综合ARPES测量和DFT计算表明,在界面上存在电子杂化。PtSe2/PtTe2的层间耦合与反转对称性破缺和自旋轨道耦合引起的平带特征和价带分裂有关。此外,在带隙分别为0.40和0.25 eV的MX和XX位点,态的局域密度显示了金属行为,而在带隙分别为0.40和0.25 eV的MX和XX位点则保持了半导体性质。进一步分析表明,PtSe2和PtTe2之间的电子杂化和电荷转移对层间距离很敏感,这与莫尔波特性是一致的。这些结果强调了界面相互作用如何控制vdW异质结构的电子特性。
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