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.
{"title":"Nontoxic CuInS2/ZnS Colloidal Quantum Dots for White Light-Emitting Diodes","authors":"Xiangda Deng,Wenxin Yang,Tianmin Wu","doi":"10.1021/acsnano.5c12714","DOIUrl":"https://doi.org/10.1021/acsnano.5c12714","url":null,"abstract":"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.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"276 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111148","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}
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。
{"title":"Enabling Ultrahigh-Power-Density LiMn0.6Fe0.4PO4 Cathodes via Kinetics Limitation Breakthrough and Jahn–Teller Distortion Mitigation","authors":"Pengxu Wang, Haifeng Yu, Ling Chen, Yaoguo Fang, Qian Cheng, Hao Jiang, Chunzhong Li","doi":"10.1021/acsnano.5c21496","DOIUrl":"https://doi.org/10.1021/acsnano.5c21496","url":null,"abstract":"Development of high-power LiMn<sub>x</sub>Fe<sub>1-x</sub>PO<sub>4</sub> (LMFP) cathodes is fundamentally challenged by the interplay between sluggish one-dimensional Li<sup>+</sup> diffusion and severe Jahn–Teller distortion. Herein, we propose a synergistic substitution strategy to concurrently tackle these issues. Partial replacement of PO<sub>4</sub> tetrahedra by planar BO<sub>3</sub> groups creates three-dimensional interconnected Li-ion diffusion networks, while doping Nb<sup>5+</sup> into transition-metal sites widens the diffusion channels. This tailored microstructure not only overcomes the intrinsic Li<sup>+</sup> diffusion kinetics limitation but also dissipates the mechanical stress arising from high-rate operating conditions, suppressing the Jahn–Teller distortion in MnO<sub>6</sub> octahedra by 36%. The optimized LMFP cathode delivers an ultrahigh reversible capacity of 126 mAh g<sup>–1</sup> 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<sup>+</sup> diffusion kinetics and structural stability, providing an available paradigm for designing high-power, long-life Mn-based cathode materials.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"290 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101927","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}
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.
{"title":"Unravel Electrolyte-Dependent Interphase Structures in Lithium-Sulfurized Polyacrylonitrile Batteries via Cryogenic Transmission Electron Microscopy","authors":"Cheng Zhen, Xianbin Wei, Yuxuan Cui, Xinzhen Lu, Jiashu Chen, Menghao Li, Tingting Zhang, Shaobo Han, Xuming Yang, Meng Danny Gu","doi":"10.1021/acsnano.5c14570","DOIUrl":"https://doi.org/10.1021/acsnano.5c14570","url":null,"abstract":"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.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"30 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101965","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}
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.
{"title":"Unveiling Spin Transition at Single-Particle Level in Levitating Spin Crossover Nanoparticles","authors":"Elena Pinilla-Cienfuegos, Lucas Mascaró-Burguera, Ramón Torres-Cavanillas, J. Ignacio Echavarría, Alejandro Regueiro, Eugenio Coronado, Javier Hernandez-Rueda","doi":"10.1021/acsnano.5c18794","DOIUrl":"https://doi.org/10.1021/acsnano.5c18794","url":null,"abstract":"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.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"1 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101966","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}
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.
{"title":"Polymer-Derived Amorphous Aluminosilicate Nanomembranes for H2 Purification","authors":"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","doi":"10.1021/acsnano.5c18108","DOIUrl":"https://doi.org/10.1021/acsnano.5c18108","url":null,"abstract":"Aluminosilicate zeolite membranes with robust microporous crystalline structures are attractive for the molecular separation of H<sub>2</sub> 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 H<sub>2</sub>/CO<sub>2</sub> selectivity from 39 to 200 and H<sub>2</sub>/CH<sub>4</sub> selectivity from 190 to 500, while decreasing H<sub>2</sub> 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.","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":"146097927","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}
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.
{"title":"Oxygen Self-Sufficient Ir–MnII/III Coordination-Assembled Nanoparticles Evoke Apoptosis and Ferroptosis for Boosting Hypoxic Melanoma Photoimmunotherapy","authors":"Zixin Tang,Jun Shu,Ai-Ling Luo,Xianbo Wu,Tao Feng,Hui Chao","doi":"10.1021/acsnano.5c21399","DOIUrl":"https://doi.org/10.1021/acsnano.5c21399","url":null,"abstract":"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.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"92 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146098009","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}
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}
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。
{"title":"Boosting Electrocatalytic Ammonia Synthesis via Main-Group Metal Doping and Ionic Liquid Encapsulation in Copper Metal–Organic Frameworks","authors":"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","doi":"10.1021/acsnano.5c19267","DOIUrl":"https://doi.org/10.1021/acsnano.5c19267","url":null,"abstract":"The electrochemical nitrogen reduction reaction (EN<sub>2</sub>RR) 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 EN<sub>2</sub>RR 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 EN<sub>2</sub>RR. The IL-AlCu-MOF achieves an NH<sub>3</sub> yield of 124.7 μg·h<sup>–1</sup>·mg<sub>cat</sub><sup>–1</sup> with an FE<sub>NH<sub>3</sub></sub> of 20.3% at −0.3 V (vs reversible hydrogen electrode, RHE) in 0.1 M K<sub>2</sub>SO<sub>4</sub>. 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 EN<sub>2</sub>RR intermediates. Density functional theory (DFT) calculations show that Al doping modulates the Cu electronic structure for enhanced N<sub>2</sub> activation, while IL encapsulation strengthens water adsorption at the MOF surface and thus accelerates water dissociation, both of which contribute to boosting the EN<sub>2</sub>RR performance.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"1 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101925","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}
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.
{"title":"Interpretable Machine Learning for Solid-State Batteries","authors":"Xinyu Ye, Yaxin Cheng, Xuexia Lan, Yiwei You, Jing Peng, Guojin Liang, Xin Guo, Chenglong Zhao, Ho Seok Park, Yuanmiao Sun, Hui-Ming Cheng","doi":"10.1021/acsnano.5c21738","DOIUrl":"https://doi.org/10.1021/acsnano.5c21738","url":null,"abstract":"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.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"82 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097978","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}
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.
{"title":"Moiré-Induced Electronic Reconstruction in van der Waals Heterobilayer PtSe2/PtTe2","authors":"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","doi":"10.1021/acsnano.5c19273","DOIUrl":"https://doi.org/10.1021/acsnano.5c19273","url":null,"abstract":"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 PtSe<sub>2</sub> and PtTe<sub>2</sub> 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 PtSe<sub>2</sub>/PtTe<sub>2</sub> 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 PtSe<sub>2</sub> and PtTe<sub>2</sub> 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.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"1 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097976","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}
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