Circular RNAs (circRNAs) play an important role in tumorigenesis induced by carbon nanotubes (CNTs) exposure, but the specific mechanism remains unclear. Here, we demonstrate for the first time that circTNIK promotes CNTs-induced malignant transformation by regulating the endoplasmic reticulum (ER) chaperone GRP78, thereby disrupting ER homeostasis and inhibiting type I interferon (IFN-I)-mediated antitumor immunity. Mechanistically, circTNIK interacts with GRP78 and interferes with its interaction with UPR sensors, thereby activating the ER stress response and promoting the transformation of cells toward a malignant phenotype. Meanwhile, circTNIK upregulates the expression of GRP78 and promotes its partial translocation into the nucleus. In the nucleus, GRP78 competitively binds to ID2, preventing its interaction with p65, a subunit of nuclear factor-κB (NF-κB), thereby inhibiting the phosphorylation of both NF-κB and IRF3, attenuating the IFN-I-mediated antitumor immune response and accelerating malignant transformation. Animal experiments showed that overexpression of circTNIK aggravated lung lesions in CNTs-exposed mice, accompanied by increased recruitment of M2 macrophages and decreased infiltration of CD8+ T cells. In clinical lung cancer tissue samples, circTNIK expression was positively correlated with GRP78 expression and negatively correlated with IFN-I signaling intensity, further supporting its oncogenic role in vivo. In summary, this study reveals that circTNIK plays a key role in CNTs-induced lung cancer development by regulating GRP78-mediated ER stress and IFN-I immunosuppression, providing a potential biomarker and therapeutic target for the early diagnosis and treatment of environmental-exposure-related lung cancer.
{"title":"circTNIK Promotes Carbon Nanotubes-Induced Lung Carcinogenesis via GRP78-Mediated Endoplasmic Reticulum Stress and Suppression of Type I Interferon Signaling","authors":"Wenlong Peng,Kexin Chen,Yi Hu,Ziyao Xiao,Zhenyu Pan,Xiliang Yang,Yuqing Tang,Wei Xue,Hongxing Liu,Wen Liu","doi":"10.1021/acsnano.5c16536","DOIUrl":"https://doi.org/10.1021/acsnano.5c16536","url":null,"abstract":"Circular RNAs (circRNAs) play an important role in tumorigenesis induced by carbon nanotubes (CNTs) exposure, but the specific mechanism remains unclear. Here, we demonstrate for the first time that circTNIK promotes CNTs-induced malignant transformation by regulating the endoplasmic reticulum (ER) chaperone GRP78, thereby disrupting ER homeostasis and inhibiting type I interferon (IFN-I)-mediated antitumor immunity. Mechanistically, circTNIK interacts with GRP78 and interferes with its interaction with UPR sensors, thereby activating the ER stress response and promoting the transformation of cells toward a malignant phenotype. Meanwhile, circTNIK upregulates the expression of GRP78 and promotes its partial translocation into the nucleus. In the nucleus, GRP78 competitively binds to ID2, preventing its interaction with p65, a subunit of nuclear factor-κB (NF-κB), thereby inhibiting the phosphorylation of both NF-κB and IRF3, attenuating the IFN-I-mediated antitumor immune response and accelerating malignant transformation. Animal experiments showed that overexpression of circTNIK aggravated lung lesions in CNTs-exposed mice, accompanied by increased recruitment of M2 macrophages and decreased infiltration of CD8+ T cells. In clinical lung cancer tissue samples, circTNIK expression was positively correlated with GRP78 expression and negatively correlated with IFN-I signaling intensity, further supporting its oncogenic role in vivo. In summary, this study reveals that circTNIK plays a key role in CNTs-induced lung cancer development by regulating GRP78-mediated ER stress and IFN-I immunosuppression, providing a potential biomarker and therapeutic target for the early diagnosis and treatment of environmental-exposure-related lung cancer.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"295 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111119","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 stability of perovskite precursors significantly impacts the performance of perovskite solar cell (PSCs). Notably, in the vapor–solid reaction perovskite fabrication process, both organic amine salt precursors and inorganic lead halide precursors are involved. Consequently, the long-term stability of these precursor materials plays a critical role in enabling the industrial-scale production of PSCs. Our observations revealed that the inherent instability of iodide ions (I–) in formamidinium iodide (FAI) precursor solutions accelerates solution aging. Additionally, the photoinstability of lead iodide (PbI2) promotes I– loss, generating iodine vacancies in the material. To address these issues, we introduced l-ascorbic acid (LAA) into the organic amine salt precursor solution to create an acidic and reducing environment, thereby reducing side reactions of the amine salt. Additionally, we effectively enhanced the stability of the PbI2 film by performing a surface dimensional regulation strategy on the PbI2 precursor film with 2-thiophenethylammonium iodide (2-ThEAI) vapor, inhibiting the formation of Pb0. As a result, PSCs fabricated by the optimized precursors achieve a power conversion efficiency (PCE) of 22.51% (@0.16 cm2) and 20.02% (@10 cm2). Remarkably, the four-terminal tandem photovoltaic device integrated with silicon solar cells achieves a PCE of 29.39%, demonstrating exceptional performance potential for next-generation solar technologies.
{"title":"Precursor Stabilization Strategies via Vapor–Solid Reaction for Reproducible and High-Efficiency Vapor-Deposited Perovskite Solar Cells","authors":"Shenghan Hu,Peiran Hou,Yichen Dou,Changyu Duan,Xinyu Deng,Yong Peng,Yi-Bing Cheng,Guijie Liang,Xiong Li,Zhiliang Ku","doi":"10.1021/acsnano.5c18423","DOIUrl":"https://doi.org/10.1021/acsnano.5c18423","url":null,"abstract":"The stability of perovskite precursors significantly impacts the performance of perovskite solar cell (PSCs). Notably, in the vapor–solid reaction perovskite fabrication process, both organic amine salt precursors and inorganic lead halide precursors are involved. Consequently, the long-term stability of these precursor materials plays a critical role in enabling the industrial-scale production of PSCs. Our observations revealed that the inherent instability of iodide ions (I–) in formamidinium iodide (FAI) precursor solutions accelerates solution aging. Additionally, the photoinstability of lead iodide (PbI2) promotes I– loss, generating iodine vacancies in the material. To address these issues, we introduced l-ascorbic acid (LAA) into the organic amine salt precursor solution to create an acidic and reducing environment, thereby reducing side reactions of the amine salt. Additionally, we effectively enhanced the stability of the PbI2 film by performing a surface dimensional regulation strategy on the PbI2 precursor film with 2-thiophenethylammonium iodide (2-ThEAI) vapor, inhibiting the formation of Pb0. As a result, PSCs fabricated by the optimized precursors achieve a power conversion efficiency (PCE) of 22.51% (@0.16 cm2) and 20.02% (@10 cm2). Remarkably, the four-terminal tandem photovoltaic device integrated with silicon solar cells achieves a PCE of 29.39%, demonstrating exceptional performance potential for next-generation solar technologies.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"215 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111117","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}
III–V Colloidal quantum dots (CQDs) have been widely studied for their applications as detectors and emitters from visible to short-wave infrared. They might also be used in the mid-infrared if they can be stably n-doped to access their intraband transitions. Mid-infrared intraband transitions are therefore studied for InAs, InAs/InP, and InAs/ZnSe CQDs with an energy gap of 1.4 μm. Using electrochemistry, the quantum dot films show state-resolved mobility, state-resolved electron filling, and intraband absorption in the 3–8 μm range. The InAs/ZnSe films need a more reducing potential than the InAs, but the InAs/InP films need a lower reduction potential. As a result, we found that dry films of InAs/InP dots show stable n-doping of the 1Se state, with a steady-state intraband absorption in the 3–5 μm range and intraband luminescence at 5 μm. With low toxicity, high thermal stability, and stable n-doping, InAs quantum dots become an interesting material for mid-infrared applications.
{"title":"Mid-infrared Intraband Transitions in InAs Colloidal Quantum Dots","authors":"Shraman Kumar Saha,Philippe Guyot-Sionnest","doi":"10.1021/acsnano.5c20445","DOIUrl":"https://doi.org/10.1021/acsnano.5c20445","url":null,"abstract":"III–V Colloidal quantum dots (CQDs) have been widely studied for their applications as detectors and emitters from visible to short-wave infrared. They might also be used in the mid-infrared if they can be stably n-doped to access their intraband transitions. Mid-infrared intraband transitions are therefore studied for InAs, InAs/InP, and InAs/ZnSe CQDs with an energy gap of 1.4 μm. Using electrochemistry, the quantum dot films show state-resolved mobility, state-resolved electron filling, and intraband absorption in the 3–8 μm range. The InAs/ZnSe films need a more reducing potential than the InAs, but the InAs/InP films need a lower reduction potential. As a result, we found that dry films of InAs/InP dots show stable n-doping of the 1Se state, with a steady-state intraband absorption in the 3–5 μm range and intraband luminescence at 5 μm. With low toxicity, high thermal stability, and stable n-doping, InAs quantum dots become an interesting material for mid-infrared applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"398 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111150","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}
Laurell F. Kessler, Yunqing Li, Ashwin Balakrishnan, Mike Heilemann
Stimulated emission depletion (STED) microscopy enables super-resolution imaging of complex biological samples in 3D, in large volumes, and live. However, molecular quantification with STED has remained underexplored. Here, we present a straightforward approach for quantitative STED that enables molecule counting. For this purpose, we designed DNA-fluorophore labels that enable signal amplification and allow for reliable intensity-based quantitative imaging. We demonstrate accurate molecule counting on DNA origami. Furthermore, we visualized and quantified EGF receptor monomers and dimers in cells. In summary, we introduce a robust, fast, and easy-to-implement tool for quantitative STED microscopy with single-protein resolution.
{"title":"Quantitative Stimulated Emission Depletion (STED) Microscopy with DNA-Fluorophore Labels","authors":"Laurell F. Kessler, Yunqing Li, Ashwin Balakrishnan, Mike Heilemann","doi":"10.1021/acsnano.5c21411","DOIUrl":"https://doi.org/10.1021/acsnano.5c21411","url":null,"abstract":"Stimulated emission depletion (STED) microscopy enables super-resolution imaging of complex biological samples in 3D, in large volumes, and live. However, molecular quantification with STED has remained underexplored. Here, we present a straightforward approach for quantitative STED that enables molecule counting. For this purpose, we designed DNA-fluorophore labels that enable signal amplification and allow for reliable intensity-based quantitative imaging. We demonstrate accurate molecule counting on DNA origami. Furthermore, we visualized and quantified EGF receptor monomers and dimers in cells. In summary, we introduce a robust, fast, and easy-to-implement tool for quantitative STED microscopy with single-protein resolution.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"95 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101926","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}
Hongwei Wang,Gan Jin,Mingyang Du,Yuxin Li,Xu Li,Xudong Zhu,Yurong Yang,Baomin Wang,Xiaohui Liu,Chengwang Niu,Lixin He,Tian Cui,Karin M. Rabe,Feng Liu
Rashba-type spin–orbit coupling is an important physical phenomenon for spintronic device applications. The size of Rashba splitting is generally enhanced by increasing inversion symmetry breaking, typically by increasing the spontaneous polarization of ferroelectric materials. Here, we identify an intriguing mechanism to enhance Rashba splitting by topological band inversion induced by strain. Using density functional theory, we show that monolayer quasi-1D ferroelectric chalcogenides BaTiSe3 and BaZrSe3 exhibit in-plane polarization, giving rise to Rashba splitting in the valence and conduction band edges with a persistent spin texture. Remarkably, under 1% compressive biaxial strain, the Rashba parameter and splitting energy of monolayer BaZrSe3 are enhanced to ∼3.0 eV Å and ∼60 meV, respectively, among the highest in 2D materials, and concurrently, a giant Berry curvature is induced, which is ∼1400 Å2 in magnitude. Our analysis shows that these enhancements result from a generic mechanism of strain-induced phase transition from semiconductor to topological insulator, which in turn changes interband transitions. Our findings manifest a unique strain-induced interplay between topology and ferroelectricity, and the integration of topological bands with Rashba splitting may provide promising applications to advancing spintronics technology.
rashba型自旋轨道耦合是自旋电子器件应用中的重要物理现象。Rashba分裂的大小通常通过增加反转对称性破缺来增强，特别是通过增加铁电材料的自发极化来增强。在这里，我们确定了一个有趣的机制，以增强Rashba分裂由应变引起的拓扑能带反转。利用密度泛函理论，我们发现单层准一维铁电硫族化合物BaTiSe3和BaZrSe3表现出面内极化，在价带和导带边缘产生Rashba分裂，并具有持续的自旋织体。值得注意的是，在1%的双轴压缩应变下，单层BaZrSe3的Rashba参数和分裂能分别提高到~ 3.0 eV Å和~ 60 meV，是二维材料中最高的，同时产生了一个巨大的Berry曲率，其量级为~ 1400 Å2。我们的分析表明，这些增强来自于从半导体到拓扑绝缘体的应变诱导相变的一般机制，这反过来又改变了带间转变。我们的发现表明了一种独特的应变诱导的拓扑和铁电性之间的相互作用，并且拓扑带与Rashba分裂的集成可能为推进自旋电子学技术提供有前途的应用。
{"title":"Strain-Induced Giant Topological Rashba Splitting","authors":"Hongwei Wang,Gan Jin,Mingyang Du,Yuxin Li,Xu Li,Xudong Zhu,Yurong Yang,Baomin Wang,Xiaohui Liu,Chengwang Niu,Lixin He,Tian Cui,Karin M. Rabe,Feng Liu","doi":"10.1021/acsnano.5c16503","DOIUrl":"https://doi.org/10.1021/acsnano.5c16503","url":null,"abstract":"Rashba-type spin–orbit coupling is an important physical phenomenon for spintronic device applications. The size of Rashba splitting is generally enhanced by increasing inversion symmetry breaking, typically by increasing the spontaneous polarization of ferroelectric materials. Here, we identify an intriguing mechanism to enhance Rashba splitting by topological band inversion induced by strain. Using density functional theory, we show that monolayer quasi-1D ferroelectric chalcogenides BaTiSe3 and BaZrSe3 exhibit in-plane polarization, giving rise to Rashba splitting in the valence and conduction band edges with a persistent spin texture. Remarkably, under 1% compressive biaxial strain, the Rashba parameter and splitting energy of monolayer BaZrSe3 are enhanced to ∼3.0 eV Å and ∼60 meV, respectively, among the highest in 2D materials, and concurrently, a giant Berry curvature is induced, which is ∼1400 Å2 in magnitude. Our analysis shows that these enhancements result from a generic mechanism of strain-induced phase transition from semiconductor to topological insulator, which in turn changes interband transitions. Our findings manifest a unique strain-induced interplay between topology and ferroelectricity, and the integration of topological bands with Rashba splitting may provide promising applications to advancing spintronics technology.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"66 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111149","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}
Bioinspired nanofluidic systems that utilize ions as signal carriers hold great promise for emulating neural processing in biochemical sensing and neuromorphic computing. However, achieving parallel, brain-like processing of multiple biochemical signals remains a significant challenge. Herein, we present a nanofluidic artificial postsynaptic membrane (APM) functionalized with confined DNA aptamers to construct a neuromorphic signal processing platform. Target-induced conformational switching of DNA aptamers dynamically modulates ionic transport through nanochannels, effectively mimicking synaptic information transmission. The integration of cross-responsive aptamer-based APM units into a cascaded logic system enables signal processing without relying on the physical series network of nanochannels. By independently addressing and reading each unit, dendritic multi-input integration and brain-like information fusion are achieved at the signal-algorithm level, and 100% accurate discrimination of multiple targets is reached. This approach marks a conceptual shift from the traditional “one-probe-one-target” model toward a brain-inspired, multitarget recognition architecture. The fusion of DNA probes with nanofluidic logic and their cascade at the signal level enables the development of neuromorphic biochips with integrated processing capabilities for multiplexed signals.
{"title":"Nanofluidic Confined DNA Aptamers for Neuromorphic Multiplex Discrimination","authors":"Yonghuan Chen,Xinru Yue,Yixin Ling,Yang Liu,Weihua Yu,Qi Zhu,Zilong He,Minrui Long,Xin-Qi Hao,Xu Hou,Fengyu Li","doi":"10.1021/acsnano.5c16862","DOIUrl":"https://doi.org/10.1021/acsnano.5c16862","url":null,"abstract":"Bioinspired nanofluidic systems that utilize ions as signal carriers hold great promise for emulating neural processing in biochemical sensing and neuromorphic computing. However, achieving parallel, brain-like processing of multiple biochemical signals remains a significant challenge. Herein, we present a nanofluidic artificial postsynaptic membrane (APM) functionalized with confined DNA aptamers to construct a neuromorphic signal processing platform. Target-induced conformational switching of DNA aptamers dynamically modulates ionic transport through nanochannels, effectively mimicking synaptic information transmission. The integration of cross-responsive aptamer-based APM units into a cascaded logic system enables signal processing without relying on the physical series network of nanochannels. By independently addressing and reading each unit, dendritic multi-input integration and brain-like information fusion are achieved at the signal-algorithm level, and 100% accurate discrimination of multiple targets is reached. This approach marks a conceptual shift from the traditional “one-probe-one-target” model toward a brain-inspired, multitarget recognition architecture. The fusion of DNA probes with nanofluidic logic and their cascade at the signal level enables the development of neuromorphic biochips with integrated processing capabilities for multiplexed signals.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"61 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111147","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}
Electrochemical carbon–nitrogen (C–N) coupling using simple inorganic feedstocks offers a sustainable route to valuable organonitrogen compounds such as amino acids. Herein, we present an atomically thin and acid-resistant p-block bismuthene (Bi-ene) derived via the reconstruction of a Bi-based metal–organic framework, where the enriched atomic misarrangement induces significant lattice strain that modulates the local electronic structure of the resultant Bi-ene, significantly boosting its electrocatalytic activity. Such defective Bi-ene exhibits an exceptional electrocatalytic performance for reductive C–N coupling in a salt-free acidic system, achieving a Faradaic efficiency (FE) of 95.7% and an ultrahigh yield rate of 1161 μmol cm–2 h–1 for NH2OH generation via the nitrate reduction reaction (NtrRR). Further, the efficient coreduction of HNO3 and oxalic acid (OA) over Bi-ene simultaneously generates NH2OH and glyoxylic acid (GX) respectively, which undergo effective C–N coupling to produce glycine with a high yield of 455.4 μmol cm–2 h–1. Moreover, the Bi-ene demonstrates stable performance for over 120 h at an industrial-relevant current density of 200 mA cm–2. Operando spectroscopy and calculations reveal that the strain in lattice-distorted Bi-ene optimizes the intermediate adsorption through modulating local electronic structure and thus enhances the efficacy for glycine electrosynthesis.
电化学碳氮（C-N）偶联使用简单的无机原料提供了一个可持续的途径有价值的有机氮化合物，如氨基酸。在此，我们提出了一种原子薄且耐酸的p-嵌段铋（Bi-ene），通过重建bi基金属有机框架，其中富集的原子错排引起显著的晶格应变，从而调节所得Bi-ene的局部电子结构，显著提高其电催化活性。该缺陷双烯在无盐酸性体系中对还原性C-N偶联具有优异的电催化性能，通过硝酸盐还原反应（NtrRR）生成NH2OH的法拉第效率（FE）达到95.7%，产率高达1161 μmol cm-2 h-1。此外，HNO3和草酸（OA）在双烯上有效共还原，分别生成NH2OH和乙醛酸（GX），并通过有效的C-N偶联生成甘氨酸，产率高达455.4 μmol cm-2 h-1。此外，在工业相关的200 mA cm-2电流密度下，Bi-ene表现出超过120小时的稳定性能。Operando光谱和计算结果表明，晶格畸变双烯中的应变通过调节局部电子结构来优化中间吸附，从而提高了甘氨酸电合成的效率。
{"title":"Salt-Free Glycine Electrosynthesis via Carbon–Nitrogen Coupling Boosted by the Lattice Strain in Atomically Thin p-Block Bismuthene","authors":"Minghong Huang,Sheng-Hua Zhou,Cheng-Jie Yang,Chung-Li Dong,Lei Jiao,Dong-Dong Ma,Qi-Long Zhu,Zhenguo Huang","doi":"10.1021/acsnano.5c19472","DOIUrl":"https://doi.org/10.1021/acsnano.5c19472","url":null,"abstract":"Electrochemical carbon–nitrogen (C–N) coupling using simple inorganic feedstocks offers a sustainable route to valuable organonitrogen compounds such as amino acids. Herein, we present an atomically thin and acid-resistant p-block bismuthene (Bi-ene) derived via the reconstruction of a Bi-based metal–organic framework, where the enriched atomic misarrangement induces significant lattice strain that modulates the local electronic structure of the resultant Bi-ene, significantly boosting its electrocatalytic activity. Such defective Bi-ene exhibits an exceptional electrocatalytic performance for reductive C–N coupling in a salt-free acidic system, achieving a Faradaic efficiency (FE) of 95.7% and an ultrahigh yield rate of 1161 μmol cm–2 h–1 for NH2OH generation via the nitrate reduction reaction (NtrRR). Further, the efficient coreduction of HNO3 and oxalic acid (OA) over Bi-ene simultaneously generates NH2OH and glyoxylic acid (GX) respectively, which undergo effective C–N coupling to produce glycine with a high yield of 455.4 μmol cm–2 h–1. Moreover, the Bi-ene demonstrates stable performance for over 120 h at an industrial-relevant current density of 200 mA cm–2. Operando spectroscopy and calculations reveal that the strain in lattice-distorted Bi-ene optimizes the intermediate adsorption through modulating local electronic structure and thus enhances the efficacy for glycine electrosynthesis.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"105 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111143","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}
Transitional metals (TMs)-based high-entropy alloys (HEAs) have demonstrated exceptional oxygen evolution reaction (OER) activity due to tunable electronic configurations and multimetallic synergy. However, their stability is hindered by oxidation and structural degradation resulting from intermetallic electron interactions during operation. Herein, we propose a cerium-mediated charge redistribution strategy in FeCoNiMnCe HEA, facilitating charge transfer from electron-rich Ce to neighboring TMs. This Ce-introduced HEA features increased dissolving activation energy of Fe/Mn and optimized electronic orbitals of Co/Ni, which inhibits the deactivation of active sites induced by high oxidized states during OER. Benefiting from charge accumulation on TMs, FeCoNiMnCe HEA achieves outstanding durability with negligible decay over 1000 h for OER at 10 mA cm–2 and enables stable zinc-air batteries operation for 4600 h at 2 mA cm–2. This work provides a robust strategy for designing stable HEA electrocatalysts through targeted electronic modulation.
基于过渡金属（TMs）的高熵合金（HEAs）由于可调谐的电子构型和多金属协同作用而表现出优异的析氧反应（OER）活性。然而，在操作过程中，金属间电子相互作用导致的氧化和结构降解阻碍了它们的稳定性。在此，我们提出了在FeCoNiMnCe HEA中铈介导的电荷再分配策略，促进电荷从富电子Ce转移到邻近的TMs。引入ce的HEA提高了Fe/Mn的溶解活化能，优化了Co/Ni的电子轨道，抑制了OER过程中高氧化态引起的活性位点失活。得益于TMs上的电荷积累，FeCoNiMnCe HEA在10 mA cm-2下的OER超过1000小时的衰减可以忽略不计，并且可以使锌-空气电池在2 mA cm-2下稳定运行4600小时。这项工作为通过定向电子调制设计稳定的HEA电催化剂提供了强有力的策略。
{"title":"Rare-Earth Element-Induced Charge Redistribution in High-Entropy Alloys toward Highly Stable Oxygen Evolution Catalysis","authors":"Junjie Hu,Zhitong Li,Xia Lei,Yanyi Wang,Wenbo Peng,Shuyu Cui,Kelin Chen,Gaole Liu,Tian Lang,Peide Zhu,Xiaolong Zhou,Sarayut Tunmee,Jintara Padchasri,Suttipong Wannapaiboon,Xingzhu Wang,Lei Yan,Xiongwei Zhong,Baomin Xu","doi":"10.1021/acsnano.5c18246","DOIUrl":"https://doi.org/10.1021/acsnano.5c18246","url":null,"abstract":"Transitional metals (TMs)-based high-entropy alloys (HEAs) have demonstrated exceptional oxygen evolution reaction (OER) activity due to tunable electronic configurations and multimetallic synergy. However, their stability is hindered by oxidation and structural degradation resulting from intermetallic electron interactions during operation. Herein, we propose a cerium-mediated charge redistribution strategy in FeCoNiMnCe HEA, facilitating charge transfer from electron-rich Ce to neighboring TMs. This Ce-introduced HEA features increased dissolving activation energy of Fe/Mn and optimized electronic orbitals of Co/Ni, which inhibits the deactivation of active sites induced by high oxidized states during OER. Benefiting from charge accumulation on TMs, FeCoNiMnCe HEA achieves outstanding durability with negligible decay over 1000 h for OER at 10 mA cm–2 and enables stable zinc-air batteries operation for 4600 h at 2 mA cm–2. This work provides a robust strategy for designing stable HEA electrocatalysts through targeted electronic modulation.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"11 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111146","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}
Lateral semiconductor homojunctions offer the advantages of perfect lattice matching and efficient carrier transport at the junctions, providing an ideal platform for high-performance optoelectronic devices. However, the fabrication of high-quality homostructures and the simultaneous realization of strong photovoltaic and photodetection performance remain challenging. In this work, we directly fabricated n+–n– MoS2 homostructures, consisting of partly pristine MoS2 and partly MoS2 stacked on a CrOCl insulator. Efficient charge transfer occurs at the MoS2/CrOCl interface, as confirmed by a ∼200 meV band shift observed in micro-ARPES measurements, consistent with our DFT calculations. As a result, the portion of MoS2 stacked on CrOCl can be modulated to p-type by controlling the gate voltage, in sharp contrast to the pristine MoS2 region. Moreover, the n+–n– MoS2 homostructures exhibit an open-circuit voltage of 0.87 V, a detectivity exceeding 1012 Jones, and a responsivity of 0.98 A/W without external stimuli, demonstrating both ultrahigh photovoltaic and self-powered photodetection capabilities. The results presented in our work provide a strategy for developing efficient optoelectronic devices based on two-dimensional homostructures.
横向半导体同质结具有完美的晶格匹配和高效的载流子输运等优点，为高性能光电器件提供了理想的平台。然而，制造高质量的同质结构并同时实现强大的光伏和光探测性能仍然具有挑战性。在这项工作中，我们直接制作了n+ - n - MoS2同质结构，由部分原始MoS2和部分堆叠在CrOCl绝缘体上的MoS2组成。有效的电荷转移发生在MoS2/CrOCl界面，正如在微arpes测量中观察到的~ 200 meV带移所证实的那样，与我们的DFT计算一致。因此，通过控制栅极电压，可以将堆叠在CrOCl上的MoS2部分调制为p型，与原始MoS2区域形成鲜明对比。此外，n+ - n- MoS2同构结构的开路电压为0.87 V，探测率超过1012 Jones，响应率为0.98 a /W，在没有外部刺激的情况下，显示出超高的光伏和自供电光探测能力。我们的工作结果为开发基于二维同构结构的高效光电器件提供了一种策略。
{"title":"Giant Photovoltaic Effect and Self-Powered Photodetection in Lateral MoS2 Homojunctions via Strong Interface Coupling","authors":"Jiyuan Xu,Yinglun Sun,Gangqiang Zhou,Jiajun Fang,Alexei Barinov,Nitin Mallik,Azzedine Bendounan,Marino Marsi,Zailan Zhang,Yingchun Cheng,Zhesheng Chen","doi":"10.1021/acsnano.5c18507","DOIUrl":"https://doi.org/10.1021/acsnano.5c18507","url":null,"abstract":"Lateral semiconductor homojunctions offer the advantages of perfect lattice matching and efficient carrier transport at the junctions, providing an ideal platform for high-performance optoelectronic devices. However, the fabrication of high-quality homostructures and the simultaneous realization of strong photovoltaic and photodetection performance remain challenging. In this work, we directly fabricated n+–n– MoS2 homostructures, consisting of partly pristine MoS2 and partly MoS2 stacked on a CrOCl insulator. Efficient charge transfer occurs at the MoS2/CrOCl interface, as confirmed by a ∼200 meV band shift observed in micro-ARPES measurements, consistent with our DFT calculations. As a result, the portion of MoS2 stacked on CrOCl can be modulated to p-type by controlling the gate voltage, in sharp contrast to the pristine MoS2 region. Moreover, the n+–n– MoS2 homostructures exhibit an open-circuit voltage of 0.87 V, a detectivity exceeding 1012 Jones, and a responsivity of 0.98 A/W without external stimuli, demonstrating both ultrahigh photovoltaic and self-powered photodetection capabilities. The results presented in our work provide a strategy for developing efficient optoelectronic devices based on two-dimensional homostructures.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"17 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111144","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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