ACS Earth and Space Chemistry最新文献

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A Biomimetic Nociceptor Based on a Vertical Multigate, Multichannel Neuromorphic Transistor 基于垂直多导多通道神经晶体管的仿生痛觉感受器
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-27 DOI: 10.1021/acsnano.4c0963210.1021/acsnano.4c09632
Han Xu, Da-Shan Shang*, Jianshi Tang*, Qing Luo, Xiaoxin Xu, Renrong Liang, Liyang Pan, Bin Gao, Qi Wang, Deyan He, Qi Liu*, Ming Liu, He Qian and Huaqiang Wu*, 
{"title":"A Biomimetic Nociceptor Based on a Vertical Multigate, Multichannel Neuromorphic Transistor","authors":"Han Xu,&nbsp;Da-Shan Shang*,&nbsp;Jianshi Tang*,&nbsp;Qing Luo,&nbsp;Xiaoxin Xu,&nbsp;Renrong Liang,&nbsp;Liyang Pan,&nbsp;Bin Gao,&nbsp;Qi Wang,&nbsp;Deyan He,&nbsp;Qi Liu*,&nbsp;Ming Liu,&nbsp;He Qian and Huaqiang Wu*,&nbsp;","doi":"10.1021/acsnano.4c0963210.1021/acsnano.4c09632","DOIUrl":"https://doi.org/10.1021/acsnano.4c09632https://doi.org/10.1021/acsnano.4c09632","url":null,"abstract":"<p >Nociceptors, crucial sensory receptors within biological systems, are essential for survival in diverse and potentially hazardous environments. Efforts to replicate nociceptors through advanced electronic devices, such as memristors and neuromorphic transistors, have achieved limited success, capturing basic nociceptive functions while more advanced characteristics like various forms of central sensitization and analgesic effect remain out of reach. Here, we introduce a vertical multigate, multichannel electrolyte-gated transistor (Vm-EGT), designed to mimic nociceptors. Utilizing the hybrid mechanism combining electric-double-layer (EDL) with ion intercalation/deintercalation in EGTs, our approach successfully replicates peripheral sensitization and desensitization characteristics of nociceptors. The intricate multigate and multichannel design of the Vm-EGT enables the emulation of more advanced nociceptive functionalities, including central sensitization and analgesic effect. Furthermore, we demonstrate that by exploiting the inherent current–voltage relationship, the Vm-EGT can simulate these advanced nociceptive features and seamlessly transition between them. Integrating a Vm-EGT with a thermistor and a heating plate, we have developed an artificial thermal nociceptor that closely mirrors the sensory attributes of its biological counterpart. Our approach significantly advances the emulation of nociceptors, providing a basis for the development of sophisticated artificial sensory systems and intelligent robotics.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 44","pages":"30668–30680 30668–30680"},"PeriodicalIF":15.8,"publicationDate":"2024-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577700","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Screening Na-Excess Cation-Disordered Rocksalt Cathodes with High Performance 筛选具有高性能的析出 Na 阳离子的岩盐阴极
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-27 DOI: 10.1021/acsnano.4c0928510.1021/acsnano.4c09285
Zichang Zhang, Jiahui Liu, Peng-Hu Du, Dingguo Xia and Qiang Sun*, 
{"title":"Screening Na-Excess Cation-Disordered Rocksalt Cathodes with High Performance","authors":"Zichang Zhang,&nbsp;Jiahui Liu,&nbsp;Peng-Hu Du,&nbsp;Dingguo Xia and Qiang Sun*,&nbsp;","doi":"10.1021/acsnano.4c0928510.1021/acsnano.4c09285","DOIUrl":"https://doi.org/10.1021/acsnano.4c09285https://doi.org/10.1021/acsnano.4c09285","url":null,"abstract":"<p >The practical application of Na-ion cathode materials is currently restricted by their low energy density and sluggish dynamics, while the cation-disordered rocksalt (DRX) structures offer a possible solution to the challenge. In this study, among the 24 candidates containing <i>d</i><sup>0</sup> elements, we use mixing temperature as a descriptor to screen the synthesizable Na-excess DRX, and we have identified Na<sub>1.2</sub>Mn<sub>0.4</sub>Mo<sub>0.4</sub>O<sub>2</sub> as the most promising candidate that exhibits a Na percolating fraction of 53%, which is higher than that of Li<sub>1.2</sub>Mn<sub>0.4</sub>Ti<sub>0.4</sub>O<sub>2</sub> (35%) proposed in the previous study due to the larger lattice constant in Na-excess DRX cathodes. More importantly, Na<sub>1.2</sub>Mn<sub>0.4</sub>Mo<sub>0.4</sub>O<sub>2</sub> is predicted to have a capacity of 228 mAh/g with an energy density of 552 Wh/kg derived from percolation theory and cluster-expansion Monte Carlo simulations, which is higher than that of Na<sub>1.3</sub>Nb<sub>0.3</sub>Mn<sub>0.4</sub>O<sub>2</sub> and Na<sub>1.14</sub>Mn<sub>0.57</sub>Ti<sub>0.29</sub>O<sub>2</sub> synthesized recently. For a better understanding, the redox mechanism is explored, which involves Mo<sup>4+</sup>/Mo<sup>6+</sup>, Mn<sup>3+</sup>/Mn<sup>4+</sup>, and O<sup>2–</sup>/O<sup>n–</sup> (0 &lt; <i>n</i> &lt; 2), indicating the participation of anionic redox. Meanwhile, the Na<sup>+</sup> diffusion prefers a divacancy mechanism via an o-t-o diffusion channel with a low diffusion barrier of 0.29 eV. This study expands the family of DRX for the cathode of Na-ion batteries with enhanced performance.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 44","pages":"30584–30592 30584–30592"},"PeriodicalIF":15.8,"publicationDate":"2024-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577714","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Heralded Generation of Correlated Photon Pairs from CdS/CdSe/CdS Quantum Shells 碲化镉/碲化镉/碲化镉量子壳相关光子对的预示性生成
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-26 DOI: 10.1021/acsnano.4c1172310.1021/acsnano.4c11723
Andrew A. Marder, Sean S. Smith, James Cassidy, Dulanjan Harankahage, Zhongjian Hu, Steve M. Savoy, George C. Schatz, Mikhail Zamkov* and Anton V. Malko*, 
{"title":"Heralded Generation of Correlated Photon Pairs from CdS/CdSe/CdS Quantum Shells","authors":"Andrew A. Marder,&nbsp;Sean S. Smith,&nbsp;James Cassidy,&nbsp;Dulanjan Harankahage,&nbsp;Zhongjian Hu,&nbsp;Steve M. Savoy,&nbsp;George C. Schatz,&nbsp;Mikhail Zamkov* and Anton V. Malko*,&nbsp;","doi":"10.1021/acsnano.4c1172310.1021/acsnano.4c11723","DOIUrl":"https://doi.org/10.1021/acsnano.4c11723https://doi.org/10.1021/acsnano.4c11723","url":null,"abstract":"<p >Quantum information processing demands efficient quantum light sources (QLS) capable of producing high-fidelity single photons or entangled photon pairs. Single epitaxial quantum dots (QDs) have long been proven to be efficient sources of deterministic single photons; however, their production via molecular-beam epitaxy presents scalability challenges. Conversely, colloidal semiconductor QDs offer scalable solution processing and tunable photoluminescence, but suffer from broader linewidths and unstable emissions. This leads to spectrally inseparable emission from exciton (X) and biexciton (XX) states, complicating the production of single photons and triggered photon pairs. Here, we demonstrate that colloidal semiconductor quantum shells (QSs) achieve significant spectral separation (∼75–80 meV) and long temporal stability of X and XX emissive states, enabling the observation of exciton-biexciton bunching in colloidal QDs. Our low-temperature single-particle measurements show cascaded XX-X emission of single photon pairs for over 200 s, with minimal overlap between X and XX features. The X-XX distinguishability allows for an in-depth theoretical characterization of cross-correlation strength, placing it in perspective with photon pairs of epitaxial counterparts. These findings highlight a strong potential of semiconductor quantum shells for applications in quantum information processing.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 44","pages":"30863–30870 30863–30870"},"PeriodicalIF":15.8,"publicationDate":"2024-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577623","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Realizing Dual-Mode Zinc-Ion Storage of Generic Vanadium-Based Cathodes via Organic Molecule Intercalation 通过有机分子互嵌实现通用钒基阴极的锌离子双模式存储
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-26 DOI: 10.1021/acsnano.4c1284910.1021/acsnano.4c12849
Hongwei Tang, Kexin Wan, Kang Zhang, Ao Wang, Mingkun Wang, Juan Xie, Pengcheng Su, Huilong Dong*, Jingyu Sun* and Yihui Li*, 
{"title":"Realizing Dual-Mode Zinc-Ion Storage of Generic Vanadium-Based Cathodes via Organic Molecule Intercalation","authors":"Hongwei Tang,&nbsp;Kexin Wan,&nbsp;Kang Zhang,&nbsp;Ao Wang,&nbsp;Mingkun Wang,&nbsp;Juan Xie,&nbsp;Pengcheng Su,&nbsp;Huilong Dong*,&nbsp;Jingyu Sun* and Yihui Li*,&nbsp;","doi":"10.1021/acsnano.4c1284910.1021/acsnano.4c12849","DOIUrl":"https://doi.org/10.1021/acsnano.4c12849https://doi.org/10.1021/acsnano.4c12849","url":null,"abstract":"<p >Intercalation engineering is a promising strategy to promote zinc-ion storage of layered cathodes; however, is impeded by the complex fabrication routes and inert electrochemical behaviors of intercalators. Herein, an organic imidazole intercalation strategy is proposed, where V<sub>2</sub>O<sub>5</sub> and NH<sub>4</sub>V<sub>3</sub>O<sub>8</sub> (NVO) model materials are adopted to verify the feasibility of the imidazole intercalator in improving the zinc storage capabilities of vanadium-based cathodes. The intercalated imidazole molecules could not only expand interlayer spacing and strengthen structural stability by serving as extra “pillars” but also provide extra coordination sites for zinc storage via the coordination reaction between Zn<sup>2+</sup> and the C═N group. This gives rise to a dual-mode ion storage mechanism and favorable electrochemical performances. As a result, imidazole-intercalated V<sub>2</sub>O<sub>5</sub> delivers a capacity of 179.9 mAh g<sup>–1</sup> after 5000 cycles at 20 A g<sup>–1</sup>, while the imidazole-intercalated NVO harvests a high capacity output of 170.2 mAh g<sup>–1</sup> after 700 cycles at 2 A g<sup>–1</sup>. This work is anticipated to boost the application potentials of vanadium-based cathodes in aqueous zinc-ion batteries.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 44","pages":"30896–30909 30896–30909"},"PeriodicalIF":15.8,"publicationDate":"2024-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577614","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Engineered Outer Membrane Vesicles as Nanosized Immune Cell Engagers for Enhanced Solid Tumor Immunotherapy 将工程外膜囊泡作为纳米级免疫细胞参与因子用于增强实体瘤免疫疗法
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-25 DOI: 10.1021/acsnano.4c0736410.1021/acsnano.4c07364
Jianan Sun, Liu Tan, Bang-Ce Ye* and Xiaobao Bi*, 
{"title":"Engineered Outer Membrane Vesicles as Nanosized Immune Cell Engagers for Enhanced Solid Tumor Immunotherapy","authors":"Jianan Sun,&nbsp;Liu Tan,&nbsp;Bang-Ce Ye* and Xiaobao Bi*,&nbsp;","doi":"10.1021/acsnano.4c0736410.1021/acsnano.4c07364","DOIUrl":"https://doi.org/10.1021/acsnano.4c07364https://doi.org/10.1021/acsnano.4c07364","url":null,"abstract":"<p >Although tumor immunotherapy has achieved significant success in recent years, tackling solid tumors remains a formidable challenge. Here, we present an approach that utilizes outer membrane vesicles (OMVs) from bacterial cells as scaffolds to engage immune cells in solid tumor immunotherapy. Two types of nanobodies targeting CD47/SIRPα and PD-1/PD-L1 pathways were simultaneously conjugated onto the surfaces of the OMVs in divalent and trivalent forms using orthogonal SpyCatcher-SpyTag and SnoopCatcher-SnoopTag chemistry. This resulted in the generation of an OMV-based nanosized immune cell engager (OMV-NICE) with dual-targeting abilities. <i>In vitro</i> assays confirmed the retention of the function of the two nanobodies on the OMV-NICE, as evidenced by the synergistically enhanced macrophage phagocytosis and T cell cytotoxicity against tumor cells. <i>In vivo</i> studies using a B16-F10 melanoma mouse model also revealed the superior antitumor activity of OMV-NICE compared to those of unconjugated nanobodies and OMVs alone. Subsequent mechanistic investigations further supported the enhanced recruitment of macrophages and T cells to the tumor region by OMV-NICE. Overall, this work expands the current repertoire of immune cell engagers, and the developed OMV-NICE platform holds great promise for broad applications, particularly in solid tumor immunotherapy.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 44","pages":"30332–30344 30332–30344"},"PeriodicalIF":15.8,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577558","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Ultralow-Power Circuit and Sensing Applications Based on Subthermionic Threshold Switching Transistors 基于亚热态阈值开关晶体管的超低功耗电路和传感应用
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-25 DOI: 10.1021/acsnano.4c0865010.1021/acsnano.4c08650
Anupom Devnath, Junseong Bae, Batyrbek Alimkhanuly, Gisung Lee, Seunghyun Lee, Arman Kadyrov, Shubham Patil and Dr Seunghyun Lee*, 
{"title":"Ultralow-Power Circuit and Sensing Applications Based on Subthermionic Threshold Switching Transistors","authors":"Anupom Devnath,&nbsp;Junseong Bae,&nbsp;Batyrbek Alimkhanuly,&nbsp;Gisung Lee,&nbsp;Seunghyun Lee,&nbsp;Arman Kadyrov,&nbsp;Shubham Patil and Dr Seunghyun Lee*,&nbsp;","doi":"10.1021/acsnano.4c0865010.1021/acsnano.4c08650","DOIUrl":"https://doi.org/10.1021/acsnano.4c08650https://doi.org/10.1021/acsnano.4c08650","url":null,"abstract":"<p >The most recent breakthrough in state-of-the-art electronics and optoelectronics involves the adoption of steep-slope field-effect transistors (FETs), promoting sub-60 mV/dec subthreshold swing (SS) at ambient temperature, effectively overcoming “Boltzmann limit” to minimize power consumption. Here, a series integration of nanoscale copper-based resistive-filamentary threshold switch (TS) with the IGZO channel-based FET is used to develop a TS-FET, in which the turn-on characteristics exhibit an abrupt transition over five decades, with an extremely low SS of 7 mV/dec, a high on/off ratio (&gt;10<sup>9</sup>), and ultralow leakage current (40-fold decrease), ensuring excellent repeatability and device yield. Unlike previous device-centric studies, this work highlights potential circuit applications (logic-inverter, pulse-sensor amplification, and photodetector) based on TS-FET. The sharp transition behavior of TS-FET enables the establishment of logic inverters with a high voltage gain of ≈800, with a circuit-level demonstration achieving a bias-independent record-high intrinsic gain (&gt;1000). A wearable pulse sensor integrated with an amplifier circuit ensured the precise amplification of electrophysical signals by 450 times. In addition, the application of a TS-FET-based photodetector features high responsivity (1.08 × 10<sup>4</sup> mA/W) and detectivity (1.03 × 10<sup>20</sup> Jones). The low-power strategy of TS-FETs is promising for the development of energy-efficient integrated circuits alongside sensor-interconnected biomedical applications in wearable technology.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 44","pages":"30497–30511 30497–30511"},"PeriodicalIF":15.8,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577591","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Colloidal Synthesis of Blue-Emitting Cs3TmCl6 Nanocrystals via Localized Excitonic Recombination for Down-Conversion White Light-Emitting Diodes 通过局部激子重组胶体合成用于下转换白光发光二极管的蓝色发光 Cs3TmCl6 纳米晶体
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-25 DOI: 10.1021/acsnano.4c0764110.1021/acsnano.4c07641
Meng Wang, Xu Chen*, Fei Zhang, Zhuangzhuang Ma, Xinzhen Ji, Shanshan Cheng, Gencai Pan, Di Wu, Xin-Jian Li, Yu Zhang, Chongxin Shan and Zhifeng Shi*, 
{"title":"Colloidal Synthesis of Blue-Emitting Cs3TmCl6 Nanocrystals via Localized Excitonic Recombination for Down-Conversion White Light-Emitting Diodes","authors":"Meng Wang,&nbsp;Xu Chen*,&nbsp;Fei Zhang,&nbsp;Zhuangzhuang Ma,&nbsp;Xinzhen Ji,&nbsp;Shanshan Cheng,&nbsp;Gencai Pan,&nbsp;Di Wu,&nbsp;Xin-Jian Li,&nbsp;Yu Zhang,&nbsp;Chongxin Shan and Zhifeng Shi*,&nbsp;","doi":"10.1021/acsnano.4c0764110.1021/acsnano.4c07641","DOIUrl":"https://doi.org/10.1021/acsnano.4c07641https://doi.org/10.1021/acsnano.4c07641","url":null,"abstract":"<p >Lead-halide perovskite nanocrystals (NCs) have gained significant attention for their promising applications in lighting and display technologies. However, blue-emitting NCs have struggled to match the high efficiency of their red and green counterparts. Moreover, many reported blue-emitting perovskite NCs contain heavy metal lead (Pb), which poses risks to human health and the environment. In this study, we synthesized rare-earth-based Cs<sub>3</sub>TmCl<sub>6</sub> NCs via the hot injection method, which exhibit a broadband blue emission at 440 nm. Combined experimental and theoretical studies indicate that the broadband emission in Cs<sub>3</sub>TmCl<sub>6</sub> arises from self-trapped excitons due to the excited-state structural distortion of the [TmCl<sub>6</sub>]<sup>3–</sup> cluster. Furthermore, the ultrafast dynamics of charge carriers were analyzed using time-resolved photoluminescence and transient absorption measurements. Encouraged by the remarkable thermal, light, and water stabilities of Cs<sub>3</sub>TmCl<sub>6</sub> NCs, as evidenced by experimental and theoretical results, a white light-emitting diode was further designed and fabricated using the Cs<sub>3</sub>TmCl<sub>6</sub> NCs as the color converter. The device exhibits outstanding performance, achieving a long half-lifetime of 336 h and a large color-rendering index of 87.0. Combining eco-friendly features and a facile synthesis method, the rare-earth-based Cs<sub>3</sub>TmCl<sub>6</sub> NCs mark a significant breakthrough as a reliable blue emitter, showcasing their future potential in lighting and display applications.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 44","pages":"30421–30432 30421–30432"},"PeriodicalIF":15.8,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577506","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Transforming Nanocrystals into Superhard Boron Carbide Nanostructures 将纳米晶体转化为超硬碳化硼纳米结构
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-25 DOI: 10.1021/acsnano.4c0859910.1021/acsnano.4c08599
Fernando Igoa Saldaña, Thomas Gaudisson, Sylvie Le Floch, Benoît Baptiste, Ludovic Delbes, Virgile Malarewicz, Olivier Beyssac, Keevin Béneut, Cristina Coelho Diogo, Christel Gervais, Gwenaëlle Rousse, Karsten Rasim, Yuri Grin, Alexandre Maître, Yann Le Godec* and David Portehault*, 
{"title":"Transforming Nanocrystals into Superhard Boron Carbide Nanostructures","authors":"Fernando Igoa Saldaña,&nbsp;Thomas Gaudisson,&nbsp;Sylvie Le Floch,&nbsp;Benoît Baptiste,&nbsp;Ludovic Delbes,&nbsp;Virgile Malarewicz,&nbsp;Olivier Beyssac,&nbsp;Keevin Béneut,&nbsp;Cristina Coelho Diogo,&nbsp;Christel Gervais,&nbsp;Gwenaëlle Rousse,&nbsp;Karsten Rasim,&nbsp;Yuri Grin,&nbsp;Alexandre Maître,&nbsp;Yann Le Godec* and David Portehault*,&nbsp;","doi":"10.1021/acsnano.4c0859910.1021/acsnano.4c08599","DOIUrl":"https://doi.org/10.1021/acsnano.4c08599https://doi.org/10.1021/acsnano.4c08599","url":null,"abstract":"<p >Boron carbide (B<sub>4+δ</sub>C) possesses a large potential as a structural material owing to its lightness, refractory character, and outstanding mechanical properties. However, its large-scale industrialization is set back by its tendency to amorphize when subjected to an external stress. In the present work, we design a path toward nanostructured boron carbide with greatly enhanced hardness and resistance to amorphization. The reaction pathway consists of triggering an isomorphic transformation of covalent nanocrystals of Na<sub>1–<i>x</i></sub>B<sub>5–<i>x</i></sub>C<sub>1+<i>x</i></sub> (<i>x</i> = 0.18) produced in molten salts. The resulting 10 nm B<sub>4.1</sub>C nanocrystals exhibit a 4-fold decrease of size compared to previous works. Solid-state <sup>11</sup>B and <sup>13</sup>C NMR coupled to density functional theory (DFT) reveal that the boron carbide nanocrystals are made of a complex mixture of atomic configurations, which are located at the covalent structural chains between B<sub>11</sub>C icosahedral building units. These nanocrystals are combined with a spark plasma-sintering-derived method operated at high pressure. This yields full densification while maintaining the particle size. The nanoscaled grains and high density of grain boundaries provide the resulting nanostructured bodies with significantly enhanced hardness and resistance to amorphization, thus delivering a superhard material.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 44","pages":"30473–30483 30473–30483"},"PeriodicalIF":15.8,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577559","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Wave Function Engineering on Superconducting Substrates: Chiral Yu-Shiba-Rusinov Molecules 超导基底上的波函数工程:手性 Yu-Shiba-Rusinov 分子
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-25 DOI: 10.1021/acsnano.4c1099810.1021/acsnano.4c10998
Lisa M. Rütten, Harald Schmid, Eva Liebhaber, Giada Franceschi, Ali Yazdani, Gaël Reecht, Kai Rossnagel, Felix von Oppen and Katharina J. Franke*, 
{"title":"Wave Function Engineering on Superconducting Substrates: Chiral Yu-Shiba-Rusinov Molecules","authors":"Lisa M. Rütten,&nbsp;Harald Schmid,&nbsp;Eva Liebhaber,&nbsp;Giada Franceschi,&nbsp;Ali Yazdani,&nbsp;Gaël Reecht,&nbsp;Kai Rossnagel,&nbsp;Felix von Oppen and Katharina J. Franke*,&nbsp;","doi":"10.1021/acsnano.4c1099810.1021/acsnano.4c10998","DOIUrl":"https://doi.org/10.1021/acsnano.4c10998https://doi.org/10.1021/acsnano.4c10998","url":null,"abstract":"<p >Magnetic adatoms on superconductors give rise to Yu-Shiba-Rusinov (YSR) states that hold considerable interest for the design of topological superconductivity. Here, we show that YSR states are also an ideal platform to engineer structures with intricate wave function symmetries. We assemble structures of iron atoms on the quasi-two-dimensional superconductor 2<i>H</i>-NbSe<sub>2</sub>. The Yu-Shiba-Rusinov wave functions of individual atoms extend over several nanometers enabling hybridization even at large adatom spacing. We show that the substrate can be exploited to deliberately break symmetries of the adatom structure leading to hybridized YSR states exhibiting symmetries that cannot be found in orbitals of iso-structural planar molecules in the gas phase. We exploit this potential by designing chiral YSR wave functions of triangular adatom structures. Our results significantly expand the range of interesting quantum states that can be engineered using arrays of magnetic adatoms on superconductors.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 44","pages":"30798–30804 30798–30804"},"PeriodicalIF":15.8,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnano.4c10998","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577592","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mitochondrial Bioenergetics of Functional Wound Closure is Dependent on Macrophage–Keratinocyte Exosomal Crosstalk 功能性伤口闭合的线粒体生物能取决于巨噬细胞-角质形成细胞外泌体的串联作用
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-25 DOI: 10.1021/acsnano.4c0761010.1021/acsnano.4c07610
Anu Sharma, Rajneesh Srivastava, Surya C. Gnyawali, Pramod Bhasme, Adam J. Anthony, Yi Xuan, Jonathan C. Trinidad, Chandan K. Sen, David E. Clemmer, Sashwati Roy and Subhadip Ghatak*, 
{"title":"Mitochondrial Bioenergetics of Functional Wound Closure is Dependent on Macrophage–Keratinocyte Exosomal Crosstalk","authors":"Anu Sharma,&nbsp;Rajneesh Srivastava,&nbsp;Surya C. Gnyawali,&nbsp;Pramod Bhasme,&nbsp;Adam J. Anthony,&nbsp;Yi Xuan,&nbsp;Jonathan C. Trinidad,&nbsp;Chandan K. Sen,&nbsp;David E. Clemmer,&nbsp;Sashwati Roy and Subhadip Ghatak*,&nbsp;","doi":"10.1021/acsnano.4c0761010.1021/acsnano.4c07610","DOIUrl":"https://doi.org/10.1021/acsnano.4c07610https://doi.org/10.1021/acsnano.4c07610","url":null,"abstract":"<p >Tissue nanotransfection (TNT)-based fluorescent labeling of cell-specific exosomes has shown that exosomes play a central role in physiological keratinocyte–macrophage (mϕ) crosstalk at the wound-site. Here, we report that during the early phase of wound reepithelialization, macrophage-derived exosomes (Exo<sub>mϕ</sub>), enriched with the outer mitochondrial membrane protein TOMM70, are localized in leading-edge keratinocytes. TOMM70 is a 70 kDa adaptor protein anchored in the mitochondrial outer membrane and plays a critical role in maintaining mitochondrial function and quality. TOMM70 selectively recognizes cytosolic chaperones by its tetratricopeptide repeat (TPR) domain and facilitates the import of preproteins lacking a positively charged mitochondrial targeted sequence. Exosomal packaging of TOMM70 in mϕ was independent of mitochondrial fission. TOMM70-enriched Exo<sub>mϕ</sub> compensated for the hypoxia-induced depletion of epidermal TOMM70, thereby rescuing mitochondrial metabolism in leading-edge keratinocytes. Thus, macrophage-derived TOMM70 is responsible for the glycolytic ATP supply to power keratinocyte migration. Blockade of exosomal uptake from keratinocytes impaired wound closure with the persistence of proinflammatory mϕ in the wound microenvironment, pointing toward a bidirectional crosstalk between these two cell types. The significance of such bidirectional crosstalk was established by the observation that in patients with nonhealing diabetic foot ulcers, TOMM70 is deficient in keratinocytes of wound-edge tissues.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 44","pages":"30405–30420 30405–30420"},"PeriodicalIF":15.8,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnano.4c07610","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577605","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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