Pub Date : 2024-07-03DOI: 10.1007/s12274-024-6791-2
Yuwei Xiong, Kuibo Yin, Weiwei Sun, Jingcang Li, Shangyang Shang, Lei Xin, Qiyun Wu, Xiaoran Gong, Yidong Xia, Litao Sun
The solid-electrolyte-based memristors have attracted tremendous attention for the next-generation nonvolatile memory for both logic and neuromorphic applications. However, they encounter variability performance challenges which originated from the random ionic transport and conductive filaments formation. Evidently, the electrochemical metallized mechanism associated with ion transport has been elucidated. Nonetheless, the failure mechanism caused by ion transport during cycles is rarely reported. Hereafter, the five stages of failure in the Ag/Ag10Ge15Te75/W memristor are elucidated through ex-situ current-voltage measurements combined with in-situ transmission electron microscopy characteristics. Our investigation reveals that the migration and enrichment of Ag ions result in the precipitation of Ag2Te. The formation of Ag2Te hinders the device’s ability to maintain its bipolar characteristics and also decreases the resistance value of the high resistance state, thereby reducing the device’s switching ratio. The promising results provide important guidance for the future design of structures and the manipulation of ion transport for high-performance memristors.
{"title":"Observation of the failure mechanism in Ag10Ge15Te75-based memristor induced by ion transport","authors":"Yuwei Xiong, Kuibo Yin, Weiwei Sun, Jingcang Li, Shangyang Shang, Lei Xin, Qiyun Wu, Xiaoran Gong, Yidong Xia, Litao Sun","doi":"10.1007/s12274-024-6791-2","DOIUrl":"https://doi.org/10.1007/s12274-024-6791-2","url":null,"abstract":"<p>The solid-electrolyte-based memristors have attracted tremendous attention for the next-generation nonvolatile memory for both logic and neuromorphic applications. However, they encounter variability performance challenges which originated from the random ionic transport and conductive filaments formation. Evidently, the electrochemical metallized mechanism associated with ion transport has been elucidated. Nonetheless, the failure mechanism caused by ion transport during cycles is rarely reported. Hereafter, the five stages of failure in the Ag/Ag<sub>10</sub>Ge<sub>15</sub>Te<sub>75</sub>/W memristor are elucidated through <i>ex-situ</i> current-voltage measurements combined with <i>in-situ</i> transmission electron microscopy characteristics. Our investigation reveals that the migration and enrichment of Ag ions result in the precipitation of Ag<sub>2</sub>Te. The formation of Ag<sub>2</sub>Te hinders the device’s ability to maintain its bipolar characteristics and also decreases the resistance value of the high resistance state, thereby reducing the device’s switching ratio. The promising results provide important guidance for the future design of structures and the manipulation of ion transport for high-performance memristors.\u0000</p>","PeriodicalId":713,"journal":{"name":"Nano Research","volume":null,"pages":null},"PeriodicalIF":9.9,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524336","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-02DOI: 10.1007/s12274-024-6807-y
Sanjun Fan, Brian T. Scarpitti, Zhewen Luo, Abigail E. Smith, Jian Ye, Zachary D. Schultz
Hot spot engineering in plasmonic nanostructures plays a significant role in surface-enhanced Raman scattering (SERS) for bioanalysis and cell imaging. However, creating stable, reproducible, and strong SERS signals remains challenging due to the potential interference from surrounding chemicals and locating SERS-active analytes into hot-spot regions. Herein, we developed a straightforward approach to synthesize intra-gap nanoparticles encapsulating 4-nitrobenzenethiol (4-NBT) as a reporter molecule within these gaps to avoid outside interference. We made three kinds of intra-gap nanoparticles using nanorods, bipyramids, and nanospheres as cores, in which the nanorods based intra-gap nanoparticles exhibit the highest SERS activity. The advantage of our method is the ease of preparation of high-yield and stable intra-gap nanoparticles characterized by a short incubation time (10 min) with 4-NBT and quick synthesis without requiring an additional step to centrifuge for the purification of core nanoparticles. The intense localized field in the synthesized hot spots of these plasmonic gap nanostructures holds great promise as a SERS substrate for a broad range of quantitative optical applications.
{"title":"Facile synthesis of intra-nanogap enhanced Raman tags with different shapes","authors":"Sanjun Fan, Brian T. Scarpitti, Zhewen Luo, Abigail E. Smith, Jian Ye, Zachary D. Schultz","doi":"10.1007/s12274-024-6807-y","DOIUrl":"https://doi.org/10.1007/s12274-024-6807-y","url":null,"abstract":"<p>Hot spot engineering in plasmonic nanostructures plays a significant role in surface-enhanced Raman scattering (SERS) for bioanalysis and cell imaging. However, creating stable, reproducible, and strong SERS signals remains challenging due to the potential interference from surrounding chemicals and locating SERS-active analytes into hot-spot regions. Herein, we developed a straightforward approach to synthesize intra-gap nanoparticles encapsulating 4-nitrobenzenethiol (4-NBT) as a reporter molecule within these gaps to avoid outside interference. We made three kinds of intra-gap nanoparticles using nanorods, bipyramids, and nanospheres as cores, in which the nanorods based intra-gap nanoparticles exhibit the highest SERS activity. The advantage of our method is the ease of preparation of high-yield and stable intra-gap nanoparticles characterized by a short incubation time (10 min) with 4-NBT and quick synthesis without requiring an additional step to centrifuge for the purification of core nanoparticles. The intense localized field in the synthesized hot spots of these plasmonic gap nanostructures holds great promise as a SERS substrate for a broad range of quantitative optical applications.\u0000</p>","PeriodicalId":713,"journal":{"name":"Nano Research","volume":null,"pages":null},"PeriodicalIF":9.9,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524334","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
As an energy-free cooling technique, radiative cooling has garnered significant attention in the field of energy conservation. However, traditional radiative cooling films often possess static optical properties and their inherent opacity limits their applications in building such as windows. Therefore, there exists a requirement for passive radiative cooling films endowed with adjustable transmittance. Here we report the porous block copolymer films with self-adjustable optical transmittance and passive radiative cooling. In a result, the film exhibited a high solar reflectance (0.3–2.5 µm) of 96.9% and a high infrared emittance (8–13 µm) of 97.9%. Outdoor experiments demonstrated that the film surface temperature was 6.6 °C lower than ambient temperature, with a cooling power of 104.8 W·m−2. In addition, the film’s transmittance can be regulated by altering the polarity of the postprocessing solvent, providing an effective approach for regulating indoor light intensity and thermal balance, thereby enhancing the applicability of radiative cooling.
{"title":"Porous block copolymer films with self-adjustable optical transmittance and passive radiative cooling","authors":"Xue Meng, Weiming Tang, Shuyun Zhuo, Jince Zhao, Zixuan Ren, Zhonghe Sun, Hao Yan, Tianyi Zhao, Ziguang Zhao, Mingjie Liu","doi":"10.1007/s12274-024-6778-z","DOIUrl":"https://doi.org/10.1007/s12274-024-6778-z","url":null,"abstract":"<p>As an energy-free cooling technique, radiative cooling has garnered significant attention in the field of energy conservation. However, traditional radiative cooling films often possess static optical properties and their inherent opacity limits their applications in building such as windows. Therefore, there exists a requirement for passive radiative cooling films endowed with adjustable transmittance. Here we report the porous block copolymer films with self-adjustable optical transmittance and passive radiative cooling. In a result, the film exhibited a high solar reflectance (0.3–2.5 µm) of 96.9% and a high infrared emittance (8–13 µm) of 97.9%. Outdoor experiments demonstrated that the film surface temperature was 6.6 °C lower than ambient temperature, with a cooling power of 104.8 W·m<sup>−2</sup>. In addition, the film’s transmittance can be regulated by altering the polarity of the postprocessing solvent, providing an effective approach for regulating indoor light intensity and thermal balance, thereby enhancing the applicability of radiative cooling.\u0000</p>","PeriodicalId":713,"journal":{"name":"Nano Research","volume":null,"pages":null},"PeriodicalIF":9.9,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524335","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-02DOI: 10.1007/s12274-024-6774-3
Nannan Ji, Haoyun Sheng, Shilong Liu, Yangyuan Zhang, Hongfei Sun, Lingzhi Wei, Ziqi Tian, Peng Jiang, Qianwang Chen, Jianwei Su
Optimization of Pt atom utilization efficiency is critical for the development of proton-exchange-membrane fuel cells. Here we aim to develop an efficient oxygen reduction reaction (ORR) catalyst with a low Pt content through the concurrent modification of Pt-Co alloy catalysts and carbon substrate. In the present study, ultrafine Pt-Co alloy nanoparticles are successfully synthesized and stabilized by topological carbon defects via adopting the ammonia thermal treatment. Despite the low Pt loading, the obtained catalyst exhibits an impressive half-wave potential of 0.926 V versus the reversible hydrogen electrode in 0.1 M HClO4 electrolyte. Furthermore, the durability testing using the timed-current method demonstrates a tiny loss of only 3.6% after 12 h. Both experimental results and theoretical calculations demonstrate that topological carbon defects significantly enhance the charge transfer processes at the alloy/carbon interface, contributing to the strong electronic metal-support interactions between the Pt-Co alloy nanoparticles and topological carbon defects. These interactions, along with the alloy effect, play a crucial role in promoting the ORR performance in acidic media.
优化铂原子的利用效率对于质子交换膜燃料电池的开发至关重要。在此,我们旨在通过同时改性铂-钴合金催化剂和碳衬底,开发一种铂含量较低的高效氧还原反应(ORR)催化剂。在本研究中,我们成功合成了超细铂钴合金纳米颗粒,并通过氨热处理使其因碳的拓扑缺陷而变得稳定。尽管铂负载量较低,但所获得的催化剂在 0.1 M HClO4 电解液中与可逆氢电极相比,半波电位达到了惊人的 0.926 V。实验结果和理论计算均表明,拓扑碳缺陷显著增强了合金/碳界面的电荷转移过程,从而促进了铂-钴合金纳米颗粒与拓扑碳缺陷之间强烈的电子金属支撑相互作用。这些相互作用以及合金效应在促进酸性介质中的 ORR 性能方面发挥了至关重要的作用。
{"title":"Boosting oxygen reduction in acidic media through integration of Pt-Co alloy effect and strong interaction with carbon defects","authors":"Nannan Ji, Haoyun Sheng, Shilong Liu, Yangyuan Zhang, Hongfei Sun, Lingzhi Wei, Ziqi Tian, Peng Jiang, Qianwang Chen, Jianwei Su","doi":"10.1007/s12274-024-6774-3","DOIUrl":"https://doi.org/10.1007/s12274-024-6774-3","url":null,"abstract":"<p>Optimization of Pt atom utilization efficiency is critical for the development of proton-exchange-membrane fuel cells. Here we aim to develop an efficient oxygen reduction reaction (ORR) catalyst with a low Pt content through the concurrent modification of Pt-Co alloy catalysts and carbon substrate. In the present study, ultrafine Pt-Co alloy nanoparticles are successfully synthesized and stabilized by topological carbon defects via adopting the ammonia thermal treatment. Despite the low Pt loading, the obtained catalyst exhibits an impressive half-wave potential of 0.926 V versus the reversible hydrogen electrode in 0.1 M HClO<sub>4</sub> electrolyte. Furthermore, the durability testing using the timed-current method demonstrates a tiny loss of only 3.6% after 12 h. Both experimental results and theoretical calculations demonstrate that topological carbon defects significantly enhance the charge transfer processes at the alloy/carbon interface, contributing to the strong electronic metal-support interactions between the Pt-Co alloy nanoparticles and topological carbon defects. These interactions, along with the alloy effect, play a crucial role in promoting the ORR performance in acidic media.\u0000</p>","PeriodicalId":713,"journal":{"name":"Nano Research","volume":null,"pages":null},"PeriodicalIF":9.9,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524333","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The fabrication of light-weight, highly impact-resistant, and energy-absorbent materials is urgently demanded in many facets of the society from body armor to aerospace engineering, especially under an extreme environment. Carbon nanotubes (CNTs), one of the strongest and toughest materials ever found, also have good conductivity, chemical stability, and thermal stability, etc, making them a competitive candidate as building blocks to help achieve the above goal. In this work, a kind of CNT network was prepared by using chlorosulfonic acid (CSA) to release the internal stress of super-aligned carbon nanotube films (SA-CNTF) and dendritic polyamide amine (PAMAM) to further introduce multiple hydrogen bonds and interlocking structures. The fabricated bioinspired carbon nanotube network films (PAMAM@C-CNTF) have a high toughness of 45.97 MJ/m3, showing an increase of 420% compared to neat SA-CNTF. More importantly, the anti-impact performance of the films (e.g., with a maximum specific energy absorption of 1.40 MJ/kg under 80–100 m/s projectile impact) is superior to that of conventional protective materials from steel and Kevlar fiber, and also exceeds that of any other reported carbon-based materials. The hierarchical energy dissipation mechanism was further revealed through experiment and simulation. Additional functions including intelligent heating/anti-icing, ultraviolet protection, as well as electromagnetic interference shielding properties make these network films have great potential in practical multi-protection applications, especially under an extreme environment.
{"title":"Fabricating bio-inspired high impact resistance carbon nanotube network films for multi-protection under an extreme environment","authors":"Mingquan Zhu, Kailu Xiao, Wei Zhang, Xudong Lei, Yunxiang Bai, Shijun Wang, Peng Zhang, Feng Gao, Congying Wang, Wenqiang Xu, Huiyong Li, Xianqian Wu, Chao Wang, Hui Zhang, Luqi Liu, Zhong Zhang","doi":"10.1007/s12274-024-6790-3","DOIUrl":"https://doi.org/10.1007/s12274-024-6790-3","url":null,"abstract":"<p>The fabrication of light-weight, highly impact-resistant, and energy-absorbent materials is urgently demanded in many facets of the society from body armor to aerospace engineering, especially under an extreme environment. Carbon nanotubes (CNTs), one of the strongest and toughest materials ever found, also have good conductivity, chemical stability, and thermal stability, etc, making them a competitive candidate as building blocks to help achieve the above goal. In this work, a kind of CNT network was prepared by using chlorosulfonic acid (CSA) to release the internal stress of super-aligned carbon nanotube films (SA-CNTF) and dendritic polyamide amine (PAMAM) to further introduce multiple hydrogen bonds and interlocking structures. The fabricated bioinspired carbon nanotube network films (PAMAM@C-CNTF) have a high toughness of 45.97 MJ/m<sup>3</sup>, showing an increase of 420% compared to neat SA-CNTF. More importantly, the anti-impact performance of the films (e.g., with a maximum specific energy absorption of 1.40 MJ/kg under 80–100 m/s projectile impact) is superior to that of conventional protective materials from steel and Kevlar fiber, and also exceeds that of any other reported carbon-based materials. The hierarchical energy dissipation mechanism was further revealed through experiment and simulation. Additional functions including intelligent heating/anti-icing, ultraviolet protection, as well as electromagnetic interference shielding properties make these network films have great potential in practical multi-protection applications, especially under an extreme environment.\u0000</p>","PeriodicalId":713,"journal":{"name":"Nano Research","volume":null,"pages":null},"PeriodicalIF":9.9,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141531987","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-01DOI: 10.1007/s12274-024-6785-0
Jijie Huang, Yuan Fang, Ping Lu, Juanjuan Lu, Haiyan Wang
Multi-phase vertically aligned nanocomposite (MP-VAN) thin films represent a promising avenue for achieving complex multifunctionality, exploring novel interfacial phenomena, and enabling complex metamaterial designs and exploration. In this study, a novel self-assembled all-oxides three-phase VAN system was conceptualized and fabricated utilizing pulsed laser deposition (PLD) with a single composite target. Detailed microstructural analysis reveals the presence of three distinct phases: LiNbO3, CeO2−x, and LiNbCe1−xOy within the MP-VAN films. Subsequently, ferroelectric, dielectric, optical anisotropy, and magnetic properties were systematically investigated to showcase the multifunctionality inherent in these films. This work presents a pioneering approach to designing and realizing MP-VAN systems, and opens up opportunities for tailoring the complex three-dimensional (3D) physical properties and property coupling of VAN films towards diverse device applications.
多相垂直排列纳米复合材料(MP-VAN)薄膜是实现复杂多功能性、探索新型界面现象以及进行复杂超材料设计和探索的一条大有可为的途径。本研究构思了一种新型自组装全氧化物三相 VAN 系统,并利用脉冲激光沉积(PLD)与单个复合目标进行了制造。详细的微观结构分析表明存在三种不同的相:LiNbO3、CeO2-x 和 LiNbCe1-xOy。随后,对这些薄膜的铁电、介电、光学各向异性和磁性能进行了系统研究,以展示其固有的多功能性。这项研究提出了一种设计和实现 MP-VAN 系统的开创性方法,并为定制 VAN 薄膜的复杂三维(3D)物理特性和特性耦合以实现各种器件应用提供了机会。
{"title":"Self-assembled all-oxides three-phase vertically aligned nanocomposite thin film with multifunctionality","authors":"Jijie Huang, Yuan Fang, Ping Lu, Juanjuan Lu, Haiyan Wang","doi":"10.1007/s12274-024-6785-0","DOIUrl":"https://doi.org/10.1007/s12274-024-6785-0","url":null,"abstract":"<p>Multi-phase vertically aligned nanocomposite (MP-VAN) thin films represent a promising avenue for achieving complex multifunctionality, exploring novel interfacial phenomena, and enabling complex metamaterial designs and exploration. In this study, a novel self-assembled all-oxides three-phase VAN system was conceptualized and fabricated utilizing pulsed laser deposition (PLD) with a single composite target. Detailed microstructural analysis reveals the presence of three distinct phases: LiNbO<sub>3</sub>, CeO<sub>2−<i>x</i></sub>, and LiNbCe<sub>1−<i>x</i></sub>O<sub><i>y</i></sub> within the MP-VAN films. Subsequently, ferroelectric, dielectric, optical anisotropy, and magnetic properties were systematically investigated to showcase the multifunctionality inherent in these films. This work presents a pioneering approach to designing and realizing MP-VAN systems, and opens up opportunities for tailoring the complex three-dimensional (3D) physical properties and property coupling of VAN films towards diverse device applications.\u0000</p>","PeriodicalId":713,"journal":{"name":"Nano Research","volume":null,"pages":null},"PeriodicalIF":9.9,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524341","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
All inorganic metal halide perovskite nanocrystals (NCs) have attracted much attention for their outstanding optoelectronic properties, which can be tuned by the composition, surface, size and morphology in nanoscale. Herein, we report the microfluidic synthesis of hollow CsPbBr3 perovskite NCs through the nanoscale Kirkendall effect. The formation mechanism of the hollow structure (Kirkendall void) controlled by the temperature, flow rate, ratios of precursors and ligands was investigated. Compared with the solid CsPbBr3 NCs of the same size, the hollow CsPbBr3 NCs exhibit blue shifts in ultraviolet–visible (UV–vis) absorption and photoluminescence (PL) spectra, and remarkably longer PL average lifetime (~ 98.2 ns). Quantum confinement effect, inner surface induced additional trap states and lattice strain of the hollow CsPbBr3 NCs were discussed in understanding their unique optoelectronic properties. The hollow CsPbBr3 NC based photodetector exhibits an outstanding negative photoconductivity (NPC) detectivity of 8.9 × 1012 Jones. They also show potentials in perovskite NC based photovoltaic and light emitting diodes (LEDs).
{"title":"Microfluidic synthesis of hollow CsPbBr3 perovskite nanocrystals through the nanoscale Kirkendall effect","authors":"Yue Chen, Xiaoyu Zhang, Jinzhou Jiang, Gaoyu Chen, Kunhong Zhou, Xinwen Zhang, Fajing Li, Caojin Yuan, Jianchun Bao, Xiangxing Xu","doi":"10.1007/s12274-024-6786-z","DOIUrl":"https://doi.org/10.1007/s12274-024-6786-z","url":null,"abstract":"<p>All inorganic metal halide perovskite nanocrystals (NCs) have attracted much attention for their outstanding optoelectronic properties, which can be tuned by the composition, surface, size and morphology in nanoscale. Herein, we report the microfluidic synthesis of hollow CsPbBr<sub>3</sub> perovskite NCs through the nanoscale Kirkendall effect. The formation mechanism of the hollow structure (Kirkendall void) controlled by the temperature, flow rate, ratios of precursors and ligands was investigated. Compared with the solid CsPbBr<sub>3</sub> NCs of the same size, the hollow CsPbBr<sub>3</sub> NCs exhibit blue shifts in ultraviolet–visible (UV–vis) absorption and photoluminescence (PL) spectra, and remarkably longer PL average lifetime (~ 98.2 ns). Quantum confinement effect, inner surface induced additional trap states and lattice strain of the hollow CsPbBr<sub>3</sub> NCs were discussed in understanding their unique optoelectronic properties. The hollow CsPbBr<sub>3</sub> NC based photodetector exhibits an outstanding negative photoconductivity (NPC) detectivity of 8.9 × 10<sup>12</sup> Jones. They also show potentials in perovskite NC based photovoltaic and light emitting diodes (LEDs).\u0000</p>","PeriodicalId":713,"journal":{"name":"Nano Research","volume":null,"pages":null},"PeriodicalIF":9.9,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524338","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-01DOI: 10.1007/s12274-024-6799-7
Pengcheng Liu, Yanyi Liu, Kaili Wang, Shuai Shi, Mengmeng Jin, Jingxiu Liu, Tao Qin, Qian Liu, Xijun Liu, Jia He
Elucidation the relationship between electrode potentials and heterogeneous electrocatalytic reactions has attracted widespread attention. Herein we construct the well-defined Mn single-atom (MnSA) catalyst with four N-coordination through a simple thermal pyrolysis preparation method to investigate the electrode potential micro-environments effect on carbon dioxide reduction reactions (CO2RR) and oxygen reduction reactions (ORR). MnSA catalysts generate higher CO production Faradaic efficiency of exceeding 90% at −0.9 V for CO2RR and higher H2O2 yield from 0.1 to 0.6 V with excellent ORR activity. Density functional theory (DFT) calculations based on constant potential models were performed to study the mechanism of MnSA on CO2RR. The thermodynamic energy barrier of CO2RR is lowest at −0.9 V vs. reversible hydrogen electrode (RHE). Similar DFT calculations on the H2O2 yield of ORR showed that the H2O2 yield at 0.2 V was higher. This study provides a reasonable explanation for the role of electrode potential micro-environments.
阐明电极电位与异质电催化反应之间的关系已引起广泛关注。在此,我们通过简单的热解制备方法,构建了具有四个 N 配位的定义明确的锰单原子(MnSA)催化剂,研究了电极电位微环境对二氧化碳还原反应(CO2RR)和氧气还原反应(ORR)的影响。MnSA 催化剂在 -0.9 V 的 CO2RR 生成 CO 的法拉第效率超过 90%,在 0.1 至 0.6 V 的 H2O2 产率较高,具有优异的 ORR 活性。为了研究 MnSA 在 CO2RR 上的作用机理,我们基于恒定电位模型进行了密度泛函理论(DFT)计算。与可逆氢电极(RHE)相比,CO2RR 的热力学能垒在 -0.9 V 时最低。对 ORR 的 H2O2 产率进行的类似 DFT 计算表明,0.2 V 时的 H2O2 产率较高。这项研究为电极电位微环境的作用提供了合理的解释。
{"title":"Revealing the role of electrode potential micro-environments in single Mn atoms for carbon dioxide and oxygen electrolysis","authors":"Pengcheng Liu, Yanyi Liu, Kaili Wang, Shuai Shi, Mengmeng Jin, Jingxiu Liu, Tao Qin, Qian Liu, Xijun Liu, Jia He","doi":"10.1007/s12274-024-6799-7","DOIUrl":"https://doi.org/10.1007/s12274-024-6799-7","url":null,"abstract":"<p>Elucidation the relationship between electrode potentials and heterogeneous electrocatalytic reactions has attracted widespread attention. Herein we construct the well-defined Mn single-atom (MnSA) catalyst with four N-coordination through a simple thermal pyrolysis preparation method to investigate the electrode potential micro-environments effect on carbon dioxide reduction reactions (CO<sub>2</sub>RR) and oxygen reduction reactions (ORR). MnSA catalysts generate higher CO production Faradaic efficiency of exceeding 90% at −0.9 V for CO<sub>2</sub>RR and higher H<sub>2</sub>O<sub>2</sub> yield from 0.1 to 0.6 V with excellent ORR activity. Density functional theory (DFT) calculations based on constant potential models were performed to study the mechanism of MnSA on CO<sub>2</sub>RR. The thermodynamic energy barrier of CO<sub>2</sub>RR is lowest at −0.9 V vs. reversible hydrogen electrode (RHE). Similar DFT calculations on the H<sub>2</sub>O<sub>2</sub> yield of ORR showed that the H<sub>2</sub>O<sub>2</sub> yield at 0.2 V was higher. This study provides a reasonable explanation for the role of electrode potential micro-environments.\u0000</p>","PeriodicalId":713,"journal":{"name":"Nano Research","volume":null,"pages":null},"PeriodicalIF":9.9,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524339","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-01DOI: 10.1007/s12274-024-6789-9
Ziyang Huang, Zhenghua Wang, Lei Zhou, Jun Pu
Lithium-sulfur (Li-S) batteries hold the potential to revolutionize energy storage due to the high theoretical capacity and energy density. However, the commercialization process is seriously hindered by the rapid capacity decay and low utilization of sulfur, caused by the inevitable slow dynamics and the “shuttle effect”. The incorporation of metal-based electrocatalysts into sulfur cathodes shows promise in promoting the conversion of lithium polysulfides (LiPSs), reducing the “shuttle effect”, and enhancing cell kinetics and cycle life. Among these, Fe-based materials, characterized by environmental friendliness, low cost, abundant reserves, and high activity, are extensively used in sulfur cathode modification. This article reviews the advancements of Fe-based materials in enhancing Li-S batteries in recent years. Starting from single/multi-component Fe-based metal compounds and single/bimetallic atoms, the influence of different Fe coordination environments on the conversion mechanism of LiPSs is analyzed. It is hoped that this review and the proposed prospects can further stimulate the development and application of the Fe element in Li-S batteries in the future.
{"title":"Research progress in performance improvement strategies and sulfur conversion mechanisms of Li-S batteries based on Fe series nanomaterials","authors":"Ziyang Huang, Zhenghua Wang, Lei Zhou, Jun Pu","doi":"10.1007/s12274-024-6789-9","DOIUrl":"https://doi.org/10.1007/s12274-024-6789-9","url":null,"abstract":"<p>Lithium-sulfur (Li-S) batteries hold the potential to revolutionize energy storage due to the high theoretical capacity and energy density. However, the commercialization process is seriously hindered by the rapid capacity decay and low utilization of sulfur, caused by the inevitable slow dynamics and the “shuttle effect”. The incorporation of metal-based electrocatalysts into sulfur cathodes shows promise in promoting the conversion of lithium polysulfides (LiPSs), reducing the “shuttle effect”, and enhancing cell kinetics and cycle life. Among these, Fe-based materials, characterized by environmental friendliness, low cost, abundant reserves, and high activity, are extensively used in sulfur cathode modification. This article reviews the advancements of Fe-based materials in enhancing Li-S batteries in recent years. Starting from single/multi-component Fe-based metal compounds and single/bimetallic atoms, the influence of different Fe coordination environments on the conversion mechanism of LiPSs is analyzed. It is hoped that this review and the proposed prospects can further stimulate the development and application of the Fe element in Li-S batteries in the future.\u0000</p>","PeriodicalId":713,"journal":{"name":"Nano Research","volume":null,"pages":null},"PeriodicalIF":9.9,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524342","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-01DOI: 10.1007/s12274-024-6762-7
Yanming Wang, Junrong Zhang, Tianhua Ren, Meng Xia, Long Fang, Xiangyi Wang, Xingwang Zhang, Kai Zhang, Junyong Wang
Electrical modulation of luminescence is significant to modern light-emitting devices. Monolayer transition metal dichalcogenides are emerging direct-bandgap luminescent materials with unique excitonic properties, and the multiple exciton complexes provide new opportunities to modulate the property of luminescence in atomically thin semiconductors. Here, we report an electrical control of exciton emission in the oscillator strength and spatial distribution of excitons in a monolayer WS2. Effective modulation of excitonic emission intensity with a degree of modulation of ~ 92% has been demonstrated by an electric field at room temperature. The spatial carrier redistribution tuned by a lateral electric field results in distinct excitonic emission patterns by design. The modulation approach to exciton oscillator strength and distribution provides an efficient way to investigate the exciton diffusion dynamics and to construct electrically tunable optoelectronic devices.
{"title":"Electrical control of excitonic oscillator strength and spatial distribution in a monolayer semiconductor","authors":"Yanming Wang, Junrong Zhang, Tianhua Ren, Meng Xia, Long Fang, Xiangyi Wang, Xingwang Zhang, Kai Zhang, Junyong Wang","doi":"10.1007/s12274-024-6762-7","DOIUrl":"https://doi.org/10.1007/s12274-024-6762-7","url":null,"abstract":"<p>Electrical modulation of luminescence is significant to modern light-emitting devices. Monolayer transition metal dichalcogenides are emerging direct-bandgap luminescent materials with unique excitonic properties, and the multiple exciton complexes provide new opportunities to modulate the property of luminescence in atomically thin semiconductors. Here, we report an electrical control of exciton emission in the oscillator strength and spatial distribution of excitons in a monolayer WS<sub>2</sub>. Effective modulation of excitonic emission intensity with a degree of modulation of ~ 92% has been demonstrated by an electric field at room temperature. The spatial carrier redistribution tuned by a lateral electric field results in distinct excitonic emission patterns by design. The modulation approach to exciton oscillator strength and distribution provides an efficient way to investigate the exciton diffusion dynamics and to construct electrically tunable optoelectronic devices.\u0000</p>","PeriodicalId":713,"journal":{"name":"Nano Research","volume":null,"pages":null},"PeriodicalIF":9.9,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141524340","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}