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A low-melting-point metal doping strategy for the synthesis of small-sized intermetallic Pt5Ce fuel cell catalysts 合成小尺寸金属间 Pt5Ce 燃料电池催化剂的低熔点金属掺杂策略
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-05 DOI: 10.1007/s12274-024-6800-5
Zi-Jun Zou, Shi-Yi Yin, Yao Tang, Sheng-Liang Zhong, Lei Wang, Shi-Long Xu, Hai-Wei Liang

Carbon-supported platinum-lanthanum (Pt-Ln) intermetallic compound (IMC) nanoparticles with high activity and robust stability have been demonstrated as promising cathode catalysts for proton-exchange membrane fuel cells. However, the preparation of Pt-Ln IMC catalysts needs high-temperature annealing treatment that inevitably causes nanoparticle sintering, resulting in significant reduction of the electrochemical surface area and mass-based activity. Here, we prepare small-sized M-doped Pt5Ce (M = Ga, Cd, and Sb) IMCs catalysts via a low-melting-point metal doping strategy. We speculate that the doping of low-melting-point metals can facilitate the generation of vacancies in the crystal lattice through thermal activation and thus reduce the kinetic barriers for the formation of intermetallic Pt5Ce catalysts. The prepared Ga-doped Pt5Ce catalyst exhibits a higher electrochemical active surface area (81 m2·gPt−1) and a larger mass activity (0.45 A·mgPt−1 at 0.9 V) over the undoped Pt5Ce and commercial Pt/C catalysts. In the membrane electrode assembly test, the Ga-doped Pt5Ce cathode delivers a power density of 0.98 W·cm−2 at 0.67 V, along with a voltage loss of only 27 mV at 0.8 A·cm−2 at the end of accelerated stability test.

碳支撑铂-镧(Pt-Ln)金属间化合物(IMC)纳米粒子具有高活性和强大的稳定性,已被证明可作为质子交换膜燃料电池的阴极催化剂。然而,Pt-Ln IMC 催化剂的制备需要高温退火处理,这不可避免地会导致纳米颗粒烧结,从而显著降低电化学表面积和质量活性。在此,我们通过低熔点金属掺杂策略制备了小尺寸的 M 掺杂 Pt5Ce(M = Ga、Cd 和 Sb)IMCs 催化剂。我们推测,掺杂低熔点金属可通过热活化促进晶格中空位的产生,从而降低金属间 Pt5Ce 催化剂形成的动力学障碍。与未掺杂的 Pt5Ce 和商用 Pt/C 催化剂相比,制备的掺镓 Pt5Ce 催化剂具有更高的电化学活性表面积(81 m2-gPt-1)和更大的质量活性(0.9 V 时为 0.45 A-mgPt-1)。在膜电极组装测试中,掺杂 Ga 的 Pt5Ce 阴极在 0.67 V 时的功率密度为 0.98 W-cm-2,在加速稳定性测试结束时,0.8 A-cm-2 的电压损失仅为 27 mV。
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引用次数: 0
Skin-inspired interface modification strategy toward a structure-function integrated hybrid smart fabric system with self-powered sensing property for versatile applications 受皮肤启发的界面改性策略,实现具有自供电传感特性的结构-功能一体化混合智能织物系统的多功能应用
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-04 DOI: 10.1007/s12274-024-6806-z
Xiang Cheng, Teng Chen, De Gong, Pengcheng Ma, Bo Chen, Jun Cai

Fabric-based composites with superior mechanical properties and excellent perceptive function are highly desirable. However, it remains a huge challenge to attain structure-function integration, especially for hybrid fabric composites. Herein, a skin-inspired interface modification strategy is proposed toward this target by constructing a hybrid smart fabric system consisting of two types of smart fabrics: carbon nanotube (CNT)/MXene-modified aramid fabrics and zinc oxide nanorod (ZnO NR)-modified carbon fabrics. Based on that, flexible piezoelectric pressure sensors with skin-like hierarchical perception interfaces are fabricated, which demonstrate superb sensitivity of 2.39 V·kPa-1 and are capable of various wearable monitoring tasks. Besides, the interface-modified hybrid fabric reinforced plastics can also be fabricated, which are proven to possess 13.6% higher tensile strength, 10.1% elastic modulus. More impressively, their average energy absorption can be improved by 111.9%, accompanied with inherent damage alert capability. This offers a paradigm to fabricate structure-function integrated hybrid smart fabric composites for the smart clothing and intelligent aerial vehicles.

具有优异机械性能和卓越感知功能的织物基复合材料非常受欢迎。然而,要实现结构与功能的一体化,尤其是混合织物复合材料的一体化,仍然是一个巨大的挑战。本文针对这一目标提出了一种受皮肤启发的界面改性策略,构建了一种混合智能织物系统,该系统由两种类型的智能织物组成:碳纳米管(CNT)/MXene 改性芳纶织物和氧化锌纳米棒(ZnO NR)改性碳织物。在此基础上,制备出具有类皮肤分层感知界面的柔性压电压力传感器,其灵敏度高达 2.39 V-kPa-1,能够胜任各种可穿戴监测任务。此外,还制作出了界面改性混合织物增强塑料,其拉伸强度提高了 13.6%,弹性模量提高了 10.1%。更令人印象深刻的是,它们的平均能量吸收能力提高了 111.9%,同时还具有固有的损伤预警能力。这为制造用于智能服装和智能飞行器的结构-功能一体化混合智能织物复合材料提供了范例。
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引用次数: 0
Observation of the failure mechanism in Ag10Ge15Te75-based memristor induced by ion transport 观察基于 Ag10Ge15Te75 的忆阻器在离子传输诱导下的失效机制
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-03 DOI: 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.

基于固态电解质的忆阻器在逻辑和神经形态应用的下一代非易失性存储器方面引起了极大关注。然而,它们在性能上遇到了多变性的挑战,这些挑战源于随机离子传输和导电丝的形成。显然,与离子传输相关的电化学金属化机制已被阐明。然而,离子传输在循环过程中导致的失效机制却鲜有报道。下面,我们将通过原位电流-电压测量结合原位透射电子显微镜特性,阐明银/银10Ge15Te75/W记忆晶闸管失效的五个阶段。我们的研究发现,银离子的迁移和富集导致了 Ag2Te 的沉淀。Ag2Te 的形成阻碍了器件保持其双极特性的能力,同时也降低了高阻态的电阻值,从而降低了器件的开关比。这些令人鼓舞的结果为未来高性能忆阻器的结构设计和离子传输操纵提供了重要指导。
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引用次数: 0
Facile synthesis of intra-nanogap enhanced Raman tags with different shapes 轻松合成不同形状的纳米间隙内增强拉曼标签
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-02 DOI: 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.

质子纳米结构中的热点工程在用于生物分析和细胞成像的表面增强拉曼散射(SERS)中发挥着重要作用。然而,由于周围化学物质的潜在干扰以及将 SERS 活性分析物定位到热点区域,要产生稳定、可重现和强烈的 SERS 信号仍然具有挑战性。在此,我们开发了一种简单直接的方法来合成间隙内纳米粒子,在这些间隙内封装 4-硝基苯硫醇(4-NBT)作为报告分子,以避免外界干扰。我们以纳米棒、双锥体和纳米球为核心制备了三种间隙内纳米粒子,其中以纳米棒为核心的间隙内纳米粒子具有最高的 SERS 活性。我们的方法的优点是容易制备高产且稳定的间隙内纳米粒子,其特点是与 4-NBT 的孵育时间短(10 分钟),合成速度快,无需额外的离心步骤来纯化核心纳米粒子。这些等离子体间隙纳米结构的合成热点具有强烈的局部场,很有希望作为 SERS 基底用于广泛的定量光学应用。
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引用次数: 0
Porous block copolymer films with self-adjustable optical transmittance and passive radiative cooling 具有自动调节透光率和被动辐射冷却功能的多孔嵌段共聚物薄膜
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-02 DOI: 10.1007/s12274-024-6778-z
Xue Meng, Weiming Tang, Shuyun Zhuo, Jince Zhao, Zixuan Ren, Zhonghe Sun, Hao Yan, Tianyi Zhao, Ziguang Zhao, Mingjie Liu

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.

作为一种无能源冷却技术,辐射冷却在节能领域备受关注。然而,传统的辐射冷却薄膜通常具有静态光学特性,其固有的不透明性限制了其在窗户等建筑中的应用。因此,人们需要可调节透射率的被动式辐射冷却薄膜。在此,我们报告了具有自动调节光学透过率和被动辐射冷却功能的多孔嵌段共聚物薄膜。结果表明,该薄膜的太阳反射率(0.3-2.5 微米)高达 96.9%,红外发射率(8-13 微米)高达 97.9%。室外实验表明,薄膜表面温度比环境温度低 6.6 °C,制冷功率为 104.8 W-m-2。此外,还可以通过改变后处理溶剂的极性来调节薄膜的透射率,为调节室内光照强度和热平衡提供了一种有效方法,从而提高了辐射制冷的适用性。
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引用次数: 0
Boosting oxygen reduction in acidic media through integration of Pt-Co alloy effect and strong interaction with carbon defects 通过整合铂钴合金效应和与碳缺陷的强相互作用,促进酸性介质中的氧气还原
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-02 DOI: 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}
引用次数: 0
Fabricating bio-inspired high impact resistance carbon nanotube network films for multi-protection under an extreme environment 制作生物启发的高抗冲击性碳纳米管网络薄膜,实现极端环境下的多重保护
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-02 DOI: 10.1007/s12274-024-6790-3
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

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.

从人体装甲到航空航天工程,特别是在极端环境下,社会的许多方面都迫切需要制造重量轻、抗冲击性强和吸能的材料。碳纳米管(CNT)是迄今为止发现的最坚固、最坚韧的材料之一,同时还具有良好的导电性、化学稳定性和热稳定性等特点,因此是实现上述目标的理想构件。在这项工作中,利用氯磺酸(CSA)释放超对齐碳纳米管薄膜(SA-CNTF)的内应力,并利用树枝状聚酰胺胺(PAMAM)进一步引入多重氢键和连锁结构,制备了一种碳纳米管网络。制成的生物启发碳纳米管网络薄膜(PAMAM@C-CNTF)具有 45.97 MJ/m3 的高韧性,与纯 SA-CNTF 相比提高了 420%。更重要的是,薄膜的抗冲击性能(例如,在 80-100 m/s 的弹丸冲击下,最大比能量吸收为 1.40 MJ/kg)优于传统的钢和凯夫拉纤维防护材料,也超过了其他任何已报道的碳基材料。通过实验和模拟,进一步揭示了分层消能机制。智能加热/防结冰、紫外线防护以及电磁干扰屏蔽等附加功能使这些网络薄膜在实际的多重防护应用中具有巨大潜力,尤其是在极端环境下。
{"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}
引用次数: 0
Self-assembled all-oxides three-phase vertically aligned nanocomposite thin film with multifunctionality 具有多功能性的自组装全氧化物三相垂直排列纳米复合薄膜
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-01 DOI: 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。
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引用次数: 0
Microfluidic synthesis of hollow CsPbBr3 perovskite nanocrystals through the nanoscale Kirkendall effect 通过纳米级 Kirkendall 效应微流体合成空心 CsPbBr3 包晶石纳米晶体
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-01 DOI: 10.1007/s12274-024-6786-z
Yue Chen, Xiaoyu Zhang, Jinzhou Jiang, Gaoyu Chen, Kunhong Zhou, Xinwen Zhang, Fajing Li, Caojin Yuan, Jianchun Bao, Xiangxing Xu

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).

所有无机金属卤化物透辉石纳米晶体(NCs)都因其卓越的光电特性而备受关注,这些特性可以通过纳米尺度的成分、表面、尺寸和形貌进行调节。在此,我们报告了通过纳米级 Kirkendall 效应微流体合成空心 CsPbBr3 包晶石 NC 的过程。我们研究了由温度、流速、前驱体和配体的比例控制的空心结构(Kirkendall空隙)的形成机理。与相同尺寸的实心 CsPbBr3 NCs 相比,空心 CsPbBr3 NCs 在紫外可见吸收和光致发光光谱中表现出蓝色偏移,并且显著延长了光致发光平均寿命(约 98.2 ns)。讨论了量子约束效应、内表面诱导的附加陷阱态以及空心 CsPbBr3 NCs 的晶格应变,以了解其独特的光电特性。基于 CsPbBr3 NC 的空心光电探测器表现出了出色的负光电导(NPC)检测率(8.9 × 1012 琼斯)。它们还显示了基于过氧化物 NC 的光伏和发光二极管 (LED) 的潜力。
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引用次数: 0
Revealing the role of electrode potential micro-environments in single Mn atoms for carbon dioxide and oxygen electrolysis 揭示单个锰原子在二氧化碳和氧气电解中的电极电位微环境作用
IF 9.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-01 DOI: 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}
引用次数: 0
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