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Light-enhanced osmotic energy generation with an aramid nanofiber membrane 利用芳纶纳米纤维膜进行光增强渗透发电
IF 8.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-12-08 DOI: 10.1038/s41427-023-00507-7
Cheng Chen, Yunxiao Lin, Weiwei Lei, Guoliang Yang, Yuchen Liu, Mao Xu, Xinhao Li, Dan Liu
Osmotic energy generation with reverse electrodialysis through membranes provides a worldwide free energy resource. Photo-driven proton transport in photosynthesis supplies basal energy for plants and living organisms on the planet. Here, we utilized aramid nanofiber (ANF) semiconductor-based membranes to enable light-driven proton transport for osmotic energy generation. Under unilateral illumination, the light-driven proton transport system converted light energy into electrical energy and showed wavelength- and intensity-dependent transmembrane potentials and currents. Interestingly, the synergistic effects of simultaneous illumination and pressure provided a five-fold increase in the voltage and a three-fold increase in the current relative to pressure alone. Density functional theory calculations and spectroscopic measurements demonstrated that the ANF and photoinduced electrons enabled proton transport during illumination and generated a transmembrane potential and current. The light-driven proton transport system supports the development of devices with flexible and stable ANF membranes. Osmotic energy generation, using aramid nanofiber (ANF) semiconductor membranes for light-driven proton transport, displayed wavelength and intensity-dependent potential and current under unilateral illumination. The simultaneous application of illumination and pressure led to a five-fold voltage increase and a three-fold current increase. Density functional theory calculations and spectroscopic measurements confirmed ANF’s role in photoinduced proton transport. This research has significant implications for developing flexible, stable ANF membrane-based energy devices.
通过膜反向电渗析产生的渗透能为全球提供了免费的能源资源。光合作用中的光驱动质子传输为地球上的植物和生物提供基础能源。在这里,我们利用芳纶纳米纤维(ANF)半导体膜实现了光驱动质子传输以产生渗透能。在单侧光照下,光驱动质子传输系统将光能转化为电能,并显示出与波长和强度相关的跨膜电位和电流。有趣的是,在同时光照和压力的协同作用下,电压增加了五倍,电流增加了三倍。密度泛函理论计算和光谱测量表明,ANF 和光诱导电子在光照期间促成了质子转运,并产生了跨膜电位和电流。光驱动质子传输系统有助于开发具有灵活稳定的 ANF 膜的设备。
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引用次数: 0
BaZrO3/MgO-templated epitaxy showing a conductivity increase of three orders of magnitude for the Ba0.95La0.05SnO3 films on Al2O3 substrates, with very high transparency and X-band electromagnetic shielding BaZrO3/ mgo模板外延在Al2O3衬底上的Ba0.95La0.05SnO3薄膜的电导率提高了3个数量级,具有很高的透明度和x波段电磁屏蔽
IF 8.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-12-01 DOI: 10.1038/s41427-023-00512-w
Youngkyoung Ha, Jingyeong Jeon, Subhin Hwang, Judith L. MacManus-Driscoll, Shinbuhm Lee
Transparent conductors with electromagnetic shielding capabilities (TC-EMS) are rare, despite their significant potential for creating new functionalities in energy and military applications. Here, we investigate the potential of La-doped BaSnO3 (BLSO) for TC-EMS since its epitaxial film has been known to have low sheet resistance and high visible transmittance. However, films grown on industrially practical Al2O3 substrates exhibit a sheet resistance three orders of magnitude higher than that of reported films grown on perovskites. Here, this problem is addressed by templating a BaZrO3/MgO bilayer on (0001)-oriented Al2O3 substrates to yield single-crystalline BLSO epitaxial films. The absence of grain boundaries in the epitaxial films minimizes the electron scattering. Due to the affirmative correlation between the conductivity and crystallinity, 5% La doping is optimal among the 5−20% La concentrations studied; these 480-nm-thick films have the highest crystallinity and the lowest sheet resistances of ~28 Ω ▯−1; this value is similar to that of single-crystalline levels. Due to their very high transmittances (~82% in a range 400−1000 nm) and effective X-band electromagnetic shielding (~18.6 dB), the BLSO epitaxial films grown on Al2O3 have great potential to be used for inexpensive TC-EMS applications. Ba0.95La0.05SnO3 epitaxial films grown on (0001)-oriented Al2O3 with a BaZrO3/MgO template bilayer exhibit lower sheet resistance by three orders of magnitude compared with template-free films. These epitaxial films with single-crystalline level properties, including high ultraviolet‒visible transmittance (~82%) and high electromagnetic shielding effectiveness (~18.6 dB at 10 GHz), can be used for the development of stable and inexpensive optoelectronic and energy applications of epitaxial BLSO films grown on Al2O3.
具有电磁屏蔽能力的透明导体(TC-EMS)非常罕见,尽管它们在能源和军事应用中具有创造新功能的巨大潜力。在这里,我们研究了la掺杂BaSnO3 (BLSO)用于TC-EMS的潜力,因为它的外延膜已知具有低片电阻和高可见光透过率。然而,在工业上实际使用的Al2O3衬底上生长的薄膜显示出比在钙钛矿上生长的薄膜高三个数量级的片电阻。本文通过在(0001)取向Al2O3衬底上模板化BaZrO3/MgO双分子层来制备单晶BLSO外延膜。外延薄膜中晶界的缺失使电子散射最小化。由于电导率与结晶度呈正相关关系,在5 ~ 20%的La浓度下,5%的La掺杂效果最佳;这些480 nm厚的薄膜具有最高的结晶度和最低的片电阻~28 Ω −1;这个值与单晶水平相似。由于在Al2O3上生长的BLSO外延膜具有很高的透射率(在400 ~ 1000 nm范围内~82%)和有效的x波段电磁屏蔽(~18.6 dB),因此在廉价的TC-EMS应用中具有很大的潜力。
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引用次数: 0
Triplet-mediated spin entanglement between organic radicals: integrating first principles and open-quantum-system simulations 有机自由基之间的三重态介导自旋纠缠:整合第一原理和开放量子系统模拟
IF 8.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-12-01 DOI: 10.1038/s41427-023-00510-y
Tianhong Huang, Jiawei Chang, Lin Ma, Andrew J. Fisher, Nicholas M. Harrison, Taoyu Zou, Hai Wang, Wei Wu
Controlling molecular spin quantum bits optically offers the potential to effectively reduce decoherence and raise the working temperature of quantum computers. Here, exchange interactions and spin dynamics, as mediated by an optically driven triplet state, are calculated for a molecule that consists of a pair of radicals and represents a potential quantum-circuit building block. Consistent with the previous experimental observation of spin coherence induced by the triplet state, our work demonstrates an optically driven quantum gate operation scheme in a molecule. A technological blueprint combining a two-dimensional molecular network and programmable nanophotonics, both of which are sufficiently developed, is proposed. We thus realize computational exploration of chemical databases to identify suitable candidates for molecular spin quantum bits and couplers to be hybridized with nanophotonic devices. The work presented here is proposed to realize a new approach for exploring molecular excited states and click chemistry, toward advancing molecular quantum technology. Controlling molecular spin quantum bits optically could help us reduce decoherence and raise the working temperature of quantum computing. Here we show theoretically exchange interactions and spin dynamics could be mediated by optically driven triplet state, leading to quantum gate operations. This indicates a great potential for radical as molecular building block for quantum circuits. A molecular quantum architecture, combining molecular network and nano-photonics, was also proposed. We thus expect the computational exploration of chemical database for molecular quantum computing. This work would therefore open up a new direction to use optical instruments and ‘Click Chemistry’ towards molecular quantum technology.
光学控制分子自旋量子比特提供了有效降低退相干和提高量子计算机工作温度的潜力。在这里,交换相互作用和自旋动力学,作为介导的光驱动三重态,计算了一个分子,由一对自由基组成,代表一个潜在的量子电路的构建块。与之前实验观察到的三重态诱导的自旋相干性一致,我们的工作证明了分子中光驱动的量子门操作方案。提出了一种将二维分子网络与可编程纳米光子学相结合的技术蓝图。因此,我们实现了对化学数据库的计算探索,以确定分子自旋量子比特和耦合器与纳米光子器件杂交的合适候选者。本文提出的工作是为了实现探索分子激发态和点击化学的新方法,朝着推进分子量子技术的方向发展。
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引用次数: 0
Rejuvenation engineering in metallic glasses by complementary stress and structure modulation 基于互补应力和结构调制的金属玻璃回春工程
IF 8.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-11-24 DOI: 10.1038/s41427-023-00509-5
Daniel Şopu, Florian Spieckermann, Xilei Bian, Simon Fellner, Jonathan Wright, Megan Cordill, Christoph Gammer, Gang Wang, Mihai Stoica, Jürgen Eckert
Residual stress engineering is widely used in the design of new advanced lightweight materials. For metallic glasses, attention has been given to structural changes and rejuvenation processes. High-energy scanning X-ray diffraction strain mapping reveals large elastic fluctuations in notched metallic glasses after deformation under triaxial compression. Microindentation hardness mapping hints at a competing hardening–softening mechanism after compression and reveals the complementary effects of stress and structure modulation. Transmission electron microscopy proves that structure modulation and elastic heterogeneity distribution under room temperature deformation are related to shear band formation. Molecular dynamics simulations provide an atomistic understanding of the confined deformation mechanism in notched metallic glasses and the related fluctuations in the elastic and plastic strains. Thus, future focus should be given to stress modulation and elastic heterogeneity, which, together with structure modulation, may allow the design of metallic glasses with enhanced ductility and strain-hardening ability. In this work, by involving high-energy scanning X-ray diffraction strain mapping, we identify and distinguish between structural and elastic heterogeneity in the extremely rejuvenated metallic glasses under triaxial compression. Microindentation hardness hints at an unsymmetrical hardening/softening picture and further reveals the complementary effects of stress and structure modulation. Our results suggest that simultaneous stress and structural modulation can be used to enhance rejuvenation beyond the limits known to date, and may therefore aid in the design of MGs with enhanced ductility and strain-hardening capability.
残余应力工程广泛应用于新型先进轻量化材料的设计。对于金属玻璃,人们关注的是结构变化和回春过程。高能扫描x射线衍射应变图揭示了缺口金属玻璃在三轴压缩变形后的弹性波动。微压痕硬度映射提示了压缩后的硬化-软化竞争机制,揭示了应力和结构调节的互补效应。透射电镜证实了室温变形下的结构调制和弹性非均质分布与剪切带的形成有关。分子动力学模拟提供了对缺口金属玻璃的受限变形机制和相关的弹性和塑性应变波动的原子性理解。因此,未来的重点应放在应力调制和弹性非均质性上,它们与结构调制一起,可以设计出具有增强延展性和应变硬化能力的金属玻璃。
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引用次数: 0
Izod impact resistance of 3D printed discontinuous fibrous composites with Bouligand structure 3D打印Bouligand结构不连续纤维复合材料的抗冲击性能
IF 8.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-11-24 DOI: 10.1038/s41427-023-00508-6
Lizhi Guan, Weixiang Peng, Rachel Ng Jing Wen, Jingbo Fan, Hortense Le Ferrand
The Bouligand structure found in the dactyl club of mantis shrimps is known for its impact resistance. However, Bouligand-inspired reinforced composites with 3D shapes and impact resistance characteristics have not yet been demonstrated. Herein, direct ink writing was used to 3D print composites reinforced with glass microfibers assembled into Bouligand structures with controllable pitch angles. The energy absorption levels of the Bouligand composites under impact were found to surpass those of composites with unidirectional microfiber alignment. Additionally, the Bouligand composites with a pitch angle of 40° exhibited a maximum energy absorption of 2.4 kJ/m2, which was 140% higher than that of the unidirectional composites. Furthermore, the characterization of the topography of the fractured surface, supplemented with numerical simulations, revealed a combination of crack twisting and crack bridging mechanisms. Flexural tests conducted on the composites with a pitch angle of 40° revealed that these composites had the strongest properties, including a flexural strength of 36.9 MPa, a stiffness of 2.26 GPa, and energy absorption of 8 kJ/m2. These findings are promising for the microstructural design of engineered composites using direct ink writing for applications in aerospace, transportation, and defense. Inspired by Bouligand structure in the dactyl club of the mantis shrimp, direct ink writing is used to 3D print Bouligand composites reinforced with glass microfibres at controllable pitch angles. The Bouligand composites with a pitch angle of 40˚ exhibited a maximum energy absorption of 2.4 kJ/m2, which was 140 % higher than the unidirectional composites. The topography of the fractured surface supplemented with numerical simulations revealed the combination of crack twisting and crack bridging mechanisms. These findings have implications for the microstructural design of engineered composites using direct ink writing for applications in aerospace, transportation, defense, etc.
在螳螂虾的dactyl俱乐部中发现的Bouligand结构以其抗冲击性而闻名。然而,bouligand启发的具有三维形状和抗冲击特性的增强复合材料尚未得到证实。本文采用直接墨水书写的方法,3D打印由玻璃微纤维增强的复合材料,将其组装成具有可控俯仰角的布利甘结构。结果表明,Bouligand复合材料在冲击作用下的能量吸收水平高于单向超细纤维定向复合材料。此外,当俯仰角为40°时,Bouligand复合材料的最大能量吸收为2.4 kJ/m2,比单向复合材料高140%。此外,通过对裂缝表面形貌的表征和数值模拟,揭示了裂缝扭转和裂缝桥接机制的结合。当俯仰角为40°时,复合材料的抗弯强度为36.9 MPa,刚度为2.26 GPa,吸能为8 kJ/m2,抗弯性能最强。这些发现对于在航空航天、交通运输和国防领域使用直接墨水书写的工程复合材料的微结构设计具有很大的前景。
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引用次数: 0
Two high-pressure superconducting phases in pressurized optical semiconductor GaP 加压光学半导体GaP中的两个高压超导相
IF 8.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-11-10 DOI: 10.1038/s41427-023-00506-8
Nixian Qian, Chunhua Chen, Yonghui Zhou, Shuyang Wang, Liangyu Li, Ranran Zhang, Xiangde Zhu, Yifang Yuan, Xuliang Chen, Chao An, Ying Zhou, Min Zhang, Xiaoping Yang, Zhaorong Yang
Pressure engineering in semiconductors leads to a variety of novel physical phenomena and has recently received considerable attention. Here, we report on pressure-induced superconductivity in III–V gallium phosphide (GaP), a commercially important semiconductor that exhibits excellent optical performance. We show that the emergence of superconductivity is accompanied by the concurrence of piezochromic transition and metallization and can be correlated to a structural transition from the cubic to orthorhombic phase. In line with the structural origin of superconductivity, the critical temperature Tc monotonically decreases with increasing pressure up to ~50 GPa. Moreover, the superconductivity could be preserved toward ambient pressure because of the irreversibility of the structural transition. Nevertheless, the superconducting transition displays evident broadening associated with the presence of amorphization in the depressurized sample. The synchronous evolution of the structural and electronic properties not only shows a vivid structure-property relationship but also could facilitate the exploration of novel functionalities by means of pressure treatment. III-V commercial optical semiconductor GaP crystalizes in either zincblende or wurtzite structure at ambient pressure. Zincblende GaP transforms into orthorhombic phase across a critical pressure during compression, accompanying piezochromic transition, metallization and superconductivity. Upon decompression, superconductivity could be preserved toward ambient pressure and displays broadening features due to amorphization. It reveals the presence of two high-pressure superconducting phases.
半导体领域的压力工程引发了一系列新的物理现象,近年来受到了广泛的关注。在这里,我们报告了III-V磷化镓(GaP)的压力诱导超导性,这是一种具有优异光学性能的重要商业半导体。我们发现超导性的出现伴随着压致变色转变和金属化的同时发生,并且可以与从立方相到正交相的结构转变相关。临界温度随压力的增加而单调降低,直至~50 GPa,这与超导性的结构起源一致。此外,由于结构转变的不可逆性,超导性可以在环境压力下保持。然而,在减压样品中,由于非晶化的存在,超导转变显示出明显的展宽。结构性能和电子性能的同步演变不仅显示了一种生动的结构-性能关系,而且可以通过压力处理促进新功能的探索。
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引用次数: 0
Visualizing the spatial distribution of inflammation in the depressed brain with a targeted MRI nanoprobe in vivo 用靶向MRI纳米探针在体内观察抑郁脑内炎症的空间分布
IF 8.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-10-27 DOI: 10.1038/s41427-023-00505-9
Peisen Zhang, Jiaoqiong Guan, Ni Zhang, Lichong Zhu, Yu Wang, Wenyue Li, Zhe Shi, Xueyuan Liu, Xue Li, Meng Qin, Yi Hou, Yue Lan
Depression is a prevalent mental illness that imposes a substantial public health burden. However, the diverse clinical phenotypes observed in patients make it difficult to realize precise diagnosis. Recently, accumulating preclinical and clinical evidence has suggested that inflammation is involved in the pathophysiology of depression. Herein, a molecular imaging–based strategy was proposed as a means to diagnose depression precisely by specifically visualizing the inflammation status associated with depression. Inflammation-targeting MRI nanoprobes were constructed by attaching an intercellular cell adhesion molecule-1 (ICAM-1)-targeting peptide to biocompatible Fe3O4 nanoparticles. Systematic studies demonstrated that the nanoprobes could specifically target inflamed vascular endothelial cells and visualize the spatial distribution of inflammation in the depressed brain in vivo through susceptibility-weighted imaging (SWI), which was further confirmed by histological analysis. Additionally, these inflammatory brain regions identified by nanoprobe-based imaging are consistent with the focal regions closely associated with the symptoms of depression as reported in previous behavioral studies. Overall, this is the first study to directly visualize the distribution of inflammation in the depressed brain in vivo through a molecular imaging strategy, which may not only facilitate insight into the biological mechanism underlying depression but also provide a potential target within the depressed brain for the further development of anti-inflammatory therapies. A molecular imaging-based strategy was proposed for precise diagnosing the depression through specifically visualizing the inflammation status associated with depressed brain. The inflammation-targeting MRI nanoprobe that can specifically target the inflamed vascular endothelial cells was constructed through attaching the ICAM-1 targeting peptides on biocompatible Fe3O4 nanoparticle. Through nanoprobe-based SWI, the spatial distribution of inflammation in depressed brain can be mapped in vivo. This strategy not only facilitate insight into the biological mechanism underlying depression, but also provide a target within the depressed brain for the further development of anti-inflammatory therapies.
抑郁症是一种普遍存在的精神疾病,对公众健康造成了沉重的负担。然而,患者观察到的临床表型多样,难以实现精确诊断。近年来,越来越多的临床前和临床证据表明,炎症参与了抑郁症的病理生理。本文提出了一种基于分子成像的策略,通过特异性地可视化与抑郁症相关的炎症状态来精确诊断抑郁症。通过将细胞间细胞粘附分子-1 (ICAM-1)靶向肽连接到生物相容性铁3o纳米颗粒上,构建了炎症靶向MRI纳米探针。系统研究表明,纳米探针可以特异性靶向炎症血管内皮细胞,并通过敏感性加权成像(SWI)在体内可视化炎症在抑郁脑中的空间分布,组织学分析进一步证实了这一点。此外,这些由纳米探针成像确定的炎症脑区与先前行为研究中报道的与抑郁症状密切相关的病灶区域一致。总的来说,这是第一个通过分子成像策略直接可视化炎症在抑郁症大脑中的体内分布的研究,这不仅有助于深入了解抑郁症的生物学机制,而且还为进一步开发抗炎疗法提供了抑郁症大脑内的潜在靶点。
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引用次数: 0
All-optical observation of giant spin transparency at the topological insulator BiSbTe1.5Se1.5/Co20Fe60B20 interface 拓扑绝缘体bisbte1.5 . se1.5 /Co20Fe60B20界面巨型自旋透明的全光学观察
IF 8.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-10-20 DOI: 10.1038/s41427-023-00504-w
Suchetana Mukhopadhyay, Pratap Kumar Pal, Subhadeep Manna, Chiranjib Mitra, Anjan Barman
The rise of three-dimensional topological insulators as an attractive playground for the observation and control of various spin-orbit effects has ushered in the field of topological spintronics. To fully exploit their potential as efficient spin-orbit torque generators, it is crucial to investigate the efficiency of spin injection and transport at various topological insulator/ferromagnet interfaces, as characterized by their spin-mixing conductances and interfacial spin transparencies. Here, we use all-optical time-resolved magneto-optical Kerr effect magnetometry to demonstrate efficient room-temperature spin pumping in Sub/BiSbTe1.5Se1.5(BSTS)/Co20Fe60B20(CoFeB)/SiO2 thin films. From the modulation of Gilbert damping with BSTS and CoFeB thicknesses, the spin-mixing conductances of the BSTS/CoFeB interface and the spin diffusion length in BSTS are determined. For BSTS thicknesses far exceeding the spin diffusion length, in the so-called “perfect spin sink” regime, we obtain an interfacial spin transparency as high as 0.9, promoting such systems as scintillating candidates for spin-orbitronic devices. The rise of three-dimensional topological insulators as an attractive playground for the observation and control of various spin-orbit effects has ushered in the field of topological spintronics. To fully exploit their potential as efficient spin-orbit torque generators, investigating the efficiency of spin injection and transport at various topological insulator/ferromagnet interfaces is crucial. Here, using all-optical time-resolved magneto-optical Kerr effect magnetometry, we demonstrate efficient room-temperature spin pumping in Sub/BiSbTe1.5Se1.5(BSTS)/Co20Fe60B20(CoFeB)/SiO2 thin films characterized by the spin-mixing conductances of the interface and the spin diffusion length in BSTS, and obtain an ultrahigh interfacial spin transparency.
三维拓扑绝缘体的兴起为观察和控制各种自旋轨道效应提供了一个有吸引力的平台,从而迎来了拓扑自旋电子学领域的发展。为了充分发挥其作为高效自旋轨道转矩发生器的潜力,研究自旋注入和输运在不同拓扑绝缘体/铁磁体界面上的效率是至关重要的,其特征是自旋混合电导和界面自旋透明度。在这里,我们使用全光时间分辨磁光克尔效应磁强计来证明在Sub/BiSbTe 1.5 Se 1.5 (BSTS)/Co 20 Fe 60 b20 (CoFeB)/ sio2薄膜中有效的室温自旋泵浦。通过BSTS和CoFeB厚度对Gilbert阻尼的调制,确定了BSTS/CoFeB界面的自旋混合电导和BSTS中的自旋扩散长度。当BSTS厚度远远超过自旋扩散长度时,在所谓的“完美自旋汇”机制下,我们获得了高达0.9的界面自旋透明度,促进了该系统成为自旋轨道电子器件的闪烁候点。
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引用次数: 0
Implanting HxYO2−x sites into Ru-doped graphene and oxygen vacancies for low-overpotential alkaline hydrogen evolution 在钌掺杂石墨烯和氧空位中植入HxYO2−x位用于低过电位碱性析氢
IF 8.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-10-20 DOI: 10.1038/s41427-023-00501-z
Xiang Li, Wei Deng, Yun Weng, Jingjing Zhang, Haifang Mao, Tiandong Lu, Wenqian Zhang, Renqiang Yang, Fei Jiang
Highly efficient electrocatalysts for the hydrogen evolution reaction (HER) are essential for sustainable hydrogen energy. The controllable production of hydrogen energy by water decomposition depends heavily on the catalyst, and it is extremely important to seek sustainable and highly efficient water-splitting electrocatalysts for energy applications. Herein, bimetallic RuYO2−x nanoparticles (Ru: 8.84 at.% and Y: 13 at.%) with high densities and low loadings were synthesized and anchored on graphene through a simple solvothermal strategy by synthesizing hydrogen yttrium ketone (HxYO2−x) serving as an inserted medium. Electron microscopy demonstrated that the RuYO2−x/C was composed of densely arranged particles and graphene flakes. Electrochemical results showed that the RuYO2−x/C had a remarkably low overpotential of η10 = 56 mV at a current density of 10 mA cm−2 in alkaline media, a Tafel slope of 63.18 mV dec−1, and 24 h of stability. The oxygen vacancies of RuYO2−x/C provided a large proton storage capacity and a strong tendency to bind hydrogen atoms. DFT calculations showed that RuYO2−x/C catalysts with more Ru-O-Y bonds and VO dramatically decreased the energy barrier for breaking H-OH bonds. Moreover, the robust metal-support interactions provided optimized energies for hydrogen adsorption and desorption, which explained the high activity and favorable kinetics for RuYO2−x/C catalytic hydrogen precipitation in alkaline electrolyte reactions. This work presents a hydrogen insertion method for the preparation of low-loading, high-density, high-performance and stable water decomposition catalysts for hydrogen production. We present a strategy for significantly increasing the H contents on catalysts for the HER in alkaline electrolyte solutions, which were generated by combining ruthenium with HxYO2−x on an oxygen vacancy-rich graphene system. This strategy greatly increased the hydrogen coverage on the RuYO2−x/C catalyst to enhance the HER performance.
高效的析氢反应电催化剂是实现可持续氢能的必要条件。水分解氢能源的可控生产在很大程度上依赖于催化剂,寻求可持续、高效的水分解电催化剂对能源应用至关重要。本文制备了双金属RuYO 2−x纳米粒子(Ru: 8.84 at。通过简单的溶剂热策略,通过合成氢钇酮(H x YO 2 - x)作为插入介质,合成了高密度和低负载的氢钇酮(Y: 13 at.%)并锚定在石墨烯上。电镜观察表明,RuYO 2−x /C由致密排列的颗粒和石墨烯薄片组成。电化学结果表明,在碱性介质中,当电流密度为10 mA cm−2时,RuYO 2−x /C具有较低的过电位η 10 = 56 mV, Tafel斜率为63.18 mV dec−1,稳定时间为24 h。RuYO 2−x /C的氧空位提供了大的质子存储容量和强的结合氢原子的倾向。DFT计算表明,含有较多Ru-O-Y键和vo的RuYO 2−x/ C催化剂显著降低了H-OH键断裂的能垒。此外,强大的金属-载体相互作用为氢的吸附和解吸提供了优化的能量,这解释了在碱性电解质反应中RuYO 2−x /C催化氢沉淀的高活性和良好的动力学。提出了一种低负荷、高密度、高性能、稳定的水分解制氢催化剂的插氢方法。
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引用次数: 0
Rational engineering of high-entropy oxides for Li-ion battery anodes with finely tuned combustion syntheses 精细调节燃烧合成的锂离子电池阳极高熵氧化物的合理工程
IF 8.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-10-13 DOI: 10.1038/s41427-023-00502-y
Dongjoon Shin, Seunghoon Chae, Seonghyun Park, Byungseok Seo, Wonjoon Choi
High-entropy oxides (HEOs) are promising conversion-type anode materials for Li-ion batteries (LIBs) owing to their excellent cycling stabilities and rate capabilities. However, the conventional syntheses and screening processes are time-consuming and complex and require phase and interfacial segregation of individual elements. Herein, we report a rational screening strategy for LIB anodes using precisely tunable HEOs fabricated by one-step combustion syntheses with different fuel-to-oxidizer ratios (φ). A slightly lean fuel mixture (φ-0.95) enabled a suitable temperature and non-reducing atmosphere for optimal HEO syntheses. This provided high crystallinity, perfectly homogeneous elemental distributions, and adequate pore structures without selective precipitation, whereas lower or higher fuel-to-oxidizer ratios resulted in excessively porous morphologies or elemental segregation. HEO-based anodes with φ-0.95 exhibited outstanding specific capacities (1165 mAh g−1, 80.9% retention at 0.1 A g−1, and 791 mAh g−1 even at 3 A g−1), excellent rate capabilities, and stable cycling lifetimes (1252 mAh g−1, 80.9% retention after 100 cycles at 0.2 A g−1). This design strategy will provide fascinating HEO electrodes that cannot be prepared with conventional fabrication methods. Precisely tunable high-entropy oxides (HEO) via controllable one-step combustion within a few seconds offers the rational design capability of optimal phases, structures and configurational entropy. The screened HEO-based anodes exhibit outstanding specific capacity (1165 mAh g−1, 80.9% retention at 0.1 A g−1, and 791 mAh g−1 even at 3 A g−1), excellent rate capability, and stable cycling life (1252 mAh g−1, 80.9% retention after 100 cycles at 0.2 A g−1).
摘要:高熵氧化物(HEOs)具有良好的循环稳定性和倍率性能,是锂离子电池(LIBs)极有前途的转换型负极材料。然而,传统的合成和筛选过程耗时且复杂,并且需要对单个元素进行相分离和界面分离。在此,我们报告了一种合理的筛选策略,使用一步燃烧合成的具有不同燃料-氧化剂比(φ)的精确可调谐HEOs来筛选锂离子电池阳极。稍稀薄的燃料混合物(φ-0.95)为最佳的HEO合成提供了合适的温度和非还原气氛。这提供了高结晶度、完全均匀的元素分布和足够的孔隙结构,没有选择性沉淀,而较低或较高的燃料与氧化剂比会导致过度多孔形态或元素偏析。φ-0.95的heo基阳极具有出色的比容量(1165 mAh g−1,在0.1 A g−1下保持80.9%,在3 A g−1下保持791 mAh g−1),优异的倍率能力和稳定的循环寿命(1252 mAh g−1,在0.2 A g−1下循环100次后保持80.9%)。这种设计策略将提供传统制造方法无法制备的令人着迷的HEO电极。
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