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High-Entropy Materials in Focus 聚焦高熵材料
IF 9.6 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-01 DOI: 10.1021/acsmaterialslett.4c01060
Yuyin Li, Zhengtang Luo*, Sara E. Skrabalak* and Yujie Xiong*, 
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引用次数: 0
Advances in Quantum Dot Direct Photolithographic Patterning 量子点直接光刻图案技术的进展
IF 9.6 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-06-21 DOI: 10.1021/acsmaterialslett.4c00762
Yanyan Qiu, Yixin Yu, Shanshan Wang and Menglu Chen*, 

Quantum Dots (QDs) with unique electrical and optical properties have wide applications on patterned or pixelated devices such as display devices, integrated photoelectric devices, etc. However, conventional patterning methods have some obvious drawbacks such as complex processing, blurred film boundaries, and degradation on the photophysical properties. Recently, direct photolithographic patterning has appeared as a novel strategy to realize high-resolution patterning solids and high-performance patterned devices. In this review, we summarize the research progress on the direct photolithographic patterning on QDs as well as their applications. We also discuss the current challenges and future development in this field.

量子点(QDs)具有独特的电学和光学特性,可广泛应用于图案化或像素化设备,如显示设备、集成光电设备等。然而,传统的图案化方法存在一些明显的缺点,如加工过程复杂、薄膜边界模糊、光物理性能下降等。最近,直接光刻图案化作为一种新策略出现了,它可以实现高分辨率图案化固体和高性能图案化器件。在这篇综述中,我们总结了在 QDs 上直接光刻图案化的研究进展及其应用。我们还讨论了该领域当前面临的挑战和未来的发展。
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引用次数: 0
Emerging Electrocatalytic Textile Electrodes for Highly Efficient Alkaline Water Electrolysis 用于高效碱性水电解的新兴电催化纺织电极
IF 9.6 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-06-20 DOI: 10.1021/acsmaterialslett.4c00659
Jeongmin Mo, Wondo Choi, Hyaemin Kim, Jaesung Lyu, Cheong Hoon Kwon, Dongsoo Yang* and Jinhan Cho*, 

Alkaline water electrolysis using non-noble electrocatalysts represents a sustainable method of hydrogen production, but optimizing/maximizing its performance still remains a challenge. While extensive research has focused mainly on the synthesis and design of electrocatalysts, less attention has been given to the structural and interfacial design of electrodes, which critically affects the water-splitting performance. Of particular importance is the interfacial controlled host electrode, which serves as a uniform electrocatalyst reservoir through interfacial interactions and a highly conductive current collector. Its porous structure, in addition to electrocatalyst size and host-electrocatalyst interface, significantly influences the total active surface area and operational stability. Here, we review recent advances in alkaline water electrolysis, highlighting the crucial role of interfacial interactions between host electrode and electrocatalysts, and among adjacent electrocatalysts, as well as the structural design of host electrode. Additionally, we explain how these interactions significantly contribute to operational stability. Commercialization challenges are also discussed.

使用非贵金属电催化剂进行碱性水电解是一种可持续的制氢方法,但优化/最大化其性能仍然是一项挑战。虽然大量研究主要集中在电催化剂的合成和设计上,但对电极的结构和界面设计关注较少,而这对水分离性能有着至关重要的影响。其中尤为重要的是界面控制主机电极,它通过界面相互作用成为均匀的电催化剂贮存器和高导电性集流器。除了电催化剂的尺寸和宿主-电催化剂界面外,其多孔结构也对总活性表面积和运行稳定性产生重大影响。在此,我们回顾了碱性水电解的最新进展,强调了宿主电极与电催化剂之间、相邻电催化剂之间的界面相互作用以及宿主电极结构设计的关键作用。此外,我们还解释了这些相互作用如何显著提高运行稳定性。我们还讨论了商业化所面临的挑战。
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引用次数: 0
Homochiral and Heterochiral Cation Mixing in 2D Perovskites for Enhanced Structural Asymmetry and Spin Splitting 二维过氧化物中的同手性和异手性阳离子混合,以增强结构不对称和自旋分裂能力
IF 9.6 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-06-20 DOI: 10.1021/acsmaterialslett.4c00558
Yi Xie, Heshan Hewa-Walpitage, Jack Morgenstein, Volker Blum, Zeev Valy Vardeny and David B. Mitzi*, 

Overcoming the constraints of single-cation phases and further enhancing structural asymmetry represent critical objectives for optimizing emergent optoelectronic and spin-related properties in two-dimensional (2D) hybrid organic–inorganic perovskites (HOIPs). Here, we demonstrate homochiral (S/S) and heterochiral (R/S) cation mixing in 2D HOIPs via a 1:1 mixing of S- and R-4-bromo-α-methylbenzylammonium with S-1-methylhexyammonium. The R/S system achieves an enhanced structural asymmetry, marked by a significant Pb–I–Pb bond angle disparity (Δβ = 9.24°), attributed to the distinctive asymmetric templating effects from mixed cations with distinct molecular structures and opposite absolute configurations. Consequently, spin–orbit-coupled hybrid density functional theory (DFT) calculations indicate a substantial spin splitting (ΔE = 78.5 meV), among the largest reported for PbI42–-based 2D HOIPs. Nonequivalent chiral information from homo- and heterochiral mixing further modulates the Cotton effect for the same elemental composition. Our study demonstrates an important materials design strategy for enhancing structural asymmetry and advancing symmetry-breaking-reliant properties in organic–inorganic hybrids.

克服单阳离子相的限制并进一步提高结构的不对称性是优化二维(2D)有机-无机混合包晶石(HOIPs)的新兴光电和自旋相关特性的关键目标。在这里,我们通过 S- 和 R-4-bromo-α-methylbenzylammonium 与 S-1-methylhexyammonium 的 1:1 混合,展示了二维 HOIPs 中的同手性(S/S)和异手性(R/S)阳离子混合。R/S 体系的结构不对称性增强,表现为显著的 Pb-I-Pb 键角差异(Δβ = 9.24°),这归因于具有不同分子结构和相反绝对构型的混合阳离子所产生的独特的不对称模板效应。因此,自旋轨道耦合混合密度泛函理论(DFT)计算表明存在大量的自旋分裂(ΔE = 78.5 meV),是已报道的基于 PbI42 的二维 HOIPs 中最大的自旋分裂之一。同手性和异手性混合产生的非等价手性信息进一步调节了相同元素组成的科顿效应。我们的研究展示了一种重要的材料设计策略,可用于增强有机-无机杂化物的结构不对称性和提高依赖对称性的特性。
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引用次数: 0
Ultrastretchable Transparent Electrodes of Liquid Metal Serpentine Micromeshes 液态金属蛇形微针的超拉伸透明电极
IF 9.6 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-06-20 DOI: 10.1021/acsmaterialslett.4c00385
Cheng Yang, Xiaohui Ma, Xinyuan Zhou, Yong Lin, Weixi Huang, Xing Chen, Qian Wang, Qianying Lu, Yurui Xu, Xinghai Ning* and Desheng Kong*, 

Stretchable transparent electrodes are crucial components for deformable electronics. While solid-state electrodes struggle to achieve significant stretchability, liquid metal electrodes have emerged as a potential alternative. However, their widespread application has been limited by their complex fabrication and reduced performance when stretched. This study introduces stretchable transparent electrodes composed of liquid metal in serpentine micromesh patterns. These electrodes are constructed cost-effectively to show high optical transmittance and low sheet resistance. They can endure 800% strain with limited variations in resistance due to the serpentine design. A transparent proximity and touch sensor is combined with soft pneumatic actuators to enable a deformable haptic interface. Additionally, transparent heaters are prepared to conform to the curvilinear body surface, allowing for thermotherapy on subcutaneous tumors while concurrently monitoring the skin’s responses. Liquid metal serpentine micromeshes represent promising transparent electrodes for stretchable devices and systems.

可拉伸透明电极是可变形电子器件的关键部件。固态电极难以实现显著的可拉伸性,而液态金属电极则成为一种潜在的替代品。然而,由于其复杂的制造工艺和拉伸后的性能降低,其广泛应用受到了限制。本研究介绍了由蛇形微网状液态金属组成的可拉伸透明电极。这些电极的制造成本低,具有高光学透射率和低薄层电阻。由于采用了蛇形设计,它们可以承受 800% 的应变,而电阻变化有限。透明的接近和触摸传感器与软气动致动器相结合,实现了可变形的触觉界面。此外,还准备了透明加热器,以适应曲线体表,从而可以对皮下肿瘤进行热疗,同时监测皮肤的反应。液态金属蛇形微米是用于可拉伸设备和系统的前景广阔的透明电极。
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引用次数: 0
Challenges in Electrolyzer Performance Evaluation for Green Hydrogen Production 绿色制氢电解槽性能评估面临的挑战
IF 9.6 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-06-20 DOI: 10.1021/acsmaterialslett.4c00690
Seok-Jin Kim, Javeed Mahmood, Phil Woong Kang, Zhonghua Xue and Cafer T. Yavuz*, 

The transition to sustainable energy increasingly relies on hydrogen gas produced by water electrolysis. Current performance metrics for electrolyzers, typically measured in megawatts or kilowatts, inadequately capture the full scope of the system efficiency and hydrogen output rates. The gap between academic and industrial evaluations can distort the perceived effectiveness of these technologies. This Perspective proposes a refined dual-metric evaluation system that integrates both energy efficiency (kWh/kg H2) and production rate (Nm3/h) to provide a balanced view of performance. A standardized framework similar to that for photovoltaic technologies is suggested to enable transparent comparisons and support advancements in electrolyzer design. Emphasizing the need for consistent testing conditions, the framework aims to ensure that the evaluations of the electrodes, stacks, and overall systems remain reliable across various operational scenarios. Adopting such a comprehensive evaluation approach is essential for accurately communicating the capabilities of water electrolyzers and propelling the widespread use of green hydrogen.

向可持续能源的过渡越来越依赖于水电解产生的氢气。目前电解槽的性能指标通常以兆瓦或千瓦为单位,不足以全面反映系统效率和氢气产出率。学术评估与工业评估之间的差距会扭曲这些技术的预期效果。本视角提出了一套完善的双指标评估系统,该系统综合了能效(千瓦时/千克氢气)和产出率(Nm3/h),以提供一个平衡的性能视角。建议采用与光伏技术类似的标准化框架,以便进行透明的比较,支持电解槽设计的进步。该框架强调需要一致的测试条件,旨在确保电极、堆栈和整体系统的评估在各种运行情况下都能保持可靠。采用这种全面的评估方法对于准确宣传水电解槽的能力和推动绿色氢气的广泛使用至关重要。
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引用次数: 0
From Theory to Practice: A Critical and Comparative Assessment of Tafel Slope Analysis Techniques in Electrocatalytic Water Splitting 从理论到实践:电催化水分离中塔菲尔斜率分析技术的批判性比较评估
IF 9.6 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-06-20 DOI: 10.1021/acsmaterialslett.4c00831
Suprobhat Singha Roy, Ragunath Madhu, Arun Karmakar and Subrata Kundu*, 

Water splitting for clean hydrogen production is gaining popularity, driving researchers to develop efficient electrocatalysts with minimal energy input, reduced overpotentials, lower Tafel slopes, and enhanced stability. The Tafel slope is an important kinetic parameter to assess an electrocatalyst’s performance. Hence, an accurate determination of the Tafel slope experimentally using appropriate techniques, along with knowledge of multielectron transfer reactions’ kinetics, is of utmost importance. For such reactions, identifying whether the rate-determining step involves an electron transfer or chemical transformation is a key factor. The Tafel slope provides insight into this, revealing the exact equilibrium and mechanism of the reaction. This Perspective explores the theoretical background of the Tafel slope and current experimental techniques for its accurate determination. It discusses the pros and cons of each technique, providing step-by-step guidance for precise Tafel slope calculation, which is essential for assessing electrocatalyst performance in water splitting reactions.

用于清洁制氢的水分离技术越来越受欢迎,这促使研究人员开发能量输入最小、过电位降低、塔菲尔斜率较低和稳定性增强的高效电催化剂。塔菲尔斜率是评估电催化剂性能的一个重要动力学参数。因此,利用适当的技术和多电子转移反应动力学知识,通过实验准确测定塔菲尔斜率至关重要。对于此类反应,确定决定速率的步骤是电子转移还是化学转化是一个关键因素。塔菲尔斜率可以揭示反应的确切平衡和机理。本视角探讨了塔菲尔斜率的理论背景以及当前准确测定塔菲尔斜率的实验技术。它讨论了每种技术的优缺点,为精确计算塔菲尔斜率提供了逐步指导,这对于评估电催化剂在水分离反应中的性能至关重要。
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引用次数: 0
Advancing the Development of Hollow Micro/nanostructured Materials for Electrocatalytic Water Splitting: Current State, Challenges, and Perspectives 推进用于电催化水分离的中空微/纳米结构材料的开发:现状、挑战和前景
IF 9.6 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-06-19 DOI: 10.1021/acsmaterialslett.4c00777
Muhammad Asim Mushtaq, Muhammad Ahmad, Attia Shaheen, Andleeb Mehmood, Ghulam Yasin, Muhammad Arif, Zahid Ali, Pengyan Li, Sumaira Nazar Hussain, Mohammad Tabish, Anuj Kumar, Saira Ajmal, Waseem Raza, Mansoor Akhtar, Ali Saad and Dongpeng Yan*, 

Electrocatalytic water splitting is commonly regarded as a sustainable and clean method to generate hydrogen and oxygen, which is deemed to be efficient for the utilization of renewable energy. Electrocatalysts are essential components to enhance electrochemical efficiency and optimize product yield. Hollow micro/nanostructures possess large specific surface areas, multiple voids, and tunable chemical compositions, making them suitable for use as direct catalysts or as supports for electrochemical reactions. This review summarizes recent advancements in structural and functional designs of micro/nanostructured hollow materials as electrocatalysts for an enhanced water-splitting process. We emphasize ideas and strategies to create various hollow electrocatalysts for oxygen/hydrogen evolution processes. Subsequently, a comprehensive summary of recent studies on hollow borides, carbides, oxides, phosphides, selenides, sulfides, alloys, MXenes, and various heterostructured electrocatalysts containing hollow hosts is provided. Furthermore, we highlight the current challenges and perspectives of hollow micro/nanostructures for electrocatalytic water splitting.

电催化水分裂通常被认为是产生氢气和氧气的一种可持续和清洁的方法,被认为是利用可再生能源的有效方法。电催化剂是提高电化学效率和优化产品产量的重要组成部分。中空微/纳米结构具有大比表面积、多空隙和可调整的化学成分,因此适合用作直接催化剂或电化学反应的支持物。本综述总结了作为电催化剂的微/纳米空心结构材料在结构和功能设计方面的最新进展,以增强水分离过程。我们强调了为氧/氢进化过程创造各种中空电催化剂的想法和策略。随后,我们全面总结了近期有关空心硼化物、碳化物、氧化物、磷化物、硒化物、硫化物、合金、MXenes 以及各种含有空心主机的异质结构电催化剂的研究。此外,我们还重点介绍了中空微/纳米结构在电催化水分离方面目前面临的挑战和前景。
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引用次数: 0
Recent Progress and Challenges in Hybrid Water Electrolysis through Economic Evaluation 通过经济评估了解混合水电解的最新进展和挑战
IF 9.6 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-06-18 DOI: 10.1021/acsmaterialslett.4c00676
Hyogyun Roh, Sehun Oh, Changhyun Lim and Kijung Yong*, 

Water electrolysis is a sustainable method of hydrogen production with low levels of CO2 emissions. However, the problem of high economic costs must be resolved. Hybrid water electrolysis (HWE), derived by replacing the sluggish oxygen evolution reaction, emerges as an alternative method to reduce power consumption. Recent studies on HWEs have focused on reporting cell potential reductions, but their impact on hydrogen production costs is still unclear. In this paper, power consumption and levelized cost of hydrogen (LCOH) were evaluated to understand the economic impact of HWEs. Among various HWEs, HzOR showed an excellent energy consumption reduction (43.3 kWh/kg) resulting in the lowest LCOH ($1.92 kg–1). These results prove one of the most effective alternatives to water electrolysis in its current state. Although other HWEs show only small reductions in energy consumption and LCOH in their current state, these reactions still show high potential to reduce energy consumption and LCOH.

水电解是一种二氧化碳排放量低的可持续制氢方法。然而,必须解决经济成本高的问题。混合水电解法(HWE)取代了缓慢的氧进化反应,成为降低功耗的替代方法。最近关于混合水电解的研究主要集中在报告电池电位的降低,但其对制氢成本的影响仍不明确。本文对耗电量和氢气平准化成本(LCOH)进行了评估,以了解 HWEs 的经济影响。在各种 HWEs 中,HzOR 的能耗降低效果极佳(43.3 kWh/kg),其 LCOH 也最低(1.92 美元 kg-1)。这些结果证明,HzOR 是目前电解水最有效的替代方法之一。尽管其他 HWE 在目前的状态下只能减少少量的能耗和 LCOH,但这些反应仍然显示出减少能耗和 LCOH 的巨大潜力。
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引用次数: 0
Highly Selective Separation of Benzene/Cyclohexane by Three-Dimensional Covalent Organic Framework with 8,8-Connected bcu Net Topology 利用具有 8,8 连接 bcu 网拓扑结构的三维共价有机框架实现苯/环己烷的高选择性分离
IF 9.6 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-06-18 DOI: 10.1021/acsmaterialslett.4c00756
Yu Zhao, Tsukasa Irie, Dan Wen, Haruna Mabuchi, Kohki Sasaki, Mika Nozaki, Rina Tomioka, Weidong Zhu, Saikat Das*, Teng Ben* and Yuichi Negishi*, 

Here, we report the discovery of the first (8,8)-connected three-dimensional (3D) covalent organic framework (COF), TUS-88, having bcu topology by linking an 8-connected D4h-symmetric quadrangular prism node to an 8-connected D2h-symmetric tetragonal prism node. Derived from the π-aromatic conjugated system of pyrene and the abundant aromatic phenyl rings composing the COF scaffold, which promotes stronger π···π interactions with aromatic benzene (Bz) molecules, a superlative Bz uptake of 464 cm3 g–1 was achieved for TUS-88, coupled with exemplary cyclohexane (Cy) uptake of 224 cm3 g–1 and ideal Bz/Cy selectivity of 2.07 which are the current benchmark. Breakthrough experiments accomplished using a Bz/Cy (1:1, v/v) mixture corroborated the preferential adsorption of Bz by the COF from the mixture to generate high-purity Cy with a significant time interval of 75.4 min g–1 and a record-setting Bz/Cy breakthrough selectivity of 2.46.

在这里,我们报告了发现的首个 (8,8) 连接的三维共价有机框架 (COF)--TUS-88,它通过将一个 8 连接的 D4h 对称四棱柱节点连接到一个 8 连接的 D2h 对称四方棱柱节点,从而形成了 bcu 拓扑结构。芘的π芳香共轭体系和构成 COF 支架的大量芳香苯基环促进了与芳香苯(Bz)分子之间更强的 π---π 相互作用,因此 TUS-88 的 Bz 吸收率达到了 464 cm3 g-1,环己烷(Cy)吸收率为 224 cm3 g-1,理想的 Bz/Cy 选择性为 2.07(这是目前的基准)。使用 Bz/Cy(1:1,v/v)混合物进行的突破实验证实了 COF 优先吸附混合物中的 Bz,生成高纯度 Cy 的时间间隔为 75.4 分钟 g-1,Bz/Cy 的突破选择性达到创纪录的 2.46。
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引用次数: 0
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