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High-entropy-driven half-Heusler alloys boost thermoelectric performance 高熵驱动半休斯勒合金提升热电性能
IF 39.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-09 DOI: 10.1016/j.joule.2024.08.008
Subrata Ghosh, Amin Nozariasbmarz, Huiju Lee, Lavanya Raman, Shweta Sharma, Rabeya B. Smriti, Dipika Mandal, Yu Zhang, Sumanta K. Karan, Na Liu, Jennifer L. Gray, Mohan Sanghadasa, Yi Xia, Shashank Priya, Wenjie Li, Bed Poudel

High-entropy engineering effectively reduces lattice thermal conductivity (κL) in thermoelectric (TE) materials; however, the chemical complexity of multiple elements in high-entropy materials often leads to phase segregation, limiting their electrical transport properties and overall TE performance. Herein, we report a p-type high-entropy stabilized single-phase half-Heusler alloy, MFeSb, specifically designed to enhance configurational entropy by introducing multiple element species on a single atomic site. This material exhibited low κL due to phonon group velocity reduction and strong phonon scattering from lattice strain generated through distorted lattices while maintaining a high power factor. The material demonstrated a record high figure of merit (zT) of 1.5 at 1,060 K, with an average zT of ∼0.92 over 300–1,060 K. Furthermore, superior conversion efficiencies of 15% and 14% for a single-leg and a unicouple module at a temperature difference of ΔT ∼671 K were achieved. Our findings provide a new avenue for enhancing TE material performance through high-entropy engineering.

高熵工程可有效降低热电(TE)材料的晶格热导率(κL);然而,高熵材料中多种元素的化学复杂性往往会导致相分离,从而限制其电气传输特性和整体热电性能。在此,我们报告了一种 p 型高熵稳定单相半赫斯勒合金 MFeSb,该合金专门设计用于通过在单个原子位点上引入多种元素来增强构型熵。由于声子群速度降低以及扭曲晶格产生的晶格应变对声子的强烈散射,这种材料表现出较低的κL,同时保持了较高的功率因数。此外,在 ΔT ∼ 671 K 的温差条件下,单腿模块和单耦合模块的转换效率分别达到了 15%和 14%。我们的研究结果为通过高熵工程提高 TE 材料性能提供了一条新途径。
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引用次数: 0
Conveyor mode enabling continuous ionic thermoelectric conversion 可实现连续离子热电转换的输送模式
IF 39.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-09 DOI: 10.1016/j.joule.2024.08.004
Dongxing Song, Chunyu Zhao, Bin Chen, Weigang Ma, Ke Wang, Xing Zhang

The huge thermopower observed in the thermodiffusion mechanism of ionic thermoelectric (i-TE) materials has led researchers to conceive of the upgrading of thermoelectric technology. However, the intermittent power generation in the capacitor mode has been a major hindrance to achieving optimal performance. This work proposes a conveyor mode for continuous i-TE conversion in mixed ion-electron-conducting i-TE material with an ionic circuit. In this conveyor mode, ion-electronic friction serves as the link between ions and electrons, enabling the thermally diffused ions to convey electrons to power the load, and persistent ionic transport, owing to the ionic circuit, ensures continuous power generation. Experiments demonstrate continuous power generation and significant improvements of power density in the conveyor mode. Theoretical analysis shows that the conveyor mode is competitive to not only the capacitor mode but also a general electronic thermoelectric conversion. Our study points out a direction for the development of i-TE technology.

在离子热电(i-TE)材料的热扩散机制中观察到的巨大热功率促使研究人员构想热电技术的升级。然而,电容器模式下的间歇性发电一直是实现最佳性能的主要障碍。这项研究提出了一种在具有离子回路的离子-电子混合传导 i-TE 材料中进行连续 i-TE 转换的传送带模式。在这种传输模式中,离子-电子摩擦是离子和电子之间的纽带,使热扩散离子能够传输电子,为负载供电,而离子回路带来的持续离子传输则确保了持续发电。实验证明,在输送模式下可持续发电并显著提高功率密度。理论分析表明,输送模式不仅对电容器模式有竞争力,而且对一般的电子热电转换也有竞争力。我们的研究为 i-TE 技术的发展指明了方向。
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引用次数: 0
Molecule-triggered strain regulation and interfacial passivation for efficient inverted perovskite solar cells 分子触发应变调节和界面钝化,实现高效倒置包晶太阳能电池
IF 39.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-30 DOI: 10.1016/j.joule.2024.08.003
Mingquan Tao, Yang Wang, Kun Zhang, Zhaofei Song, Yangjie Lan, Haodan Guo, Lutong Guo, Xiwen Zhang, Junfeng Wei, Dongqiang Cao, Yanlin Song

Residual tensile strain impedes the improvement of efficiency and intrinsic stability of perovskite solar cells (PSCs), resulting from the perovskite lattice distortion and different thermal expansion coefficients. Herein, we propose a molecule-triggered strain regulation and interfacial passivation strategy to enhance the efficiency and stability (especially photostability) of PSCs, which utilizes the [2 + 2] cycloaddition reaction of 6-bromocoumarin-3-carboxylic acid ethyl ester (BAEE), consuming the incident UV light to suppress the tensile strain evolution. Meanwhile, the BAEE can form a strong bond with NiOx, assisting the perovskite growth and the interface defect passivation. We obtain the efficiency of 26.32% (certified 26.08%), the open-circuit voltage (Voc) up to 1.201 V with low Voc loss (0.342 V), as well as the long-term stability (continuous 365 nm UV illumination: T90 > 110 h in N2, T90 > 6 h in ambient air, and continuous LED white light irradiation at 100 mWcm−2: T90 > 1,000 h).

由于包晶晶格畸变和不同的热膨胀系数,残余拉伸应变阻碍了包晶太阳能电池(PSCs)效率和内在稳定性的提高。在此,我们提出了一种分子触发的应变调节和界面钝化策略,利用 6-溴香豆素-3-羧酸乙酯(BAEE)的[2 + 2]环加成反应,消耗入射紫外光来抑制拉伸应变的演化,从而提高 PSC 的效率和稳定性(尤其是光稳定性)。同时,BAEE 还能与 NiOx 形成强键,促进包晶生长和界面缺陷钝化。我们获得了 26.32% 的效率(认证为 26.08%)、高达 1.201 V 的开路电压(Voc)和较低的 Voc 损耗(0.342 V),以及长期稳定性(连续 365 nm 紫外光照射:在氮气中的 T90 > 110 小时,在环境空气中的 T90 > 6 小时,以及 100 mWcm-2 的 LED 白光连续照射:T90 > 1,000 小时)。
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引用次数: 0
Thermoelectric cyclic-thermal regulation: A new operational mode of thermoelectric materials with high energy efficiency 热电循环热调节:具有高能效的热电材料新运行模式
IF 39.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-30 DOI: 10.1016/j.joule.2024.08.002
Yupeng Wang, Xinzhi Wu, Mao Yu, Xuehua Shen, Shuaihua Wang, Huan Li, Zuotai Zhang, Weishu Liu

The thermoelectric cyclic-thermal-regulation (TEcR) system was defined as cyclical heat pumping between two vessels in a transient mode, which has emerged as a new application in gas separation and temperature-driven soft robots. Here, we provided systematic theoretical fundamentals relative to the TEcR system and proposed the determining factors and performance scales. We have also designed and fabricated a thermoelectric CO2-gas-separation system based on low-temperature adsorption and high-temperature desorption, verifying the feasibility of the TEcR system. Our experiments unequivocally demonstrate the significant potential of the TEcR system, with energy consumption savings of 42% and cycle frequency improvements of 2.5 times compared with electrical heater systems. We also proposed an empirical figure of merit to guide the thermoelectric material optimization strategies for the TEcR application. Our work sheds light on the new application of thermoelectric materials, which would generate implications for a wide range of industrial applications that use multi-plate thermal energy.

热电循环-热调节(TEcR)系统被定义为两个容器之间在瞬态模式下的循环热泵,它已成为气体分离和温度驱动软机器人的新应用。在此,我们提供了与 TEcR 系统相关的系统理论基础,并提出了决定因素和性能标度。我们还设计并制造了基于低温吸附和高温解吸的热电二氧化碳气体分离系统,验证了 TEcR 系统的可行性。我们的实验明确证明了 TEcR 系统的巨大潜力,与电加热器系统相比,能耗可节省 42%,循环频率可提高 2.5 倍。我们还提出了一个经验值,用于指导 TEcR 应用的热电材料优化策略。我们的工作揭示了热电材料的新应用,这将对使用多板热能的广泛工业应用产生影响。
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引用次数: 0
Data-driven analysis of battery formation reveals the role of electrode utilization in extending cycle life 对电池化成的数据驱动分析揭示了电极利用在延长循环寿命中的作用
IF 39.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-29 DOI: 10.1016/j.joule.2024.07.024
Xiao Cui, Stephen Dongmin Kang, Sunny Wang, Justin A. Rose, Huada Lian, Alexis Geslin, Steven B. Torrisi, Martin Z. Bazant, Shijing Sun, William C. Chueh

Formation is a critical step in battery manufacturing. During this process, lithium inventory is consumed to form the solid electrolyte interphase (SEI), which in turn determines the battery lifetime. To tackle the vast parameter space and complexity of formation, we employ a data-driven workflow on 186 lithium-ion battery cells across 62 formation protocols. We identify two key parameters, formation charge current and temperature, that control battery longevity via distinct mechanisms. Surprisingly, high-formation charge current on the first cycle extends battery cycle life by an average of 50%. Unlike elevated formation temperature, which boosts battery performance by forming a robust SEI, the cycle life improvement for fast-formed cells arises from a shifted electrode-specific utilization after formation. Apart from the widely acknowledged role of formation in governing SEI properties, we demonstrate how formation protocols determine the stoichiometry range over which the positive and negative electrodes are cycled.

形成是电池制造的关键步骤。在此过程中,锂库存被消耗以形成固态电解质间相(SEI),这反过来又决定了电池的使用寿命。为了应对庞大的参数空间和复杂的化成过程,我们采用了数据驱动工作流程,对 186 个锂离子电池单元进行了 62 种化成协议的分析。我们确定了两个关键参数:化成充电电流和温度,它们通过不同的机制控制电池的寿命。令人惊讶的是,第一个循环的高化成充电电流可将电池循环寿命平均延长 50%。化成温度的升高可通过形成稳固的 SEI 来提高电池性能,而快速化成电池则不同,其循环寿命的提高源于化成后电极利用率的改变。除了公认的化成对 SEI 性能的影响外,我们还展示了化成协议如何决定正负极循环的化学计量范围。
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引用次数: 0
Achieving 20.8% organic solar cells via additive-assisted layer-by-layer fabrication with bulk p-i-n structure and improved optical management 通过添加剂辅助逐层制造具有块状 pi-n 结构和改进光学管理的 20.8% 有机太阳能电池
IF 39.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-29 DOI: 10.1016/j.joule.2024.08.001
Lei Zhu, Ming Zhang, Guanqing Zhou, Zaiyu Wang, Wenkai Zhong, Jiaxin Zhuang, Zichun Zhou, Xingyu Gao, Lixuan Kan, Bonan Hao, Fei Han, Rui Zeng, Xiaonan Xue, Shengjie Xu, Hao Jing, Biao Xiao, Haiming Zhu, Yongming Zhang, Feng Liu

Additive-assisted layer-by-layer (LBL) deposition affords interpenetrating fibril network active layer morphology with a bulk p-i-n feature and proper vertical segregation in organic solar cells (OSCs). This approach captures the balance between material interaction and crystallization that locks the characteristic length scales at tens of nanometers to suit exciton and carrier diffusion, thereby reducing recombination losses. On the other hand, the wrinkle-pattern morphology generated due to Marangoni-Bénard instability and radial flow during spin-coating couples with the reflective back electrode, inducing diffuse reflection and thus enhancing light capture capability. The nano-to-micron hierarchical morphology in proper vertical segregation achieves a record-breaking power conversion efficiency (PCE) of 20.8% for small-area devices and 17.0% for mini-module devices. The new processing and the resulted 3D morphology better suit photon and carrier dynamics in operation, such that a notable improvement in device operational stability is recorded, which offers a plausible strategy toward practical organic photovoltaic technology.

添加剂辅助逐层沉积(LBL)技术使有机太阳能电池(OSC)中的穿插纤维网络活性层形态具有大块 pi-n 特征和适当的垂直隔离。这种方法能在材料相互作用和结晶之间取得平衡,将特征长度尺度锁定在几十纳米,以适应激子和载流子扩散,从而减少重组损耗。另一方面,在旋涂过程中,由于马兰戈尼-贝纳德不稳定性和径向流动而产生的皱纹图案形态与反射背电极耦合,引起漫反射,从而增强了光捕获能力。纳米到微米的分层形态在适当的垂直偏析中实现了破纪录的功率转换效率(PCE),小面积器件达到 20.8%,微型模块器件达到 17.0%。新的加工工艺和由此产生的三维形态更适合运行中的光子和载流子动力学,因此显著提高了器件的运行稳定性,为实现实用有机光伏技术提供了可行的策略。
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引用次数: 0
A scalable integrated solar device for the autonomous production of green methane 用于自主生产绿色甲烷的可扩展集成太阳能装置
IF 38.6 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-21 DOI: 10.1016/j.joule.2024.05.012

The solar-driven conversion of CO2 into molecules with high calorific value is a major challenge to reduce the carbon footprint of industrialized countries. Many concepts are proposed, but limited action has been undertaken so far to design, integrate, and scale commercially viable technologies. Here, we report on the long-term performance of an autonomous solar-driven device that continuously converts CO2 into CH4 under mild conditions. It couples a biomethanation reactor to a set of integrated photoelectrochemical cells, combining silicon/perovskite tandem solar cells with proton exchange membrane electrolyzers, for the production of solar hydrogen from water. The 5.5% solar-to-fuel yield (calculated from global horizontal irradiance) achieved by the bench-scale device during 72 h of outdoor operation at JRC, Ispra, Italy, in July 2022, demonstrates that re-design and close integration of proven lab-scale concepts can overcome the technological barriers to the industrial deployment of artificial photosynthesis process.

利用太阳能将二氧化碳转化为高热值分子是减少工业化国家碳足迹的一大挑战。人们提出了许多概念,但迄今为止,在设计、集成和推广商业上可行的技术方面所采取的行动十分有限。在此,我们报告了一种自主太阳能驱动装置的长期性能,该装置可在温和条件下持续将二氧化碳转化为甲烷。该装置将一个生物甲烷化反应器与一套集成光电化学电池结合在一起,将硅/过氧化物串联太阳能电池与质子交换膜电解槽结合在一起,利用太阳能从水中制氢。2022 年 7 月,在意大利伊斯普拉的 JRC 进行的 72 小时室外操作中,台式装置实现了 5.5% 的太阳能转化为燃料的产量(根据全球水平辐照度计算),这表明重新设计和紧密集成已被证实的实验室规模概念可以克服工业应用人工光合作用过程的技术障碍。
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引用次数: 0
Electrified inductive heating for sustainable utilization of liquid hydrogenated organics 电感应加热促进液态氢化有机物的可持续利用
IF 38.6 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-21 DOI: 10.1016/j.joule.2024.05.020

We propose the electrified catalytic inductive heating system (ECIHS), which utilizes electromagnetic induction heating (IH) of a monolithic catalytic composite to induce direct and efficient heat transfer to the liquid-phase reaction environment. Herein, we demonstrated that the ECIHS could be utilized to extract hydrogen from liquid-phase perhydro-dibenzyltoluene (H18-DBT) within just 3.5 s, accounting for a 16.4-fold improvement in the reaction rate compared with conventional heating methods. This remarkable observation underscores the potential of the ECIHS for on-site hydrogen utilization, empowering various advanced applications such as hydrogen-powered vehicles. Furthermore, the capabilities of the ECIHS for efficient heat and mass transfer in the liquid phase are also translatable to a myriad of different chemical processing schemes with high industrial value. Overall, the ECIHS represents a major breakthrough in the development of sustainable chemical processing methods, further propelling efforts to achieve full decarbonization in the global chemical processing industry.

我们提出了电气化催化感应加热系统(ECIHS),该系统利用电磁感应加热(IH)整体催化复合材料,将热量直接有效地传递到液相反应环境中。在这里,我们证明了 ECIHS 可用于在短短 3.5 秒内从液相全氢二苄甲苯(H18-DBT)中提取氢气,与传统加热方法相比,反应速率提高了 16.4 倍。这一引人注目的观察结果凸显了 ECIHS 在现场氢气利用方面的潜力,为氢动力汽车等各种先进应用提供了动力。此外,ECIHS 在液相中高效传热和传质的能力还可应用于各种不同的化学处理方案,具有极高的工业价值。总之,ECIHS 代表着可持续化学处理方法开发方面的重大突破,进一步推动了全球化学处理行业实现全面脱碳的努力。
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引用次数: 0
Mechanically durable chiral-structured heterointerfaces 具有机械耐久性的手性结构异质界面
IF 38.6 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-21 DOI: 10.1016/j.joule.2024.07.014

While interface engineering of perovskite solar cells (PSCs) for defect passivation and band alignment optimization has contributed to recent breakthroughs in the efficiency and stability of PSCs, consideration of the mechanical reliability of the heterointerface has been relatively overlooked. Published in Science, the study by Duan et al.1 proposes that chiral-structured heterointerfaces are mechanically more durable compared to the widely used non-chiral heterointerfaces in PSCs.

虽然用于缺陷钝化和带排列优化的过氧化物太阳能电池(PSCs)界面工程有助于最近在 PSCs 的效率和稳定性方面取得突破,但对异质界面的机械可靠性的考虑却相对被忽视了。Duan 等人1 发表在《科学》杂志上的研究提出,与 PSC 中广泛使用的非手性异质界面相比,手性结构异质界面的机械耐久性更高。
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引用次数: 0
Disorder and spin-electron interaction in oxide cathodes 氧化物阴极中的无序和自旋电子相互作用
IF 38.6 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-21 DOI: 10.1016/j.joule.2024.07.022

The quest for high-performance lithium-ion batteries has led to extensive research on developing the advanced cathodes. A recent report in Nature by Wang et al. presents a strategy of integrating chemical short-range disorder into the bulk structure of layered oxide cathodes, which significantly enhances their durability and rate capability due to the subtle tuning of spin-electron interactions of transition metal ions.

对高性能锂离子电池的追求促使人们对先进阴极的开发进行了广泛的研究。Wang 等人最近在《自然》(Nature)杂志上发表的一篇报告介绍了一种将化学短程无序整合到层状氧化物阴极体结构中的策略,由于过渡金属离子自旋电子相互作用的微妙调整,这种策略显著提高了阴极的耐久性和速率能力。
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引用次数: 0
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