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Mechano-electrochemical impedance spectroscopy: Experimentation, interpretation, and application 机械-电化学阻抗谱:实验、解释和应用
IF 35.4 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-12-17 DOI: 10.1016/j.joule.2025.102177
Ruqing Fang , Junning Jiao , Wei Li , Royal C. Ihuaenyi , Martin Z. Bazant , Juner Zhu
We introduce mechano-electrochemical impedance spectroscopy (MEIS) as a technique that complements electrochemical impedance spectroscopy (EIS) by probing coupled mechanical-electrochemical dynamics in batteries. MEIS leverages electrode expansion and contraction during ion intercalation, which induces measurable pressure fluctuations under mechanical constraint. By applying a small sinusoidal current and recording the pressure response, MEIS defines its spectrum as the frequency-domain ratio of pressure to current. Experiments across multiple chemistries reveal distinct MEIS features that depend strongly on state of charge (SOC) and are sensitive to state of health (SOH), underscoring its diagnostic potential. An idealized analytical model links semicircles to mechanical stiffness and vertical features to intercalation-induced pseudo-damping, while a porous-electrode model incorporating a poro-viscoelastic bridge explains counterintuitive behaviors such as phase reversals and quadrant shifts. By connecting particle-scale deformation to electrode-level responses, MEIS opens new avenues for SOC estimation, degradation analysis, and health diagnostics in energy storage systems.
本文介绍了机械-电化学阻抗谱(MEIS)作为电化学阻抗谱(EIS)的补充技术,通过探测电池中耦合的机械-电化学动力学。MEIS利用离子插入过程中电极的膨胀和收缩,在机械约束下引起可测量的压力波动。通过施加一个小的正弦电流并记录压力响应,MEIS将其频谱定义为压力与电流的频域之比。多种化学实验揭示了MEIS的不同特征,这些特征强烈依赖于荷电状态(SOC),并对健康状态(SOH)敏感,强调了其诊断潜力。理想的分析模型将半圆与机械刚度联系起来,将垂直特征与插层引起的伪阻尼联系起来,而结合孔隙粘弹性桥的多孔电极模型则解释了相反转和象限偏移等反直觉行为。通过将颗粒级变形与电极级响应联系起来,MEIS为储能系统的SOC估算、退化分析和健康诊断开辟了新的途径。
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引用次数: 0
Breaking the activity-stability trade-off with a high-entropy perovskite oxygen electrode for sustainable solid oxide cells 利用高熵钙钛矿氧电极打破了可持续性固体氧化物电池的活性-稳定性权衡
IF 35.4 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-12-17 DOI: 10.1016/j.joule.2025.102198
Yucun Zhou , Xueyu Hu , Weilin Zhang , Zheyu Luo , Yuechao Yao , Tongtong Li , Yong Ding , Yu Chen , Meilin Liu
Reversible solid oxide cells (RSOCs) represent a promising technology for efficient, long-term, and large-scale co-generation of power and fuel. However, commercializing RSOCs has been hindered by the inadequate electrocatalytic activity and stability of conventional oxygen (or air) electrode materials. In this work, we demonstrate that a high-entropy strategy effectively overcomes the classic activity-stability trade-off in perovskite-based air electrode materials. The developed Pr0.25Nd0.25Gd0.25Sm0.25Ba0.25La0.25Sr0.25Ca0.25Co2O5+δ (HE-PBC) air electrode exhibits exceptional electrocatalytic activity and stability under realistic operating conditions. When integrated into oxygen ion-conducting RSOCs, the HE-PBC electrode nearly doubles the cell performance compared with the conventional electrode while reducing the degradation rate by more than an order of magnitude. Furthermore, proton-conducting RSOCs with the HE-PBC electrode exhibit outstanding performance, achieving a peak power density of 1.13 W cm−2 in fuel cell mode and a current density of 2.56 A cm−2 at 1.3 V in electrolysis mode at 600°C while maintaining excellent stability for over 1,000 h.
可逆固体氧化物电池(rsoc)是一种很有前途的高效、长期和大规模热电联产技术。然而,由于传统氧(或空气)电极材料的电催化活性和稳定性不足,rsoc的商业化一直受到阻碍。在这项工作中,我们证明了高熵策略有效地克服了钙钛矿基空气电极材料中经典的活性-稳定性权衡。所研制的Pr0.25Nd0.25Gd0.25Sm0.25Ba0.25La0.25Sr0.25Ca0.25Co2O5+δ (HE-PBC)空气电极在实际操作条件下表现出优异的电催化活性和稳定性。当集成到氧离子导电rsoc中时,HE-PBC电极的电池性能几乎是传统电极的两倍,同时将降解率降低了一个数量级以上。此外,具有HE-PBC电极的质子导电rsoc表现出出色的性能,在燃料电池模式下实现了1.13 W cm - 2的峰值功率密度,在600°C电解模式下在1.3 V下实现了2.56 a cm - 2的电流密度,同时保持了1000小时以上的优异稳定性。
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引用次数: 0
Confined crystallization strategy enabling high-quality perovskite film for advanced photovoltaics 限制结晶策略使高质量的钙钛矿薄膜用于先进的光伏
IF 39.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-12-16 DOI: 10.1016/j.joule.2025.102228
Xiaopeng Feng, Fuzong Xu, Cheng Peng, Zhipeng Shao, Zaiwei Wang, Chongwen Li, Qichao Meng, Bingqian Zhang, Hongguang Meng, Yaliang Han, Lin Han, Boyang Lu, Changcheng Cui, Hao Wei, Yimeng Li, Hongpei Ji, Qiangqiang Zhao, Kaiyu Wang, Xiaofan Du, Chaojie Chen, Guanglei Cui
Spray coating offers great potential for optoelectronic devices with complex geometries, but uniform crystallization remains challenging because of limited control over the process. Herein, we present a localized high-concentration (LHC) precursor strategy that enables homogeneous and confined bulk-phase pre-nucleation within droplets during spraying, effectively addressing spatiotemporal inconsistencies in nucleation. The LHC approach employs weak ligand solvents to restrict the diffusion of A-site cations while enhancing their interaction with [PbIx]2x complexes, thereby suppressing the formation of solvated intermediate phases and achieving direct α-phase perovskite with high crystallographic orientation and low defect-state density (∼1014 cm−3). This work also established a correlation between solvent-related parameters and device performance, using machine learning. The spray-coated devices achieved power conversion efficiencies (PCEs) of 25.5% (0.09 cm2 small cells), 22.5% (14 cm2 mini-modules), and 23.2% (curved cells). The strategy has been proven to have versatile applications, including in high-humidity environments (relative humidity [(R.H.] ∼80%, 23.1%), complex surfaces, and mask-assisted patterning.
喷涂为具有复杂几何形状的光电器件提供了巨大的潜力,但由于对工艺的控制有限,均匀结晶仍然具有挑战性。在此,我们提出了一种局部高浓度(LHC)前体策略,该策略可以在喷雾过程中在液滴内实现均匀和受限的体相预成核,有效地解决了成核的时空不一致性。LHC方法采用弱配体溶剂来限制a位阳离子的扩散,同时增强它们与[PbIx]2−x配合物的相互作用,从而抑制溶剂化中间相的形成,从而获得具有高结晶取向和低缺陷态密度(~ 1014 cm−3)的α-相钙钛矿。这项工作还利用机器学习建立了溶剂相关参数与设备性能之间的相关性。喷涂器件的功率转换效率(pce)分别为25.5% (0.09 cm2的小电池)、22.5% (14 cm2的迷你模块)和23.2%(弯曲电池)。该策略已被证明具有广泛的应用,包括在高湿度环境中(相对湿度[(R.H.)] ~ 80%, 23.1%),复杂表面和掩模辅助图案化。
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引用次数: 0
Semi-artificial leaf interfacing organic semiconductors and enzymes for solar chemical synthesis 半人工叶界面有机半导体和酶的太阳能化学合成
IF 35.4 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-19 DOI: 10.1016/j.joule.2025.102165
Celine Wing See Yeung , Yongpeng Liu , David M. Vahey , Samuel J. Cobb , Virgil Andrei , Ana M. Coito , Rita R. Manuel , Inês A.C. Pereira , Erwin Reisner
Photoelectrochemical biohybrids combine the advantages of light-harvesting semiconductors and biocatalysts into a single compact device. However, limited device stability, the use of toxic elements, and non-innocent external components make a sustainable artificial photosynthetic reaction difficult to achieve. Here, we introduce organic photoelectrodes connected to an inverse opal TiO2 matrix that hosts efficient hydrogenase or formate dehydrogenase, driving direct solar fuel synthesis. By co-immobilizing carbonic anhydrase, the organic bulk heterojunction photobiocathodes generate onset potentials of 1 V vs. RHE and photocurrent densities of up to −8 mA cm−2 in a pH-neutral bicarbonate solution, attaining stable H2 production or selective CO2-to-formate conversion over 10 h. Sufficient aqueous formate was produced (∼2.5 mM) to serve as a hydride source for the asymmetric hydrogenation of acetophenone using a synthetic Noyori-Ikariya catalyst. The semi-artificial organic semiconductor—BiVO4 tandem leaves achieve a solar-to-fuel efficiency of 0.6% and a Faradaic yield of 87% for formate.
光电化学生物杂化体将光收集半导体和生物催化剂的优点结合到一个单一的紧凑装置中。然而,有限的设备稳定性、有毒元素的使用以及非无害的外部成分使得可持续的人工光合反应难以实现。在这里,我们引入了有机光电极连接到反向蛋白石TiO2基质,该基质承载高效的氢化酶或甲酸脱氢酶,驱动直接太阳能燃料合成。通过共固定化碳酸酐酶,有机体异质结光生物阴极在ph中性碳酸氢盐溶液中产生1 V相对于RHE的起始电位和高达- 8 mA cm - 2的光电流密度,在10小时内实现稳定的H2生成或选择性的二氧化碳到甲酸转化。使用合成Noyori-Ikariya催化剂产生足够的甲酸水(~ 2.5 mM)作为苯乙酮不对称氢化的氢化物源。半人工有机半导体- bivo4串联叶片的太阳能-燃料效率为0.6%,甲酸的法拉第产率为87%。
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引用次数: 0
Paving the way for high activity and stability platinum-free fuel cells 为高活性和稳定性的无铂燃料电池铺平了道路
IF 35.4 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-19 DOI: 10.1016/j.joule.2025.102210
Quentin Meyer , Chuan Zhao
In a recent issue of Nature, Wang and co-workers present a new Fe/N–C catalyst for fuel cells, achieving a record power density of 0.75 W cm−2 under 1.0 bar H₂-air and 86% of retention over 303 h of operations.1 This preview highlights the significance of this breakthrough, placing platinum-free catalysts in close competition with platinum for fuel cells.
在最近一期的《自然》杂志上,Wang和他的同事们展示了一种新的用于燃料电池的Fe/ N-C催化剂,在1.0 bar H₂-空气下实现了0.75 W cm - 2的创纪录功率密度,在运行303小时内保持了86%这个预览强调了这一突破的重要性,将无铂催化剂与铂燃料电池密切竞争。
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引用次数: 0
A robust metal-organic framework-based electrocatalyst for durable green hydrogen production 一种坚固的金属有机框架电催化剂,用于持久的绿色氢气生产
IF 35.4 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-19 DOI: 10.1016/j.joule.2025.102220
Wenjuan Wang , Xin Xiao , Qiang Xu
In a recent issue of Nature Chemical Engineering, Zhao and coworkers reported a scalable and rapid synthesis of a cobalt-cerium-based metal-organic framework (MOF) for an alkaline water-splitting electrolyzer, achieving low energy consumption and outstanding stability. This preview provides insights into the development of MOF-based electrocatalysts for green hydrogen production.
在最近一期的《自然化学工程》杂志上,Zhao及其同事报道了一种用于碱性水分解电解槽的钴-铈基金属有机框架(MOF)的可扩展和快速合成,实现了低能耗和出色的稳定性。该预览提供了对基于mof的绿色制氢电催化剂的发展的见解。
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引用次数: 0
Unraveling degradation mechanism of electrolyte at high voltage and a hybridization strategy for non-flammable 4.8 V LiCoO2 battery 非可燃4.8 V LiCoO2电池电解液高压解解降解机理及杂化策略
IF 35.4 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-19 DOI: 10.1016/j.joule.2025.102166
Zhaoyu Sun , Yuxuan Liu , Jiahe Chen , Junhao Liu , Xuanyi Zhou , Fangkun Li , Jingwei Zhao , Min Zhu , Jun Liu
The potential risk of transition-metal (TM) ion dissolution is a prevalent issue in nearly all layered TM oxide cathodes. Severe decomposition of the electrolyte frequently occurs after the dissolution of TM ions. This phenomenon is typically attributed to the catalytic effects of TM ions. However, there is a lack of research that clearly explains this destabilization of the electrolyte. This study provides an explanation of the interfacial behavior of Co ions and addresses the issue of dissolved Co ions in the electrolyte through a hybridization strategy. LiCoO2 (LCO) batteries utilizing the isobutyronitrile (IBN)-F electrolyte demonstrate an impressive increase in capacity retention, rising from 56.6% to 84.5% after 300 cycles at 4.7 V. Additionally, the capacity retention of LCO batteries in this electrolyte is 73.3% after 200 cycles at 4.8 V. This electrolyte is flame retardant. 1 Ah pouch cells with the IBN-F electrolyte remain fireproof even when punctured in a charged state.
过渡金属(TM)离子溶解的潜在风险是几乎所有层状TM氧化物阴极中普遍存在的问题。在TM离子溶解后,电解液经常发生严重的分解。这种现象通常归因于TM离子的催化作用。然而,缺乏能够清楚解释这种电解质不稳定的研究。本研究解释了Co离子的界面行为,并通过杂化策略解决了Co离子在电解质中的溶解问题。使用异丁腈(IBN)-F电解质的LiCoO2 (LCO)电池在4.7 V电压下循环300次后,容量保持率从56.6%提高到84.5%。在4.8 V电压下循环200次后,LCO电池的容量保持率为73.3%。这种电解质是阻燃的。使用IBN-F电解液的Ah袋电池即使在带电状态下被刺穿也能保持防火。
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引用次数: 0
Multiscale mass transfer at carbonaceous catalyst-mediated electrocatalytic interface 碳质催化剂介导的电催化界面的多尺度传质
IF 35.4 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-19 DOI: 10.1016/j.joule.2025.102170
Fei Sun , Chaowei Yang , Yi Zhang , Zhibin Qu , Jiayu Zuo , Jihui Gao , Shaoqin Liu , Yunfeng Lu
Carbonaceous electrocatalysts have demonstrated superior performance and cost-effectiveness in the field of electrocatalysis for sustainable energy development. Beyond the conventional focus on active site engineering, optimizing mass transfer across the multiscale functional units of carbon catalysts is also essential for bridging the lab-to-industry gap. Herein, this review provides a systematic overview of multiscale mass transfer dynamics at carbon-based electrocatalytic interfaces, aiming to establish mass transfer theories and principles from macroscale electrodes and mesoscale pores to nanoscale carbon surfaces. Building upon this foundation, the scale interactions within critical devices (e.g., membrane electrode assemblies [MEAs] and flow cells) are examined, and the broad applicability of this engineering philosophy is further demonstrated by extending the principles to non-carbon systems. Furthermore, a synergistic framework combining multiscale in situ characterization maps with a cross-scale modeling map is proposed for molecular-level insights. The review also outlines challenges and future directions for designing cross-scale processes from nano-catalysts to macro-reactors.
碳质电催化剂在促进能源可持续发展的电催化领域表现出了优越的性能和成本效益。除了对活性位点工程的传统关注之外,优化碳催化剂多尺度功能单元之间的传质对于弥合实验室与工业之间的差距也至关重要。本文对碳基电催化界面的多尺度传质动力学进行了系统的综述,旨在建立从宏观尺度电极和中尺度孔隙到纳米尺度碳表面的传质理论和原理。在此基础上,研究了关键设备(例如膜电极组件[mea]和流动电池)内的尺度相互作用,并通过将该原理扩展到非碳系统进一步证明了该工程哲学的广泛适用性。此外,提出了一个将多尺度原位表征图与跨尺度建模图相结合的协同框架,以获得分子水平的见解。综述还概述了设计从纳米催化剂到宏观反应器的跨尺度工艺的挑战和未来方向。
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引用次数: 0
Waste heat is mostly a waste of time 废热主要是浪费时间
IF 35.4 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-19 DOI: 10.1016/j.joule.2025.102157
Addison Killean Stark , Ashwin Salvi , Todd Bandhauer
Dr. Addison Stark is co-founder and CEO of AtmosZero. He previously served as associate director for energy innovation at the Bipartisan Policy Center and as a fellow and acting program director at the U.S. Department of Energy’s Advanced Research Projects Agency—Energy (ARPA-E). Stark holds a PhD in mechanical engineering from MIT. His work spans research, policy, and commercialization of technologies to decarbonize industry.
Dr. Ashwin Salvi is co-founder of AtmosZero. He previously served as an ARPA-E fellow at the U.S. Department of Energy, where he helped design and manage over $75 million in federal R&D programs. He earned his PhD in mechanical engineering from the University of Michigan. His background covers thermodynamics, heat transfer, and technology commercialization in advanced energy systems.
Dr. Todd Bandhauer is co-founder and chief technology officer of AtmosZero and professor of mechanical engineering at Colorado State University. His research focuses on advanced thermal systems and industrial decarbonization. Bandhauer holds a PhD in mechanical engineering from Georgia Tech and is an inventor on over 20 patents.
Addison Stark博士是AtmosZero的联合创始人兼首席执行官。他曾担任两党政策中心能源创新副主任,以及美国能源部高级研究计划局(ARPA-E)的研究员和代理项目主任。Stark拥有麻省理工学院机械工程博士学位。他的工作涵盖了研究、政策和工业脱碳技术的商业化。Ashwin Salvi是AtmosZero的联合创始人。他曾在美国能源部担任ARPA-E研究员,在那里他帮助设计和管理了超过7500万美元的联邦研发项目。他在密歇根大学获得机械工程博士学位。他的背景包括热力学、传热和先进能源系统的技术商业化。托德·班德豪尔是AtmosZero的联合创始人兼首席技术官,也是科罗拉多州立大学机械工程教授。他的研究重点是先进的热系统和工业脱碳。Bandhauer拥有佐治亚理工学院机械工程博士学位,拥有20多项专利。
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引用次数: 0
Scalable polymer for large-area semitransparent organic photovoltaics 用于大面积半透明有机光伏的可伸缩聚合物
IF 35.4 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-19 DOI: 10.1016/j.joule.2025.102173
Dongsheng Xie , Baoqi Wu , Qiong Wu , Baozhong Deng , Jianglong Li , Zhili Chen , Jiayuan Zhu , Ruoxi Xia , Langheng Pan , Kangda Liu , Qiuju Jiang , Haozhe Feng , Xiyue Yuan , Yue Zhang , Qianqing Jiang , Dianyi Liu , Tao Xu , Hongxiang Li , Fei Huang , Yong Cao , Chunhui Duan
Organic solar cells (OSCs) have achieved power conversion efficiencies (PCEs) exceeding 20%, yet the transition from lab to market remains challenging. This study proposes a systematic molecular engineering paradigm for developing cost-effective polymer donors, exemplified by PPT-3, specifically engineered for semitransparent solar windows. Using simple monocyclic aromatic units, we simplified the synthesis, enabling scalable production from milligrams to 20 g. Opaque OSCs based on PPT-3 achieved PCEs exceeding 18%, with excellent batch-to-batch reproducibility across multiple scales, including three Stille batches (0.2–5.0 g) and four direct-arylation batches (0.2–20.0 g). Moreover, ambient blade-coated semitransparent modules achieved a record PCE of 6.69%, an average visible transmittance of 40.30%, and a light-utilization efficiency of 2.70% over a 120 cm2 active area. This work demonstrates the first scalable synthesis of high-performance polymers (PCE >18%) via a tin-free polymerization route, offering a transformative pathway for advancing OSCs from lab-scale research to commercial viability.
有机太阳能电池(OSCs)已经实现了超过20%的功率转换效率(pce),但从实验室到市场的过渡仍然具有挑战性。本研究提出了一种系统的分子工程范例,用于开发具有成本效益的聚合物供体,例如专门为半透明太阳能窗设计的PPT-3。使用简单的单环芳香族单位,我们简化了合成,使可扩展生产从毫克到20克。基于pt -3的不透明OSCs实现了超过18%的pce,在多个尺度上具有出色的批对批再现性,包括三个蒸馏批次(0.2-5.0 g)和四个直接芳基化批次(0.2-20.0 g)。此外,环境叶片涂层半透明组件在120 cm2的有效面积上实现了创纪录的6.69%的PCE, 40.30%的平均可见光透过率和2.70%的光利用效率。这项工作展示了通过无锡聚合途径首次可扩展合成高性能聚合物(PCE >18%),为推进OSCs从实验室规模研究到商业可行性提供了一条变革性途径。
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引用次数: 0
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Joule
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