{"title":"Control Over Vertical Composition in Low Complexity Polymer Solar Cells","authors":"Xinyun Dong, Byongkyu Lee, Runqiao Song, Justin Neu, Somayeh Kashani, Wei You, Harald Ade","doi":"10.1002/aenm.202404962","DOIUrl":"https://doi.org/10.1002/aenm.202404962","url":null,"abstract":"Inverted organic solar cells are promising due to their better stability compared to conventional structures. Donors with low synthetic complexity are desirable to lower costs. However, inverted devices are rarely used in low-complexity systems. To investigate the reasons, the low-complexity PTQ10:BTP-eC9 binary system is benchmarked against the high-complexity PM6:BTP-eC9 system. In PTQ10:BTP-eC9, where the efficiency of inverted devices lags the conventional structure significantly, distinct wetting layers are observed in conventional and inverted device structures. Conversely, the vertical distribution of PM6:BTP-eC9 remains unaffected by changes in interlayer materials. The surface is always enriched in BTP-eC9, but less for PM6. Importantly, the addition of PC<sub>71</sub> BM reduces the nonuniform vertical composition gradients. As the PC<sub>71</sub> BM concentration increases, the efficiency of the inverted PTQ10 devices approach that of the conventional devices and PTQ10:BTP-eC9:PC<sub>71</sub> BM (1:1.2:0.4) exhibits negligible efficiency differences between inverted (14.01%) and conventional (14.49%) architectures. The concentration-gradients aredriven by the interfacial energy between the active layer and interlayer materials and the casting kinetics in the case of the surface. Understanding the thermodynamic and kinetic aspects provides valuable insights for optimizing the performance of inverted organic solar cells, bringing them closer to practical applications.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"16 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142911658","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuzhe Zhang, Rouya Wang, Huaisheng Ao, Tao Ma, Xuekun Zhu, Xiaotan Zhang, Jian Rong, Ziyao Zhou, Zhongchao Bai, Shi Xue Dou, Nana Wang, Zhongyu Li
{"title":"Zn2⁺-Rich Chelate Layer Facilitates Ultrahigh-Rate Zinc Anodes Via Cation Compensation and Anion Repulsion","authors":"Yuzhe Zhang, Rouya Wang, Huaisheng Ao, Tao Ma, Xuekun Zhu, Xiaotan Zhang, Jian Rong, Ziyao Zhou, Zhongchao Bai, Shi Xue Dou, Nana Wang, Zhongyu Li","doi":"10.1002/aenm.202404203","DOIUrl":"https://doi.org/10.1002/aenm.202404203","url":null,"abstract":"Aqueous Zn ion batteries hold great promise for next-generation large-scale energy storage systems due to their low cost, intrinsic safety, and environmental friendliness. However, the reversibility of Zn metal anodes is limited by severe side reactions and dendritic growth, caused by interfacial concentration gradients. To address this, a Zn<sup>2+</sup>-rich zinc phytate (ZP) chelate layer is introduced as artificial solid electrolyte interphase (SEI) that eliminates these concentration gradients through ions compensation. Theoretical calculations and experimental results demonstrate that the ZP layer, rich in Zn<sup>2</sup>⁺ ions and exhibiting strong chelating ability to capture more Zn<sup>2+</sup>, enables rapid and dynamic ion replenishment at the interface, significantly improving Zn<sup>2</sup>⁺ transport kinetics and ensuring a uniform Zn<sup>2</sup>⁺ flux. Moreover, the strong chelation of PO₄ groups restricts the 2D diffusion of Zn<sup>2</sup>⁺ ions, promoting the uniform Zn deposition. Additionally, the ZP layer repels anions and restricts water molecules migration at the Zn anode surface, fundamentally suppressing side reactions. As a result, the modified Zn anode exhibits stable Zn plating/stripping for ≈2400 h at 1 mA cm<sup>−2</sup> and 1 mAh cm<sup>−2</sup>, with an average Coulombic efficiency of 99.8%. Furthermore, the assembled ZP@Zn//VO<sub>2</sub> cell displays 87.5% capacity retention after 6000 cycles at the current density of 5 A g<sup>−1</sup>.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"20 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142917615","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Limin Liu, Yujian Liu, Xiaoliang Zhou, Frank Tietz, Daniel Grüner, Tingting Yang, Lei Jin, Xingyu Liu, Jürgen Malzbender, Ruth Schwaiger, Rafal E. Dunin-Borkowski, Qianli Ma
{"title":"Nominal Lanthanum Niobate, a Versatile Additive for Reducing Grain Boundary Resistance in Conductive Ceramics","authors":"Limin Liu, Yujian Liu, Xiaoliang Zhou, Frank Tietz, Daniel Grüner, Tingting Yang, Lei Jin, Xingyu Liu, Jürgen Malzbender, Ruth Schwaiger, Rafal E. Dunin-Borkowski, Qianli Ma","doi":"10.1002/aenm.202404985","DOIUrl":"https://doi.org/10.1002/aenm.202404985","url":null,"abstract":"Conductive ceramics currently play a vital role in human life. In practical applications, most conductive ceramics are polycrystalline, and their overall conductivity (<i>σ</i><sub>total</sub>) is influenced by both bulk and grain boundary resistances (<i>R</i><sub>bulk</sub> and <i>R</i><sub>gb</sub>, respectively). While <i>R</i><sub>bulk</sub> is mainly of academic interest, <i>R</i><sub>gb</sub> often determines the quality of a conductive ceramic component. Currently, studies discussing the influence of specific methods on grain boundary resistances are typically related to individual ceramics. In this study, it is discovered that the addition of 0.5–3 mol% nominal LaNbO<sub>4</sub> significantly reduces the <i>R</i><sub>gb</sub> of several well-known conductive ceramics, such as rhombohedral NaSICON-type Na<sup>+</sup>-ion-conducting Na<sub>3.4</sub>Zr<sub>2</sub>Si<sub>2.4</sub>P<sub>0.6</sub>O<sub>12</sub> and Li<sup>+</sup>-ion conducting Li<sub>1.5</sub>Al<sub>0.5</sub>Ti<sub>1.5</sub>P<sub>3</sub>O<sub>12</sub>, Li<sup>+</sup>-ion-conducting tetragonal perovskite Li<sub>0.34</sub>La<sub>0.56</sub>TiO<sub>3</sub>, oxygen-ion-conducting cubic fluorite 8 mol% Y<sub>2</sub>O<sub>3</sub> stabilized ZrO<sub>2</sub>, and electron-conducting perovskite SrTiO<sub>3</sub> (sintered in a reducing atmosphere). In particular, for NZSP and LATP, the enhanced <i>σ</i><sub>total</sub> reaches 9.3 × 10<sup>−3</sup> S cm<sup>−1</sup> and 2.1 × 10<sup>−3</sup> S cm<sup>−1</sup> at 25 °C, surpassing previously published results. Detailed investigations reveal that the microstructure of the grain boundaries in all the ceramics undergoes significant improvements. The findings elevate the importance of research on grain boundaries, inspiring the development of conductive ceramics with higher σ<sub>total</sub> for superior applications.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"68 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142911745","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jiyun Zhang, Vincent M. Le Corre, Jianchang Wu, Tian Du, Tobias Osterrieder, Kaicheng Zhang, Handan Zhang, Larry Lüer, Jens Hauch, Christoph J. Brabec
{"title":"Autonomous Optimization of Air-Processed Perovskite Solar Cell in a Multidimensional Parameter Space","authors":"Jiyun Zhang, Vincent M. Le Corre, Jianchang Wu, Tian Du, Tobias Osterrieder, Kaicheng Zhang, Handan Zhang, Larry Lüer, Jens Hauch, Christoph J. Brabec","doi":"10.1002/aenm.202404957","DOIUrl":"https://doi.org/10.1002/aenm.202404957","url":null,"abstract":"Traditional optimization methods often face challenges in exploring complex process parameter spaces, which typically result in suboptimal local maxima. Here an autonomous framework driven by a machine learning (ML)-guided automated platform is introduced to optimize the fabrication conditions of additive- and passivation-free perovskite solar cells (PSCs) under ambient conditions. By effectively exploring a 6D parameter space, this method identifies five parameter sets achieving efficiencies above 23%, with a peak efficiency of 23.7% with limited experimental budgets. Feature importance analysis indicates that the rotation speeds during the first and second steps of perovskite processing are the most influential factors affecting device performance, thereby meriting prioritization in the optimization efforts. These results demonstrate the exceptional capability of the autonomous framework in addressing complex process parameter optimization challenges and its potential to advance perovskite photovoltaic technology. Beyond PSCs, this work provides a reliable and comprehensive strategy for optimizing solution-processed semiconductors and highlights the broader applications of autonomous methodologies in materials science.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"26 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142911747","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lu Zhang, Hang Zhou, Yongchao Xie, Wenjing Xu, Hongyue Tian, Xingchao Zhao, Yuheng Ni, Sang Young Jeong, Ye Zou, Xixiang Zhu, Xiaoling Ma, Han Young Woo, Fujun Zhang
{"title":"Cascaded Energy and Charge Transfer Synergistically Prompting 18.7% Efficiency of Layered Organic Solar Cells with 1.48 eV Bandgap","authors":"Lu Zhang, Hang Zhou, Yongchao Xie, Wenjing Xu, Hongyue Tian, Xingchao Zhao, Yuheng Ni, Sang Young Jeong, Ye Zou, Xixiang Zhu, Xiaoling Ma, Han Young Woo, Fujun Zhang","doi":"10.1002/aenm.202404718","DOIUrl":"https://doi.org/10.1002/aenm.202404718","url":null,"abstract":"Series of layer-by-layer organic solar cells (LOSCs) are constructed by sequentially spin-coating donor layer and acceptor layers. A champion power conversion efficiency (PCE) of 18.79% is achieved from the LOSCs with PBQx-TCl/ITIC/PY-DT as active layers, which should be one of the top values among the OSCs with optical bandgap over 1.48 eV. The middle bandgap material ITIC has a complementary photon harvesting range with PBQx-TCl and PY-DT, leading to the enhanced photon harvesting of active layers. Meanwhile, ITIC can play a vital role in energy and charge transfer relay to increase exciton utilization and charge transport, which can be confirmed from the varied FFs of normal or inverted LOSCs with ITIC/PY-DT or PY-DT/ITIC as acceptor layers. Over 7% PCE improvement of LOSCs can be achieved by employing ITIC as the middle layer to form cascaded energy and charge transfer in the active layers. This work may provide an efficient strategy for improving the performance of LOSCs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"73 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142917617","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"A Multi-Colored, Structure-Tolerant Vanadate Cathode for High-Performance Aqueous Zinc-Ion Batteries","authors":"Qian Zhang, Shidi Ju, Shaohua Zhang, Shilong Xu, Zhipan Zhang","doi":"10.1002/aenm.202404597","DOIUrl":"https://doi.org/10.1002/aenm.202404597","url":null,"abstract":"Vanadium-based cathode materials for aqueous zinc-ion batteries (AZIBs) have attracted much attention in large-scale energy storage devices yet their unsatisfactory cyclic stability and slow diffusion rate of Zn<sup>2+</sup> ions during insertion and extraction hinder further commercial applications. Therefore, the development of vanadium-based cathode materials with stable crystal structures and fast Zn<sup>2+</sup> storage remains challenging. Herein, Na<sub>2</sub>CaV<sub>4</sub>O<sub>12</sub> (NCVO) nanowires are reported as a promising cathode of excellent electrochemical performance in AZIBs, simultaneously rendering high specific capacity (443.2 mAh g<sup>−1</sup> at 0.1 A g<sup>−1</sup>) and high average voltage plateau (0.91 V) with impressive energy density (403.3 Wh kg<sup>−1</sup>) and power density (1533 W kg<sup>−1</sup>). As NCVO features a unique open crystal structure with alternately arranged inactive layers ([NaO<sub>6</sub>] and [CaO<sub>8</sub>] polyhedra) and active layers ([VO<sub>4</sub>] tetrahedra), the expansion of the [VO<sub>4</sub>] tetrahedra during Zn<sup>2+</sup> insertion is well balanced by the contraction of the inactive layer, thus enabling remarkable long-term cycling stability (91.9% and 80% capacity retention after 5000 and 10 000 cycles at 10 A g<sup>−1</sup>, respectively). With the electrochromic property of the NCVO cathode, the AZIB can further be used for adaptive camouflage under a range of scenarios, shedding light on the future development of high-performance cathodes for AZIBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"13 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142917618","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Lattice Plainification and Intercalation Advances Power Generation and Thermoelectric Cooling in n-type Bi2(Te, Se)3","authors":"Jiayi Peng, Dongrui Liu, Shulin Bai, Yi Wen, Huiqiang Liang, Lizhong Su, Xin Qian, Dongyang Wang, Xiang Gao, Zhihai Ding, Qian Cao, Yanling Pei, Bingchao Qin, Li-Dong Zhao","doi":"10.1002/aenm.202404653","DOIUrl":"https://doi.org/10.1002/aenm.202404653","url":null,"abstract":"Bismuth telluride (Bi<sub>2</sub>Te<sub>3</sub>) has been the only commercialized material in thermoelectric cooling and waste heat recovery. However, the inferior performance for n-type Bi<sub>2</sub>(Te, Se)<sub>3</sub> largely restricts the practical applications. In this study, additional Ag atoms are introduced utilizing lattice plainification strategy to enhance electrical performance. Observations indicate that Ag atoms situate in the van der Waals layers, acting as n-type dopants to increase carrier concentration, bonding with adjacent Te as intercalating atoms to form electron transport channels, while also suppressing the formation of Te vacancies to boost carrier mobility, substantially favoring carrier transport. Consequently, Bi<sub>2</sub>Te<sub>2.79</sub>Se<sub>0.21</sub>I<sub>0.004</sub>+0.3%Ag achieves an excellent room-temperature <i>ZT</i> of ≈1.1, while Bi<sub>2</sub>Te2<sub>.79</sub>Se<sub>0.21</sub>I<sub>0.004</sub> + 0.4%Ag demonstrates a higher average <i>ZT</i> of ≈1.1 at 300–523 K. Furthermore, a full-scale thermoelectric cooler using optimized Bi<sub>2</sub>Te<sub>2.79</sub>Se<sub>0.21</sub>I<sub>0.004</sub>+0.3%Ag combined with commercial p-type Bi<sub>0.5</sub>Sb<sub>1.5</sub>Te<sub>3</sub> has achieved a maximum cooling temperature difference (Δ<i>T</i><sub>max</sub>) of ≈68.3 K at 300 K and a larger Δ<i>T</i><sub>max</sub> of ≈84.8 K at 343 K. Additionally, the Bi<sub>2</sub>Te<sub>2.79</sub>Se<sub>0.21</sub>I<sub>0.004</sub> + 0.4%Ag/Bi<sub>0.5</sub>Sb<sub>1.5</sub>Te<sub>3</sub>-based power generator realizes a conversion efficiency of ≈6.0% under a Δ<i>T</i> of ≈240 K. These results outperform commercial Bi<sub>2</sub>Te<sub>3</sub>-based devices, illustrating the effectiveness of lattice plainification for Bi<sub>2</sub>Te<sub>3</sub>-based thermoelectrics.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"32 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142911660","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Traps, Tail States and Their Consequences on the Open-circuit Voltage in Organic Solar Cells","authors":"Tobias Krebs, Clemens Göhler, Martijn Kemerink","doi":"10.1002/aenm.202405087","DOIUrl":"https://doi.org/10.1002/aenm.202405087","url":null,"abstract":"All that remains to reliably beat the 20% efficiency hurdle in organic solar cells are the relatively low open-circuit voltages (<i>V<sub>OC</sub></i>). A still-needed step toward solving this problem is to shed light on the mechanisms behind these losses, and herein it is focused on understanding the roll-off of <i>V<sub>OC</sub></i> at low temperatures, which has been linked to various detrimental processes. Here, a light intensity sweep is added to the temperature-dependent measurements and the resulting trends are compared with a kinetic analytical model that not only incorporates all previously suggested explanations for the temperature dependence of <i>V<sub>OC</sub></i>, but, importantly, also includes carrier density contributions to the electron and hole mobilities by treating the density of states (DOS) of the active layer as a two-level system. It is found that this description is sufficient to quantitatively explain <i>V<sub>OC</sub></i> roll-off in terms of charges getting trapped in intrinsic tail states of the Gaussian DOS without having to assume the presence of extrinsic traps.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"34 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142911746","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Electrolyte Design Strategies to Construct Stable Cathode-Electrolyte Interphases for High-Voltage Sodium-Ion Batteries","authors":"Kunchen Xie, Yuchen Ji, Luyi Yang, Feng Pan","doi":"10.1002/aenm.202405301","DOIUrl":"https://doi.org/10.1002/aenm.202405301","url":null,"abstract":"Elevating the working voltage of sodium-ion batteries is crucial for expanding their application scenarios. However, as the operating voltage of these batteries increases, the interfacial stability of existing electrolytes becomes inadequate to meet the demands of high-voltage cathode materials. Along with the interaction with cathode interface, electrolyte trends to be decomposed forming an interphase between the cathode and electrolyte, which plays an essential role in the performance of batteries. This review systematically focuses on the reconstruction of cathode-electrolyte interphase maintaining the interfacial stability via various strategies at high voltage range. The state-of-the-art characterization techniques and modeling approaches associated with cathode-electrolyte interphase are also discussed. From the perspective of electrolyte design, the interphase reconstruction strategies focus on solvent molecule manipulation, solute ion manipulation, and the regulation of solvation-ion interaction. By summarizing strategies for constructing a stable CEI on the cathode, this review aims to provide new insights into achieving high-voltage sodium-ion batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"34 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142917614","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hanna Türk, Xuan Quy Tran, Patricia König, Adnan Hammud, Vaibhav Vibhu, Franz-Philipp Schmidt, Dirk Berger, Sören Selve, Vladimir Roddatis, Daniel Abou-Ras, Frank Girgsdies, Yu-Te Chan, Thomas Götsch, Hebatallah Ali, Izaak C. Vinke, L.G.J (Bert) de Haart, Michael Lehmann, Axel Knop-Gericke, Karsten Reuter, Rüdiger-A. Eichel, Christoph Scheurer, Thomas Lunkenbein
{"title":"Boon and Bane of Local Solid State Chemistry on the Performance of LSM-Based Solid Oxide Electrolysis Cells","authors":"Hanna Türk, Xuan Quy Tran, Patricia König, Adnan Hammud, Vaibhav Vibhu, Franz-Philipp Schmidt, Dirk Berger, Sören Selve, Vladimir Roddatis, Daniel Abou-Ras, Frank Girgsdies, Yu-Te Chan, Thomas Götsch, Hebatallah Ali, Izaak C. Vinke, L.G.J (Bert) de Haart, Michael Lehmann, Axel Knop-Gericke, Karsten Reuter, Rüdiger-A. Eichel, Christoph Scheurer, Thomas Lunkenbein","doi":"10.1002/aenm.202405599","DOIUrl":"https://doi.org/10.1002/aenm.202405599","url":null,"abstract":"High-temperature solid oxide cells are highly efficient energy converters. However, their lifetime is limited by rapid deactivation. Little is known about the local, atomic scale transformation that drive this degradation. Here, reaction-induced changes are unraveled at the atomic scale of a solid oxide electrolysis cell (SOEC) operated for 550 h by combining high-resolution scanning transmission electron microscopy with first-principles and force-field-based atomistic simulations. We focus on the structural evolution of lanthanum strontium manganite (LSM)/yttria-stabilized zirconia (YSZ) regions and the corresponding solid–solid interface. It is found that the strong inter-diffusion of cations leads to the additional formation and growth of a multitude of localized structures such as a solid solution of La/Mn, nano-domains of secondary structures or antisite defects in the YSZ, as well as a mixed ion and electron conduction region in the LSM and complexion. These local structures can be likewise beneficial or detrimental to the performance, by either increasing the catalytically active area or by limiting the supply of reactants. The work provides unprecedented atomistic insights into the influence of local solid-state chemistry on the functioning of SOECs and deepens the understanding of the degradation mechanism in SOECs, paving the way towards nanoscopic rational interface design for more efficient and durable cells.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"25 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2024-12-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142904966","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}