{"title":"Force‐Field Regulation Engineered Heterogeneous Graphene Micro‐Aerogels as Versatile Platforms for High‐Mass‐Loading Energy Storage","authors":"Jianren Wang, Tianshuo Yang, Adekunle Adedapo Obisanya, Yan Ma, Zhibin Ren, Xinyi Tan, Wenwei Lei, Ailing Song, Faming Gao","doi":"10.1002/aenm.202500992","DOIUrl":"https://doi.org/10.1002/aenm.202500992","url":null,"abstract":"Achieving high areal energy density requires the development of advanced electrodes capable of maintaining excellent performance under high mass‐loading conditions. Herein, a novel force‐field regulation strategy has been proposed to fabricate graphene oxide/exfoliated graphene heterogeneous micro‐aerogels (GM) electrodes with precisely engineered channel structures and interconnected conductive frameworks. This innovative design effectively mitigates the limitations of conventional graphene aerogels (GA) and graphene films (EGF), such as prolonged ion transport paths and severe internal potential gradients, particularly under high mass‐loading. As a result, GM electrode, with a high mass loading of 20 mg cm<jats:sup>−2</jats:sup>, demonstrates an outstanding capacitance of 2.53 F cm<jats:sup>−2</jats:sup> at an operational time of 200 s, and maintains a superior 58.7% capacitance retention at a shorter time of 5 s, significantly outperforming its GA and EGF counterparts. Moreover, GM architecture can serve as a universal platform to host redox‐active faradic materials (e.g., PANI, MnO<jats:sub>2</jats:sub>, and Co(OH)<jats:sub>2</jats:sub>), achieving exceptional areal capacitances up to 16.9 F cm<jats:sup>−2</jats:sup>, demonstrating its versatility and scalability for energy storage applications. The underlying mechanisms driving the superior performance of GM electrodes are comprehensively elucidated through multiscale characterizations, electrochemical analyses, and finite element simulations, offering a robust framework for the design of next‐generation high‐mass‐loading energy storage systems.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"22 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144520540","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}
Li Xu, Zhixian Mao, Junxian Liu, Mengfan Bi, Tengxiu Tu, Yongying Tian, Xiao Zhou, Jun Wu, Yijin Wu, Jianwei Su, Shan Chen, Huajie Yin
{"title":"Carbon‐Encapsulated CeO2‐Co Heterostructure via Tight Coupling Enables Corrosion‐Resistant Bifunctional Catalysis in Zinc‐Air Battery","authors":"Li Xu, Zhixian Mao, Junxian Liu, Mengfan Bi, Tengxiu Tu, Yongying Tian, Xiao Zhou, Jun Wu, Yijin Wu, Jianwei Su, Shan Chen, Huajie Yin","doi":"10.1002/aenm.202501790","DOIUrl":"https://doi.org/10.1002/aenm.202501790","url":null,"abstract":"Developing efficient bifunctional electrocatalysts for oxygen reduction (ORR) and oxygen evolution reactions (OER) is crucial to enhancing rechargeable zinc‐air batteries (ZABs). Here, a rationally designed catalyst consisting of nitrogen‐doped porous carbon‐encapsulated cobalt nanoparticles coupled tightly with CeO<jats:sub>2</jats:sub> nanoparticles (Co<jats:sub>NPs</jats:sub>/NC/CeO<jats:sub>2</jats:sub>) is reported, demonstrating superior bifunctional performance. In situ Raman and ATR‐FTIR spectroscopic analyses reveal that CeO<jats:sub>2</jats:sub> nanoparticles, located adjacent to cobalt nanoparticles, serve as electron modulators, suppressing the irreversible oxidation of metallic Co into CoOOH during OER, while promoting its reversible reduction back to Co during subsequent ORR. Additionally, CeO<jats:sub>2</jats:sub> effectively scavenges reactive oxygen species, significantly improving catalytic stability. Due to the synergy between Co and CeO<jats:sub>2</jats:sub> within the carbon matrix, Co<jats:sub>NPs</jats:sub>/NC/CeO<jats:sub>2</jats:sub> achieves a high ORR half‐wave potential (E₁/₂) of 0.86 V (vs RHE) with minimal performance loss (18 mV) after 10 000 cycles, an excellent OER overpotential of only 230 mV at 10 mA cm<jats:sup>−2</jats:sup>, and a low bifunctional potential gap (ΔE) of 0.60 V, surpassing commercial Pt/C + RuO<jats:sub>2</jats:sub>. When applied as a cathode in practical ZABs, the catalyst delivers exceptional specific capacity (814.7 mAh g<jats:sub>Zn</jats:sub><jats:sup>−1</jats:sup>), peak power density (254.6 mW cm<jats:sup>−</jats:sup><jats:sup>2</jats:sup>), and remarkable cycling durability over 2200 h.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"13 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144500794","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}
Christopher G. Bailey, Adrian Mena, Tik Lun Leung, Nicholas P. Sloane, Chwenhaw Liao, David R. McKenzie, Dane R. McCamey, Anita W. Y. Ho‐Baillie
{"title":"Revealing Localized Dark‐Exciton Populations in 2D Perovskites via Magneto‐Optical Microscopy","authors":"Christopher G. Bailey, Adrian Mena, Tik Lun Leung, Nicholas P. Sloane, Chwenhaw Liao, David R. McKenzie, Dane R. McCamey, Anita W. Y. Ho‐Baillie","doi":"10.1002/aenm.202501593","DOIUrl":"https://doi.org/10.1002/aenm.202501593","url":null,"abstract":"The successful development of optoelectronic devices is contingent on a detailed understanding of interactions between light and excited energy states in photoactive materials. In 2D perovskites, excitons are the dominant photogenerated species and their energetic structure plays a pivotal role, governing photon absorption and emission processes. In these materials, dark exciton states can undergo photoluminescence due to relaxation of selection rules and this process can be modulated by an external magnetic field, enabling unambiguous identification of the exciton fine structure. Previous reports of magneto‐optical spectroscopy on 2D perovskites are restricted to the macroscopic response, where key information is lost regarding the microscopic heterogeneity of the photoluminescence. Here, magneto‐optical microscopy is used for the first time on perovskite materials to elucidate the spatial variation of exciton emission processes. In 2D perovskite thin films, regions of localized bright and dark exciton populations are distinguished, correlated to the film morphology. In single crystals, dark excitons become localised at the edges, where excitons can be trapped in two distinct types of sub‐gap states. This work represents significant progress in understanding the properties of exciton emission in 2D perovskites, which is crucial for the development and optimization of optoelectronic technology.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"53 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144500793","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}
Jiarui Lin, Xiaoyan Shi, Junling Xu, Lianyi Shao, Zhipeng Sun
{"title":"Enabling Accelerated Na+ Dynamics Through Li‐Induced Electrostatic Shielding for High‐Performance Na3V2(PO4)2F3 Cathode","authors":"Jiarui Lin, Xiaoyan Shi, Junling Xu, Lianyi Shao, Zhipeng Sun","doi":"10.1002/aenm.202501979","DOIUrl":"https://doi.org/10.1002/aenm.202501979","url":null,"abstract":"Na<jats:sub>3</jats:sub>V<jats:sub>2</jats:sub>(PO<jats:sub>4</jats:sub>)<jats:sub>2</jats:sub>F<jats:sub>3</jats:sub> is an attractive cathode for sodium‐ion batteries due to its stable structure, high voltage, and impressive energy density. Nonetheless, its practical application is constrained by sluggish Na<jats:sup>+</jats:sup> diffusion kinetics and inferior rate capability, stemming from insufficient electronic conductivity, strong Coulombic attraction between mobile Na<jats:sup>+</jats:sup> with F<jats:sup>−</jats:sup>, and electrostatic repulsion among neighboring ions. Herein, Li‐doped Na<jats:sub>2.9</jats:sub>Li<jats:sub>0.1</jats:sub>V<jats:sub>2</jats:sub>(PO<jats:sub>4</jats:sub>)<jats:sub>2</jats:sub>F<jats:sub>3</jats:sub> is obtained to regulate the electronic environment within Na<jats:sup>+</jats:sup> diffusion channels. Theoretical calculations indicate that Li doping reduces electron density surrounding pendant F<jats:sup>−</jats:sup> and mitigates repulsive forces between adjacent Na<jats:sup>+</jats:sup> through electrostatic shielding, facilitating Na<jats:sup>+</jats:sup> mobility. Li doping also disrupts the ordered Na<jats:sup>+</jats:sup> arrangement, lowering the energy barrier for ion migration. Besides, the integration of carbon nanotube network and carbon‐coated aluminum foil substrate enhances external electronic conductivity and reduces polarization. In situ electrochemical impedance spectroscopy and distribution of relaxation times techniques confirm that these strategies lower charge transfer resistance during the sodium storage process. Hence, the optimized electrode delivers enhanced rate capability (75.27 mAh g<jats:sup>−1</jats:sup> at 50C) and outstanding long‐term cycling stability (with a capacity decay of only 0.0012% per cycle over 30000 cycles at 10C) in half‐cells and excellent rate performance across wide temperature range in full‐cells.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"631 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144500795","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}
Chandan Pramanik, Rabindranath Garai, Naga Prathibha Jasti, Nilanjana Nandi, Aditya D. Mohite, K. S. Narayan
{"title":"Direct Evaluation of Perovskite Solar Cell Performance and Stability Using Transient and Steady‐State Transport Measurements","authors":"Chandan Pramanik, Rabindranath Garai, Naga Prathibha Jasti, Nilanjana Nandi, Aditya D. Mohite, K. S. Narayan","doi":"10.1002/aenm.202502346","DOIUrl":"https://doi.org/10.1002/aenm.202502346","url":null,"abstract":"In this study, a direct correlation between charge transport properties and the stability of perovskite solar cells (PSCs) using time‐ and frequency‐domain measurements is provided. Faster charge carrier extraction and reduced nonradiative recombination serve as key indicators of stability and performance, implying the prevention of charge accumulation and defect formation, thereby reducing degradation. Stable, phase‐pure formamidinium lead iodide (FAPbI₃, or FAPI) templated with 2D perovskite‐based PSCs is compared, against conventional methylammonium chloride (MACl)‐stabilized FAPI‐based PSCs. Lattice‐engineered, strain‐relaxed growth in 2D‐templated FAPI‐based devices leads to enhanced charge extraction and faster transport timescales, as confirmed by Transient Photocurrent (TPC) and Intensity‐Modulated Photocurrent Spectroscopy (IMPS) measurements are demonstrated. Furthermore, Transient Photovoltage (TPV) and Impedance Spectroscopy (IS) reveal reduced non‐radiative recombination losses in these 2D‐templated FAPI devices. Moreover, the use of these techniques highlights their effectiveness in monitoring fundamental processes and deriving key parameters to evaluate the intrinsic stability of PSCs, also under prolonged UV light exposure. This integrated approach underscores the critical role of combining time and frequency‐domain analyses in understanding the performance, durability, and long‐term stability of PSCs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"17 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144500797","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":"Asymmetric Acceptor Featuring Fused‐Imidazole Central Core Enabling Organic Solar Cells with 19.4% Efficiency","authors":"Huihuang Zhang, Yongqiang Chai, Jinpeng Zhao, Enwei Zhu, Yu Chen, Liping Liu, Dirk M. Guldi","doi":"10.1002/aenm.202500332","DOIUrl":"https://doi.org/10.1002/aenm.202500332","url":null,"abstract":"Manipulating the central cores of non‐fullerene acceptors is crucial for enhancing the performance of organic solar cells (OSCs). While recent Y‐acceptors have leveraged a two‐dimensional (2D) π‐expansion strategy to incorporate symmetric fused‐pyrazine central cores, challenges remain in achieving higher device performance. In this study, BTQT‐4F, a novel Y‐acceptor with an asymmetric fused‐imidazole core is introduced. Density functional theory calculations reveal that the asymmetric geometry causes a molecular dipole moment of ≈8.5 Debye. Single‐crystal X‐ray diffraction confirms versatile packing modes that establish efficient 3D charge‐transport channels. Using BTQT‐4F, a power conversion efficiency (PCE) of 18.22% with an open‐circuit voltage (<jats:italic>V<jats:sub>OC</jats:sub></jats:italic>) of 0.890 V is achieved in PM6:BTQT‐4F binary OSCs. Notably, PM6:BTP‐eC9:BTQT‐4F ternary OSCs realized a PCE of 19.4%, surpassing previously reported efficiencies for OSCs based on 2D π‐conjugated Y‐acceptors. This work underscores the potential of implementing an asymmetric fused‐imidazole central core in pushing the boundaries of the Y‐acceptor design, opening avenues for further OSC performance enhancements.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"26 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144500791","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":"Ultra‐Fast Charging High‐voltage Spinel LiNi0.5Mn1.5O4 Batteries Enabled by Mn─O Bond Regulating Strategy to Defeat Jahn─Teller Distortion","authors":"Mengting Guo, Changping Wang, Yize Niu, Mingyue Ruan, Dong Yang, Fei Wang, Haonan Wang, Nankai Wang, Ying Jiang, Tianyi Li, Yan He, Qiang Li","doi":"10.1002/aenm.202502226","DOIUrl":"https://doi.org/10.1002/aenm.202502226","url":null,"abstract":"The high‐voltage spinel LiNi<jats:sub>0.5</jats:sub>Mn<jats:sub>1.5</jats:sub>O<jats:sub>4</jats:sub> (LNMO) is a promising cathode material for lithium‐ion batteries due to its high energy and power densities, excellent thermal stability, low cost, and environmental benignity. However, the presence of Mn<jats:sup>3+</jats:sup> induces Jahn─Teller (J─T) distortion, leading to Mn─O bond elongation, lattice stress, and degradation of both structural and electrochemical stability during cycling. To address this,a bond‐length engineering strategy is proposed by co‐doping Fe at the Mn 16d sites and Sb at the vacant 16c positions to suppress the J─T effect and stabilize the crystal structure. Electron paramagnetic resonance (EPR), in situ X‐ray diffraction (XRD), and density functional theory (DFT) calculations confirm that the Mn─O bond regulation strategy effectively mitigates MnO<jats:sub>6</jats:sub> octahedral distortion, reduces phase transitions, and enhances structural robustness. Moreover, Sb incorporation expands the lattice, facilitating Li<jats:sup>+</jats:sup> diffusion. As a result, the optimized FeSb‐LNMO delivers remarkable electrochemical performance, retaining 98% of its initial capacity after 200 cycles at 1C, and achieving 85.6% capacity retention over 1000 cycles at 5C. This work introduces a novel bond‐length engineering approach via multi‐site doping to overcome degradation in high‐voltage LNMO, enabling ultra‐fast charging and long‐term cycling stability.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"190 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144500792","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":"Seawater‐Adaptable Electrochemical Energy Conversion and Storage for Future Smart Ocean","authors":"Quanjun Tang, Yingxin Liu, Rongwei Meng, Ziyi Pan, Yuxiang He, Chen Zhang, Guowei Ling, Wei Chen, Quan‐Hong Yang","doi":"10.1002/aenm.202502407","DOIUrl":"https://doi.org/10.1002/aenm.202502407","url":null,"abstract":"Establishing a spatial marine energy network constitutes a pivotal pathway for realizing the smart ocean. Seawater has intrinsic advantages for use as an electrolyte in electrochemical energy conversion and storage systems due to its high conductivity. However, the complicated chemical nature of seawater imposes significant challenges in stabilizing the electrode/seawater interface. This perspective discusses recent strategies to enhance the seawater adaptability of electrode materials, with a focus on two reaction mechanisms: redox conversion and ion migration. For redox conversion, impurities like Cl<jats:sup>−</jats:sup>, Ca<jats:sup>2+</jats:sup>, Mg<jats:sup>2+</jats:sup>, and dissolved oxygen usually show a negative influence on the electrodes by causing shielding or poisoning. While for ion migration reactions, seawater as a high‐entropy electrolyte can supply sufficient charge carriers for ion storage, and the match between various ions and the electrode materials is critical for the high stability, capacity, and reversibility of the devices. State‐of‐the‐art advances in how to achieve seawater‐adaptability of the materials are comprehensively reviewed, and furthermore, the synergetic potential of coupling redox conversion and ion migration to construct new‐concept energy devices is underscored. The integration of these strategies into practical applications, addressing real‐world marine conditions, is proposed to pave the way toward robust, efficient, and sustainable marine energy systems.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"39 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144500796","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":"Stepwise Screening of Doping Elements for High‐Voltage LiCoO2 via Materials Genome Approach","authors":"Yutong Yao, Xiaokun Zhang, Zhiyu Xue, Xiehang Chen, Chunyue Li, Jixiao Li, Weidong Xue, Xiaobin Niu, Yong Xiang","doi":"10.1002/aenm.202502026","DOIUrl":"https://doi.org/10.1002/aenm.202502026","url":null,"abstract":"Lithium cobalt oxide (LCO), due to its high energy and compacted density, has attracted great interests and become a prevalent cathodes in consumer electronics. Elevating the charging cutoff voltage enables the attainment of higher specific capacity, but irreversible phase transitions and side reactions happened above 4.45 V would cause severe capacity fading in LCO. Although element doping is promising to improve the LCO performance under high voltages, only depending on the trial‐and‐error method for dopant selection is inefficient. Herein, this study examines the feasibility of doping strategies to alleviate the abovementioned high‐voltage LCO issues via materials genome approach combing theoretical calculation and experimental validation. Specifically, a five‐step pruning process is designed for 63 potential elements to evaluate their effectiveness in reducing chemo‐mechanical lattice strain, oxygen release, and cation mixing of LCO during cycling. The final candidates (Sb‐doped LCO/Ge‐doped LCO) are experimentally synthesized, with reduced lattice contraction, less intergranular microcracks, and fewer surface rock‐salt formation in comparison with undoped counterpart, thus exhibiting excellent electrochemical performance. The calculation data obtained from the screening process would benefit for rapid identification of promising dopants and act as a comprehensive map that provides rational guidance to future exploration of multielement doping recipes for high‐voltage LCO.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"48 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144500800","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}
Yijing Zhang, Zongyuan Yang, Mengyuan Li, Zhihui Wang, Yonglian Xiong, Xingyan Guo, Xueping Zong, Yang Wang, Mao Liang
{"title":"Indenocarbazole‐Engineered Self‐Assembled Monolayers with Sterically Tuned π‐Stacking for High‐Efficiency p–i–n Perovskite Solar Cells","authors":"Yijing Zhang, Zongyuan Yang, Mengyuan Li, Zhihui Wang, Yonglian Xiong, Xingyan Guo, Xueping Zong, Yang Wang, Mao Liang","doi":"10.1002/aenm.202501855","DOIUrl":"https://doi.org/10.1002/aenm.202501855","url":null,"abstract":"Terminal π‐extension is crucial for fabricating highly ordered self‐assembled monolayers (SAMs) that facilitate efficient hole transport in perovskite solar cells (PSCs). However, π‐expanded conjugation may compromise SAM film quality and ultimately degrading interfacial properties in p–i–n PSCs. To resolve this trade‐off, SAMs incorporating an indenocarbazole (InCz) terminal group are designed, which simultaneously addresses both molecular ordering and film formation challenges. The InCz‐terminated PAInCz demonstrates optimal balance through: 1) strengthened <jats:italic>π</jats:italic>‐interactions enabling dense, ordered molecular stacking, and 2) dimethyl steric hindrance enhancing film quality. Notably, while PAInCz exhibits superior performance‐including enhanced perovskite interfacial contact, robust ITO substrate anchoring, and favorable energy alignment, its <jats:italic>π</jats:italic>‐extended counterpart Ph‐PAInCz (featuring both extended terminal and linker groups) showed diminished device performance. This contrast highlights the importance of controlled π‐conjugation in SAM design. The optimized PAInCz‐based inverted PSCs achieved a champion power conversion efficiency of 25.51% with exceptional operational stability, maintaining > 85% of initial PCE after 500 h of continuous light soaking (AM1.5G) and thermal stress testing (65 °C). These findings provide fundamental insights into how the π‐extension terminal and linker of SAMs influence the performance of perovskite solar cells.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"428 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144478973","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}