{"title":"Pore‐Stitching Engineering of Biomass‐Derived Hard Carbon for Enhanced Sodium‐Ion Storage","authors":"Xueting Shen, Guiyu Liu, Wenjun Shi, Cheng Wang, Xuhui Li, Hongzhi Wang, Chengyu Yang, Yulin Cao, Lijie Ci, Hua Cheng, Zhouguang Lu","doi":"10.1002/aenm.71681","DOIUrl":"https://doi.org/10.1002/aenm.71681","url":null,"abstract":"Biomass‐derived hard carbon (HC) is a promising and cost‐effective anode for sodium‐ion batteries (SIBs). Prior to carbonization, biomass precursors are commonly subjected to acid/alkali purification to remove metallic and non‐metallic impurities. However, the accompanying ionic etching process often generates abundant through‐pores and disrupts the carbon framework, leading to increased irreversible capacity loss. Herein, we propose a “pore stitching” strategy using hydroxyethyl cellulose (HEC) as a functional reconstruction precursor. The hydroxyl‐rich HEC is proposed to interact with oxygen‐containing sites in the demineralized precursor and to be retained within accessible pore regions during mixing and drying. During subsequent carbonization, HEC‐derived carbon contributes to the reconstruction of the disrupted carbon framework, resulting in reduced open surface exposure and a redistributed micro/ultramicroporous architecture while preserving favorable Na <jats:sup>+</jats:sup> storage domains. Consequently, the optimized HC delivers a high reversible capacity of 375.3 mAh g <jats:sup>−</jats:sup> <jats:sup>1</jats:sup> at 20 mA g <jats:sup>−</jats:sup> <jats:sup>1</jats:sup> . A 700 mAh pouch cell pairing this HC with sodium iron phosphate pyrophosphate (Na <jats:sub>4</jats:sub> Fe <jats:sub>3</jats:sub> (PO <jats:sub>4</jats:sub> ) <jats:sub>2</jats:sub> P <jats:sub>2</jats:sub> O <jats:sub>7</jats:sub> , NFPP) delivers 150 Wh kg <jats:sup>−</jats:sup> <jats:sup>1</jats:sup> based on the combined active‐material mass of both electrodes and retains 97.8% capacity after 200 cycles at 1 C. This work provides a viable route for converting impurity‐rich agricultural waste into high‐performance HC anodes for practical sodium‐ion energy storage.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"14 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172906","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":"Photoelectrochemical Nitrate‐to‐Ammonia Conversion: Cocatalyst Design Principles and Mechanistic Insights from Electrocatalysis","authors":"Seongi Lee, Wonjin Jeong, Wan Jae Dong","doi":"10.1002/aenm.71692","DOIUrl":"https://doi.org/10.1002/aenm.71692","url":null,"abstract":"Photoelectrochemical reduction of nitrate to ammonia (PEC NO <jats:sub>3</jats:sub> RR) offers a solar‐driven route to NH <jats:sub>3</jats:sub> synthesis under ambient conditions, converting an environmental pollutant into a value‐added product. However, the overall performance of a PEC photoelectrode has been largely governed by the cocatalyst deposited on the light absorber since NO <jats:sub>3</jats:sub> RR conversion is kinetically demanding. Electrochemical NO <jats:sub>3</jats:sub> RR research has produced an extensive library of high‐performance catalysts together with a mature mechanistic understanding. Yet this knowledge has rarely been translated into photoelectrode design. This review summarizes recent advances in PEC NO <jats:sub>3</jats:sub> RR, spanning light‐absorber engineering, photoelectrode–cocatalyst integration, intrinsic semiconductor catalytic activity, and architectures that decouple light absorption from catalysis. On this basis, we reframe the electrochemical NO <jats:sub>3</jats:sub> RR catalyst library as a design resource for PEC cocatalysts and identify key evaluation criteria, such as catalytic activity, interfacial charge‐transfer, optical shading, and stability under illumination and electrically biased conditions. By bridging the mechanistic maturity of electrochemistry with the energetic advantages of photoelectrochemistry, this review provides a coherent design framework for advancing PEC NH <jats:sub>3</jats:sub> synthesis.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"11 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172681","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":"Dual Descriptor‐Guided Design of Hydrated Eutectic Electrolytes for Stable Zinc Batteries","authors":"Qian Li, Chen Zhang, Yida Hu, Xueer Xu, Mingyue Zhu, Yu Zhong, Jiangping Tu, Changdong Gu","doi":"10.1002/aenm.71695","DOIUrl":"https://doi.org/10.1002/aenm.71695","url":null,"abstract":"Aqueous zinc‐ion batteries promise large‐scale storage, yet anode irreversibility remains the principal barrier. Eutectic electrolytes, comprising hydrogen‐bond donors (HBDs) and acceptors (HBAs), can suppress H <jats:sub>2</jats:sub> O activity and regulate Zn <jats:sup>2+</jats:sup> desolvation through hydrogen‐bond networks, offering a promising remedy. However, the screening of polyol‐based HBDs still relies on empirical trials, lacking quantitative molecular criteria. Herein, two orthogonal descriptors, effective hydroxyl density (EOD) and minimum electrostatic potential (MEP), are proposed based on the saturation and directionality of hydrogen bonds to evaluate polyols from two aspects of hydrogen‐bond network formation and Zn <jats:sup>2+</jats:sup> coordination. A series of C <jats:sub>2</jats:sub> –C <jats:sub>6</jats:sub> polyols are explored for hydrated eutectic electrolytes, revealing inconsistency between bulk hydrogen‐bond strength and battery performance. Erythritol (Ery, C <jats:sub>4</jats:sub> , EOD = 0.022 Å <jats:sup>−3</jats:sup> , MEP = −1.73 eV) optimizes interfacial adsorption stability and desolvation kinetics. It constructs an Ery‐enriched interfacial layer to induce preferred (101) Zn texture. The symmetric cell stably cycles over 6740 h at 2 mA cm <jats:sup>−2</jats:sup> with 1 mAh cm <jats:sup>−2</jats:sup> , and the Zn||I <jats:sub>2</jats:sub> full cell exhibited 11 400 cycles at 10 C. This work establishes theoretical design principles for the selection of polyol HBDs when keeping the HBA component fixed as a zinc salt, shifting the paradigm from trial and error to rational design.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"53 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172628","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}
Tianyu Jia, Mengnan Ruan, Chengyi Wang, Li Zhou, Zhifeng Liu
{"title":"Jahn–Teller Distortion of MnO 6 Octahedra Enhances Piezoelectric Polarization and Lattice Oxygen Activation of BaTiO 3 for Efficient Piezo‐PEC Water Splitting","authors":"Tianyu Jia, Mengnan Ruan, Chengyi Wang, Li Zhou, Zhifeng Liu","doi":"10.1002/aenm.71700","DOIUrl":"https://doi.org/10.1002/aenm.71700","url":null,"abstract":"Piezo‐photoelectrochemical (Piezo‐PEC) water splitting enables efficient solar conversion, yet its practical implementation is limited by an insufficient piezoelectric polarization field and sluggish water‐splitting kinetics. Herein, we firstly propose a Jahn–Teller effect‐driven strategy to regulate the local B‐site octahedral structure of perovskite BaTiO <jats:sub>3</jats:sub> for efficient Piezo‐PEC water splitting. By introducing Mn <jats:sup>3+</jats:sup> ions with asymmetric e <jats:sub>g</jats:sub> orbital occupancy (t <jats:sub>2g</jats:sub> <jats:sup>3</jats:sup> e <jats:sub>g</jats:sub> <jats:sup>1</jats:sup> ), a local MnO <jats:sub>6</jats:sub> octahedral coordination environment is constructed and pronounced Jahn–Teller distortion is induced. Experimental characterizations and density functional theory (DFT) calculations reveal that the Jahn–Teller distortion drives the cooperative displacement of Ti and O atoms and enhances crystal non‐centrosymmetry, thereby generating a stronger piezoelectric polarization field under mechanical stress. Meanwhile, the introduction of Mn <jats:sup>3+</jats:sup> strengthens Ti─O bond covalency, thereby activating lattice oxygen species and promoting the water‐splitting pathway from the conventional adsorbate evolution mechanism (AEM) toward the lattice oxygen mechanism (LOM), thus accelerating reaction kinetics. Under coupled ultrasonic vibration and illumination, the optimized BTMO‐6 photoanode delivers a high photocurrent density of 2.18 mA cm <jats:sup>−2</jats:sup> at 1.23 V <jats:sub>RHE</jats:sub> and exhibits a piezoelectric coefficient (d <jats:sub>33</jats:sub> ) of 52.3 pm V <jats:sup>−1</jats:sup> . This work reveals that Jahn–Teller distortion simultaneously enhances piezo‐polarization and tunes reaction pathways, offering new insights for robust Piezo‐PEC water‐splitting systems.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"471 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172629","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}
Yanxue Wang, Roman Kučera, Sinuhé Perea‐Puente, Mykhailo Sytnyk, Andrew Hainer, Zijian Peng, Savannah Bennett, Juan S. Rocha‐Ortiz, Albert These, Hakan U Dag, Qi Fan, Anastasia Barabash, Zhenni Wu, Chaohui Li, Jens Hauch, Olga Kasian, Christoph J. Brabec, Ian Marius Peters
{"title":"Nickel‐Free Perovskite Solar Cells Enabled by Self‐Assembled Monolayers: A Pathway to Efficient and Recyclable Devices","authors":"Yanxue Wang, Roman Kučera, Sinuhé Perea‐Puente, Mykhailo Sytnyk, Andrew Hainer, Zijian Peng, Savannah Bennett, Juan S. Rocha‐Ortiz, Albert These, Hakan U Dag, Qi Fan, Anastasia Barabash, Zhenni Wu, Chaohui Li, Jens Hauch, Olga Kasian, Christoph J. Brabec, Ian Marius Peters","doi":"10.1002/aenm.71693","DOIUrl":"https://doi.org/10.1002/aenm.71693","url":null,"abstract":"High efficiency inverted perovskite solar cells often rely on nickel‐containing hole‐selective interfaces such as NiOx. However, the use of nickel presents sustainability challenges, as the material is inherently toxic and cross‐contamination during end‐of‐life processing can compromise material recovery and recyclability. Here, we develop a nickel‐free hole‐selective interface material based on phenyl‐substituted phosphonic‐acid carbazole self‐assembled monolayers (Ph‐nPACz). Candidate molecules were identified through rational structure‐property screening of the substituents of the carbazole core, anchoring groups and linkers. Among this molecular family, Ph‐5PACz delivers the best overall performance, offering improved interfacial wettability and enhanced buried‐interface stability compared to the NiOx/Me‐4PACz reference. Devices incorporating Ph‐5PACz achieve a power conversion efficiency of 25.3%, compared to 21.7% for the control, driven by a higher fill factor and efficient charge extraction. The chemical robustness of the nickel‐free interface enables a closed‐loop recycling route unavailable to nickel‐based devices, with recycled‐ITO devices retaining close to 98% of their initial performance. Coupled life‐cycle and techno‐economic analyses further indicate substantial sustainability gains, including reduced energy demand, markedly lower raw metal usage and toxicity‐related impacts, and a generalized reduction of up to 29% across ReCiPe endpoint indicators.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"21 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172631","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":"Gravity‐Differential Modulated Triboelectric Nanogenerator for Continuous and Stable Energy Harvesting From Disordered Vibrations","authors":"Sheng Zhang, Yuhe Wu, Menghe Gao, Yinxi Da, Miaoze Min, Yijia Dong, Qiang Tang, Cheng Xu","doi":"10.1002/aenm.71688","DOIUrl":"https://doi.org/10.1002/aenm.71688","url":null,"abstract":"Low‐frequency, random, and intermittent vibrational energy is an important energy source for self‐powered sensing systems in engineering environments. However, the high dependence of triboelectric nanogenerators on periodic excitation limits their continuous energy output. Here, a gravity‐differential modulated triboelectric nanogenerator (GDM‐TENG) is proposed to transform intermittent vibrations into a continuously enhanced energy conversion process. Through the synergistic effect of mechanical rectification, inertial energy storage, gravity‐driven propulsion, and differential motion amplification, the GDM‐TENG directionally transmits and delays the release of discrete vibrational inputs, thereby forming a more continuous and higher‐frequency relative sliding motion at the triboelectric interface and improving the effective charge transfer rate per unit time. Compared to the single pendulum system, the double‐sided pendulum shortens the energy storage time by 64.2%, compressing the energy response to the millisecond level, while increasing output power by 2.81 times and capacitor charging rate by 2.55 times. After 216,000 cycles, the voltage output of the GDM‐TENG remains almost unchanged, indicating its excellent long‐term operational stability. Furthermore, combined with a power management circuit, the GDM‐TENG can stably charge a 1000 µF capacitor and power warning lights and acoustic flame sensors. This work provides a design idea for distributed self‐powered sensing systems toward the infrastructure monitoring.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"13 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172630","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}
Yin Yang, Henglong Ren, Maoxin Cai, Xinlong Ma, Yongfeng Li
{"title":"Catalytic Activity Matching Governs Scaffold–Coating Competition in Silicon Anodes","authors":"Yin Yang, Henglong Ren, Maoxin Cai, Xinlong Ma, Yongfeng Li","doi":"10.1002/aenm.71685","DOIUrl":"https://doi.org/10.1002/aenm.71685","url":null,"abstract":"Carbon scaffolds are widely used to accommodate lithiation‐induced volume changes of silicon (Si) nanoparticles and maintain electrode integrity, yet whether increasing scaffold rigidity provides sufficient mechanical benefit to offset its cost in surface coating quality remains unexamined. The scaffold template and the native SiO <jats:sub>x</jats:sub> on Si surfaces compete for the same finite carbon source, so that scaffold wall thickness and coating uniformity are inversely coupled rather than independently tunable. We formalize this coupling as catalytic activity matching and probe it using MgSO <jats:sub>4</jats:sub> and CaSO <jats:sub>4</jats:sub> whisker templates, whose activity contrast is quantified by density functional theory and H <jats:sub>2</jats:sub> temperature‐programmed reduction. The high‐activity MgSO <jats:sub>4</jats:sub> template diverts carbon flux toward the scaffold, leaving nonuniform Si coatings, whereas the moderate‐activity CaSO <jats:sub>4</jats:sub> template yields a compliant scaffold with uniform coatings. The uniform coating governs solid electrolyte interphase quality, while the compliant scaffold reduces peak lithiation stress to only 53.4% of its rigid counterpart. The matched CaSO <jats:sub>4</jats:sub> system delivers 91.0% initial Coulombic efficiency and enables full cells up to 510 Wh kg <jats:sup>−1</jats:sup> (based on the combined mass of active materials). Matching rather than maximizing template catalytic activity is thus established as a general design principle for balancing scaffold formation and Si‐surface protection in template‐catalyzed CVD.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"11 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149130506","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}
Bing Xie, Yuhang Hu, Wenqiang Xiang, Zhiyong Liu, Kun Guo, Haibo Zhang, Huajie Luo, Tianyu Li
{"title":"Local Atomic Disorder‐Driven Deep Relaxor State for Ultrahigh Dielectric Energy Storage With High Thermal Stability","authors":"Bing Xie, Yuhang Hu, Wenqiang Xiang, Zhiyong Liu, Kun Guo, Haibo Zhang, Huajie Luo, Tianyu Li","doi":"10.1002/aenm.71652","DOIUrl":"https://doi.org/10.1002/aenm.71652","url":null,"abstract":"Lead‐free dielectric ceramic capacitors are indispensable for advanced high‐power electronic pulse systems owing to their exceptional power density and rapid charge‐discharge kinetics. However, the simultaneous realization of ultrahigh recoverable energy density ( <jats:italic>W</jats:italic> <jats:sub>rec</jats:sub> ) and high efficiency ( <jats:italic>η</jats:italic> ), especially with robust thermal stability, remains challenging. Here, we propose a local structural design strategy focused on implementing atomic‐scale disorder within relaxor ferroelectrics to achieve a deep relaxor state across a wide temperature window. Atomic‐scale structure characterizations reveal that this local chemical/structural disorder induces ultrafine, highly active polar nanoregions, fostering an optimized polarization response while remaining resilient against thermal fluctuations. Consequently, the designed ceramics exhibit superior energy‐storage performance, characterized by a large <jats:italic>W</jats:italic> <jats:sub>rec</jats:sub> of 13.1 J cm <jats:sup>−3</jats:sup> and ultrahigh <jats:italic>η</jats:italic> of 93%, leading to a high figure of merit up to 187.1. Notably, exceptional performance stability across diverse operating conditions is bestowed, with <jats:italic>η</jats:italic> remaining above 90% at temperatures up to 200°C. This study thus provides a robust paradigm for designing dielectric capacitors that deliver both high energy‐storage performance and reliability in harsh working environments.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"407 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149130490","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":"Ni‐MOFs Mediated Ni 2+/4+ Balancing and Enhanced Metal–Oxygen Covalency Unlocks Fast and Stable Sodium Storage in High‐Entropy Layered Cathode","authors":"Shengkui Zhong, Bo Yang, Jishu Zeng, Xingyu Luo, Jiequn Liu, Zejun Jiang, Yanfang Wang, Fangping Wang, Xueling Hu, Huijue Luo, Yan Su, Zongkang Sun, Zhuokui Zhong, Shibao Tang, Renzong Hu, Wei Li, Fanbo Meng","doi":"10.1002/aenm.71686","DOIUrl":"https://doi.org/10.1002/aenm.71686","url":null,"abstract":"O3‐type cathodes suffer from heterogeneous metal distribution and insufficient active nickel content, limiting specific capacity, cyclic stability, and electrochemical kinetics. Herein, Ni‐based metal‐organic frameworks (Ni‐MOFs) are applied as precursors to enable atomic‐level control over regulated active nickel content and metal‐oxygen bonds in high‐entropy NaTMO <jats:sub>2</jats:sub> cathodes. It is found that the introduction of Ni‐MOFs can accelerate the crystallization and purity of O3‐type structures. Ni‐MOFs‐derived high‐entropy cathode (M‐HEO) exhibits an optimized electrochemically active Ni <jats:sup>2+</jats:sup> , which can balance the capacity depth and structural stability, contrasting with excessive Ni <jats:sup>2+</jats:sup> in normal high‐entropy oxide or insufficient Ni <jats:sup>2+</jats:sup> in commercial oxide. Concurrently, enhanced transition metal‐oxygen covalency, especially Ni‐O covalency, could form a robust metal‐oxygen network with an ultrafast Na <jats:sup>+</jats:sup> transport path and suppress lattice degradation. The reinforced covalent Ni‐O‐TM network enables a highly reversible phase transition with a small volume change, as well as the modified, thinner double‐layer cathode‐electrolyte interface, together with fast Na <jats:sup>+</jats:sup> ion transport kinetics. As a result, M‐HEO delivers a higher discharge capacity of ∼130 mAh g <jats:sup>−1</jats:sup> with an initial Coulombic efficiency of 92.6% under 0.1C and stable cyclic property under 1C and 2C.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"10 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149130501","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}
Huyen Tran, Dong Gyu Lee, Ahreum Lee, Inchan Hwang, Van Hung Tran, Jun Hyeok Choi, Junseop Byeon, Yu Jin Kim, Sang Hwan Nam, Jihye Gwak, Seung Kyu Ahn, Sungjun Hong, Kihwan Kim, Bong Joo Kang, Minwoo Park, SeJin Ahn, Tae Kyung Lee, Inyoung Jeong
{"title":"Counter‐Halide‐Directed Ion‐Pair Passivation Enables High‐Performance Wide‐Bandgap Perovskites for Perovskite/Cu(in,Ga)Se 2 Tandem Solar Cells","authors":"Huyen Tran, Dong Gyu Lee, Ahreum Lee, Inchan Hwang, Van Hung Tran, Jun Hyeok Choi, Junseop Byeon, Yu Jin Kim, Sang Hwan Nam, Jihye Gwak, Seung Kyu Ahn, Sungjun Hong, Kihwan Kim, Bong Joo Kang, Minwoo Park, SeJin Ahn, Tae Kyung Lee, Inyoung Jeong","doi":"10.1002/aenm.71691","DOIUrl":"https://doi.org/10.1002/aenm.71691","url":null,"abstract":"Wide‐bandgap (WBG) perovskites (PVSK) are key top‐cell absorbers for tandem photovoltaics but remain limited by severe open‐circuit voltage ( <jats:italic>V</jats:italic> <jats:sub>OC</jats:sub> ) losses and photoinduced halide segregation. Since iodide‐ and bromide‐related defects coexist at the surface and bulk of Br/I mixed‐halide WBG PVSK, the counter‐halide identity in ammonium passivators may critically influence defect passivation effectiveness. Moreover, while deprotonation of ammonium passivator has emerged as an important factor governing interfacial stability, its discussion has focused mainly on organic cation structure, leaving the counter‐halide's role in regulating deprotonation‐driven side reactions largely unexplored. Here, we establish a counter‐halide‐directed ion‐pair passivation strategy using 4‐fluorobenzylammonium halides (FBz‐Cl, FBz‐Br, and FBz‐I). Density functional theory calculations combined with optoelectronic and interfacial characterizations reveal that the counter‐halide simultaneously governs defect‐binding affinity, nonradiative recombination, energy‐level alignment, and deprotonation‐driven degradation. Among the passivators, FBz‐Br achieves the optimal balance of strong defect passivation, favorable band alignment with C <jats:sub>60</jats:sub> , and enhanced stability. Consequently, FBz‐Br‐treated PVSK exhibits suppressed nonradiative recombination and reduced <jats:italic>V</jats:italic> <jats:sub>OC</jats:sub> deficit, delivering a power conversion efficiency (PCE) of 21.89% with improved resistance to moisture, thermal, and light‐induced degradation. Integrated with Cu(In,Ga)Se <jats:sub>2</jats:sub> (CIGS) bottom cells, the optimized WBG PVSK enables PVSK/CIGS tandem solar cells with PCEs of 29.51% in four‐terminal and 25.65% in two‐terminal configurations.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"29 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149130500","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}