Jamil Ur Rahman, Shuping Guo, Nicolás Pérez, Kyuseon Jang, Chanwon Jung, Pingjun Ying, Christina Scheu, Duncan Zavanelli, Siyuan Zhang, Andrei Sotnikov, Gerald Jeffrey Snyder, Jeroen van den Brink, Kornelius Nielsch, Ran He
{"title":"Grain Boundary Engineering Enhances the Thermoelectric Properties of Y2Te3","authors":"Jamil Ur Rahman, Shuping Guo, Nicolás Pérez, Kyuseon Jang, Chanwon Jung, Pingjun Ying, Christina Scheu, Duncan Zavanelli, Siyuan Zhang, Andrei Sotnikov, Gerald Jeffrey Snyder, Jeroen van den Brink, Kornelius Nielsch, Ran He","doi":"10.1002/aenm.202404243","DOIUrl":"https://doi.org/10.1002/aenm.202404243","url":null,"abstract":"The performance of thermoelectric materials is typically assessed using the dimensionless figure of merit, <jats:italic>zT</jats:italic>. Increasing <jats:italic>zT</jats:italic> is challenging due to the intricate relationships between electrical and thermal transport properties. This study focuses on Y<jats:sub>2</jats:sub>Te<jats:sub>3</jats:sub>‐based thermoelectric materials, which are predicted to be promising for high‐temperature applications due to their inherently low lattice thermal conductivity. A series of Y<jats:sub>2+</jats:sub><jats:italic><jats:sub>x</jats:sub></jats:italic>Te<jats:sub>3</jats:sub> compositions with excess Y is synthesized to explore the effects on electronic and structural characteristics. Density functional theory calculations suggest that additional Y atoms increase charge carriers, thereby enhancing electrical conductivity and boosting thermoelectric performance. X‐ray diffraction analysis reveals that the presence of excess Y reduces lattice volume and alters bonding structures. Furthermore, the addition of Bi significantly enhances the power factor by promoting the segregation of elemental Bi particles and the formation of Y‐Bi‐rich grain boundaries, which improve weighted mobility. This microstructural optimization leads to a fourfold increase in the Seebeck coefficient, resulting in a peak <jats:italic>zT</jats:italic> of 1.23 at 973 K and a predicted maximum conversion efficiency of 10.3% under a temperature difference of 673 K. These findings highlight the potential of Y<jats:sub>2</jats:sub>Te<jats:sub>3</jats:sub> for high‐temperature thermoelectric applications and demonstrate the effectiveness of grain boundary engineering in enhancing thermoelectric performance.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"50 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758363","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}
Senke Tan, Rui Zeng, Jiawei Deng, Fei Han, Yi Lin, Fan Xu, Lixuan Kan, Zheng Tang, Yufei Gong, Ming Zhang, Lei Zhu, Guanqing Zhou, Xingyu Gao, Xiaojun Li, Xiaonan Xue, Hao Jing, Yongming Zhang, Shengjie Xu, Feng Liu
{"title":"Dimeric Acceptors Using Different Central Linkers to Manipulate Electronic and Morphological Properties","authors":"Senke Tan, Rui Zeng, Jiawei Deng, Fei Han, Yi Lin, Fan Xu, Lixuan Kan, Zheng Tang, Yufei Gong, Ming Zhang, Lei Zhu, Guanqing Zhou, Xingyu Gao, Xiaojun Li, Xiaonan Xue, Hao Jing, Yongming Zhang, Shengjie Xu, Feng Liu","doi":"10.1002/aenm.202404567","DOIUrl":"https://doi.org/10.1002/aenm.202404567","url":null,"abstract":"Dimerized acceptors show promise in combining the high performance of small‐molecule non‐fullerene acceptors (NFAs) with the excellent stability of polymer acceptors. The central linking units that connect two acceptor molecules together have a profound impact on dimeric acceptor properties and structure‐performance relationships in blended thin films. It is seen that different linkers significantly affect the electronic properties and morphology in blended thin film. The electron‐donating linker elevates the absorption coefficient, affords a lower bandgap, and reduces energy loss, and thus better photovoltaic device performance. Better fibrillar morphology can be obtained. The best material DY‐EDOT‐based device shows a power conversion efficiency (PCE) of 18.21%, an open‐circuit voltage (<jats:italic>V</jats:italic><jats:sub>oc</jats:sub>) of 0.924 V, a short‐circuit current density (<jats:italic>J</jats:italic><jats:sub>sc</jats:sub>) of 25.20 mA cm<jats:sup>−2</jats:sup>, a fill factor (FF) of 78.19%, which is among the highest value for dimerized acceptors. This study reveals the fundamental importance of linker units in determining the dimerized acceptor properties and provides useful strategies for developing oligomeric and polymeric acceptors, which is critical in simultaneously improving the performance and stability of organic solar cells (OSCs).","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"116 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758362","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":"Spatial Confinement Effect of Mineral‐Based Colloid Electrolyte Enables Stable Interface Reaction for Aqueous Zinc–Manganese Batteries","authors":"Chuancong Zhou, Zhenming Xu, Qing Nan, Jie Zhang, Yating Gao, Fulong Li, Zaowen Zhao, Zhenyue Xing, Jing Li, Peng Rao, Zhenye Kang, Xiaodong Shi, Xinlong Tian","doi":"10.1002/aenm.202405387","DOIUrl":"https://doi.org/10.1002/aenm.202405387","url":null,"abstract":"The rational design of inorganic colloid electrolytes enables the manipulation of the solvation structure of Zn<jats:sup>2+</jats:sup> ions and addresses zinc dendrite formation and manganese dissolution in aqueous zinc–manganese batteries. In this study, magnesium aluminosilicate (MAS) powder is used to fabricate a mineral‐based colloid electrolyte for Zn//α‐MnO<jats:sub>2</jats:sub> batteries. According to theoretical calculations, MAS has a stronger binding energy with Zn<jats:sup>2+</jats:sup>/Mn<jats:sup>2+</jats:sup> ions than with H<jats:sub>2</jats:sub>O molecules, suggesting the possibility of regulating the solvation structure of Zn<jats:sup>2+</jats:sup>/Mn<jats:sup>2+</jats:sup> ions in a MAS–colloid electrolyte. Based on the experimental results, a high ionic conductivity, wide operating voltage, low activation energy barrier, and stable pH environment is achieved in the MAS–colloid electrolyte. As expected, long‐term cyclic stability can be maintained for 3500 h at 0.2 mA cm<jats:sup>−2</jats:sup> in Zn//Zn cells, and high capacities of 255.5 and 239.8 mAh g<jats:sup>−1</jats:sup> are retained at 0.2 and 0.5 A g<jats:sup>−1</jats:sup> after 100 cycles in Zn//α‐MnO<jats:sub>2</jats:sub> batteries, respectively. This performance is attributed to the spatial confinement effect of MAS on the active H<jats:sub>2</jats:sub>O molecules, which effectively reshapes the solvation structure of Zn<jats:sup>2+</jats:sup> ions, guaranteeing reversible zinc deposition, suppressing active manganese dissolution, and ensuring stable interfacial reactions. This work will drive the development of mineral‐based electrolytes in zinc‐based batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"18 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758360","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}
Yujing Zhang, Yiming Zhang, Xiaoyi Wang, Haochen Gong, Yu Cao, Kang Ma, Shaojie Zhang, Shaowei Wang, Wensheng Yang, Lve Wang, Jie Sun
{"title":"Trace Multifunctional Additive Enhancing 4.8 V Ultra-High Voltage Performance of Ni-Rich Cathode and SiOx Anode Battery","authors":"Yujing Zhang, Yiming Zhang, Xiaoyi Wang, Haochen Gong, Yu Cao, Kang Ma, Shaojie Zhang, Shaowei Wang, Wensheng Yang, Lve Wang, Jie Sun","doi":"10.1002/aenm.202403751","DOIUrl":"https://doi.org/10.1002/aenm.202403751","url":null,"abstract":"The combination of high-voltage Ni-rich cathodes and high-capacity Si-based anodes can result in high energy density for next-generation batteries. However, the practical capacities accesses are severely hindered by unstable electrode/electrolyte interphases (EEI) and irreversible structural degradation, which necessitates efficient additives in electrolyte for generating stable EEI. Herein, a multifunctional additive, 3-Fluoro-5-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)picolinonitrile (FTDP) is proposed to construct robust interfaces at both cathodic and anodic surface, so as to enhance electrochemical performance. FTDP is preferentially decomposed to form B-contained and cyano (CN) group-rich cathode electrolyte interphase (CEI), as well as LiF-, Li<sub>3</sub>N-rich solid electrolyte interphase (SEI), simultaneously, resulting in the integrity and stability of electrodes. Moreover, the FTDP-derived CEI can suppress transition metal ions dissolution, further facilitating battery cyclability. The multifunctionality of FTDP, including quenching free radicals, alleviating the hydrolysis of LiPF<sub>6</sub> and inhibiting HF generation, thus greatly improving interfacial stability. With trace addition of 0.2 wt.%, NCM811/Li cell can be performed at an extreme condition, i.e., ultra-high voltage (4.8 V), high temperature (60 °C) and high rate (10C). 1.6 Ah NCM811/SiO<sub>x</sub> pouch cell delivers a high capacity retention of 84.0% after 300 cycles.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"66 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142760410","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}
Yuan Teng, Jing Zhao, Zi‐Ming Ye, Chao‐Wen Tan, Ling‐Ling Ning, Yi‐Yang Zhou, Zhilian Wu, Dai‐Bin Kuang, Youji Li
{"title":"Covalent Organic Framework Encapsulating Layered Oxide Perovskite for Efficient Photosynthesis of H2O2","authors":"Yuan Teng, Jing Zhao, Zi‐Ming Ye, Chao‐Wen Tan, Ling‐Ling Ning, Yi‐Yang Zhou, Zhilian Wu, Dai‐Bin Kuang, Youji Li","doi":"10.1002/aenm.202404029","DOIUrl":"https://doi.org/10.1002/aenm.202404029","url":null,"abstract":"Driving efficient artificial photosynthesis of H<jats:sub>2</jats:sub>O<jats:sub>2</jats:sub> is highly desirable in both academic and industrial fields. Here, a new core–shell Bi<jats:sub>3</jats:sub>TiNbO<jats:sub>9</jats:sub>@C<jats:sub>4</jats:sub>N heterojunction is constructed for efficient photocatalytic H<jats:sub>2</jats:sub>O<jats:sub>2</jats:sub> production by in situ encapsulating an ultrathin layer of covalent organic framework material (C<jats:sub>4</jats:sub>N) on Aurivillius‐type Bi<jats:sub>3</jats:sub>TiNbO<jats:sub>9</jats:sub> microsheets. The porous C<jats:sub>4</jats:sub>N layer is found to enhance visible‐light absorption ability and facilitate the adsorption and activation of the reactants and intermediates. The hybrid heterojunction follows an S‐scheme charge transfer with the assistance of a strong internal electric field (IEF), which promotes the spatial separation of photogenerated carriers effectively and maintains their strong redox abilities. As a result, the optimized Bi<jats:sub>3</jats:sub>TiNbO<jats:sub>9</jats:sub>@C<jats:sub>4</jats:sub>N unveils a high H<jats:sub>2</jats:sub>O<jats:sub>2</jats:sub> yield rate of 1.25(2) mmol g<jats:sup>−1</jats:sup> h<jats:sup>−1</jats:sup> in the absence of sacrificial agents and cocatalyst, 10.9 and 3.5 folds higher than those of pristine Bi<jats:sub>3</jats:sub>TiNbO<jats:sub>9</jats:sub> and C<jats:sub>4</jats:sub>N catalysts, respectively. This work provides an in situ encapsulating strategy to decorate covalent organic frameworks (COFs) on oxide perovskites for artificial photosynthesis of H<jats:sub>2</jats:sub>O<jats:sub>2</jats:sub>, which may stimulate the intensive investigation interests of functional materials/COFs heterojunction materials for various photocatalysis applications.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"205 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758361","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}
Peng Gu, Yidong Song, Yihe Fan, Xin Meng, Jin Liu, Guofeng Wang, Zhouguanwei Li, Heyuan Sun, Ziyu Zhao, Jinlong Zou
{"title":"Crystalline‐Amorphous Interface‐Triggered Electron Redistribution on Copper(II) Sulfide@Metal (Ni, Co, and Fe) Oxyhydroxides for Ultra‐Efficient Overall Water/Seawater Splitting","authors":"Peng Gu, Yidong Song, Yihe Fan, Xin Meng, Jin Liu, Guofeng Wang, Zhouguanwei Li, Heyuan Sun, Ziyu Zhao, Jinlong Zou","doi":"10.1002/aenm.202403657","DOIUrl":"https://doi.org/10.1002/aenm.202403657","url":null,"abstract":"Rearranging the electronic orbitals of metal sites through interface engineering is the breakthrough for achieving high efficiencies in hydrogen/oxygen evolution reactions (HER/OER) on bimetallic catalysts. Here, via a multistep liquid‐phase synthesis strategy, the crystalline‐amorphous (c‐a) interface is built by coating amorphous oxyhydroxide layer on the surface of crystallized copper(II) sulfide (CuS@MOOH, M = iron (Fe), cobalt (Co) and nickel (Ni)) with an internal cavity. For HER, c‐a interface facilitates the electron filling of the 3d orbitals of Cu, thereby enhancing the coordination between Cu sites (Cu<jats:sup>2+</jats:sup>/Cu<jats:sup>+</jats:sup>) and *H and reducing the energy barrier for *H adsorption. For OER, c‐a interface triggers electronic rearrangement in the 3d orbitals of M sites, prompting electron transition from the t2g orbitals to the eg orbitals to achieve a half‐filled state, optimizing the oxygen‐intermediates adsorption on M sites (M<jats:sup>3+</jats:sup>/M<jats:sup>4+</jats:sup>). Among CuS@MOOH, the as‐marked CuS@CoOOH‐6 exhibits the best activities with ultra‐low overpotentials of 62 mV (HER) and 136 mV (OER). Only 1.52 V is sufficient to power the electrolyzer with CuS@CoOOH‐6‐based cathode/anode, maintaining a ultra‐stable efficiency (96.9 %) over 72 h. Notably, CuS@CoOOH‐6 also exhibits impressive activity/durability for natural seawater electrolysis. This study enhances understanding of the properties and electronic structure of the c‐a interface for water splitting.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"27 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758364","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":"Regulating Compressive Strain Enables High-Performance Tin-Based Perovskite Solar Cells","authors":"Jialun Jin, Zhihao Zhang, Shengli Zou, Fangfang Cao, Yuanfang Huang, Yiting Jiang, Zhiyu Gao, Yuliang Xu, Junyu Qu, Xiaoxue Wang, Cong Chen, Chuanxiao Xiao, Shengqiang Ren, Dewei Zhao","doi":"10.1002/aenm.202403718","DOIUrl":"https://doi.org/10.1002/aenm.202403718","url":null,"abstract":"Tin (Sn)-based perovskites have emerged as promising alternatives to lead (Pb)-based perovskites in thin-film photovoltaics due to their comparable properties and reduced toxicity. Strains in perovskites can be tailored to modulate their optoelectronic properties, but mechanisms for the effects of strains on Sn-based perovskite films and devices are unrevealed and corresponding strain engineering is unexplored. Herein, a strain engineering strategy is developed through incorporating 4-fluorobenzylammonium halide salts (FBZAX, X = I, Br, Cl) into the perovskite precursor to regulate the strain effects in resultant Sn-based perovskite films. It is found that a moderate level of compressive strain achieved by FBZABr alleviates the dislocations within perovskites to enhance carrier transport and reduces the defect density to prolong carrier lifetime. These improvements enable a champion efficiency exceeding 14% of Sn-based perovskite solar cells with excellent operational stability.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"7 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758600","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":"Sulfonated Lignin Binder Blocks Active Iodine Dissolution and Polyiodide Shuttle Toward Durable Zinc-Iodine Batteries","authors":"Zhixiang Chen, Jie Zhang, Chuancong Zhou, Shan Guo, Daoxiong Wu, Zaowen Zhao, Zhitong Wang, Jing Li, Zhenyue Xing, Peng Rao, Zhenye Kang, Xinlong Tian, Xiaodong Shi","doi":"10.1002/aenm.202404814","DOIUrl":"https://doi.org/10.1002/aenm.202404814","url":null,"abstract":"The issues of active iodine dissolution and polyiodide shuttle severely hinder the development of zinc-iodine batteries (ZIBs). Binder engineering is considered a valid strategy to kill two birds with one stone. Herein, sodium lignosulfonate (LS), an important derivative of lignin, is optimized as a neotype binder for the fabrication of an iodine-loading cathode. Owing to the existence of the -SO<sub>3</sub>Na group, the electrostatic potential of LS molecule contains both negative and positive regions, which prefer to block the polyiodide shuttle behavior through the electrostatic repulsion effect, and adsorb the polyiodides through the electrostatic attraction effect, respectively. Meanwhile, LS molecule holds more negative Gibbs free energies for the consecutive radical reaction, and much stronger adsorption energies for iodine species, manifesting fast iodine conversion reaction kinetics, and effective inhibition for iodine dissolution behavior. As expected, the ZIBs based on LS binder delivers a high capacity of 153.6 mAh g<sup>−1</sup> after 400 cycles at 0.1 A g<sup>−1</sup>, reversible capacity of 152.8 mAh g<sup>−1</sup> after 500 cycles at 0.5 A g<sup>−1</sup> (50 °C), and durable cycling stability for 12000 cycles at 5 A g<sup>−1</sup>, implying excellent iodine fixation ability of LS binder. This work guides the design of a special binder for iodine-based electrodes and facilitates the practical application of ZIBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"69 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758597","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}
Heejun Yun, Eunji Lee, Juyeon Han, Eunbin Jang, Jinil Cho, Heebae Kim, Jeewon Lee, Byeongyun Min, Jemin Lee, Yuanzhe Piao, Jeeyoung Yoo, Youn Sang Kim
{"title":"Voltage Noise Failure Induced by Li Dendritic Micro-Penetration in All-Solid-State Li-Metal Battery with Composite Solid Electrolyte","authors":"Heejun Yun, Eunji Lee, Juyeon Han, Eunbin Jang, Jinil Cho, Heebae Kim, Jeewon Lee, Byeongyun Min, Jemin Lee, Yuanzhe Piao, Jeeyoung Yoo, Youn Sang Kim","doi":"10.1002/aenm.202404044","DOIUrl":"https://doi.org/10.1002/aenm.202404044","url":null,"abstract":"All-solid-state Li-metal batteries (ASSLBs) are the most attractive next-generation batteries due to intrinsic safety and high energy density. Particularly, composite solid electrolyte (CSE)-based ASSLBs, highly compatible with conventional Li-ion batteries, are nearing commercialization. However, the understanding of ASSLBs’ failure remains deficient, thereby considerably hindering their advancement. Herein, the unrecognized failing mode of ASSLBs, voltage noise failure (VNF), characterized by irregular charging voltage configuration, is identified using comprehensive techniques, including laser-induced breakdown spectroscopy. The VNF originates from micro-penetration of Li dendrites, which is demonstrated through direct observation of 3D Li concentration map in CSE. In this phenomenon, the transition metals, dissolved from the cathode, hop to the anode and serve as seeds for dendritic growth in VNF. Inspired by this mechanism and with the aid of DFT calculations, a transition metal scavenging layer is proposed using Prussian blue analogue at the cathode-CSE interface. Consequently, ASSLBs with transition metal scavenging layer exhibit superior capacity (189 mAh g<sup>−1</sup> at 0.5 C, NCM811) and stable cyclability (1200 cycles without failure).","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"11 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758557","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}
Anupam Sadhu, Teddy Salim, Qingde Sun, Stener Lie, Edwin Julianto, Lydia H. Wong
{"title":"Enhancing Perovskite Solar Cell Durability via Strategic Cation Management in Chalcogenide‐Based Hole Transport Layer","authors":"Anupam Sadhu, Teddy Salim, Qingde Sun, Stener Lie, Edwin Julianto, Lydia H. Wong","doi":"10.1002/aenm.202403676","DOIUrl":"https://doi.org/10.1002/aenm.202403676","url":null,"abstract":"Copper‐chalcogenide‐based inorganic holetransport layers (HTLs) are widely studied in perovskite solar cells (PSCs) because of their favorable valence band maximum and their ability to passivate interfacial defects through Pb‐S interactions. These compounds are shown to produce stable PSCs because of their high intrinsic stability. However, the density functional theory (DFT) calculations and X‐ray photoelectron spectroscopy analysis presented here reveal that the presence of Cu in the HTL can weaken the interfacial Pb‐S interactions and compromise the device stability. A clear inverse relationship is observed between the stability of perovskite film and the Cu‐concentration in the HTL underneath. Therefore, to minimize the detrimental effect of Cu, this work explores Cu‐deficient chalcopyrite compounds, CuIn<jats:sub>3</jats:sub>S<jats:sub>5</jats:sub> and Cu(In<jats:sub>x</jats:sub>Ga<jats:sub>(1‐x)</jats:sub>)<jats:sub>3</jats:sub>S<jats:sub>5</jats:sub>, as HTLs for PSCs, which results in improved device stability. DFT calculations reveal that incorporating gallium into the HTL reduces the HTL‐perovskite interfacial energy, which results in further enhancement of device stability. The average T<jats:sub>80</jats:sub> lifetimes (the time to retain 80% of the initial efficiency) under ambient conditions for the NiO, CuIn<jats:sub>3</jats:sub>S<jats:sub>5</jats:sub>, and Cu(In<jats:sub>0.3</jats:sub>Ga<jats:sub>0.7</jats:sub>)<jats:sub>3</jats:sub>S<jats:sub>5</jats:sub> HTL‐based devices are 200, 449, and 656 h, respectively. These findings underscore the significant roles of cations and anions of the inorganic transport layer in enhancing the stability of the PSCs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"76 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2024-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142756270","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}