Yongju Lee, Swarup Biswas, Dong Hyun Nam, Jae Won Park, Hyowon Jang, Hyojeong Choi, Juhwan Kim, Dong-Wook Park, Hyeok Kim
{"title":"Functionalized Interlayers in Self-Powered Organic Photodiodes for Enhanced Near-Infrared Sensing (Adv. Energy Mater. 16/2025)","authors":"Yongju Lee, Swarup Biswas, Dong Hyun Nam, Jae Won Park, Hyowon Jang, Hyojeong Choi, Juhwan Kim, Dong-Wook Park, Hyeok Kim","doi":"10.1002/aenm.202570077","DOIUrl":"https://doi.org/10.1002/aenm.202570077","url":null,"abstract":"<p><b>Near-Infrared Photodetectors</b></p><p>In article number 2403532, Hyeok Kim and co-workers utilized a newly synthesized PPY:PSS as the hole transport layer to develop a near-infrared photodetector with significantly superior electrical properties, enhanced stability, and improved performance compared to commercially available PEDOT:PSS. Additionally, this device offers the advantage of being over 100 times more cost-effective than conventional counterparts, making it highly efficient.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"15 16","pages":""},"PeriodicalIF":24.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/aenm.202570077","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143871488","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Unveiling the Role of Nontrivial Electronic Structure and Lattice Softening in the Excellent Thermoelectric Performance of MnGeTe2 Alloys near the Ioffe–Regel Limit","authors":"Qicai Mei, Chenghao Xie, Jiabei Liu, Yixuan Wang, Jingjing Cui, Lin Liao, Chengyun Liao, Weibin Xu, Songlin Li, Qingjie Zhang, Xinfeng Tang, Gangjian Tan","doi":"10.1002/aenm.202500937","DOIUrl":"https://doi.org/10.1002/aenm.202500937","url":null,"abstract":"State-of-the-art thermoelectric materials typically exhibit high charge carrier mobility. However, this study reveals an exception in MnGeTe<sub>2</sub> alloys, where the room-temperature hole mobility is intrinsically low, approaching the Ioffe–Regel limit. Through heavy alloying with AgSbTe<sub>2</sub>, the electronic band structure of MnGeTe<sub>2</sub> transitions from a single valence band to multiple bands, driven by enhanced spin-orbit coupling due to the incorporation of heavier Ag and Sb elements. This electronic restructuring increases the density of states effective mass by 50%, from 10 <i>m</i><sub>e</sub> to 15 <i>m</i><sub>e</sub>, significantly enhancing the Seebeck coefficient despite higher hole concentrations. Remarkably, the carrier mobility remains unchanged, as the mean free path of charge carriers has already reached its minimum. Additionally, heavy alloying induces lattice softening in MnGeTe<sub>2</sub>, as confirmed by sound velocity measurements. This lattice softening, combined with the alloying effect, reduces the lattice thermal conductivity to its amorphous limit. Further optimization of the Ag/Sb ratio enables precise tuning of carrier density, resulting in an exceptional peak <i>ZT</i> value of 1.7 at 868 K for the Mn<sub>0.7</sub>Ge<sub>0.7</sub>Ag<sub>0.2</sub>Sb<sub>0.4</sub>Te<sub>2</sub> sample — a 60% improvement over pristine MnGeTe<sub>2</sub>. This work demonstrates the promise of low-mobility systems near the Ioffe–Regel limit for high-performance thermoelectrics, revealing synergistic electronic–lattice interactions.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"37 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872598","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":"Exploring Challenging C2+ Products During CO2 Reduction via Machine Learning Acceleration (Adv. Energy Mater. 16/2025)","authors":"Mingzi Sun, Bolong Huang","doi":"10.1002/aenm.202570079","DOIUrl":"https://doi.org/10.1002/aenm.202570079","url":null,"abstract":"<p><b>CO<sub>2</sub> Reduction</b></p><p>In article number 2500177, Mingzi Sun and Bolong Huang have applied the first-principles machine learning method to unravel the reaction mechanisms of challenging C<sub>2+</sub> products during the CO<sub>2</sub> reduction reaction on graphdiyne-supported atomic catalysts, which supply insights into improving the selectivity of designed catalysts.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"15 16","pages":""},"PeriodicalIF":24.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/aenm.202570079","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143871595","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Michael J. Counihan, Zachary D. Hood, Hong Zheng, Till Fuchs, Leonardo Merola, Matilde Pavan, Sebastian L. Benz, Tianyi Li, Artem Baskin, Junsoo Park, Joakim Halldin Stenlid, Xinglong Chen, Daniel P. Phelan, John W. Lawson, Justin G. Connell, Jürgen Janek, Felix H. Richter, Sanja Tepavcevic
{"title":"Effect of Propagating Dopant Reactivity on Lattice Oxygen Loss in LLZO Solid Electrolyte Contacted with Lithium Metal","authors":"Michael J. Counihan, Zachary D. Hood, Hong Zheng, Till Fuchs, Leonardo Merola, Matilde Pavan, Sebastian L. Benz, Tianyi Li, Artem Baskin, Junsoo Park, Joakim Halldin Stenlid, Xinglong Chen, Daniel P. Phelan, John W. Lawson, Justin G. Connell, Jürgen Janek, Felix H. Richter, Sanja Tepavcevic","doi":"10.1002/aenm.202406020","DOIUrl":"https://doi.org/10.1002/aenm.202406020","url":null,"abstract":"Lithium lanthanum zirconium oxide (LLZO) is widely known as the most stable solid electrolyte against lithium metal electrodes. This thermodynamic stability can be lost by the presence of dopants which are required to stabilize the cubic phase of LLZO and can be reduced by lithium metal. However, the role of oxygen in such reactions is taken for granted. In this work, the reduction of Nb-substituted LLZO (Nb-LLZO) is explored by Li metal and shows that interfacial reactions propagate and lead to the decomposition with substantial Nb<sup>5+</sup> reduction deep into the bulk electrolyte. Scanning Transmission Electron Microscopy with Energy Dispersive X-ray Spectroscopy and thermogravimetric analyses show much of the reduction is due to oxygen vacancies formed, leading to increased electronic conductivity mapped with conductive Atomic Force Microscopy. Density functional theory calculations indicate oxygen release is favored by increased excess lithiation of Nb-LLZO. Electrochemical impedance of polycrystalline Nb-LLZO shows the continuous evolution of ionically resistive interphases near the lithium metal interface with Nb-LLZO while single crystals show little reactivity at room temperature and self-limiting reduction at 60°C. This work underlines the role of grain boundaries in propagating destructive solid electrolyte reactions and highlights previously unseen mechanisms involving lattice oxygen in LLZO.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"6 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872599","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}
A. Vignesh, G. Gnana kumar, Ponniah Vajeeston, Arumugam Manthiram
{"title":"Bimetallic Organic Framework-Derived 3D Hierarchical Ni–Cu/MWCNTs as Anode Catalysts for High-Performance, Durable Direct Urea Fuel Cells","authors":"A. Vignesh, G. Gnana kumar, Ponniah Vajeeston, Arumugam Manthiram","doi":"10.1002/aenm.202405025","DOIUrl":"https://doi.org/10.1002/aenm.202405025","url":null,"abstract":"The electrochemical urea oxidation reaction (UOR) is substantiated as a promising pathway for transforming waste into renewable power. Hollow ball-like architectures composed of 3D carbon shell-encased Ni–Cu nanoparticles in multi-walled carbon nanotubes (Ni<sub>x</sub>-Cu<sub>y</sub>/MWCNTs) have been synthesized, utilizing a bimetallic organic framework as a soft template in conjunction with chemical vapor deposition. The configurational and electronic traits of the as-formulated catalysts and their impact on charge-transfer processes are elucidated with density functional theory, and their influence on UOR kinetics is then explicated with various electrochemical techniques. The hierarchical porous hollow spherical bundles of Ni<sub>x</sub>-Cu<sub>y</sub>/MWCNTs accelerate urea utilization efficacy, as their interior and exterior surfaces are exposed to urea fuel. The synergistic interaction between bimetallic nanoparticles and graphitic carbon helps enhance the electron conduction pathways, electrocatalytic activity, and anti-poisoning ability toward UOR. Compared to commercial Ni/C, the Ni<sub>x</sub>-Cu<sub>y</sub>/MWCNTs catalyst enables direct urea fuel cells (DUFC) with a high-power density (47.3 mW cm<sup>−2</sup>) and longevity (200 h), benefiting from the energetically favored oxidation of UOR intermediates and suppressed N─C bond cleavage facilitated by the surface and interstitial vacancies in Ni<sub>x</sub>-Cu<sub>y</sub>/MWCNTs. Moreover, 32.7 mW cm<sup>−2</sup> along with resilience against human urine fuel is achieved in DUFC, opening up research endeavors in sustainable energy development.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"6 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872597","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}
Alvin Joseph, Anitha B. Pillai, Muthukrishnan Sundaram, Birabar Ranjit Kumar Nanda, Manoj A. G. Namboothiry
{"title":"Mitigation of Illumination Sensitive Dark Current in Broadband Organic Photodiode Enabled by Robust Interface Engineering","authors":"Alvin Joseph, Anitha B. Pillai, Muthukrishnan Sundaram, Birabar Ranjit Kumar Nanda, Manoj A. G. Namboothiry","doi":"10.1002/aenm.202500748","DOIUrl":"https://doi.org/10.1002/aenm.202500748","url":null,"abstract":"The reliability of performance metrics in organic photodiodes (OPDs) is a fundamental factor for their efficacy in real‐time applications. Among these metrics, the dark current density stands out for its direct impact on the sensitivity of the detectors. In this study, an anomalous illumination‐sensitive variation in dark current is observed in fabricated near‐infrared OPDs, which undermines the device reliability. The systematic investigation reveals that this behavior stems from the photocatalytic nature of zinc oxide (ZnO), the electron transport layer used in the OPD. The photocatalytic nature of ZnO detrimentally affects the stability of the active material, particularly the nonfullerene acceptor employed in this study. Through robust interface engineering approach, which involves modifying the interface between ZnO and the active layer, the anomalies in the dark current are successfully mitigated, enhancing the consistency and reliability of the OPDs. In addition to reducing the dark current, this interface engineering strategy improves the overall performance and operational stability of the OPDs, especially under ultraviolet exposure.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"68 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866657","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":"Weakly Solvating Electrolytes for Lithium and Post‐Lithium Rechargeable Batteries: Progress and Outlook","authors":"Xue Li, Fei Luo, Naigen Zhou, Henry Adenusi, Shan Fang, Fanglin Wu, Stefano Passerini","doi":"10.1002/aenm.202501272","DOIUrl":"https://doi.org/10.1002/aenm.202501272","url":null,"abstract":"In the rapidly evolving global landscape of renewable energy sources, there is an increasing demand for high‐energy‐density rechargeable batteries essential for energy storage. Simultaneously, there is a growing emphasis on developing high‐stability electrolytes. The concepts of high concentration electrolytes (HCEs) and localized high concentration electrolytes (LHCEs) have emerged, with notable progress achieved by altering cation‐solvent and cation–anion solvation coordination environments. However, challenges persist, including high costs and low ionic conductivity. A recent development is the introduction of the weakly solvating electrolyte (WSE), which offers a new perspective on the design of stable electrolytes at conventional or low concentrations. This approach enables high‐performance rechargeable batteries by modulating the coordination structure of electrolytes to generate a unique anion‐driven interphase reaction chemistry. This review outlines the design principles of WSEs and their operating mechanisms when applied to rechargeable lithium and post‐lithium batteries. An outlook is also presented on the future research directions of WSE, coupled with an analysis of the technological challenges.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"3 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866934","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":"Probe the Role of Oxygen Anionic Redox in High‐Energy‐Density Battery with Advanced Characterization Techniques","authors":"Qianwen Dong, Junxiu Wu, Jun Lu","doi":"10.1002/aenm.202500282","DOIUrl":"https://doi.org/10.1002/aenm.202500282","url":null,"abstract":"The rapid advancement of the new energy industry has resulted in an urgent demand for batteries with superior energy density. To this end, oxygen anionic redox (OAR) emerges as a new paradigm for significantly enhancing battery energy density, which is initially explored in diverse battery systems. Although the feasibility of OAR in various cathode materials is affirmed, it is essential to consider the inevitable consequent issues, such as the irreversibility of OAR process and potential damage to electrode structure. To achieve a comprehensive understanding and effectively leverage the potential of OAR for high‐energy‐density batteries, extensive research has focused on the performance enhancement and failure mechanisms of OAR in different battery systems. However, owing to the limitation of the characterization techniques, a systematic and comprehensive research approaches for studying OAR is lacking. Herein, combing the advanced characterization techniques, an overview is provided from local OAR to full OAR in different cathodes, in which the triggers, working processes and challenges associated with OAR are presented. This perspective will end with a discussion on how to develop the advanced characterization technology applied for OAR along with a caution of practical application for OAR.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"219 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866650","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}
Xuqi Nie, Zhongteng Chen, Biwen Deng, Lianyi Shao, Junling Xu, Xiaoyan Shi, Zhipeng Sun
{"title":"Synergistic Modulation of Electronic Structure and Sodium-Ion Diffusion in Iron Sulfides via High-Entropy Doping for High Performance Sodium-Ion Batteries","authors":"Xuqi Nie, Zhongteng Chen, Biwen Deng, Lianyi Shao, Junling Xu, Xiaoyan Shi, Zhipeng Sun","doi":"10.1002/aenm.202500069","DOIUrl":"https://doi.org/10.1002/aenm.202500069","url":null,"abstract":"Iron sulfides are promising anode materials for high-energy-density sodium-ion batteries (SIBs) due to their high theoretical capacity, exceptional safety features, and abundant resources. However, their practical application is limited by limited intrinsic electronic conductivity, low sodium ion diffusion rates, and rapid capacity degradation. A novel high-entropy doping strategy is developed using a scalable ball-milling method to form a solid solution of doped elements (cation dopants: Ni, Mo, Cr, W, and Si; anion dopant: Se) with the primary components (iron and sulfur). Simultaneously, expanded graphite (EG) is incorporated and exfoliated through ball milling to provide abundant active sites for the growth of high-entropy-doped FeS during the subsequent high-temperature vulcanization process. Systematic experiments and theoretical calculations demonstrate that high-entropy doping substantially improves electronic and ionic conductivity as well as polysulfide adsorption capabilities. This high-entropy cation- and anion-doped FeS/EG (HED-FeS<sub>1−</sub><i><sub>x</sub></i>Se<i><sub>x</sub></i>/EG) delivers a discharge capacity of 511 mAh g<sup>−1</sup> at 20 A g<sup>−1</sup>. Remarkably, at an extremely high current density of 100 A g<sup>−1</sup>, the reversible capacity remains at 222.3 mAh g<sup>−1</sup>. After 3000 cycles (40 days) at 5 A g<sup>−1</sup>, the electrode in the sodium half-cell shows a specific capacity of 832 mAh g<sup>−1</sup>. These findings offer valuable technological insights for next-generation SIBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"128 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862169","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":"Sodium-Ion Pump Enhanced Composite Sodium Anode Toward Fast-Charging and Practical N/P Ratio Solid-State Sodium Metal Batteries","authors":"Jiayu Chen, Zhongqin Dai, Huan Chen, Zhongdu He, Yanchao Dai, Wei Shan, Wuhan Liu, Xiangwei Wu, Zhaoyin Wen","doi":"10.1002/aenm.202501061","DOIUrl":"https://doi.org/10.1002/aenm.202501061","url":null,"abstract":"Solid-state sodium metal batteries (SSSMBs) employing NASICON-type solid-state electrolytes and sodium metal anodes promise enhanced safety and high-energy density, yet the poor anodic interface compatibility induced growth of Na dendrites and excessive consumption of sodium metal still hinder their application. In this work, a 3D porous carbon-supported ultrathin sodium anode with superionic conductivity and high diffusivity is designed on the surface of the NASICON electrolytes, which serve as sodium-ion pump to improve the sodium-ion-transfer kinetics. The fast ion/electron transfer within the composite anode effectively solved the problem of rapid consumption of Na<sup>+</sup> and local charge accumulation at the anodic interface, thereby achieving dendrite-free Na deposition. A high critical current density of 3.5 mA cm<sup>−2</sup> and a long cycling life of 6000 h at 0.2 mA cm<sup>−2</sup> are achieved for the symmetrical cells. Coupled with Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> cathode, the full cells exhibit a high-capacity retention of 90.2% after 5100 cycles at 10 C. Most importantly, SSSMBs using a limited Na metal anode paired with 17.3 mg cm<sup>−2</sup> Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> cathode (1.05 negative/positive capacity ratio) deliver an outstanding capacity retention of 97% for 100 cycles. This work demonstrates a promising ultrathin Na anode toward the development of practical and sustainable high-performance SSSMBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"126 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862358","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}