Jin Hyeok Yang, Yeon Kyeong Jeong, Wontak Kim, Min A Lee, Jang Wook Choi, Hyun‐seung Kim, Ki Jae Kim
{"title":"Dual Flame‐Retardant Mechanism‐Assisted Suppression of Thermal Runaway in Lithium Metal Batteries with Improved Electrochemical Performances (Adv. Energy Mater. 2/2025)","authors":"Jin Hyeok Yang, Yeon Kyeong Jeong, Wontak Kim, Min A Lee, Jang Wook Choi, Hyun‐seung Kim, Ki Jae Kim","doi":"10.1002/aenm.202570006","DOIUrl":"https://doi.org/10.1002/aenm.202570006","url":null,"abstract":"","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"30 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988176","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}
Philip Bellchambers, Louis Ammon, Arielle Fitkin, Matthew Dingley, Marc Walker, Szymon Abrahamczyk, Callum Pritchard, Gabriele C. Sosso, Ross A. Hatton
{"title":"Zinc Grid Based Transparent Electrodes for Organic Photovoltaics","authors":"Philip Bellchambers, Louis Ammon, Arielle Fitkin, Matthew Dingley, Marc Walker, Szymon Abrahamczyk, Callum Pritchard, Gabriele C. Sosso, Ross A. Hatton","doi":"10.1002/aenm.202405148","DOIUrl":"https://doi.org/10.1002/aenm.202405148","url":null,"abstract":"Zinc is the fifth most electrically conductive metal and is available at a fraction of the cost of the most widely used transparent electrode materials; silver, indium-tin oxide, and poly(3,4-ethylenedioxythiophene) polystyrene sulfonate, but has been surprisingly overlooked as a current carrying element in organic photovoltaics. Here, a transparent flexible electrode based on an embedded zinc grid with ≈1 µm linewidth is reported and its utility as a drop-in replacement for indium-tin oxide coated glass electrodes in model organic photovoltaic devices is demonstrated. The zinc grids are fabricated using the unconventional approach of condensation coefficient modulation, using a micro-contact printed patterned layer of poly(perfluorooctylmethylmethacrylate) to resist zinc condensation in the gaps between grid lines, together with a copper acetylacetonate seed layer to nucleate zinc condensation where grid lines are required. Density functional theory calculations of the strength of the interaction between zinc atoms and this fluorinated polymer provide fundamental insight into why the latter is so effective at resisting zinc condensation. The resulting zinc grid is embedded in a flexible polymer support and transferred to a flexible plastic substrate by delamination, which enables recovery and reuse of the fluorinated polymer.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"21 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987124","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}
Qi Qian, Hanlin Cheng, Hang Xie, Yihong Wu, Yuanlai Fang, Qiujian Le, Shizhong Yue, Jianyong Ouyang
{"title":"A Mixed Ion/Electron Thermoelectric Generator with Ultrahigh Steady Thermopower by Exploring Both the Hole Tunneling and Ion Accumulations","authors":"Qi Qian, Hanlin Cheng, Hang Xie, Yihong Wu, Yuanlai Fang, Qiujian Le, Shizhong Yue, Jianyong Ouyang","doi":"10.1002/aenm.202404522","DOIUrl":"https://doi.org/10.1002/aenm.202404522","url":null,"abstract":"Ionic thermoelectric (TE) materials are promising candidate for efficient heat harvesting mainly because they can have a thermopower higher than the electronic TE materials by 2–3 orders in magnitude. However, they cannot be directly exploited in conventional thermoelectric generators (TEGs) since ions cannot transport across the electrodes into the external circuit, and they cannot be used to harvest heat under steady temperature gradient. Here, a mixed ion/electron thermoelectric generator (MTEG) is reported that can continuously generate electricity under not only temperature fluctuation but also steady temperature gradient. It is consisted of a layer of an ionogel added with reduced graphene oxide (rGO). The ionic liquid is an ionic conductor, while rGO is an electronic conductor. The MTEG can supply a constant output voltage to the external load under steady temperature gradient, and the behavior is similar to that of the conventional TEGs, particularly when the external resistance is relatively high. The thermopower can be more than 7.0 mV K<sup>−1</sup>, higher than the Seebeck coefficient of the best electronic TE materials by 1–2 orders in magnitude. The operation mechanism is attributed to the hole tunneling across the rGO sheets and the high thermopower due to the Soret effect of the ions.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"5 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987126","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}
Mingcong Du, Zhuobin He, Yuqiao Zhang, Yue-Peng Cai, Qifeng Zheng
{"title":"Sustainable Release of LiNO3 from a Fluorine-Decorated Metal–Organic Framework Separator to Enable High-Performance Li-Metal Batteries in Carbonate Electrolytes","authors":"Mingcong Du, Zhuobin He, Yuqiao Zhang, Yue-Peng Cai, Qifeng Zheng","doi":"10.1002/aenm.202403674","DOIUrl":"https://doi.org/10.1002/aenm.202403674","url":null,"abstract":"High-voltage Li-metal batteries hold great prospects for boosting energy density, while the Li-metal anodes show poor compatibility with high-voltage tolerant carbonate electrolytes, leading to unstable solid-electrolyte interphase (SEI) and uncontrolled Li dendrites growth. Herein, a F-decorated UIO-66/polyimide (PI) functional separator encapsulated with LiNO<sub>3</sub> (LNO@UIO-66F/PI) is rationally designed to regulate the interfacial chemistry and Li deposition behavior. Specifically, the UIO-66F nanoparticles in situ grown on the PI fibers form continuous electronegative nanochannels, which promote rapid and uniform Li<sup>+</sup> flux while repelling the anion migration. Furthermore, the LiNO<sub>3</sub> encapsulated in the UIO-66F nanopores sustainably releases to form a thin and conductive Li<sub>3</sub>N-rich SEI. This synergy effect induces a dense and spherical Li deposition behavior, effectively inhibiting the growth of Li dendrites. Consequently, this LNO@UIO-66F/PI separator demonstrates highly reversible Li plating/stripping over 1000 h at an extremely high current density of 10 mA cm<sup>−2</sup> in carbonate electrolytes, and also enables the stable cycling of Li||LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> cell over 1000 cycles under a high cut-off voltage of 4.5 V, paving the way for practical application of high-energy-density Li-metal batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"74 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987128","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}
Yurim Bae, Sang Ah Park, Sungryong Kim, Haeryang Lim, Jeongsu Kim, Long Ye, Taiho Park
{"title":"Boosting the Mechanical Stability and Power Output of Intrinsically Stretchable Organic Photovoltaics with Stretchable Electron Transporting Layer","authors":"Yurim Bae, Sang Ah Park, Sungryong Kim, Haeryang Lim, Jeongsu Kim, Long Ye, Taiho Park","doi":"10.1002/aenm.202405217","DOIUrl":"https://doi.org/10.1002/aenm.202405217","url":null,"abstract":"Intrinsically stretchable organic photovoltaics (IS-OPVs) are emerging as power sources for wearable technologies, enabling seamless integration into flexible and stretchable systems. A key feature of IS-OPVs is the potential for increased power output as the photoactive area expands during stretching. However, current mechanical performance and stability still fall short of meeting the demands for practical applications. To overcome this limitation, the study introduces, for the first time, a polymer:gel blend system as a highly stretchable electron transporting layer (ETL), which significantly enhances both the power output and mechanical stability of IS-OPVs. This novel ETL plays a pivotal role in dissipating mechanical stress and protecting the brittle underlying layers. By incorporating this stretchable ETL, the device stretchability is reinforced by introducing the stretchable ETL, thereby maintaining the initial power conversion efficiency under 20% strain. As a result, the maximum power output substantially increases by 23%, from 0.28 to 0.35 mW, under large strain, while devices with conventionally brittle ETLs caused a 33% reduction in power output. This study thus offers a pathway toward durable and efficient stretchable photovoltaics.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"54 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987129","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}
Nathan James Pataki, Shubhradip Guchait, Badr Jismy, Nicolas Leclerc, Adrica Kyndiah, Martin Brinkmann, Mario Caironi
{"title":"A Label-Like Monolithic Organic Thermoelectric Generator Enabled by Local Inkjet Doping of Aligned Polymer Films","authors":"Nathan James Pataki, Shubhradip Guchait, Badr Jismy, Nicolas Leclerc, Adrica Kyndiah, Martin Brinkmann, Mario Caironi","doi":"10.1002/aenm.202404656","DOIUrl":"https://doi.org/10.1002/aenm.202404656","url":null,"abstract":"The proliferation of distributed microelectronics and sensors necessitates adaptable, scalable, and cost-effective power supplies. Organic thermoelectric generators (TEGs) that promise to harness heat sustainably and cost-effectively are seen as pivotal elements in shaping future sensor infrastructures. Recent strides in morphological control through the alignment of conjugated polymer backbones have enhanced the thermoelectric performance of doped organic semiconductors to record values, matching expectations for real applications. However, the hurdles in crafting and deploying organic TEGs effectively exploiting aligned polymer films remain unexplored. This work presents a design and fabrication method to incorporate aligned films into a thin label-like TEG. Thin films of regioregular poly(3-hexylthiophene) (P3HT) and poly(2,5-bis((7-butoxyheptyl)thiophen-2-yl)thieno[3,2-<i>b</i>]thiophene) (PBTTT-<sup>8</sup>O) are aligned via high-temperature rubbing technique inducing a high degree of anisotropy in their charge transport properties. The crystal structure and anisotropy of the films are exploited to realize monolithic TEGs by patterning conductive thermoelements via local inkjet doping of films transferred on ultrathin parylene substrates. The TEGs based on aligned P3HT and PBTTT-<sup>8</sup>O exhibit exceptional TEG power factors of 0.33 and 1.04 nW cm<sup>−2</sup> K<sup>−2</sup>, respectively. Lastly, as a proof-of-concept use case for the TEGs, a thermoelectrically-powered volume-indicating label is presented as a potential application in the healthcare and food industries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"94 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987218","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}
Seungyun Jeon, Gukhyun Lim, Hoseok Lee, Hyunyoung Park, Min Kyung Cho, Chan Kim, YeEun Lee, Jaehoon Kim, Minhyung Kwon, Jung-Keun Yoo, Hyangsoo Jeong, Jinwoo Kim, Seung-Ho Yu, Minah Lee, Jongsoon Kim, Jihyun Hong
{"title":"Reduction-Induced Oxygen Loss: the Hidden Surface Reconstruction Mechanism of Layered Oxide Cathodes in Lithium-Ion Batteries","authors":"Seungyun Jeon, Gukhyun Lim, Hoseok Lee, Hyunyoung Park, Min Kyung Cho, Chan Kim, YeEun Lee, Jaehoon Kim, Minhyung Kwon, Jung-Keun Yoo, Hyangsoo Jeong, Jinwoo Kim, Seung-Ho Yu, Minah Lee, Jongsoon Kim, Jihyun Hong","doi":"10.1002/aenm.202404193","DOIUrl":"https://doi.org/10.1002/aenm.202404193","url":null,"abstract":"The surface reconstruction from the layered to rocksalt-type phase represents a primary deterioration pathway of layered-oxide cathodes in lithium-ion batteries, involving irreversible oxygen loss and transition metal migration. This degradation mechanism has primarily been attributed to the oxidative instability of highly delithiated cathodes at high voltages (>4.3 V vs Li/Li<sup>+</sup>). However, the battery degradation also occurs under seemingly stable voltage ranges, the origin of which remains unclear. Herein, a hidden mechanism to induce surface reconstruction and oxygen loss is proposed, termed the “quasi-conversion reaction”, which is revealed to occur during electrochemical reduction (discharge) processes just below 3.0 V (vs Li/Li<sup>+</sup>). Combined experiments and first-principles calculations unveil that the oxygens at the surface can be extracted from the cathode lattice by forming lithium oxides and oxygen vacancies, at significantly higher potentials than conventional conversion reaction, due to the instability of surface oxygens coordinated with fewer cations than in the bulk. The chemical incompatibility between lithium oxides and commercial carbonate-based electrolytes results in electrolyte decomposition, forming an organic-rich blocking layer and gaseous byproducts, which further increases the cell impedance. This study emphasizes the necessity of a thorough understanding of surface instability upon reduction to develop long-lasting batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"10 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987219","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}
Sean Scott, Wenjia Du, Rosie Horwood, Chunhong Lei, Paul Shearing, Andrew P. Abbott
{"title":"An Assessment of Blended Short Loop Recycled Graphite Electrodes Using X-Ray Micro-Computed Tomography","authors":"Sean Scott, Wenjia Du, Rosie Horwood, Chunhong Lei, Paul Shearing, Andrew P. Abbott","doi":"10.1002/aenm.202403498","DOIUrl":"https://doi.org/10.1002/aenm.202403498","url":null,"abstract":"With various battery directives necessitating the composition of recycled electrode materials this study manufactures anodes containing various ratios of pristine and reclaimed graphite from end-of-life (EOL) cells. Two approaches that can be used to delaminate graphite are using ultrasonication (USD) and simple water delamination (WD). X-ray micro-computed tomography is used to characterize the graphite particles and show that particle fracturing is evident with both methods, but key structural metrics such as particle radius and diffusivity varied significantly. It is shown that blending 20% recovers material with 80% pristine graphite causes no statistically significant difference in the performance of the cells. This suggests that recycling anode materials can be achieved without significant post-processing required. For WD anode material, the spherical graphite particles are maintained, whereas USD significantly changes the morphology and produces a large amount of “needle-like” particles. Using 100% reclaimed anode material causes the performance of the cell to decrease to 279 mAh g<sup>−1</sup> for WD material and 254 mAh g<sup>−1</sup> for USD graphite. The use of “blended” electrodes using WD graphite and pristine material creates electrodes with a comparable Li<sup>+</sup> flux and electrochemical performance to a pristine graphite reference of 300–315 mAh g<sup>−1</sup>.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"27 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987217","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":"Tailoring the Electron and Phonon Transport in Metavalently Bonded GeTe by Stepwise Doping","authors":"Ming Liu, Muchun Guo, Yuxuan Yang, Xingyan Dong, Haiyan Lyu, Yingda Lai, Yang Zhang, Yuke Zhu, Hao Wu, Fengkai Guo, Zihang Liu, Wei Cai, Matthias Wuttig, Haijun Wu, Yuan Yu, Jiehe Sui","doi":"10.1002/aenm.202405178","DOIUrl":"https://doi.org/10.1002/aenm.202405178","url":null,"abstract":"The intertwining between thermal and electrical transport poses significant challenges to enhancing thermoelectric performance. Chemical doping with a single element often can optimize one of the parameters yet may deteriorate others, restricting the upper limit of <i>ZT</i> achievable. Multi-element doping can address this interdependence, allowing for simultaneous optimization of electrical and thermal properties. However, a clear selection rule for multiple dopants remains unclear. Here, a stepwise strategy is shown to improve the thermoelectric performance of metavalently bonded GeTe by enhancing density-of-states effective mass, increasing carrier mobility, and reducing thermal conductivity. These effects are realized by continuously introducing band convergence, lattice plainification, and structural defects. Specifically, band convergence is achieved by Cd doping to reduce the energy offset between light and heavy bands. The lattice plainification is enabled by filling Ge vacancies with Cu, which improves carrier mobility. Lastly, the lattice thermal conductivity is reduced via increasing phonon scattering by point defects caused by Pb doping and nanoprecipitates associated with all these dopants. Consequently, a peak <i>ZT</i> of 2.2 at 773 K and an average <i>ZT</i><sub>ave</sub> of 1.27 within 300–773 K are realized in Ge<sub>0.86</sub>Pb<sub>0.1</sub>Cd<sub>0.04</sub>Te-2%Cu<sub>2</sub>Te. This work provides a synergistic strategy to modulate electron and phonon transport in metavalently bonded materials.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"8 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987132","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}
Patrick Dörflinger, Philipp Rieder, Vladimir Dyakonov
{"title":"Temperature-Dependent Charge-Carrier Dynamics in Lead-Halide Perovskites: Indications for Dynamic Disorder Dominated Scattering Mechanism","authors":"Patrick Dörflinger, Philipp Rieder, Vladimir Dyakonov","doi":"10.1002/aenm.202403332","DOIUrl":"https://doi.org/10.1002/aenm.202403332","url":null,"abstract":"Lead-halide perovskites have emerged as a promising material class in light-harvesting and light-emitting applications due to their exceptional semiconductor properties. Nonetheless, crucial semiconducting properties such as the charge carrier scattering mechanism and its impact on recombination dynamics are not well studied. Here, five different lead-halide perovskite compositions are systematically examined to determine their temperature-dependent mobility, and the prevalent scattering mechanisms involved are identified. Dynamic disorder is proposed to be the predominant scattering mechanism at room temperature and above, as evidenced by a change in the power-law <i>T<sup>m</sup></i>. Notably, the onset temperature for this behavior varies with the perovskite composition. Additionally, it is found that this scattering process coincides with changes in fast-trapping behavior in MAPbI<sub>3</sub> perovskite, which in turn alters recombination dynamics such as carrier lifetime and diffusion length. These results suggest that this scattering mechanism contributes to the defect tolerance of perovskites, providing valuable insights for further investigations.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"28 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987125","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}