Nikita Vostrov, Isaac Martens, Mattia Colalongo, Edoardo Zatterin, Michal Ronovsky, Adrien Boulineau, Steven Leake, Xiaobo Zhu, Lianzhou Wang, Marie-Ingrid Richard, Tobias Schulli
The nanoscale mechanisms of ion deintercalation in battery cathode materials remain poorly understood, especially the relationship between crystallographic defects (dislocations, small angle grain boundaries, vacancies, etc), device performance, and durability. In this work, operando scanning X-ray diffraction microscopy (SXDM) and multi-crystal X-ray diffraction (MCXD) are used to investigate microstrain and lattice tilt inhomogeneities inside Li1 − xNi0.5Mn1.5O4 cathode particles during electrochemical cycling and their influence on the material degradation. Using these techniques, microscale lattice degradation mechanisms are investigated inside single crystals, extend it to an inter-particle scale, and correlate it with the long-term degradation of the cathode. During cycling, a crystal lattice deformation is observed, associated with phase transitions and inherent lattice defects in the measured particle. Residual misorientations are observed in the structure even after full discharge, indicating an irreversible structural change of the lattice. However, after long-term cycling such lattice misorientations together with active material dissolution are further exacerbated only in a subset of particles, suggesting high heterogeneity of degradation mechanisms between the cathode particles. Selective degradation of particles could be caused by varying crystal quality across the sample, highlighting the need for a deep understanding of defect microstructures to enable a more rational design of materials with enhanced durability.
{"title":"Plastic Deformation of LiNi0.5Mn1.5O4 Single Crystals Caused by Domain Orientation Dynamics","authors":"Nikita Vostrov, Isaac Martens, Mattia Colalongo, Edoardo Zatterin, Michal Ronovsky, Adrien Boulineau, Steven Leake, Xiaobo Zhu, Lianzhou Wang, Marie-Ingrid Richard, Tobias Schulli","doi":"10.1002/aenm.202404933","DOIUrl":"https://doi.org/10.1002/aenm.202404933","url":null,"abstract":"The nanoscale mechanisms of ion deintercalation in battery cathode materials remain poorly understood, especially the relationship between crystallographic defects (dislocations, small angle grain boundaries, vacancies, <i>etc</i>), device performance, and durability. In this work, <i>operando</i> scanning X-ray diffraction microscopy (SXDM) and multi-crystal X-ray diffraction (MCXD) are used to investigate microstrain and lattice tilt inhomogeneities inside Li<sub>1 − <i>x</i>\u0000</sub>Ni<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> cathode particles during electrochemical cycling and their influence on the material degradation. Using these techniques, microscale lattice degradation mechanisms are investigated inside single crystals, extend it to an inter-particle scale, and correlate it with the long-term degradation of the cathode. During cycling, a crystal lattice deformation is observed, associated with phase transitions and inherent lattice defects in the measured particle. Residual misorientations are observed in the structure even after full discharge, indicating an irreversible structural change of the lattice. However, after long-term cycling such lattice misorientations together with active material dissolution are further exacerbated only in a subset of particles, suggesting high heterogeneity of degradation mechanisms between the cathode particles. Selective degradation of particles could be caused by varying crystal quality across the sample, highlighting the need for a deep understanding of defect microstructures to enable a more rational design of materials with enhanced durability.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"5 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987414","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}
Reversible protonic ceramic cells (r-PCCs) are highly attractive energy storage and conversion technology, while the insufficient activity of state-of-the-art air electrodes at reduced temperatures strongly limits their practical applications. Herein, this work reports a reduction/re-oxidation strategy to design a new highly efficient, and durable nanocomposite air electrode for boosting the performance of r-PCCs operated at intermediate temperatures. Specifically, single-phase Ba(Co0.4Fe0.4Zr0.1Y0.1)0.9Ni0.1O3-δ perovskite is selected as the precursor, its treatment in hydrogen atmosphere at 450 °C and then re-oxidation in air leads to the formation of a nanocomposite, consisted of a perovskite-based main phase and BaCoO3-δ and NiO secondary-phase nanoparticles, where the BaCoO3-δ phase facilitates oxygen surface exchange while NiO nanoparticles promote surface oxygen/steam adsorption. The corresponding r-PCC exhibits superior performance at 550 °C in a symmetrical cell (0.162 Ω cm2), a single fuel cell (0.690 W cm−2) and an electrolysis cell (−1.066 A cm−2 at 1.3 V). Such nanocomposite is thermodynamically stable at intermediate temperatures and offers better thermomechanical compatibility with protonic electrolyte because of the reduced thermal expansion coefficient. As a result, superior durability in both fuel and electrolysis cell modes is demonstrated. This study paves a new way for designing outstanding air electrodes for r-PCCs with great application potential.
{"title":"A New Nanocomposite Electrode Developed from Environmental Atmosphere Triggered Reconstruction for Efficient Reversible Protonic Ceramic Cells","authors":"Jie Wu, Zhenghui Xie, Mingzhuang Liang, Wanqing Chen, Dongliang Liu, Yongning Yi, Zhixin Luo, Ran Ran, Wei Zhou, Wei Wang, Zongping Shao","doi":"10.1002/aenm.202404118","DOIUrl":"https://doi.org/10.1002/aenm.202404118","url":null,"abstract":"Reversible protonic ceramic cells (r-PCCs) are highly attractive energy storage and conversion technology, while the insufficient activity of state-of-the-art air electrodes at reduced temperatures strongly limits their practical applications. Herein, this work reports a reduction/re-oxidation strategy to design a new highly efficient, and durable nanocomposite air electrode for boosting the performance of r-PCCs operated at intermediate temperatures. Specifically, single-phase Ba(Co<sub>0.4</sub>Fe<sub>0.4</sub>Zr<sub>0.1</sub>Y<sub>0.1</sub>)<sub>0.9</sub>Ni<sub>0.1</sub>O<sub>3-δ</sub> perovskite is selected as the precursor, its treatment in hydrogen atmosphere at 450 °C and then re-oxidation in air leads to the formation of a nanocomposite, consisted of a perovskite-based main phase and BaCoO<sub>3-δ</sub> and NiO secondary-phase nanoparticles, where the BaCoO<sub>3-δ</sub> phase facilitates oxygen surface exchange while NiO nanoparticles promote surface oxygen/steam adsorption. The corresponding r-PCC exhibits superior performance at 550 °C in a symmetrical cell (0.162 Ω cm<sup>2</sup>), a single fuel cell (0.690 W cm<sup>−2</sup>) and an electrolysis cell (−1.066 A cm<sup>−2</sup> at 1.3 V). Such nanocomposite is thermodynamically stable at intermediate temperatures and offers better thermomechanical compatibility with protonic electrolyte because of the reduced thermal expansion coefficient. As a result, superior durability in both fuel and electrolysis cell modes is demonstrated. This study paves a new way for designing outstanding air electrodes for r-PCCs with great application potential.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"27 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987412","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}
Albert L. Lipson, Jessica D. Macholz, Qiang Dai, Peyton Melin, Sabine M. Gallagher, Michael LeResche, Bryant J. Polzin, Jeffrey S. Spangenberger
Li-ion battery recycling presents a promising opportunity to decrease dependence on foreign sources of materials and harvest precious materials within the United States. Herein, a superior complete direct recycling process on individual end-of-life cells is reported where the recovered high-purity cathode active material, as well as electrolyte salt Li hexafluorophosphate (LiPF6) can be reused without significant processing. This new process utilizes a series of mechanical separation steps that enable the separation of the cathode and anode active materials while they are still attached to their current collectors. Using this type of process can significantly reduce metal contamination and enable a clean cathode that can be directly recycled. The process if implemented commercially can greatly reduce the environmental burden of batteries as the greenhouse gas emissions of 8.25 kg CO2e kg−1 from the direct recycling process are 64% lower compared to those from virgin production of cathode material. During electrochemical testing of the recovered LiNi0.6Mn0.2Co0.2O2 a discharge capacity of ≈160 mAh g−1 and good cyclability of over 250 cycles at 0.33C are achieved. This success paves a new pathway to explore and optimize existing Li-ion battery recycling procedures.
{"title":"Cost-Effective and Scalable Approach for the Separation and Direct Cathode Recovery from End-of-Life Li-Ion Batteries","authors":"Albert L. Lipson, Jessica D. Macholz, Qiang Dai, Peyton Melin, Sabine M. Gallagher, Michael LeResche, Bryant J. Polzin, Jeffrey S. Spangenberger","doi":"10.1002/aenm.202405430","DOIUrl":"https://doi.org/10.1002/aenm.202405430","url":null,"abstract":"Li-ion battery recycling presents a promising opportunity to decrease dependence on foreign sources of materials and harvest precious materials within the United States. Herein, a superior complete direct recycling process on individual end-of-life cells is reported where the recovered high-purity cathode active material, as well as electrolyte salt Li hexafluorophosphate (LiPF<sub>6</sub>) can be reused without significant processing. This new process utilizes a series of mechanical separation steps that enable the separation of the cathode and anode active materials while they are still attached to their current collectors. Using this type of process can significantly reduce metal contamination and enable a clean cathode that can be directly recycled. The process if implemented commercially can greatly reduce the environmental burden of batteries as the greenhouse gas emissions of 8.25 kg CO<sub>2</sub>e kg<sup>−1</sup> from the direct recycling process are 64% lower compared to those from virgin production of cathode material. During electrochemical testing of the recovered LiNi<sub>0.6</sub>Mn<sub>0.2</sub>Co<sub>0.2</sub>O<sub>2</sub> a discharge capacity of ≈160 mAh g<sup>−1</sup> and good cyclability of over 250 cycles at 0.33C are achieved. This success paves a new pathway to explore and optimize existing Li-ion battery recycling procedures.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"83 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987123","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
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.
{"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}
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}
Qi Qian, Hanlin Cheng, Hang Xie, Yihong Wu, Yuanlai Fang, Qiujian Le, Shizhong Yue, Jianyong Ouyang
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−1, 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.
{"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
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 LiNO3 (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+ flux while repelling the anion migration. Furthermore, the LiNO3 encapsulated in the UIO-66F nanopores sustainably releases to form a thin and conductive Li3N-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−2 in carbonate electrolytes, and also enables the stable cycling of Li||LiNi0.8Co0.1Mn0.1O2 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.
{"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
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.
{"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
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-b]thiophene) (PBTTT-8O) 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-8O exhibit exceptional TEG power factors of 0.33 and 1.04 nW cm−2 K−2, 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.
{"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
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+). 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+). 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.
{"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}
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