Pub Date : 2025-01-15DOI: 10.1016/j.joule.2024.10.007
Matthew J.W. Ogley , Ashok S. Menon , Gaurav C. Pandey , Galo J. Páez Fajardo , Beth J. Johnston , Innes McClelland , Veronika Majherova , Steven Huband , Debashis Tripathy , Israel Temprano , Stefano Agrestini , Veronica Celorrio , Gabriel E. Pérez , Samuel G. Booth , Clare P. Grey , Serena A. Cussen , Louis F.J. Piper
This study refutes the commonly used ionic-bonding model that demarcates transition metal (TM) and oxygen redox using an archetypal Ni-rich layered oxide cathode, LiNi0.8Mn0.1Co0.1O2. Here, charge compensation during delithiation occurs without formal (ionic) Ni oxidation. Instead, oxygen-dominated states control the redox process, facilitated by strong TM-O hybridization, forming bulk-stable 3d8L and 3d8L2 electronic states, where L is a ligand hole. Bulk O–O dimers are observed with O K-edge resonant inelastic X-ray scattering but, critically, without the long-range TM migration or void formation observed in Li-rich layered oxides. Above 4.34 V vs. Li+/Li, the cathode loses O, forming a resistive surface rock-salt layer that causes capacity fade. This highlights the importance of cathode engineering when attempting to achieve higher energy densities with layered oxide cathodes, especially in those where O dominates the charge compensation mechanism.
本研究利用典型的富镍层状氧化物阴极 LiNi0.8Mn0.1Co0.1O2，驳斥了划分过渡金属（TM）和氧氧化还原的常用离子键模型。在这里，脱硫过程中的电荷补偿是在没有正式（离子）镍氧化的情况下发生的。相反，氧主导态控制了氧化还原过程，并通过强 TM-O 杂化作用形成了大量稳定的 3d8L 和 3d8L2 电子态，其中 L 是配体空穴。通过 O K 边共振非弹性 X 射线散射可以观察到块状 O-O 二聚体，但重要的是，在富含锂的层状氧化物中没有观察到长程 TM 迁移或空隙形成。对 Li+/Li 的电压高于 4.34 V 时，阴极会失去 O，形成电阻性表面岩盐层，导致容量衰减。这凸显了在尝试使用层状氧化物阴极实现更高能量密度时阴极工程的重要性，尤其是在 O 主导电荷补偿机制的阴极中。
{"title":"Metal-ligand redox in layered oxide cathodes for Li-ion batteries","authors":"Matthew J.W. Ogley , Ashok S. Menon , Gaurav C. Pandey , Galo J. Páez Fajardo , Beth J. Johnston , Innes McClelland , Veronika Majherova , Steven Huband , Debashis Tripathy , Israel Temprano , Stefano Agrestini , Veronica Celorrio , Gabriel E. Pérez , Samuel G. Booth , Clare P. Grey , Serena A. Cussen , Louis F.J. Piper","doi":"10.1016/j.joule.2024.10.007","DOIUrl":"10.1016/j.joule.2024.10.007","url":null,"abstract":"<div><div>This study refutes the commonly used ionic-bonding model that demarcates transition metal (TM) and oxygen redox using an archetypal Ni-rich layered oxide cathode, LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub>. Here, charge compensation during delithiation occurs without formal (ionic) Ni oxidation. Instead, oxygen-dominated states control the redox process, facilitated by strong TM-O hybridization, forming bulk-stable 3d<sup>8</sup><u>L</u> and 3d<sup>8</sup><u>L</u><sup>2</sup> electronic states, where <u>L</u> is a ligand hole. Bulk O–O dimers are observed with O K-edge resonant inelastic X-ray scattering but, critically, without the long-range TM migration or void formation observed in Li-rich layered oxides. Above 4.34 V vs. Li<sup>+</sup>/Li, the cathode loses O, forming a resistive surface rock-salt layer that causes capacity fade. This highlights the importance of cathode engineering when attempting to achieve higher energy densities with layered oxide cathodes, especially in those where O dominates the charge compensation mechanism.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 1","pages":"Article 101775"},"PeriodicalIF":38.6,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142541898","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}
Pub Date : 2025-01-15DOI: 10.1016/j.joule.2024.09.010
Siqi Gong , Kaixian Li , Jianfeng Sun , Jie Chen , Hengyu Guo
Droplet-based nanogenerators, harnessing the dynamic interaction between droplets and tribo-layer surfaces for electricity generation, demonstrate substantial promise in nano-micro energy harvesting. However, conventional devices face limitations in charge and voltage outputs due to the constrained liquid-solid interface and intrinsic parasitic capacitance, resulting in comparatively low power density. Herein, regulated by heterogeneous wetting surfaces, the periodic squeezing of a 3D droplet to a 2D plate maximizes the effective interface for triboelectrification and electrostatic induction, leading to a remarkable charge density of ∼2.0 C m−3. Additionally, optimizing electrode configuration reduces parasitic capacitance and elevates output voltage by 80 folds. A recorded peak power density of 5,865 W m−3 is obtained, which is 48 times higher than previous works. Furthermore, the droplet’s non-Hookean elastic behavior extends the frequency response band by 89.3%, enabling small electronics to operate under micro-vibration conditions. This study offers valuable insights for efficient electric energy extraction from interfacial droplets.
基于液滴的纳米发电机利用液滴与三层表面之间的动态相互作用进行发电，在纳米微能量收集方面前景广阔。然而，由于液固界面的限制和固有寄生电容，传统设备在电荷和电压输出方面面临限制，导致功率密度相对较低。在这里，在异质润湿表面的调节下，三维液滴周期性地挤压到二维板上，使三电化和静电感应的有效界面最大化，从而使电荷密度达到 2.0 C m-3。此外，电极配置的优化降低了寄生电容，并将输出电压提高了 80 倍。所记录的峰值功率密度为 5,865 W m-3，比以前的研究成果高出 48 倍。此外，液滴的非胡肯弹性行为将频率响应带扩展了 89.3%，使小型电子设备能够在微振动条件下运行。这项研究为从界面液滴中高效提取电能提供了宝贵的见解。
{"title":"Interfacial droplet-based triboelectric nanogenerator with optimized architecture for highly efficient vibrational energy conversion","authors":"Siqi Gong , Kaixian Li , Jianfeng Sun , Jie Chen , Hengyu Guo","doi":"10.1016/j.joule.2024.09.010","DOIUrl":"10.1016/j.joule.2024.09.010","url":null,"abstract":"<div><div>Droplet-based nanogenerators, harnessing the dynamic interaction between droplets and tribo-layer surfaces for electricity generation, demonstrate substantial promise in nano-micro energy harvesting. However, conventional devices face limitations in charge and voltage outputs due to the constrained liquid-solid interface and intrinsic parasitic capacitance, resulting in comparatively low power density. Herein, regulated by heterogeneous wetting surfaces, the periodic squeezing of a 3D droplet to a 2D plate maximizes the effective interface for triboelectrification and electrostatic induction, leading to a remarkable charge density of ∼2.0 C m<sup>−3</sup>. Additionally, optimizing electrode configuration reduces parasitic capacitance and elevates output voltage by 80 folds. A recorded peak power density of 5,865 W m<sup>−3</sup> is obtained, which is 48 times higher than previous works. Furthermore, the droplet’s non-Hookean elastic behavior extends the frequency response band by 89.3%, enabling small electronics to operate under micro-vibration conditions. This study offers valuable insights for efficient electric energy extraction from interfacial droplets.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 1","pages":"Article 101763"},"PeriodicalIF":38.6,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142448901","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}
Pub Date : 2025-01-15DOI: 10.1016/j.joule.2024.10.011
Yun Seop Shin , Ji Won Song , Dong Gyu Lee , Jaehwi Lee , Jongdeuk Seo , Jina Roe , Gwang Yong Shin , Dongshin Kim , Jiwoo Yeop , Dongmin Lee , Minjin Kim , Yimhyun Jo , Hyungsu Jang , Jung Geon Son , Woojin Lee , Jeongmin Son , Sujung Park , Shinuk Cho , Tae Joo Shin , Gi-Hwan Kim , Dong Suk Kim
In conventional n-i-p perovskite solar cells, unsolved issues persist, particularly concerning notorious performance degradation under prolonged heat exposure at 85°C. By reducing the concentration of 4-tert-butylpyridine (tBP) and lithium bis(trifluoromethanesulfonyl)imide and adjusting their molar ratio to one, we achieved a dramatic increase in the heat stability of the PSC while boosting its power conversion efficiency (PCE). The formation of a 1:1 Li+-tBP complex was crucial for preventing free tBP molecules in the hole-transporting layer (HTL), suppressing the de-doping of the p-type HTL by tBP and the release of tBP vapor under heat stress. Consequently, the PSCs accomplished a PCE of 26.18% (certified 26.00%) while demonstrating remarkable resilience to heat exposure at 85°C due to the raised glass transition temperature of the HTL. Furthermore, a perovskite solar mini-module with an aperture area of 25 cm2 achieved a PCE of 23.29%, highlighting their potential for commercial PSC deployment.
{"title":"De-doping engineering for efficient and heat-stable perovskite solar cells","authors":"Yun Seop Shin , Ji Won Song , Dong Gyu Lee , Jaehwi Lee , Jongdeuk Seo , Jina Roe , Gwang Yong Shin , Dongshin Kim , Jiwoo Yeop , Dongmin Lee , Minjin Kim , Yimhyun Jo , Hyungsu Jang , Jung Geon Son , Woojin Lee , Jeongmin Son , Sujung Park , Shinuk Cho , Tae Joo Shin , Gi-Hwan Kim , Dong Suk Kim","doi":"10.1016/j.joule.2024.10.011","DOIUrl":"10.1016/j.joule.2024.10.011","url":null,"abstract":"<div><div>In conventional n-i-p perovskite solar cells, unsolved issues persist, particularly concerning notorious performance degradation under prolonged heat exposure at 85°C. By reducing the concentration of 4-<em>tert</em>-butylpyridine (<em>t</em>BP) and lithium bis(trifluoromethanesulfonyl)imide and adjusting their molar ratio to one, we achieved a dramatic increase in the heat stability of the PSC while boosting its power conversion efficiency (PCE). The formation of a 1:1 Li<sup>+</sup>-<em>t</em>BP complex was crucial for preventing free <em>t</em>BP molecules in the hole-transporting layer (HTL), suppressing the de-doping of the p-type HTL by <em>t</em>BP and the release of <em>t</em>BP vapor under heat stress. Consequently, the PSCs accomplished a PCE of 26.18% (certified 26.00%) while demonstrating remarkable resilience to heat exposure at 85°C due to the raised glass transition temperature of the HTL. Furthermore, a perovskite solar mini-module with an aperture area of 25 cm<sup>2</sup> achieved a PCE of 23.29%, highlighting their potential for commercial PSC deployment.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 1","pages":"Article 101779"},"PeriodicalIF":38.6,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599684","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}
Pub Date : 2025-01-15DOI: 10.1016/j.joule.2024.11.016
Russell McKenna , Johan Lilliestam , Heidi U. Heinrichs , Jann Weinand , Johannes Schmidt , Iain Staffell , Andrea N. Hahmann , Peter Burgherr , Arne Burdack , Monika Bucha , Ruihong Chen , Michael Klingler , Paul Lehmann , Jens Lowitzsch , Riccardo Novo , James Price , Romain Sacchi , Patrick Scherhaufer , Eva M. Schöll , Piero Visconti , Luis Ramirez Camargo
Wind power accounted for 8% of global electricity generation in 2023 and is one of the cheapest forms of low-carbon electricity. Although fully commercial, many challenges remain in achieving the required scale-up, relating to integrating wind farms into wider technical, economic, social, and natural systems. We review the main challenges, outline existing solutions, and propose future research needed to overcome existing problems. Although the techno-economic challenges of grid and market integration are seen as significant obstacles to scaling up wind power, the field is replete with solutions. In many countries, planning and permitting are immediate barriers to wind-power deployment; although solutions are emerging in the EU and several countries, the effectiveness and long-term acceptance of fast-track permissions and go-to areas remains to be seen. Environmental impacts on wildlife and recycling challenges are rising issues for which tested and scalable solutions are often still lacking, pointing to large remaining research requirements.
{"title":"System impacts of wind energy developments: Key research challenges and opportunities","authors":"Russell McKenna , Johan Lilliestam , Heidi U. Heinrichs , Jann Weinand , Johannes Schmidt , Iain Staffell , Andrea N. Hahmann , Peter Burgherr , Arne Burdack , Monika Bucha , Ruihong Chen , Michael Klingler , Paul Lehmann , Jens Lowitzsch , Riccardo Novo , James Price , Romain Sacchi , Patrick Scherhaufer , Eva M. Schöll , Piero Visconti , Luis Ramirez Camargo","doi":"10.1016/j.joule.2024.11.016","DOIUrl":"10.1016/j.joule.2024.11.016","url":null,"abstract":"<div><div>Wind power accounted for 8% of global electricity generation in 2023 and is one of the cheapest forms of low-carbon electricity. Although fully commercial, many challenges remain in achieving the required scale-up, relating to integrating wind farms into wider technical, economic, social, and natural systems. We review the main challenges, outline existing solutions, and propose future research needed to overcome existing problems. Although the techno-economic challenges of grid and market integration are seen as significant obstacles to scaling up wind power, the field is replete with solutions. In many countries, planning and permitting are immediate barriers to wind-power deployment; although solutions are emerging in the EU and several countries, the effectiveness and long-term acceptance of fast-track permissions and go-to areas remains to be seen. Environmental impacts on wildlife and recycling challenges are rising issues for which tested and scalable solutions are often still lacking, pointing to large remaining research requirements.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 1","pages":"Article 101799"},"PeriodicalIF":38.6,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142967949","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}
Pub Date : 2025-01-15DOI: 10.1016/j.joule.2024.101819
Xiaona Li
Solid-state electrolytes are essential for enabling safe, high-performance all-solid-state batteries by providing a stable, non-flammable ionic pathway for lithium-ion transport while also improving overall battery safety and energy density. Recently in Joule, Ohta et al. combined nonconductive lithium chloride and iron oxychloride to form a [Li1+δCl]δ+/[FeOCl]δ− heterointerface composite with ionic conductivities exceeding 1 mS cm−1, offering a new methodology to design solid-state electrolyte materials.
固态电解质通过为锂离子传输提供稳定、不易燃的离子通道，同时提高电池的整体安全性和能量密度，对于实现安全、高性能的全固态电池至关重要。最近在Joule上，Ohta等人将不导电的氯化锂和氯化铁结合形成离子电导率超过1 mS cm−1的[Li1+δ cl]δ+/[FeOCl]δ−异质界面复合材料，为设计固态电解质材料提供了一种新的方法。
{"title":"Harnessing heterointerfaces for superionic conductivity","authors":"Xiaona Li","doi":"10.1016/j.joule.2024.101819","DOIUrl":"10.1016/j.joule.2024.101819","url":null,"abstract":"<div><div>Solid-state electrolytes are essential for enabling safe, high-performance all-solid-state batteries by providing a stable, non-flammable ionic pathway for lithium-ion transport while also improving overall battery safety and energy density. Recently in <em>Joule</em>, Ohta et al. combined nonconductive lithium chloride and iron oxychloride to form a [Li<sub>1+δ</sub>Cl]<sup>δ+</sup>/[FeOCl]<sup>δ−</sup> heterointerface composite with ionic conductivities exceeding 1 mS cm<sup>−1</sup>, offering a new methodology to design solid-state electrolyte materials.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 1","pages":"Article 101819"},"PeriodicalIF":38.6,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981649","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}
Pub Date : 2025-01-15DOI: 10.1016/j.joule.2024.09.014
Anand Selvin Subbiah , Subhashri Mannar , Vladyslav Hnapovskyi , Anil Reddy Pininti , Badri Vishal , Luis Victor Torres Merino , Oleksandr Matiash , Orestis Karalis , Hannes Hempel , Adi Prasetio , Bumin Yildirim , Pia Dally , Diego Rosas Villalva , Maxime Babics , Lujia Xu , Arsalan Razzaq , Randi Azmi , Fuzong Xu , Helen L. Bristow , Esma Ugur , Stefaan De Wolf
Monolithic perovskite/silicon tandem solar cells have recently reached a certified record power conversion efficiency (PCE) of 34.6%. However, most of the high-efficiency tandems rely on spin coating to fabricate the perovskite absorber, which generally has limited scope for mass production. To address this, we demonstrate the potential of linear printing techniques, systematically improving 1.66 eV wide-band-gap (WBG) perovskites in single-junction perovskite solar cells (PSCs) via blade coating. Also, we enhance defect passivation and energy alignment between adjacent contacts, thus improving charge extraction in such blade-coated PSCs by introducing 2D/3D perovskite heterojunctions at their electron- and hole-collecting interfaces. Translating the 2D integrated blade-coated PSCs to our monolithic perovskite/silicon tandems significantly improved their performance, enabling an independently certified PCE of 31.2% for blade-coated tandems. Importantly, the encapsulated tandems retain 80% of their initial PCE for ∼1,700 h under ∼1-sun continuous illumination, demonstrating their durability and potential toward long-term deployment.
{"title":"Efficient blade-coated perovskite/silicon tandems via interface engineering","authors":"Anand Selvin Subbiah , Subhashri Mannar , Vladyslav Hnapovskyi , Anil Reddy Pininti , Badri Vishal , Luis Victor Torres Merino , Oleksandr Matiash , Orestis Karalis , Hannes Hempel , Adi Prasetio , Bumin Yildirim , Pia Dally , Diego Rosas Villalva , Maxime Babics , Lujia Xu , Arsalan Razzaq , Randi Azmi , Fuzong Xu , Helen L. Bristow , Esma Ugur , Stefaan De Wolf","doi":"10.1016/j.joule.2024.09.014","DOIUrl":"10.1016/j.joule.2024.09.014","url":null,"abstract":"<div><div>Monolithic perovskite/silicon tandem solar cells have recently reached a certified record power conversion efficiency (PCE) of 34.6%. However, most of the high-efficiency tandems rely on spin coating to fabricate the perovskite absorber, which generally has limited scope for mass production. To address this, we demonstrate the potential of linear printing techniques, systematically improving 1.66 eV wide-band-gap (WBG) perovskites in single-junction perovskite solar cells (PSCs) via blade coating. Also, we enhance defect passivation and energy alignment between adjacent contacts, thus improving charge extraction in such blade-coated PSCs by introducing 2D/3D perovskite heterojunctions at their electron- and hole-collecting interfaces. Translating the 2D integrated blade-coated PSCs to our monolithic perovskite/silicon tandems significantly improved their performance, enabling an independently certified PCE of 31.2% for blade-coated tandems. Importantly, the encapsulated tandems retain 80% of their initial PCE for ∼1,700 h under ∼1-sun continuous illumination, demonstrating their durability and potential toward long-term deployment.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 1","pages":"Article 101767"},"PeriodicalIF":38.6,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452320","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}
Pub Date : 2025-01-15DOI: 10.1016/j.joule.2024.11.001
Ivette Aguilar , John Brown , Louis Godeffroy , Florian Dorchies , Véronique Balland , Frédéric Kanoufi , Jean-Marie Tarascon
Rechargeable aqueous devices, such as alkaline Zn/MnO2 batteries, hold strong potential for large-scale energy storage. However, they face limitations related to zinc and electrolyte degradation. Here, in the spirit of practicality, we have addressed these limitations by developing strategies aiming at resolving issues with the electrolyte, anode, and cathode independently at first, and then in synergy. We propose innovative electrolyte designs that incorporate select organic molecules to leverage hydrogen bonding interactions, reducing Zn nuclei reactivity via the formation of a stable solid electrolyte interphase (SEI). Our optimized Zn/MnO2 batteries demonstrate high stability, achieving a gravimetric capacity of ∼450 mAh/g (MnO2) and 90% capacity retention. Furthermore, we systematically show the scalability of our methods, moving from a Swagelok cell prototype (3–6 mg/cm2 of mass loading) to cylindrical-type cell (30 mg/cm2). These batteries can operate at unprecedentedly high temperatures of up to 55°C, while offering an energy density of 150 Wh/kg.
{"title":"A key advance toward practical aqueous Zn/MnO2 batteries via better electrolyte design","authors":"Ivette Aguilar , John Brown , Louis Godeffroy , Florian Dorchies , Véronique Balland , Frédéric Kanoufi , Jean-Marie Tarascon","doi":"10.1016/j.joule.2024.11.001","DOIUrl":"10.1016/j.joule.2024.11.001","url":null,"abstract":"<div><div>Rechargeable aqueous devices, such as alkaline Zn/MnO<sub>2</sub> batteries, hold strong potential for large-scale energy storage. However, they face limitations related to zinc and electrolyte degradation. Here, in the spirit of practicality, we have addressed these limitations by developing strategies aiming at resolving issues with the electrolyte, anode, and cathode independently at first, and then in synergy. We propose innovative electrolyte designs that incorporate select organic molecules to leverage hydrogen bonding interactions, reducing Zn nuclei reactivity via the formation of a stable solid electrolyte interphase (SEI). Our optimized Zn/MnO<sub>2</sub> batteries demonstrate high stability, achieving a gravimetric capacity of ∼450 mAh/g (MnO<sub>2</sub>) and 90% capacity retention. Furthermore, we systematically show the scalability of our methods, moving from a Swagelok cell prototype (3–6 mg/cm<sup>2</sup> of mass loading) to cylindrical-type cell (30 mg/cm<sup>2</sup>). These batteries can operate at unprecedentedly high temperatures of up to 55°C, while offering an energy density of 150 Wh/kg.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 1","pages":"Article 101784"},"PeriodicalIF":38.6,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142718885","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}
Electrochemical CO2 reduction reaction (ECO2RR) usually requires high-purity CO2 gas feeding. However, capturing CO2 from flue gas is still a cost- and energy-intensive process. Here, we design a bipolar membrane-integrated single-cell cyclic system that directly converts simulated flue gas into syngas. The system features a circulating gas-liquid mixed flow between the anode and cathode in an integrated cell, enabling it to simultaneously absorb CO2 from flue gas and convert captured CO2 into syngas. At an industrial current density of 250 mA/cm2, we successfully decrease the CO2 concentration in flue gas from 15% to 4.3% (with a 61.7% CO2 capture efficiency) and obtain high-selectivity (up to 100%) syngas (H2:CO = 3:1). Moreover, this cell has excellent tolerance to SOx and NOx due to the Ni single-atom catalyst in the cathode compared with previous studies. These results pave the way for low-concentration carbon dioxide conversion and promote the application of ECO2RR technology.
{"title":"Continuous conversion of flue gas into syngas by a bipolar membrane-integrated single-cell cyclic system","authors":"Dayin He, Xianhui Ma, Huang Zhou, Yu Zhang, Yuen Wu","doi":"10.1016/j.joule.2024.12.007","DOIUrl":"https://doi.org/10.1016/j.joule.2024.12.007","url":null,"abstract":"Electrochemical CO<sub>2</sub> reduction reaction (ECO<sub>2</sub>RR) usually requires high-purity CO<sub>2</sub> gas feeding. However, capturing CO<sub>2</sub> from flue gas is still a cost- and energy-intensive process. Here, we design a bipolar membrane-integrated single-cell cyclic system that directly converts simulated flue gas into syngas. The system features a circulating gas-liquid mixed flow between the anode and cathode in an integrated cell, enabling it to simultaneously absorb CO<sub>2</sub> from flue gas and convert captured CO<sub>2</sub> into syngas. At an industrial current density of 250 mA/cm<sup>2</sup>, we successfully decrease the CO<sub>2</sub> concentration in flue gas from 15% to 4.3% (with a 61.7% CO<sub>2</sub> capture efficiency) and obtain high-selectivity (up to 100%) syngas (H<sub>2</sub>:CO = 3:1). Moreover, this cell has excellent tolerance to SO<sub>x</sub> and NO<sub>x</sub> due to the Ni single-atom catalyst in the cathode compared with previous studies. These results pave the way for low-concentration carbon dioxide conversion and promote the application of ECO<sub>2</sub>RR technology.","PeriodicalId":343,"journal":{"name":"Joule","volume":"22 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142939527","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}
Pub Date : 2025-01-09DOI: 10.1016/j.joule.2024.12.001
Yongxi Li, Karthik Kamaraj, Yogita Silori, Haonan Zhao, Claire Arneson, Bin Liu, Jennifer Ogilvie, Stephen R. Forrest
We investigate the resilience of organic photovoltaic (OPV) cells to proton irradiation at doses equivalent to that experienced by spacecraft in low earth orbit. The OPVs, with their inherent flexibility, light weight, low temperature processing, and potential to achieve high specific power of 40 W/g, are promising candidates for energy production in space. However, their ability to withstand irradiation by high-energy incident radiation and subatomic particles characteristic of harsh space environments is yet unproven. We find that small-molecule OPVs grown by vacuum thermal evaporation are resistant to degradation by 30 keV proton irradiation, in contrast to polymer-based OPVs that suffer a 50% efficiency loss under similar conditions. Thermal annealing at low temperatures significantly restores the polymer-based OPV power conversion efficiency. The loss of efficiency is attributed to cleavage of pendant alkyl groups on the polymers, resulting in cross-linking and the subsequent formation of deep electronic traps.
{"title":"Radiation hardness of organic photovoltaics","authors":"Yongxi Li, Karthik Kamaraj, Yogita Silori, Haonan Zhao, Claire Arneson, Bin Liu, Jennifer Ogilvie, Stephen R. Forrest","doi":"10.1016/j.joule.2024.12.001","DOIUrl":"https://doi.org/10.1016/j.joule.2024.12.001","url":null,"abstract":"We investigate the resilience of organic photovoltaic (OPV) cells to proton irradiation at doses equivalent to that experienced by spacecraft in low earth orbit. The OPVs, with their inherent flexibility, light weight, low temperature processing, and potential to achieve high specific power of 40 W/g, are promising candidates for energy production in space. However, their ability to withstand irradiation by high-energy incident radiation and subatomic particles characteristic of harsh space environments is yet unproven. We find that small-molecule OPVs grown by vacuum thermal evaporation are resistant to degradation by 30 keV proton irradiation, in contrast to polymer-based OPVs that suffer a 50% efficiency loss under similar conditions. Thermal annealing at low temperatures significantly restores the polymer-based OPV power conversion efficiency. The loss of efficiency is attributed to cleavage of pendant alkyl groups on the polymers, resulting in cross-linking and the subsequent formation of deep electronic traps.","PeriodicalId":343,"journal":{"name":"Joule","volume":"20 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937354","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}
Pub Date : 2025-01-09DOI: 10.1016/j.joule.2024.12.002
Deokjae Choi, Donghoon Shin, Chongwen Li, Yuan Liu, Abdulaziz S.R. Bati, Dana E. Kachman, Yi Yang, Jiachen Li, Yoon Jung Lee, Muzhi Li, Saivineeth Penukula, Da Bin Kim, Heejong Shin, Chiung-Han Chen, So Min Park, Cheng Liu, Aidan Maxwell, Haoyue Wan, Nicholas Rolston, Edward H. Sargent, Bin Chen
Mixed-halide wide-band-gap perovskites are critical components of highly efficient tandem cells, but their operating stability is limited by halide migration. Metal oxides deposited via atomic layer deposition (ALD) have been shown to block halide migration; however, previously pursued methods result in inhomogeneous nucleation and growth. We hypothesized that functionalizing the perovskite surface with ALD-active carboxyl groups could promote nucleation and enable higher-temperature metal oxide growth. We find that 5-ammonium valeric acid iodide (5-AVAI) facilitates the formation of a compact and uniform aluminum oxide (Al2O3) layer and allows growth at 100°C compared with the previous limit of 75°C. We demonstrate that halide migration into the C60 electron transport layer is reduced by a factor of 10 compared with the reference case. Al2O3-capped perovskite solar cells with a band gap of 1.78 eV retain 90% of their initial power conversion efficiency after 1,000 h of continuous operation under 1-sun illumination at 55°C.
{"title":"Carboxyl-functionalized perovskite enables ALD growth of a compact and uniform ion migration barrier","authors":"Deokjae Choi, Donghoon Shin, Chongwen Li, Yuan Liu, Abdulaziz S.R. Bati, Dana E. Kachman, Yi Yang, Jiachen Li, Yoon Jung Lee, Muzhi Li, Saivineeth Penukula, Da Bin Kim, Heejong Shin, Chiung-Han Chen, So Min Park, Cheng Liu, Aidan Maxwell, Haoyue Wan, Nicholas Rolston, Edward H. Sargent, Bin Chen","doi":"10.1016/j.joule.2024.12.002","DOIUrl":"https://doi.org/10.1016/j.joule.2024.12.002","url":null,"abstract":"Mixed-halide wide-band-gap perovskites are critical components of highly efficient tandem cells, but their operating stability is limited by halide migration. Metal oxides deposited via atomic layer deposition (ALD) have been shown to block halide migration; however, previously pursued methods result in inhomogeneous nucleation and growth. We hypothesized that functionalizing the perovskite surface with ALD-active carboxyl groups could promote nucleation and enable higher-temperature metal oxide growth. We find that 5-ammonium valeric acid iodide (5-AVAI) facilitates the formation of a compact and uniform aluminum oxide (Al<sub>2</sub>O<sub>3</sub>) layer and allows growth at 100°C compared with the previous limit of 75°C. We demonstrate that halide migration into the C<sub>60</sub> electron transport layer is reduced by a factor of 10 compared with the reference case. Al<sub>2</sub>O<sub>3</sub>-capped perovskite solar cells with a band gap of 1.78 eV retain 90% of their initial power conversion efficiency after 1,000 h of continuous operation under 1-sun illumination at 55°C.","PeriodicalId":343,"journal":{"name":"Joule","volume":"27 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937597","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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