Pub Date : 2024-09-03DOI: 10.1038/s41560-024-01628-1
Timo Boehler, Dominic Bresser
Nickel-rich lithium-ion cathode materials face severe structural and interfacial instabilities when cycled at high potentials and high degrees of delithiation. Now, a LiNi0.8Mn0.1Co0.1O2 material with a complementary composition and structure gradient, composed of an ordered, layered Co-poor bulk phase and a Co-enriched disordered rock-salt surface layer, is shown to efficiently address the issues.
{"title":"Preserving order by controlled disorder","authors":"Timo Boehler, Dominic Bresser","doi":"10.1038/s41560-024-01628-1","DOIUrl":"10.1038/s41560-024-01628-1","url":null,"abstract":"Nickel-rich lithium-ion cathode materials face severe structural and interfacial instabilities when cycled at high potentials and high degrees of delithiation. Now, a LiNi0.8Mn0.1Co0.1O2 material with a complementary composition and structure gradient, composed of an ordered, layered Co-poor bulk phase and a Co-enriched disordered rock-salt surface layer, is shown to efficiently address the issues.","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":49.7,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142123616","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 : 2024-08-26DOI: 10.1038/s41560-024-01583-x
Jin Suntivich, Geoffroy Hautier, Ismaila Dabo, Ethan J. Crumlin, Dhananjay Kumar, Tanja Cuk
The oxygen evolution reaction is crucial to sustainable electro- and photo-electrochemical approaches to chemical energy production (for example, H2). Although mechanistic descriptions of the oxygen evolution reaction have been proposed, the frontier challenge is to extract the molecular details of its elementary steps. Here we discuss how advances in spectroscopy and theory are allowing for configurations of reaction intermediates to be elucidated, distinguishing between experimental approaches (static and dynamic) across a range of surface oxygen binding energies on catalysts (from ruthenium to titanium oxides). We outline how interpreting X-ray and optical spectra relies on established and newly implemented computational techniques. A key emphasis is on detecting adsorbed oxygen intermediates at the oxide/water interface by their chemical composition, electronic and vibrational levels and ion–electron kinetic pathways. Integrating the computational advances with the experimental spectra along these lines could ultimately resolve the elementary steps, elucidating how each intermediate leads to another during oxygen evolution reaction. Oxygen evolution is a critical reaction in the context of renewable fuel production via (photo)electrochemical approaches, yet our understanding of the molecular details of the reaction is limited. Here, the authors explore how specific spectroscopic probes and theory can be combined to reveal the elementary reaction steps.
氧进化反应对于以可持续的电化学和光电化学方法生产化学能（如 H2）至关重要。虽然已经提出了氧进化反应的机理描述，但前沿挑战是提取其基本步骤的分子细节。在此，我们将讨论光谱学和理论的进步如何使反应中间产物的构型得以阐明，并区分催化剂（从钌到钛氧化物）表面氧结合能范围内的实验方法（静态和动态）。我们概述了 X 射线和光学光谱的解释如何依赖于已有的和新实施的计算技术。重点是通过化学成分、电子和振动水平以及离子-电子动力学路径来检测氧化物/水界面上吸附的氧中间体。按照这些思路将计算进展与实验光谱相结合，最终可以解决基本步骤问题，阐明在氧进化反应过程中每个中间体如何导致另一个中间体。
{"title":"Probing intermediate configurations of oxygen evolution catalysis across the light spectrum","authors":"Jin Suntivich, Geoffroy Hautier, Ismaila Dabo, Ethan J. Crumlin, Dhananjay Kumar, Tanja Cuk","doi":"10.1038/s41560-024-01583-x","DOIUrl":"10.1038/s41560-024-01583-x","url":null,"abstract":"The oxygen evolution reaction is crucial to sustainable electro- and photo-electrochemical approaches to chemical energy production (for example, H2). Although mechanistic descriptions of the oxygen evolution reaction have been proposed, the frontier challenge is to extract the molecular details of its elementary steps. Here we discuss how advances in spectroscopy and theory are allowing for configurations of reaction intermediates to be elucidated, distinguishing between experimental approaches (static and dynamic) across a range of surface oxygen binding energies on catalysts (from ruthenium to titanium oxides). We outline how interpreting X-ray and optical spectra relies on established and newly implemented computational techniques. A key emphasis is on detecting adsorbed oxygen intermediates at the oxide/water interface by their chemical composition, electronic and vibrational levels and ion–electron kinetic pathways. Integrating the computational advances with the experimental spectra along these lines could ultimately resolve the elementary steps, elucidating how each intermediate leads to another during oxygen evolution reaction. Oxygen evolution is a critical reaction in the context of renewable fuel production via (photo)electrochemical approaches, yet our understanding of the molecular details of the reaction is limited. Here, the authors explore how specific spectroscopic probes and theory can be combined to reveal the elementary reaction steps.","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":49.7,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142085368","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 : 2024-08-26DOI: 10.1038/s41560-024-01616-5
Feixiang Ding, Pengxiang Ji, Zhen Han, Xueyan Hou, Yang Yang, Zilin Hu, Yaoshen Niu, Yuan Liu, Jiao Zhang, Xiaohui Rong, Yaxiang Lu, Huican Mao, Dong Su, Liquan Chen, Yong-Sheng Hu
High-entropy oxides have expanded the potential for high-performance Na-ion battery cathodes due to their vast compositional space and entropy-driven stabilization. However, a rational design approach for optimizing their composition is still lacking. Here, we develop an O3-type oxide cathode composed of all-3d transition metals, NaNi0.3Cu0.1Fe0.2Mn0.3Ti0.1O2 (NCFMT), which exhibits improved reversible specific capacity and exceptional cycling stability. Replacing Ti4+ with Sn4+ ions (NaNi0.3Cu0.1Fe0.2Mn0.3Sn0.1O2; NCFMS) results in poor structural reversibility and diminished cycling stability. Our investigations suggest that the structural integrity of the layered cathode is affected by the compatibility of constituent elements within the transition metal layers (TMO2). In NCFMS, planar strain induced by metal-ion displacement triggers elemental segregation and crack formation during repeated cycling. In contrast, NCFMT demonstrates a robust structural framework for stable Na+ storage due to its high mechanochemical compatibility among constituent elements. This understanding provides insights for designing outstanding layered high-entropy cathode materials.
{"title":"Tailoring planar strain for robust structural stability in high-entropy layered sodium oxide cathode materials","authors":"Feixiang Ding, Pengxiang Ji, Zhen Han, Xueyan Hou, Yang Yang, Zilin Hu, Yaoshen Niu, Yuan Liu, Jiao Zhang, Xiaohui Rong, Yaxiang Lu, Huican Mao, Dong Su, Liquan Chen, Yong-Sheng Hu","doi":"10.1038/s41560-024-01616-5","DOIUrl":"https://doi.org/10.1038/s41560-024-01616-5","url":null,"abstract":"<p>High-entropy oxides have expanded the potential for high-performance Na-ion battery cathodes due to their vast compositional space and entropy-driven stabilization. However, a rational design approach for optimizing their composition is still lacking. Here, we develop an O3-type oxide cathode composed of all-3<i>d</i> transition metals, NaNi<sub>0.3</sub>Cu<sub>0.1</sub>Fe<sub>0.2</sub>Mn<sub>0.3</sub>Ti<sub>0.1</sub>O<sub>2</sub> (NCFMT), which exhibits improved reversible specific capacity and exceptional cycling stability. Replacing Ti<sup>4+</sup> with Sn<sup>4+</sup> ions (NaNi<sub>0.3</sub>Cu<sub>0.1</sub>Fe<sub>0.2</sub>Mn<sub>0.3</sub>Sn<sub>0.1</sub>O<sub>2</sub>; NCFMS) results in poor structural reversibility and diminished cycling stability. Our investigations suggest that the structural integrity of the layered cathode is affected by the compatibility of constituent elements within the transition metal layers (TMO<sub>2</sub>). In NCFMS, planar strain induced by metal-ion displacement triggers elemental segregation and crack formation during repeated cycling. In contrast, NCFMT demonstrates a robust structural framework for stable Na<sup>+</sup> storage due to its high mechanochemical compatibility among constituent elements. This understanding provides insights for designing outstanding layered high-entropy cathode materials.</p>","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":56.7,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142085373","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 : 2024-08-23DOI: 10.1038/s41560-024-01626-3
Giulia Tregnago
{"title":"Improvements at the junction","authors":"Giulia Tregnago","doi":"10.1038/s41560-024-01626-3","DOIUrl":"10.1038/s41560-024-01626-3","url":null,"abstract":"","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":49.7,"publicationDate":"2024-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142045339","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 : 2024-08-23DOI: 10.1038/s41560-024-01617-4
Dominic P. Parker, Sarah Johnston, Bryan Leonard, Daniel Stewart, Justin B. Winikoff
Could renewable energy development on American Indian Reservations alleviate poverty? This Article combines data on wind and solar endowments, reservation characteristics and utility-scale renewable energy projects to offer three insights. First, the colonial process of reservation creation that intentionally deprived tribes of other natural resources unintentionally left them with favourable wind and solar, especially on reservations with the lowest-income populations. Second, despite favourable endowments, renewable projects are rare: reservation lands are 46% less likely to host wind farms and 110% less likely to host solar than comparable adjacent lands. Third, if this disparity persists, tribes may forgo over US$19 billion in lease and tax earnings that could be accrued under forecasts of renewable energy demand through 2050. We highlight barriers—such as regulatory complexity and uncertainty—that help explain this disparity and emphasize this is not a call to impose federal energy priorities on unwilling tribes.
{"title":"Economic potential of wind and solar in American Indian communities","authors":"Dominic P. Parker, Sarah Johnston, Bryan Leonard, Daniel Stewart, Justin B. Winikoff","doi":"10.1038/s41560-024-01617-4","DOIUrl":"https://doi.org/10.1038/s41560-024-01617-4","url":null,"abstract":"<p>Could renewable energy development on American Indian Reservations alleviate poverty? This Article combines data on wind and solar endowments, reservation characteristics and utility-scale renewable energy projects to offer three insights. First, the colonial process of reservation creation that intentionally deprived tribes of other natural resources unintentionally left them with favourable wind and solar, especially on reservations with the lowest-income populations. Second, despite favourable endowments, renewable projects are rare: reservation lands are 46% less likely to host wind farms and 110% less likely to host solar than comparable adjacent lands. Third, if this disparity persists, tribes may forgo over US$19 billion in lease and tax earnings that could be accrued under forecasts of renewable energy demand through 2050. We highlight barriers—such as regulatory complexity and uncertainty—that help explain this disparity and emphasize this is not a call to impose federal energy priorities on unwilling tribes.</p>","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":56.7,"publicationDate":"2024-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142042636","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 : 2024-08-23DOI: 10.1038/s41560-024-01615-6
Yimeng Huang, Yanhao Dong, Yang Yang, Tongchao Liu, Moonsu Yoon, Sipei Li, Baoming Wang, Ethan Yupeng Zheng, Jinhyuk Lee, Yongwen Sun, Ying Han, Jim Ciston, Colin Ophus, Chengyu Song, Aubrey Penn, Yaqi Liao, Haijin Ji, Ting Shi, Mengyi Liao, Zexiao Cheng, Jingwei Xiang, Yu Peng, Lu Ma, Xianghui Xiao, Wang Hay Kan, Huaican Chen, Wen Yin, Lingling Guo, Wei-Ren Liu, Rasu Muruganantham, Chun-Chuen Yang, Yuntong Zhu, Qingjie Li, Ju Li
Co- and Ni-free disordered rocksalt cathodes utilize oxygen redox to increase the energy density of lithium-ion batteries, but it is challenging to achieve good cycle life at high voltages >4.5 V (versus Li/Li+). Here we report a family of Li-excess Mn-rich cathodes that integrates rocksalt- and polyanion-type structures. Following design rules for cation filling and ordering, we demonstrate the bulk incorporation of polyanion groups into the rocksalt lattice. This integration bridges the two primary families of lithium-ion battery cathodes—layered/spinel and phosphate oxides—dramatically enhancing the cycling stability of disordered rocksalt cathodes with 4.8 V upper cut-off voltage. The cathode exhibits high gravimetric energy densities above 1,100 Wh kg−1 and >70% retention over 100 cycles. This study opens up a broad compositional space for developing battery cathodes using earth-abundant elements such as Mn and Fe.
{"title":"Integrated rocksalt–polyanion cathodes with excess lithium and stabilized cycling","authors":"Yimeng Huang, Yanhao Dong, Yang Yang, Tongchao Liu, Moonsu Yoon, Sipei Li, Baoming Wang, Ethan Yupeng Zheng, Jinhyuk Lee, Yongwen Sun, Ying Han, Jim Ciston, Colin Ophus, Chengyu Song, Aubrey Penn, Yaqi Liao, Haijin Ji, Ting Shi, Mengyi Liao, Zexiao Cheng, Jingwei Xiang, Yu Peng, Lu Ma, Xianghui Xiao, Wang Hay Kan, Huaican Chen, Wen Yin, Lingling Guo, Wei-Ren Liu, Rasu Muruganantham, Chun-Chuen Yang, Yuntong Zhu, Qingjie Li, Ju Li","doi":"10.1038/s41560-024-01615-6","DOIUrl":"https://doi.org/10.1038/s41560-024-01615-6","url":null,"abstract":"<p>Co- and Ni-free disordered rocksalt cathodes utilize oxygen redox to increase the energy density of lithium-ion batteries, but it is challenging to achieve good cycle life at high voltages >4.5 V (versus Li/Li<sup>+</sup>). Here we report a family of Li-excess Mn-rich cathodes that integrates rocksalt- and polyanion-type structures. Following design rules for cation filling and ordering, we demonstrate the bulk incorporation of polyanion groups into the rocksalt lattice. This integration bridges the two primary families of lithium-ion battery cathodes—layered/spinel and phosphate oxides—dramatically enhancing the cycling stability of disordered rocksalt cathodes with 4.8 V upper cut-off voltage. The cathode exhibits high gravimetric energy densities above 1,100 Wh kg<sup>−1</sup> and >70% retention over 100 cycles. This study opens up a broad compositional space for developing battery cathodes using earth-abundant elements such as Mn and Fe.</p>","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":56.7,"publicationDate":"2024-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142042635","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}
Cation solvation is well understood in the bulk solution phase, but knowledge is limited regarding the electrode–electrolyte interface. The process by which cation solvation conforms to the interfacial field to form interphases remains unclear. Here we examine the synergistic effects of external and intramolecular fields on accommodating Li+ solvates to the Li-metal anode, leading to dielectric-mediated transfer dynamics on the interface. At charged interfaces, cation–anion pairs arrange in a periodic oscillatory distribution. A low-oscillation amplitude exacerbates the electrolyte decomposition and increases surface impedance. We propose a dielectric protocol that maintains cation–anion coordination with a high oscillation amplitude at the interfaces, addressing these issues. Accordingly, we demonstrate a Li-metal pouch cell with an energy density of 500 Wh kg−1 at the Ah level using an ultra-lean electrolyte (1 g Ah−1). Our study offers insights into solid/liquid interfaces that are crucial in advancing battery technologies. Cation solvation in batteries is well understood in bulk solutions but less so at electrode/electrolyte interfaces. This study reveals how external and intramolecular fields affect Li-ion solvation, proposing a dielectric protocol to enhance cation–anion coordination and improve performance in Li-metal pouch cells.
人们对阳离子溶解在溶液体相中的作用了解甚多，但对电解质-电解质界面的了解却很有限。阳离子溶解符合界面场以形成相间的过程仍不清楚。在此，我们研究了外部场和分子内场对锂金属阳极容纳 Li+ 溶解物的协同效应，从而导致界面上介电介质介导的转移动力学。在带电界面上，阳离子-阴离子对呈周期性振荡分布。低振荡振幅会加剧电解质分解并增加表面阻抗。为了解决这些问题，我们提出了一种电介质协议，它能在界面上以高振荡幅度保持阳离子-阴离子配位。因此，我们利用超低电解质（1 g Ah-1）演示了能量密度为 500 Wh kg-1 的锂金属袋电池。我们的研究为固态/液态界面提供了深入的见解，这对推动电池技术的发展至关重要。
{"title":"Oscillatory solvation chemistry for a 500 Wh kg−1 Li-metal pouch cell","authors":"Shuoqing Zhang, Ruhong Li, Tao Deng, Qiang Ma, Xiang Hong, Hao Zhang, Ruixin Zhang, Shouhong Ding, Yongjian Wu, Haotian Zhu, Menglu Li, Haikuo Zhang, Di Lu, Baochen Ma, Ling Lv, Yong Li, Lixin Chen, Yanbin Shen, Rui Guo, Xiulin Fan","doi":"10.1038/s41560-024-01621-8","DOIUrl":"10.1038/s41560-024-01621-8","url":null,"abstract":"Cation solvation is well understood in the bulk solution phase, but knowledge is limited regarding the electrode–electrolyte interface. The process by which cation solvation conforms to the interfacial field to form interphases remains unclear. Here we examine the synergistic effects of external and intramolecular fields on accommodating Li+ solvates to the Li-metal anode, leading to dielectric-mediated transfer dynamics on the interface. At charged interfaces, cation–anion pairs arrange in a periodic oscillatory distribution. A low-oscillation amplitude exacerbates the electrolyte decomposition and increases surface impedance. We propose a dielectric protocol that maintains cation–anion coordination with a high oscillation amplitude at the interfaces, addressing these issues. Accordingly, we demonstrate a Li-metal pouch cell with an energy density of 500 Wh kg−1 at the Ah level using an ultra-lean electrolyte (1 g Ah−1). Our study offers insights into solid/liquid interfaces that are crucial in advancing battery technologies. Cation solvation in batteries is well understood in bulk solutions but less so at electrode/electrolyte interfaces. This study reveals how external and intramolecular fields affect Li-ion solvation, proposing a dielectric protocol to enhance cation–anion coordination and improve performance in Li-metal pouch cells.","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":49.7,"publicationDate":"2024-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142022035","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 : 2024-08-22DOI: 10.1038/s41560-024-01618-3
Bernd Stannowski, Lars Korte
The highest power conversion efficiencies for silicon heterojunction solar cells have been achieved on devices based on n-type doped silicon wafers, yet these wafers are usually more expensive than p-type ones. Now, researchers reduce charge recombination in the bulk of p-type silicon, demonstrating comparable efficiency to devices based on n-type silicon.
硅异质结太阳能电池的最高功率转换效率是在基于 n 型掺杂硅晶片的设备上实现的，但这些晶片通常比 p 型晶片昂贵。现在，研究人员减少了 p 型硅块中的电荷重组，显示出与基于 n 型硅的设备相当的效率。
{"title":"Top performance whatever the doping","authors":"Bernd Stannowski, Lars Korte","doi":"10.1038/s41560-024-01618-3","DOIUrl":"10.1038/s41560-024-01618-3","url":null,"abstract":"The highest power conversion efficiencies for silicon heterojunction solar cells have been achieved on devices based on n-type doped silicon wafers, yet these wafers are usually more expensive than p-type ones. Now, researchers reduce charge recombination in the bulk of p-type silicon, demonstrating comparable efficiency to devices based on n-type silicon.","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":null,"pages":null},"PeriodicalIF":49.7,"publicationDate":"2024-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142022038","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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