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":"740 1","pages":""},"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":"3 1","pages":""},"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":"9 10","pages":"1285-1296"},"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":"9 9","pages":"1058-1059"},"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}
Pub Date : 2024-08-21DOI: 10.1038/s41560-024-01612-9
Giulia Tregnago
POWERful Women is a professional initiative established in 2014 targeting a gender-balanced, diverse and inclusive energy sector in the UK. To mark the tenth anniversary, Katie Jackson — Chair of POWERful Women — talks to Nature Energy about progress so far and the challenges ahead.
POWERful Women 是一项成立于 2014 年的专业倡议,旨在实现英国能源行业的性别平衡、多元化和包容性。为纪念成立十周年,POWERful Women 主席凯蒂-杰克逊(Katie Jackson)向《自然-能源》杂志讲述了迄今为止取得的进展以及未来面临的挑战。
{"title":"Increasing women’s representation in the energy sector","authors":"Giulia Tregnago","doi":"10.1038/s41560-024-01612-9","DOIUrl":"10.1038/s41560-024-01612-9","url":null,"abstract":"POWERful Women is a professional initiative established in 2014 targeting a gender-balanced, diverse and inclusive energy sector in the UK. To mark the tenth anniversary, Katie Jackson — Chair of POWERful Women — talks to Nature Energy about progress so far and the challenges ahead.","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":"9 10","pages":"1177-1178"},"PeriodicalIF":49.7,"publicationDate":"2024-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142013828","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 : 2024-08-21DOI: 10.1038/s41560-024-01585-9
Holly Caggiano, Sara M. Constantino, Chris Greig, Elke U. Weber
In the United States, Democrats and Republicans are more likely to support energy projects that are community-owned, create jobs, and generate solar energy, but local elected officials underestimate their constituents’ support for projects with these characteristics. Since these officials play a key role in approving new energy projects and negotiating the benefits they bring to communities, aligning local elected officials’ perceptions with the public’s could improve progress toward just energy transitions.
{"title":"Community benefits can build bipartisan support for large-scale energy infrastructure","authors":"Holly Caggiano, Sara M. Constantino, Chris Greig, Elke U. Weber","doi":"10.1038/s41560-024-01585-9","DOIUrl":"10.1038/s41560-024-01585-9","url":null,"abstract":"In the United States, Democrats and Republicans are more likely to support energy projects that are community-owned, create jobs, and generate solar energy, but local elected officials underestimate their constituents’ support for projects with these characteristics. Since these officials play a key role in approving new energy projects and negotiating the benefits they bring to communities, aligning local elected officials’ perceptions with the public’s could improve progress toward just energy transitions.","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":"9 10","pages":"1187-1188"},"PeriodicalIF":49.7,"publicationDate":"2024-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41560-024-01585-9.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142013827","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 : 2024-08-20DOI: 10.1038/s41560-024-01619-2
Ai-Min Li, Zeyi Wang, Taeyong Lee, Nan Zhang, Tianyu Li, Weiran Zhang, Chamithri Jayawardana, Munaiah Yeddala, Brett L. Lucht, Chunsheng Wang
Micro-sized alloying anodes offer lower cost and higher capacity than graphite in Li-ion batteries. However, they suffer from fast capacity decay and low Coulombic efficiency in carbonate electrolytes because the organic solid electrolyte interphase (SEI) strongly bonds to the alloys, leading to cracks of both SEI and alloying particles, which allows electrolyte penetration and forms new SEI during lithiation–delithiation cycles. Using nano-sized alloying anodes can enhance the cell cycle life but also reduces the battery calendar life and increases the manufacturing costs. Here we significantly improved the cycle performance of micro-sized Si, Al, Sn and Bi anodes by developing asymmetric electrolytes (solvent-free ionic liquids and molecular solvent) to form LiF-rich inorganic SEI, enabling 90 mAh μSi||LiNi0.8Mn0.1Co0.1O2 and 70 mAh Li3.75Si||SPAN pouch cells (areal capacity of 4.5 mAh cm−2; N/P of 1.4) to achieve >400 cycles with a high capacity retention of >85%. The asymmetric electrolyte design forms LiF-rich interphases that enable high-capacity anodes and high-energy cathodes to achieve a long cycle life and provide a general solution for high-energy Li-ion batteries.
在锂离子电池中,微尺寸合金阳极比石墨成本更低,容量更大。然而,它们在碳酸盐电解质中存在容量衰减快和库仑效率低的问题,这是因为有机固体电解质相(SEI)与合金紧密结合,导致 SEI 和合金颗粒出现裂缝,从而使电解质渗透,并在锂化-退锂循环过程中形成新的 SEI。使用纳米尺寸的合金阳极可以提高电池循环寿命,但同时也会缩短电池日历寿命并增加制造成本。在这里,我们通过开发非对称电解质(无溶剂离子液体和分子溶剂)来形成富含 LiF 的无机 SEI,从而大幅提高了微尺寸 Si、Al、Sn 和 Bi 阳极的循环性能,使 90 mAh μSi||LiNi0.8Mn0.1Co0.1O2 和 70 mAh Li3.75Si||SPAN 袋式电池(等容量为 4.5 mAh cm-2;N/P 为 1.4)实现了 400 次循环,容量保持率高达 85%。非对称电解质设计形成了富含锂富相间,使高容量阳极和高能量阴极实现了长循环寿命,为高能量锂离子电池提供了通用解决方案。
{"title":"Asymmetric electrolyte design for high-energy lithium-ion batteries with micro-sized alloying anodes","authors":"Ai-Min Li, Zeyi Wang, Taeyong Lee, Nan Zhang, Tianyu Li, Weiran Zhang, Chamithri Jayawardana, Munaiah Yeddala, Brett L. Lucht, Chunsheng Wang","doi":"10.1038/s41560-024-01619-2","DOIUrl":"https://doi.org/10.1038/s41560-024-01619-2","url":null,"abstract":"<p>Micro-sized alloying anodes offer lower cost and higher capacity than graphite in Li-ion batteries. However, they suffer from fast capacity decay and low Coulombic efficiency in carbonate electrolytes because the organic solid electrolyte interphase (SEI) strongly bonds to the alloys, leading to cracks of both SEI and alloying particles, which allows electrolyte penetration and forms new SEI during lithiation–delithiation cycles. Using nano-sized alloying anodes can enhance the cell cycle life but also reduces the battery calendar life and increases the manufacturing costs. Here we significantly improved the cycle performance of micro-sized Si, Al, Sn and Bi anodes by developing asymmetric electrolytes (solvent-free ionic liquids and molecular solvent) to form LiF-rich inorganic SEI, enabling 90 mAh μSi||LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> and 70 mAh Li<sub>3.75</sub>Si||SPAN pouch cells (areal capacity of 4.5 mAh cm<sup>−2</sup>; N/P of 1.4) to achieve >400 cycles with a high capacity retention of >85%. The asymmetric electrolyte design forms LiF-rich interphases that enable high-capacity anodes and high-energy cathodes to achieve a long cycle life and provide a general solution for high-energy Li-ion batteries.</p>","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":"23 1","pages":""},"PeriodicalIF":56.7,"publicationDate":"2024-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142007635","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 : 2024-08-19DOI: 10.1038/s41560-024-01601-y
Ben Farrer, Robert Holahan, Kellyanne Allen, Lydia Allen, Jonathan E. Doriscar, Victoria Johnson, Tara Riggs, Soleil Smith
To extract natural gas through hydraulic fracturing, energy companies often need to obtain consent from many different private landowners, whose properties lie atop the gas reservoir. Negotiations with these landowners have important economic, environmental and social implications. In this paper we present a dataset on negotiations in Ohio and use these data to investigate how landowners may be advantaged or disadvantaged in these lease negotiations. We find that they are disadvantaged in two ways. First, because energy companies can use persistent and personal strategies to overcome landowner reluctance. Second, because of the institutional context: specifically the widespread use of compulsory unitization. We conclude by discussing the implications of these findings for equity in energy policy and by drawing out the other potential uses of these data.
{"title":"Assessing how energy companies negotiate with landowners when obtaining land for hydraulic fracturing","authors":"Ben Farrer, Robert Holahan, Kellyanne Allen, Lydia Allen, Jonathan E. Doriscar, Victoria Johnson, Tara Riggs, Soleil Smith","doi":"10.1038/s41560-024-01601-y","DOIUrl":"https://doi.org/10.1038/s41560-024-01601-y","url":null,"abstract":"<p>To extract natural gas through hydraulic fracturing, energy companies often need to obtain consent from many different private landowners, whose properties lie atop the gas reservoir. Negotiations with these landowners have important economic, environmental and social implications. In this paper we present a dataset on negotiations in Ohio and use these data to investigate how landowners may be advantaged or disadvantaged in these lease negotiations. We find that they are disadvantaged in two ways. First, because energy companies can use persistent and personal strategies to overcome landowner reluctance. Second, because of the institutional context: specifically the widespread use of compulsory unitization. We conclude by discussing the implications of these findings for equity in energy policy and by drawing out the other potential uses of these data.</p>","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":"67 1","pages":""},"PeriodicalIF":56.7,"publicationDate":"2024-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142002805","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 : 2024-08-16DOI: 10.1038/s41560-024-01614-7
Andong Liu, Charles B. Musgrave, Xing Li, William A. Goddard, Yayuan Liu
Electrochemically mediated carbon capture utilizing redox-tunable organic sorbents has emerged as a promising strategy to mitigate anthropogenic carbon dioxide emissions. However, most reported systems are sensitive to molecular oxygen, severely limiting their application under ambient air conditions. Here we demonstrate an electrochemical carbon capture concept via non-aqueous proton-coupled electron transfer, where alkoxides are employed as the active sorbent while carbon dioxide absorption and desorption are modulated reversibly by the redox-tunable Brønsted basicity of certain organic molecules. Since all species involved in the process have outstanding oxygen stability and relatively low vapour pressure, our electrochemically mediated carbon capture mechanism intrinsically minimizes parasitic reactions and evaporative losses under aerobic conditions. Flow-based prototypes are demonstrated to operate efficiently in the presence of 20% oxygen under various practically relevant carbon dioxide feed concentrations, paving a way towards effective carbon capture driven by electrochemical stimuli.
{"title":"Non-aqueous alkoxide-mediated electrochemical carbon capture","authors":"Andong Liu, Charles B. Musgrave, Xing Li, William A. Goddard, Yayuan Liu","doi":"10.1038/s41560-024-01614-7","DOIUrl":"https://doi.org/10.1038/s41560-024-01614-7","url":null,"abstract":"<p>Electrochemically mediated carbon capture utilizing redox-tunable organic sorbents has emerged as a promising strategy to mitigate anthropogenic carbon dioxide emissions. However, most reported systems are sensitive to molecular oxygen, severely limiting their application under ambient air conditions. Here we demonstrate an electrochemical carbon capture concept via non-aqueous proton-coupled electron transfer, where alkoxides are employed as the active sorbent while carbon dioxide absorption and desorption are modulated reversibly by the redox-tunable Brønsted basicity of certain organic molecules. Since all species involved in the process have outstanding oxygen stability and relatively low vapour pressure, our electrochemically mediated carbon capture mechanism intrinsically minimizes parasitic reactions and evaporative losses under aerobic conditions. Flow-based prototypes are demonstrated to operate efficiently in the presence of 20% oxygen under various practically relevant carbon dioxide feed concentrations, paving a way towards effective carbon capture driven by electrochemical stimuli.</p>","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":"23 1","pages":""},"PeriodicalIF":56.7,"publicationDate":"2024-08-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141991812","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 : 2024-08-15DOI: 10.1038/s41560-024-01613-8
Chongwen Li, Lei Chen, Fangyuan Jiang, Zhaoning Song, Xiaoming Wang, Adam Balvanz, Esma Ugur, Yuan Liu, Cheng Liu, Aidan Maxwell, Hao Chen, Yanjiang Liu, Zaiwei Wang, Pan Xia, You Li, Sheng Fu, Nannan Sun, Corey R. Grice, Xuefei Wu, Zachary Fink, Qin Hu, Lewei Zeng, Euidae Jung, Junke Wang, So Min Park, Deying Luo, Cailing Chen, Jie Shen, Yu Han, Carlo Andrea Riccardo Perini, Juan-Pablo Correa-Baena, Zheng-Hong Lu, Thomas P. Russell, Stefaan De Wolf, Mercouri G. Kanatzidis, David S. Ginger, Bin Chen, Yanfa Yan, Edward H. Sargent
Perovskite tandem solar cells show promising performance, but non-radiative recombination and its progressive worsening with time, especially in the mixed Sn–Pb low-bandgap layer, limit performance and stability. Here we find that mixed Sn–Pb perovskite thin films exhibit a compositional gradient, with an excess of Sn on the surface—and we show this gradient exacerbates oxidation and increases the recombination rate. We find that diamines preferentially chelate Sn atoms, removing them from the film surface and achieving a more balanced Sn:Pb stoichiometry, making the surface of the film resistive to the oxidation of Sn. The process forms an electrically resistive low-dimensional barrier layer, passivating defects and reducing interface recombination. Further improving the homogeneity of the barrier layer using 1,2-diaminopropane results in more uniform distribution and passivation. Tandems achieve a power conversion efficiency of 28.8%. Encapsulated tandems retain 90% of initial efficiency following 1,000 h of operating at the maximum power point under simulated one-sun illumination in air without cooling.
{"title":"Diamine chelates for increased stability in mixed Sn–Pb and all-perovskite tandem solar cells","authors":"Chongwen Li, Lei Chen, Fangyuan Jiang, Zhaoning Song, Xiaoming Wang, Adam Balvanz, Esma Ugur, Yuan Liu, Cheng Liu, Aidan Maxwell, Hao Chen, Yanjiang Liu, Zaiwei Wang, Pan Xia, You Li, Sheng Fu, Nannan Sun, Corey R. Grice, Xuefei Wu, Zachary Fink, Qin Hu, Lewei Zeng, Euidae Jung, Junke Wang, So Min Park, Deying Luo, Cailing Chen, Jie Shen, Yu Han, Carlo Andrea Riccardo Perini, Juan-Pablo Correa-Baena, Zheng-Hong Lu, Thomas P. Russell, Stefaan De Wolf, Mercouri G. Kanatzidis, David S. Ginger, Bin Chen, Yanfa Yan, Edward H. Sargent","doi":"10.1038/s41560-024-01613-8","DOIUrl":"https://doi.org/10.1038/s41560-024-01613-8","url":null,"abstract":"<p>Perovskite tandem solar cells show promising performance, but non-radiative recombination and its progressive worsening with time, especially in the mixed Sn–Pb low-bandgap layer, limit performance and stability. Here we find that mixed Sn–Pb perovskite thin films exhibit a compositional gradient, with an excess of Sn on the surface—and we show this gradient exacerbates oxidation and increases the recombination rate. We find that diamines preferentially chelate Sn atoms, removing them from the film surface and achieving a more balanced Sn:Pb stoichiometry, making the surface of the film resistive to the oxidation of Sn. The process forms an electrically resistive low-dimensional barrier layer, passivating defects and reducing interface recombination. Further improving the homogeneity of the barrier layer using 1,2-diaminopropane results in more uniform distribution and passivation. Tandems achieve a power conversion efficiency of 28.8%. Encapsulated tandems retain 90% of initial efficiency following 1,000 h of operating at the maximum power point under simulated one-sun illumination in air without cooling.</p>","PeriodicalId":19073,"journal":{"name":"Nature Energy","volume":"35 1","pages":""},"PeriodicalIF":56.7,"publicationDate":"2024-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141986477","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}