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Breaking the molecular symmetricity of sulfonimide anions for high-performance lithium metal batteries under extreme cycling conditions 打破磺酰亚胺阴离子的分子对称性,实现极端循环条件下的高性能锂金属电池
IF 56.7 1区 材料科学 Q1 ENERGY & FUELS Pub Date : 2024-11-28 DOI: 10.1038/s41560-024-01679-4
Yang Lu, Qingbin Cao, Weili Zhang, Tianyou Zeng, Yu Ou, Shuaishuai Yan, Hao Liu, Xuan Song, Haiyu Zhou, Wenhui Hou, Pan Zhou, Nan Hu, Qingqing Feng, Yong Li, Kai Liu

Lithium metal batteries operating under extreme conditions are limited by the sluggish desolvation process and poor stability of the electrode–electrolyte interphase. However, rational interphase design is hindered by the ill-defined understanding of interphasial chemistry at the molecular level. Here we design and synthesize a series of sulfoximide salts, lithium bis(trifluoromethanesulfinyl)imide (LiBSTFSI) and lithium (trifluoromethanesulfinyl)(trifluoromethanesulfonyl)imide (LiSTFSI), that possess distinctive oxidizability. Their molecular structure and interphasial chemistry were correlated. An anionic electro-polymerization was induced by the asymmetric LiSTFSI to establish a bilayer catholde–electrolyte interphase (CEI) with LiF dominated inner covered by negative-charged inorganic polymers. LiSTFSI-derived CEI enables superior mechanical stability and accelerated Li+ desolvation that contribute to the stable cycling and superior energy and power densities under ultra-high rate and ultra-low temperature conditions. Industrial pouch cells of 474 Wh kg−1 achieved extreme power density of 5,080 W kg−1 at 30 °C and exceptional low-temperature energy and power densities at −20 °C (382 Wh kg−1, 3,590 W kg−1) and −40 °C (321 Wh kg−1, 1,517 W kg−1).

在极端条件下工作的锂金属电池受限于缓慢的去溶过程和电极-电解质间相的低稳定性。然而,合理的间相设计却因对分子水平的间相化学认识不清而受到阻碍。在此,我们设计并合成了一系列具有独特氧化性的亚磺酰亚胺盐--双(三氟甲烷亚磺酰基)亚胺锂(LiBSTFSI)和(三氟甲烷亚磺酰基)(三氟甲烷磺酰基)亚胺锂(LiSTFSI)。对它们的分子结构和相间化学性质进行了相关研究。不对称 LiSTFSI 诱导了阴离子电聚合,从而建立了双层阴电解质间相(CEI),其中以 LiF 为主,负电荷无机聚合物覆盖其内部。源自 LiSTFSI 的 CEI 具有出色的机械稳定性和加速 Li+ 解溶的能力,有助于在超高速和超低温条件下实现稳定的循环以及出色的能量和功率密度。474 Wh kg-1 的工业袋式电池在 30 °C 时的功率密度达到 5,080 W kg-1,在 -20 °C (382 Wh kg-1、3,590 W kg-1)和 -40 °C (321 Wh kg-1、1,517 W kg-1)时的低温能量和功率密度也非常出色。
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引用次数: 0
A hybrid modelling approach to compare chemical separation technologies in terms of energy consumption and carbon dioxide emissions 从能耗和二氧化碳排放角度比较化学分离技术的混合建模方法
IF 56.7 1区 材料科学 Q1 ENERGY & FUELS Pub Date : 2024-11-27 DOI: 10.1038/s41560-024-01668-7
Gergo Ignacz, Aron K. Beke, Viktor Toth, Gyorgy Szekely

Accurate energy system modelling of chemical separations is a critical component of technology selection to minimize operating costs, energy consumption and emissions. Here we report a hybrid modelling approach based on data-driven and mechanistic models to holistically compare chemical separation performance. Our model can be used to select the most suitable technology for a given chemical separation, such as membrane separation, evaporation, extraction or hybrid configurations, by training a machine learning model to predict solute rejection using an open-access membrane dataset. We estimated an average 40% reduction in energy consumption and carbon dioxide emissions for industrially relevant separations using our methodology. We predicted and analysed 7.1 million solute rejections across several industrial sectors. Pharmaceutical purification could realize carbon dioxide emissions reductions of up to 90% by selecting the most efficient technology. We mapped the reduction in carbon dioxide emissions and the reduction in operating costs globally, establishing parameter thresholds to facilitate corporate and governmental decision-making.

准确的化学分离能源系统建模是技术选择的重要组成部分,可最大限度地降低运营成本、能耗和排放。在此,我们报告了一种基于数据驱动和机械模型的混合建模方法,以全面比较化学分离性能。我们的模型可用于为给定的化学分离选择最合适的技术,如膜分离、蒸发、萃取或混合配置,通过训练机器学习模型,使用开放获取的膜数据集预测溶质排斥。我们估计,使用我们的方法,工业相关分离的能耗和二氧化碳排放量平均可减少 40%。我们预测并分析了多个工业部门的 710 万次溶质剔除。通过选择最高效的技术,制药纯化可实现高达 90% 的二氧化碳减排。我们绘制了全球二氧化碳排放量减少和运营成本降低的地图,建立了参数阈值,以方便企业和政府决策。
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引用次数: 0
Topological semimetals with intrinsic chirality as spin-controlling electrocatalysts for the oxygen evolution reaction 具有本征手性的拓扑半金属作为氧进化反应的自旋控制电催化剂
IF 49.7 1区 材料科学 Q1 ENERGY & FUELS Pub Date : 2024-11-25 DOI: 10.1038/s41560-024-01674-9
Xia Wang, Qun Yang, Sukriti Singh, Horst Borrmann, Vicky Hasse, Changjiang Yi, Yongkang Li, Marcus Schmidt, Xiaodong Li, Gerhard H. Fecher, Dong Zhou, Binghai Yan, Claudia Felser
Electrocatalytic water splitting is a promising approach for clean hydrogen production, but the process is hindered by the sluggish kinetics of the anodic oxygen evolution reaction (OER) owing to the spin-dependent electron transfer process. Efforts to control spin through chirality and magnetization have shown potential in enhancing OER performance. Here we harnessed the potential of topological chiral semimetals (RhSi, RhSn and RhBiS) and their spin-polarized Fermi surfaces to promote the spin-dependent electron transfer in the OER, addressing the traditional volcano-plot limitations. We show that OER activities follow the trend RhSi < RhSn < RhBiS, corresponding to the increasing extent of spin–orbit coupling (SOC). The chiral single crystals outperform achiral counterparts (RhTe2, RhTe and RuO2) in alkaline electrolyte, with RhBiS exhibiting a specific activity two orders of magnitude higher than RuO2. Our work reveals the pivotal roles of chirality and SOC in spin-dependent catalysis, facilitating the design of ultra-efficient chiral catalysts. Oxygen evolution is a key reaction in electrolysers and involves a spin-dependent, multi-electron transfer process. Here the authors use topological semimetals with intrinsic chirality as a means to control spin in oxygen evolution catalysts, and explore the role of spin–orbit coupling in determining activity.
电催化水分离是一种很有前景的清洁制氢方法,但由于电子传递过程依赖于自旋,阳极氧进化反应(OER)的动力学缓慢,阻碍了这一过程的进行。通过手性和磁化控制自旋的努力已显示出提高阳极氧演化性能的潜力。在这里,我们利用拓扑手性半金属(RhSi、RhSn 和 RhBiS)及其自旋极化费米面的潜力,在 OER 中促进自旋依赖性电子转移,解决了传统火山图的局限性。我们发现,随着自旋轨道耦合(SOC)程度的增加,OER 活动也呈现出 RhSi < RhSn < RhBiS 的趋势。手性单晶在碱性电解质中的表现优于非手性单晶(RhTe2、RhTe 和 RuO2),其中 RhBiS 的比活度比 RuO2 高两个数量级。我们的研究揭示了手性和 SOC 在自旋依赖催化中的关键作用,有助于设计超高效手性催化剂。
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引用次数: 0
Capacity estimation of home storage systems using field data 利用现场数据估算家庭存储系统的容量
IF 49.7 1区 材料科学 Q1 ENERGY & FUELS Pub Date : 2024-11-20 DOI: 10.1038/s41560-024-01662-z
Although regulation within the European Union requires manufacturers of battery storage systems to provide state-of-health estimates to customers, no standardized methods for such estimates exist. Now, a large open-access dataset from eight years of field measurements of home storage systems is presented, enabling the development of a capacity estimation method.
虽然欧盟的法规要求电池储能系统制造商向客户提供健康状况估算,但目前还没有标准化的估算方法。现在,通过对家用储能系统进行长达八年的实地测量,我们获得了一个大型开放式数据集,从而能够开发出一种容量估算方法。
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引用次数: 0
Scalable fabrication of wide-bandgap perovskites using green solvents for tandem solar cells 利用绿色溶剂为串联太阳能电池规模化制造宽带隙过氧化物
IF 56.7 1区 材料科学 Q1 ENERGY & FUELS Pub Date : 2024-11-15 DOI: 10.1038/s41560-024-01672-x
Chenyang Duan, Han Gao, Ke Xiao, Vishal Yeddu, Bo Wang, Renxing Lin, Hongfei Sun, Pu Wu, Yameen Ahmed, Anh Dinh Bui, Xuntian Zheng, Yurui Wang, Jin Wen, Yinke Wang, Wennan Ou, Chenshuaiyu Liu, Yuhong Zhang, Hieu Nguyen, Haowen Luo, Ludong Li, Ye Liu, Xin Luo, Makhsud I. Saidaminov, Hairen Tan

Commercializing perovskite-based tandems necessitates environmentally friendly solvents for scalable fabrication of efficient wide-bandgap (WBG) (1.65–1.80 eV) perovskites. However, the green solvents developed for formamidinium lead iodide-based ~1.50-eV-bandgap perovskites are unsuitable for WBG perovskites due to the low solubility of caesium and bromide salts, leading to reliance on toxic N,N-dimethylformamide solvent. Here we present a green solvent system comprising dimethyl sulfoxide and acetonitrile to effectively dissolve the named salts, with the addition of ethyl alcohol to prevent precursor degradation and to extend the solution processing window. Using this green solvent mixture, we achieve blade-coated WBG perovskite solar cells with power conversion efficiencies of 19.6% (1.78 eV) and 21.5% (1.68 eV). We then demonstrate 20.25-cm2 all-perovskite tandem solar modules with a power conversion efficiency of 23.8%. Furthermore, we achieved WBG perovskites deposited in ambient air and narrow-bandgap perovskites fabricated using the same green solvents, which promotes the viability of environmentally friendly fabrication.

要实现基于包光体的串联产品的商业化,就必须使用环保溶剂,以实现高效宽带隙(WBG)(1.65-1.80 eV)包光体的规模化制造。然而,由于铯盐和溴盐的溶解度较低,为碘化甲脒铅基 ~1.50 eV 带隙包光体开发的绿色溶剂并不适合 WBG 包光体,从而导致对有毒的 N,N-二甲基甲酰胺溶剂的依赖。在这里,我们提出了一种由二甲亚砜和乙腈组成的绿色溶剂系统,可有效溶解上述盐类,同时添加乙醇以防止前驱体降解并延长溶液处理时间。利用这种绿色混合溶剂,我们实现了叶片涂层 WBG 包晶太阳能电池,其功率转换效率分别为 19.6% (1.78 eV) 和 21.5% (1.68 eV)。然后,我们展示了 20.25 平方厘米的全包晶串联太阳能模块,其功率转换效率为 23.8%。此外,我们还实现了在环境空气中沉积 WBG 包晶石,并使用相同的绿色溶剂制造窄带隙包晶石,从而提高了环保制造的可行性。
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引用次数: 0
Polyanions stabilize anion redox 多阴离子可稳定阴离子氧化还原
IF 49.7 1区 材料科学 Q1 ENERGY & FUELS Pub Date : 2024-11-15 DOI: 10.1038/s41560-024-01664-x
Jagjit Nanda
Traditionally, lithium-ion battery cathodes face a trade-off between the energy density afforded by high-voltage anion reduction−oxidation and long-term stability. Now, incorporating polyanion motifs into a disordered oxide crystal structure is shown to stabilize the oxygen sublattice, improving capacity retention at high energy densities.
传统上,锂离子电池阴极需要在高压阴离子还原-氧化所提供的能量密度与长期稳定性之间进行权衡。现在,在无序氧化物晶体结构中加入多阴离子图案可以稳定氧亚晶格,提高高能量密度下的容量保持率。
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引用次数: 0
Homogeneous coverage of the low-dimensional perovskite passivation layer for formamidinium–caesium perovskite solar modules 用于甲脒铯包晶太阳能模块的低维包晶石钝化层的均匀覆盖率
IF 49.7 1区 材料科学 Q1 ENERGY & FUELS Pub Date : 2024-11-12 DOI: 10.1038/s41560-024-01667-8
Jing Li, Chengkai Jin, Ruixuan Jiang, Jie Su, Ting Tian, Chunyang Yin, Jiashen Meng, Zongkui Kou, Sai Bai, Peter Müller-Buschbaum, Fuzhi Huang, Liqiang Mai, Yi-Bing Cheng, Tongle Bu
The formation of a homogeneous passivation layer based on phase-pure two-dimensional (2D) perovskites is a challenge for perovskite solar cells, especially when upscaling the devices to modules. Here we reveal a chain-length-dependent and halide-related phase separation problem of 2D perovskite growing on top of three-dimensional perovskites. We demonstrate that a homogeneous 2D perovskite passivation layer can be formed upon treatment of the perovskite layer with formamidinium bromide in long-chain ( >10) alkylamine ligand salts. We achieve champion active-area efficiencies of 25.61%, 24.62% and 23.60% for antisolvent-free processed small- (0.14 cm2) and large-size (1.04 cm2) devices and mini-modules (13.44 cm2), respectively. This passivation strategy is compatible with printing technology, enabling champion aperture-area efficiencies of 18.90% and 17.59% for fully slot-die printed large solar modules with areas of 310 cm2 and 802 cm2, respectively, demonstrating the feasibility of the upscaling manufacturing. Achieving uniform coverage of interfacial layers in perovskite solar cells is challenging, especially over large areas. Li et al. present design guidelines to fabricate these layers with uniform morphology, suppressed defects and improved charge transport.
基于相纯的二维(2D)包晶石形成均匀的钝化层是包晶石太阳能电池面临的一项挑战,尤其是在将设备升级为模块时。在这里,我们揭示了生长在三维包晶之上的二维包晶的链长依赖性和卤化物相关相分离问题。我们证明,在长链(>10)烷基胺配体盐中使用溴化甲脒处理包晶层时,可以形成均匀的二维包晶钝化层。在无抗溶剂处理的小型(0.14 平方厘米)和大型(1.04 平方厘米)器件以及微型模块(13.44 平方厘米)中,我们实现的冠军有效面积效率分别为 25.61%、24.62% 和 23.60%。这种钝化策略与印刷技术兼容,使面积分别为 310 平方厘米和 802 平方厘米的全槽模印刷大型太阳能模块的孔径面积效率分别达到 18.90% 和 17.59%,证明了升级制造的可行性。
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引用次数: 0
A wind of change in sustainability 可持续发展的变革之风
IF 49.7 1区 材料科学 Q1 ENERGY & FUELS Pub Date : 2024-11-05 DOI: 10.1038/s41560-024-01666-9
Yi Guo, Xing-Yuan Miao
Fibre-reinforced epoxy-amine resins are common materials for wind turbine blades, yet they are challenging to recycle. Now, researchers formulate an alternative resin using biomass-derived polyester with easier-to-break covalent linkages, demonstrating the industrial manufacturability and recyclability of the resin with a nine-metre blade prototype.
纤维增强环氧胺树脂是风力涡轮机叶片的常用材料,但其回收利用却很困难。现在,研究人员利用从生物质中提取的聚酯配制出一种共价键更容易断裂的替代树脂,并用一个九米长的叶片原型展示了这种树脂的工业可制造性和可回收性。
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引用次数: 0
The role of policy and module manufacturing learning in industrial decarbonization by small modular reactors 政策和模块制造学习在小型模块化反应堆工业脱碳中的作用
IF 49.7 1区 材料科学 Q1 ENERGY & FUELS Pub Date : 2024-11-04 DOI: 10.1038/s41560-024-01665-w
Max Vanatta, William R. Stewart, Michael T. Craig
Small modular reactors (SMRs) offer a unique solution to the challenge of decarbonizing mid- and high-temperature industrial processes. Here we develop deployment pathways for four SMR designs displacing natural gas in industrial heat processes at 925 facilities across the United States under diverse policy and factory or onsite learning conditions. We find that widespread SMR deployment in industry requires gas prices above US$6 per metric million British thermal unit, low capital cost over-runs and/or aggressive carbon taxes. At gas prices of US$6–10 per metric million British thermal unit, 7–55 gigawatt-thermal (GWt) of SMRs could be economically deployed by 2050, reducing annual emissions by up to 59 Mt of CO2-equivalent. Of this deployment, 2–24 GWt rely on module manufacturing learning within a factory. Widespread deployment potential hinges on avoiding substantial cost escalation for early investments. Policy levers such as direct subsidies are not effective at incentivizing sustainable deployment, but aggressive carbon taxes and investment tax credits provide effective support for SMR success. Nuclear small modular reactors could help decarbonize industrial heat processes in the United States, but widespread deployment (of up to a thousand reactors) hinges on factory learning, extended tax credits and avoiding cost escalations.
小型模块化反应堆(SMR)为中高温工业过程的脱碳挑战提供了一种独特的解决方案。在此,我们根据不同的政策和工厂或现场学习条件,为四种 SMR 设计制定了在全美 925 个设施的工业热流程中替代天然气的部署路径。我们发现,在工业中广泛部署 SMR 需要天然气价格高于每百万英热单位 6 美元、低资本成本超支和/或积极的碳税。在天然气价格为每百万英国热量单位 6-10 美元的情况下,到 2050 年可经济地部署 7-55 千兆瓦热量(GWt)的 SMR,每年可减少多达 5900 万二氧化碳当量的排放。其中,2-24 千兆瓦热依靠在工厂内学习模块制造。广泛部署的潜力取决于避免早期投资成本大幅上升。直接补贴等政策杠杆无法有效激励可持续部署,但积极的碳税和投资税收抵免可为 SMR 的成功提供有效支持。
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引用次数: 0
The impact of interfacial quality and nanoscale performance disorder on the stability of alloyed perovskite solar cells 界面质量和纳米级性能紊乱对合金化过氧化物太阳能电池稳定性的影响
IF 49.7 1区 材料科学 Q1 ENERGY & FUELS Pub Date : 2024-10-30 DOI: 10.1038/s41560-024-01660-1
Kyle Frohna, Cullen Chosy, Amran Al-Ashouri, Florian Scheler, Yu-Hsien Chiang, Milos Dubajic, Julia E. Parker, Jessica M. Walker, Lea Zimmermann, Thomas A. Selby, Yang Lu, Bart Roose, Steve Albrecht, Miguel Anaya, Samuel D. Stranks
Microscopy provides a proxy for assessing the operation of perovskite solar cells, yet most works in the literature have focused on bare perovskite thin films, missing charge transport and recombination losses present in full devices. Here we demonstrate a multimodal operando microscopy toolkit to measure and spatially correlate nanoscale charge transport losses, recombination losses and chemical composition. By applying this toolkit to the same scan areas of state-of-the-art, alloyed perovskite cells before and after extended operation, we show that devices with the highest macroscopic performance have the lowest initial performance spatial heterogeneity—a crucial link that is missed in conventional microscopy. We show that engineering stable interfaces is critical to achieving robust devices. Once the interfaces are stabilized, we show that compositional engineering to homogenize charge extraction and to minimize variations in local power conversion efficiency is critical to improve performance and stability. We find that in our device space, perovskites can tolerate spatial disorder in chemistry, but not charge extraction. Conventional microscopy is unable to correlate nanoscale properties of metal halide perovskites with the performance of solar cells. Frohna et al. present a multimodal operando microscopy toolkit as a diagnostic tool to address the issue.
显微镜为评估包晶体太阳能电池的运行情况提供了一种替代方法,但文献中的大多数工作都集中在裸包晶体薄膜上,而忽略了完整设备中存在的电荷传输和重组损耗。在这里,我们展示了一种多模态操作显微镜工具包,用于测量和空间关联纳米级电荷传输损耗、重组损耗和化学成分。通过将该工具包应用于最先进的合金包晶电池在长时间运行前后的相同扫描区域,我们发现具有最高宏观性能的器件具有最低的初始性能空间异质性--这是传统显微镜所忽略的关键环节。我们表明,设计稳定的界面对于实现稳健的器件至关重要。一旦界面稳定下来,我们就会发现,要提高性能和稳定性,关键是要进行成分工程,使电荷提取均匀化,并尽量减少局部功率转换效率的变化。我们发现,在我们的设备空间中,过氧化物晶石可以容忍化学空间紊乱,但不能容忍电荷萃取。
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引用次数: 0
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Nature Energy
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