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Molecular Recombination Junction for Vacuum-Deposited Perovskite/Silicon Two-Terminal Tandem Solar Cells
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-03-17 DOI: 10.1021/acsenergylett.5c00155
Sofía Chozas-Barrientos, Abhyuday Paliwal, Federico Ventosinos, Cristina Roldán-Carmona, Lidón Gil-Escrig, Vladimir Held, Perrine Carroy, Delfina Muñoz, Henk J. Bolink
{"title":"Molecular Recombination Junction for Vacuum-Deposited Perovskite/Silicon Two-Terminal Tandem Solar Cells","authors":"Sofía Chozas-Barrientos, Abhyuday Paliwal, Federico Ventosinos, Cristina Roldán-Carmona, Lidón Gil-Escrig, Vladimir Held, Perrine Carroy, Delfina Muñoz, Henk J. Bolink","doi":"10.1021/acsenergylett.5c00155","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00155","url":null,"abstract":"The use of commercial, Czochralski-grown silicon wafers as bottom cells in two-terminal perovskite/silicon tandem configurations often leads to defects in the top perovskite absorber due to their rough surfaces, featuring μm-sized pyramids and saw damages. Most recombination junctions in two-terminal tandem cells employ high conductive indium tin oxide which increases the effect of local shunts in the top cell by connecting them. We use Suns–<i>V</i><sub>OC</sub> with selective illumination and external quantum efficiency measurements to identify these shunts. Additionally, we show that a molecular recombination junction composed of an n-doped C<sub>60</sub> layer and a p-doped conjugated arylamine layer alleviates the effect of the shunts in the top cell, which we attribute to the lower lateral conductivity of the organic layers. This enables us to prepare two-terminal tandem devices using fully evaporated top cells on Czochralski textured silicon heterojunction cells with <i>V</i><sub>OC</sub>s of up to 1.84 V and efficiencies above 22%.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"24 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143635389","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}
引用次数: 0
Recrystallization-Driven Quasi-Spherical Prussian Blue Analogs with High Tap Density and Crystallinity for Sodium-Ion Batteries
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-03-17 DOI: 10.1021/acsenergylett.5c00080
Siwei Fan, Yun Gao, Yang Liu, Li Li, Lingling Zhang, Zhiming Zhou, Shu-Lei Chou, Xueting Liu, Yue Shen, Yunhui Huang, Yun Qiao
{"title":"Recrystallization-Driven Quasi-Spherical Prussian Blue Analogs with High Tap Density and Crystallinity for Sodium-Ion Batteries","authors":"Siwei Fan, Yun Gao, Yang Liu, Li Li, Lingling Zhang, Zhiming Zhou, Shu-Lei Chou, Xueting Liu, Yue Shen, Yunhui Huang, Yun Qiao","doi":"10.1021/acsenergylett.5c00080","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00080","url":null,"abstract":"Prussian blue analogs (PBAs) are widely applicable as cathode materials due to their straightforward synthesis procedures, low cost, and considerable theoretical capacity. However, structural defects and low tap density pose substantial challenges to their commercial application. Herein, we propose a recrystallization-driven strategy to synthesize monoclinic binary hexacyanoferrate (CFHCF) with high crystallinity and a remarkably high tap density of 0.992 g cm<sup>–3</sup>. Moreover, the detailed process of quasi-spherical morphology evolution and defect repair is systematically investigated during recrystallization. Furthermore, various in situ and ex situ techniques are employed to reveal the origin of the high specific capacity and the structural evolution mechanism. Additionally, the designed CFHCF//HC pouch cell demonstrates satisfactory capacity retention over 250 cycles and successfully powers a toy platform for flag raising and lowering. Notably, this recrystallization-driven strategy offers valuable insights into the synthesis and commercial applications of highly crystallized PBAs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"183 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143635407","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}
引用次数: 0
Correction to “Toward High-Capacity Li–S Solid-State Batteries: The Role of Partial Ionic Transport in the Catholyte”
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-03-16 DOI: 10.1021/acsenergylett.5c00580
Henry M. Woolley, Martin Lange, Elina Nazmutdinova, Nella M. Vargas-Barbosa
{"title":"Correction to “Toward High-Capacity Li–S Solid-State Batteries: The Role of Partial Ionic Transport in the Catholyte”","authors":"Henry M. Woolley, Martin Lange, Elina Nazmutdinova, Nella M. Vargas-Barbosa","doi":"10.1021/acsenergylett.5c00580","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00580","url":null,"abstract":"After the final version of the manuscript was published, we (the authors) realized that Figure 4F–I did not render properly and the shaded regions corresponding the standard deviations (noted in the caption) were not visible. The new figure is below and the original caption remains unchanged. This article has not yet been cited by other publications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"22 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143635415","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}
引用次数: 0
All-Climate and Nonflammable Electrolyte with a Strong Anion–Solvent Interaction for High-Performance Lithium Metal Batteries
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-03-16 DOI: 10.1021/acsenergylett.4c03307
Chi Ma, Chuankai Fu, Sheng Chang, Xing Xu, Guangxiang Zhang, Ziwei Liu, Hua Huo, Lishuang Fan, Geping Yin, Yulin Ma
{"title":"All-Climate and Nonflammable Electrolyte with a Strong Anion–Solvent Interaction for High-Performance Lithium Metal Batteries","authors":"Chi Ma, Chuankai Fu, Sheng Chang, Xing Xu, Guangxiang Zhang, Ziwei Liu, Hua Huo, Lishuang Fan, Geping Yin, Yulin Ma","doi":"10.1021/acsenergylett.4c03307","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03307","url":null,"abstract":"Reinforced security and temperature tolerance are key prerequisites for the practical application of lithium metal batteries (LMBs). Achieving an optimal balance between maintaining a stable interface at a high temperature and ensuring rapid ion transport under a low temperature remains a critical challenge. Herein, an all-climate nonflammable electrolyte comprised of triethyl phosphate (TEP), lithium bis((trifluoromethyl)sulfonyl) azide (LiTFSI), and lithium nitrate (LiNO<sub>3</sub>) is proposed. The strong interaction between NO<sub>3</sub><sup>–</sup> and TEP broadens the melting point of the electrolyte to −91.5 °C. A well-regulated lithium-ion solvation structure with low desolvation energy contributes to the formation of a durable inorganic–organic hybrid solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI), thereby enhancing the interfacial compatibility significantly. Consequently, the LMBs with the optimized TEP-based electrolyte demonstrate remarkable electrochemical performance in a wide temperature range of −60∼100 °C. The valuable insights gained from this work can offer theoretical guidance for developing wide-temperature electrolytes and high-performance LMBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"17 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143635410","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}
引用次数: 0
Correlation, Causation and Comparison
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-03-14 DOI: 10.1021/acsenergylett.5c00631
Prashant V. Kamat
{"title":"Correlation, Causation and Comparison","authors":"Prashant V. Kamat","doi":"10.1021/acsenergylett.5c00631","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00631","url":null,"abstract":"Figure 1. Rate constants (solid points) and theoretical fits (solid line) based on Marcus electron transfer expression. From ref (4). Copyright 2020 American Chemical Society. Figure 2. Examples of graphs showing causality between two variables. (A) Normalized incident photoconversion efficiency (IPCE) of 3D and 2D/3D perovskite solar cells in response to excitation wavelength. (B) The dependence of observed pseudo-first-order rate constant of biphenyl triplet decay (<i>k</i><sub>obs</sub>) on the concentration of rubrene. From refs (5) and (6). Copyright 2022 and 2024 American Chemical Society. Figure 3. Examples of sample property comparison using (A) trend line and (B) column graph. Since there is neither correlation or causality between the two variables, the data is better presented using a column chart. From ref (8). Copyright 2024 American Chemical Society. I would like to thank Prof. Gregory H. Hartland for helpful discussions. This article references 8 other publications. This article has not yet been cited by other publications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"18 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143619061","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}
引用次数: 0
Time-Resolved Fourier Transform Infrared Spectroelectrochemical Investigation of Nitrate Reduction to Ammonia
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-03-14 DOI: 10.1021/acsenergylett.5c00553
David Kumar Yesudoss, Bright Ngozichukwu, Ibrahima Gning, Balla D. Ngom, Abdoulaye Djire
{"title":"Time-Resolved Fourier Transform Infrared Spectroelectrochemical Investigation of Nitrate Reduction to Ammonia","authors":"David Kumar Yesudoss, Bright Ngozichukwu, Ibrahima Gning, Balla D. Ngom, Abdoulaye Djire","doi":"10.1021/acsenergylett.5c00553","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00553","url":null,"abstract":"This study explores the electrocatalytic nitrate reduction reaction (NO<sub>3</sub><sup>–</sup>RR) using nitride-based two-dimensional Ti<sub>2</sub>NT<i><sub><i>x</i></sub></i> MXene (also known as MNene) synthesized via O<sub>2</sub>-assisted molten salt fluoride etching and its parent Ti<sub>2</sub>AlN MAX phase. Ti<sub>2</sub>NT<i><sub><i>x</i></sub></i> MNene achieved an ammonia (NH<sub>3</sub>) yield rate of ∼550 μmol h<sup>–1</sup> g<sup>–1</sup> with a Faradaic efficiency (FE) of ∼80%. Unexpectedly, the Ti<sub>2</sub>AlN MAX phase exhibited an even higher NH<sub>3</sub> yield rate of ∼800 μmol h<sup>–1</sup> g<sup>–1</sup> at a comparable FE, despite its lower surface area and being traditionally considered a poor electrocatalyst. The enhanced performance of the MAX phase is likely due to −OH functionalization under alkaline conditions, leading to enhanced reaction kinetics. Postelectrolysis analyses, including Raman spectroscopy, X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS), confirmed no significant changes in crystallinity but indicated surface chemical changes. Control experiments with blank electrolytes and isotopically labelled <sup>15</sup>NO<sub>3</sub><sup>–</sup> substantiate that NH<sub>3</sub> originates exclusively from nitrate reduction on the surface terminations. Time-resolved <i>in situ</i> spectroelectrochemical studies identified nitrite (NO<sub>2</sub><sup>–</sup>) reduction to further intermediates as the rate-determining step. These findings not only challenge the conventional perception of MAX phases as poor electrocatalysts but also underscore the potential of nitride-based MAX and MXene materials as robust and efficient electrocatalysts for the NO<sub>3</sub><sup>–</sup>RR.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143619054","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}
引用次数: 0
Unlocking the Capacity and Stability Limitations of Perovskite Electrodes and Achieving the Design of a Flame-Retardant Supercapacitor Through the “Tree Canopy” Structure
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-03-14 DOI: 10.1021/acsenergylett.5c00154
Jiahao He, Yang Zhou, Shibo Wu, Jingrui Cao, Bin Han, Zhiqiang Wang, Zaizai Tong, Muslum Demir, Pianpian Ma
{"title":"Unlocking the Capacity and Stability Limitations of Perovskite Electrodes and Achieving the Design of a Flame-Retardant Supercapacitor Through the “Tree Canopy” Structure","authors":"Jiahao He, Yang Zhou, Shibo Wu, Jingrui Cao, Bin Han, Zhiqiang Wang, Zaizai Tong, Muslum Demir, Pianpian Ma","doi":"10.1021/acsenergylett.5c00154","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00154","url":null,"abstract":"The present study depicts innovative electrode and electrolyte designs to achieve advanced supercapacitor performance and stability. The mechanism of how the electronic structure of substitution ions impacts the phase structure and properties of SrCoO<sub>3−δ</sub> was in-depth elucidated, overcoming the inherent trade-off between specific capacity and cycle stability in perovskite materials. The as-prepared SrCo<sub>0.925</sub>Sc<sub>0.075</sub>O<sub>3−δ</sub> electrode achieves a high capacity of 467.7 C g<sup>–1</sup> (129.92 mAh g<sup>–1</sup>) at 1 A g<sup>–1</sup>, with retention of 97.4% of its initial capacity after 10,000 cycles. Inspired by canopy structures, a “branch”-like dual-network 3D gel system was created and in situ integrated with the electrode as the “trunk”. This unique structure offers robust mechanical strength and flame retardancy, establishing an efficient conductive network. Devices featuring this design show electrochemical stability and flexibility, ensuring safe operation at extreme temperatures while balancing the stability and energy density. This research opens avenues for high-performance supercapacitors and quasi-solid-state gel batteries tailored applications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"7 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143619053","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}
引用次数: 0
Correlation, Causation and Comparison
IF 19.3 1区 材料科学
ACS Energy Letters Pub Date : 2025-03-14 DOI: 10.1021/acsenergylett.5c0063110.1021/acsenergylett.5c00631
Prashant V. Kamat*, 
{"title":"Correlation, Causation and Comparison","authors":"Prashant V. Kamat*,&nbsp;","doi":"10.1021/acsenergylett.5c0063110.1021/acsenergylett.5c00631","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00631https://doi.org/10.1021/acsenergylett.5c00631","url":null,"abstract":"","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 3","pages":"1540–1541 1540–1541"},"PeriodicalIF":19.3,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143609087","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}
引用次数: 0
Graded Cathode Design for Enhanced Performance of Sulfide-Based Solid-State Batteries
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-03-13 DOI: 10.1021/acsenergylett.4c03243
Eva Schlautmann, Janina Drews, Lukas Ketter, Martin A. Lange, Timo Danner, Arnulf Latz, Wolfgang G. Zeier
{"title":"Graded Cathode Design for Enhanced Performance of Sulfide-Based Solid-State Batteries","authors":"Eva Schlautmann, Janina Drews, Lukas Ketter, Martin A. Lange, Timo Danner, Arnulf Latz, Wolfgang G. Zeier","doi":"10.1021/acsenergylett.4c03243","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03243","url":null,"abstract":"Solid-state batteries present a promising technology to overcome the energy density limitations of lithium-ion batteries. However, achieving a high areal loading in cathodes without introducing significant transport limitations remains a key challenge, particularly in thick electrodes. In this work, we study the impact of a three-layer graded cathode design on the performance of a LiNi<sub>0.83</sub>Co<sub>0.11</sub>Mn<sub>0.06</sub>O<sub>2</sub> (NCM83)/Li<sub>6</sub>PS<sub>5</sub>Cl (LPSCl) composite cathode using a combination of experiments and microstructure-resolved simulations. An increased LPSCl content at the separator and higher NCM83 content toward the current collector improve effective charge transport, resulting in better rate performance and reduced overpotentials at high current densities. This comprehensive experimental and theoretical study demonstrates that the optimization of cathode design has the potential to significantly enhance the performance of solid-state batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"23 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143619055","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}
引用次数: 0
Fluorine-Free Electrolytes for Lithium Metal Batteries: Challenges and Opportunities in Solvation Structure and Interphase Design
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-03-13 DOI: 10.1021/acsenergylett.5c00319
Sapna L. Ramesh, Jeffrey Lopez
{"title":"Fluorine-Free Electrolytes for Lithium Metal Batteries: Challenges and Opportunities in Solvation Structure and Interphase Design","authors":"Sapna L. Ramesh, Jeffrey Lopez","doi":"10.1021/acsenergylett.5c00319","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00319","url":null,"abstract":"Electrolyte design has emerged as a key strategy to overcome performance and safety challenges in lithium metal batteries. In this Perspective, we examine the recent movement toward fluorinated electrolyte solvents for high performance lithium metal batteries. We highlight the state-of-the-art understanding of the role of fluorine in modifying solvent properties and influencing electrolyte reactivity and further discuss the role of fluorinated species in the interphases at both the anode and cathode. In light of risks associated with per- and polyfluoroalkyl substances (PFAS), we propose that a deeper understanding of the role of fluorine in electrolytes and interphases is essential to eventually design fluorine-free molecules for high performance batteries and discuss areas for further research.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"89 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143619057","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}
引用次数: 0
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