ACS Energy Letters 最新文献

{"title":"A Practical Efficiency Target for Perovskite/Silicon Tandem Solar Cells","authors":"Thomas G. Allen, Esma Ugur, Erkan Aydin, Anand S. Subbiah, Stefaan De Wolf","doi":"10.1021/acsenergylett.4c02152","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02152","url":null,"abstract":"Monolithic two-terminal (2T) perovskite/silicon tandem solar cells are rapidly progressing toward higher power conversion efficiencies (PCEs), which has led to a prominent role for this technology within the photovoltaics (PV) research community and, increasingly, in industrial PV R&D. Here, we define a practical PCE target of 37.8% for 2T perovskite/silicon tandems based on metrics derived from state-of-the-art silicon and perovskite solar cells and discuss possible pathways toward that goal. It is hoped that this PCE target will serve to guide future research directions, most notably into continued improvements in the radiative efficiency of the mixed-halide perovskite top cell via bulk and surface passivation strategies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"85 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832546","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}

{"title":"Solvation Structure Engineering of Weakly Coordinating Sulfonamide Electrolytes for 4.6 V Lithium Metal Batteries","authors":"Lea Pompizii, Mingliang Liu, Leonie Braks, Timur Ashirov, Tianhong Zhou, Mounir Mensi, Dongmin Park, Jang Wook Choi, Ali Coskun","doi":"10.1021/acsenergylett.4c03030","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03030","url":null,"abstract":"A series of trifluoromethanesulfonamide solvents were synthesized with systematically controlled ring size (4–6) at the <i>N</i>-terminal to tune their steric and electronic properties to realize enhanced contact ion pairs for the formation of an anion-derived solid-electrolyte interface (SEI) and compatibility with the NMC811 cathode. Comparative analyses of electrolytes revealed that the 1.6 M LiFSI 1-azetidine trifluoromethanesulfonamide (AzTFSA) electrolyte presents the ideal combination of steric and electronic effects along with high oxidation stability up to 5 V and a Coulombic efficiency of 99.2% in Cu–Li half-cells at 1 mA cm^–2 and 1 mAh cm^–2. The corresponding full cells using 20 μm of Li foil paired with the NCM811 cathode by a negative and positive capacity ratio (N/P) of 2.5, achieve 80% capacity retention after 150 cycles at 0.5<i>C</i>. Even at a high charge cutoff voltage of 4.6 V, the Li|NCM811 full cell still realizes 92% retention at 0.5<i>C</i> after 100 cycles.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"82 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832572","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}

{"title":"The Effect of Antisolvent Treatment on the Growth of 2D/3D Tin Perovskite Films for Solar Cells","authors":"Ganghong Min, Robert J. E. Westbrook, Meihuizi Jiang, Margherita Taddei, Ang Li, Thomas Webb, Sanjayan Sathasivam, Amanz Azaden, Robert G. Palgrave, David S. Ginger, Thomas J. Macdonald, Saif A. Haque","doi":"10.1021/acsenergylett.4c02745","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02745","url":null,"abstract":"Antisolvent treatment is used in the fabrication of perovskite films to control grain growth during spin coating. We study widely incorporated aromatic hydrocarbons and aprotic ethers, discussing the origin of their performance differences in 2D/3D Sn perovskite (PEA_0.2FA_0.8SnI₃) solar cells. Among the antisolvents that we screen, diisopropyl ether yields the highest power conversion efficiency in solar cells. We use a combination of optical and structural characterization techniques to reveal that this improved performance originates from a higher concentration of 2D phase, distributed evenly throughout the 2D/3D Sn perovskite film, leading to better crystallinity. This redistribution of the 2D phase, as a result of diisopropyl ether antisolvent treatment, has the combined effect of decreasing the Sn⁴⁺ defect density and background hole density, leading to devices with improved open-circuit voltage, short-circuit current, and power conversion efficiency.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"4 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832574","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}

{"title":"Optimized Gas–Liquid Transport via Local Flow Field Management for Efficient Overall Water Splitting","authors":"Yingjie Ji, Shuyun Yao, Shiyu Wang, Jingxian Li, Yuanming Liu, Kang Ji, Zishan Hou, Xiaojun Wang, Weijie Fu, Lanlan Shi, Jiangzhou Xie, Zhiyu Yang, Yi-Ming Yan","doi":"10.1021/acsenergylett.4c02892","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02892","url":null,"abstract":"Electrochemical water splitting is a key technique for sustainable hydrogen production, but its efficiency is often compromised by bubble formation during electrolysis. In this work, we introduce a new electrolyzer design that strategically optimizes gas and liquid flow distributions to facilitate rapid bubble removal, thereby enhancing the electrochemical process. By incorporating a hydrophobic and gas-venting layer, our design significantly shortens the bubble transfer path and reduces the level of accumulation. This advancement results in a voltage reduction of more than 50 mV and a decrease in performance fluctuations exceeding 50% compared with traditional systems. Through detailed optical analyses and finite element simulations, we further elucidate the effects of the gas–liquid transport, enabling high-performance electrolysis with a volumetric current density of 333 mA cm^–3 at 1.8 V. These findings underscore the potential of local flow field management in advancing electrolyzer design and other electrochemical systems.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841542","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}

{"title":"Scalable Electrode Engineering Techniques for Achieving Selective Ethanol Production Using Commercial Copper Catalysts","authors":"Haoran Qiu, Lingchun Zeng, Feng Wang, Ya Liu, Liejin Guo","doi":"10.1021/acsenergylett.4c02916","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02916","url":null,"abstract":"In the field of electrochemical CO₂ reduction (CO₂R), electrode engineering plays a crucial role in modulating the distribution of complex products. Here, based on multiphysics modeling, we demonstrate that CO₂R product selectivity varies spatially along the thickness of the catalyst layer of the gas diffusion electrode (GDE). Our calculations indicate that maintaining a moderately low local CO₂ concentration around catalytic sites enables optimal ethanol Faradaic efficiency on Cu. We further developed an optimized electrode using commercial Cu nanoparticles with a low catalyst loading of 0.1 mg cm^–2. Even under a low CO₂ feed concentration of 30%, we achieved a Faradaic efficiency of approximately 65% for ethanol at an industrial-scale current density of–156 mA cm^–2 and over 80% for C₂₊ products, along with a promising cathodic energy efficiency of more than 37% for ethanol. This study serves as a scalable and instructive guide for tuning the local CO₂ concentration to achieve optimal production of a single high-selectivity C₂₊ product.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"52 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841543","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}

{"title":"Ultrafast UV Curing Enabling A Stable Interphase and Interface for Solid-State Sodium–Metal Batteries","authors":"Fupeng Li, Kun Ren, Minjie Hou, Mingcan Lin, Xiecheng Yang, Yingjie Zhou, Shizhao Xiong, Feng Liang","doi":"10.1021/acsenergylett.4c03043","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03043","url":null,"abstract":"Designing advanced solid-state sodium batteries (SSBs) demands simultaneously overcoming the low ionic conductivity of solid-state electrolytes (SSEs) and the poor interfacial compatibility between electrodes and SSEs. Herein, a composite solid-state electrolyte (CSE) with high ionic conductivity was prepared by using an efficient UV polymerization in 45 s. A stable interphase and interface were achieved simultaneously through solvent structure tuning and <i>in situ</i> curing. By introduction of fluoroethylene carbonate (FEC) to form a competitive solvation structure in CSE-F, the low lowest unoccupied molecular orbital (LUMO) allowed preferential reduction of FEC in the solvation shell. A dense and uniform NaF-rich interphase was constructed to inhibit the growth of the dendrites. Simultaneously, the integrated cathode and electrolyte constructed a tight-contact interface, enabling uniform and efficient ion transport. The Na||CSE-F@Na₃V₂(PO₄)₃ (NVP) cell showed a capacity retention of 91.78% after 2100 cycles. This work provides a solution to simultaneously achieve a rational interphase and an electrode/electrolyte interface design for SSBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"85 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832582","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}

{"title":"The Detail Matters: Unveiling Overlooked Parameters in the Mechanochemical Synthesis of Solid Electrolytes","authors":"Abdulkadir Kızılaslan, Mustafa Çelik, Yuta Fujii, Zheng Huang, Chikako Moriyoshi, Shogo Kawaguchi, Satoshi Hiroi, Koji Ohara, Mariko Ando, Kiyoharu Tadanaga, Saneyuki Ohno, Akira Miura","doi":"10.1021/acsenergylett.4c02156","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02156","url":null,"abstract":"The advent of all-solid-state lithium-ion batteries has advanced energy storage technologies with the development of highly conductive solid electrolytes. Numerous researchers have reported the structural and electrochemical performance of solid electrolytes obtained through different production techniques and with different compositions. (1,2) However, even in relatively robust production techniques using ball-milling with the same composition and stoichiometry, only a minute difference in the synthesis process can significantly affect the crystallization mechanisms and resulting ionic conductivity, thereby highlighting the importance of overlooked parameters. This Viewpoint demonstrates the effects of “premixing”─mixing the precursors with a mortar and pestle prior to the mechanochemical synthesis of glassy solid electrolytes, particularly Li&lt;sub&gt;2&lt;/sub&gt;S–P&lt;sub&gt;2&lt;/sub&gt;S&lt;sub&gt;5&lt;/sub&gt; sulfides and the newly emerging NaTaCl&lt;sub&gt;6&lt;/sub&gt; halides─on the structure and transport of the resulting products. Crystal structures and amorphous configurations of sulfide and chloride electrolytes with high ionic conductivities and excellent mechanical properties have been identified. (3−11) These electrolytes are commonly produced through mechanochemical synthesis using ball-milling, which has been widely utilized with various chemical compounds. (12−14) Li&lt;sub&gt;7&lt;/sub&gt;P&lt;sub&gt;3&lt;/sub&gt;S&lt;sub&gt;11&lt;/sub&gt; is recognized as a metastable phase that is nucleated by the subsequent heat treatment of Li&lt;sub&gt;2&lt;/sub&gt;S–P&lt;sub&gt;2&lt;/sub&gt;S&lt;sub&gt;5&lt;/sub&gt; glasses produced by planetary ball-milling. NaTaCl&lt;sub&gt;6&lt;/sub&gt; is recognized as a mixture of crystal and amorphous phases that shows an excellent electrochemical window. In both cases, a wide range of ball-milling experimental parameters have been investigated, including the amount of powder, number of balls, rotation speed, and ball-milling time, leading to the successful synthesis of the target phases. (15−24) This experimental fact makes these synthesis methods for producing Li&lt;sub&gt;7&lt;/sub&gt;P&lt;sub&gt;3&lt;/sub&gt;S&lt;sub&gt;11&lt;/sub&gt; and NaTaCl&lt;sub&gt;6&lt;/sub&gt; seemingly very robust. Nonetheless, although the apparent crystal structures evaluated by X-ray diffraction (XRD) are almost identical, there are significant differences in their ion conductivities. (18,25−27) Moreover, only three of 15 studies reported on Li&lt;sub&gt;7&lt;/sub&gt;P&lt;sub&gt;3&lt;/sub&gt;S&lt;sub&gt;11&lt;/sub&gt; syntheses (3,28,29) have described the hand-mixing of starting powders prior to or intermittently during ball-milling, as given in Table S1. Similarly, one out of three studies of NaTaCl&lt;sub&gt;6&lt;/sub&gt; have described the hand-mixing of starting powders (Table S2). Although the details of the hand-mixing have been deemed to have negligible effects, this study demonstrates the importance of such a process. This Viewpoint demonstrates the impact of the unspecified details of mechanochemical synthesis on the crystallization mechanisms and ionic conductivities of the products, highlighting the importance of parameter","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"46 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832578","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}

{"title":"Stable Hard X-ray Detectors by High-Charge-Mobility Two-Dimensional Cu(Gly)2Pb2Br4 Single Crystal","authors":"Jinghui Han, Weijun Li, Jinmei Song, Mingbian Li, Yuhong He, Wei Wei, Bai Yang, Haotong Wei","doi":"10.1021/acsenergylett.4c02866","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02866","url":null,"abstract":"Two-dimensional (2D) perovskites have better long-term stability, better ion migration inhibition ability, and lower dark current in X-ray detection due to the hindrance effect of organic cations. However, this also limits the charge carrier transport and lowers the device sensitivity. Here, we report a new trans-copper glycinate lead bromide (Cu(Gly)₂Pb₂Br₄) perovskite-like single crystal. Through the cross-linking strategy of metal ions, the charge carrier transport ability of Cu(Gly)₂Pb₂Br₄ along the out-of-plane direction was greatly improved. The record high hole mobility of 54.1 cm² V^–1 s^–1 enables a high sensitivity of 26 589 μC Gy_air^–1 cm^–2. The cross-linking structure of the organic interlayer also inhibits ion migration paths and enhances stability with a small dark current drift as low as 4.93 × 10^–18 A cm^–1 V^–1 s^–1. The Cu(Gly)₂Pb₂Br₄ single crystal also shows good stability and X-ray imaging capability as a potential candidate for X-ray detection.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"19 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832580","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}

{"title":"Sulfur Vacancies Limit the Open-Circuit Voltage of Sb2S3 Solar Cells","authors":"Xinwei Wang, Seán R. Kavanagh, Aron Walsh","doi":"10.1021/acsenergylett.4c02722","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02722","url":null,"abstract":"Antimony sulfide (Sb₂S₃) is a promising candidate as an absorber layer for single-junction solar cells and the top subcell in tandem solar cells. However, the power conversion efficiency of Sb₂S₃-based solar cells has remained stagnant over the past decade, largely due to trap-assisted nonradiative recombination. Here we assess the trap-limited conversion efficiency of Sb₂S₃ by investigating nonradiative carrier capture rates for intrinsic point defects using first-principles calculations and Sah–Shockley statistics. Our results show that sulfur vacancies act as effective recombination centers, limiting the maximum light-to-electricity efficiency of Sb₂S₃ to 16%. The equilibrium concentrations of sulfur vacancies remain relatively high, regardless of growth conditions, indicating the intrinsic limitations imposed by these vacancies on the performance of Sb₂S₃.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"14 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832577","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}

{"title":"Thiocyanate Coordination Regulates the Interlayer Ammonium Ion Storage Structure of Molybdenum Disulfide","authors":"Hang Li, Ruohan Yu, Haibo Chen, Jing Hu, Jianli Zhang, Guangya Hou, Qiang Chen, Jun Lu, Yiping Tang","doi":"10.1021/acsenergylett.4c02712","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02712","url":null,"abstract":"Aqueous ammonium ion storage utilizes the intercalation and coordination diffusion mechanisms of NH₄⁺ within the host material, resulting in a low-cost, high-safety energy storage device. However, the capacity of the NH₄⁺ storage hosts, represented by layered materials, is mainly limited by the limited interlayer size and coordination sites. Here, a strategy is proposed to enhance NH₄⁺ storage by utilizing nonmetallic ions with long-chain structures to regulate the interlayer spacing and coordination activity of MoS₂. Atomic-level electron microscopy, chemical reactions, and theoretical simulations revealed that SCN^– was successfully intercalated into MoS₂ and coordinated with S atoms to construct an interlayer network. The intercalation of SCN^– provides sufficient space and abundant hydrogen-bonding sites. This work effectively solves the dilemma of traditional layered materials in NH₄⁺ storage and demonstrates the broad prospects of interlayer coordination engineering strategies for energy storage devices.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"18 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832575","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}