ACS Energy Letters 最新文献

{"title":"Resilience to Demixing and Phase Segregation in Perovskite Solar Cells under Light–Dark Cycles and Temperature","authors":"Alessandra Alberti, Salvatore Valastro, Elisa Nonni, Fabio Matteocci, Lucio Cinà, Aldo Di Carlo, Antonino La Magna","doi":"10.1021/acsenergylett.5c00232","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00232","url":null,"abstract":"Light soaking impacts perovskite solar cells, causing cation rotation, octahedral distortion, and weakened hydrogen bonding. Using a unique <i>in-operando</i> setup for ISOS protocols, we monitor structural, optical, and electrical responses under prolonged light exposure, revealing progressive average changes without sample reloading uncertainties. Over 20 h intervals, light-induced lattice deformation causes progressive local demixing, partially reversible in dark, and residual amorphization that hinders electrical recovery. Lattice expansion and bandgap red-shift indicate increasing iodide local enrichment, while a bandgap blue-shift occurs under heating. FA-MA-Cs-perovskites resist to this ionic demixing more than FA-Cs. Sunlight is the primary trigger for that, surpassing the effects of bias or induced heating. Stress tests at 65 °C drive both formulations from demixing to irreversible phase segregation, with FA-Cs devices showing greater structural and electrical resilience than FA-MA-Cs. Since a demixing–remixing interplay governs the device operation, we recommend tracking it using <i>in-operando</i> protocols over 24–48 h of unaccelerated sunlight–dark testing.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"5 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832116","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":"Highly Selective Photoelectrochemical Glycerol Valorization toward Lactic Acid with Low-Valence Bimetallic Overlayer on CuWO4","authors":"Yuankai Li, Jaekyum Kim, Won Tae Hong, Jun Young Kim, Qian Lei, Hyungu Han, Unbeom Baeck, Dong Hyun Kim, Chang Hyuck Choi, Byung-Hyun Kim, Chan-Hwa Chung, Jung Kyu Kim","doi":"10.1021/acsenergylett.5c00551","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00551","url":null,"abstract":"Selective glycerol valorization to lactic acid is a promising approach for upgrading biomass-derived waste into value-added chemicals. Herein, we demonstrate photoelectrochemical lactic acid production via glycerol oxidation using a surface-reconstructed n-type CuWO₄ photoanode (R-CuWO₄). The R-CuWO₄ exhibits a solution selectivity of 95.9%, a yield rate of 159.8 mmol m^–2 h^–1, and a Faraday efficiency of 59.5%. The reconstructed surface overlayer improves catalytic kinetics, reducing the overpotential and increasing the glycerol conversion rate. Additionally, the presence of low-valence copper in the overlayer tailors the reaction pathway, favoring lactic acid formation. Density functional theory calculations reveal that this effect is associated with a change in the glycerol adsorption configuration from terminal to middle hydroxyl groups on the reduced Cu sites in R-CuWO₄. Our findings suggest that surface engineering through electrochemical treatment can control the adsorption behavior and guide product selectivity in photoelectrochemical biomass conversion.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"1 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832118","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 Alloying Interlayers on Lithium Anode Morphology and Microstructure in “Anode-Free” Solid-State Batteries","authors":"Catherine G. Haslam, Till Fuchs, Daniel W. Liao, Juri Becker, Neil P. Dasgupta, Jürgen Janek, Jeff Sakamoto","doi":"10.1021/acsenergylett.5c00149","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00149","url":null,"abstract":"“Lithium–metal-free” manufacturing of solid-state battery cells could simplify cell assembly and increase the energy density. However, the performance of these cells benefits from a more homogeneous anode formation. The use of thin alloying interlayers in “lithium–metal-free” cells can improve cycle life, but their influence on the morphology and microstructure of plated lithium is yet unknown. Gold and silver interlayers allow for lithium plating at higher current density (0.25 mA cm^–2) without short-circuiting compared to cells without interlayers. The lithium homogeneity is substantially improved, as shown by optical microscopy and 3D profiling. In addition, electron backscatter diffraction determined that the grain size and grain boundary orientation can be controlled by changing the lithium layer composition in the case of silver or by introducing inert particles when using gold interlayers. These findings further the understanding of how thin alloying interlayers can substantially alter the cycling performance of lithium in “lithium–metal-free” solid-state batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"7 1","pages":"2285-2291"},"PeriodicalIF":22.0,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832119","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":"Surface-Modified Lithium Enabling High-Performance All-Solid-State Lithium Metal Batteries","authors":"Hui-Tae Sim, Myung-Keun Oh, Hyo-Jin Kim, Ye-Eun Park, Yun-Sun Cho, Jaeyoung Choi, Seong-Jin Park, Dong-Won Kim","doi":"10.1021/acsenergylett.5c00656","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00656","url":null,"abstract":"Sulfide-based all-solid-state lithium metal batteries (ASSLMBs) are promising next-generation batteries due to their high energy density and safety. However, lithium anodes face challenges like dendrite growth and side reactions at the lithium metal-sulfide electrolyte interface. In this study, we eliminated the resistive native layer on lithium metal and formed a protective layer with high ionic conductivity, mechanical strength, and cohesion by reacting lithium metal with a solution containing nitromethane, dimethoxyethene, and lithium nitrate. The lithium symmetric cell with the surface-modified Li exhibited a high critical current density of 2.8 mA cm^–2 and stable cycling over 1000 h at 30 °C. The ASSLMB with surface-modified Li anode, Li₆PS₅Cl electrolyte, and LiNi_0.78Co_0.10Mn_0.12O₂ cathode achieved a high discharge capacity (183.2 mAh g^–1) and stable cycling for 300 cycles without short-circuit at 0.3 C and 30 °C, which enabled solving the critical challenging issues of Li metal for the development of ASSLMBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"118 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827446","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":"Improving the Stability of Colloidal CsPbBr3 Nanocrystals with an Alkylphosphonium Bromide as Surface Ligand Pair","authors":"Meenakshi Pegu, Hossein Roshan, Clara Otero-Martínez, Luca Goldoni, Juliette Zito, Nikolaos Livakas, Pascal Rusch, Francesco De Boni, Francesco Di Stasio, Ivan Infante, Luca De Trizio, Liberato Manna","doi":"10.1021/acsenergylett.5c00124","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00124","url":null,"abstract":"In this study, we synthesized a phosphonium-based ligand, trimethyl(tetradecyl)phosphonium bromide (TTP-Br), and employed it in the postsynthesis surface treatment of Cs-oleate-capped CsPbBr₃ nanocrystals (NCs). The photoluminescence quantum yield (PLQY) of the NCs increased from ∼60% to more than 90% as a consequence of replacing Cs-oleate with TTP-Br ligand pairs. Density functional theory calculations revealed that TTP⁺ ions bind to the NC surface by occupying Cs⁺ surface sites and orienting one of their P–CH₃ bonds perpendicular to the surface, akin to quaternary ammonium passivation. Importantly, TTP-Br-capped NCs exhibited higher stability in air compared to didodecyldimethylammonium bromide-capped CsPbBr₃ NCs (which are considered a benchmark system), retaining ∼90% of their PLQY after 6 weeks of air exposure. Light-emitting diodes fabricated with TTP-Br-capped NCs achieved a maximum external quantum efficiency of 17.2%, demonstrating the potential of phosphonium-based molecules as surface ligands for CsPbBr₃ NCs in optoelectronic applications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"4 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819631","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":"Shall we give up writing scientific papers to AI?","authors":"Filippo De Angelis","doi":"10.1021/acsenergylett.5c00928","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00928","url":null,"abstract":"Artificial Intelligence (AI) tools for language processing are currently being used in many fields where the write up of a summary or a commentary is required. Most internet content is, as a matter of fact, AI-generated ones, sometimes supervised by a human Editor. Scientific writing makes no exception, with AI tools being increasingly adopted for text generation. Should we be alarmed by AI text generation tools or let AI write our papers? Writing a scientific paper is just the last task in a logical scientific workflow, which I tried to represent in Scheme 1. Typically, such a workflow is initiated by curiosity, possibly linked to unanswered questions in a given scientific field that generate the idea of researching and investigating the underlying phenomenon. We typically associate this stage with the creativity of a researcher. This initiating phase is then followed by a likewise creative stage where researchers start planning experiments (or simulations) to address the questions raised by point 1. This stage requires a combination of global field knowledge, technical skills and inventive capabilities. Researchers in the group then execute the experiments (or calculations) planned at stage 2. This is when deep technical skills come into play. The quality (accuracy) of the data produced at stage 3 many times equally contribute to the research success as it is planned in stage 2. Analysis of the results produced at stage 3 and their interpretation according to commonly accepted physical or chemical laws is also a creative stage, including knowledge of the literature of the field. Although apparently less exciting than 1 and 2, this is, in my opinion, what really makes the difference between having an interesting result, possibly of technical relevance, and having a scientific result worth being published to address a broader audience. Last but not least, we have to write the paper according to some commonly accepted structure (e.g., Introduction, Methods, Results and Discussion, and Conclusions), resembling somehow in parallel the structure to the workflow of Scheme 1. Without a well composed write up, the efforts of stages 1–4 go unnoticed. Writing a good scientific paper is usually a cooperative effort involving almost the entire research team, with a different degree of contribution depending on the role, skills, and personal vocation. In my experience as a researcher, I have to admit that sometimes the last stage can be tedious, especially when one needs to start writing from scratch the “Introduction” section. Those first two or three paragraphs, embodying literature references, may represent an obstacle which significantly delays the paper write up, leading to coauthors emailing “about the status of our paper”. AI tools can be of great help in overcoming such an “activation barrier”, (1) although one cannot expect much depth or insight being achieved by a typical chat bot, with a similar output to that achieved by performing an Internet se","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"106 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819632","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":"Molecular-level Regulation of PEO-Based Electrolytes with CaF2 Nanoparticles for Advanced Solid-State Lithium Metal Batteries","authors":"Tao Li, Quan Zheng, Jiantao Li, Zhiyi Zhao, Wenbin Huang, Bin Zhang, Guohao Zhao, Tianli Wu, Dong-Liang Peng, Qingshui Xie, Ying Xu, Khalil Amine","doi":"10.1021/acsenergylett.5c00455","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00455","url":null,"abstract":"The poly(ethylene oxide) (PEO)-based electrolyte has caught much attention for its flexibility, interfacial compatibility, and low cost, but the low ionic conductivity and poor mechanical strength severely hinder its further application in solid-state batteries. Herein, a molecular level regulation through adding CaF₂ nanoparticle fillers is proposed to enhance the electrochemical performance of the PEO-based electrolyte. The strong coordination effects of the Ca cation with a Li salt anion and ether-oxygen increase the dissociated Li ion concentration and accelerate Li ion migration, thus enhancing the ionic conductivity of the electrolyte when combined with their physical disruption in the PEO matrix (0.31 mS cm^–1 at 55 °C). Moreover, the spontaneous reaction between Li and CaF₂ generates a LiF-rich solid electrolyte interphase, which promotes homogeneous Li deposition. Consequently, the PEO-CaF₂ electrolyte delivers symmetric cells over 6300 h and maintains full batteries over 1000 cycles with 80% capacity retention. The assembled pouch-cell displays robust performance, further demonstrating its potential practical application.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"43 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806074","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":"Pathways to Electrochemical Ironmaking at Scale Via the Direct Reduction of Fe2O3","authors":"Anastasiia Konovalova, Andrew C. Goldman, Raj Shekhar, Isaac Triplett, Louka J. Moutarlier, Minkyoung Kwak, Paul A. Kempler","doi":"10.1021/acsenergylett.5c00166","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00166","url":null,"abstract":"Electrochemical ironmaking can provide an energy efficient, zero-emissions alternative to traditional methods of ironmaking, but the scalability of low-temperature electrochemical cells may be constrained by reactor throughput and the availability of acceptable feedstocks. Electrodes directly converting solid iron-oxide particles to metal circumvent traditional mass-transport limitations but are sensitive to both the particle size and nanoscale morphology of reactants. The effect of these properties on reactor throughput has not been systematically studied at model electrowinning surfaces. Here, we have used size-controlled, homologous α-Fe₂O₃ particles to study how the nanoscale morphology of oxides influences the obtainable current density toward Fe metal and integrated these results in a technoeconomic model for alkaline iron electrowinning systems. Micron-scale α-Fe₂O₃ with nanoscale porosity can be used to form Fe at current densities commensurate with industrial water electrolysis (&gt;0.6 A cm^–2) in the absence of external convection, providing a path to cost-competitive and scalable ironmaking using electrochemistry.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"1 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806016","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":"Reversible Li+/H+ Exchange Impairs Si/C/Li7La3Zr2O12 Mixed Anodes","authors":"Yingjie Gao, Yanan Yang, Zhikun Huang, Yu Zhuang, Ye Zeng, Kangning Gao, Zhiqian Hou, Fan Bai, Zhuang Sun, Tao Zhang","doi":"10.1021/acsenergylett.5c00728","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00728","url":null,"abstract":"Silicon is a promising anode material for both liquid- and solid-state batteries due to its high theoretical capacity and low operating voltage. Among solid-state electrolytes, Li₇La₃Zr₂O₁₂ (LLZO) is considered a promising candidate due to its good stability against highly reducible anodes. However, the chemical and electrochemical stabilities of LLZO in silicon-based anodes, particularly in industrially mature aqueous slurries, remains insufficiently explored. In this study, we report that mixing LLZO with silicon in aqueous slurries leads to a reversible Li⁺/H⁺ exchange during the lithiation process. This exchange results in a significant influx of protons into the battery, triggering a hydrogen evolution reaction (HER) at low voltage, which severely degrades the silicon-based electrodes and the performance of batteries. To address this issue, we propose a solution by incorporating sulfolane into the electrolyte, which can effectively confine free H⁺ and mitigate HER. With this modification, the battery retains 22.2% and 10.4% of its capacity at 3C and 5C charge rates, respectively, providing a potential strategy for the application of mixed LLZO in silicon-based anodes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"38 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806018","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":"Thermal Cross-Linking Hole-Transport Self-Assembled Monolayers for Perovskite Solar Cells","authors":"Wanhai Wang, Xiaofeng Li, Liang Gao, Gaoqi Liu, Li Yang, Wei Zhou, Jianfei Hu, Yinhu Gao, Yuliang Che, Zhijun Ning, Jinbao Zhang, Weihua Tang","doi":"10.1021/acsenergylett.5c00457","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00457","url":null,"abstract":"Inverted perovskite solar cells (PSCs) adopting hole-transport self-assembled monolayers (SAMs) face the challenge of inadequate interfacial affinity and inherent instability. A thermal cross-linking SAM design strategy is herein reported to simultaneously improve their surface wettability and thermal stability. The in situ cross-linking networks of molecular-engineered SAMs promote charge transport at the perovskite buried interface. A champion efficiency of 24.17% was achieved for 1.56 eV bandgap PSCs, outperforming non-cross-linked counterparts (22.02%). Over 90% initial efficiency was retained after 1000 h of exposure at 100 °C. Cross-linked SAMs also endow 1.25 eV PSCs with an impressive efficiency of 22.05%. This research offers valuable insights for designing inherently stable SAMs to promote the development of inverted PSCs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"25 1","pages":"2250-2258"},"PeriodicalIF":22.0,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813861","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}