Alexander Diercks, Julian Petry, Thomas Feeney, Roja Singh, Tonghan Zhao, Hang Hu, Yang Li, Ulrich W. Paetzold, Paul Fassl
{"title":"Sequential Evaporation of Inverted FAPbI3 Perovskite Solar Cells – Impact of Substrate on Crystallization and Film Formation","authors":"Alexander Diercks, Julian Petry, Thomas Feeney, Roja Singh, Tonghan Zhao, Hang Hu, Yang Li, Ulrich W. Paetzold, Paul Fassl","doi":"10.1021/acsenergylett.4c03315","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03315","url":null,"abstract":"Recent advances in sequential evaporation of perovskite solar cells (PSCs) have culminated in a rapid increase in reported power conversion efficiencies (PCEs), now on par with those of the best solution-processed counterparts. This development triggered vast interest from industry and academics. To date, however, very few studies addressed sequentially evaporated PSCs in the <i>p-i-n</i> architecture, and an in-depth process understanding is lacking. Here, we investigate the impact of the hole transport layer (HTL) on the formation of formamidinium lead triiodide (FAPI) perovskite thin films fabricated via an evaporated two-step process. We find that the crystal orientation of lead iodide (PbI<sub>2</sub>) changes significantly for different HTLs, thereby affecting the subsequent conversion and crystallization process. Adjusting the amount of deposited FAI reveals an unexpected correlation of the PbI<sub>2</sub>-to-perovskite X-ray diffraction peak intensity ratio to final PSC performance that depends on the employed HTL. Our approach enables PCEs of more than 17%, the highest reported for fully vacuum-processed pure FAPI PSCs in the <i>p-i-n</i> architecture.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"128 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385669","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}
Noah P. Holzapfel, Veronica Augustyn, Véronique Balland
{"title":"Fundamentals of Proton-Insertion Coupled Electron Transfer (PICET) in Metal Oxides for Aqueous Batteries","authors":"Noah P. Holzapfel, Veronica Augustyn, Véronique Balland","doi":"10.1021/acsenergylett.4c03076","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03076","url":null,"abstract":"The need for sustainable and low-cost energy storage for grid-scale applications motivates research into new types of aqueous rechargeable batteries. Within this context, proton-insertion coupled electron transfer (PICET) into transition metal oxide electrodes presents an attractive charge storage mechanism that utilizes non-metallic charge carriers in high conductivity electrolytes. The purpose of this Review is to present the fundamentals of PICET into transition metal oxides from neutral or acidic electrolytes as it relates to aqueous rechargeable batteries. We elaborate on the electrochemical features of PICET and the choice of transition metal oxide hosts, the electrochemical thermodynamics and kinetics of PICET, and the properties of hydrogenated transition metal oxides. A particular emphasis is placed on the composition and properties of the aqueous electrolyte used for PICET, which influences the kinetics and thermodynamics of the charge storage mechanism. Finally, we conclude with a discussion of the practical considerations and outlook for proton-based aqueous batteries utilizing transition metal oxide electrodes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"29 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375531","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}
Zhiming Zhao, Georgian Melinte, Yongjiu Lei, Dong Guo, Mohamed N. Hedhili, Zixiong Shi, Hussam Qasem, Husam N. Alshareef
{"title":"New Dissolution Chemistry of Nylon Promises Reversible Li-Metal Batteries","authors":"Zhiming Zhao, Georgian Melinte, Yongjiu Lei, Dong Guo, Mohamed N. Hedhili, Zixiong Shi, Hussam Qasem, Husam N. Alshareef","doi":"10.1021/acsenergylett.4c03221","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03221","url":null,"abstract":"Integrating additives into electrolytes serves as an effective strategy for cultivating robust interphases in batteries. Traditionally, the emphasis has been placed on small-molecule additives, whereas macromolecules have been largely overlooked due to their insolubility in conventional solvents. In this study, we establish that the macromolecule polyamide (nylon, <b>PA</b>) can be effectively solubilized in Li<sup>+</sup> electrolytes and utilized as a macromolecular additive. The dissolution capability of the electrolyte is governed by multiple parameters. Specifically, the dissolution of PA is facilitated by stronger Lewis acidity of the cations, weaker solvating capabilities of the solvents, smaller anions, and higher salt concentrations. At the molecular level, coordination of cations with carbonyl groups and the formation of H-bonds between anions and amido groups disrupt the crystalline structure of PA, thereby enhancing its solubility. As a paradigm for practicability, the solubilized PA in carbonate-based electrolytes induces Li<sub>3</sub>N-rich interphases, significantly boosting the rechargeability of Li-metal batteries (LMBs).","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"41 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375532","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":"International Conference on Carbon Capture and Utilization (ICCCU-24): A Platform to Sustainability and Net-Zero Goals","authors":"Sebastian C. Peter","doi":"10.1021/acsenergylett.5c00245","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00245","url":null,"abstract":"The International Conference on Carbon Capture and Utilization (ICCCU-24; https://www.icccu24.com), held from December 9–13, 2024, at the Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR), Bengaluru, emerged as a pivotal platform for addressing CO<sub>2</sub> mitigation and advancing solutions toward sustainability. (1) This conference was organized by the National Centre for Carbon Capture and Utilization (NCCCU) at JNCASR, one of the first Centres of Excellence (CoE) on Carbon Capture and Utilization (CCU) in India with a generous support of Department of Science and Technology (DST). This conference was planned with an intend to expedite shifting to a low-carbon economy by exchanging best practices, emerging technologies, and successful case studies emphasizing pragmatic solutions and interdisciplinary collaboration. This conference aims to unite scientists, engineers, innovators, policymakers, stakeholders in CCU, and leaders in a cooperative effort to address the issues of CO<sub>2</sub> emissions and climate change, promoting practical solutions for a sustainable future. By fostering collaboration among academia, industry, and policymakers, the conference underscored the critical role of CCU in achieving India’s ambitious net-zero emissions target by 2070. The major themes of the conference were Carbon Capture and Carbon Utilization (Figure 1). The ICCCU-24 convenor, Sebastian C Peter (JNCASR), pointed out in the opening session that “<i>CCU is an important research activity as it can help reduce emissions and contribute to global decarbonization efforts. The cross-disciplinary training through the ICCCU-2024 will develop a deep understanding and problem-oriented approach in next-generation researchers working in different dimensions of CCU</i>”. Figure 1. Overall themes of ICCCU-24. The first approach focused on theoretical studies, providing a fundamental background for CCU chemistry. Biswarup Pathak (IIT Indore), Ali Haider (IIT Delhi), and Vidya Avasare (Ashoka University) extensively discussed their computational explorations of CO<sub>2</sub> behavior through various pathways. (2,3) Soujanya Yarasi (CSIR-IICT) highlighted how quantum mechanical (QM) methods integrated with AI/ML techniques can predict the adsorption and interaction behaviors of amine solvents and solid adsorbent materials, enabling the optimization of CO<sub>2</sub> capture processes. (4) Vikram Vishal (IIT Bombay) and Rajnish Kumar (IIT Madras) discussed strategies for mitigating risks in CO<sub>2</sub>-enhanced petroleum recovery and gas hydrates for capture and sequestration, respectively. (5,6) K. V. Agrawal (EPFL) explored membrane-based CO<sub>2</sub> capture, focusing on unit-cell-thick MOF membranes precisely tuned with Å-scale pore sizes. (7) These membranes enable a highly scalable and uniform CO<sub>2</sub> capture process. Raju Kumar Gupta (IIT Kanpur) emphasized the importance of solid sorbents, particularly nanostructured solid adsorbents","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"21 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375533","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}
Yiwen Wu, Linwei Zhao, Jiadong Shen, Tengteng Gu, Yan Yang, Shaomin Ji, Min Zhu, Jun Liu
{"title":"Raising the Redox Potential in a Quinone-Based Positive Organic Cathode via Space Charge Modulation","authors":"Yiwen Wu, Linwei Zhao, Jiadong Shen, Tengteng Gu, Yan Yang, Shaomin Ji, Min Zhu, Jun Liu","doi":"10.1021/acsenergylett.4c03283","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03283","url":null,"abstract":"Recently, π-d conjugated coordination polymers (CCPs) have been emerging in the field of energy storage due to their high conductivity, low solubility, and structural diversity. In this paper, we report a nickel tetrahydroxy-p-benzoquinone complex (Ni-PTHBQ) with a detailed analysis of its structure and components for the first time. The application of Ni-PTHBQ to lithium storage was found to have a high lithium storage potential of 3.12 V. The charging–discharging mechanism of the 2.5 e<sup>–</sup> transfer of Ni-PTHBQ was demonstrated by in situ Raman spectroscopy and other tests. In addition, the reason for the capacity degradation of Ni-PTHBQ was revealed by in situ XRD. This work clarifies the structure and lithium storage mechanism of Ni-PTHBQ, which provides a strong guidance for the synthesis and preparation of CCPs materials as well as their application in energy storage.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"16 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143258615","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":"Lewis Base Strategy for Crystallization Control and Buried Interface Passivation on Hydrophobic PTAA Substrate for Efficient Tin–Lead Perovskite and All-Perovskite Tandem Solar Cells","authors":"Jinling Chen, Jiajun Du, Jingyu Cai, Beilin Ouyang, Ziyi Li, Xiling Wu, Congcong Tian, Anxin Sun, Rongshan Zhuang, Xueyun Wu, Chen Chen, Tiantian Cen, Ran Li, Teng Xue, Yuyang Zhao, Kaibo Zhao, Qianwen Chen, Chun-Chao Chen","doi":"10.1021/acsenergylett.4c03370","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03370","url":null,"abstract":"Nonionic PTAA is an ideal substitute for PEDOT:PSS as a hole-selective layer to improve the stability of mixed tin–lead (Sn–Pb) perovskite solar cells (PSCs). However, its hydrophobic nature aggravates the unbalanced crystallization and poor buried contacts of Sn–Pb perovskite films. Here, we report a Lewis base strategy to tackle these issues by introducing 4-bromophenylurea (BPU) or 4-bromophenylthiourea (BPSU) to interact with precursor ingredients to form large clusters, which accelerate nucleation and delay crystal growth as well as suppress buried interfacial nonradiative recombination. Compared to BPU, the more polar BPSU enables stronger interactions with Sn-halides than Pb-halides, resulting in improved film and interface qualities. Consequently, the Sn–Pb PSCs achieve a power conversion efficiency of 23.87%, the highest reported value for Sn–Pb cells on PTAA. Furthermore, the all-perovskite tandems deliver an efficiency of 27.61% (certified 27.17%) and retain 90% of their initial value after 1200 h of maximum power point tracking in nitrogen.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"55 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143367393","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}
Julian F. Baumgärtner, Dragos C. Stoian, Kenneth P. Marshall, Mohammad Jafarpour, Matthias Klimpel, Huanyu Zhang, Faruk Okur, Wouter van Beek, Dmitry Chernyshov, Sina Abdolhosseinzadeh, Michael Wörle, Maksym V. Kovalenko, Kostiantyn V. Kravchyk
{"title":"Single-Phase Lithiation in Iron Hydroxy Fluorides with Pyrochlore Structure","authors":"Julian F. Baumgärtner, Dragos C. Stoian, Kenneth P. Marshall, Mohammad Jafarpour, Matthias Klimpel, Huanyu Zhang, Faruk Okur, Wouter van Beek, Dmitry Chernyshov, Sina Abdolhosseinzadeh, Michael Wörle, Maksym V. Kovalenko, Kostiantyn V. Kravchyk","doi":"10.1021/acsenergylett.5c00218","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00218","url":null,"abstract":"3D transition metal fluorides have long been recognized as appealing low-cost, high-energy-density cathode materials for Li-ion batteries, but their conversion-type lithiation mechanism induces structural and morphological changes, limiting their cycling stability. Our findings now suggest that metal fluorides may undergo single-phase lithiation when crystallized in a pyrochlore structure, enabled by the presence of Li-ion storage sites within interconnected hexagonal channels. By conducting a detailed analysis of pyrochlore iron(III) hydroxy fluorides during lithiation using <i>operando</i> X-ray absorption spectroscopy, X-ray total scattering, and electron microscopy, we provide evidence for a possible single-phase lithiation mechanism and robust structural stability. These results challenge the traditional view of conversion-type lithiation in metal fluorides and highlight their potential for achieving high cycling stability and eventual commercialization in Li-ion batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"55 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143192705","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}
Aniello Langella, Arianna Massaro, Ana B. Muñoz-García, Michele Pavone
{"title":"Atomistic Insights into Solid-State Phase Transition Mechanisms of P2-Type Layered Mn Oxides for High-Energy Na-Ion Battery Cathodes","authors":"Aniello Langella, Arianna Massaro, Ana B. Muñoz-García, Michele Pavone","doi":"10.1021/acsenergylett.4c03335","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03335","url":null,"abstract":"Mn-based layered oxides hold great promise as high-energy, cost-effective cathodes for sodium-ion batteries (NIBs), but repetitive Na<sup>+</sup> cycling induces harmful phase transitions. Understanding these mechanisms is essential for designing better performing NIB cathodes. Applying density functional theory (DFT) and variable cell-nudged elastic band (VC-NEB) calculations, we provide atomistic insights into phase transformation pathways and energy barriers in P2-Na<sub><i>x</i></sub>MnO<sub>2</sub> material and its Ni-doped variant. We reveal the key P2-to-OP4/O2 and P2-to-P2′ transitions that occur across various sodiation levels, involving substantial rearrangements around the transition metal sites, with tetrahedral transition states accountable for energy barriers. Our analysis of bond length and angle distortions highlights that shear deformations are pivotal in triggering P-to-O gliding at low sodium levels. Based on these insights, our structural distortion metrics offer a straightforward and computationally efficient descriptor to evaluate structural integrity for these layered oxides, enabling the design of NIBs with improved stability and extended lifespan.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"41 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143258619","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}
Wenzao Li, Jeffrey D. Cain, Nicholas Paul William Pieczonka, Zhongyi Liu, Sayed Youssef Sayed, Yue Qi
{"title":"A Hybrid Intercalation and Conversion Mechanism for Reversible Lithium Storage in Layered Silicane (SiH) with Low Molar Volume Change","authors":"Wenzao Li, Jeffrey D. Cain, Nicholas Paul William Pieczonka, Zhongyi Liu, Sayed Youssef Sayed, Yue Qi","doi":"10.1021/acsenergylett.4c03063","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03063","url":null,"abstract":"Conversion-type anode materials generally suffer from significant volume change upon lithiation despite a high energy storage capacity. Here we report a new intercalation and conversion hybrid-type lithiation mechanism that enables a layered silicane (L-SiH) material to balance high capacity with low volume change. Using first-principles simulations of lithiation and delithiation processes, we predict L-SiH only shows a 3.8 cm<sup>3</sup>/mol volume expansion upon lithiation, significantly lower than that of crystalline Si (∼9.2 cm<sup>3</sup>/mol). During lithium intercalation, hydrogen in L-SiH is redox active, and LiH bonds are formed in the interlayer, without destruction of Si planes. The predicted lithiation proceeds via a two-phase coexisting process at an open-circuit voltage (OCV) plateau of ∼0.43 V, which coincides with experimental observation of a 0.4 V plateau upon the lithiation of synthesized L-SiH. This study introduces a promising anode material with a low volume change fulfilled by an intriguing mechanism.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"9 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143258616","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}
Vladimir Sayevich, Whi Dong Kim, Zachary L. Robinson, Oleg V. Kozlov, Clément Livache, Namyoung Ahn, Heeyoung Jung, Victor I. Klimov
{"title":"Inverted CdSe/PbSe Core/Shell Quantum Dots with Electrically Accessible Photocarriers","authors":"Vladimir Sayevich, Whi Dong Kim, Zachary L. Robinson, Oleg V. Kozlov, Clément Livache, Namyoung Ahn, Heeyoung Jung, Victor I. Klimov","doi":"10.1021/acsenergylett.4c03502","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03502","url":null,"abstract":"Heterostructured quantum dots (QDs) based on narrow-bandgap PbSe and wide-bandgap CdSe have been studied for applications in near-infrared light sources, photodetection, and solar energy conversion. A common structural motif is a QD consisting of a PbSe core enclosed in a CdSe shell. However, the CdSe shell complicates extraction of band-edge charge carriers from the QD. Therefore, conventional PbSe/CdSe QDs are not suitable for application in photoelectric devices. Here we report inverted CdSe/PbSe core/shell QDs that overcome this drawback. In these structures, both the electron and hole exhibit a significant degree of shell localization and can therefore be easily extracted from the QD. To create these structures, we employ a thin, atomically controlled wetting layer that homogenizes the CdSe core surface and thus promotes directionally uniform growth of the PbSe shell. The synthesized CdSe/PbSe QD films exhibit good photocarrier transport, making them suitable for application in photoelectric devices.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"52 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124797","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}