ACS Energy Letters Pub Date : 2025-04-09DOI: 10.1021/acsenergylett.5c0016610.1021/acsenergylett.5c00166
Anastasiia Konovalova, Andrew C. Goldman, Raj Shekhar, Isaac Triplett, Louka J. Moutarlier, Minkyoung Kwak and Paul A. Kempler*,
{"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 and Paul A. Kempler*, ","doi":"10.1021/acsenergylett.5c0016610.1021/acsenergylett.5c00166","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00166https://doi.org/10.1021/acsenergylett.5c00166","url":null,"abstract":"<p >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-Fe<sub>2</sub>O<sub>3</sub> 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-Fe<sub>2</sub>O<sub>3</sub> with nanoscale porosity can be used to form Fe at current densities commensurate with industrial water electrolysis (>0.6 A cm<sup>–2</sup>) in the absence of external convection, providing a path to cost-competitive and scalable ironmaking using electrochemistry.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 4","pages":"1851–1857 1851–1857"},"PeriodicalIF":19.3,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143818914","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}
Daniela De Luca, Jia Sheng Lee, Herlina Arianita Dewi, Thambidurai Mariyappan, Riyas Ahmad, Shyam Sundar Balaji, Subodh G. Mhaisalkar, Annalisa Bruno
{"title":"Buffer-Layer-Free Semitransparent Perovskite Solar Cells with Soft Sputtered Electrodes Optimized via Design of Experiments","authors":"Daniela De Luca, Jia Sheng Lee, Herlina Arianita Dewi, Thambidurai Mariyappan, Riyas Ahmad, Shyam Sundar Balaji, Subodh G. Mhaisalkar, Annalisa Bruno","doi":"10.1021/acsenergylett.5c00903","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00903","url":null,"abstract":"Semitransparent p-i-n perovskite solar cells (ST-PSCs) hold great potential for multijunction and building-integrated photovoltaics. However, depositing transparent top electrodes, such as indium tin oxide (ITO), using magnetron sputtering often requires buffer layers to prevent sputter-induced damage. This study presents a Design of Experiment approach to implement a fast ITO deposition optimization, enabling the fabrication of buffer-layer-free ST-PSCs with losses in power conversion efficiency (PCE) of less than 0.5% compared to the PSCs using metal electrodes. The developed process is transferable to different ST-PSCs incorporating perovskite of various compositions and fabrication techniques, demonstrating scalability and industrial viability for next-generation ST-PSC technologies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"14 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806017","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-Reconstructed High-Nickel Cathodes for Ultrastable 4.5 V Tolerant Sulfide-Based All-Solid-State Batteries","authors":"Yuanyuan Li, Jianwei Li, Zhen Zeng, Yulong Zhu, Ying Deng, Jun Cheng, Jing Li, Hongqiang Zhang, Jingyu Lu, Lijie Ci, Deping Li","doi":"10.1021/acsenergylett.5c00071","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00071","url":null,"abstract":"Sulfide solid-state electrolytes combined with high-nickel cathodes present a compelling option due to their high safety and high energy density at high voltages. However, the practical implementation remains challenging, particularly concerning the cathode structural degradation and the unfavorable interfacial reaction between the cathode and the sulfide solid electrolyte. To tackle these issues, we propose a surface reconstruction approach to convert the residual lithium compounds on the surface of LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811) particles into a uniform Li<sub>3</sub>VO<sub>4</sub> coating (LVO-NCM). Benefiting from the suppressed interfacial side reactions and enhanced structural stability at high cutoff voltages, all-solid-state batteries (ASSBs) with LVO-NCM demonstrate an impressive cyclic stability at 4.5 V. The capacity retention after 2000 cycles is 80.0%, and even after a cycle duration of 270 days, the capacity retention remains as high as 86.24%. This work provides a promising strategy to stabilize the high-nickel cathode–sulfide electrolyte interface, boosting the development of high-energy-density all-solid-state batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"24 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798258","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":"Lead-Free Cs3Bi2I9 Perovskite Memristors for Energy-Efficient Neuromorphic Computing","authors":"Sujaya Kumar Vishwanath, Chaya Karkera, Tauheed Mohammad, Pritish Sharma, Rantej Naik Badavathu, Upanya Khandelwal, Anil Kanwat, Poulomi Chakrabarty, Devamrutha Suresh, Shubham Sahay, Aditya Sadhanala","doi":"10.1021/acsenergylett.5c00411","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00411","url":null,"abstract":"In-memory computing offers a transformative alternative to traditional von Neumann architecture, with memristors enabling accelerated, low-power computation. Halide perovskites, known for ion migration with low activation energy and synapse-like switching behavior, hold great potential but face challenges in conductance linearity and predictability. Here, we report flexible lead-free Cs<sub>3</sub>Bi<sub>2</sub>I<sub>9</sub> 8 × 8 crossbar memristors exhibiting bipolar resistive switching with a high on/off ratio (10<sup>6</sup>), endurance (10<sup>4</sup> cycles), long retention (10<sup>5</sup> s), and a device yield exceeding 93%. Electrical pulse engineering reveals synaptic behaviors such as paired-pulse facilitation, potentiation, and depression with excellent linearity and minimal variability. In situ training of artificial neural networks, including MLP and VGG-8, achieves 88.19% accuracy on reduced MNIST and 91.38% on CIFAR-10 data sets. This work demonstrates energy-efficient, high-performance neuromorphic hardware, paving the way for advanced parallel computing to address the growing demands of AI and data science.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"28 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143789712","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":"Cation-Disordered Structure in Li3VO4 Anodes Achieved via Simple Spray-Drying for Unprecedented Rate Capability","authors":"Keisuke Matsumura, Yuka Hikichi, Daisuke Saito, Etsuro Iwama, Wako Naoi, Patrick Rozier, Patrice Simon, Katsuhiko Naoi","doi":"10.1021/acsenergylett.5c00540","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00540","url":null,"abstract":"Cation-disordered materials offer attractive potential for high-power energy storage by unlocking diversified ionic transport pathways, yet their practical realization remains challenging due to difficulties in stabilizing disorder. Here, we demonstrate spray-drying as a direct and scalable route to synthesize cation-disordered Li<sub>3</sub>VO<sub>4</sub> without requiring postannealing or additional lithiation steps. By leveraging ultrafast solvent removal, this method induces flash crystallization in less than 1 s, kinetically “freezing” the metastable disordered phase. Structural analysis using synchrotron X-ray diffraction, Pair-Distribution Function analysis, and high-resolution Transmission Electron Microscopy reveals that ultrafast drying disrupts long-range cation ordering while preserving short-range periodicity, forming local cation-ordered domains within an average disordered structure. This nanoscale disorder, stabilized by antiphase domain boundaries, enhances lithium-ion diffusivity, delivering a high-power performance of 138 mAh g<sup>–1</sup> at a 60C rate. By enabling precise control of cation disorder through drying kinetics, this study establishes spray-drying as a powerful and scalable platform for next-generation energy storage materials.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"23 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143784761","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}
Nan Li, Yan Wei, Shujie Liu, Zhaoshi Yu, Yan Shen, Mingkui Wang
{"title":"Boosting Oxygen Evolution Reaction Performance on BiVO4 Photoanode via Gradient Oxygen Vacancies","authors":"Nan Li, Yan Wei, Shujie Liu, Zhaoshi Yu, Yan Shen, Mingkui Wang","doi":"10.1021/acsenergylett.5c00507","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00507","url":null,"abstract":"BiVO<sub>4</sub> is extensively studied in photoelectrochemical water splitting systems. Its relatively large bandgap and low charge carrier mobility severely limit the solar-driven oxygen evolution reaction on BiVO<sub>4</sub>. A gradient distribution of oxygen vacancies can modulate the structural and electrical properties of BiVO<sub>4</sub>. However, the formation of oxygen vacancies remains a daunting challenge. Here, we propose a simple hydrothermal post-treatment method to deposit a thin amorphous BiO<sub><i>x</i></sub> layer (∼8 nm) with gradient oxygen vacancies on the surface of BiVO<sub>4</sub> and enable directional hole migration. The resultant BiVO<sub>4</sub>/BiO<sub><i>x</i></sub>/NiFeO<sub><i>x</i></sub> photoanode achieves a high photocurrent density of 6.34 mA cm<sup>–2</sup> at 1.23 V (vs RHE) in 1.0 M potassium borate solution. A solar-to-hydrogen conversion efficiency of 0.89% is obtained in a device using a BiVO<sub>4</sub>/BiO<sub><i>x</i></sub>/NiFeO<sub><i>x</i></sub> photoanode and a CuBi<sub>2</sub>O<sub>4</sub> photocathode at zero bias. This work highlights a novel strategy for modulating the oxygen vacancy gradient and provides insights into the design of unbiased solar water splitting systems.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"62 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776187","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}
Jie Zhao, Rui Jiang, Maoyuan Huang, Yifei Qiao, Sinong Wang, Wanlu Zhang, Pengfei Tian, Jun Wang, Ruiqian Guo, Shiliang Mei
{"title":"Advancing Ecofriendly Indium Phosphide Quantum Dots: Comprehensive Strategies toward Color-Pure Luminescence for Wide Color Gamut Displays","authors":"Jie Zhao, Rui Jiang, Maoyuan Huang, Yifei Qiao, Sinong Wang, Wanlu Zhang, Pengfei Tian, Jun Wang, Ruiqian Guo, Shiliang Mei","doi":"10.1021/acsenergylett.4c03510","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03510","url":null,"abstract":"Indium phosphide (InP) quantum dots (QDs) are promising eco-friendly emitters for next-generation displays and optoelectronics, offering high efficiency, narrow spectral linewidths, and tunable luminescence. However, their commercialization faces challenges due to synthesis and fabrication difficulties, particularly slow progress in improving photoluminescence quantum yield (PLQY), full-width at half-maximum (FWHM), and external quantum efficiency (EQE). Despite persistent shared challenges such as stability and operational lifetime, the broader FWHM of InP QDs has increasingly emerged as a critical bottleneck for their commercialization, especially given recent breakthroughs, including near-unity PLQY in core-only/core–shell InP QDs and over 20% EQE in their electroluminescent applications. This review examines FWHM broadening mechanisms in InP QDs and outlines strategies to narrow FWHM through size, lattice, bandgap, surface, and device architecture engineering. It also highlights trends and future directions for high-performance InP QDs and their electroluminescent applications, aiming to advance their commercialization in heavy metal-free displays and optoelectronics.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"141 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776217","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":"Wide-Bandgap Perovskite and Perovskite/Silicon Tandem Solar Cells through Strong Hydrogen Bonding Interaction","authors":"Cong Sun, Lu Jin, Xinjiang Wang, Biao Shi, Pengyang Wang, Ningyu Ren, Xiaojing Han, Lizetong Sun, Zhao Zhu, Qian Huang, Shengzhi Xu, Ying Zhao, Lijun Zhang, Xiaodan Zhang","doi":"10.1021/acsenergylett.5c00147","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00147","url":null,"abstract":"Enhancing the crystallization quality of wide-bandgap perovskite film is vital to raise the open-circuit voltage (<i>V</i><sub>OC</sub>) and performance of the device. Based on this, we present an approach involving the incorporation of 4-morpholino formamidine hydrochloride (MFC) as an additive in the antisolvent to facilitate crystal growth through the strong hydrogen bonding interactions and concurrently mitigate the deep-level defects. With this method, we can obtain increased grain size and achieve a transition toward a more n-type surface, which synergistically results in favorable carrier transport and reduced carrier recombination. Consequently, we were able to obtain an efficiency of 23.13% for 1.68 eV-inverted perovskite solar cells (PSCs) and 30.65% with a <i>V</i><sub>OC</sub> of 1.951 V for the two-terminal perovskite/silicon tandem solar cells (TSCs) while maintaining long-term stability. This additive approach provides a fresh perspective in wide-bandgap PSCs and further pushes the development of perovskite/silicon TSCs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"59 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782969","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":"Near-Infrared and Visible Dual-Band Self-Trapped Exciton Emissions from Li+-Doped Cs2NaScCl6 Double Perovskites","authors":"Yuhan Liu, Datao Tu, Mingjie Yang, Huihong Li, Chenliang Li, Zhi Xie, Shanshan Zhou, Shaohua Yu, Jin Xu, Xueyuan Chen","doi":"10.1021/acsenergylett.5c00182","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00182","url":null,"abstract":"Self-trapped excitons (STEs) have garnered significant attention due to their broadband emission and large Stokes shift. However, achieving multiband, particularly near-infrared (NIR) STE emissions remains a challenge, restricting their optoelectronic applications. Herein, we realize efficient dual-band STE emissions encompassing blue and NIR regions based on Cs<sub>2</sub>NaScCl<sub>6</sub> double perovskites (DPs) via minor Li<sup>+</sup>-doping structural engineering. The dual-band emissions in the blue and NIR regions originated from the STE states associated with [ScCl<sub>6</sub>]<sup>3–</sup> and [NaCl<sub>6</sub>]<sup>5–</sup> octahedra, respectively. Li<sup>+</sup> doping markedly enhanced the photoluminescence (PL) quantum yields of dual-band STE emissions from 3.2% and 2.7% to 98.2% and 45.4%, respectively. Steady-state/transient PL spectroscopies and density functional theory calculations revealed that Li<sup>+</sup> doping intensified sublattice distortion and enhanced charge carrier localization within Cs<sub>2</sub>NaScCl<sub>6</sub> DPs, thus boosting the dual-band STE emissions. These findings gain deep insights into STE manipulation in DPs through local structural engineering, thus stimulating the exploitation of DPs toward versatile applications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"259 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776218","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}
Luis Lanzetta, Luis Huerta Hernandez, Badri Vishal, Han Xu, Anirudh Sharma, Stefaan De Wolf, Derya Baran
{"title":"Tin–Lead Perovskite Solar Cells with Enhanced Reverse Bias Stability","authors":"Luis Lanzetta, Luis Huerta Hernandez, Badri Vishal, Han Xu, Anirudh Sharma, Stefaan De Wolf, Derya Baran","doi":"10.1021/acsenergylett.5c00727","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00727","url":null,"abstract":"We address reverse bias instability in tin–lead perovskite solar cells by introducing Cr/Cu bilayer electrodes in their electron-selective contacts, which raise thermal breakdown voltage from −7.6 V to −14.5 V. Chromium prevents catastrophic device failure by mitigating hotspot shunting, being chemically stable against I<sub>2</sub> formed during reverse bias stress.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"3 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776219","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}