Sreeram Jayan, Yuvaraj Sivalingam, Yoshiyuki Kawazoe and Surya Velappa Jayaraman*,
{"title":"Monolayer α-Tellurene as Anode for Metal Ion Rechargeable Batteries: A Comprehensive Investigation through DFT and AIMD Studies","authors":"Sreeram Jayan, Yuvaraj Sivalingam, Yoshiyuki Kawazoe and Surya Velappa Jayaraman*, ","doi":"10.1021/acsaem.4c0272210.1021/acsaem.4c02722","DOIUrl":"https://doi.org/10.1021/acsaem.4c02722https://doi.org/10.1021/acsaem.4c02722","url":null,"abstract":"<p >Herein, we have performed combined density functional theory (DFT) and <i>ab initio</i> molecular dynamics (AIMD) calculations to investigate the potential of α-tellurene (α-Te) monolayer as anode materials for metal ion batteries. Initial investigations explore the adsorption of lithium(Li)/sodium(Na)/magnesium(Mg) ions and their diffusion on α-Te anode. The Li-ion showed higher adsorption energy (−2.21 eV) compared to Na and Mg ions. The diffusion barrier of Li and Na is found to be 0.23 and 0.17 eV, respectively, compared to the Mg ion (0.53 eV). To understand the electrolyte–electrode interface characteristics, Li salt electrolytes with bis(fluorosulfonyl) imide (FSI) and bis-trifluoromethane sulfonyl imide (TFSI) anions are made to interact in parallel and perpendicular orientations with the surface of the α-Te anode. The adsorption of both FSI and TFSI anions is energetically favorable, and it induces a semiconductor-to-metal transition in the anode. Furthermore, the AIMD study on Li<sup>+</sup> integrated FSI/TFSI anions with α-Te was performed to understand the structural and dynamical parameters including the radial distribution function (RDF), diffusivity, etc. The α-Te monolayer has retained its structural integrity throughout the simulations. The RDF plots confirm that the oxygen of FSI and TFSI are more aggregating around the Li ions forming the solvation shell that initiates ion migration. Also, the pathway of Li<sup>+</sup> ion migration through the anions involves both vehicular and structural diffusion mechanisms. The self-diffusion coefficient of Li-ion is calculated as 4.48 × 10<sup>–9</sup> m<sup>2</sup>/s and 3.05 × 10<sup>–9</sup> m<sup>2</sup>/s in FSI and TFSI systems, respectively. In summary, our results demonstrate that the α-Te monolayer can be regarded as a reliable anode with excellent ion diffusion for future metal ion rechargeable batteries.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"5625–5635 5625–5635"},"PeriodicalIF":5.4,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933757","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pramod Madhukar Gawal, and , Animes Kumar Golder*,
{"title":"Plant-Derived Phytochemicals for the Synthesis of p–n Junction CuO/CdS Heterostructures for Photocatalytic Carbon Dioxide Reduction to Ethanol and Carbon Monoxide","authors":"Pramod Madhukar Gawal, and , Animes Kumar Golder*, ","doi":"10.1021/acsaem.5c0049710.1021/acsaem.5c00497","DOIUrl":"https://doi.org/10.1021/acsaem.5c00497https://doi.org/10.1021/acsaem.5c00497","url":null,"abstract":"<p >Photocatalytic reduction of CO<sub>2</sub> to value-added fuels is a promising strategy to mitigate the energy crisis and reduce greenhouse gas emissions. Herein, a bio-based zero-dimensional (0D) p–n heterojunction CuO/CdS photocatalyst (7.2 nm, 136.65 m<sup>2</sup>/g) with a conduction band of −1.12 V was synthesized using bio-analytes from <i>Aegle marmelos</i> via microwave irradiation. The p–n heterojunction enhanced the CO<sub>2</sub> adsorption capacity (0.643 mmol/g) and photocurrent response (0.94 μA/cm<sup>2</sup>) compared to CdS QDs(bio) and CuO QDs(bio). Additionally, it improved charge carrier dynamics by reducing PL intensities by 73 and 67% and increasing decay times by 74 and 54.6%, respectively. The internal electric field generated by the Fermi level difference between n-type CdS (−4.21 V) and p-type CuO (−4.7 V) enhanced charge separation and transport, suppressed recombination, and prevented photocorrosion (SO<sub>4</sub><sup>2–</sup>) of CdS QDs(bio). Density functional theory (DFT) analysis revealed alterations in the density of states (DOS) of CdS within the band gap region due to the incorporation of CuO, further facilitating efficient charge separation and transport at the local junctions. The optimal 0.50CuO/CdS QDs(bio) heterostructure exhibited remarkable photocatalytic performance for CO<sub>2</sub> reduction, achieving an ethanol (EtOH) and carbon monoxide (CO) production rate of 158.48/182.68 μmol/g/h (AQY 8.24/1.58%) while maintaining its structural and morphological stability. This work highlights the potential of bio-based p–n junction photocatalysts for efficient CO<sub>2</sub> reduction into value-added chemicals.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"6087–6099 6087–6099"},"PeriodicalIF":5.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933937","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Murtaza Manzoor Bhat, Feroz Ahmad Sofi, Sajad Ahmad Bhat, Adil Amin Wani, Aamir Yaseen Bhat, Pravin P. Ingole and Mohsin Ahmad Bhat*,
{"title":"MnO2-Templated CuBDC Metal Organic Framework: A Noble-Metal-Free Stable and Efficient pH-Universal Electrocatalyst for Oxygen Reduction Reaction","authors":"Murtaza Manzoor Bhat, Feroz Ahmad Sofi, Sajad Ahmad Bhat, Adil Amin Wani, Aamir Yaseen Bhat, Pravin P. Ingole and Mohsin Ahmad Bhat*, ","doi":"10.1021/acsaem.4c0331510.1021/acsaem.4c03315","DOIUrl":"https://doi.org/10.1021/acsaem.4c03315https://doi.org/10.1021/acsaem.4c03315","url":null,"abstract":"<p >The development of noble-metal-free, efficient, cost-effective, and stable pH-universal electrocatalysts for the oxygen reduction reaction (ORR) is essential for enabling the widespread adoption of ORR-based fuel cells and batteries in practical applications. Herein, we report the design and fabrication of a MnO<sub>2</sub>-supported Cu-Metal Organic Framework (Cu-MOF) as a cost-effective, efficient, stable, and above all a pH-universal ORR electrocatalyst. Specifically, a simple and scalable synthetic approach for the templated synthesis of CuBDC MOF networks over presynthesized MnO<sub>2</sub> nanosheets for the fabrication of CuBDC/MnO<sub>2</sub> composite is presented. The so-crafted CuBDC/MnO<sub>2</sub> composite well-characterized for its chemical, morphological, and electrochemical characteristics is demonstrated to be a pH-universal ORR electrocatalyst exhibiting excellent stability and electrocatalytic performance that is at par with that reported recently for the state-of-the-art noble metal-based ORR catalysts. The CuBDC/MnO<sub>2</sub> composite exhibits a mass transfer limited four-electron pathway ORR at a potential of just 0.74 V versus the reversible hydrogen electrode (RHE), with an overpotential (η<sub>ORR</sub>) of 0.45 V under alkaline conditions. The as-fabricated electrocatalyst delivers a specific activity (current per unit area) of −4.58 ± 0.01 mA/cm<sup>2</sup> and the mass activity (current per unit mass) of 8641.50 ± 0.01 mA/mg<sub>cat</sub>. Our detailed physicochemical and electrochemical investigations clearly establish that the unique synergism among the metal-oxide and MOF components in the CuBDC/MnO<sub>2</sub> composite endows it with unique features that result in the abundant availability and redox accessibility of Cu-redox sites and easy mass transportation of oxygen across an electronically and ionically good conducting [CuBDC/MnO<sub>2</sub>]/electrolyte interface. The work presented herein signifies a significant advancement toward the development of cost-effective and sustainable ORR electrocatalysts, potentially paving the way for their widespread adoption in clean and affordable electrochemical technologies for storage and conversion of energy.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"5745–5758 5745–5758"},"PeriodicalIF":5.4,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933924","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chenyu Zhang, Kai Chen, Xiaoxiao Li, Zhaoyang Wang, Shengyuan Yang, Roohollah Bagherzadeh, Feili Lai, Chao Zhang, Guanjie He, Ivan P. Parkin*, Yue-E Miao* and Tianxi Liu*,
{"title":"Carbon Nanofiber Host with Directed Gradient Pore Size for Dendrite-Free Lithium Metal Anodes","authors":"Chenyu Zhang, Kai Chen, Xiaoxiao Li, Zhaoyang Wang, Shengyuan Yang, Roohollah Bagherzadeh, Feili Lai, Chao Zhang, Guanjie He, Ivan P. Parkin*, Yue-E Miao* and Tianxi Liu*, ","doi":"10.1021/acsaem.5c0063210.1021/acsaem.5c00632","DOIUrl":"https://doi.org/10.1021/acsaem.5c00632https://doi.org/10.1021/acsaem.5c00632","url":null,"abstract":"<p >Three-dimensional carbon nanofibers with high conductivity, high specific surface area, and high porosity (≥70%) can be used as hosts for lithium metal storage. However, lithium ions easily concentrate at the top surface of the conductive carbon hosts during electrodeposition, making the internal space of the hosts largely inaccessible and ultimately leading to the growth of lithium dendrites on the top surface. Therefore, a conductive carbon nanofiber host with a directed gradient pore structure is reported in this work (signed as GPCF), based on two carbon nanofiber networks with both a small pore size (∼2.6 μm) as the current collector side and a large pore size (∼3.9 μm) facing the separator side. As a result, the uniform lithium-ion flow with a small ion concentration gradient from the separator to the current collector side is formed within GPCF, to enable the dendrite-free lithium deposition morphology. The GPCF anode can run for more than 160 cycles at 0.5 mA cm<sup>–2</sup> and 1 mAh cm<sup>–2</sup>, and the Coulombic efficiency is up to 99%. In contrast, the carbon nanofiber hosts with only small, large, or inverse gradient pore size structures easily form significant “dead Li” after 80, 120, and 100 cycles, respectively, and the Coulombic efficiency fluctuates severely. The above results reveal that the elaborately designed carbon nanofiber hosts with a directed gradient pore size can significantly homogenize the lithium-ion flow at the anode side to improve the electrochemical performance of lithium metal batteries.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"6203–6212 6203–6212"},"PeriodicalIF":5.4,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933986","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Siyuan Song, Changmin Shi, Akshay Pakhare, Brian W. Sheldon* and Pradeep R. Guduru*,
{"title":"Investigation of the Mechanical Properties of Porous Argyrodite Sulfide Electrolytes for All-Solid-State Batteries","authors":"Siyuan Song, Changmin Shi, Akshay Pakhare, Brian W. Sheldon* and Pradeep R. Guduru*, ","doi":"10.1021/acsaem.4c0314310.1021/acsaem.4c03143","DOIUrl":"https://doi.org/10.1021/acsaem.4c03143https://doi.org/10.1021/acsaem.4c03143","url":null,"abstract":"<p >Argyrodite sulfide (Li<sub>6</sub>PS<sub>5</sub>Cl) has been recognized as a promising solid electrolyte material for all-solid-state high-energy-density lithium ion batteries. However, the issue of Li dendrite penetration through Li<sub>6</sub>PS<sub>5</sub>Cl continues to be a challenge that limits its performance and wider applications. To understand dendrite growth that is mediated by fracture, measurement of the relevant mechanical properties, i.e., the elastic modulus and the fracture toughness of Li<sub>6</sub>PS<sub>5</sub>Cl, is necessary to develop quantitative predictive models of dendrite initiation and propagation and help develop strategies to toughen Li<sub>6</sub>PS<sub>5</sub>Cl. Here, an investigation to measure the Young’s modulus and fracture toughness of porous Li<sub>6</sub>PS<sub>5</sub>Cl material is reported; it makes use of a custom-built experimental setup. An analysis of the experimental data in conjunction with finite element simulations shows the Young’s modulus of porous Li<sub>6</sub>PS<sub>5</sub>Cl to be 4.7 ± 1.1 GPa and the fracture toughness to be <i></i><math><mn>0.17</mn><mo>±</mo><mn>0.03</mn><mspace></mspace><mrow><mi>M</mi><mi>P</mi><mi>a</mi></mrow><msqrt><mi>m</mi></msqrt></math>. These results characterize the bulk behavior of the material at a millimeter scale in contrast to the local surface properties at the micrometer scale through nanoindentation. Based on these values, for a pre-existing crack of size 1 μm, the corresponding critical overpotential and critical current density are estimated to be approximately 12 mV and 1 mA/cm<sup>2</sup> respectively. The measurements reported here contribute to the body of knowledge on Li<sub>6</sub>PS<sub>5</sub>Cl toward the larger goal of enhancing the ability to predict Li dendrite initiation and propagation in it.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"5636–5644 5636–5644"},"PeriodicalIF":5.4,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933983","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zilong Su, Mengyuan Jin, Chunxi Hu, Ran Liu, Renbing Wu, Deliang Xu* and Yanhui Guo*,
{"title":"A Novel Oxidized Na2B12H12–Based Electrolyte for High-Voltage All-Solid-State Sodium Batteries","authors":"Zilong Su, Mengyuan Jin, Chunxi Hu, Ran Liu, Renbing Wu, Deliang Xu* and Yanhui Guo*, ","doi":"10.1021/acsaem.4c0318510.1021/acsaem.4c03185","DOIUrl":"https://doi.org/10.1021/acsaem.4c03185https://doi.org/10.1021/acsaem.4c03185","url":null,"abstract":"<p >Developing practical solid electrolytes is a tough challenge and an urgent necessity for future cell applications. The Na<sub>2</sub>B<sub>12</sub>H<sub>12</sub> solid electrolyte (SE) is considered as one of the most promising candidates due to its high stability, excellent alkali metal compatibility, low density, and safe properties. However, its inherent low ionic conductivity at room temperature and narrow electrochemical stability window (ESW) limit its development. Herein, a simple method of ball milling Na<sub>2</sub>B<sub>12</sub>H<sub>12</sub> in an oxygen atmosphere has been developed, which can significantly increase the ionic conductivity by 3 orders of magnitude and broaden the ESW. Distinctively, high ionic conductivity (1.3 × 10<sup>–3</sup> S cm<sup>–1</sup>), wide ESW (5.2 V), favorable thermal stability (>300 °C), and good electrode adaptability have been achieved by an oxidized Na<sub>2</sub>B<sub>12</sub>H<sub>12</sub>-20 wt % SiO<sub>2</sub> composite. The Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub>O<sub>2</sub>F/oxidized Na<sub>2</sub>B<sub>12</sub>H<sub>12</sub>-20 wt % SiO<sub>2</sub>/Na cell shows a specific capacity retention of 83.7% after 100 cycles at 0.1 C and a specific capacity of 49.1 mAh g<sup>–1</sup> at 2 C. Hence, the oxidized Na<sub>2</sub>B<sub>12</sub>H<sub>12</sub> SE proposed in this study has the potential to function as a practical material for all-solid-state batteries (ASSBs).</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"5656–5663 5656–5663"},"PeriodicalIF":5.4,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933921","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Peikai Qiu, Yuze Chen, Wenjie Wang, Tianyi Liu and Jinghua Wu*,
{"title":"A Scalable and Versatile Synthetic Strategy of Halide Electrolytes for High-Performance All-Solid-State Lithium Batteries","authors":"Peikai Qiu, Yuze Chen, Wenjie Wang, Tianyi Liu and Jinghua Wu*, ","doi":"10.1021/acsaem.5c0045410.1021/acsaem.5c00454","DOIUrl":"https://doi.org/10.1021/acsaem.5c00454https://doi.org/10.1021/acsaem.5c00454","url":null,"abstract":"<p >Halide electrolytes have emerged as promising candidates due to their high ionic conductivity, good compatibility with high-voltage cathodes, and excellent mechanical properties. However, traditional synthesis methods, such as high-energy ball milling, face challenges, including high energy consumption, long processing times, and limited scalability. Additionally, the large particle size of electrolytes results in poor interfacial contact and ion transport, making it difficult to achieve stable cycling in all-solid-state batteries (ASSLBs). Here, we developed a scalable ammonia-assisted hydrolysis combined with a freeze-drying (AAH-FD) method for synthesizing halide electrolytes. The Li<sub>3</sub>YCl<sub>6</sub> electrolyte synthesized via AAH-FD exhibited an orthorhombic (Pnma) structure with a high ionic conductivity of 0.50 mS cm<sup>–1</sup>. The method was also successfully applied to synthesize Li<sub>3</sub>ErCl<sub>6</sub> and Li<sub>3</sub>HoCl<sub>6</sub>, confirming its versatility. ASSLBs with AAH-FD Li<sub>3</sub>YCl<sub>6</sub> demonstrated superior electrochemical performance, including a higher discharge capacity, better rate capability, and enhanced cycling stability. The LiCoO<sub>2</sub>-based ASSLB retained 77.6% of its capacity after 400 cycles at 1C, while the NCM622-based battery retained 79%. These improvements result from the optimized microstructure, smaller particle size, and reduced interfacial resistance, enhancing the lithium-ion transport. Moreover, AAH-FD enables 100 g of batch production, demonstrating excellent scalability. This study establishes AAH-FD as an efficient, versatile, and scalable synthesis strategy, offering a promising approach for the next-generation high-performance ASSLBs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"6035–6043 6035–6043"},"PeriodicalIF":5.4,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143934193","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Facile Synthesis of a Highly Efficient and Durable Bifunctional Oxygen Electrocatalyst CFS@CN/F Composite for Rechargeable Zinc-Air Batteries","authors":"Shiqi Song, Maochong Tang, Chupeng Wang, Mingsheng Luo, Xiaoxia Wang* and Hui Liu, ","doi":"10.1021/acsaem.5c0038210.1021/acsaem.5c00382","DOIUrl":"https://doi.org/10.1021/acsaem.5c00382https://doi.org/10.1021/acsaem.5c00382","url":null,"abstract":"<p >Synthesis of bifunctional oxygen electrocatalysts with high ORR and OER catalytic activity is important for the development of next-generation rechargeable zinc-air batteries. CoFeSNC with high ORR catalytic activity and CoNiLDH/FeOOH with high OER catalytic activity are prepared using wet chemistry and ion exchange strategies, respectively. CFS@CN/F composite electrocatalysts are prepared by grinding and mixing CoFeSNC and CoNiLDH/FeOOH together. The introduction of bimetallic sites and weakly electronegative S atoms into M–N–C catalytic materials synergistically improves the adsorption and activation of oxygenated intermediates, effectively overcoming the limitations of single-heteroatom catalytic materials. Space charge effects and built-in electric fields in CoNiLDH/FeOOH heterojunctions improve electron transfer and reduce the OER reaction energy barriers. The CFS@CN/F catalyst exhibits excellent bifunctional electrocatalytic activity (Δ<i>E</i> = 0.689 V vs RHE); the zinc-air battery based on CFS@CN/F shows a high peak power density (183.8 mW cm<sup>–2</sup>) and specific capacity (792 mAh g<sup>–1</sup>). This work provides a valuable reference for the design and development of efficient ORR/OER bifunctional electrocatalysts with practical applicability.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"5963–5974 5963–5974"},"PeriodicalIF":5.4,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933789","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Eun Young Lim, Taekyun Kwon, Eunsol Lee, Ji-Oh Kim, Jae Bin Park, Byeong Jin Kim, Yewon Park, Hyeonchul So, Ah Reum Choi, Seungjo Hong, Se Yeong Jung, Dong-Gyun Kim, Jae Hyuk Hwang*, Minjoon Park* and Jin Hong Lee*,
{"title":"A Synergistic Binder with Stress-Resilient and Polysulfide Adsorption to Enhance the Cycle Stability of Lithium–Sulfur Batteries","authors":"Eun Young Lim, Taekyun Kwon, Eunsol Lee, Ji-Oh Kim, Jae Bin Park, Byeong Jin Kim, Yewon Park, Hyeonchul So, Ah Reum Choi, Seungjo Hong, Se Yeong Jung, Dong-Gyun Kim, Jae Hyuk Hwang*, Minjoon Park* and Jin Hong Lee*, ","doi":"10.1021/acsaem.5c0025110.1021/acsaem.5c00251","DOIUrl":"https://doi.org/10.1021/acsaem.5c00251https://doi.org/10.1021/acsaem.5c00251","url":null,"abstract":"<p >Lithium–sulfur batteries (LSBs) are regarded as a promising high-density energy storage system due to their high theoretical capacity (1675 mA h g<sup>–1</sup>) and energy density (2500 W h kg<sup>–1</sup>). However, the commercialization of LSBs has been impeded by the shuttle effect of intermediate lithium polysulfides (LiPSs) and the significant volume expansion of sulfur species during the discharge process. These disadvantages result in rapid capacity decay and the irreversible loss of active material, ultimately leading to the short cycle life of the LSBs. In this study, we propose a synergistic polyurethane-polyethylenimine (PEP) binder designed to provide exceptional stress resilience and strong chemical interactions with LiPSs, addressing the critical challenges of the shuttle effect and electrode instability in sulfur cathodes of LSBs. The excellent stress resilience of the PEP binder accommodates the stress generated during the volume expansion of sulfur species over repeated cycling conditions, leading to stabilizing the sulfur cathode surface and preserving Li-ion (Li<sup>+</sup>) transfer pathways. Furthermore, the abundant polar groups in PEP, including ether, urethane, and amine groups, facilitate Li<sup>+</sup> transport while effectively interacting with soluble LiPSs to suppress the shuttling behavior. Consequently, the cell with the PEP binder demonstrated favorable LiPSs conversion, superior electrochemical performances, and improved redox reaction kinetics compared to those with poly(vinylidene fluoride) (PVDF) and epoxy-terminated polyurethane (PUE) binders. This research offers a strategic methodology for designing a multifunctional polymer binder to develop high-performance LSBs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"5811–5822 5811–5822"},"PeriodicalIF":5.4,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933747","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Wei Zhang, Hanxiao Zhang, Yuyan Zhou, Can Wang and Jiulong Sha*,
{"title":"A Bilayer Hydrogel with Heterogeneous Structures for Highly Efficient Moisture Energy Harvesting","authors":"Wei Zhang, Hanxiao Zhang, Yuyan Zhou, Can Wang and Jiulong Sha*, ","doi":"10.1021/acsaem.5c0033510.1021/acsaem.5c00335","DOIUrl":"https://doi.org/10.1021/acsaem.5c00335https://doi.org/10.1021/acsaem.5c00335","url":null,"abstract":"<p >Moist-electric generators (MEG), which extract energy from ambient moisture, offer a potential solution to the escalating energy crisis. However, current MEG technologies encounter significant challenges, including pulsed output and limited power generation capacity. In this study, a heterogeneous hydrogel-based MEG (H-MEG), incorporating both hydrophilicity and double ion concentration gradients, was developed. A single H-MEG device (1 × 1 cm<sup>2</sup>) achieved a maximum open-circuit voltage (<i>V</i><sub>OC</sub>) of 0.64 V and a short-circuit current (<i>I</i><sub>SC</sub>) of 72.12 μA at 80% relative humidity. Furthermore, by employing series and parallel integration of H-MEG banks, enhanced performance was achieved with voltages of 6.62 V and currents of up to 670.86 μA, respectively. These scalable H-MEG devices could directly power commercial electronic devices, including light-emitting diodes and commercial calculators. This study proposes a cost-effective and highly efficient approach for harvesting electricity from moist air, significantly contributing to the advancement of green power sources.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 9","pages":"5925–5935 5925–5935"},"PeriodicalIF":5.4,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933791","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}