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Entropy Engineering in the Off-Stoichiometric Ti2NiCoSn0.5Sb1.5 Double Half-Heusler Alloy
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-03-06 DOI: 10.1021/acsaem.4c0338210.1021/acsaem.4c03382
Soumya Ranjan Mishra, Pattamadai Sundaram Sankara Rama Krishnan, Karl P. Davidson, Raju Vijayaraghavan Ramanujan and Budaraju Srinivasa Murty*, 
{"title":"Entropy Engineering in the Off-Stoichiometric Ti2NiCoSn0.5Sb1.5 Double Half-Heusler Alloy","authors":"Soumya Ranjan Mishra,&nbsp;Pattamadai Sundaram Sankara Rama Krishnan,&nbsp;Karl P. Davidson,&nbsp;Raju Vijayaraghavan Ramanujan and Budaraju Srinivasa Murty*,&nbsp;","doi":"10.1021/acsaem.4c0338210.1021/acsaem.4c03382","DOIUrl":"https://doi.org/10.1021/acsaem.4c03382https://doi.org/10.1021/acsaem.4c03382","url":null,"abstract":"<p >Lowering the thermal conductivity by phonon scattering has been previously studied in high-entropy alloys (HEAs). This concept has been extended to half-Heusler (HH) alloys in the form of entropy engineering by substituting one of the elements with multiple elements or by combining 2 HH alloys to form a double half-Heusler alloy. Here, entropy engineering of double HH Ti<sub>2</sub>NiCoSn<sub>0.5</sub>Sb<sub>1.5</sub> by the substitution of Ti with Al, Ta, and Zr was studied. Due to their low solubility in Ti, Al and Ta formed Ni-based intermetallic phases. Compositional tuning was performed based on the optimum individual dopant levels of Al, Ta, and Zr. Compositional tuning revealed that the introduction of Ta and Al improved the power factor and lowered thermal conductivity due to the formation of the TaNiCoAl quaternary full Heusler (FH) secondary phase. Zr was completely soluble in the HH alloy, lowering the thermal conductivity at the expense of the power factor. Ti<sub>1.6</sub>Ta<sub>0.2</sub>Al<sub>0.2</sub>NiCoSn<sub>0.5</sub>Sb<sub>1.5</sub> with a power factor of 3.83 mW/mK<sup>2</sup> had a ZT of 0.71 at 823 K, which is higher than those of other double HH alloys. Ti<sub>0.6</sub>Ta<sub>0.2</sub>Al<sub>0.2</sub>ZrNiCoSn<sub>0.5</sub>Sb<sub>1.5</sub> also exhibited a low lattice thermal conductivity of 2.19 W/mK at 420 K, which is comparable to that of Hf-substituted HH alloys. On the other hand, entropy engineering by equimolar substitution of elements did not lead to improvement in properties, underlining the need for compositional tuning in the HH alloys.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3715–3731 3715–3731"},"PeriodicalIF":5.4,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675826","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}
引用次数: 0
Tuning the Electrochemical Performance of Cu2S/Co3S4 via Optimized CNT Incorporation for High Energy and High Power Supercapacitor Application
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-03-06 DOI: 10.1021/acsaem.5c0004410.1021/acsaem.5c00044
Arkapriya Das, Ankita Mondal and Bhanu Bhusan Khatua*, 
{"title":"Tuning the Electrochemical Performance of Cu2S/Co3S4 via Optimized CNT Incorporation for High Energy and High Power Supercapacitor Application","authors":"Arkapriya Das,&nbsp;Ankita Mondal and Bhanu Bhusan Khatua*,&nbsp;","doi":"10.1021/acsaem.5c0004410.1021/acsaem.5c00044","DOIUrl":"https://doi.org/10.1021/acsaem.5c00044https://doi.org/10.1021/acsaem.5c00044","url":null,"abstract":"<p >Transition metal sulfides are emerging as promising materials for supercapacitor applications due to their excellent conductivity, high theoretical capacities, and stability. Exploring these materials, along with enhancements like doping of carbonaceous materials, could lead to high-performance solutions that address the growing need for renewable energy technologies and sustainable energy storage systems. Herein, mixed metal sulfide Cu<sub>2</sub>S/Co<sub>3</sub>S<sub>4</sub> composites with varying percentages of multiwalled carbon nanotubes (MWCNTs) were synthesized through a facile one-step hydrothermal method. The resulting materials displayed outstanding electrochemical behavior. This performance was optimized by tuning the weight percentage of CNTs doped in the metal sulfide scaffold. Among the prepared nanocomposites, i.e., Cu<sub>2</sub>S/Co<sub>3</sub>S<sub>4</sub>@CNT-<i>x</i>, referred to as CCS@CNT-<i>x</i> (where <i>x</i> is the wt % of CNT), CCS@CNT-10 showed the maximum specific capacitance (<i>C</i><sub>sp</sub>) of 960 F g<sup>–1</sup> at 1 A g<sup>–1</sup> (specific capacity, <i>C</i><sub>s</sub> of 638 C g<sup>–1</sup>), as revealed from electrochemical measurements. The as-fabricated device CCS@CNT-10//activated carbon sustained a broad potential window of 1.7 V, showing a high power density of 17000 W kg<sup>–1</sup> along with a high energy density of 68 Wh kg<sup>–1</sup> at 20 A g<sup>–1</sup>. The device was able to maintain its cyclic stability up to 95% even after 20,000 cycles. The exceptional electrochemical performance of the device can be attributed to the synergistic interactions between Cu<sub>2</sub>S and Co<sub>3</sub>S<sub>4</sub>, combined with the highly conductive interconnected network created by CNT incorporation. This combination facilitates efficient redox reactions at the electrode–electrolyte interface and accelerates electron transport throughout the material.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3812–3825 3812–3825"},"PeriodicalIF":5.4,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675824","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}
引用次数: 0
Influence of Commercial Ionomers and Membranes on a PGM-Free Catalyst in the Alkaline Oxygen Reduction.
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-03-06 eCollection Date: 2025-03-24 DOI: 10.1021/acsaem.4c02929
Simon Kellner, Ziyang Liu, Francesco D'Acierno, Angus Pedersen, Jesús Barrio, Sandrine Heutz, Ifan E L Stephens, Silvia Favero, Maria-Magdalena Titirici
{"title":"Influence of Commercial Ionomers and Membranes on a PGM-Free Catalyst in the Alkaline Oxygen Reduction.","authors":"Simon Kellner, Ziyang Liu, Francesco D'Acierno, Angus Pedersen, Jesús Barrio, Sandrine Heutz, Ifan E L Stephens, Silvia Favero, Maria-Magdalena Titirici","doi":"10.1021/acsaem.4c02929","DOIUrl":"10.1021/acsaem.4c02929","url":null,"abstract":"<p><p>Hitherto, research into alkaline exchange membrane fuel cells lacked a commercial benchmark anionomer and membrane, analogous to Nafion in proton-exchange membrane fuel cells. Three commercial alkaline exchange ionomers (AEIs) have been scrutinized for that role in combination with a commercial platinum-group-metal-free Fe-N-C (Pajarito Powder) catalyst for the cathode. The initial rotating disc electrode benchmarking of the Fe-N-C catalyst's oxygen reduction reaction activity using Nafion in an alkaline electrolyte seems to neglect the restricted oxygen diffusion in the AEIs and is recommended to be complemented by measurements with the same AEI as used in the alkaline exchange membrane fuel cell (AEMFC) testing. Evaluation of the catalyst layer in a gas-diffusion electrode setup offers a way to assess the performance in realistic operating conditions, without the additional complications of device-level water management. Blending of a porous Fe-N-C catalyst with different types of AEI yields catalyst layers with different pore size distributions. The catalyst layer with Piperion retains the highest proportion of the original BET surface area of the Fe-N-C catalyst. The water adsorption capacity is also influenced by the AEI, with Fumion FAA-3 and Piperion having equally high capabilities surpassing Sustainion. Finally, the choice of the membrane influences the ORR performance as well; particularly, the low hydroxide conductivity of Fumion FAA-3 in the room temperature experiments mitigates the ORR performance irrespective of the AEI in the catalyst layer. The best overall performance at high current densities is shown by the Piperion anion exchange ionomer matched with Sustainion X37-50 membrane.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3470-3480"},"PeriodicalIF":5.4,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11938204/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143727005","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Boosting Performance of PEMFCs via Optimization of Oxygen Transport Resistance in Catalyst Layers Using Mesoporous Carbons
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-03-06 DOI: 10.1021/acsaem.5c0000910.1021/acsaem.5c00009
Guo-Rui Zhao, Wen-Zhen Fang*, Han Ling, Kai-Bo An, Yu-Hao Lu and Wen-Quan Tao, 
{"title":"Boosting Performance of PEMFCs via Optimization of Oxygen Transport Resistance in Catalyst Layers Using Mesoporous Carbons","authors":"Guo-Rui Zhao,&nbsp;Wen-Zhen Fang*,&nbsp;Han Ling,&nbsp;Kai-Bo An,&nbsp;Yu-Hao Lu and Wen-Quan Tao,&nbsp;","doi":"10.1021/acsaem.5c0000910.1021/acsaem.5c00009","DOIUrl":"https://doi.org/10.1021/acsaem.5c00009https://doi.org/10.1021/acsaem.5c00009","url":null,"abstract":"<p >Mesoporous carbons, as the catalyst support in proton exchange membrane fuel cells (PEMFCs), can improve the specific activity of catalysts and the high-power performance of cells, but the underlying physics remains elusive. In this work, a model is proposed to describe the oxygen transport process for both exterior and interior platinum (Pt) catalysts on the mesoporous carbon catalyst layers (CLs) under various relative humidity (RH) conditions, considering the structure evolution of interior pores induced by the condensed water. We find that although the local oxygen transport resistance (<i>R</i><sub>Pt</sub><sup>O<sub>2</sub></sup>) of interior Pt catalysts is less than that of exterior Pt catalysts, too much Pt deposit in the interior pores would still lead to the remarkable increase of <i>R</i><sub>Pt</sub><sup>O<sub>2</sub></sup>. The output performance of mesoporous carbon CLs is better than that of solid carbon CLs at a high RH but is instead worse at a low RH value. A data-driven model is then built to unravel the structure–performance relation of the mesoporous carbon. By reducing <i>R</i><sub>Pt</sub><sup>O<sub>2</sub></sup> via microstructure optimization, we determine an optimal pore size of mesoporous carbons where the output performance is the best within the studied range of RH values.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3732–3744 3732–3744"},"PeriodicalIF":5.4,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675791","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}
引用次数: 0
Dynamic Overcharge Performance and Mechanism of Lithium-Ion Batteries during High-Temperature Calendar Aging 锂离子电池在高温历时老化过程中的动态过充电性能和机理
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-03-06 DOI: 10.1021/acsaem.4c0301510.1021/acsaem.4c03015
Deyou Yin*, Jimin Ni*, Xiuyong Shi, Hua Liu, Meng Lv, Wei Shen and Guangxu Zhang*, 
{"title":"Dynamic Overcharge Performance and Mechanism of Lithium-Ion Batteries during High-Temperature Calendar Aging","authors":"Deyou Yin*,&nbsp;Jimin Ni*,&nbsp;Xiuyong Shi,&nbsp;Hua Liu,&nbsp;Meng Lv,&nbsp;Wei Shen and Guangxu Zhang*,&nbsp;","doi":"10.1021/acsaem.4c0301510.1021/acsaem.4c03015","DOIUrl":"https://doi.org/10.1021/acsaem.4c03015https://doi.org/10.1021/acsaem.4c03015","url":null,"abstract":"<p >Battery safety plays a critical role in ensuring the reliable operation of lithium-ion batteries during the service lifetime. Lithium-ion batteries often remain in a static state for extended periods during vehicle applications, particularly in high-temperature conditions, which poses significant challenges to their safety performance. In this content, this work investigates the evolution of overcharge performances and underlying mechanism during high-temperature calendar aging. The findings reveal that overcharge tolerance, represented by thermal runaway triggering temperature and duration time, decreases with aging. Simultaneously, thermal hazards, indicated by maximum temperature and maximum temperature rise rate, also diminish with aging. Multidimensional characterization demonstrates that lithium plating, gas generation, and transition metal dissolution are key failure mechanisms leading to performance degradation. Specifically, the reduced thermal stability of the anode and cathode is identified as the primary cause of the decline in overcharge tolerance. In contrast, the loss of active materials and active lithium emerges as the major factor contributing to the reduction in thermal hazard with aging.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3491–3499 3491–3499"},"PeriodicalIF":5.4,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675787","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}
引用次数: 0
3D Graphene Nanoflake/Vertically Aligned Carbon Nanotube/CoAl Layered Double Oxide Composites for High-Performance Lithium-Ion Batteries
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-03-06 DOI: 10.1021/acsaem.5c0016410.1021/acsaem.5c00164
Kang-Ming Liao, Yu Kevin Dai, Hao-Yu Wang, Shuguang Deng and Gui-Ping Dai*, 
{"title":"3D Graphene Nanoflake/Vertically Aligned Carbon Nanotube/CoAl Layered Double Oxide Composites for High-Performance Lithium-Ion Batteries","authors":"Kang-Ming Liao,&nbsp;Yu Kevin Dai,&nbsp;Hao-Yu Wang,&nbsp;Shuguang Deng and Gui-Ping Dai*,&nbsp;","doi":"10.1021/acsaem.5c0016410.1021/acsaem.5c00164","DOIUrl":"https://doi.org/10.1021/acsaem.5c00164https://doi.org/10.1021/acsaem.5c00164","url":null,"abstract":"<p >Using a urea-assisted precipitation method, we synthesized CoAl-layered double hydroxide (LDH) nanosheets that were uniformly aligned perpendicular to the surface of the silicon wafer. Then, a carbon nanocomposite consisting of vertically aligned carbon nanotubes (VACNTs) and graphene nanoflakes (GNFs) was prepared by plasma-enhanced chemical vapor deposition (PECVD) using LDH as the catalyst precursor. After heat treatment, LDH formed a layered double oxide (LDO). The VACNTs were attached to both sides of the LDO nanosheets, while GNFs were uniformly distributed on the VACNTs’ surface. Next, the three-dimensional (3D) GNF/VACNT-LDO material was used as a conductive agent for the LiFePO<sub>4</sub> cathode with a practical commercialized state-of-the-art cathode recipe of lithium-ion batteries. The results showed that the cathode had a high specific capacity and excellent cycling stability. The discharge specific capacity was as high as 168.6 mAh g<sup>–1</sup> at a current rate of 0.2 C. Amazingly, when the current rate was increased to 10 C, the discharge capacity reached 105.3 mAh g<sup>–1</sup>, which was much higher than that with the conventional conductive agent Super P (65.1 mAh g<sup>–1</sup>). After 500 cycles at 0.5 C current density, the discharge specific capacity was still 118.2 mAh g<sup>–1</sup>, with a capacity retention rate of 72.7% and an average capacity loss of only 0.089 mAh g<sup>–1</sup> per cycle. The excellent rate performance and cycling stability of the LFP cathode are largely attributed to the GNF/VACNT-LDO. The unique 3D conductive network constructed by GNF/VACNT-LDO can greatly increase the electron transport rate and accelerate the shuttling of Li<sup>+</sup> between the electrolyte and the electrode material.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3892–3903 3892–3903"},"PeriodicalIF":5.4,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675801","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}
引用次数: 0
Molecular Crystalline Electrolyte Based on Li{N(SO2CF3)2} and Succinonitrile with Closely Contacted Grain Boundary Interfaces Exhibiting Selective Li-Ion Conductivity and 5 V-Class Electrochemical Stability
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-03-06 DOI: 10.1021/acsaem.4c0320710.1021/acsaem.4c03207
Hiroto Katsuragawa, Sawako Mori, Yusuke Tago, Shota Maeda, Shuichi Matsuda, Hikaru Toriu, Ryo Nakayama, Shigeru Kobayashi, Taro Hitosugi* and Makoto Moriya*, 
{"title":"Molecular Crystalline Electrolyte Based on Li{N(SO2CF3)2} and Succinonitrile with Closely Contacted Grain Boundary Interfaces Exhibiting Selective Li-Ion Conductivity and 5 V-Class Electrochemical Stability","authors":"Hiroto Katsuragawa,&nbsp;Sawako Mori,&nbsp;Yusuke Tago,&nbsp;Shota Maeda,&nbsp;Shuichi Matsuda,&nbsp;Hikaru Toriu,&nbsp;Ryo Nakayama,&nbsp;Shigeru Kobayashi,&nbsp;Taro Hitosugi* and Makoto Moriya*,&nbsp;","doi":"10.1021/acsaem.4c0320710.1021/acsaem.4c03207","DOIUrl":"https://doi.org/10.1021/acsaem.4c03207https://doi.org/10.1021/acsaem.4c03207","url":null,"abstract":"<p >Achieving all-solid-state batteries requires the development of solid electrolytes with high ionic conductivities, high Li-ion transference numbers, and wide-range electrochemical stabilities. Molecular crystals, which combine a moderate flexibility similar to that of polymer electrolytes with ion conduction paths resembling those of ceramic electrolytes, have attracted attention as promising candidates for innovative solid electrolytes. Improving the properties of molecular crystalline electrolytes requires clarifying the correlations between their hierarchical structures and electrolyte properties, as well as establishing material design guidelines. Herein, we report the organic molecular crystal Li<sub>2</sub>{N(SO<sub>2</sub>CF<sub>3</sub>)}<sub>2</sub>(NCCH<sub>2</sub>CH<sub>2</sub>CN)<sub>3</sub>, hereafter referred to as Li<sub>2</sub>(TFSA)<sub>2</sub>(SN)<sub>3</sub>, as a promising solid electrolyte. This molecular crystal exhibits an ionic conductivity of 3.6 × 10<sup>–5</sup> S cm<sup>–1</sup> at 30 °C with a considerably high Li-ion transference number of 0.98. In addition, we confirmed the wide electrochemical stability of the 5 V-class cathodes and their compatibility with Li metal anodes. Scanning electron microscopy observations revealed the formation of tightly contacted grain boundaries in the powder-molded pellets of Li<sub>2</sub>(TFSA)<sub>2</sub>(SN)<sub>3</sub>. Notably, the previously reported molecular crystalline electrolyte Li(PF<sub>6</sub>)(NC(CH<sub>2</sub>)<sub>4</sub>CN)<sub>2</sub> (Li(PF<sub>6</sub>)(ADN)<sub>2</sub>) formed an interface containing liquid components of substantial thickness with a Li-ion transference number of only 0.54. These results highlight that both, the selection of constituent molecules and anions and the design of the grain boundary interface, play crucial roles in achieving superior electrochemical stability and selective Li-ion conductivity in the development of molecular crystalline electrolytes.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3599–3605 3599–3605"},"PeriodicalIF":5.4,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675825","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}
引用次数: 0
Designing Two-Dimensional Graphullerene C36 as High-Performance Anode Materials for Li-Ion Batteries: A First-Principles Study
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-03-05 DOI: 10.1021/acsaem.4c0332210.1021/acsaem.4c03322
Xin-Yue Qiu, Shi-Cong Mo, Jing Nie, Guang-Ye Li, Pei-Yi Liang, Jun-Xi Li, Chudong Xu* and Shi-Zhang Chen*, 
{"title":"Designing Two-Dimensional Graphullerene C36 as High-Performance Anode Materials for Li-Ion Batteries: A First-Principles Study","authors":"Xin-Yue Qiu,&nbsp;Shi-Cong Mo,&nbsp;Jing Nie,&nbsp;Guang-Ye Li,&nbsp;Pei-Yi Liang,&nbsp;Jun-Xi Li,&nbsp;Chudong Xu* and Shi-Zhang Chen*,&nbsp;","doi":"10.1021/acsaem.4c0332210.1021/acsaem.4c03322","DOIUrl":"https://doi.org/10.1021/acsaem.4c03322https://doi.org/10.1021/acsaem.4c03322","url":null,"abstract":"<p >Two-dimensional (2D) structures hold promise as advanced lithium-ion battery (LIB) anode materials. Recently synthesized 2D graphullerene faces challenges due to its large electronic insulating band gap. In this study, we construct a quasi-tetragonal graphullerene, C<sub>36</sub>, denoted as GrF-C<sub>36</sub>, using C<sub>36</sub> fullerenes with <i>D</i><sub>6<i>h</i></sub> symmetry as the structural unit. First-principles calculations revealed that the delocalized p<sub><i>z</i></sub> orbitals lead to metallicity, combined with intrinsic porosity, resulting in a large theoretical capacity of 496 mAh/g when they are used as LIB anode material. However, the structure exhibits a large migration barrier for lithium ions (Li<sup>+</sup>), limiting its rate performance. To address this, we further adopt the strategy for constructing long-range-ordered carbon by “removing” the [2 + 2] cycloaddition bonds to form intrinsic one-dimensional channels in the structure, denoted as LOPC-C<sub>32</sub>. Calculations showed that LOPC-C<sub>32</sub> maintains metallicity and enhances the structural stability while achieving a Li capacity of 906 mAh/g. The migration barrier for Li<sup>+</sup> within these channels is only 0.12 eV, significantly improving the rate performance. Coupled with an average open-circuit voltage of 0.43 V and a structural deformation of only 5% at a maximum Li capacity, LOPC-C<sub>32</sub> emerges as an excellent anode material. Our work provides a design strategy for the application of graphullerenes in LIBs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3698–3706 3698–3706"},"PeriodicalIF":5.4,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675785","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}
引用次数: 0
Development of a Thin Three-Dimensional Ag Gradient Cu-Separator Scaffold for Stable and High-Energy Lithium Metal Batteries
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-03-04 DOI: 10.1021/acsaem.4c0295510.1021/acsaem.4c02955
Seoyoung Choi, Jinhyeon Jo and KwangSup Eom*, 
{"title":"Development of a Thin Three-Dimensional Ag Gradient Cu-Separator Scaffold for Stable and High-Energy Lithium Metal Batteries","authors":"Seoyoung Choi,&nbsp;Jinhyeon Jo and KwangSup Eom*,&nbsp;","doi":"10.1021/acsaem.4c0295510.1021/acsaem.4c02955","DOIUrl":"https://doi.org/10.1021/acsaem.4c02955https://doi.org/10.1021/acsaem.4c02955","url":null,"abstract":"<p >Adopting three-dimensional (3D) scaffolds onto lithium metal anode has emerged as a promising strategy to improve the charge/discharge stability of next-generation high-energy-density lithium metal batteries (LMBs). However, the undesirable growth of Li dendrites on the scaffold’s surface and their high-cost fabrication methods remain challenging. To address these issues, herein, a functional 3D scaffold employing a lithiophilic Ag concentration gradient (3D Ag@Cu) is designed, which can be prepared via a simple galvanic displacement. The lithiophilic Ag reacts with Li to form a solid solution, reducing the Li nucleation overpotential and promoting uniform Li deposition. Furthermore, the Ag-gradient structure facilitates the bottom-up growth of Li within the scaffold, maximizing the use of the internal space. Consequently, a full-cell equipped with the 3D Ag@Cu scaffold demonstrated higher cycling stability (89.03% capacity retention after 110 cycles) and rate performance (65.6% capacity retention at 2 C) compared to both LMBs with the planar Cu foil and the bare 3D Cu scaffold.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 6","pages":"3425–3433 3425–3433"},"PeriodicalIF":5.4,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675756","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}
引用次数: 0
Next-Generation Aluminum-Air Batteries: Integrating New Materials and Technologies for Superior Performance 下一代铝-空气电池:整合新材料和新技术,实现卓越性能
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2025-03-04 DOI: 10.1021/acsaem.4c0292610.1021/acsaem.4c02926
Maham Dilshad, Tao Li, Shern-Long Lee* and Lei Qin*, 
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