ACS Energy Letters 最新文献_第4页

Ti Substitution Strategy Improves Electrochemical Performance of Na3V2(PO4)2F3 Cathode

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-21 DOI: 10.1021/acsenergylett.5c00315

Qingxia Hu, Mengjiao Sun, Yunchun Zha, Guiquan Zhao, Hanlin Tang, Li Yang, Mou Yang, Bohuai Pang, Yongjiang Sun, Hong Guo

{"title":"Ti Substitution Strategy Improves Electrochemical Performance of Na3V2(PO4)2F3 Cathode","authors":"Qingxia Hu, Mengjiao Sun, Yunchun Zha, Guiquan Zhao, Hanlin Tang, Li Yang, Mou Yang, Bohuai Pang, Yongjiang Sun, Hong Guo","doi":"10.1021/acsenergylett.5c00315","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00315","url":null,"abstract":"NASICON-type Na3V2(PO4)2F3 (NVPF) is a promising cathode for sodium-ion batteries (SIBs), but its performance is hindered by Na3V2(PO4)3 (NVP) impurities and intrinsic limitations. To overcome these challenges, Ti-substituted NVPF cathodes are successfully synthesized using the sol–gel method in this study. Theoretical calculations and advanced analyses confirm that substituting Ti ions for V in the NVPF lattice effectively eliminates NVP impurities, mitigates the low-voltage plateau issue, and enhances both electronic conductivity and sodium-ion diffusion kinetics. Hence, the optimized Na3V1.95Ti0.05(PO4)2F3 cathode demonstrated a high initial capacity of 129.10 mAh g–1 at 0.2 C. Notably, it exhibited excellent cycling stability, with capacity retentions of 91.98% after 500 cycles at 5 C and 81.14% after 6000 cycles at 30 C, significantly outperforming the unsubstituted NVPF sample. This study provides a practical new approach for the development of high-performance cathode materials for SIBs and is expected to accelerate the commercialization process of SIBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"183 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672299","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}

引用次数: 0

Elucidating Charge Carrier Solvation in Biredox Eutectic Electrolytes for Nonaqueous Symmetrical Organic Redox Flow Batteries

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-21 DOI: 10.1021/acsenergylett.5c00150

Chengxin Peng, Yunjie Cao, Wanghao Li, Yue Liu, Zhou Zhang, Liang Wang, Wenjing Tang, Ting Yi, Shixue Dou, Yu Zhao

{"title":"Elucidating Charge Carrier Solvation in Biredox Eutectic Electrolytes for Nonaqueous Symmetrical Organic Redox Flow Batteries","authors":"Chengxin Peng, Yunjie Cao, Wanghao Li, Yue Liu, Zhou Zhang, Liang Wang, Wenjing Tang, Ting Yi, Shixue Dou, Yu Zhao","doi":"10.1021/acsenergylett.5c00150","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00150","url":null,"abstract":"Charge carrier solvation is crucial for mass transfer rates and redox kinetics of redox couples in organic redox flow batteries (ORFBs), yet it remains underexplored. This study employs molecular dynamics simulations to investigate charge carrier solvation in biredox eutectic electrolytes (BEEs) under diverse solvent and salt conditions. Results demonstrate that acetonitrile (ACN) molecules preferentially occupy the primary solvation shell of the bis(trifluoromethanesulfonimide) anions (TFSI–) in the catholyte and the tetrabutylammonium cations (TBA+) in the anolyte, forming charge carrier solvation, thus decoupling the molecular interactions within the BEEs and accelerating the redox kinetics in ORFBs. With an optimized ACN-TBATFSI electrolyte, a prototype symmetrical flow cell can achieve a high output voltage of 2.35 V, high material utilization of 93%, and stable cyclability with a capacity retention rate of 99.97% per cycle after 1200 cycles. This work highlights the potential of modulating the charge carrier solvation to enhance the electrochemical performance of ORFBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"15 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672298","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}

引用次数: 0

Bismuth Confined in Thick Nitrogen-Doped Carbon for Durable Low-Temperature Potassium-Ion Batteries

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-19 DOI: 10.1021/acsenergylett.4c03489

Guanghai Chen, Biao Feng, Gengchen Xu, Qinghua Gong, Lijie Yan, Changkai Zhou, Jietao Jiang, Lijun Yang, Qiang Wu, Xizhang Wang, Zheng Hu

{"title":"Bismuth Confined in Thick Nitrogen-Doped Carbon for Durable Low-Temperature Potassium-Ion Batteries","authors":"Guanghai Chen, Biao Feng, Gengchen Xu, Qinghua Gong, Lijie Yan, Changkai Zhou, Jietao Jiang, Lijun Yang, Qiang Wu, Xizhang Wang, Zheng Hu","doi":"10.1021/acsenergylett.4c03489","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03489","url":null,"abstract":"Bismuth is an alloying-type anode for potassium-ion batteries (PIBs) but faces the challenges of large volume expansion and sluggish potassiation/depotassiation kinetics. Herein, a composite of Bi nanoparticles confined in 10 nm-thick nitrogen-doped carbon layer (Bi@NC) exhibits notable rate capability (333 mAh g–1@30 A g–1) and cycling stability (290 mAh g–1@10 A g–1 after 2000 cycles) in K-storage. The high performance of Bi@NC is mainly ascribed to the encapsulation of Bi with thick N-doped carbon and a partial K+-solvent co-intercalation mechanism in the ether-based electrolyte, which enable the formation of a conductive c-K3Bi discharge product and stable solid electrolyte interphase, ensuring loss-free pulverization while avoiding high energy-consuming desolvation, leading to fast charge transfer kinetics even at low temperature. Accordingly, the PIB assembled with the Bi@NC anode and TiS2 cathode exhibits exceptional rate and cycling performance especially at −40 °C. This study provides an advanced Bi@NC anode for PIBs with exceptional low-temperature performance.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"90 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660830","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}

引用次数: 0

Realizing an N-Type Organic Thermoelectric ZT of 0.46

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-19 DOI: 10.1021/acsenergylett.4c03590

Mingyu Ma, Gang Ye, Soyeong Jang, Yazhuo Kuang, Linlong Zhang, Shuyan Shao, L. Jan Anton Koster, Derya Baran, Jian Liu

{"title":"Realizing an N-Type Organic Thermoelectric ZT of 0.46","authors":"Mingyu Ma, Gang Ye, Soyeong Jang, Yazhuo Kuang, Linlong Zhang, Shuyan Shao, L. Jan Anton Koster, Derya Baran, Jian Liu","doi":"10.1021/acsenergylett.4c03590","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03590","url":null,"abstract":"The performance of n-type organic thermoelectric materials is significantly limited by a lack of a deep understanding of the structure–property relationship. In this study, we aim to establish a connection between the molecular structure and the density of states (DOS) profile related to thermoelectric performance. We synthesized three new diketopyrrolopyrrole-based polymers, each functionalized with amphipathic side chains. The only difference among these polymers is the number of sp2-N substitutions. Our findings indicate that as the number of substitutions increases, the DOS profile widens and intensifies, creating new peaks that extend toward the bandgap. This enables more efficient doping and coherent charge transport. Consequently, we achieved a high electrical conductivity of 63.8 S cm–1, a power factor of 111.8 μW m–1 K–2, and a ZT of 0.46, representing a significant advancement in n-type organic thermoelectrics. This work provides valuable guidelines for designing high-performance thermoelectric materials by rationally tailoring the DOS profile.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"70 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143654118","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}

引用次数: 0

Surface Configuration Enables PbSe Quantum Dot Solar Cells with Efficiency beyond 12%

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-18 DOI: 10.1021/acsenergylett.4c03326

Muhammad Irfan Ullah, Xiaobo Ding, Yang Liu, Yuquan Zou, Qura Tul Ain, Lin Yuan, Haotian Gao, Yu Yin, Ihsan Ullah, Guozheng Shi, Xiangqiang Pan, Zeke Liu, Wanli Ma

引用次数: 0

Comparing Intrinsic Catalytic Activity and Practical Performance of Ni- and Pt-Based Alkaline Anion Exchange Membrane Water Electrolyzer Cathodes

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-18 DOI: 10.1021/acsenergylett.5c00439

Advay Shirwalkar, Manjodh Kaur, Sichen Zhong, Max Pupucevski, Keda Hu, Yushan Yan, Judith Lattimer, James McKone

{"title":"Comparing Intrinsic Catalytic Activity and Practical Performance of Ni- and Pt-Based Alkaline Anion Exchange Membrane Water Electrolyzer Cathodes","authors":"Advay Shirwalkar, Manjodh Kaur, Sichen Zhong, Max Pupucevski, Keda Hu, Yushan Yan, Judith Lattimer, James McKone","doi":"10.1021/acsenergylett.5c00439","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00439","url":null,"abstract":"The stringent cost and performance requirements of renewable hydrogen production systems dictate that electrolyzers benefit from the use of nonprecious catalysts only if they deliver the same level of activity and durability as their precious metal counterparts. Here we report on recent work to understand interrelationships between the intrinsic activity of Ni- and Pt-based electrolyzer cathode catalysts and their performance in zero-gap alkaline water electrolyzer assemblies. Our results suggest that nanoparticulate Ni–Mo exhibits HER activity that is roughly 10-fold lower than Pt–Ru on the basis of turnover frequency under low (≤100 mV) polarization conditions. We further found that the HER activity of Ni–Mo/C cathodes is inhibited by aryl piperidinium anion-exchange ionomers bearing bicarbonate counter-anions. After addressing this poisoning effect, we produced electrolyzer assemblies based on Ni–Mo/C cathodes that delivered indistinguishable current density vs cell potential relationships compared to otherwise identical assemblies with Pt–Ru cathodes. This result indicates that the contribution of the cathode to the total cell polarization is small, even for the less active Ni–Mo/C catalyst, and further implies that Pt-based cathodes can indeed be replaced by nonprecious alternatives with no loss in performance.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"95 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640187","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}

引用次数: 0

Achieving Safe and Stable Lithium-Based Batteries via Molecular Dipole Interactions

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-18 DOI: 10.1021/acsenergylett.5c00710

Siru He, Peide Zhu, Zhixin Liu, Lida Wang, Zhitong Li, Yuejiao Chen, Libao Chen, Xingzhu Wang, Baomin Xu

引用次数: 0

A Janus Membrane with Asymmetrical Proton Transport for Cross-Communication Harmony for an Extreme Lean Electrolyte Zn–V Battery

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-18 DOI: 10.1021/acsenergylett.5c00369

Chaozheng Liu, Bo Lin, Zhenglin Li, Chuhang Liu, Yao Wang, Weimin Chen, Wangwang Xu, Mei-Chun Li, Shu Hong, Lei Zhang, Pei Yang, Min Wang, Kangning Zhao, Changtong Mei

{"title":"A Janus Membrane with Asymmetrical Proton Transport for Cross-Communication Harmony for an Extreme Lean Electrolyte Zn–V Battery","authors":"Chaozheng Liu, Bo Lin, Zhenglin Li, Chuhang Liu, Yao Wang, Weimin Chen, Wangwang Xu, Mei-Chun Li, Shu Hong, Lei Zhang, Pei Yang, Min Wang, Kangning Zhao, Changtong Mei","doi":"10.1021/acsenergylett.5c00369","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00369","url":null,"abstract":"The Zn metal anode demands a reduction in water activity and proton concentration to prevent undesirable side reactions, while the V-based cathode necessitates water as a “lubricant” and protons as intercalation guests, presenting a challenge in balancing these needs. Herein, we report a Janus membrane with asymmetrical proton transport for cross-communication harmony in Zn–V batteries, designed to harmonize these contrasting requirements. The MXene-rich phase blocks the proton/water transport through the F-termination site and effectively suppresses dendrite formation through epitaxial growth. Meanwhile, the proton selective cellulose-rich phase (H+/Zn2+ selectivity of over 21) stabilizes the cathode/electrolyte interface by capturing dissolved vanadium and enhancing proton intercalation into the cathode. This designed Janus membrane enables a practical Zn–V full battery at a high depth of discharge of 66.7% and extreme lean electrolyte (1 g/Ah) conditions, enabling the high energy zinc battery (214.8 Wh/kgelectrode). Our approach introduces a sustainable separator for long-lasting, high-performance zinc metal batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"183 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143654121","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}

引用次数: 0

Machine Learning Prediction of Organic–Inorganic Halide Perovskite Solar Cell Performance from Optical Properties

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-17 DOI: 10.1021/acsenergylett.4c03592

Ruiqi Zhang, Brandon Motes, Shaun Tan, Yongli Lu, Meng-Chen Shih, Yilun Hao, Karen Yang, Shreyas Srinivasan, Moungi G. Bawendi, Vladimir Bulović

{"title":"Machine Learning Prediction of Organic–Inorganic Halide Perovskite Solar Cell Performance from Optical Properties","authors":"Ruiqi Zhang, Brandon Motes, Shaun Tan, Yongli Lu, Meng-Chen Shih, Yilun Hao, Karen Yang, Shreyas Srinivasan, Moungi G. Bawendi, Vladimir Bulović","doi":"10.1021/acsenergylett.4c03592","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03592","url":null,"abstract":"Numerical toolsets have the potential to enable accelerated development of hybrid organic–inorganic halide perovskite (HOIP) solar cells. In the present study, we develop a machine learning (ML) approach that accurately predicts the current–voltage behavior of 3D/2D-structured (FAMA)Pb(IBr)3/OABr HOIP solar cells under AM1.5 illumination. Using measured responses from 368 devices, we train a neural network (NN) with three optical inputs of constituent HOIP films (transmission, spectrally resolved photoluminescence, and time-resolved photoluminescence) to predict the solar cell’s open-circuit voltage (Voc), short-circuit current (Jsc), and fill factors (FF). The model achieves 91%, 94%, and 89% accuracy for 95% of Voc, Jsc, and FF predictions, with coefficient of determination (R2) values of 0.47, 0.77, and 0.58, respectively. By linking ML predictions to extracted physical parameters from the measured HOIP films optical properties, we identify key factors influencing the prediction results. Furthermore, we develop separate ML-classification algorithms that identify degraded solar cells with >90% accuracies using the same optical data. This work demonstrates an efficient, nondestructive approach for HOIP solar cell assessment that can assist in accelerating the next generation of perovskite solar cell developments.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"17 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143635388","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}

引用次数: 0

The Crucial Role of Vacancy Concentration in Enabling Superatomic Diffusion in Lithium Intermetallics

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-17 DOI: 10.1021/acsenergylett.5c00266

Sesha Sai Behara, Anton Van der Ven

{"title":"The Crucial Role of Vacancy Concentration in Enabling Superatomic Diffusion in Lithium Intermetallics","authors":"Sesha Sai Behara, Anton Van der Ven","doi":"10.1021/acsenergylett.5c00266","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00266","url":null,"abstract":"Anode-free solid-state Li batteries promise significant increases in energy densities compared to current commercial batteries that rely on liquid electrolytes. Major challenges persist in controlling morphological evolution during the plating and stripping of lithium metal at the anode current collector. Elemental additives that alloy with lithium have been found to modify the plating and stripping behavior of lithium. Many alloying elements form intermetallics with lithium and the mobility of Li through these intermetallics is believed to have an important effect on morphological evolution. This study shows that Li transport coefficients through intermetallics span a wide range in values, with the B32 LiAl intermetallic predicted to have a Li tracer diffusion coefficient as high as 10–6 cm2/s at room temperature, which is 8 orders of magnitude larger than that of isostructural B32 LiZn. This work demonstrates the crucial role of vacancy concentration in controlling the mobility of Li atoms through intermetallics. While the migration barriers for Li-vacancy exchanges in both LiAl and LiZn are remarkably low, the superatomic conductivity in LiAl is shown to arise from the unique electronic structure of the B32 LiAl compound, which favors high concentrations of vacancies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"42 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640138","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}

引用次数: 0