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Self-Passivation at the SnO2/Perovskite Interface
IF 19.3 1区 材料科学
ACS Energy Letters Pub Date : 2025-02-28 DOI: 10.1021/acsenergylett.5c0052110.1021/acsenergylett.5c00521
Kai-Ping Wang, Xue Dong, Ji-Zhe Yuan, Bo Wen, Jun He, Chuan-Jia Tong* and Oleg V. Prezhdo, 
{"title":"Self-Passivation at the SnO2/Perovskite Interface","authors":"Kai-Ping Wang,&nbsp;Xue Dong,&nbsp;Ji-Zhe Yuan,&nbsp;Bo Wen,&nbsp;Jun He,&nbsp;Chuan-Jia Tong* and Oleg V. Prezhdo,&nbsp;","doi":"10.1021/acsenergylett.5c0052110.1021/acsenergylett.5c00521","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00521https://doi.org/10.1021/acsenergylett.5c00521","url":null,"abstract":"<p >Interfaces are crucial to the performance of solar cells, as they significantly affect charge transport. Using density functional theory and nonadiabatic molecular dynamics simulations, we reveal a self-passivation mechanism at the SnO<sub>2</sub>/CH<sub>3</sub>NH<sub>3</sub>PbI<sub>3</sub> interface to enhance the stability and efficiency of the device, which is mainly attributed to a benign iodine vacancy (V<sub>Iact</sub>). Unlike the typical defects of accelerating the charge recombination and reducing efficiency, this distinctive V<sub>Iact</sub> facilitates charge transfer and decelerates nonradiative recombination by passivating the potential trap states. Additionally, the benign V<sub>Iact</sub> at the interface reduces structural distortion and suppresses electron–vibration interactions, which in turn, extends the charge carrier lifetime and enhances the electron injection. Furthermore, V<sub>Iact</sub> exhibits both thermodynamic and kinetics stability. Our findings rationalize the high performance of SnO<sub>2</sub>-based perovskite solar cells and highlight the importance of the defect self-passivation strategy in optimizing interfacial properties for enhanced solar cell efficiency.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 3","pages":"1466–1473 1466–1473"},"PeriodicalIF":19.3,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608803","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
Imaging Phase Boundary Kinetics in Lithium Titanate Using Operando Electron Energy-Loss Spectroscopy
IF 19.3 1区 材料科学
ACS Energy Letters Pub Date : 2025-02-27 DOI: 10.1021/acsenergylett.5c0020910.1021/acsenergylett.5c00209
Yuki Nomura*, Kazuo Yamamoto, Naoaki Kuwata and Tsukasa Hirayama, 
{"title":"Imaging Phase Boundary Kinetics in Lithium Titanate Using Operando Electron Energy-Loss Spectroscopy","authors":"Yuki Nomura*,&nbsp;Kazuo Yamamoto,&nbsp;Naoaki Kuwata and Tsukasa Hirayama,&nbsp;","doi":"10.1021/acsenergylett.5c0020910.1021/acsenergylett.5c00209","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00209https://doi.org/10.1021/acsenergylett.5c00209","url":null,"abstract":"<p >Lithium titanate accommodates and releases lithium ions through phase separation. The dynamics of the phase boundary movement are critical to battery performance, particularly for maximizing the charge/discharge rates. However, details of this boundary movement remain unclear. Here, we visualize the phase boundary movement by tracking the Li distribution using operando scanning transmission electron microscopy coupled with electron energy-loss spectroscopy. For Li insertion, the rate constants of the phase boundary movement were 3.6 ± 0.9 × 10<sup>–13</sup> cm<sup>2</sup>/s at 30 °C and 3.2 ± 0.3 × 10<sup>–11</sup> cm<sup>2</sup>/s at 105 °C, whereas for Li extraction they were 4.0 ± 0.7 × 10<sup>–11</sup> cm<sup>2</sup>/s at 30 °C and 1.9 ± 0.6 × 10<sup>–9</sup> cm<sup>2</sup>/s at 105 °C. The activation energies for Li-ion diffusion were 0.49 and 0.59 eV for Li<sub>4</sub>Ti<sub>5</sub>O<sub>12</sub> and Li<sub>7</sub>Ti<sub>5</sub>O<sub>12</sub>, respectively. The relatively low activation energy of 0.49 eV is the reason lithium titanate exhibits a high-rate discharge performance.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 3","pages":"1404–1410 1404–1410"},"PeriodicalIF":19.3,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143609118","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
Imaging Phase Boundary Kinetics in Lithium Titanate Using Operando Electron Energy-Loss Spectroscopy
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-02-27 DOI: 10.1021/acsenergylett.5c00209
Yuki Nomura, Kazuo Yamamoto, Naoaki Kuwata, Tsukasa Hirayama
{"title":"Imaging Phase Boundary Kinetics in Lithium Titanate Using Operando Electron Energy-Loss Spectroscopy","authors":"Yuki Nomura, Kazuo Yamamoto, Naoaki Kuwata, Tsukasa Hirayama","doi":"10.1021/acsenergylett.5c00209","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00209","url":null,"abstract":"Lithium titanate accommodates and releases lithium ions through phase separation. The dynamics of the phase boundary movement are critical to battery performance, particularly for maximizing the charge/discharge rates. However, details of this boundary movement remain unclear. Here, we visualize the phase boundary movement by tracking the Li distribution using operando scanning transmission electron microscopy coupled with electron energy-loss spectroscopy. For Li insertion, the rate constants of the phase boundary movement were 3.6 ± 0.9 × 10<sup>–13</sup> cm<sup>2</sup>/s at 30 °C and 3.2 ± 0.3 × 10<sup>–11</sup> cm<sup>2</sup>/s at 105 °C, whereas for Li extraction they were 4.0 ± 0.7 × 10<sup>–11</sup> cm<sup>2</sup>/s at 30 °C and 1.9 ± 0.6 × 10<sup>–9</sup> cm<sup>2</sup>/s at 105 °C. The activation energies for Li-ion diffusion were 0.49 and 0.59 eV for Li<sub>4</sub>Ti<sub>5</sub>O<sub>12</sub> and Li<sub>7</sub>Ti<sub>5</sub>O<sub>12</sub>, respectively. The relatively low activation energy of 0.49 eV is the reason lithium titanate exhibits a high-rate discharge performance.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518563","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
Multisite Coordination Ligand Strategy for FAPbBr3 Nanocrystal Light-Emitting Diodes
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-02-27 DOI: 10.1021/acsenergylett.5c00359
Dongryeol Lee, Seung Min Lee, Ah-young Lee, Jongbeom Kim, Jeongjae Lee, Dae Hyeon Kwon, Jongmin Han, Young Wook Noh, Woo Gyeong Shin, Su Seok Choi, Bo Ram Lee, Seungjin Lee, Sang Kyu Kwak, Myoung Hoon Song
{"title":"Multisite Coordination Ligand Strategy for FAPbBr3 Nanocrystal Light-Emitting Diodes","authors":"Dongryeol Lee, Seung Min Lee, Ah-young Lee, Jongbeom Kim, Jeongjae Lee, Dae Hyeon Kwon, Jongmin Han, Young Wook Noh, Woo Gyeong Shin, Su Seok Choi, Bo Ram Lee, Seungjin Lee, Sang Kyu Kwak, Myoung Hoon Song","doi":"10.1021/acsenergylett.5c00359","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00359","url":null,"abstract":"Passivation strategies have been proven to improve the optoelectronic properties of perovskite nanocrystals (PNCs) and to suppress their ion migration; however, previous studies have predominantly focused on their binding affinity to uncoordinated Pb<sup>2+</sup> ions, overlooking additional interactions with monovalent cations. Here, we introduce multisite coordination ligands (composed of multiple fluorine atoms) to achieve additional interactions with formamidinium lead bromide (FAPbBr<sub>3</sub>) PNCs. One fluorine atom passivates an uncoordinated Pb<sup>2+</sup> ion, while the other fluorine atoms form hydrogen bonds with the surrounding FA<sup>+</sup> ions, thereby strongly binding to the PNC surface and suppressing ion migration. This strong passivation enables postsynthetic ligand exchange using polar solvents without compromising the optoelectronic properties of PNCs by protecting them from polar solvents. As a result, we achieve efficient PNC-LEDs with a maximum external quantum efficiency (EQE) of 25.2% at a luminance of 4474 cd m<sup>–2</sup>, maintaining an EQE of over 20% up to approximately 8000 cd m<sup>–2</sup>.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"66 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518566","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
Beyond Flat: Undulated Perovskite Solar Cells on Microscale Si Pyramids by Solution Processing
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-02-27 DOI: 10.1021/acsenergylett.5c00221
Deniz Turkay, Kerem Artuk, Mostafa Othman, Florent Sahli, Lisa Champault, Christophe Allebé, Aïcha Hessler-Wyser, Quentin Jeangros, Christophe Ballif, Christian M. Wolff
{"title":"Beyond Flat: Undulated Perovskite Solar Cells on Microscale Si Pyramids by Solution Processing","authors":"Deniz Turkay, Kerem Artuk, Mostafa Othman, Florent Sahli, Lisa Champault, Christophe Allebé, Aïcha Hessler-Wyser, Quentin Jeangros, Christophe Ballif, Christian M. Wolff","doi":"10.1021/acsenergylett.5c00221","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00221","url":null,"abstract":"Microscale pyramids of silicon solar cells are often considered incompatible with solution-processed perovskite films. Thus, solution processing has mainly been used with submicron pyramids that are buried under thick perovskite films with flattened front surfaces. Yet, while this modification simplifies the fabrication process, it compromises optical performance compared to conformal perovskite films (e.g., obtained by vapor processing). Here, we show that protrusion-free perovskite films can be formed on random pyramids much higher than the film thickness by tailoring the film thickness to match the pyramids’ height profile, notably without modifying the pyramid facets. Accordingly, we demonstrate perovskite cells spin-coated on over 2 μm-high random pyramids with electronic performance comparable to those fabricated on flat substrates, and proof-of-concept perovskite-silicon tandem devices with efficiencies reaching 33%. Finally, we show that the undulated films with enhanced conformality enable optical performance superior to flat surfaces, especially upon encapsulation, most relevant to outdoor applications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"66 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143506886","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
Efficient and Stable Hole-Transport Material for Solar Cells: from PEDOT:PSS to Carbon Nanotubes:PSS
IF 19.3 1区 材料科学
ACS Energy Letters Pub Date : 2025-02-27 DOI: 10.1021/acsenergylett.4c0357510.1021/acsenergylett.4c03575
Yan Zhao, Qing Gao*, Dehua Yang, Xuning Zhang, Jing Guo, Yuke Ren, Xuan Chang, Yiming Xu, Xiaoyang Yuan, Lu Zhang, Kangping Zhang, Jianfang Dai, Beihai Yuan, Chunyang Su, Xin Fang, Dengyuan Song and Jianhui Chen*, 
{"title":"Efficient and Stable Hole-Transport Material for Solar Cells: from PEDOT:PSS to Carbon Nanotubes:PSS","authors":"Yan Zhao,&nbsp;Qing Gao*,&nbsp;Dehua Yang,&nbsp;Xuning Zhang,&nbsp;Jing Guo,&nbsp;Yuke Ren,&nbsp;Xuan Chang,&nbsp;Yiming Xu,&nbsp;Xiaoyang Yuan,&nbsp;Lu Zhang,&nbsp;Kangping Zhang,&nbsp;Jianfang Dai,&nbsp;Beihai Yuan,&nbsp;Chunyang Su,&nbsp;Xin Fang,&nbsp;Dengyuan Song and Jianhui Chen*,&nbsp;","doi":"10.1021/acsenergylett.4c0357510.1021/acsenergylett.4c03575","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03575https://doi.org/10.1021/acsenergylett.4c03575","url":null,"abstract":"<p >Hole transport materials (HTMs) are crucial for achieving high power conversion efficiency (PCE) of solar cells, which has facilitated the development of novel HTMs. In this work, an effective HTM with high conductivity, effective hole-transport, and high stability is fabricated by combining carbon nanotubes (CNT) and PSS. High-dispersive CNT in PSS solution forms a uniformly CNT network without doping, which shows a high conductivity due to carrier highways from the CNT ballistic transport mechanism. The conducting network is not affected by the humidity of the air and enhances the device stability. A synergistic effect of CNT and PSS gives the CNT:PSS composition film a high work function and a full-area passivation contact with Si. Finally, the highest PCE of 23.30% for organic:Si solar cells is achieved with a fill factor (FF) of 84.4%. These data demonstrate that the CNT:PSS film has excellent hole transport characteristics, which can also be applied to other photoelectric devices.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 3","pages":"1439–1447 1439–1447"},"PeriodicalIF":19.3,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143609122","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
Multisite Coordination Ligand Strategy for FAPbBr3 Nanocrystal Light-Emitting Diodes
IF 19.3 1区 材料科学
ACS Energy Letters Pub Date : 2025-02-27 DOI: 10.1021/acsenergylett.5c0035910.1021/acsenergylett.5c00359
Dongryeol Lee, Seung Min Lee, Ah-young Lee, Jongbeom Kim, Jeongjae Lee, Dae Hyeon Kwon, Jongmin Han, Young Wook Noh, Woo Gyeong Shin, Su Seok Choi, Bo Ram Lee, Seungjin Lee*, Sang Kyu Kwak* and Myoung Hoon Song*, 
{"title":"Multisite Coordination Ligand Strategy for FAPbBr3 Nanocrystal Light-Emitting Diodes","authors":"Dongryeol Lee,&nbsp;Seung Min Lee,&nbsp;Ah-young Lee,&nbsp;Jongbeom Kim,&nbsp;Jeongjae Lee,&nbsp;Dae Hyeon Kwon,&nbsp;Jongmin Han,&nbsp;Young Wook Noh,&nbsp;Woo Gyeong Shin,&nbsp;Su Seok Choi,&nbsp;Bo Ram Lee,&nbsp;Seungjin Lee*,&nbsp;Sang Kyu Kwak* and Myoung Hoon Song*,&nbsp;","doi":"10.1021/acsenergylett.5c0035910.1021/acsenergylett.5c00359","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00359https://doi.org/10.1021/acsenergylett.5c00359","url":null,"abstract":"<p >Passivation strategies have been proven to improve the optoelectronic properties of perovskite nanocrystals (PNCs) and to suppress their ion migration; however, previous studies have predominantly focused on their binding affinity to uncoordinated Pb<sup>2+</sup> ions, overlooking additional interactions with monovalent cations. Here, we introduce multisite coordination ligands (composed of multiple fluorine atoms) to achieve additional interactions with formamidinium lead bromide (FAPbBr<sub>3</sub>) PNCs. One fluorine atom passivates an uncoordinated Pb<sup>2+</sup> ion, while the other fluorine atoms form hydrogen bonds with the surrounding FA<sup>+</sup> ions, thereby strongly binding to the PNC surface and suppressing ion migration. This strong passivation enables postsynthetic ligand exchange using polar solvents without compromising the optoelectronic properties of PNCs by protecting them from polar solvents. As a result, we achieve efficient PNC-LEDs with a maximum external quantum efficiency (EQE) of 25.2% at a luminance of 4474 cd m<sup>–2</sup>, maintaining an EQE of over 20% up to approximately 8000 cd m<sup>–2</sup>.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 3","pages":"1411–1420 1411–1420"},"PeriodicalIF":19.3,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608811","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
Aqueous Zn-ORR/CER Battery in Tandem Electrolyte Utilizing Dual-Function Ag Catalyst
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-02-27 DOI: 10.1021/acsenergylett.5c00343
Sukhjot Kaur, Kalpana Garg, Tharamani C. Nagaiah
{"title":"Aqueous Zn-ORR/CER Battery in Tandem Electrolyte Utilizing Dual-Function Ag Catalyst","authors":"Sukhjot Kaur, Kalpana Garg, Tharamani C. Nagaiah","doi":"10.1021/acsenergylett.5c00343","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00343","url":null,"abstract":"Amidst ever-growing energy demands, the development of efficient energy storage devices for carrying out a sustainable electrocatalytic reaction along with energy storage has proven to be viable. In this work, we report a Zn-ORR/CER battery in a tandem electrolyte for the first time, wherein a cost-effective silver (Ag) catalyst was used as a bifunctional electrocatalyst. It exhibits exceptional stability performance in mimicked industrial conditions, even under multiple shutdowns in chlorine-rich electrolytes. Moreover, the local electrocatalytic activity for ORR and the stability of the catalyst in a chlorine-rich electrolyte were probed through scanning electrochemical microscopy (SECM). Interestingly, when employed as a cathode for the Zn-ORR/CER battery (which runs on the electrocatalytic ORR and CER), it displays an open circuit voltage of 1.6 V with outstanding long-term stability for 380 cycles @ 10 mA cm<sup>–2</sup>. The proposed Zn-ORR/CER battery exhibits a power density of 4.84 mW cm<sup>–2</sup> with efficient chlorine production (75%) during charging.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"12 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518564","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
A Low-Strain Lithium Cathode Material Li2–2xFe1+xCl4 for Halide-Based All-Solid-State Batteries
IF 19.3 1区 材料科学
ACS Energy Letters Pub Date : 2025-02-27 DOI: 10.1021/acsenergylett.4c0314710.1021/acsenergylett.4c03147
Dezhao Peng, Rui Li, Kaiqi Xu, Rui Si*, Zhizhen Zhang* and Yong-Sheng Hu*, 
{"title":"A Low-Strain Lithium Cathode Material Li2–2xFe1+xCl4 for Halide-Based All-Solid-State Batteries","authors":"Dezhao Peng,&nbsp;Rui Li,&nbsp;Kaiqi Xu,&nbsp;Rui Si*,&nbsp;Zhizhen Zhang* and Yong-Sheng Hu*,&nbsp;","doi":"10.1021/acsenergylett.4c0314710.1021/acsenergylett.4c03147","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03147https://doi.org/10.1021/acsenergylett.4c03147","url":null,"abstract":"<p >Halide electrolytes are of particular interest due to their high ionic conductivity and ductile nature. However, halide-electrolyte-based all-solid-state batteries (ASSBs) are subject to degradation when conventional layer oxide cathodes are used. Herein we report a class of halide cathode materials, Li<sub>2–2<i>x</i></sub>Fe<sub>1+<i>x</i></sub>Cl<sub>4</sub> (0 ≤ <i>x</i> ≤ 1/3). Among this series, Li<sub>2</sub>FeCl<sub>4</sub> experiences no phase changes upon the (de)lithiation process, contributing to exceptionally high reversibility and stable cycling. ASSBs utilizing Li<sub>2</sub>FeCl<sub>4</sub> as the cathode demonstrate good rate performance (122.4 mAh g<sup>–1</sup> at 0.2C rate and 91.4 mAh g<sup>–1</sup> at 10C rate) and cycling stability (i.e., a capacity retention of 85.1% is maintained upon 5000 cycles at 10C rate). By optimizing the Li/Fe ratio in Li<sub>2–2<i>x</i></sub>Fe<sub>1+<i>x</i></sub>Cl<sub>4</sub>, a maximum lithium storage capacity of 155.2 mAh g<sup>–1</sup> was achieved with Li<sub>4/3</sub>Fe<sub>4/3</sub>Cl<sub>4</sub>, which is comparable to that of a commercial LiFePO<sub>4</sub> cathode. This study proves the advantage of halide cathode materials in halide-based ASSBs.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 3","pages":"1421–1429 1421–1429"},"PeriodicalIF":19.3,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608978","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
A Low-Strain Lithium Cathode Material Li2–2xFe1+xCl4 for Halide-Based All-Solid-State Batteries
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-02-27 DOI: 10.1021/acsenergylett.4c03147
Dezhao Peng, Rui Li, Kaiqi Xu, Rui Si, Zhizhen Zhang, Yong-Sheng Hu
{"title":"A Low-Strain Lithium Cathode Material Li2–2xFe1+xCl4 for Halide-Based All-Solid-State Batteries","authors":"Dezhao Peng, Rui Li, Kaiqi Xu, Rui Si, Zhizhen Zhang, Yong-Sheng Hu","doi":"10.1021/acsenergylett.4c03147","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03147","url":null,"abstract":"Halide electrolytes are of particular interest due to their high ionic conductivity and ductile nature. However, halide-electrolyte-based all-solid-state batteries (ASSBs) are subject to degradation when conventional layer oxide cathodes are used. Herein we report a class of halide cathode materials, Li<sub>2–2<i>x</i></sub>Fe<sub>1+<i>x</i></sub>Cl<sub>4</sub> (0 ≤ <i>x</i> ≤ 1/3). Among this series, Li<sub>2</sub>FeCl<sub>4</sub> experiences no phase changes upon the (de)lithiation process, contributing to exceptionally high reversibility and stable cycling. ASSBs utilizing Li<sub>2</sub>FeCl<sub>4</sub> as the cathode demonstrate good rate performance (122.4 mAh g<sup>–1</sup> at 0.2C rate and 91.4 mAh g<sup>–1</sup> at 10C rate) and cycling stability (i.e., a capacity retention of 85.1% is maintained upon 5000 cycles at 10C rate). By optimizing the Li/Fe ratio in Li<sub>2–2<i>x</i></sub>Fe<sub>1+<i>x</i></sub>Cl<sub>4</sub>, a maximum lithium storage capacity of 155.2 mAh g<sup>–1</sup> was achieved with Li<sub>4/3</sub>Fe<sub>4/3</sub>Cl<sub>4</sub>, which is comparable to that of a commercial LiFePO<sub>4</sub> cathode. This study proves the advantage of halide cathode materials in halide-based ASSBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"31 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518561","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
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