Pub Date : 2025-01-17DOI: 10.1016/j.ensm.2025.104041
Su Hwan Jeong, In-Kyung Kim, Suyoon Eom, Hwiryeong Hwang, Young Hwa Jung, Joo-Hyung Kim
Sodium-ion batteries (SIBs) are considered promising alternatives to lithium-ion batteries (LIBs) for large-scale applications. Layered transition metal oxides are mainly used as cathode materials to enhance energy density and electrochemical performances. In this study, we compare Mn-based P2-type Na0.7Ni0.2Co0.2Mn0.6O2 (NCM) with partially Fe-substituted Na0.7Ni0.2Co0.2Mn0.5Fe0.1O2 (NCMF) via facile solid-state synthesis. Interestingly, Fe-substitution improves not only structural stability but also Na+ diffusion kinetics. It is found that the P2-O2 phase transition at high voltage region is mitigated with smaller volume change and enhanced oxygen redox reaction as demonstrated by in-situ X-ray diffraction and ex-situ X-ray photoelectron spectroscopy. In addition, density functional theory calculations exhibit that NCMF expedites Na+ diffusion and reduces the site energy difference between Naf and Nae by decreasing Na occupancy in the Naf site, which is located right below the transition metal ions. As a result, the NCMF electrode delivers a high initial energy density of 601.5 Wh kg-1 with an average discharge voltage of 3.05 V (V vs. Na+/Na). It also shows a high discharge capacity of 168.15 mAh g-1 at 0.5 C with excellent capacity retention of 68.7% after 100 cycles within a wide voltage range of 1.5-4.5 V. These findings provide a significant impact of Na site occupancy difference for improving electrochemical performance and structural stability as a rational method for the commercialization of SIBs.
{"title":"Engineering the Local Chemistry through Fe Substitution in Layered P2-Na0.7Ni0.2Co0.2Mn0.6O2 for High-Performance Sodium-Ion Batteries","authors":"Su Hwan Jeong, In-Kyung Kim, Suyoon Eom, Hwiryeong Hwang, Young Hwa Jung, Joo-Hyung Kim","doi":"10.1016/j.ensm.2025.104041","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104041","url":null,"abstract":"Sodium-ion batteries (SIBs) are considered promising alternatives to lithium-ion batteries (LIBs) for large-scale applications. Layered transition metal oxides are mainly used as cathode materials to enhance energy density and electrochemical performances. In this study, we compare Mn-based P2-type Na<sub>0.7</sub>Ni<sub>0.2</sub>Co<sub>0.2</sub>Mn<sub>0.6</sub>O<sub>2</sub> (NCM) with partially Fe-substituted Na<sub>0.7</sub>Ni<sub>0.2</sub>Co<sub>0.2</sub>Mn<sub>0.5</sub>Fe<sub>0.1</sub>O<sub>2</sub> (NCMF) via facile solid-state synthesis. Interestingly, Fe-substitution improves not only structural stability but also Na<sup>+</sup> diffusion kinetics. It is found that the P2-O2 phase transition at high voltage region is mitigated with smaller volume change and enhanced oxygen redox reaction as demonstrated by in-situ X-ray diffraction and ex-situ X-ray photoelectron spectroscopy. In addition, density functional theory calculations exhibit that NCMF expedites Na<sup>+</sup> diffusion and reduces the site energy difference between Na<sub>f</sub> and Na<sub>e</sub> by decreasing Na occupancy in the Na<sub>f</sub> site, which is located right below the transition metal ions. As a result, the NCMF electrode delivers a high initial energy density of 601.5 Wh kg<sup>-1</sup> with an average discharge voltage of 3.05 V (V vs. Na<sup>+</sup>/Na). It also shows a high discharge capacity of 168.15 mAh g<sup>-1</sup> at 0.5 C with excellent capacity retention of 68.7% after 100 cycles within a wide voltage range of 1.5-4.5 V. These findings provide a significant impact of Na site occupancy difference for improving electrochemical performance and structural stability as a rational method for the commercialization of SIBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"2 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987482","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}
This paper provides sustainable solutions for the urban mining of end-of-life (EOL) batteries and highlights their significant role in advancing the circular economy. Influenced by geopolitics and investment strategies, establishing a sustainable supply chain can create cost-saving opportunities while meeting the rising demand for battery materials. Urban mining, by recycling valuable metals from EOL batteries, can considerably reduce reliance on new raw materials by providing sustainable resources, thereby facilitating a cleaner energy transition. The research also emphasizes the importance of traceability and emerging innovations, such as the battery passport, which enhance transparency in the supply chain. Additionally, it explores the recycling industry's potential through techno-economic assessments to improve lithium-ion battery (LIB) recycling. Despite the challenges faced by different segments of the battery value chain, commercialization and technological advancements present promising opportunities for future development. The emergence of new battery systems or chemistries, such as sodium-ion, solid-state, and lithium-iron-phosphate batteries, must be considered in the further adaptation of existing plants. In conclusion, this paper discusses how the circular economy and urban mining can drive a sustainable, profitable, and resilient future for the LIB industry, ensuring an efficient and environmentally sound approach to the battery revolution.
{"title":"Advancing the Circular Economy by Driving Sustainable Urban Mining of End-of-Life Batteries and Technological Advancements","authors":"Mina Rezaei, Atiyeh Nekahi, Ebrahim Feyzi, Anil Kumar MR, Jagjit Nanda, Karim Zaghib","doi":"10.1016/j.ensm.2025.104035","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104035","url":null,"abstract":"This paper provides sustainable solutions for the urban mining of end-of-life (EOL) batteries and highlights their significant role in advancing the circular economy. Influenced by geopolitics and investment strategies, establishing a sustainable supply chain can create cost-saving opportunities while meeting the rising demand for battery materials. Urban mining, by recycling valuable metals from EOL batteries, can considerably reduce reliance on new raw materials by providing sustainable resources, thereby facilitating a cleaner energy transition. The research also emphasizes the importance of traceability and emerging innovations, such as the battery passport, which enhance transparency in the supply chain. Additionally, it explores the recycling industry's potential through techno-economic assessments to improve lithium-ion battery (LIB) recycling. Despite the challenges faced by different segments of the battery value chain, commercialization and technological advancements present promising opportunities for future development. The emergence of new battery systems or chemistries, such as sodium-ion, solid-state, and lithium-iron-phosphate batteries, must be considered in the further adaptation of existing plants. In conclusion, this paper discusses how the circular economy and urban mining can drive a sustainable, profitable, and resilient future for the LIB industry, ensuring an efficient and environmentally sound approach to the battery revolution.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"8 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142987481","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}
Enhancing the performance of hybrid lithium-ion capacitors (HLICs) by regulating the structural characteristics of covalent organic frameworks (COFs) has been a challenge. In this study, electron-rich thiophene units combining with the electroactive tetrathiafulvalene (TTF) motif consists the designable organic linker, tetrathiafulvalene tetrathiophenal (TTFTTA). A novel 2D COF, TTFTTA-PDA (PDA, p-phenylenediamine), was assembled via a solvothermal method. TTFTTA-PDA exhibits reversible redox activity, a large Brunauer−Emmett−Teller surface area (457 m2 g−1) and high stability (pH 3∼14). Furthermore, compared to the reported tetrathiafulvalene-tetrabenzaldehyde (TTFTBA)-based COF, TTFTBA-PDA, the introduction of thiophene rings enhances the capability of electron transfer, characterized by a smaller band gap (1.45 eV) and a lower calculated energy gap (0.89 eV). As a result, the electrochemical performance of TTFTTA-PDA in HLICs is outstanding. In the full-cell configurations, TTFTTA-PDA||activated carbon HLICs exhibit impressive energy density (140 Wh kg−1 at 233 W kg−1), power density (9328 W kg−1 at 91 Wh kg−1), and cycling lifespan (the capacity retention of 81.3% after 2200 cycles), demonstrating a certain level of competitiveness among the reported state-of-the-art HLICs utilizing metal organic framework-/COF-based anode materials. These results illustrate that the precise structural design of pristine COFs can be an effective strategy to enhancing the performance of HLICs.
{"title":"Electroactive Tetrathiafulvalene-Based Covalent Organic Framework with Thiophene Units as Anode for High-Performance Hybrid Lithium-Ion Capacitors","authors":"Zhi-Mei Yang, Yaoda Wang, Meng-Hang Zhang, Zhe-Yuan Hou, Shu-Peng Zhao, Xiao Han, Shuai Yuan, Jian Su, Zhong Jin, Jing-Lin Zuo","doi":"10.1016/j.ensm.2025.104038","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104038","url":null,"abstract":"Enhancing the performance of hybrid lithium-ion capacitors (HLICs) by regulating the structural characteristics of covalent organic frameworks (COFs) has been a challenge. In this study, electron-rich thiophene units combining with the electroactive tetrathiafulvalene (TTF) motif consists the designable organic linker, tetrathiafulvalene tetrathiophenal (TTFTTA). A novel 2D COF, TTFTTA-PDA (PDA, <em>p</em>-phenylenediamine), was assembled via a solvothermal method. TTFTTA-PDA exhibits reversible redox activity, a large Brunauer−Emmett−Teller surface area (457 m<sup>2</sup> g<sup>−1</sup>) and high stability (pH 3∼14). Furthermore, compared to the reported tetrathiafulvalene-tetrabenzaldehyde (TTFTBA)-based COF, TTFTBA-PDA, the introduction of thiophene rings enhances the capability of electron transfer, characterized by a smaller band gap (1.45 eV) and a lower calculated energy gap (0.89 eV). As a result, the electrochemical performance of TTFTTA-PDA in HLICs is outstanding. In the full-cell configurations, TTFTTA-PDA||activated carbon HLICs exhibit impressive energy density (140 Wh kg<sup>−1</sup> at 233 W kg<sup>−1</sup>), power density (9328 W kg<sup>−1</sup> at 91 Wh kg<sup>−1</sup>), and cycling lifespan (the capacity retention of 81.3% after 2200 cycles), demonstrating a certain level of competitiveness among the reported state-of-the-art HLICs utilizing metal organic framework-/COF-based anode materials. These results illustrate that the precise structural design of pristine COFs can be an effective strategy to enhancing the performance of HLICs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"45 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142986942","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}
The uniform plating on zinc metal anode (ZMA) is imperative for stable aqueous zinc-ion batteries (AZIBs). However, the sluggish desolvation of hydrated Zn2+ is identified as the primary source of kinetic barriers in plating process, leading to dendrite growth and parasitic reaction. Herein, we introduce chitosan oligosaccharide (COS) as an interfacial hydrogen bond network constructor on ZMA surface to enhance the desolvation kinetics of hydrated Zn2+. Specifically, COS molecules preferentially adsorb on the ZMA surface, where desolvated H2O from plating process can be immobilized by the multiple hydroxyl groups of COS. In addition, COS molecules capture hydrated Zn2+ through their amino groups, resulting in superior Zn2+ transport capability. Consequently, the introduction of COS into Zn(OTF)2 electrolyte enables a lower nucleation overpotential (358 mV) and activation energy (32.34 kJ mol-1) for plating. Such advantages further enable Zn||Zn symmetric battery to achieve a cycle life exceeding 1800 hours, Zn||Cu battery to realize a high Coulombic efficiency of 99.68%, and Zn||ZnxV2O5 full battery to reach a considerable capacity retention of 83.56% over 1000 cycles. The application of interfacial hydrogen bond network provides a novel perspective for optimizing the desolvation of Zn2+ plating on ZMAs.
{"title":"Regulation of Zn2+ Desolvation Kinetics via Interfacial Hydrogen-Bond Network for a Highly Reversible Zn Metal Anode","authors":"Qi Yang, Li Guo, Zhenjie Liu, Jingyuan Wang, Haihan Luo, Xiaofeng Zhang, Qizhi He, Xueyi Chen, Meilin Li, Zihan Wang, Yue Jiang, Rongfeng Yuan, Zhuoxin Liu, Kai Zhang, Zhe Hu, Yang Huang","doi":"10.1016/j.ensm.2025.104028","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104028","url":null,"abstract":"The uniform plating on zinc metal anode (ZMA) is imperative for stable aqueous zinc-ion batteries (AZIBs). However, the sluggish desolvation of hydrated Zn<sup>2+</sup> is identified as the primary source of kinetic barriers in plating process, leading to dendrite growth and parasitic reaction. Herein, we introduce chitosan oligosaccharide (COS) as an interfacial hydrogen bond network constructor on ZMA surface to enhance the desolvation kinetics of hydrated Zn<sup>2+</sup>. Specifically, COS molecules preferentially adsorb on the ZMA surface, where desolvated H<sub>2</sub>O from plating process can be immobilized by the multiple hydroxyl groups of COS. In addition, COS molecules capture hydrated Zn<sup>2+</sup> through their amino groups, resulting in superior Zn<sup>2+</sup> transport capability. Consequently, the introduction of COS into Zn(OTF)<sub>2</sub> electrolyte enables a lower nucleation overpotential (358 mV) and activation energy (32.34 kJ mol<sup>-1</sup>) for plating. Such advantages further enable Zn||Zn symmetric battery to achieve a cycle life exceeding 1800 hours, Zn||Cu battery to realize a high Coulombic efficiency of 99.68%, and Zn||Zn<sub>x</sub>V<sub>2</sub>O<sub>5</sub> full battery to reach a considerable capacity retention of 83.56% over 1000 cycles. The application of interfacial hydrogen bond network provides a novel perspective for optimizing the desolvation of Zn<sup>2+</sup> plating on ZMAs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"26 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981650","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}
Pub Date : 2025-01-14DOI: 10.1016/j.ensm.2025.104040
Jong Hui Choi, Hoje Chun, Dong Won Kim, Mrinal Kanti Kabiraz, Jeonghyeon Kim, Jihoon Kim, Keon-Han Kim, Benzhi Wang, Hyung Mo Jeong, Sang-Il Choi, Byungchan Han, Jeung Ku Kang
Zn-air batteries (ZABs) are promising electrochemical energy storages for many applications, yet their performance is limited by their cathode's poor activity and reversibility for oxygen evolution reaction (OER) in charge and oxygen reduction reaction (ORR) in discharge. Herein, we report a bifunctional CoO-Mn3O4 heterostructure (CMH) cathode synthesized from an Mn-doped zeolitic imidazolate framework as a solution to these challenges. Combined machine learning-augmented density functional theory simulations and operando differential electrochemical mass spectrometry with 18O isotope labeling reveal dynamic O-vacancy (Ov) formation through OH- desorption from Mn sites during ORR or bidentate oxygen adsorption at Mn-Mn sites during OER, with dynamic Ov healing through OH- adsorption and deprotonation. This dynamic process lowers O* binding energy to activate the lattice oxidation mechanism for efficient OER/ORR, exhibited by record-low overpotential and stable operation over 2000 cycles for OER and a diffusion-limited current density of 7.1 mA·cm-2 surpassing Pt/C (5.0 mA cm-2) for ORR. Moreover, the ZAB with the CMH cathode benefits from an ideal open-circuit voltage (1.43 V) and a high capacity of 802 mAh·g-1 (97.8 % of theoretical), to achieve its record-high energy density (898 Wh·kg-1), ultrahigh peak-power density (394.2 mW·cm-2), and stability with negligible voltage degradation over 600 cycles.
{"title":"Zeolitic Imidazolate Framework-Derived Bifunctional CoO-Mn3O4 Heterostructure Cathode Enhancing Oxygen Reduction/Evolution via Dynamic O-Vacancy Formation and Healing for High-Performance Zn-Air Batteries","authors":"Jong Hui Choi, Hoje Chun, Dong Won Kim, Mrinal Kanti Kabiraz, Jeonghyeon Kim, Jihoon Kim, Keon-Han Kim, Benzhi Wang, Hyung Mo Jeong, Sang-Il Choi, Byungchan Han, Jeung Ku Kang","doi":"10.1016/j.ensm.2025.104040","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104040","url":null,"abstract":"Zn-air batteries (ZABs) are promising electrochemical energy storages for many applications, yet their performance is limited by their cathode's poor activity and reversibility for oxygen evolution reaction (OER) in charge and oxygen reduction reaction (ORR) in discharge. Herein, we report a bifunctional CoO-Mn<sub>3</sub>O<sub>4</sub> heterostructure (CMH) cathode synthesized from an Mn-doped zeolitic imidazolate framework as a solution to these challenges. Combined machine learning-augmented density functional theory simulations and <em>operando</em> differential electrochemical mass spectrometry with <sup>18</sup>O isotope labeling reveal dynamic O-vacancy (O<sub>v</sub>) formation through OH<sup>-</sup> desorption from Mn sites during ORR or bidentate oxygen adsorption at Mn-Mn sites during OER, with dynamic O<sub>v</sub> healing through OH<sup>-</sup> adsorption and deprotonation. This dynamic process lowers O* binding energy to activate the lattice oxidation mechanism for efficient OER/ORR, exhibited by record-low overpotential and stable operation over 2000 cycles for OER and a diffusion-limited current density of 7.1 mA·cm<sup>-2</sup> surpassing Pt/C (5.0 mA cm<sup>-2</sup>) for ORR. Moreover, the ZAB with the CMH cathode benefits from an ideal open-circuit voltage (1.43 V) and a high capacity of 802 mAh·g<sup>-1</sup> (97.8 % of theoretical), to achieve its record-high energy density (898 Wh·kg<sup>-1</sup>), ultrahigh peak-power density (394.2 mW·cm<sup>-2</sup>), and stability with negligible voltage degradation over 600 cycles.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"20 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142974893","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}
Pub Date : 2025-01-14DOI: 10.1016/j.ensm.2025.104039
Dan Xie, Fang-Yu Tao, Li-Han Zhu, Han-Hao Liu, Chang Liu, Jia-Wei Wang, Hong Yu, Godefroid Gahungud, Xing-Long Wu, Jing-Ping Zhang
The charge transfer kinetics of Zn plating/stripping and the parasitic reactions are affected by the adsorption of Zn2+ and the subsequent desolvation process proceeded at the electrode/electrolyte interface (EEI). Herein, this work cleverly utilizes the “chain effect” triggered by the L-Methionine (Met) molecules to improving the stability of EEI by the solvation chemistry and interfacial microstructure reconfiguration. Firstly, the introduction of Met molecules enhances the solvation ability of anions, which squeezes out solvated H2O molecules and generate anion-derived hybrid solid electrolyte interphase (SEI) layer, weakening H2O-induced parasitic reactions and expediting the migration rate of Zn2+ at EEI. Meanwhile, the strengthened anion-cation interaction quickens the desolvation kinetics of Zn2+, homogenizing Zn2+ flux at interface. Secondly, Met molecules with multiple active sites not only break the original H-bonds network between H2O molecules, further reducing the reactivity of H2O molecules, but also preferentially adsorb on the Zn(101) and Zn(110) crystal planes to increase the exposure of Zn(002) crystal face, improving the stability of SEI and inducing uniform Zn deposition. Consequently, the symmetric/asymmetric cell in the Met-containing electrolyte demonstrates a long cycling life over 2700 h and high reversibility up to 4500 cycles, respectively. And the assembled full cells and pouch-cell exhibit outstanding cycling performance.
{"title":"Chain Effect-controlled Solvation Chemistry and Interfacial Microstructure Enables Highly Reversible Zn Metal Anode","authors":"Dan Xie, Fang-Yu Tao, Li-Han Zhu, Han-Hao Liu, Chang Liu, Jia-Wei Wang, Hong Yu, Godefroid Gahungud, Xing-Long Wu, Jing-Ping Zhang","doi":"10.1016/j.ensm.2025.104039","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104039","url":null,"abstract":"The charge transfer kinetics of Zn plating/stripping and the parasitic reactions are affected by the adsorption of Zn<sup>2+</sup> and the subsequent desolvation process proceeded at the electrode/electrolyte interface (EEI). Herein, this work cleverly utilizes the “chain effect” triggered by the L-Methionine (Met) molecules to improving the stability of EEI by the solvation chemistry and interfacial microstructure reconfiguration. Firstly, the introduction of Met molecules enhances the solvation ability of anions, which squeezes out solvated H<sub>2</sub>O molecules and generate anion-derived hybrid solid electrolyte interphase (SEI) layer, weakening H<sub>2</sub>O-induced parasitic reactions and expediting the migration rate of Zn<sup>2+</sup> at EEI. Meanwhile, the strengthened anion-cation interaction quickens the desolvation kinetics of Zn<sup>2+</sup>, homogenizing Zn<sup>2+</sup> flux at interface. Secondly, Met molecules with multiple active sites not only break the original H-bonds network between H<sub>2</sub>O molecules, further reducing the reactivity of H<sub>2</sub>O molecules, but also preferentially adsorb on the Zn<sub>(101)</sub> and Zn<sub>(110)</sub> crystal planes to increase the exposure of Zn<sub>(002)</sub> crystal face, improving the stability of SEI and inducing uniform Zn deposition. Consequently, the symmetric/asymmetric cell in the Met-containing electrolyte demonstrates a long cycling life over 2700 h and high reversibility up to 4500 cycles, respectively. And the assembled full cells and pouch-cell exhibit outstanding cycling performance.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"51 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142974894","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}
Pub Date : 2025-01-13DOI: 10.1016/j.ensm.2025.104037
Jingxin He, Shuaishuai Yang, Xiong Xiao, Debao Fang, Runqing Miao, Chengzhi Wang, Lai Chen, Ning Li, Jingbo Li, Yuefeng Su, Haibo Jin
High-performance solid electrolytes with high conductivity and good electrode compatibility are critical for the operable solid-state sodium metal batteries. With the Na+ superionic conductor-typed Na3Zr2Si2PO12 as a matrix, an aliovalent cation substitution strategy using Ni2+, Mn3+, Nb5+, Mo6+ substituting Zr4+ is investigated on the ionic conductivity and interfacial performance of solid-state sodium metal batteries. The low-valence Ni2+ and Mn3+ show notable effect on both enlarging the bottlenecks in the grain lattices and reducing the barriers across the grain boundaries for Na+ migration, while the high-valence Nb5+ and Mo6+ mainly facilitate Na+ migration across the grain boundaries. By tuning the doping ratios, the Ni2+ doped Na3.4Zr1.8Ni0.2Si2PO12 achieves the optimal total conductivity of 2.284 mS cm-1 at 30 °C which is 6 times higher than the undoped Na3Zr2Si2PO12. Moreover, the aliovalent cation substitution essentially improves the interface compatibility with the sodium metal, achieving reduced interfacial resistances as low as 7.80 ohm cm2 and enlarged critical current densities as high as 1.0 mA cm-2. Besides, stable charge/discharge cycles at high rates for both the symmetric Na||Na cells over 3400 h and the full cells over 2400 cycles are achieved to signify the practical merits of the neat aliovalent cation substitution strategy.
{"title":"Aliovalent Cation Substitution in Na3Zr2Si2PO12 for Practical Solid-State Sodium Metal Batteries","authors":"Jingxin He, Shuaishuai Yang, Xiong Xiao, Debao Fang, Runqing Miao, Chengzhi Wang, Lai Chen, Ning Li, Jingbo Li, Yuefeng Su, Haibo Jin","doi":"10.1016/j.ensm.2025.104037","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104037","url":null,"abstract":"High-performance solid electrolytes with high conductivity and good electrode compatibility are critical for the operable solid-state sodium metal batteries. With the Na<sup>+</sup> superionic conductor-typed Na<sub>3</sub>Zr<sub>2</sub>Si<sub>2</sub>PO<sub>12</sub> as a matrix, an aliovalent cation substitution strategy using Ni<sup>2+</sup>, Mn<sup>3+</sup>, Nb<sup>5+</sup>, Mo<sup>6+</sup> substituting Zr<sup>4+</sup> is investigated on the ionic conductivity and interfacial performance of solid-state sodium metal batteries. The low-valence Ni<sup>2+</sup> and Mn<sup>3+</sup> show notable effect on both enlarging the bottlenecks in the grain lattices and reducing the barriers across the grain boundaries for Na<sup>+</sup> migration, while the high-valence Nb<sup>5+</sup> and Mo<sup>6+</sup> mainly facilitate Na<sup>+</sup> migration across the grain boundaries. By tuning the doping ratios, the Ni<sup>2+</sup> doped Na<sub>3.4</sub>Zr<sub>1.8</sub>Ni<sub>0.2</sub>Si<sub>2</sub>PO<sub>12</sub> achieves the optimal total conductivity of 2.284 mS cm<sup>-1</sup> at 30 °C which is 6 times higher than the undoped Na<sub>3</sub>Zr<sub>2</sub>Si<sub>2</sub>PO<sub>12</sub>. Moreover, the aliovalent cation substitution essentially improves the interface compatibility with the sodium metal, achieving reduced interfacial resistances as low as 7.80 ohm cm<sup>2</sup> and enlarged critical current densities as high as 1.0 mA cm<sup>-2</sup>. Besides, stable charge/discharge cycles at high rates for both the symmetric Na||Na cells over 3400 h and the full cells over 2400 cycles are achieved to signify the practical merits of the neat aliovalent cation substitution strategy.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"17 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142974895","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}
Color-to-color switching electrochromic polymers with a high contrast ratio and the additional ability to store energy are attractive for applications in smart display devices and energy recycling and reuse. However, developing materials that combine both optimized electrochromic and energy storage performances remains a significant challenge. To address the integration of polymer color switching and energy storage, the synthesis of a donor-acceptor-donor (D-A-D) triarylamine (TAA)-based diamine monomer with the benzothiadiazole unit as the acceptor unit and using heteroatom as ion adsorption sites is here detailed. The electroactive polyimide enabling energy storage with a visual display of the state of charge (SoC) is subsequently prepared by polycondensation of the diamine monomer with 1,2,4,5-cyclohexanetetracarboxylic acid dianhydride. The final polyimide film electrode exhibits 90% optical contrast, provides a capacitance of 304.5 F g−1 at a current density of 1 A g−1, and enables SoC monitoring through multiple color changes. Besides, we further demonstrate here that symmetric quasi-solid-state electrochromic supercapacitors constructed with a polyimide film as functional layers also exhibit excellent optical contrasts above 60% and high capacitance for energy recovery and reuse in practical applications. Additionally, the ion adsorption energy and the density of states of polyimide are calculated using density functional theory to gain insight into the energy storage mechanism. Overall, we demonstrate and rationalize here the effectiveness in color switching, energy storage, and integrated SoC displaying of triarylamine-based monomers that use electron-withdrawing conjugated heterocycles as bridges along with the corresponding polyimides.
{"title":"Triarylamine-based polyimides enable smart electrochromic displays with energy storage","authors":"Dongxu Li, Yiping Xu, Juguo Dai, Hucheng Fu, Xiaohong Wang, Yiting Xu, Qiaoyun Qin, Andreu Cabot, Lizong Dai","doi":"10.1016/j.ensm.2025.104036","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104036","url":null,"abstract":"Color-to-color switching electrochromic polymers with a high contrast ratio and the additional ability to store energy are attractive for applications in smart display devices and energy recycling and reuse. However, developing materials that combine both optimized electrochromic and energy storage performances remains a significant challenge. To address the integration of polymer color switching and energy storage, the synthesis of a donor-acceptor-donor (D-A-D) triarylamine (TAA)-based diamine monomer with the benzothiadiazole unit as the acceptor unit and using heteroatom as ion adsorption sites is here detailed. The electroactive polyimide enabling energy storage with a visual display of the state of charge (SoC) is subsequently prepared by polycondensation of the diamine monomer with 1,2,4,5-cyclohexanetetracarboxylic acid dianhydride. The final polyimide film electrode exhibits 90% optical contrast, provides a capacitance of 304.5 F g<sup>−1</sup> at a current density of 1 A g<sup>−1</sup>, and enables SoC monitoring through multiple color changes. Besides, we further demonstrate here that symmetric quasi-solid-state electrochromic supercapacitors constructed with a polyimide film as functional layers also exhibit excellent optical contrasts above 60% and high capacitance for energy recovery and reuse in practical applications. Additionally, the ion adsorption energy and the density of states of polyimide are calculated using density functional theory to gain insight into the energy storage mechanism. Overall, we demonstrate and rationalize here the effectiveness in color switching, energy storage, and integrated SoC displaying of triarylamine-based monomers that use electron-withdrawing conjugated heterocycles as bridges along with the corresponding polyimides.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"15 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142967952","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}
The rapid advancement of renewable energy technologies has intensified the demand for high-performance energy storage systems. Metal-O2 (air) batteries, specifically Li-O2 (air) and Zn-O2 (air) variants, present exceptional theoretical energy densities, positioning them as promising candidates for next-generation storage solutions. However, significant challenges remain in optimizing the oxygen reduction and evolution reactions (ORR/OER), critical for achieving high efficiency and stability. Recent developments in light-assisted metal-O2 (air) battery designs leverage photonic energy to enhance oxygen reduction and evolution reactions, offering reduced charge voltages, improved round-trip efficiencies, and extended lifetimes. This review critically evaluates the breakthroughs and limitations in photo-assisted Li/Zn-O2 (air) battery technologies, with a focus on novel photocathode materials, including advanced semiconductors, heterojunction configurations, and nanostructured catalysts. We systematically highlight the key properties of these photocathode materials, evaluating their photon-utilization efficiency, charge separation capabilities, recombination rates, charging/discharging profiles, efficient decomposition of discharge products and stability under operational conditions. Emphasis is placed on advanced strategies to enhance light absorption, aiming to optimize photocatalytic efficiency, electronic properties, and catalytic stability, thereby overcoming current performance barriers. By providing a comprehensive analysis of the current landscape and emerging trends, this review aims to chart a path forward for the development of more robust, efficient, and sustainable light-assisted Li/Zn-O2 (air) batteries, highlighting the essential role of innovative photocathode materials in achieving next-generation energy storage solutions.
{"title":"Light-Driven Photocathodes in Li/Zn-O2 (air) Batteries: An Analytical Review, Technological Breakthroughs and Future Challenges","authors":"Md Iftekher Hossain, Foysal Kabir Tareq, Souman Rudra","doi":"10.1016/j.ensm.2025.104025","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104025","url":null,"abstract":"The rapid advancement of renewable energy technologies has intensified the demand for high-performance energy storage systems. Metal-O<sub>2</sub> (air) batteries, specifically Li-O<sub>2</sub> (air) and Zn-O<sub>2</sub> (air) variants, present exceptional theoretical energy densities, positioning them as promising candidates for next-generation storage solutions. However, significant challenges remain in optimizing the oxygen reduction and evolution reactions (ORR/OER), critical for achieving high efficiency and stability. Recent developments in light-assisted metal-O<sub>2</sub> (air) battery designs leverage photonic energy to enhance oxygen reduction and evolution reactions, offering reduced charge voltages, improved round-trip efficiencies, and extended lifetimes. This review critically evaluates the breakthroughs and limitations in photo-assisted Li/Zn-O<sub>2</sub> (air) battery technologies, with a focus on novel photocathode materials, including advanced semiconductors, heterojunction configurations, and nanostructured catalysts. We systematically highlight the key properties of these photocathode materials, evaluating their photon-utilization efficiency, charge separation capabilities, recombination rates, charging/discharging profiles, efficient decomposition of discharge products and stability under operational conditions. Emphasis is placed on advanced strategies to enhance light absorption, aiming to optimize photocatalytic efficiency, electronic properties, and catalytic stability, thereby overcoming current performance barriers. By providing a comprehensive analysis of the current landscape and emerging trends, this review aims to chart a path forward for the development of more robust, efficient, and sustainable light-assisted Li/Zn-O<sub>2</sub> (air) batteries, highlighting the essential role of innovative photocathode materials in achieving next-generation energy storage solutions.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"68 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142967953","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}
Pub Date : 2025-01-13DOI: 10.1016/j.ensm.2025.104032
Yunfeng Guan, Sheng Zhou, Lidan Tan, Rong Zhao, Qin Zhang, Hui Zhu, Xuanke Li, Zhijun Dong, Haiyan Duan, Dunzhu Li, Valeria Nicolosi, Ye Cong, Ke Li
Double transition metal (DTM) MXenes are garnering increasing attention owe to their wide diversity, controllable properties, tunable electronic structure and surface chemistry. Nevertheless, research on the exciting DTM MXenes is still in its infancy. Herein, we present a novel out-of-plan ordered DTM MXene, Ti2NbC2Tx, achieved by introducing Nb species into the M (Ti) site of Ti3C2Tx MXene. In which, Ti and Nb atoms occupy the outer and middle transition metal layers, respectively. This structure endows the as-synthesized Ti2NbC2Tx MXene with significantly higher chemical affinity and absorbability for lithium ions than Ti3C2Tx, showing a high reversible capacity of up to 272 mAh g-1 at 0.1 A g-1 and exceptional long-term stability (no capacity loss after 1000 cycles). Moreover, the lithium-ion capacitors (LICs) assembled with Ti2NbC2Tx MXene anode and activated carbon (AC) cathode exhibit high energy and power densities of 39 Wh Kg-1 and 4600 W kg-1, respectively, surpassing the most state-of-the-art MXene-based LICs. This work demonstrates the significant potential of DTM MXenes in advancing energy storage applications.
{"title":"Double Transition Metal Ti2NbC2Tx MXene with Modulated Electronic Structure for Advanced Lithium-ion Capacitors","authors":"Yunfeng Guan, Sheng Zhou, Lidan Tan, Rong Zhao, Qin Zhang, Hui Zhu, Xuanke Li, Zhijun Dong, Haiyan Duan, Dunzhu Li, Valeria Nicolosi, Ye Cong, Ke Li","doi":"10.1016/j.ensm.2025.104032","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104032","url":null,"abstract":"Double transition metal (DTM) MXenes are garnering increasing attention owe to their wide diversity, controllable properties, tunable electronic structure and surface chemistry. Nevertheless, research on the exciting DTM MXenes is still in its infancy. Herein, we present a novel out-of-plan ordered DTM MXene, Ti<sub>2</sub>NbC<sub>2</sub>T<em><sub>x</sub></em>, achieved by introducing Nb species into the M (Ti) site of Ti<sub>3</sub>C<sub>2</sub>T<em><sub>x</sub></em> MXene. In which, Ti and Nb atoms occupy the outer and middle transition metal layers, respectively. This structure endows the as-synthesized Ti<sub>2</sub>NbC<sub>2</sub>T<em><sub>x</sub></em> MXene with significantly higher chemical affinity and absorbability for lithium ions than Ti<sub>3</sub>C<sub>2</sub>T<em><sub>x</sub></em>, showing a high reversible capacity of up to 272 mAh g<sup>-1</sup> at 0.1 A g<sup>-1</sup> and exceptional long-term stability (no capacity loss after 1000 cycles). Moreover, the lithium-ion capacitors (LICs) assembled with Ti<sub>2</sub>NbC<sub>2</sub>T<em><sub>x</sub></em> MXene anode and activated carbon (AC) cathode exhibit high energy and power densities of 39 Wh Kg<sup>-1</sup> and 4600 W kg<sup>-1</sup>, respectively, surpassing the most state-of-the-art MXene-based LICs. This work demonstrates the significant potential of DTM MXenes in advancing energy storage applications.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"67 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142967954","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}
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