Qin Zhang, Xi Chen, Eng Liang Lim, Lei Shi, Zhanhua Wei
Perovskite solar cell (PSC) has attracted tremendous attention because of the impressive power conversion efficiency (PCE). After extensive device engineering efforts, the PCE of the single junction PSC has reached 26.7% from the initial value of 3.8%. Thanks to the unique characteristic of the metal halide perovskite (MHP) such as tunable energy bandgap, the bandgap complementary engineering can be applied to the MHP by pairing the wide bandgap (WBG) perovskite with the narrow bandgap (NBG) perovskite in series to form all perovskite two-terminal tandem solar cell (all-Pe-2T-TSC), which is expected to break the limitation of the Shockley-Queisser limit. In a tandem architecture, the WBG perovskite and the NBG perovskite act as the top and the bottom absorbers, respectively, and the interconnecting layer (ICL) is a region to facilitate electron-hole recombination. Currently, (i) the huge VOC deficit and severe photo-induced phase separation in WBG perovskite, (ii) the fast oxidation and uncontrollable crystallization of tin element in NBG perovskite and (iii) the optical parasitic absorption loss in ICL are the problems that hinder the performance development of all-Pe-2T-TSC. In this review, a thorough discussion is given to address the issues mentioned above through an analysis of the previously published research publications. Finally, new viewpoints on boosting the PCE and stability of all-Pe-2T-TSC are discussed, intending to guide the readers in developing efficient and stable all-Pe-2T-TSC.
{"title":"Advancing All-Perovskite Two-Terminal Tandem Solar Cells: Optimization of Wide- and Narrow-Bandgap Perovskites and Interconnecting Layers","authors":"Qin Zhang, Xi Chen, Eng Liang Lim, Lei Shi, Zhanhua Wei","doi":"10.1039/d4ee06027j","DOIUrl":"https://doi.org/10.1039/d4ee06027j","url":null,"abstract":"Perovskite solar cell (PSC) has attracted tremendous attention because of the impressive power conversion efficiency (PCE). After extensive device engineering efforts, the PCE of the single junction PSC has reached 26.7% from the initial value of 3.8%. Thanks to the unique characteristic of the metal halide perovskite (MHP) such as tunable energy bandgap, the bandgap complementary engineering can be applied to the MHP by pairing the wide bandgap (WBG) perovskite with the narrow bandgap (NBG) perovskite in series to form all perovskite two-terminal tandem solar cell (all-Pe-2T-TSC), which is expected to break the limitation of the Shockley-Queisser limit. In a tandem architecture, the WBG perovskite and the NBG perovskite act as the top and the bottom absorbers, respectively, and the interconnecting layer (ICL) is a region to facilitate electron-hole recombination. Currently, (i) the huge VOC deficit and severe photo-induced phase separation in WBG perovskite, (ii) the fast oxidation and uncontrollable crystallization of tin element in NBG perovskite and (iii) the optical parasitic absorption loss in ICL are the problems that hinder the performance development of all-Pe-2T-TSC. In this review, a thorough discussion is given to address the issues mentioned above through an analysis of the previously published research publications. Finally, new viewpoints on boosting the PCE and stability of all-Pe-2T-TSC are discussed, intending to guide the readers in developing efficient and stable all-Pe-2T-TSC.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"64 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143443775","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}
Self-assembled monolayers (SAMs) play the significant roles in the rapidly-progressed inverted perovskite solar cells (PSCs). Additional metal oxide or molecular incorporations are widely adopted to ameliorate their incomplete and uneven depositions on substrates, where the underlying binding situations between SAMs and substrates are vital for further optimizations but unclear. Here, we compare the bonding types between SAMs and metal oxides from a theoretical view, and conclude that SAMs preferably form the strong chemical bonds of -P-O-Sn via reacting with hydroxyl groups (-OH) on metal oxides for solid adsorptions. We further proposed the easy but effective strategy named seeding-OH groups via hydrogen peroxide(H2O2)/ultraviolet bath to strength and homogenize SAMs deposition on substrates, yielding the superior buried interface contact and high-quality perovskite films. Integrating the benefits, the resulted PSCs realized the champion efficiency of 26.19%, and 24.68% and 21.77% during their scalable fabrications with the areas of 1.21 and 13.8 cm2 (minimodules, active area), surpassing the bare ones with inferior scalability. Moreover, the large-area devices remained over 90% of their initial efficiency after ISOS-L-3 test for 1000 h.
{"title":"Homogenizing SAMs deposition via seeding -OH groups for scalable fabrication of perovskite solar cells","authors":"Sheng Fu, Nannan Sun, Hao Chen, You Li, Yunfei Li, Xiaotian Zhu, Bo Feng, Xuemin Guo, Canglang Yao, Wenxiao Zhang, Xiaodong Li, Junfeng Fang","doi":"10.1039/d5ee00350d","DOIUrl":"https://doi.org/10.1039/d5ee00350d","url":null,"abstract":"Self-assembled monolayers (SAMs) play the significant roles in the rapidly-progressed inverted perovskite solar cells (PSCs). Additional metal oxide or molecular incorporations are widely adopted to ameliorate their incomplete and uneven depositions on substrates, where the underlying binding situations between SAMs and substrates are vital for further optimizations but unclear. Here, we compare the bonding types between SAMs and metal oxides from a theoretical view, and conclude that SAMs preferably form the strong chemical bonds of -P-O-Sn via reacting with hydroxyl groups (-OH) on metal oxides for solid adsorptions. We further proposed the easy but effective strategy named seeding-OH groups via hydrogen peroxide(H2O2)/ultraviolet bath to strength and homogenize SAMs deposition on substrates, yielding the superior buried interface contact and high-quality perovskite films. Integrating the benefits, the resulted PSCs realized the champion efficiency of 26.19%, and 24.68% and 21.77% during their scalable fabrications with the areas of 1.21 and 13.8 cm2 (minimodules, active area), surpassing the bare ones with inferior scalability. Moreover, the large-area devices remained over 90% of their initial efficiency after ISOS-L-3 test for 1000 h.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"1 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143443780","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}
Hengyuan Hu, Meisheng Han, Jie Liu, Kunxiong Zheng, Zhiyu Zou, Yongbiao Mu, Fenghua Yu, Wenjia Li, Lei Wei, Lin Zeng, Tianshou Zhao
All-vanadium redox flow batteries (VRFBs) have emerged as a research hotspot and future direction of massive energy storage systems due to their advantages of intrinsic safety, long-duration energy storage, long cycle life, and no geographical limitations. However, the challenge in cost constrains the commercial developments of the flow battery. Increasing the power density and energy efficiency of the flow battery is the key to breaking through the cost bottlenecks, which is closely related to porous fiber felt electrodes (PFFEs), in which redox reactions take place. Therefore, it is essential to summarize advanced strategies for improving the design of electrodes, which are conducive to the further expansion of low-cost and high-performing flow batteries. This paper reviews the growth rate and market size of the flow battery, and summarizes the latest research progress on the improvement strategies of PFFEs from macro and micro perspectives, including structure design based on data model, intrinsic treatment, and introduction of catalysts. Finally, this review summarizes the practicability of the above strategies and the prospective modification approaches, and looks forward to the future optimization directions of PFFEs, such as exploring the modification mechanisms using advanced in-situ characterization techniques, introducing high-entropy catalysts, adopting new preparation technologies, and incorporating artificial intelligence. The review offers the optimization strategies of PFFEs for the flow battery and bridge the gap between the academic literature and industrial manufacturing.
{"title":"Strategies for improving the design of porous fiber felt electrodes for all-vanadium redox flow batteries from macro and micro perspectives","authors":"Hengyuan Hu, Meisheng Han, Jie Liu, Kunxiong Zheng, Zhiyu Zou, Yongbiao Mu, Fenghua Yu, Wenjia Li, Lei Wei, Lin Zeng, Tianshou Zhao","doi":"10.1039/d4ee05556j","DOIUrl":"https://doi.org/10.1039/d4ee05556j","url":null,"abstract":"All-vanadium redox flow batteries (VRFBs) have emerged as a research hotspot and future direction of massive energy storage systems due to their advantages of intrinsic safety, long-duration energy storage, long cycle life, and no geographical limitations. However, the challenge in cost constrains the commercial developments of the flow battery. Increasing the power density and energy efficiency of the flow battery is the key to breaking through the cost bottlenecks, which is closely related to porous fiber felt electrodes (PFFEs), in which redox reactions take place. Therefore, it is essential to summarize advanced strategies for improving the design of electrodes, which are conducive to the further expansion of low-cost and high-performing flow batteries. This paper reviews the growth rate and market size of the flow battery, and summarizes the latest research progress on the improvement strategies of PFFEs from macro and micro perspectives, including structure design based on data model, intrinsic treatment, and introduction of catalysts. Finally, this review summarizes the practicability of the above strategies and the prospective modification approaches, and looks forward to the future optimization directions of PFFEs, such as exploring the modification mechanisms using advanced in-situ characterization techniques, introducing high-entropy catalysts, adopting new preparation technologies, and incorporating artificial intelligence. The review offers the optimization strategies of PFFEs for the flow battery and bridge the gap between the academic literature and industrial manufacturing.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"15 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143443799","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}
NaNi1/3Fe1/3Mn1/3O2 (NFM333) is a promising cobalt-free, high-capacity cathode material for sodium-ion batteries, but suffers from poor cycling stability when prepared by the conventional tube furnace method due to electroactive metal migration, leading to a passive surface layer. To address this challenge, a high-temperature shock (HTS) method was employed. Compared to the tube furnace method, HTS offers a rapid heating process that contributes to a more compact and ultra-uniform NaCaPO4 (NCP) coating, leading to enhanced structural integrity and coating quality. The HTS method first enables the formation of a compact and ultra-uniform NCP coating, which prevents nickel migration more effectively compared to tube furnace-prepared NFM333 (Tu-NFM333). By preventing nickel migration, the surface residual alkalinity is reduced, enhancing air stability and improving electrochemical performance. As a result, HTS-treated NFM333 demonstrated 80% capacity retention after 1000 cycles at a 1C rate, while a pouch cell retained 70% capacity after 700 cycles. The stabilization of NFM333 through HTS highlights a promising approach for developing durable sodium-ion batteries.
{"title":"Ultra-uniform interfacial matrix via high-temperature thermal shock for long-cycle stability cathodes of sodium-ion batteries","authors":"Zekun Li, Pengfei Huang, Jinfeng Zhang, Zhaoxin Guo, Zhedong Liu, Li Chen, Jingchao Zhang, Jiawei Luo, Xiansen Tao, Zhikai Miao, Haoran Jiang, Chunying Wang, Xinran Ye, Xiaona Wu, Wei-Di Liu, Rui Liu, Yanan Chen, Wenbin Hu","doi":"10.1039/d5ee00217f","DOIUrl":"https://doi.org/10.1039/d5ee00217f","url":null,"abstract":"NaNi<small><sub>1/3</sub></small>Fe<small><sub>1/3</sub></small>Mn<small><sub>1/3</sub></small>O<small><sub>2</sub></small> (NFM333) is a promising cobalt-free, high-capacity cathode material for sodium-ion batteries, but suffers from poor cycling stability when prepared by the conventional tube furnace method due to electroactive metal migration, leading to a passive surface layer. To address this challenge, a high-temperature shock (HTS) method was employed. Compared to the tube furnace method, HTS offers a rapid heating process that contributes to a more compact and ultra-uniform NaCaPO<small><sub>4</sub></small> (NCP) coating, leading to enhanced structural integrity and coating quality. The HTS method first enables the formation of a compact and ultra-uniform NCP coating, which prevents nickel migration more effectively compared to tube furnace-prepared NFM333 (Tu-NFM333). By preventing nickel migration, the surface residual alkalinity is reduced, enhancing air stability and improving electrochemical performance. As a result, HTS-treated NFM333 demonstrated 80% capacity retention after 1000 cycles at a 1C rate, while a pouch cell retained 70% capacity after 700 cycles. The stabilization of NFM333 through HTS highlights a promising approach for developing durable sodium-ion batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"12 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143426967","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}
Dong Suk Kim, Yun Seop Shin, Jaehwi Lee, Dong Gyu Lee, Jiwon Song, Jongdeuk Seo, Jina Roe, Min Jung Sung, Sujung Park, Gwang Yong Shin, Jiwoo Yeop, Dongmin Lee, Chang Hyeon Yoon, Minseong Kim, Jung Geon Son, Gi-Hwan Kim, Shinuk Cho, Jin Young Kim, Tae Kyung Lee
In spiro-OMeTAD-based hole-transporting layer (HTL) protocols, 4-tert-butylpyridine (tBP) constitutes an indispensable component; however, its inclusion engenders substantial detrimental ramifications, precluding realizing thermal stability. Here, a tBP-free spiro-OMeTAD approach was successfully devised by substituting ethylene carbonate (EC) electrolyte for tBP. The electronegative carbonyl functionality forms a solvation complex with Li+ ions, addressing the solubility concern of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) in chlorobenzene even without tBP. The liberated TFSI− ions facilitate the stabilization of a larger population of spiro-OMeTAD∙+ radicals, thereby enabling efficient p-doping. The EC-incorporated HTL achieved a maximum power conversion efficiency (PCE) of 25.56% (certified 25.51%). In scaled-up applications, perovskite solar mini-modules with an aperture area of 100 cm2 demonstrated a PCE of 22.14%. The elevated glass transition temperature and robustly sequestered Li+ ions endow the devices with resilience against damp-heat conditions (85 ℃/85% RH) for 1,000 hours. Our findings signify a crucial leap forward commercialization by addressing thermal stability issues.
{"title":"Damp-heat stable and efficient perovskite solar cells and mini-modules with tBP-free hole-transporting layer","authors":"Dong Suk Kim, Yun Seop Shin, Jaehwi Lee, Dong Gyu Lee, Jiwon Song, Jongdeuk Seo, Jina Roe, Min Jung Sung, Sujung Park, Gwang Yong Shin, Jiwoo Yeop, Dongmin Lee, Chang Hyeon Yoon, Minseong Kim, Jung Geon Son, Gi-Hwan Kim, Shinuk Cho, Jin Young Kim, Tae Kyung Lee","doi":"10.1039/d4ee05699j","DOIUrl":"https://doi.org/10.1039/d4ee05699j","url":null,"abstract":"In spiro-OMeTAD-based hole-transporting layer (HTL) protocols, 4-tert-butylpyridine (tBP) constitutes an indispensable component; however, its inclusion engenders substantial detrimental ramifications, precluding realizing thermal stability. Here, a tBP-free spiro-OMeTAD approach was successfully devised by substituting ethylene carbonate (EC) electrolyte for tBP. The electronegative carbonyl functionality forms a solvation complex with Li+ ions, addressing the solubility concern of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) in chlorobenzene even without tBP. The liberated TFSI− ions facilitate the stabilization of a larger population of spiro-OMeTAD∙+ radicals, thereby enabling efficient p-doping. The EC-incorporated HTL achieved a maximum power conversion efficiency (PCE) of 25.56% (certified 25.51%). In scaled-up applications, perovskite solar mini-modules with an aperture area of 100 cm2 demonstrated a PCE of 22.14%. The elevated glass transition temperature and robustly sequestered Li+ ions endow the devices with resilience against damp-heat conditions (85 ℃/85% RH) for 1,000 hours. Our findings signify a crucial leap forward commercialization by addressing thermal stability issues.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"8 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143426971","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}
Yitong Peng, Tao Meng, Pingan Li, Rongxin Li, Xianluo Hu
Significant heat is often generated within lithium-ion batteries during practical operation, particularly under fast-charging or extreme conditions. If not dissipated efficiently, this heat can induce catastrophic thermal runaway. In this study, we present a built-in thermal-responsive design based on a phase change composite current collector, which is constructed by impregnating paraffin, a phase change material, into a nanoporous copper foil, followed by sealing through electroplating. The resulting thermoregulating current collector (TCC), with a high heat storage capacity, serves as an alternative to conventional copper foils, providing self-actuated over-heating protection for temperature-sensitive anodes and their solid electrolyte interphases. When assembled with the TCC, 225-mAh LiFePO4||graphite pouch cells and 1-Ah LiNi0.8Co0.1Mn0.1O2||graphite pouch cells demonstrate enhanced thermal safety due to latent heat storage. This work provides an effective route to built-in stimuli-responsive designs for safer lithium-ion batteries with high energy density.
{"title":"Self-thermoregulating current collectors: built-in thermal protection for safe lithium-ion batteries","authors":"Yitong Peng, Tao Meng, Pingan Li, Rongxin Li, Xianluo Hu","doi":"10.1039/d4ee04896b","DOIUrl":"https://doi.org/10.1039/d4ee04896b","url":null,"abstract":"Significant heat is often generated within lithium-ion batteries during practical operation, particularly under fast-charging or extreme conditions. If not dissipated efficiently, this heat can induce catastrophic thermal runaway. In this study, we present a built-in thermal-responsive design based on a phase change composite current collector, which is constructed by impregnating paraffin, a phase change material, into a nanoporous copper foil, followed by sealing through electroplating. The resulting thermoregulating current collector (TCC), with a high heat storage capacity, serves as an alternative to conventional copper foils, providing self-actuated over-heating protection for temperature-sensitive anodes and their solid electrolyte interphases. When assembled with the TCC, 225-mAh LiFePO4||graphite pouch cells and 1-Ah LiNi0.8Co0.1Mn0.1O2||graphite pouch cells demonstrate enhanced thermal safety due to latent heat storage. This work provides an effective route to built-in stimuli-responsive designs for safer lithium-ion batteries with high energy density.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"5 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143426969","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}
Xiancheng Wang, Zihe Chen, Shiyu Liu, Shuibin Tu, Renming Zhan, Li Wang, Yongming Sun
High energy density and exceptional fast-charging capability are emerging as critical technical parameters for lithium (Li)-based rechargeable batteries, aimed at meeting the increasing demands of advanced portable electronics, electric vehicles, and grid energy storage systems. However, the sluggish charge transfer kinetics associated with contemporary graphite anodes significantly hinder both the fast-charging performance and overall energy characteristics of existing Li-based rechargeable batteries. As we transition to high-capacity anodes (such as alloying-type and Li metal anodes) for next-generation high-energy-density batteries, their inherent slow electrochemical Li+/e− combination rate presents new challenges for fast charging. Furthermore, the significant volume changes that occur during charge and discharge processes contribute to the structural instability of these high-capacity materials and electrodes. This phenomenon also leads to severe side reactions between the active material and the electrolyte, ultimately compromising the electrochemical cycling lifespan. The empirical evidence suggests that the strategic design of the interphase significantly augments the electrochemical reaction kinetics of battery anode materials, concurrently enhancing their structural stability. Nevertheless, a profound understanding of the intricate mechanisms is still lacking, making the establishment of a universal design rule for various anode materials a challenging task. In this review, we categorize the interphases of anode materials into outer and inner interphases based on their physical/chemical environments in batteries. After a comprehensive discussion on the roles and mechanisms of advanced interphases across a range of anode materials, including graphite, alloying-type, and Li metal foil anode materials, we elucidate the principles of outer and inner interphase design, with an emphasis on enhancing their electrochemical reaction kinetics. Several advanced strategies for the design of electrode structures are also proposed to synergistically enhance the Li+ transport processes. Subsequently, we provide typical examples of advanced interphase design, based on the understanding of the proposed interphase design principles for various anodes. Additionally, we offer a review on the future direction of anode interphase design, aiming at the development of high energy density Li-based rechargeable batteries with superior fast-charging capability and long lifespan.
{"title":"Anode Interphase Design for Fast-Charging Lithium-Based Rechargeable Batteries","authors":"Xiancheng Wang, Zihe Chen, Shiyu Liu, Shuibin Tu, Renming Zhan, Li Wang, Yongming Sun","doi":"10.1039/d4ee06107a","DOIUrl":"https://doi.org/10.1039/d4ee06107a","url":null,"abstract":"High energy density and exceptional fast-charging capability are emerging as critical technical parameters for lithium (Li)-based rechargeable batteries, aimed at meeting the increasing demands of advanced portable electronics, electric vehicles, and grid energy storage systems. However, the sluggish charge transfer kinetics associated with contemporary graphite anodes significantly hinder both the fast-charging performance and overall energy characteristics of existing Li-based rechargeable batteries. As we transition to high-capacity anodes (such as alloying-type and Li metal anodes) for next-generation high-energy-density batteries, their inherent slow electrochemical Li+/e− combination rate presents new challenges for fast charging. Furthermore, the significant volume changes that occur during charge and discharge processes contribute to the structural instability of these high-capacity materials and electrodes. This phenomenon also leads to severe side reactions between the active material and the electrolyte, ultimately compromising the electrochemical cycling lifespan. The empirical evidence suggests that the strategic design of the interphase significantly augments the electrochemical reaction kinetics of battery anode materials, concurrently enhancing their structural stability. Nevertheless, a profound understanding of the intricate mechanisms is still lacking, making the establishment of a universal design rule for various anode materials a challenging task. In this review, we categorize the interphases of anode materials into outer and inner interphases based on their physical/chemical environments in batteries. After a comprehensive discussion on the roles and mechanisms of advanced interphases across a range of anode materials, including graphite, alloying-type, and Li metal foil anode materials, we elucidate the principles of outer and inner interphase design, with an emphasis on enhancing their electrochemical reaction kinetics. Several advanced strategies for the design of electrode structures are also proposed to synergistically enhance the Li+ transport processes. Subsequently, we provide typical examples of advanced interphase design, based on the understanding of the proposed interphase design principles for various anodes. Additionally, we offer a review on the future direction of anode interphase design, aiming at the development of high energy density Li-based rechargeable batteries with superior fast-charging capability and long lifespan.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"2 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143426970","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 global push to keep global warming to less than 1.5 ºC, will require us to quickly adopt zero-emission energy carriers. Hydrogen, a versatile energy vector, is pivotal in this transition, especially for sectors that are challenging to electrify. Methane pyrolysis is emerging as a promising route for producing hydrogen with minimal greenhouse gas emissions. In this review, we provide a comprehensive overview of methane pyrolysis, and explore its potential to contribute to a net-zero future. Current hydrogen production methods, including steam methane reforming and water electrolysis, are also discussed in terms of efficiency, emissions, and costs for comparison with methane pyrolysis. The review then delves into the various technologies under development for methane pyrolysis, categorizing them into catalytic and non-catalytic routes. Key aspects such as reactor design, catalyst performance, and economic viability are critically examined. We also analyze the importance of the carbon co-product produced in the process, and its market potential. Finally, by evaluating industrial activities around methane pyrolysis, this paper underscores its role in the global energy transition, emphasizing the requirements to overcome current challenges and achieve large-scale deployment.
{"title":"Methane Pyrolysis for Hydrogen Production: Navigating the Path to a Net Zero Future","authors":"Alireza Lotfollahzade Moghaddam, Sohrab Hejazi, Moslem Fattahi, Md Golam Kibria, Murray Thomson, Rashed AlEisa, Mohd Adnan Khan","doi":"10.1039/d4ee06191h","DOIUrl":"https://doi.org/10.1039/d4ee06191h","url":null,"abstract":"The global push to keep global warming to less than 1.5 ºC, will require us to quickly adopt zero-emission energy carriers. Hydrogen, a versatile energy vector, is pivotal in this transition, especially for sectors that are challenging to electrify. Methane pyrolysis is emerging as a promising route for producing hydrogen with minimal greenhouse gas emissions. In this review, we provide a comprehensive overview of methane pyrolysis, and explore its potential to contribute to a net-zero future. Current hydrogen production methods, including steam methane reforming and water electrolysis, are also discussed in terms of efficiency, emissions, and costs for comparison with methane pyrolysis. The review then delves into the various technologies under development for methane pyrolysis, categorizing them into catalytic and non-catalytic routes. Key aspects such as reactor design, catalyst performance, and economic viability are critically examined. We also analyze the importance of the carbon co-product produced in the process, and its market potential. Finally, by evaluating industrial activities around methane pyrolysis, this paper underscores its role in the global energy transition, emphasizing the requirements to overcome current challenges and achieve large-scale deployment.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"12 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418328","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}
Jinuk Kim, Dong Gyu Lee, Ju Hyun Lee, Saehun Kim, Cheol-Young Park, Jiyoon Lee, Hyeokjin Kwon, Hannah Cho, Jungyoon Lee, Donghyeok Son, Hee-Tak Kim, Nam-Soon Choi, Tae Kyung Lee, Jinwoo Lee
Electrolyte engineering is emerging as a key strategy for enhancing the cycle life of lithium metal batteries (LMBs). Fluorinated electrolytes have dramatically extended cycle life; however, intractable challenges regarding the rate capability and fluorine overuse persist. Here, we introduce a lithiophilic, solvent-interactive, and fluorine-free nano-Si3N4 additive that facilitates the fine-tuning of weak Li+ solvation to form inorganic-rich solid-electrolyte interphase (SEI) layers. Additionally, the alloying and conversion reactions between nano-Si3N4 and Li generated a fast Li+-conductive SEI, overcoming the poor rate performance of weakly solvating electrolytes. Simultaneously, nano-Si3N4 interacts with ethylene carbonate (EC), minimizing hydrogen (H)-transfer reactions and scavenging HF, thus increasing the high-voltage tolerance. Consequently, nano-Si3N4 extends the cyclability of commercial carbonate-based electrolyte in 360 Wh kg-1-level LiǁLiNi0.8Co0.1Mn0.1O2 (NCM811) pouch-cells, resulting in 74% capacity retention after 100 cycles, whereas failure occurred without it. Our study provides an in-depth understanding of the working mechanisms of suspension electrolytes through comprehensive analysis.
{"title":"Concurrent electrode-electrolyte interfaces engineering via nano-Si3N4 additive for high-rate, high-voltage lithium metal batteries","authors":"Jinuk Kim, Dong Gyu Lee, Ju Hyun Lee, Saehun Kim, Cheol-Young Park, Jiyoon Lee, Hyeokjin Kwon, Hannah Cho, Jungyoon Lee, Donghyeok Son, Hee-Tak Kim, Nam-Soon Choi, Tae Kyung Lee, Jinwoo Lee","doi":"10.1039/d4ee03862b","DOIUrl":"https://doi.org/10.1039/d4ee03862b","url":null,"abstract":"Electrolyte engineering is emerging as a key strategy for enhancing the cycle life of lithium metal batteries (LMBs). Fluorinated electrolytes have dramatically extended cycle life; however, intractable challenges regarding the rate capability and fluorine overuse persist. Here, we introduce a lithiophilic, solvent-interactive, and fluorine-free nano-Si<small><sub>3</sub></small>N<small><sub>4</sub></small> additive that facilitates the fine-tuning of weak Li<small><sup>+</sup></small> solvation to form inorganic-rich solid-electrolyte interphase (SEI) layers. Additionally, the alloying and conversion reactions between nano-Si<small><sub>3</sub></small>N<small><sub>4</sub></small> and Li generated a fast Li<small><sup>+</sup></small>-conductive SEI, overcoming the poor rate performance of weakly solvating electrolytes. Simultaneously, nano-Si<small><sub>3</sub></small>N<small><sub>4</sub></small> interacts with ethylene carbonate (EC), minimizing hydrogen (H)-transfer reactions and scavenging HF, thus increasing the high-voltage tolerance. Consequently, nano-Si<small><sub>3</sub></small>N<small><sub>4</sub></small> extends the cyclability of commercial carbonate-based electrolyte in 360 Wh kg<small><sup>-1</sup></small>-level LiǁLiNi<small><sub>0.8</sub></small>Co<small><sub>0.1</sub></small>Mn<small><sub>0.1</sub></small>O<small><sub>2</sub></small> (NCM811) pouch-cells, resulting in 74% capacity retention after 100 cycles, whereas failure occurred without it. Our study provides an in-depth understanding of the working mechanisms of suspension electrolytes through comprehensive analysis.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"16 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143401760","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}
Chenyang Shi, Zhengguang Li, Mengran Wang, Shu Hong, Bo Hong, Yaxuan Fu, Die Liu, Rui Tan, Pingshan Wang, Yanqing Lai
The deployment of lithium-ion batteries, essential for military and space exploration applications, faces restrictions due to safety issues and performance degradation stemming from the uncontrollable side reactions between electrolytes and electrodes, particularly at high temperatures. Current research focuses on interfacial modification and non-flammable electrolyte development, which fails to simultaneously improve both safety and cyclic performance. This work introduces a synergistic approach by incorporating weakly polar methyl 2,2-difluoro-2-(fluorosulfonyl)acetate (MDFSA) and non-flammable 2-(2,2,2-trifluoroethoxy)-1,3,2-dioxaphospholane 2-oxide (TFP) to achieve a localized high-concentration electrolyte (LHCE) that can stabilize both anode and cathode interfaces and thus improve the cycling life and safety of batteries, particularly under evaluated temperatures. As a result, the NCM811|Gr pouch cell with MDFSA-contained LHCE exhibits a high capacity retention rate of 79.6% at 60°C after 1200 cycles due to the formation of thermally and structurally stable interfaces on the electrodes, outperforming pouch cells utilizing commercial carbonate-based (capacity retention: 23.7% after 125 cycles). Additionally, pouch cells in the charging state also exhibit commendable safety performance, indicating potential for practical applications.
{"title":"Electrolyte tailoring and interfacial engineering for safe and high-temperature lithium-ion batteries","authors":"Chenyang Shi, Zhengguang Li, Mengran Wang, Shu Hong, Bo Hong, Yaxuan Fu, Die Liu, Rui Tan, Pingshan Wang, Yanqing Lai","doi":"10.1039/d4ee05263c","DOIUrl":"https://doi.org/10.1039/d4ee05263c","url":null,"abstract":"The deployment of lithium-ion batteries, essential for military and space exploration applications, faces restrictions due to safety issues and performance degradation stemming from the uncontrollable side reactions between electrolytes and electrodes, particularly at high temperatures. Current research focuses on interfacial modification and non-flammable electrolyte development, which fails to simultaneously improve both safety and cyclic performance. This work introduces a synergistic approach by incorporating weakly polar methyl 2,2-difluoro-2-(fluorosulfonyl)acetate (MDFSA) and non-flammable 2-(2,2,2-trifluoroethoxy)-1,3,2-dioxaphospholane 2-oxide (TFP) to achieve a localized high-concentration electrolyte (LHCE) that can stabilize both anode and cathode interfaces and thus improve the cycling life and safety of batteries, particularly under evaluated temperatures. As a result, the NCM811|Gr pouch cell with MDFSA-contained LHCE exhibits a high capacity retention rate of 79.6% at 60°C after 1200 cycles due to the formation of thermally and structurally stable interfaces on the electrodes, outperforming pouch cells utilizing commercial carbonate-based (capacity retention: 23.7% after 125 cycles). Additionally, pouch cells in the charging state also exhibit commendable safety performance, indicating potential for practical applications.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"41 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143401843","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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