Fengqi You, Xueyu Tian, Samuel D Stranks, Jinsong Huang, Vasilis Fthenakis, Yang Yang
{"title":"Perspectives for Sustainability Analysis of Scalable Perovskite Photovoltaics","authors":"Fengqi You, Xueyu Tian, Samuel D Stranks, Jinsong Huang, Vasilis Fthenakis, Yang Yang","doi":"10.1039/d4ee03956d","DOIUrl":"https://doi.org/10.1039/d4ee03956d","url":null,"abstract":"Halide perovskite photovoltaics (PVs) are poised to become a critical high-efficiency renewable energy technology in the fight against climate change. This perspective aims to ensure the viability of perovskite PV as a sustainable technology by focusing on key areas such as end-of-life management and sustainability analysis. It highlights the current lack of comprehensive frameworks that incorporate circular solar economy principles, ecosystem impacts, and climate commitments. To address this gap, we propose a multi-scale analytical and modeling framework specifically designed for perovskite PVs. This approach integrates dynamic material flow analysis and life cycle assessment to reshape our understanding of material usage, with an emphasis on critical material demand and recycling opportunities. It seeks to provide in-depth insights into the socio-economic and environmental impacts of material consumption, particularly as perovskite PVs become more prevalent. Additionally, future research should explore distributed manufacturing to optimize costs and reduce environmental impacts, as well as evaluate the benefits of integrating perovskite PVs with agriculture to promote sustainable sector coupling.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"194 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142487269","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}
Ya Chen, Xin Gao, Zheng Zhen, Xiao Chen, Ling Huang, Deli Zhou, Tengfei Hu, Bozhen Ren, Runjing Xu, Jiayi Chen, Xiaodong Chen, Lifeng Cui and Guoxiu Wang
{"title":"The construction of multifunctional solid electrolyte interlayers for stabilizing Li6PS5Cl-based all-solid-state lithium metal batteries†","authors":"Ya Chen, Xin Gao, Zheng Zhen, Xiao Chen, Ling Huang, Deli Zhou, Tengfei Hu, Bozhen Ren, Runjing Xu, Jiayi Chen, Xiaodong Chen, Lifeng Cui and Guoxiu Wang","doi":"10.1039/D4EE03289F","DOIUrl":"10.1039/D4EE03289F","url":null,"abstract":"<p >The electrochemical performance of all-solid-state Li metal batteries (ASSLMBs) can be improved by resolving the challenges triggered by the uncontrolled growth of Li dendrites throughout the solid electrolytes (SEs). Herein, a well-defined composite of micro-Li<small><sub>6</sub></small>PS<small><sub>5</sub></small>Cl (LPSC) and nano-Li<small><sub>1.3</sub></small>Al<small><sub>0.3</sub></small>Ti<small><sub>1.7</sub></small>(PO<small><sub>4</sub></small>)<small><sub>3</sub></small> (LATP) is designed as a LPSC–LATP interlayer sandwiched between LPSC electrolytes for ASSLMBs. This fabrication exhibits electron-blocking functionalities, which reduce the probability of reaction with Li<small><sup>+</sup></small> ions for the formation of anode-initiated and grain boundary (GB)-initiated dendrites. More importantly, it also creates localized eliminated micro-environments of Li dendrites through the high transient reactivity between them, and the remaining cracks can be dynamically and effectively filled by decomposition products, thereby clearly suppressing Li dendrite nucleation, propagation and penetration as well as simultaneously contributing to the enhancement of battery performance and stability. With this approach, a fine-tuned LPSC–LATP (8S–2O) interlayer enables symmetrical Li/LPSC/8S–2O/LPSC/Li cells to achieve an ultra-high critical current density (CCD) of over 5 mA cm<small><sup>−2</sup></small> at room temperature, and ultra-long-term cycling at a current density of 10 mA cm<small><sup>−2</sup></small> for over 1600 h. Additionally, ASSLMBs employing commercial LiCoO<small><sub>2</sub></small> cathodes can deliver exceptional durability, with an extremely high 85.6% retention of initial discharge capacity and coulombic efficiency (CE) of >99.6% after 1200 cycles at 1C (1.28 mA cm<small><sup>−2</sup></small>). These experimental batteries demonstrate the application potential of this configuration of SEs for the commercialization of ASSLMBs.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 23","pages":" 9288-9302"},"PeriodicalIF":32.4,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142486683","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}
Gi-Hyeok Lee, Suwon Lee, Jiliang Zhang, Bernardine L. D. Rinkel, Matthew J. Crafton, Zengqing Zhuo, Youngju Choi, Jialu Li, Junghoon Yang, Jongwook W. Heo, Byungchun Park, Bryan D. McCloskey, Maxim Avdeev, Wanli Yang and Yong-Mook Kang
{"title":"Oxygen redox activities governing high-voltage charging reversibility of Ni-rich layered cathodes†","authors":"Gi-Hyeok Lee, Suwon Lee, Jiliang Zhang, Bernardine L. D. Rinkel, Matthew J. Crafton, Zengqing Zhuo, Youngju Choi, Jialu Li, Junghoon Yang, Jongwook W. Heo, Byungchun Park, Bryan D. McCloskey, Maxim Avdeev, Wanli Yang and Yong-Mook Kang","doi":"10.1039/D4EE03832K","DOIUrl":"10.1039/D4EE03832K","url":null,"abstract":"<p >The chemical reactions and phase transitions at high voltages are generally considered to determine the electrochemical properties of high-voltage layered cathodes such as Ni-rich rhombohedral oxides. Even if significantly higher SOCs (states-of-charge) are utilized above the capability of transition metal redox (primarily Ni and Co), the effect of oxygen redox on Ni-rich rhombohedral oxides still looks mysterious thereby necessitating research that can clarify the relationship between redox reactions and phase transitions. Here, we performed a comprehensive and comparative study of the cationic and anionic redox reactions, as well as the structural evolution of a series of commercial Ni-rich layered oxides with and without Al doping. We combined the results from X-ray spectroscopy, operando electrochemical mass spectrometry, and neutron diffraction with electrochemical properties and thereby revealed the different oxygen redox activities associated with structural and electrochemical degradations. We reveal that Al doping suppresses the irreversible oxygen release but enhances the lattice oxygen oxidization. With this modulated oxygen redox activity, the Ni-rich layered oxides’ notorious H2–H3 structural phase transition becomes highly reversible. Our findings disentangle the different oxygen redox activities during high-voltage cycling and clarify the role of dopants in the Ni-rich layered oxides in terms of structural and electrochemical stability, shedding light on the future direction of optimizing layered cathode materials for safer high energy-density secondary batteries.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 23","pages":" 9154-9163"},"PeriodicalIF":32.4,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452589","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}
Laiquan Li, Linyuan Xu, Hanyun Wang, Haohong Wei, Cheng Tang, Guisheng Li, Yuhai Dou, Hua Kun Liu and Shi Xue Dou
{"title":"Electrocatalytic nitrogen cycle: mechanism, materials, and momentum","authors":"Laiquan Li, Linyuan Xu, Hanyun Wang, Haohong Wei, Cheng Tang, Guisheng Li, Yuhai Dou, Hua Kun Liu and Shi Xue Dou","doi":"10.1039/D4EE03156C","DOIUrl":"10.1039/D4EE03156C","url":null,"abstract":"<p >Artificial nitrogen fixation has been pivotal in escalating agricultural productivity and sustaining exponential human population growth. Nonetheless, these practices have concurrently perturbed the natural nitrogen cycle, engendering a plethora of environmental challenges. The advent of electrochemical nitrogen transformation techniques represents a burgeoning avenue for rectifying the nitrogen cycle's imbalance and for synthesizing value-added nitrogenous products from atmospheric nitrogen. In this review, we delve into the recent progress concerning the electrocatalytic interconversion among key nitrogen species, namely N<small><sub>2</sub></small>, NO<small><sub><em>x</em></sub></small><small><sup>(−)</sup></small>, and NH<small><sub>3</sub></small>. Our examination encompasses a multifaceted analysis, including the elucidation of reaction mechanisms and a critical evaluation of the intrinsic challenges behind each reaction and the strategies to boost their translation to practical applications. Extending beyond primary nitrogen transformations, we also assess a spectrum of emergent and promising directions. These include lithium-mediated nitrogen fixation, carbon–nitrogen coupling reactions, and the development of electrochemical batteries harnessing nitrogen transformation chemistry. This review aims to offer a critical and forward-looking perspective on the role of electrocatalysis in modulating the nitrogen cycle and to highlight untapped opportunities for its application in a myriad of innovative domains.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 23","pages":" 9027-9050"},"PeriodicalIF":32.4,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452590","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}
Yang Ding, Erming Feng, Siyuan Lu, Jianhui Chang, Caoyu Long, Sichao Tong, Hengyue Li and Junliang Yang
{"title":"Stress regulation via surface micro-etching and reconstruction for enhancing triple-cation perovskite solar cells with an efficiency of 25.54%†","authors":"Yang Ding, Erming Feng, Siyuan Lu, Jianhui Chang, Caoyu Long, Sichao Tong, Hengyue Li and Junliang Yang","doi":"10.1039/D4EE04248D","DOIUrl":"10.1039/D4EE04248D","url":null,"abstract":"<p >Residual stresses generated within perovskite films during the high-temperature annealing and cooling process are the key contributors to the reduction of device performance and lifespan deterioration. Herein, a strategy of surface micro-etching and reconstruction is developed to regulate the stresses in a triple-cation (formamidine, methylamine, and cesium) perovskite film. A precise stoichiometric mixture of <small>L</small>-lactic acid (LA) and isopropanol (IPA) is used to controllably dissolve the surface of the perovskite film, followed by octylammonium iodide (OAI) post-treatment, enabling a sinking reconstruction of 2D perovskite from the surface to bulk phase and achieving a benign transition from surface tensile stress to compressive stress, as well as a more matchable interface energy level. As a result, the target perovskite solar cells (PSCs) yield an obviously enhanced power conversion efficiency (PCE) of 25.54%, which is the highest reported PCE for triple-cation PSCs. Meanwhile, PSC modules with 10.4 cm<small><sup>2</sup></small> achieve a PCE of 21.02%. Furthermore, the surface micro-etched and reconstructed PSCs exhibit superior stability, and the PSC devices without encapsulation can maintain 83% of original efficiency after 500 hour illumination at maximum power point tracking (MPPT) in a N<small><sub>2</sub></small> atmosphere. This study provides a valuable avenue to improve PSC stability and efficiency by regulating residual stresses through surface micro-etching and reconstruction.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 23","pages":" 9268-9277"},"PeriodicalIF":32.4,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452627","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}
Hong-Bo Zhang, Yu Meng, Lingzhe Fang, Fei Yang, Shangqian Zhu, Tao Li, Xiaohua Yu, Ju Rong, Weiwei Chen, Dong Su, Yi Mei, Peng-Xiang Hou, Chang Liu, Minhua Shao and Jin-Cheng Li
{"title":"A thermal evaporation–trapping strategy to synthesize flexible and robust oxygen electrocatalysts for rechargeable zinc–air batteries†","authors":"Hong-Bo Zhang, Yu Meng, Lingzhe Fang, Fei Yang, Shangqian Zhu, Tao Li, Xiaohua Yu, Ju Rong, Weiwei Chen, Dong Su, Yi Mei, Peng-Xiang Hou, Chang Liu, Minhua Shao and Jin-Cheng Li","doi":"10.1039/D4EE03005B","DOIUrl":"10.1039/D4EE03005B","url":null,"abstract":"<p >Great efforts have been devoted to the development of bifunctional electrocatalysts to accelerate the sluggish kinetics of cathodic oxygen reduction/evolution reactions (ORR/OER) in zinc–air batteries (ZABs). Here we report a thermal evaporation–trapping synergistic strategy to fabricate a bifunctional electrocatalyst of flexible N-doped carbon fiber cloth loaded with both CoFe-oxide nanoparticles and single-atom Co/Fe–N<small><sub><em>x</em></sub></small> sites, in which the thermal evaporation process functions in both downsizing CoFe-oxide nanoparticles and trapping the evaporated Co/Fe species to generate Co/Fe–N<small><sub><em>x</em></sub></small> sites. The obtained flexible electrocatalyst, directly serving as an oxygen electrode, displays a small potential gap of 0.542 V for the OER/ORR, large peak power densities (liquid-state ZAB: 237.4 mW cm<small><sup>−2</sup></small>; solid-state ZAB: 141.1 mW cm<small><sup>−2</sup></small>), and excellent charge–discharge cycling stability without decay after working more than 770 hours. Furthermore, <em>in situ</em> Raman spectroscopy characterization and theoretical calculations reveal that CoFe<small><sub>2</sub></small>O<small><sub>4</sub></small> species is responsible for the OER while atomic Fe/Co sites play a key role in the ORR.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 23","pages":" 9375-9382"},"PeriodicalIF":32.4,"publicationDate":"2024-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142450109","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}
Jingyu Shi, Pengfei Ding, Jintao Zhu, Zhenyu Chen, Shuangjiao Gao, Xueliang Yu, Xiaochun Liao, Quan Liu and Ziyi Ge
{"title":"Well-regulated structure-featuring giant-molecule acceptors enable long-term stability and high-performance binary organic solar cells†","authors":"Jingyu Shi, Pengfei Ding, Jintao Zhu, Zhenyu Chen, Shuangjiao Gao, Xueliang Yu, Xiaochun Liao, Quan Liu and Ziyi Ge","doi":"10.1039/D4EE03754E","DOIUrl":"10.1039/D4EE03754E","url":null,"abstract":"<p >Well-defined structure-featuring giant-molecule acceptors (GMAs) can exhibit unique properties of small-molecule acceptors and polymers simultaneously, and the consecutive innovations in materials design have enabled GMA-based organic solar cells (OSCs) to exhibit outstanding device power conversion efficiency (PCE) over 19% and extended long-term stability. Here, through systematically selecting the numbers and positions of the selenium atom, π-spacer linking units and the outermost conjugate ring of the central core of monomers, four novel GMAs are successfully synthesized, GMA-SSS, GMA-SSeS, GMA-SeSSe and GMA-SeSeSe. Surprisingly, the PM6:GMA-SSeS-based OSC yields the highest PCE of 19.37% with a remarkable open current voltage of 0.917 V with reduced voltage loss (Δ<em>E</em><small><sub>3</sub></small> = 0.246 eV) and excellent fill factor of 77.12%. Furthermore, when devices were annealed at 100 °C, the PM6:GMA-SSeS and PM6:GMA-SSS-based OSCs exhibited remarkably extended <em>t</em><small><sub>80%</sub></small> lifetimes of 5600 and 5250 h, respectively. Our work indicates that the selenium substituted regulation of linking units and monomers of GMA structures is a valuable approach to obtain devices with high-performance and long-term stability at the same time, shedding light on the further development of GMA-based OSCs.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 23","pages":" 9144-9153"},"PeriodicalIF":32.4,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142448186","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}
Airan Li, Longquan Wang, Jiankang Li and Takao Mori
{"title":"Global softening to manipulate sound velocity for reliable high-performance MgAgSb thermoelectrics†","authors":"Airan Li, Longquan Wang, Jiankang Li and Takao Mori","doi":"10.1039/D4EE03521F","DOIUrl":"10.1039/D4EE03521F","url":null,"abstract":"<p >High-performance thermoelectric materials at room temperature are eagerly pursued due to their promising applications in the Internet of Things for sustainable power supply. Reducing sound velocity by softening chemical bonds is considered an effective approach to lowering thermal conductivity and enhancing thermoelectric performance. Here, different from softening chemical bonds at the atomic scale, we introduce a global softening strategy, which macroscopically softens the overall material to manipulate its sound velocity. This is demonstrated in MgAgSb, one of the most promising p-type thermoelectric materials at room temperature to replace (Bi,Sb)<small><sub>2</sub></small>Te<small><sub>3</sub></small>, that the addition of inherently soft organic compounds can easily lower its sound velocity, leading to an obvious reduction in lattice thermal conductivity. Despite a simultaneous reduction of the power factor, the overall thermoelectric quality factor <em>B</em> is enhanced, enabling softened MgAgSb by C<small><sub>18</sub></small>H<small><sub>36</sub></small>O<small><sub>2</sub></small> addition to achieve a figure of merit <em>zT</em> value of ∼0.88 at 300 K and a peak <em>zT</em> value of ∼1.30. Consequently, an impressive average <em>zT</em> of ∼1.17 over a wide temperature range has been realized. Moreover, this high-performance MgAgSb is verified to be highly repeatable and stable. With this MgAgSb, a decent conversion efficiency of 8.6% for a single thermoelectric leg and ∼7% for a two-pair module have been achieved under a temperature difference of ∼276 K, indicating its great potential for low-grade heat harvesting. This work will not only advance MgAgSb for low-grade power generation, but also inspire the development of high-performance thermoelectrics with global softening in the future.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 22","pages":" 8810-8819"},"PeriodicalIF":32.4,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ee/d4ee03521f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142448184","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xinpeng Han, Jinpeng Han, Kang Ma, Jiaqi Wen, Lianpeng Li, Daliang Han and Jie Sun
{"title":"A fluoride gradient, Zn-salt-rich hydrophobic interphase formed by a zincophilic, hydrophobic, anion-philic polymer “skin” for an anode-free solid Zn battery†","authors":"Xinpeng Han, Jinpeng Han, Kang Ma, Jiaqi Wen, Lianpeng Li, Daliang Han and Jie Sun","doi":"10.1039/D4EE01978D","DOIUrl":"10.1039/D4EE01978D","url":null,"abstract":"<p >Manipulating ion solvation sheath behaviour is of great significance for alleviating dendritic growth, hydrogen production, and metal corrosion in order to achieve the long-term stability of zinc ion batteries. Herein, we rationally design a Zn<small><sup>2+</sup></small>·O<img>C group-derived contact ion pair (CIP)/aggregate (AGG)-rich electrolyte with zincophilic and hydrophobic features through <em>in situ</em> polymerization of 3-methacryloxypropyl trimethoxysilane monomers. Due to its unique design, this electrolyte “skin” enables the generation of a fluoride gradient, Zn-salt-rich hydrophobic solid electrolyte interface (SEI) layer through increasing the ratio of ZnF<small><sub>2</sub></small>/ZnO in the SEI layer. Moreover, the amount of ZnF<small><sub>2</sub></small> in the inner SEI is higher than that in the outer SEI. Due to the higher dendrite-suppressing and desolvation ability of ZnF<small><sub>2</sub></small> than that of ZnO, the SEI exhibits excellent capability to suppress the growth of Zn dendrites and restrain H<small><sub>2</sub></small>O-related side reactions. Owing to its unprecedented average modulus (71.25 GPa), the SEI effectively inhibits the external stress originating from dendritic growth, the undesirable volume expansion of Zn and the long-lasting anode/electrolyte side reactions. Consequently, at a high depth of discharge of 34.2%, the symmetric cell shows long-term stability for over 1000 h, and the anode-free battery shows a high capacity retention of 99.2% after 110 cycles.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 23","pages":" 9244-9254"},"PeriodicalIF":32.4,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142448187","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}
Tao Zhou, Jinze Wang, Ling Lv, Ruhong Li, Long Chen, Shuoqing Zhang, Haikuo Zhang, Baochen Ma, Jiajie Huang, Bing Wu, Lixin Chen, Tao Deng and Xiulin Fan
{"title":"Anion–π interaction and solvent dehydrogenation control enable high-voltage lithium-ion batteries†","authors":"Tao Zhou, Jinze Wang, Ling Lv, Ruhong Li, Long Chen, Shuoqing Zhang, Haikuo Zhang, Baochen Ma, Jiajie Huang, Bing Wu, Lixin Chen, Tao Deng and Xiulin Fan","doi":"10.1039/D4EE03027C","DOIUrl":"10.1039/D4EE03027C","url":null,"abstract":"<p >Extending the charging cutoff voltage of lithium cobalt oxide (LCO) cathodes is an effective strategy to enhance the energy density of lithium-ion batteries (LIBs), while the formation of a poor cathode–electrolyte interphase (CEI) has limited their widespread application. Various electrolyte additives, particularly nitrile compounds, have shown promise in addressing these interfacial issues, though the fundamental design principles remain unclear. Herein, we introduce an interfacial leverage mechanism utilizing nitriles adsorbed on the LCO surface to fine-tune the CEI composition. The suitability of a nitrile additive for high-voltage LCO is determined by the repulsive interaction with the solvent (<em>E</em><small><sub>sol</sub></small>) and the attractive interaction with the anion (<em>E</em><small><sub>anion</sub></small>). The former inhibits solvent decomposition, while the latter facilitates the anion decomposition during CEI construction. These interactions can be tailored through the functional design of nitrile compounds, as demonstrated using 3,5-bis(trifluoromethyl)benzonitrile (BFBN) in a commercial carbonate electrolyte. The BFBN molecules adsorb onto the LCO surface through coordination between cyano groups (–CN) and cobalt (Co) atoms. Exhibiting repulsive interactions with the solvent and attractive interactions with the anion through anion–π interactions, BFBN suppresses carbonate solvent dehydrogenation while promoting the decomposition of PF<small><sub>6</sub></small><small><sup>−</sup></small> anions to form an inorganic-rich CEI. A 1 wt% addition of BFBN enables 4.55 V-graphite‖LCO pouch cells to achieve a lifespan over 550 cycles at 25 °C and more than 145 cycles at 45 °C, significantly surpassing the lifespan of around 110 and 50 cycles observed in the baseline electrolyte. This work provides new insights into the design of high-voltage electrolyte additives for high-energy-density LIBs.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 23","pages":" 9185-9194"},"PeriodicalIF":32.4,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142448185","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}