Hwiyoon Noh, Hyunki Yeo, Bryan W Boudouris, Brian M. Tackett
{"title":"Conducting Polymer Transforms Hydrophobic Porous Membranes into Robust Gas Diffusion Layers in Electrochemical Applications","authors":"Hwiyoon Noh, Hyunki Yeo, Bryan W Boudouris, Brian M. Tackett","doi":"10.1039/d4ee04163a","DOIUrl":"https://doi.org/10.1039/d4ee04163a","url":null,"abstract":"The increasing demand for sustainable chemical production due to strict regulations for carbon emission aligns with growing availability of solar and wind energy, making electrochemical manufacturing a viable route toward decarbonized chemical syntheses. Electrodes with gas diffusion layers (GDLs) critically enhance reaction efficiency for continuous-flow electrochemical reactors with liquid electrolytes fed with gaseous reactants, but they currently suffer from challenges like electrolyte flooding and poor long-term stability. Porous polytetrafluoroethylene (PTFE) membrane-based GDLs overcome some of these issues, but they require additional functionality to enable conductivity. Herein, we demonstrate a novel GDL structure, introducing a porous conductive polymer, poly(3,4-ethylenedioxythiophene) (PEDOT), onto a porous PTFE membrane. Compared to a carbon-based GDL, the PEDOT-coated PTFE GDL exhibited similar electrochemical performance with enhanced stability under industrially relevant conditions for the CO2 reduction reaction. PEDOT-coated PTFE GDL demonstrates remarkable resistance to electrolyte flooding, making it a promising candidate for various gas-fed electrocatalytic reactions.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"113 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142805267","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}
{"title":"Engineered biocatalytic architecture for enhanced light utilisation in algal H2 production","authors":"Sergey Kosourov, Tekla Tammelin, Yagut Allahverdiyeva","doi":"10.1039/d4ee03075c","DOIUrl":"https://doi.org/10.1039/d4ee03075c","url":null,"abstract":"Thin-layer photosynthetic biocatalysts (PBCs) offer an innovative and promising approach to the solar-powered generation of renewable chemicals and fuels. Thin-layer PBCs incorporate photosynthetic microbes, engineered for the production of targeted chemicals, into specifically tailored bio-based polymeric matrices. This unique integration forms a biocatalytic architecture that allows controlled distribution of light, nutrients, and substrates to the entrapped cells, optimising their performance. The research outlined in this study offers a systematic engineering approach to developing a biocatalytic architecture with improved light utilisation and enhanced photosynthetic conversion of captured light energy to molecular hydrogen (H<small><sub>2</sub></small>), an important energy carrier and fuel. This was achieved by entrapping wild-type green alga <em>Chlamydomonas reinhardtii</em> and its mutants with truncated light-harvesting chlorophyll antenna (Tla) complexes within thin-layer (up to 330 μm-thick) polymeric matrices under sulphur-deprived conditions. Our step-by-step engineering strategy involved: (i) synchronising culture growth to select cells with the highest photosynthetic capacity for entrapment, (ii) implementing a photosynthetic antenna gradient in the matrix by placing Tla cells atop the wild-type algae for better light distribution, (iii) replacing the conventional alginate formulation with TEMPO-oxidised cellulose nanofibers for improved matrix stability and porosity, and (iv) employing a semi-wet production approach to simplify the removal of produced H<small><sub>2</sub></small> from the matrix with entrapped cells, thus preventing H<small><sub>2</sub></small> recycling. The engineered PBCs achieved a fourfold increase in H<small><sub>2</sub></small> photoproduction yield compared to conventional alginate films under the same irradiance (0.65 <em>vs</em>. 0.16 mol m<small><sup>−2</sup></small> under 25 μmol photons m<small><sup>−2</sup></small> s<small><sup>−1</sup></small>, respectively) and maintained H<small><sub>2</sub></small> photoproduction activity for over 16 days. This resulted in a remarkable 4% light energy to hydrogen energy conversion efficiency at peak production activity and over 2% throughout the entire production period. These significant advancements highlight the potential of engineered thin-layer PBCs for efficient H<small><sub>2</sub></small> production. The technology could be adapted for biomanufacturing various renewable chemicals and fuels.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"21 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142805269","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}
Yan-Song Zhang, Hasan Arif Yetkin, Hakam Agha, Sevan Gharabeiki, Rijeesh Kizhakidathazhath, Lena Merges, Ricardo G. Poeira, Jan P. F. Lagerwall, Phillip J. Dale
{"title":"Arbitrary and active colouring of solar cells with negligible loss of efficiency","authors":"Yan-Song Zhang, Hasan Arif Yetkin, Hakam Agha, Sevan Gharabeiki, Rijeesh Kizhakidathazhath, Lena Merges, Ricardo G. Poeira, Jan P. F. Lagerwall, Phillip J. Dale","doi":"10.1039/d4ee03010a","DOIUrl":"https://doi.org/10.1039/d4ee03010a","url":null,"abstract":"While the current surging global energy crisis highlights the urgent need for a transition to renewable energy sources, the large physical footprint—as experienced by humans—of the required installations reduces public acceptance and therefore strongly hampers its development. Solar modules, for electricity and/or for heating, do not have the audible impact of wind turbines but their visible impact is currently prohibitive for many installation options, such as on the façades of buildings. Here we show that coatings of cholesteric liquid crystals (CLCs) can turn any black solar modules into passive surfaces with arbitrary colour or active surfaces with temperature sensitive colouration, yet with minimum loss of power conversion efficiency (PCE), thanks to their self-organized helical modulation generating structural colour. Most conspicuously, we combine red, green, and blue pixels to generate a non-spectral colour that blends into wooden or metallic backgrounds with a 50% relatively higher PCE than a ceramic ink equivalent since CLCs neither absorb nor scatter light. Further, we show thermochromic solar cells with colour tunable across the full visible spectrum, maintaining 88% of their original PCE. We argue these coatings can be developed to cover solar modules with either arbitrary full-colour images, allowing them to be aesthetically integrated into building façades and roofs in a way that is fully acceptable by the public, or with active colour changing to add functional value, while always keeping high PCE.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"200 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797214","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}
Yan Zhang, Kaiyu Feng, Miao Song, Shan Xiang, Yan Zhao, Hanyu Gong, Fan Ni, Felix Dietrich, Lovro Fulanović, Fangping Zhuo, Gerd Buntkowsky, Till Frömling, Dou Zhang, Chris Bowen, Jürgen Rödel
{"title":"Dislocation-engineered piezocatalytic water splitting in single-crystal BaTiO3","authors":"Yan Zhang, Kaiyu Feng, Miao Song, Shan Xiang, Yan Zhao, Hanyu Gong, Fan Ni, Felix Dietrich, Lovro Fulanović, Fangping Zhuo, Gerd Buntkowsky, Till Frömling, Dou Zhang, Chris Bowen, Jürgen Rödel","doi":"10.1039/d4ee03789h","DOIUrl":"https://doi.org/10.1039/d4ee03789h","url":null,"abstract":"The rapid development of society has exacerbated energy scarcity, making water splitting a promising solution for humanity to produce green hydrogen. Therefore, enhancing the relatively low catalytic performance of piezoelectric bulk catalysts is crucial to unlocking their potential for broader practical applications and potentially alleviating contemporary energy demands. Here, we introduce a sustainable doping strategy that deliberately imprints dislocations and their associated strain fields without additional elements into barium titanate single crystals to address the challenges faced by bulk piezoelectric catalysts. The presence of highly-oriented {100}〈100〉 dislocations in plastically deformed materials was observed utilizing bright-field transmission electron microscopy. The strains induced by dislocations were mapped using high-angle annular dark-field and geometric phase analysis techniques. According to experimental observations and density functional theory calculations, the deformed materials exhibit superior performance in terms of electrical conductivity, ultrasonic response, and hydrogen adsorption-free energy. As result a nearly fivefold increase in piezoelectric catalytic performance, as compared to undeformed reference materials, is achieved. Our work demonstrates the potential of dislocation engineering to boost bulk piezoelectric catalysts, thereby challenging the current reliance on powder-based catalysts.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"20 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797212","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}
{"title":"Manipulating Crystallization Kinetics and Vertical Phase Distribution via Small Molecule Donor Guest for Organic Photovoltaic Cells with 20% Efficiency","authors":"Bo Cheng, Wenwen Hou, Chenyu Han, Sixuan Cheng, Xinxin Xia, Xia Guo, Yongfang Li, Maojie Zhang","doi":"10.1039/d4ee04623d","DOIUrl":"https://doi.org/10.1039/d4ee04623d","url":null,"abstract":"Precise control over molecular crystallization and vertical phase distribution of photovoltaic bulk-heterojunction (BHJ) films is crucial for enhancing their optoelectronic properties toward high-performing polymer solar cells (PSCs). Herein, a kinetics-controlling strategy is implemented in the PM6:L8-BO blend system by introducing a small molecule donor (SMD), namely BTR-SCl, which possesses strong crystallization property and excellent miscibility with the host polymer donor. The in-situ spectroscopy characterizations indicate that BTR-SCl can effectively advance the aggregation of PM6 from the blend solution and prolong its self-assembly time during the film formation process, which leads to well-defined vertical phase distribution with more ordered polymer donor enriched at the anode, effectively facilitating charge transport and collection, alleviating trap density and energetic disorder, and reducing energy loss. Ultimately, the PM6:BTR-SCl:L8-BO ternary PSCs (T-PSCs) achieve a remarkably enhanced power conversion efficiency (PCE) of 19.4% in comparison with 18.0% for the binary device. Notably, by replacing PM6 with D18, the PCE of ternary devices is further boosted to 20.0%, which represents the highest efficiency for SMD-based T-PSCs reported to date. Our findings elucidate the great potential of crystalline SMD in optimizing the vertical phase distribution and molecular packing within BHJ film, leading to considerable improvements in the PCE of PSCs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"9 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797213","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}
Seongbeen Kim, Seung-Jae Shin, Hoyoung Kim, Bupmo Kim, Namgyu Noh, Kug-Seung Lee, Jinkyu Park, Hyunwoo Jun, Jiwon Kim, Jaeho Byeon, Seonggyu Lee, Huawei Huang, Sunghyun Noh, Han Beom Jeong, Jong Hyun Jang, Jongmin Yuk, Wooyul Kim, Hyungjun Kim, Jinwoo Lee
{"title":"Self-Assembly-Assisted Dynamic Placement of Noble Metals Selectively on Multifunctional Carbide Supports for Alkaline Hydrogen Electrocatalysis","authors":"Seongbeen Kim, Seung-Jae Shin, Hoyoung Kim, Bupmo Kim, Namgyu Noh, Kug-Seung Lee, Jinkyu Park, Hyunwoo Jun, Jiwon Kim, Jaeho Byeon, Seonggyu Lee, Huawei Huang, Sunghyun Noh, Han Beom Jeong, Jong Hyun Jang, Jongmin Yuk, Wooyul Kim, Hyungjun Kim, Jinwoo Lee","doi":"10.1039/d4ee04660a","DOIUrl":"https://doi.org/10.1039/d4ee04660a","url":null,"abstract":"Atomically dispersed catalysts are ideal for alkaline hydrogen electrocatalysis with low noble metal loadings. However, previous designs have exhibited insufficient *OH binding and low cell performance, which limit their application in anion-exchange membrane water electrolyzers. In this study, we employed a self-assembly-assisted dynamic placement to prepare atomically dispersed electrocatalysts on heterostructured Mo<small><sub>x</sub></small>C-C. The multifunctional Mo<small><sub>x</sub></small>C support bolsters the dynamic placement while optimizing the interfacial water structure. The self-assembly-assisted dynamic placement facilitates the selective loading of atomically dispersed noble metals on Mo<small><sub>x</sub></small>C at 1,373 K by leveraging molecular interactions and metal-support interactions. The dynamic placement enables the construction of interfacial active systems between noble metals and Mo<small><sub>x</sub></small>C, enhancing the reaction kinetics, stability, and CO tolerance of alkaline hydrogen electrocatalysis. Specifically, selective loading enables the effective utilization of *OH binding sites on Mo<small><sub>x</sub></small>C, promoting water dissociation by increasing the free-water population in the interfacial water structure. In an anion-exchange membrane water electrolyzer, the designed catalysts exhibited higher cell stability (500 h) than commercial PtRu/C. They also exhibited enhanced performance even with a low noble metal loading (0.060 mg<small><sub>Pt</sub></small> cm<small><sup>-2</sup></small>), achieving the US Department of Energy’s 2026 target for proton-exchange membrane water electrolyzers.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"28 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793721","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}
Hyeseong Oh, Gyu-sang Kim, Jiyoon Bang, San Kim, Kyeong-Min Jeong
{"title":"Dry-processed thick electrode design with porous conductive agent enabling 20 mA h cm-2 for high-energy-density lithium-ion Battery","authors":"Hyeseong Oh, Gyu-sang Kim, Jiyoon Bang, San Kim, Kyeong-Min Jeong","doi":"10.1039/d4ee04106b","DOIUrl":"https://doi.org/10.1039/d4ee04106b","url":null,"abstract":"Designing thick electrodes is essential for the applications of lithium-ion batteries that demand high energy density. Introducing a dry electrode process that does not require solvents during electrode fabrication has gained significant attention, enabling the production of homogeneous electrodes with significantly higher areal capacity than the conventional wet electrode process. This study reports the importance of selecting appropriate conductive agents for dry-processed electrodes and optimizing the electrode composition based on the design principles by electrode parameters. By applying various conductive agents in the dry process, we discovered that the porous spherical conductive agent improves both the electrical performance and lithium-ion transport characteristics, which are difficult to incorporate in conventional wet processes. Additionally, optimizing the content of the porous spherical conductive agents within the range of 2–3 wt% through the analysis of electrode parameters enables the fabrication of high-energy-density cathodes with areal capacities of 10–20 mA h cm<small><sup>-2</sup></small> and a composite density of 3.65 g cm<small><sup>-3</sup></small>. This dry-processed cathode outperforms graphene- or carbon nanotube-based cathodes, showing excellent rate performance (88% capacity at 1 C) and outstanding cycle life (80% capacity retention at the 418th cycle).","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"121 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793790","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}
{"title":"Collaborative multi-interface engineering and dynamic iron exchange boost robust bifunctional water electrolysis at 2 A cm-2","authors":"Dongyang Li, Yong Zhang, Weiqiang Xie, Qian Zhou, Fang Yu, Ying Qi, Ziyi Lian, Long Zhang, Hui Wang, Dongsheng Tang, Haiqing Zhou","doi":"10.1039/d4ee04619f","DOIUrl":"https://doi.org/10.1039/d4ee04619f","url":null,"abstract":"Due to the incompatibility and inconsistence of the active species for hydrogen and oxygen evolution reactions, nearly all the intermetallic catalysts present superb catalytic activity for one half reaction at the expense of another reaction activity, thus leading to large electric power consumption of alkaline water splitting. To achieve low-voltage electrochemical H2 production through water electrolysis, here we present a hierarchical trimetal hybrid catalyst comprising intermetallic nickel-molybdenum alloy (MoNi4) particles and metallic iron particles anchoring on MoO2 nanorod arrays with synergistic multimetal sites that exhibits relay catalysis for bifunctional water splitting as rationalized by operando Raman, X-ray photoelectron spectroscopic studies and density functional theory (DFT) calculations. These metal sites situated on the multilevel interfaces of Fe/MoNi4/MoO2 collaboratively promote the reaction pathway including initial water adsorption/dissociation, hydrogen adsorption and oxygen-containing intermediate adsorption, thereby substantially jeopardizing overall water splitting at 500/1000 mA cm-2 with record low cell voltages of around 1.6 V, which is exceptionally better than noble IrO2(+)||Pt/C(-) couple electrodes (> 1.9 V). This intermetallic catalyst demands extremely low overpotentials of 59 and 277 mV for hydrogen and oxygen evolution reactions at 500 mA cm-2, respectively, outperforming nearly all the inexpensive bifunctional electrocatalysts. Especially, this catalyst can survive its superior catalytic performance at an industrial-level current density of 500-2000 mA cm-2 without noticeable degradation. This work paves a promising avenue to develop efficient bifunctional non-noble catalysts for industrial-level water electrolysis via relay catalysis.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"27 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142782946","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}
{"title":"Rational Catalyst Layers Design Enables Tailored Transport Channels for Efficient CO2 Electrochemical Reduction to Multi-carbon Products","authors":"Jiping Sun, Bichao Wu, Zhixing Wang, Huajun Guo, Guochun Yan, Hui Duan, Guangchao Li, Ying Wang, Jiexi Wang","doi":"10.1039/d4ee03743j","DOIUrl":"https://doi.org/10.1039/d4ee03743j","url":null,"abstract":"Membrane electrode assemblies (MEAs) have been developed for electrochemical conversion of CO2 to high-value multi-carbon (C2+) products at industrial current densities (j>200 mA cm-2). However, the effective and simultaneous modulation of CO₂ and H₂O mass transfer within MEA remains a critical issue, particularly at the three-phase interface. Herein, CO2 and H2O channels are designed in the catalyst layer network to benefit the micro-environment. The balance of local CO2 and H2O at the reaction interface is attained by regulating the catalyst-coated ionomer. In-situ DEMS further confirms that the rational routes are successfully established for mass transfer management. The interfacial distribution of CO2 and H2O are in-depth investigated by in-situ ATR-SEIRAS and molecular dynamics (MD) simulation. By reasonable catalyst layers design, CO2-to-C2+ performance is substantially enhanced, which exhibits remarkable selectivity to C2+ products with a faradaic efficiency (FE) of 89.4±0.69% and a partial current density of 536±4.14 mA cm-2. The optimized Cu-GDE also exhibits excellent stability of >10h at a total current of 2 A.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"17 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142777091","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}
Fangkun Li, Yanchen Lin, Junhao Liu, Jiahe Chen, Xuanhong Wan, Linwei Zhao, Lei Xi, Zheng Li, Hangyu Zhang, Xijun Xu, Zhidu Zhou, Baitao Su, Min Zhu, Jun Liu
{"title":"Boosting oxygen redox reversibility in chemo-mechanically robust Li-rich oxides cathode via multi-scale defect design","authors":"Fangkun Li, Yanchen Lin, Junhao Liu, Jiahe Chen, Xuanhong Wan, Linwei Zhao, Lei Xi, Zheng Li, Hangyu Zhang, Xijun Xu, Zhidu Zhou, Baitao Su, Min Zhu, Jun Liu","doi":"10.1039/d4ee04266b","DOIUrl":"https://doi.org/10.1039/d4ee04266b","url":null,"abstract":"Li-rich oxides (LROs) cathode can deliver high-energy density established on the synergistic effect of cation and anion redox. However, continued accumulation of lattice strain and irreversible oxygen-anion redox reactions generate severe mechanically failure and rapid voltage decay in lithium-ion batteries (LIBs). Herein, we constructed a layered-spinel lattice-matched epitaxial structure with delocalized Li@Mn6 superstructural units to intercept lattice strain-induced structural evolution and facilitate oxygen redox reversibility. This multiscale regulation strategy was realized by the agency of tailoring the excess-Li distribution with the property of enhancing the cathode electrolyte interfacial (CEI) stability and prevent the rapid performance decay of LROs. The modified LROs achieved significant improvements, including uniform current distribution, minimal lattice strain change (0.00179), impressive initial Coulombic efficiency (87.1%), exceptional thermal stability and enhanced cycle stability. Specifically, the capacity retention of the pristine LROs increased from 47.6% to 90.8% after 400 cycles. These results highlight the outstanding electro-chemo-mechanical stability of the modified LROs. Therefore, this multiscale defect-regulated strategy could help to solve the structural collapse and electrochemical decay caused by irreversible anionic redox in practical application of LROs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"36 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142782942","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}