Advanced Energy Materials最新文献

{"title":"The Origin of Li2S2 Reduction Mechanism Modulated by Single-Atom Catalyst for all Solid-State Li-S Batteries","authors":"Miao He, Yuxing Fan, Shen Liu, Shuying Wang, Tongwei Wu, Dongjiang Chen, Anjun Hu, Chaoyi Yan, Yichao Yan, Jianping Long, Yin Hu, Tianyu Lei, Peng Li, Wei Chen","doi":"10.1002/aenm.202405642","DOIUrl":"https://doi.org/10.1002/aenm.202405642","url":null,"abstract":"All solid-state lithium-sulfur batteries (ASSLSBs) demonstrate tremendous potential in the next-generation energy storage system. Nevertheless, the incomplete conversion of Li<sub>2</sub>S<sub>2</sub> to Li<sub>2</sub>S within the sulfur electrode imposes a substantial impediment on the capacity release. Herein, the nickel single-atom catalyst (NiNC) materials are employed to ameliorate the sluggish reaction kinetics of polysulfides. Moreover, the unknown origin of the catalytic activity of NiNC materials on the ASSLSBs is revealed by using the ligand-field theory. The results show that the <span data-altimg=\"/cms/asset/b7f2f832-c7cd-4d00-ad00-30de44cc9615/aenm202405642-math-0001.png\"></span><mjx-container ctxtmenu_counter=\"1\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" role=\"application\" sre-explorer- style=\"font-size: 103%; position: relative;\" tabindex=\"0\"><mjx-math aria-hidden=\"true\" location=\"graphic/aenm202405642-math-0001.png\"><mjx-semantics><mjx-msub data-semantic-children=\"0,3\" data-semantic- data-semantic-role=\"latinletter\" data-semantic-speech=\"d Subscript z squared\" data-semantic-type=\"subscript\"><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"italic\" data-semantic- data-semantic-parent=\"4\" data-semantic-role=\"latinletter\" data-semantic-type=\"identifier\"><mjx-c></mjx-c></mjx-mi><mjx-script style=\"vertical-align: -0.184em;\"><mjx-msup data-semantic-children=\"1,2\" data-semantic- data-semantic-parent=\"4\" data-semantic-role=\"latinletter\" data-semantic-type=\"superscript\" size=\"s\"><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"italic\" data-semantic- data-semantic-parent=\"3\" data-semantic-role=\"latinletter\" data-semantic-type=\"identifier\"><mjx-c></mjx-c></mjx-mi><mjx-script style=\"vertical-align: 0.289em;\"><mjx-mn data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"3\" data-semantic-role=\"integer\" data-semantic-type=\"number\" size=\"s\"><mjx-c></mjx-c></mjx-mn></mjx-script></mjx-msup></mjx-script></mjx-msub></mjx-semantics></mjx-math><mjx-assistive-mml display=\"inline\" unselectable=\"on\"><math altimg=\"urn:x-wiley:16146832:media:aenm202405642:aenm202405642-math-0001\" display=\"inline\" location=\"graphic/aenm202405642-math-0001.png\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><semantics><msub data-semantic-=\"\" data-semantic-children=\"0,3\" data-semantic-role=\"latinletter\" data-semantic-speech=\"d Subscript z squared\" data-semantic-type=\"subscript\"><mi data-semantic-=\"\" data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"italic\" data-semantic-parent=\"4\" data-semantic-role=\"latinletter\" data-semantic-type=\"identifier\">d</mi><msup data-semantic-=\"\" data-semantic-children=\"1,2\" data-semantic-parent=\"4\" data-semantic-role=\"latinletter\" data-semantic-type=\"superscript\"><mi data-semantic-=\"\" data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"italic\" data-semantic-parent=\"3\" data-semantic-role=\"latinletter\" data-semantic-type=\"identifi","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"57 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385847","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":"PC-Derived SEI Film to Stabilize Graphite|Electrolyte Interface in Sulfone-Based Electrolyte for Advanced Lithium-Ion Batteries","authors":"Xinan Yan, Kean Chen, Hui Chen, Zhongxue Chen, Xinping Ai, Yuliang Cao","doi":"10.1002/aenm.202404992","DOIUrl":"https://doi.org/10.1002/aenm.202404992","url":null,"abstract":"Solid electrolyte interphase (SEI) plays a crucial role in stabilizing the anode-electrolyte interface of lithium-ion batteries. To date, extensive efforts are dedicated to the regulation of the SEI's compositions, instead the dissolution of the SEI in the electrolyte, an important factor that significantly influences the interfacial stability, received less attention. In this work, it is discovered for the first time that the dissolution of propylene carbonate (PC)-derived SEI can be restrained by employing tetramethylene sulfone (TMS) as the main solvent, thereby markedly enhancing the interfacial stability of Li||graphite half-cell and high-voltage graphite||LiCoO₂ full cell. Undoubtedly, this work provides a new electrolyte design principle for developing many solvents that are previously considered detrimental in batteries to establish robust interfaces by minimizing the solubility of SEI.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"21 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385851","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":"Configuration Design and Interface Reconstruction to Realize the Superior High-Rate Performance for Sodium Layered Oxide Cathodes","authors":"Jiandong Zhang, Zhaoshi Yu, Yanbin Zhu, Jingyao Cai, Muqin Wang, Pengkun Gao, Yali Zhang, Naiqing Zhang, Deyu Wang, Yan Shen, Mingkui Wang","doi":"10.1002/aenm.202405951","DOIUrl":"https://doi.org/10.1002/aenm.202405951","url":null,"abstract":"Charge transfer at the electrode/electrolyte interface and mass transfer within the electrode are the two main factors affecting the high-rate performance of O3-type layered oxide cathodes for sodium-ion batteries. Here a multidimensional lanthurization strategy is proposed to construct the surface LaCrO₃ heterostructure and create a Cr─O─La configuration for O3-type NaCrO₂. The electrified heterogeneous LaCrO₃ induces a built-in electric field to accelerate charge transfer at the interface. Meanwhile, the Cr─O─La configuration in the transition metal layer leads to local charge aggregation, weakens the interaction force between Na─O, and reduces the Na⁺ migration barrier. This strategy significantly improves the electrochemical reaction kinetics and the structural reversibility of the layered oxide cathode. As a result, the designed stoichiometric ratio Na_0.94Cr_0.98La_0.02O₂ electrode exhibits remarkable rate performance (101.8 mAh g⁻¹ at 40 C) as well as outstanding cycling stability (83.1% capacity retention at 20 C for 2000 cycles) in a half-cell, along with a competitive full battery performance (89.3% after 500 cycles at 2 C). This study provides a promising route to achieve capacity presentation and retention of layered oxide cathode materials at high-rate.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"63 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385849","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":"Prokaryote-Inspired and Derived Oxygen Reduction Electrocatalysts for Ultra-Long-Life Zn–Air Batteries","authors":"Wenbo Zhao, Jipeng Chen, Ximeng Liu, Yong Gao, Jie Pu, Qinghe Cao, Ting Meng, Abdelnaby M. Elshahawy, Salah A. Makhlouf, Cao Guan","doi":"10.1002/aenm.202405594","DOIUrl":"https://doi.org/10.1002/aenm.202405594","url":null,"abstract":"The design of efficient oxygen reductionreaction (ORR) catalyst with fast kinetics is crucial for high-performance Zn–air batteries but remains a challenge. Herein, inspired by the oxidative respiratory chain of prokaryotes, an ORR electrocatalyst is reported by mimicking the microstructure of Staphylococcus aureus and simitaneously utilizing this low-cost cell as the precursor. The catalyst consists of MnO₂/Co₂P nanocomposites support on Staphylococcus aureus-derived hollow spherical carbon, which not only accelerates electron transfer for improved intrinsic reaction kinetics, but also creates an OH⁻ concentration gradient for enhanced mass transfer efficiency. Such bio-inspired and derived ORR catalyst enables rechargeable Zn–air batteries with ultra-long cycling stability of more than 2800 h at a high capacity of 810.3 mAh g⁻¹, which is superior among the reported bio-derived oxygen catalysts. A flexible Zn–air battery based on the bio-inspired and derived catalyst is also assembled, and it well integrates with a wireless flexible electronic skin.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"1 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385845","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":"Elemental Stability Rules for High Entropy Disordered Rocksalt Type Li-Ion Battery Positive Electrodes","authors":"Lin Wang, Neelam Sunariwal, Yufang He, Do-hoon Kim, Dong-hee Yeon, Yan Zeng, Jordi Cabana, Bin Ouyang","doi":"10.1002/aenm.202404982","DOIUrl":"https://doi.org/10.1002/aenm.202404982","url":null,"abstract":"High entropy disordered rocksalt (HE-DRX) Li-ion battery positive electrodes have gained attention as a potential alternative to commercialized positive electrodes, aiming to eliminate or minimize the use of Ni/Co while maintaining competitive electrochemical performance. Despite their potential, understanding the intricate elemental stability across the vast HE-DRX chemical landscape remains a significant challenge. In this study, we tackle this challenge by conducting a comprehensive data-driven phase diagram analysis of 18810 potential HE-DRX compositions, each featuring common Li and F stoichiometries. Leveraging a charge balance algorithm, we systematically explore redox stability and phase stability, unveiling critical insights into chemical stability rules within the HE-DRX design space. The analysis also uncovers untapped potential of Cu as redox-active centers, with Sb and Sn contributing as stable charge compensators. The utilization of these elements is seldom reported in the literature but has been validated by the successful experimental synthesis of materials Li₂₁Zr₃Ti₃Mn₂Fe₅Cu₂O₃₆ and Li₂₁Mn₂Ti₃Fe₅Cu₂Sn₃O₃₆.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"19 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385852","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":"Adjustable Selectivity for CO2 Electroreduction to Ethylene or Ethanol by Regulating Interphases Between Copper and Tin Oxides","authors":"Huan Liu, Chenghan Yang, Tong Bian, Huijun Yu, Yuming Zhou, Yiwei Zhang, Li Sun","doi":"10.1002/aenm.202405658","DOIUrl":"https://doi.org/10.1002/aenm.202405658","url":null,"abstract":"Enhancing the selectivity of C₂ products and revealing the reaction mechanisms in CO₂ electroreduction reaction (CO₂RR) remain challenging. Regulating the interphases in catalysts is one of the most promising pathways. Herein, the interphases between copper (Cu) and tin (Sn) oxides are regulated by controlling the degree of reduction during the self-assembly process, which exhibits obvious different selectivity to ethylene and ethanol, respectively. The interphase in Cu-SnO₂ exhibits selectivity to ethanol as high as 74.6%, while the interphase in Cu₂O-SnO₂ shows selectivity to ethylene as high as 71.4% at –0.6 V versus RHE. In situ Fourier-transform infrared spectroscopy measurements and density functional theory calculations demonstrate that the interphase in Cu-SnO₂ shows strong electron interaction, preferentially forming the key *COH intermediates for asymmetrical C─C coupling to produce ethanol. In contrast, Cu₂O-SnO₂ possesses oxygen vacancies at both sites, thus enriching *CO intermediates for symmetrical C─C coupling to produce ethylene at the interphase. The findings in this work offer an advanced strategy by regulating the interphases to adjust C₂ selectivity in CO₂RR.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"60 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385846","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":"Electron-Rich Ru Clusters Anchored on Pure Phase W2C Enables Highly Active and CO-Resistant Alkaline Hydrogen Oxidation","authors":"Yanan Gao, Bo Ouyang, Yuan Shen, Wei Wen, Junxiang Wang, Mingzhe Wang, Yiqiang Sun, Kun Xu","doi":"10.1002/aenm.202406114","DOIUrl":"https://doi.org/10.1002/aenm.202406114","url":null,"abstract":"Developing highly active and CO-resistant Ru-based catalysts for the alkaline hydrogen oxidation reaction (HOR) can advance the large-scale application of alkaline hydrogen fuel cells but remains a huge challenge. Herein, a pure phase W₂C supported Ru cluster catalyst (Ru/W₂C) is successfully synthesized through a one-step carburization method. It is found that the charge transfer from W₂C to the strongly anchored Ru clusters forms the electron-rich Ru^δ− sites and electron-deficient W^δ+ sites, which significantly weakens the adsorption strength of ^*H and ^*CO, strengthens the binding of ^*OH and improves the water connectivity in the electric double layer. The Ru/W₂C catalyst shows superior mass activity (2163 mA mg_PGM⁻¹) in alkaline HOR, which is 12.52 and 20.62 times higher than that for Pt/C and Ru/C, respectively. Owing to the weak adsorption and fast removal rate of CO, the Ru/W₂C exhibits outstanding CO tolerance, with 88% of the initial activity being retained in the durability test, whereas the Ru/C and Pt/C suffer from severe deactivation. These findings may guide the design of advanced alkaline HOR catalysts based on the pure phase tungsten carbide.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"55 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385848","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":"Efficient Forward-Bias Bipolar Membrane CO2 Electrolysis in Absence of Metal Cations","authors":"Sven Brückner, Wen Ju, Peter Strasser","doi":"10.1002/aenm.202500186","DOIUrl":"https://doi.org/10.1002/aenm.202500186","url":null,"abstract":"The acid-base reaction of CO₂ with hydroxide ions to (bi)carbonate anions at the cathode of alkaline exchange membrane (AEM) CO₂ electrolyzer has detrimental impact on their performance. (Bi)carbonate buffers the local cathode pH, and in combination with metal cations, may lead to precipitation of salts at the cathode. This non-electrochemical conversion of CO₂ significantly reduces the CO₂ utilization efficiency and limits the CO₂ single pass conversion of AEM CO₂ electrolyzer to 50% if CO is desired. Acidic metal cation-free CO₂ electrolysis has the potential to address and mitigate these problems. Here, CO₂ valorization is demonstrated at faradaic CO efficiencies (FE) of up to 80% FE_CO in forward-bias BPM cell architectures using actual neutral pure water feeding at the anode. This study demonstrates how immobilized anion exchange ionomer layers thereby facilitate the metal cation-free CO₂ valorization thanks to their positively charged functional NR₄ groups. Unlike metal cations, the immobilized positively charged groups are not washed out of the reactor. This study shows that careful design of the distribution and location of the anion exchange ionomer molecules within the Gas Diffusion Electrode is key to efficient CO₂-to-CO electrolyzer cell.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"29 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375628","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":"Structural Influence on Exciton Formation and the Critical Role of Dark Excitons in Polymeric Carbon Nitrides","authors":"Changbin Im, Radim Beranek, Timo Jacob","doi":"10.1002/aenm.202405549","DOIUrl":"https://doi.org/10.1002/aenm.202405549","url":null,"abstract":"Polymeric carbon nitrides (PCNs) exhibit intriguing optical properties and exceptional performance in (photo)catalysis, optoelectronics, and energy storage. Nevertheless, the intricate phenomena involving light absorption, formation of long-lived excitons, photo-charging, and photochemical processes observed in PCNs remain poorly understood. This theoretical investigation elucidates the origin of distinct dark and bright excitons, their stability and lifetimes, and their correlation with the microstructural attributes of PCNs. Based on these results, the decisive role of dark excitons in photocatalytic reactivity is proposed, which underlies the experimentally observed differences in the photocatalytic performance of various PCN derivatives. This study thus establishes novel insights into the factors governing the light-driven processes in PCNs that can provide essential guidelines for rational design of PCNs with enhanced performance.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"12 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375597","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":"High-Entropy Driven Self-Assembled Dual-phase Composite Air Electrodes with Enhanced Performance and Stability for Reversible Protonic Ceramic Cells","authors":"Ao Hu, Chenghao Yang, Yitong Li, Kaisheng Xia, Yunfeng Tian, Jian Pu, Bo Chi","doi":"10.1002/aenm.202405466","DOIUrl":"https://doi.org/10.1002/aenm.202405466","url":null,"abstract":"Reversible proton ceramic cells (R-PCCs) offer a transformative solution for dual functionality in power generation and energy storage. However, their potential is currently obstacles by the lack of high-performance air electrodes combining high electrocatalytic activity with durability. Here, an innovative air electrode composed of high-entropy driven self-assembled xNiO-Pr_0.2La_0.2Ba_0.2Sr_0.2Ca_0.2Fe_0.8Ni_0.2−xO_3−δ (N-XFN) composites is presented, which result from the unique lattice distortion effects inherent in high-entropy perovskites. The experimental results coupled with density functional theory (DFT) calculations verify that the lattice distortion at the high-entropy A-site significantly induces NiO nanoparticles exsolved from the B-site, promoting the formation of a biphasic composite structure that dramatically increases the electrochemical active sites. Remarkably, R-PCCs using the N-XFN composite air electrode achieve an impressive peak power density of 1.30 W cm⁻² in fuel cell mode and a current density of -2.52 A cm⁻² at 1.3 V in electrolysis mode at 650 °C. In addition, the cells show excellent stability with reversibility over 830 h, including 500 h in electrolysis mode and 330 h in reversible operation at 650 °C. This research provides important insights into the design of high-entropy perovskites, paving the way for advanced R-PCCs technology.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"1 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375598","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}