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The rational design of Zn anode/electrolyte interphases (AEIs) is an effective strategy for regulating the Zn stripping/plating process, as well as suppressing the interfacial side reactions. However, the formation of defects during the cycling process is still inevitable, and the exacerbation of defects would lead to the failure of the electrode, limiting the long-term stability of the Zn anode. In recent years, self-healing AEIs (SAEIs) have received great attention in Zn anode modification, as they can self-heal and suppress the defects. This review summarizes the latest progress of SAEIs for Zn anode, including extrinsic and intrinsic SAEIs. Specifically, the design strategies and self-healing mechanisms of SAEIs, their roles in stabilizing Zn anode, as well as the research methods for self-healing performance, are discussed in detail. In addition, the challenges for the research of SAEIs are also analyzed, and prospects for the future design and research of SAEIs for Zn anode are provided. This review is expected to guide the future development of high-performance SAEIs for Zn and other metal anodes.
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http://dx.doi.org/10.1002/adma.202505982 | DOI Listing |
Angew Chem Int Ed Engl
September 2025
State Key Laboratory for Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, School of Physics and Electronics, Hunan Key Laboratory of Two-Dimensional Materials, Chongqing Research Institute, Hunan University, Changsha, 410082, P.R. China.
Controlling the electrode-electrolyte interfacial behavior is crucial for achieving a high-quality solid electrolyte interphase (SEI) and ensuring sustainable battery performance. Here, we propose a selective catalysis strategy to stabilize antimony atom-cluster (Sb) anode/electrolyte interface for robust potassium-ion batteries (PIBs). Specifically, the electrode featuring Sb in porous carbon (Sb/PC) as "electrocatalyst" unduly catalyzes the reduction of the dimethyl ether-based electrolyte, resulting in loose SEI layer and rapid capacity decay.
View Article and Find Full Text PDFJ Am Chem Soc
September 2025
Department of Chemical Engineering, Tsinghua University, Beijing 100084, China.
Molecular engineering of electrolytes for practical high-power and high-energy lithium metal batteries (LMBs) is a significant challenge due to the difficulty of simultaneously achieving high Li transport efficiency, minimal gas evolution, and stable cathode-electrolyte and anode-electrolyte interphases (CEI and SEI, respectively), with low charge-transfer resistance. Here, we introduce a fluorinated asymmetric lithium salt, lithium (2-(2-(2,2-difluoroethoxy)ethoxy)ethyl) ((trifluoromethyl)sulfonyl)amide (LiFOA), designed to optimize electrolyte physicochemical/electrochemical properties for stable LMB pouch cells under fast cycling conditions. LiFOA features a Li-affinitive side chain, which folds up and suppresses anion migration, resulting in a significantly heightened Li transference number ().
View Article and Find Full Text PDFJ Phys Chem C Nanomater Interfaces
August 2025
Department of Chemical Engineering, Department of Chemistry, Department of Materials Science and Engineering, Texas A&M University, College Station, Texas 77843, United States.
In this work, we report the results of a theoretical-computational analysis of the solid electrolyte interphase (SEI) growth and degradation dynamics occurring in lithium metal batteries during cycling. We use ab initio-kinetic Monte Carlo simulations to generate a synthetic data set, which is analyzed by machine learning methods. We aim to determine: (i) how modifications in interfacial interaction energies between solid electrolyte interphase (SEI) blocks and between Li ions and SEI facets impact the Coulombic efficiency (CE) of the battery and (ii) what factors, including reactions, microscopic transport, and other interfacial events, may lead to cell performance "failure" during prolonged charge and discharge cycles, signaled as a sharp decay in the CE over cycling.
View Article and Find Full Text PDFChem Sci
August 2025
Department of Materials Science and Engineering, City University of Hong Kong Kowloon Hong Kong 999077 China
Potassium (K) metal anodes have attracted widespread attention in the realm of energy storage due to their cost-effectiveness, abundance, and high theoretical capacity. However, the undesirable K-dendrite growth accompanied by void formation upon prolonged cycling presents formidable obstacles to their real-world applications. Herein, phosphorus-based electrolytes are developed based on the electrolyte additive design criteria of steric hindrance, polar ability, and decomposition preference to enhance the anode/electrolyte interface stability.
View Article and Find Full Text PDFACS Appl Mater Interfaces
July 2025
Beijing Key Laboratory for Theory and Technology of Advanced Cell Materials, School of Materials Science and Engineering, Peking University, Beijing 100871, China.
The practical application of a lithium (Li) metal anode is limited by the uncontrolled growth of Li dendrites during cycling. Here, we present a rationally designed trilayer protective coating for stabilizing the Li anode at high current densities. The protective coating is designed to consist of silver (Ag), lithium fluoride (LiF), and poly(ethylene oxide) (PEO), in which the Ag layer facilitates rapid Li transfer and uniform deposition, benefiting high current density operations.
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