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Constructing 3D skeletons modified with lithiophilic seeds has proven effective in achieving dendrite-free lithium metal anodes. However, these lithiophilic seeds are mostly alloy- or conversion-type materials, and they tend to aggregate and redistribute during cycling, resulting in the failure of regulating Li deposition. Herein, we address this crucial but long-neglected issue by using intercalation-type lithiophilic seeds, which enable antiaggregation owing to their negligible volume expansion and high electrochemical stability against Li. To exemplify this, a 3D carbon-based host is built, in which ultrafine TiO seeds are uniformly embedded in nitrogen-doped hollow porous carbon spheres (N-HPCSs). The TiO@N-HPCSs electrode exhibits superior Coulombic efficiency, high-rate capability, and long-term stability when evaluated as compertitive anodes for Li metal batteries. Furthermore, the superiority of intercalation-type seeds is comprehensively revealed through controlled experiments by various in situ/ex situ electron and optical microscopies, which highlights the excellent structural stability and lithiophilicity of TiO nanoseeds upon repeated cycling.
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http://dx.doi.org/10.1021/acs.nanolett.2c01736 | DOI Listing |
Small Methods
August 2025
Department of Energy System Engineering, Gyeongsang National University, Jinju-si, Gyeongnam, 52849, South Korea.
Anode-less lithium-sulfur (Li-S) batteries offer a promising route to high energy density and cost-effective energy storage, yet suffer from unstable Li deposition and polysulfide crossover at the current collector interface. Here, we introduce a hybrid interfacial modulation layer (HIML) designed to simultaneously regulate dendrite-free Li deposition behavior and block polysulfide migration. The HIML consists of lithiophilic Au nano seeds coated with a porous ionic-selective overlayer, enabling guided, uniform Li nucleation and selective Li transport.
View Article and Find Full Text PDFSmall
August 2025
Department of Applied Bioengineering, Graduate School of Convergence Science and Technology, Seoul National University, Suwon-si, Gyeonggi-do, 16229, Republic of Korea.
3D Li hosts with lithiophilic gradient structure are extensively explored to mitigate Li dendrite formation by promoting bottom-up Li plating and reducing local current density. However, the absence of well-defined nano-ionic channels in these designs limits their ability to regulate Li distribution, leading to uncontrolled Li dendrite growth under high current densities and large areal capacities. Herein, this study presents a novel graphene-based 3D Li host that integrates nano-ionic channel network into a lithiophilic gradient structure, denoted as IC-GGLH.
View Article and Find Full Text PDFNat Commun
July 2025
School of Chemical and Biological Engineering and Institute of Chemical Processes, Seoul National University, Seoul, Republic of Korea.
Achieving stable cyclability in initially anode-free all-solid-state batteries is challenging due to non-uniform Li (de)plating, especially under practical operating conditions. Here, we introduce a bilayer comprising a silver(Ag)-doped Li-argyrodite electrolyte layer in contact with the undoped Li-argyrodite electrolyte. During charging, electrochemical exsolution of Ag from the silver-doped Li argyrodite forms nanoscale, lithiophilic silver seeds along grain boundaries and in pores where they are accessible for electron transfer.
View Article and Find Full Text PDFEES Batter
June 2025
School of Chemical and Biological Engineering and Institute of Chemical Process, Seoul National University 1 Gwanak-ro Gwanak-gu Seoul 08826 Republic of Korea
Anode-less all-solid-state batteries (ALASSBs) represent a promising energy storage platform for various upcoming green mobility applications, as they offer superior energy density, manufacturing feasibility, and enhanced safety. However, their practical implementation is hindered by the formation of heterogeneous lithium (Li) deposits during repeated cycling, particularly at ambient temperatures. In this study, we introduce a novel multi-seed strategy that integrates strategically distributed nucleation sites with a highly elastic and adhesive polymer matrix.
View Article and Find Full Text PDFACS Nano
December 2024
Department of Chemical Engineering, Hanyang University, Seoul, 04763, Republic of Korea.
Dendritic challenges in Li metal batteries are commonly resolved using porous three-dimensional (3D) current collectors, which have a significant issue in that Li is deposited from the top (top growth) of the structure rather than from the bottom (bottom growth), failing to effectively suppress dendrite growth and volumetric expansion. We propose the structure incorporating a gradient lithiophilic seed within a 3D framework by pulse electroplating Mg, specifically targeting the near bottom to promote bottom growth and achieve dense Li deposition. This method achieves precise control over the catalytic seed size and distribution.
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