嵌入诱导型层状Nb₂VSe₆/碳纳米纤维膜调控多硫化物转化与锂沉积实现锂硫电池的高稳定性

Embedded Inducible Layered Nb₂VSe₆/Carbon Nanofiber Membrane Regulating Sulfide Conversion and Lithium Deposition to Achieve High-stability of Lithium-Sulfur Batteries

摘要

锂硫电池因其高达1675.0 mA·h/g的理论比容量和2600.0 W·h/kg的能量密度, 被认为是下一代最具应用前景的电化学储能器件之一. 然而, 锂硫电池中硫及硫化锂的氧化还原反应动力学缓慢、 多硫化物穿梭效应以及锂枝晶生长等问题, 严重阻碍了锂硫电池的发展及应用. 本文制备了柔性Nb₃VSe₆/碳纳米纤维复合膜(NVSCNF), 并将其作为锂硫电池的电催化膜反应器(NVS@MR). 通过V原子插层策略, 对2H-NbSe₂进行改性, 构筑了一种嵌入诱导型层状催化剂. NVSCNF对多硫化锂具有强化学吸附能力和优异的电催化活性, 提升了氧化还原反应动力学, 且NVSCNF丰富的活性位点可有效调控锂沉积行为, 抑制枝晶生长. 所组装的锂硫电池在0.1 C倍率下的放电比容量为1305.0 mA·h/g, 在5.0 C高倍率下循环800次后容量仍保持在502.3 mA·h/g, 在0.5 mA/cm²电流密度下可稳定循环超过1000 h, 初始过电位仅为18.3 mV.

Abstract

Lithium sulfur batteries are considered as one of the most promising electrochemical energy storage devices for the next generation due to their theoretical specific capacity of 1675 mA·h/g and energy density of 2600 W·h/kg. However, the slow kinetics of the oxidation-reduction reaction of sulfur and lithium sulfide in lithium sulfur batteries, the shuttle effect of polysulfides, and the growth of lithium dendrites seriously hinder the development and application of lithium sulfur batteries. In this study, a flexible Nb₂VSe₆/carbon nanofiber composite membrane (NVSCNF) was prepared and used as an electrocatalytic membrane reactor (NVS@MR) for lithium-sulfur batteries. A layered catalyst with embedded induction was constructed by modifying 2H-NbSe₂ through V atom intercalation strategy. NVSCNF exhibits strong chemical adsorption capacity and excellent electrocatalytic activity toward lithium polysulfides, enhancing redox kinetics; furthermore, the abundant active sites on NVSCNF effectively regulate lithium deposition behavior and suppress dendrite growth. The assembled lithium-sulfur battery exhibited a discharge specific capacity of 1305.0 mA·h/g at a rate of 0.1 C. After 800 cycles at a rate of 5.0 C, the capacity remained at 502.3 mA·h/g. It could cycle stably for over 1000 h at a current density of 0.5 mA/cm², with an initial overpotential of only 18.3 mV.

关键词

Nb₂VSe₆膜反应器 / V原子插层 / 多硫化物转化 / 锂沉积 / 锂硫电池

Key words

Nb₂VSe₆ membrane reactor / V-atom intercalation / Polysulfide conversion / Lithium deposition / Lithium-sulfur battery

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基金资助

国家自然科学基金(22361035, 22461030)

内蒙古自然科学基金(2024QN02013)

内蒙古草原英才-青年领军人才计划(KYCYYC24001, KYCYYC25002)

内蒙古民族大学博士科研基金(KYQD21002, KYQD23005)

内蒙古自治区直属高校基本科研业务费项目(GXKY25Z009)

内蒙古自治区重点实验室创新平台建设项目(KJJH2402, SYS25003)