Hierarchical Carbon Structures for Advanced High Areal Capacity Lithium-Ion Battery Electrodes
type: CreativeWork
description: The ever-growing energy demand from modern portable electronics and electric vehicles calls for a matching development in lithium-ion batteries (LIBs) that offer high power density, energy density, and long cycle life. However, LIBs based on traditional layered metal oxide cathodes and graphite anodes are quickly approaching their specific energy limits. The exploration of advanced electrode architectures provides a novel route to improving the energy density of LIBs and is often overlooked. This PhD thesis investigates the design, fabrication, and testing of structurally engineered and high areal capacity LIB electrodes based on hierarchical carbon structures such as carbon nanotubes (CNTs). Firstly, (surface-modified) direct-spun CNT mats are proposed as conductive scaffolds for lithium metal anodes (LMAs), which are desirable for next-generation batteries because of their ultra-high energy density. However, the practical applications of LMAs are hindered by the inhomogeneous Li dendrite formation during cycling which leads to poor efficiency and safety issues. The proposed electrode provides ample Li nucleation sites, reduces the local current densities, and promotes uniform Li plating/stripping at selective locations, thus achieving coulombic efficiencies (CEs) of 98-99% for over 130 cycles in CNT|Li half-cells (lithiation capacity: 2.0 mA h cm-2, current density: 1.0 mA cm-2). Next, a freestanding carbon fibre paper with carbon fillers (CFP) electrode is proposed with a novel dual charge storage mechanism – it acts both as a host for Li intercalation and as a conductive, porous, and lithiophilic 3D scaffold for Li plating/stripping. The CFP electrode exhibits excellent long-term cycling stability, as evidenced by CEs of over 99.5% on the 250th cycle in CFP|Li half-cells (lithiation capacity: 1.5 mA h cm-2, current density: 0.5 mA cm-2). Notably, both the CNT mat and CFP electrodes can be manufactured at an industrial scale, showing real promises for practical a…
abstract: The ever-growing energy demand from modern portable electronics and electric vehicles calls for a matching development in lithium-ion batteries (LIBs) that offer high power density, energy density, and long cycle life. However, LIBs based on traditional layered metal oxide cathodes and graphite anodes are quickly approaching their specific energy limits. The exploration of advanced electrode architectures provides a novel route to improving the energy density of LIBs and is often overlooked. This PhD thesis investigates the design, fabrication, and testing of structurally engineered and high areal capacity LIB electrodes based on hierarchical carbon structures such as carbon nanotubes (CNTs). Firstly, (surface-modified) direct-spun CNT mats are proposed as conductive scaffolds for lithium metal anodes (LMAs), which are desirable for next-generation batteries because of their ultra-high energy density. However, the practical applications of LMAs are hindered by the inhomogeneous Li dendrite formation during cycling which leads to poor efficiency and safety issues. The proposed electrode provides ample Li nucleation sites, reduces the local current densities, and promotes uniform Li plating/stripping at selective locations, thus achieving coulombic efficiencies (CEs) of 98-99% for over 130 cycles in CNT|Li half-cells (lithiation capacity: 2.0 mA h cm-2, current density: 1.0 mA cm-2). Next, a freestanding carbon fibre paper with carbon fillers (CFP) electrode is proposed with a novel dual charge storage mechanism – it acts both as a host for Li intercalation and as a conductive, porous, and lithiophilic 3D scaffold for Li plating/stripping. The CFP electrode exhibits excellent long-term cycling stability, as evidenced by CEs of over 99.5% on the 250th cycle in CFP|Li half-cells (lithiation capacity: 1.5 mA h cm-2, current density: 0.5 mA cm-2). Notably, both the CNT mat and CFP electrodes can be manufactured at an industrial scale, showing real promises for practical a…
author: Zhao, Zijian
language: eng
keywords: 3D electrode, Lithium-ion battery, Lithium-metal anode, nanomanufacturing, ultra-thick electrode
license: https://apollo8-f-pro.lib.cam.ac.uk/bitstreams/b6bf8fc9-d137-4d30-899a-b578fb442e1f/download
license: https://www.rioxx.net/licenses/all-rights-reserved/
date published: 2022-12-16
date modified: 2026-07-22T22:24:07Z
provider: Cambridge University
publisher: Networked Digital Library of Theses and Dissertations
type: WebPage
source organization: University of Cambridge

PropertyValue
property ID: DOI
value: 10.17863/CAM.96505