skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Block‐Copolymer‐Architected Materials in Electrochemical Energy Storage
The multiscale architecture of electrochemical energy storage (EES) materials critically impacts device performance, including energy, power, and durability. The pore space of nano‐ to macrostructured electrodes determines mass transport within the electrolyte and defines the effective energy density. The dimensions of the active charge‐storing materials can increase stability during cycling by accommodating strains from electrochemical–mechanical coupling while also defining surface area that increases capacitive charge storage, decreases charge‐transfer resistance, but also leads to low efficiency and degradation from interfacial reactions. Thus, elucidating and developing a fundamental understanding of these correlations requires materials with precisely tunable nanoscale architectures. Herein, approaches that take advantage of the nanoscale control offered by block copolymer (BCP) self‐assembly are reviewed and insights gained from associated nanoscale phenomena observed in EES are highlighted. Systematic studies that use custom‐tailored BCPs to reveal fundamental nanostructure–property–performance relationships are emphasized. Importantly, most reports of nanostructured materials utilize low loadings and thin electrodes and results represent mass transfer limitations at the particle scale. However, as cell‐level performance involves mass transport over 10–100s of micrometers, recently emerging BCP‐based processes are further highlighted, leading to hierarchical meso/macroporous materials needed for creating multiscale structure–performance relationships and next‐generation energy storage material architectures.  more » « less
Award ID(s):
2146597 2307013
PAR ID:
10482249
Author(s) / Creator(s):
 ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Small Science
Volume:
3
Issue:
12
ISSN:
2688-4046
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract Lithium-ion batteries (LIBs) have solidified their position as primary energy storage solutions for applications ranging from portable electronics to electric vehicles. As power-intensive applications expand, achieving fast charging/discharging performance is increasingly critical for high-energy-density batteries. However, the increased thickness of electrodes in LIBs presents significant challenges for charge (Li⁺ and electron) transfer kinetics, as longer charge migration distances hinder fast charging and discharging performance. Enormous efforts have been made to summarize advancements in materials chemistry—optimizing ionic pathways and crystal structure—to enhance Li⁺ transfer within the bulk of electrode materials. Yet, materials design and modifications fall short of fully addressing Li+and electron transport limitations in thick electrodes. Despite the significance of potentially offering a solution to these constraints, the strategic engineering of electrode architecture has been rarely discussed. In this mini-review, we highlight recent innovations in electrode structural design for fast-charging applications, examining gradient architectures, low-tortuosity structures, and novel current collector designs. By exploring these advanced approaches and offering perspectives on future developments, we aim to promote further advancements toward achieving high-energy-density, fast-charging LIBs. 
    more » « less
  2. Abstract MXenes are 2D materials with relatively high surface areas, high electrical conductivities, functional transition metal surfaces, tunable surface chemistries, and solution processability. Due to these properties, 2D MXenes have attracted widespread attention as electrode materials for energy storage devices, including electrochemical capacitors, with high power and energy densities. However, many studies have shown that the electrochemical performance of MXene electrodes is considerably affected by their structure and morphology. These properties are, for the most part, controlled by the method used for the assembly of 2D MXene flakes and the electrode fabrication methods. A successful electrode assembly and fabrication method should address several challenges, such as the restacking of 2D flakes, to achieve electrode structures and morphologies that deliver high ionic transport properties, electrical conductivity, and mechanical stability. This review aims to provide insight into the current state‐of‐the‐art assembly and fabrication methods used to design and fabricate high performance electrodes based on MXenes. The major challenges to be addressed and possible future directions in the fabrication of MXene electrodes for practical energy storage applications are highlighted. 
    more » « less
  3. Abstract Increasing the thickness of the electrodes is considered the primary strategy to elevate battery energy density. However, as the thickness increases, rate performance, cycling performance, and mechanical stability are affected due to the sluggish ion transfer kinetics and compromised structural integrity. Inspired by the natural hierarchical porous structure of trees, electrodes with bioinspired architecture are fabricated to address these challenges. Specifically, electrodes with aligned columns consist of tree‐inspired vertical channels, and hierarchical pores are constructed by screen printing and ice‐templating, imparting enhanced electrochemical and mechanical performance. Employing an aqueous‐based binder, the LiNi0.8Mn0.1Co0.1O2cathode achieves a high areal energy density of 15.1 mWh cm−2at a rate of 1C at mass loading of 26.0 mg cm−2, benefitting from the multiscale pores that elevated charge transfer kinetics in the thick electrode. The electrodes demonstrate capacity retention of 90% at the 100th cycle at a high current density of 5.2 mA cm−2. To understand the mechanisms that promote electrode performance, simplified electro‐chemo‐mechanical models are developed, the drying process and the charge‐discharge process are simulated. The simulation results suggested that the improved performance of the designed electrode benefits from the lower ohmic overpotential and less strain gradient and stress concentration due to the hierarchical porous architecture. 
    more » « less
  4. Abstract Vertically oriented graphene (VG) nanosheets exhibit unique structural characteristics, such as large accessible surface area, rich edges, high electrical conductivity, open network channels, and agglomeration resistance, for electrochemical energy‐storage applications (e. g., supercapacitors, lithium‐ion batteries, etc.). In this Review article, we summarize recent progress in the design and engineering of VG‐based electrodes for high‐performance electrochemical energy technologies within the context of energy‐storage mechanisms and charge‐transfer kinetics, and include a perspective to highlight the challenges and promises in the exploitation of vertically oriented two‐dimensional carbon nanostructures for further enhancement of the performance of electrochemical energy‐storage devices. 
    more » « less
  5. Nanostructured materials offer the potential to drive future developments and applications of electrochemical devices, but are underutilized because their nanoscale cavities can impose mass transfer limitations that constrain electrochemical signal generation. Here, we report a new signal-generating mechanism that employs a molecular redox capacitor to enable nanostructured electrodes to amplify electrochemical signals even without an enhanced reactant mass transfer. The surface-tethered molecular redox capacitor engages diffusible reactants and products in redox-cycling reactions with the electrode. Such redox-cycling reactions are facilitated by the nanostructure that increases the probabilities of both reactant–electrode and product–redox-capacitor encounters ( i.e. , the nanoconfinement effect), resulting in substantial signal amplification. Using redox-capacitor-tethered Au nanopillar electrodes, we demonstrate improved sensitivity for measuring pyocyanin (bacterial metabolite). This study paves a new way of using nanostructured materials in electrochemical applications by engineering the reaction pathway within the nanoscale cavities of the materials. 
    more » « less