Highly‐Cyclable Room‐Temperature Phosphorene Polymer Electrolyte Composites for Li Metal Batteries
Abstract
Despite significant interest toward solid‐state electrolytes owing to their superior safety in comparison to liquid‐based electrolytes, sluggish ion diffusion and high interfacial resistance limit their application in durable and high‐power density batteries. Here, a novel quasi‐solid Li+ ion conductive nanocomposite polymer electrolyte containing black phosphorous (BP) nanosheets is reported. The developed electrolyte is successfully cycled against Li metal (over 550 h cycling) at 1 mA cm−2 at room temperature. The cycling overpotential is dropped by 75% in comparison to BP‐free polymer composite electrolyte indicating lower interfacial resistance at the electrode/electrolyte interfaces. Molecular dynamics simulations reveal that the coordination number of Li+ ions around (trifluoromethanesulfonyl)imide (TFSI−) pairs and ethylene‐oxide chains decreases at the Li metal/electrolyte interface, which facilitates the Li+ transport through the polymer host. Density functional theory calculations confirm that the adsorption of the LiTFSI molecules at the BP surface leads to the weakening of N and Li atomic bonding and enhances the dissociation of Li+ ions. This work offers a new potential mechanism to tune the bulk and interfacial ionic conductivity of solid‐state electrolytes that may lead to a new generation of lithium polymer batteries with high ionic conduction kinetics and stable long‐life cycling.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Jun 08, 2020
- Source ID
- 10.1002/adfm.201910749
Entities
People
- Abhijit H Phakatkar
- Bill K Wheatle
- Farzad Mashayek
- Md Golam Rasul
- Meng Cheng
- Ramasubramonian Deivanayagam
- Ramin Rojaee
- Reza Shahbazian-Yassar
- Salvatore Cavallo
- Santosh Mogurampelly
- Seoung‐bum Son
- Soroosh Sharifi‐asl
- Tara Foroozan
- Venkat Ganesan
- Vitaliy Yurkiv
- Yayue Pan
Organizations
- Argonne National Laboratory
- Indian Institute of Technology Jodhpur
- National Science Foundation
- Polytechnic University of Turin
- Temple University
- United States Army Research Laboratory
- University of Illinois at Chicago
- University of Texas at Austin