Highly-Cyclable Room-Temperature Phosphorene Polymer Electrolyte Composites for Li Metal Batteries

Rojaee, Ramin; Cavallo, Salvatore; Mogurampelly, Santosh; Wheatle, Bill K.; Yurkiv, Vitaliy; Deivanayagam, Ramasubramonian; Foroozan, Tara; Rasul, Md Golam; Sharifi‐Asl, Soroosh; Phakatkar, Abhijit H.; Cheng, Meng; Son, Seoung‐Bum; Pan, Yayue; Mashayek, Farzad; Ganesan, Venkat; Shahbazian‐Yassar, Reza

doi:10.1002/adfm.201910749

Title: Highly-Cyclable Room-Temperature Phosphorene Polymer Electrolyte Composites for Li Metal Batteries

Journal Article · Mon Jun 08 00:00:00 EDT 2020 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.201910749· OSTI ID:1764855

^[1]; Cavallo, Salvatore ^[2];

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^[1]; Sharifi‐Asl, Soroosh ^[1];

^[1]; Cheng, Meng ^[1]; Son, Seoung‐Bum ^[5];

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^[6];

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Univ. of Illinois, Chicago, IL (United States)
Univ. of Illinois, Chicago, IL (United States); Polytechnic of Turin, Torino (Italy)
Temple Univ., Philadelphia, PA (United States); Indian Inst. of Technology (IIT), Jodhpur (India)
Department of Chemical EngineeringUniversity of Texas at Austin Austin TX 78712 USA; Univ. of Texas at Austin, TX (United States)
Chemical Sciences and Engineering DivisionArgonne National Laboratory 9700 South Cass Avenue Lemont IL 60439 USA
Univ. of Texas at Austin, TX (United States)

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. Here, 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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE; National Science Foundation (NSF); Robert A. Welch Foundation; US Army Research Office (ARO)

Grant/Contract Number:: AC02-06CH11357; 1620901; CBET-17069698; DMR-1721512; CBET-1805938; 1625061; TG-DMR180106; F1599; W911NF-16-2-0189

OSTI ID:: 1764855

Journal Information:: Advanced Functional Materials, Vol. 30, Issue 32; ISSN 1616-301X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
2D materials
black phosphorous nanosheets
lithium batteries
polymer electrolytes

Title: Highly-Cyclable Room-Temperature Phosphorene Polymer Electrolyte Composites for Li Metal Batteries

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