Upcycling linear low-density polyethylene waste to turbostratic graphene for high mass loading supercapacitors

Gao, Yuan; Huynh, Ngoc Tien; Kim, Ki-Joong; Wang, Congjun; Pham, Viet Hung; Matranga, Christopher

doi:10.1016/j.cej.2024.155873

Upcycling linear low-density polyethylene waste to turbostratic graphene for high mass loading supercapacitors

Journal Article · Mon Sep 16 00:00:00 EDT 2024 · Chemical Engineering Journal

DOI:https://doi.org/10.1016/j.cej.2024.155873· OSTI ID:2447191

Gao, Yuan ^[1]; Huynh, Ngoc Tien ^[1]; ^[1]; ^[1]; Pham, Viet Hung ^[1]; ^[1]

National Energy Technology Lab. (NETL), Pittsburgh, PA (United States)

Linear low-density polyethylene (LLDPE) waste is difficult to upcycle into more valuable carbon materials because it tends to completely decompose into small molecules during thermal processing. In this work, LLDPE is upcycled into a high quality turbostratic graphene using a pre-treatment step to oxidatively crosslink the polymer with the assistance of solid additives (KCl and K₂CO₃) that improve crosslinking by increasing the effective surface area of the polymer melt during processing. After this pretreatment step, the crosslinked polymer could then be carbonized and catalytically graphenized between 400–950°C without decomposition of the polymer feedstock. The LLDPE derived graphene (LLDPE-G) obtained from this process has a Brunauer–Emmett–Teller (BET) specific surface area, up to 1800m² g^-1 and average Raman I_D/I_G and I_2D/I_G ratios of 0.85 and 0.57, respectively, indicating high quality graphene. When used as an electrode material in symmetric supercapacitors, LLDPE-G possesses a specific capacitance up to 175Fg^-1 at a mass loading of 20mgcm^-2, which is two times the commercial requirement, yielding an areal capacitance of 3.5 Fcm^-2. Moreover, LLDPE-G exhibits exceptional cycling stability with a capacitance retention of 95.8 % after 100,000 cycles at a current density of 4.0 Ag^-1. Additionally, the KCl and K₂CO₃ solids are recycled and reused over 3 complete reaction cycles to make new LLDPE-G with the material quality and electrocapacitive performance retained and verified after each cycle. Our approach creates new opportunities for upcycling waste LLDPE and other varieties of polyethylene into a higher value graphene used for electrochemical energy storage applications.

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Research Organization:: National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)

Sponsoring Organization:: USDOE; USDOE Office of Fossil Energy and Carbon Management (FECM)

OSTI ID:: 2447191

Alternate ID(s):: OSTI ID: 2515608

Journal Information:: Chemical Engineering Journal, Journal Name: Chemical Engineering Journal Journal Issue: 2024 Vol. 498; ISSN 1385-8947

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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