The Overlooked Potential of Sulfated Zirconia: Reexamining Solid Superacidity Toward the Controlled Depolymerization of Polyolefins

Cleary, Scott R.; Starace, Anne K.; Curran-Velasco, Caleb C.; Ruddy, Daniel A.; McGuirk, C. Michael

doi:10.1021/acs.langmuir.3c03966

Title: The Overlooked Potential of Sulfated Zirconia: Reexamining Solid Superacidity Toward the Controlled Depolymerization of Polyolefins

Journal Article · 20 March 2024 · Langmuir

DOI: https://doi.org/10.1021/acs.langmuir.3c03966 · OSTI ID:2329408

Cleary, Scott R. ^[1];

^[2]; Curran-Velasco, Caleb C. ^[1];

^[2];

^[1]

Colorado School of Mines, Golden, CO (United States)
National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Closed-loop recycling via an efficient chemical process can help alleviate the global plastic waste crisis. However, conventional depolymerization methods for polyolefins, which compose more than 50% of plastics, demand high temperatures and pressures, employ precious noble metals, and yield complex mixtures of products limited to single-use fuels or oils. Superacidic sulfated zirconia (SZrO) with Hammet Acidity Functions (H₀) = -12 (i.e., stronger than 100% H₂SO₄) is an industrially deployed heterogeneous catalyst capable of activating hydrocarbons under mild conditions and is shown to decompose polyolefins at ambient pressure and temperatures near 200 °C. Additionally, confinement of active sites in porous supports is known to radically increase selectivity, coking and sintering resistance, and acid site activity, presenting a possible approach to low-energy polyolefin depolymerization. However, a critical examination of the literature on SZrO led us to a surprising conclusion: despite 40 years of catalytic study, engineering, and industrial use, the surface chemistry of SZrO is poorly understood. Ostensibly spurred by SZrO's impressive catalytic activity, the application-driven study of SZrO has resulted in deleterious ambiguity in requisite synthetic conditions and insufficient characterization of acidity, porosity, and active site structure. Here, this ambiguity has produced significant knowledge gaps surrounding the synthesis, structure, and mechanisms of hydrocarbon activation for optimized SZrO, stunting the potential of this catalyst in olefin cracking and other industrially relevant reactions, such as isomerization, esterification, and alkylation. Toward mitigating these long extant issues, we herein identify and highlight these current shortcomings and knowledge gaps, propose explicit guidelines for characterization of and reporting on characterization of solid acidity, and discuss the potential of pore-confined superacids in the efficient and selective depolymerization of polyolefins.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 2329408

Report Number(s):: NREL/JA-5100-89149; MainId:89928; UUID:6a2b1c84-a0f6-4135-b3a3-16c9a739deaf; MainAdminId:72132

Journal Information:: Langmuir, Vol. 40, Issue 13; ISSN 0743-7463

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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