Polypropylene Degradation Catalyzed by Tantalum Hydrides Supported on Sulfated Alumina

Gao, Jiaxin; Zhu, Lingchao; Conley, Matthew P.

doi:10.1021/acscatal.3c02642

Polypropylene Degradation Catalyzed by Tantalum Hydrides Supported on Sulfated Alumina

Journal Article · Tue Aug 01 00:00:00 EDT 2023 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.3c02642· OSTI ID:2544274

Gao, Jiaxin ^[1]; Zhu, Lingchao ^[1]; ^[1]

University of California, Riverside, CA (United States)

Ta–H⁺ sites supported on sulfated aluminum oxide (SAO), [Ta(H)₂(O–)₂][SAO] (1), catalyze the hydrogenolysis of isotactic polypropylene (iPP, M_n = 13.3 kDa; D = 2.4; mmmm = 94%) to form low-molecular-weight branched alkanes (C₁₁–C₃₀) in good yields (70%). Here, the alkanes formed lose stereochemical information originating from iPP, but residual iPP remains highly isotactic. In the presence of D₂, similar mixtures of alkanes are formed containing –CH_3–xD_x, –CHD, and –CD–. Residual iPP maintains high tacticity and incorporates deuterium primarily into –CH₃ groups of the polymer (–CH_3–xD_x/–CHD–/–CD– ~10:1:0). 1 reacts with pinacolborane to form [TaH(κ²-H₂BPin)(O–)₂][SAO] (2). At 200 °C in an iPP melt, 2 reacts to form products indicative of C–H bond activation at –CH₃ groups and internal –CH₂– groups in iPP in a ~1:3 ratio, indicating a slight kinetic preference for C–H bond activation at internal –CH₂– groups. 1 is more reactive toward iPP than high-density polyethylene in hydrogenolysis reactions

View Accepted Manuscript (DOE)

Research Organization:: University of California, Riverside, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0022203

OSTI ID:: 2544274

Alternate ID(s):: OSTI ID: 2422083

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 16 Vol. 13; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Polypropylene Degradation Catalyzed by Tantalum Hydrides Supported on Sulfated Alumina

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