Polyethylene Terephthalate Deconstruction Catalyzed by a Carbon-Supported Single-Site Molybdenum-Dioxo Complex

被引:153
作者
Kratish, Yosi [1 ,2 ]
Li, Jiaqi [1 ,2 ]
Liu, Shanfu [1 ,2 ]
Gao, Yanshan [1 ,2 ]
Marks, Tobin J. [1 ,2 ]
机构
[1] Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA
[2] Northwestern Univ, Inst Catalysis Energy Proc ICEP, 2145 Sheridan Rd, Evanston, IL 60208 USA
关键词
heterogenous catalysis; hydrogenolysis; molybdenum; polymers; reaction mechanisms; REDUCTIVE DEPOLYMERIZATION; THERMAL-DEGRADATION; POLY(ETHYLENE-TEREPHTHALATE); GLYCOLYSIS; ESTERS; EFFICIENT; WASTE; POLYESTERS; PYROLYSIS; TRANSESTERIFICATION;
D O I
10.1002/anie.202007423
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Polyethylene terephthalate (PET) is selectively depolymerized by a carbon-supported single-site molybdenum-dioxo catalyst to terephthalic acid (PTA) and ethylene. The solventless reactions are most efficient under 1 atmosphere of H-2. The catalyst exhibits high stability and can be recycled multiple times without loss of activity. Waste beverage bottle PET or a PET + polypropylene (PP) mixture (simulating the bottle + cap) proceeds at 260 degrees C with complete PET deconstruction and quantitative PTA isolation. Mechanistic studies with a model diester, 1,2-ethanediol dibenzoate, suggest the reaction proceeds by initial retro-hydroalkoxylation/beta-C-O scission and subsequent hydrogenolysis of the vinyl benzoate intermediate.
引用
收藏
页码:19857 / 19861
页数:5
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