Synthesis of platinum nanoparticles on strontium titanate nanocuboids via surface organometallic grafting for the catalytic hydrogenolysis of plastic waste

被引:20
|
作者
McCullough, Katherine E. [1 ]
Peczak, Ian L. [2 ]
Kennedy, Robert M. [1 ,2 ]
Wang, Yi-Yu [3 ]
Lin, James [4 ]
Wu, Xun [3 ,4 ]
Paterson, Alexander L. [4 ,8 ]
Perras, Frederic A. [4 ]
Hall, Jacklyn [1 ]
Kropf, A. Jeremy [1 ]
Hackler, Ryan A. [1 ]
Shin, Youngho [5 ]
Niklas, Jens [1 ]
Poluektov, Oleg G. [1 ]
Wen, Jianguo [6 ]
Huang, Wenyu [3 ,4 ]
Sadow, Aaron D. [3 ,4 ]
Poeppelmeier, Kenneth R. [2 ]
Delferro, Massimiliano [1 ,7 ]
Ferrandon, Magali S. [1 ]
机构
[1] Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA
[2] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
[3] Iowa State Univ, Dept Chem, Ames, IA 50011 USA
[4] US DOE Ames Natl Lab, Ames, IA 50011 USA
[5] Appl Mat Div, Argonne Natl Lab, Lemont, IL 60439 USA
[6] Argonne Natl Lab, Ctr Nanoscale Mat, Lemont, IL 60439 USA
[7] Univ Chicago, Pritzker Sch Mol Engn, Chicago, IL 60637 USA
[8] Univ Wisconsin Madison, Natl Magnet Resonance Facil Madison, Madison, WI 53706 USA
基金
美国国家科学基金会; 美国能源部;
关键词
ATOMIC LAYER DEPOSITION; HYDROTHERMAL SYNTHESIS; PYROLYSIS; CHEMISTRY; SHAPE; NMR; RECONSTRUCTION; POLARIZATION; SEQUENCES; GROWTH;
D O I
10.1039/d2ta08133d
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Pt/SrTiO3 (Pt/STO), prepared on small scale by atomic layer deposition (ALD), is a capable heterogeneous catalyst for the selective hydrogenolysis of polyolefins to hydrocarbon oils, providing a promising approach for upcycling plastic waste. However, because deposition by ALD is costly and resource-intensive, a new synthesis of Pt/STO is needed to effectively scale catalyst production and pursue the commercialization of upcycling processes. To that effect, this work details a scalable deposition method for Pt/STO made by surface organometallic chemistry (SOMC) techniques using Pt(ii) acetylacetonate or and trimethyl(methylcyclopentadienyl)platinum. The STO support was calcined (550 degrees C), treated with ozone (200 degrees C), and finally steamed (200 degrees C) to afford a clean STO surface populated with only hydroxyl groups. Pt precursors were dissolved in toluene and deposited onto STO. After reduction at 300 degrees C, the STO support was decorated with 1.0-1.5 nm Pt nanoparticles. The size and loading of these nanoparticles were varied by employing a multi-cycle deposition and oxidation and/or reduction process designed to ALD techniques. These Pt/STO catalysts hydrogenolyzed isotactic polypropylene into liquid products (>95% yield) with average molecular weights of 200-300 Da (similar to 25 carbon atoms) and narrow size distributions at 300 degrees C and 180 psi H-2.
引用
收藏
页码:1216 / 1231
页数:16
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