TY - JOUR
T1 - Synthesis of platinum nanoparticles on strontium titanate nanocuboids via surface organometallic grafting for the catalytic hydrogenolysis of plastic waste
AU - McCullough, Katherine E.
AU - Peczak, Ian L.
AU - Kennedy, Robert M.
AU - Wang, Yi Yu
AU - Lin, James
AU - Wu, Xun
AU - Paterson, Alexander L.
AU - Perras, Frédéric A.
AU - Hall, Jacklyn
AU - Kropf, A. Jeremy
AU - Hackler, Ryan A.
AU - Shin, Youngho
AU - Niklas, Jens
AU - Poluektov, Oleg G.
AU - Wen, Jianguo
AU - Huang, Wenyu
AU - Sadow, Aaron D.
AU - Poeppelmeier, Kenneth R.
AU - Delferro, Massimiliano
AU - Ferrandon, Magali S.
N1 - Funding Information:
This work was supported as part of the Institute for Cooperative Upcycling of Plastics (iCOUP), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences. This work was also partially supported by DOE/EERE/AMO and BETO for studies of catalytic hydrogenolysis of plastic waste (Award Number DE-EE0009300). Argonne National Laboratory is operated by UChicago Argonne LLC under Contract DE-AC-02-06CH11357 for the United States Department of Energy, and Ames Laboratory is operated by Iowa State University under Contract DE-AC-02-07CH11358 for the United States Department of Energy. The authors acknowledge the Materials Engineering Research Facility (MERF) at Argonne National Laboratory for synthetic contributions in the large-scale batch synthesis of STO nanocuboid supports. Use of the Advanced Photon Source is supported by the U.S. Department of Energy, Office of Science, and Office of the Basic Energy Sciences, under Contract No. DE-AC-02-06CH11357. MRCAT operations at Sector 10 are supported by the Department of Energy and the MRCAT member institutions. The EPR work at Argonne National Laboratory was supported by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, under Contract No. DE-AC-02-06CH11357. Work performed at the Center for Nanoscale Materials including ACAT and Talos, a U.S. Department of Energy Office of Science User Facility, was supported by the U.S. DOE, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. This work also made use of (i) the EPIC and BioCryo facilities of Northwestern University's NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205); the MRSEC program (NSF DMR-1720139) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois, through the IIN, (ii) CryoCluster equipment, which has received support from the MRI program (NSF DMR-1229693), and (iii) Jerome B. Cohen X-ray Diffraction Facility supported by the MRSEC program of the National Science Foundation (DMR-1720139) at the Materials Research Center of Northwestern University and the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205). The authors thank Dr Uddhav Kanbur for synthetic contributions, Dr Ahmed Farghaly for helpful discussions, and Dr Long Qi for the development and use of UPLC to analyze molecular weights of liquid samples.
Publisher Copyright:
© 2023 The Royal Society of Chemistry.
PY - 2022/12/12
Y1 - 2022/12/12
N2 - 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 °C), treated with ozone (200 °C), and finally steamed (200 °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 °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.
AB - 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 °C), treated with ozone (200 °C), and finally steamed (200 °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 °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.
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U2 - 10.1039/d2ta08133d
DO - 10.1039/d2ta08133d
M3 - Article
AN - SCOPUS:85145561196
SN - 2050-7488
VL - 11
SP - 1216
EP - 1231
JO - Journal of Materials Chemistry A
JF - Journal of Materials Chemistry A
IS - 3
ER -
