Photocatalytic production of ethylene and propionic acid from plastic waste by titania-supported atomically dispersed Pd species
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Date
2023
Authors
Zhang, S.
Xia, B.
Qu, Y.
Jing, L.
Jaroniec, M.
Ran, J.
Qiao, S.-Z.
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Science Advances, 2023; 9(49):eadk2407-1-eadk2407-11
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Shuai Zhang, Bingquan Xia, Yang Qu, Liqiang Jing, Mietek Jaroniec, Jingrun Ran, Shi-Zhang Qiao
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Abstract
Current chemical recycling of bulk synthetic plastic, polyethylene (PE), operates at high temperature/pressure and yields a complex mixture of products. PE conversion under mild conditions and with good selectivity toward value-added chemicals remains a practical challenge. Here, we demonstrate an atomic engineering strategy to modify a TiO2 photocatalyst with reversible Pd species for the selective conversion of PE to ethylene (C2H4) and propionic acid via dicarboxylic acid intermediates under moderate conditions. TiO2-supported atomically dispersed Pd species exhibits C2H4 evolution of 531.2 μmol gcat-1 hour-1, 408 times that of pristine TiO2. The liquid product is a valuable chemical propanoic acid with 98.8% selectivity. Plastic conversion with a C2 hydrocarbon yield of 0.9% and a propionic acid yield of 6.3% was achieved in oxidation coupled with 3 hours of photoreaction. In situ spectroscopic studies confirm a dual role of atomic Pd species: an electron acceptor to boost charge separation/transfer for efficient photoredox, and a mediator to stabilize reaction intermediates for selective decarboxylation.
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© 2023 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).