PMID- 37325872 OWN - NLM STAT- PubMed-not-MEDLINE LR - 20230925 IS - 1521-3773 (Electronic) IS - 1433-7851 (Linking) VI - 62 IP - 40 DP - 2023 Oct 2 TI - Mechanistic Understanding of Efficient Polyethylene Hydrocracking over Two-Dimensional Platinum-Anchored Tungsten Trioxide. PG - e202305644 LID - 10.1002/anie.202305644 [doi] AB - Chemical upcycling of polyethylene (PE) can convert plastic waste into valuable resources. However, engineering a catalyst that allows PE decomposition at low temperatures with high activity remains a significant challenge. Herein, we anchored 0.2 wt.% platinum (Pt) on defective two-dimensional tungsten trioxide (2D WO(3) ) nanosheets and achieved hydrocracking of high-density polyethylene (HDPE) waste at 200-250 degrees C with a liquid fuel (C(5-18) ) formation rate up to 1456 g(products) ⋅ g(metal species) (-1) ⋅ h(-1) . The reaction pathway over the bifunctional 2D Pt/WO(3) is elucidated by quasi-operando transmission infrared spectroscopy, where (I) well-dispersed Pt immobilized on 2D WO(3) nanosheets trigger the dissociation of hydrogen; (II) adsorption of PE and activation of C-C cleavage on WO(3) are through the formation of C=O/C=C intermediates; (III) intermediates are converted to alkane products by the dissociated H. Our study directly illustrates the synergistic role of bifunctional Pt/WO(3) catalyst in the hydrocracking of HDPE, paving the way for the development of high-performance catalysts with optimized chemical and morphological properties. CI - (c) 2023 Wiley-VCH GmbH. FAU - Zhou, Qimin AU - Zhou Q AUID- ORCID: 0000-0002-8810-3359 AD - State Key Laboratory of Chemical Engineering, College of Chemical and Biological Engineering, Zhejiang University, 866 Yuhangtang Rd, Hangzhou, 310027, Zhejiang, P. R. China. FAU - Wang, Deliang AU - Wang D AD - State Key Laboratory of Chemical Engineering, College of Chemical and Biological Engineering, Zhejiang University, 866 Yuhangtang Rd, Hangzhou, 310027, Zhejiang, P. R. China. FAU - Wang, Qingyue AU - Wang Q AD - State Key Laboratory of Chemical Engineering, College of Chemical and Biological Engineering, Zhejiang University, 866 Yuhangtang Rd, Hangzhou, 310027, Zhejiang, P. R. China. AD - Institute of Zhejiang University-Quzhou, 99 Zheda Rd, Quzhou, 324000, Zhejiang, P. R. China. FAU - He, Kailin AU - He K AD - Key Laboratory of Hunan Province for the Synergetic Control and Resource Reuse of the Multi-Pollutants of Flue Gas, National Sintering and Pelletizing Equipment System Engineering Research Center, Zhongye Changtian International Engineering Co., Ltd., Changsha, 410205, Hunan, P. R. China. FAU - Lim, Khak Ho AU - Lim KH AD - State Key Laboratory of Chemical Engineering, College of Chemical and Biological Engineering, Zhejiang University, 866 Yuhangtang Rd, Hangzhou, 310027, Zhejiang, P. R. China. AD - Institute of Zhejiang University-Quzhou, 99 Zheda Rd, Quzhou, 324000, Zhejiang, P. R. China. FAU - Yang, Xuan AU - Yang X AD - State Key Laboratory of Chemical Engineering, College of Chemical and Biological Engineering, Zhejiang University, 866 Yuhangtang Rd, Hangzhou, 310027, Zhejiang, P. R. China. AD - Institute of Zhejiang University-Quzhou, 99 Zheda Rd, Quzhou, 324000, Zhejiang, P. R. China. FAU - Wang, Wen-Jun AU - Wang WJ AD - State Key Laboratory of Chemical Engineering, College of Chemical and Biological Engineering, Zhejiang University, 866 Yuhangtang Rd, Hangzhou, 310027, Zhejiang, P. R. China. AD - Institute of Zhejiang University-Quzhou, 99 Zheda Rd, Quzhou, 324000, Zhejiang, P. R. China. FAU - Li, Bo-Geng AU - Li BG AD - State Key Laboratory of Chemical Engineering, College of Chemical and Biological Engineering, Zhejiang University, 866 Yuhangtang Rd, Hangzhou, 310027, Zhejiang, P. R. China. AD - Institute of Zhejiang University-Quzhou, 99 Zheda Rd, Quzhou, 324000, Zhejiang, P. R. China. FAU - Liu, Pingwei AU - Liu P AUID- ORCID: 0000-0002-5060-0165 AD - State Key Laboratory of Chemical Engineering, College of Chemical and Biological Engineering, Zhejiang University, 866 Yuhangtang Rd, Hangzhou, 310027, Zhejiang, P. R. China. AD - Institute of Zhejiang University-Quzhou, 99 Zheda Rd, Quzhou, 324000, Zhejiang, P. R. China. LA - eng GR - 22293061/National Natural Science Foundation of China/ GR - 22208292/National Natural Science Foundation of China/ GR - 22208293/National Natural Science Foundation of China/ GR - 22078289/National Natural Science Foundation of China/ GR - 22078282/National Natural Science Foundation of China/ GR - 21938010/National Natural Science Foundation of China/ GR - 51903218/National Natural Science Foundation of China/ GR - 2197080461/National Natural Science Foundation of China/ GR - 2022M712743/Postdoctoral Research Foundation of China/ GR - 2022SZ-TD003/Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering/ GR - IZQ2021RCZX002/Research Funds of Institute of Zhejiang University-Quzhou/ GR - IZQ2021RCZX003/Research Funds of Institute of Zhejiang University-Quzhou/ GR - IZQ2021KJ2011/Research Funds of Institute of Zhejiang University-Quzhou/ GR - IZQ2022RCZX201/Research Funds of Institute of Zhejiang University-Quzhou/ GR - 2022SK2065/the Key R&D Program of Hunan province/ GR - 2017YFC0210302/the National Key Research and Development Program of China/ GR - SKL-ChE-23D02/the State Key Laboratory of Chemical Engineering/ GR - SKL-ChE-23T04/the State Key Laboratory of Chemical Engineering/ GR - LR20B060002/the National Natural Science Foundation of China Zhejiang Provincial Natural Science Foundation of China/ PT - Journal Article DEP - 20230711 PL - Germany TA - Angew Chem Int Ed Engl JT - Angewandte Chemie (International ed. in English) JID - 0370543 SB - IM OTO - NOTNLM OT - 2D Pt/WO3 OT - HDPE Activation OT - Hydrogen Transfer OT - PE Hydrocracking OT - Quasi-Operando TIR Spectroscopy EDAT- 2023/06/16 06:42 MHDA- 2023/06/16 06:43 CRDT- 2023/06/16 04:33 PHST- 2023/04/22 00:00 [received] PHST- 2023/06/16 06:43 [medline] PHST- 2023/06/16 06:42 [pubmed] PHST- 2023/06/16 04:33 [entrez] AID - 10.1002/anie.202305644 [doi] PST - ppublish SO - Angew Chem Int Ed Engl. 2023 Oct 2;62(40):e202305644. doi: 10.1002/anie.202305644. Epub 2023 Jul 11.