Author
Listed:
- Wei Zhang
(Pacific Northwest National Laboratory, P.O. Box 999
Technische Universität München)
- Rachit Khare
(Technische Universität München)
- Sungmin Kim
(Pacific Northwest National Laboratory, P.O. Box 999)
- Lillian Hale
(Pacific Northwest National Laboratory, P.O. Box 999)
- Wenda Hu
(Pacific Northwest National Laboratory, P.O. Box 999)
- Chunlin Yuan
(Technische Universität München)
- Yaoci Sheng
(Technische Universität München)
- Peiran Zhang
(Technische Universität München)
- Lennart Wahl
(Technische Universität München)
- Jiande Mai
(Pacific Northwest National Laboratory, P.O. Box 999)
- Boda Yang
(Pacific Northwest National Laboratory, P.O. Box 999)
- Oliver Y. Gutiérrez
(Pacific Northwest National Laboratory, P.O. Box 999)
- Debmalya Ray
(Pacific Northwest National Laboratory, P.O. Box 999)
- John Fulton
(Pacific Northwest National Laboratory, P.O. Box 999)
- Donald M. Camaioni
(Pacific Northwest National Laboratory, P.O. Box 999)
- Jianzhi Hu
(Pacific Northwest National Laboratory, P.O. Box 999
Washington State University)
- Huamin Wang
(Pacific Northwest National Laboratory, P.O. Box 999)
- Mal-Soon Lee
(Pacific Northwest National Laboratory, P.O. Box 999)
- Johannes A. Lercher
(Pacific Northwest National Laboratory, P.O. Box 999
Technische Universität München)
Abstract
Chloroaluminate ionic liquids selectively transform (waste) polyolefins into gasoline-range alkanes through tandem cracking-alkylation at temperatures below 100 °C. Further improvement of this process necessitates a deep understanding of the nature of the catalytically active species and the correlated performance in the catalyzing critical reactions for the tandem polyolefin deconstruction with isoalkanes at low temperatures. Here, we address this requirement by determining the nuclearity of the chloroaluminate ions and their interactions with reaction intermediates, combining in situ 27Al magic-angle spinning nuclear magnetic resonance spectroscopy, in situ Raman spectroscopy, Al K-edge X-ray absorption near edge structure spectroscopy, and catalytic activity measurement. Cracking and alkylation are facilitated by carbenium ions initiated by AlCl3-tert-butyl chloride (TBC) adducts, which are formed by the dissociation of Al2Cl7− in the presence of TBC. The carbenium ions activate the alkane polymer strands and advance the alkylation cycle through multiple hydride transfer reactions. In situ 1H NMR and operando infrared spectroscopy demonstrate that the cracking and alkylation processes occur synchronously; alkenes formed during cracking are rapidly incorporated into the carbenium ion-mediated alkylation cycle. The conclusions are further supported by ab initio molecular dynamics simulations coupled with an enhanced sampling method, and model experiments using n-hexadecane as a feed.
Suggested Citation
Wei Zhang & Rachit Khare & Sungmin Kim & Lillian Hale & Wenda Hu & Chunlin Yuan & Yaoci Sheng & Peiran Zhang & Lennart Wahl & Jiande Mai & Boda Yang & Oliver Y. Gutiérrez & Debmalya Ray & John Fulton , 2024.
"Active species in chloroaluminate ionic liquids catalyzing low-temperature polyolefin deconstruction,"
Nature Communications, Nature, vol. 15(1), pages 1-11, December.
Handle:
RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-49827-4
DOI: 10.1038/s41467-024-49827-4
Download full text from publisher
Most related items
These are the items that most often cite the same works as this one and are cited by the same works as this one.
- Songshan Bi & Shuai Wang & Fang Yue & Zhiwei Tie & Zhiqiang Niu, 2021.
"A rechargeable aqueous manganese-ion battery based on intercalation chemistry,"
Nature Communications, Nature, vol. 12(1), pages 1-11, December.
- Jiashen Meng & Xuhui Yao & Xufeng Hong & Lujun Zhu & Zhitong Xiao & Yongfeng Jia & Fang Liu & Huimin Song & Yunlong Zhao & Quanquan Pang, 2023.
"A solution-to-solid conversion chemistry enables ultrafast-charging and long-lived molten salt aluminium batteries,"
Nature Communications, Nature, vol. 14(1), pages 1-9, December.
Corrections
All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-49827-4. See general information about how to correct material in RePEc.
If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.
If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .
If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.
For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .
Please note that corrections may take a couple of weeks to filter through
the various RePEc services.