Probing sub-5 Ångstrom micropores in carbon for precise light olefin/paraffin separation

Shengjun Du, Jiawu Huang, Matthew R. Ryder, Luke L. Daemen, Cuiting Yang, Hongjun Zhang, Panchao Yin, Yuyan Lai, Jing Xiao, Sheng Dai, Banglin Chen

Research output: Contribution to journalArticlepeer-review

44 Scopus citations

Abstract

Olefin/paraffin separation is an important but challenging and energy-intensive process in petrochemical industry. The realization of carbons with size-exclusion capability is highly desirable but rarely reported. Herein, we report polydopamine-derived carbons (PDA-Cx, where x refers to the pyrolysis temperature) with tailorable sub-5 Å micropore orifices together with larger microvoids by one-step pyrolysis. The sub-5 Å micropore orifices centered at 4.1–4.3 Å in PDA-C800 and 3.7–4.0 Å in PDA-C900 allow the entry of olefins while entirely excluding their paraffin counterparts, performing a precise cut-off to discriminate olefin/paraffin with sub-angstrom discrepancy. The larger voids enable high C2H4 and C3H6 capacities of 2.25 and 1.98 mmol g−1 under ambient conditions, respectively. Breakthrough experiments confirm that a one-step adsorption-desorption process can obtain high-purity olefins. Inelastic neutron scattering further reveals the host–guest interaction of adsorbed C2H4 and C3H6 molecules in PDA-Cx. This study opens an avenue to exploit the sub-5 Å micropores in carbon and their desirable size-exclusion effect.

Original languageEnglish
Article number1197
JournalNature Communications
Volume14
Issue number1
DOIs
StatePublished - Dec 2023

Funding

Note This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US Government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). Funding: J.X., S.-J.D., J.H., and C.Y. gratefully acknowledge the financial support from the National Natural Science Foundation of China (22022806). M.R.R. and S.D. acknowledge the U.S. Department of Energy (DOE) Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division (Separation Sciences) for research funding to support the neutron scattering experiments and data analysis. This research used resources at the Spallation Neutron Source (SNS), a DOE Office of Science User Facility operated by Oak Ridge National Laboratory. Note This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US Government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan ). Funding: J.X., S.-J.D., J.H., and C.Y. gratefully acknowledge the financial support from the National Natural Science Foundation of China (22022806). M.R.R. and S.D. acknowledge the U.S. Department of Energy (DOE) Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division (Separation Sciences) for research funding to support the neutron scattering experiments and data analysis. This research used resources at the Spallation Neutron Source (SNS), a DOE Office of Science User Facility operated by Oak Ridge National Laboratory.

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