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Article: Cross-linked graphene oxide framework membranes with robust nano-channels for enhanced sieving ability

TitleCross-linked graphene oxide framework membranes with robust nano-channels for enhanced sieving ability
Authors
Issue Date2020
PublisherAmerican Chemical Society. The Journal's web site is located at http://pubs.acs.org/journal/esthag
Citation
Environmental Science & Technology, 2020, v. 54 n. 23, p. 15442-15453 How to Cite?
AbstractIt remains challenging for graphene oxide (GO) membranes to achieve highly efficient performance and sufficient stability for aqueous molecule/ion precise separations. Herein, a molecular-level rational structure design protocol was proposed to develop ceramic-based graphene oxide framework (GOF) membranes with significantly enhanced sieving performance and stability for efficient removal of salts and micropollutants. Via a molecular cross-linking strategy, interlayered nanochannels between GO nanosheets can be rationally designed, featuring precisely tailorable channel size, promising surface chemistries and remarkably robust stability suitable for aqueous separation. Due to a significantly decreased nanochannel size, cross-linking of TU (thiourea) molecule significantly improved monovalent salt rejection (95.6% for NaCl), outperforming existing state-of-the-art GO-based, commercial organic nanofiltration and emerging two-dimensional MoS2 membranes, while moderately decreasing water permeability. In comparison, the GOF membranes cross-linked with MPD (m-phenylenediamine) exhibited a simultaneous increase in permeability and rejection for both salts and micropollutants (21.0% and 53.3% enhancement for chloramphenicol (CAP) solution), breaking their conventional trade-off issue. Cross-linking mechanism indicates that more robust nanochannels were formed by stronger covalent bonds via dehydration condensation between amine (TU/MPD) and carboxyl groups (GO), and nucleophilic addition between amine (TU/MPD) and epoxy groups (GO). Molecule/ion separation mechanism involved size sieving (steric hindrance), electrostatic interaction, Donnan effect, and partial dehydration effect. This work provides a novel protocol for rationally designing size and surface chemistry of highly robust GO nanochannels at a subnanometer level to construct water-stable functional GOF membranes with enhanced sieving performance for water treatment applications.
Persistent Identifierhttp://hdl.handle.net/10722/306357
ISSN
2023 Impact Factor: 10.8
2023 SCImago Journal Rankings: 3.516
ISI Accession Number ID

 

DC FieldValueLanguage
dc.contributor.authorYuan, B-
dc.contributor.authorWang, M-
dc.contributor.authorWang, B-
dc.contributor.authorYang, F-
dc.contributor.authorQuan, X-
dc.contributor.authorTang, C-
dc.contributor.authorDong, Y-
dc.date.accessioned2021-10-20T10:22:28Z-
dc.date.available2021-10-20T10:22:28Z-
dc.date.issued2020-
dc.identifier.citationEnvironmental Science & Technology, 2020, v. 54 n. 23, p. 15442-15453-
dc.identifier.issn0013-936X-
dc.identifier.urihttp://hdl.handle.net/10722/306357-
dc.description.abstractIt remains challenging for graphene oxide (GO) membranes to achieve highly efficient performance and sufficient stability for aqueous molecule/ion precise separations. Herein, a molecular-level rational structure design protocol was proposed to develop ceramic-based graphene oxide framework (GOF) membranes with significantly enhanced sieving performance and stability for efficient removal of salts and micropollutants. Via a molecular cross-linking strategy, interlayered nanochannels between GO nanosheets can be rationally designed, featuring precisely tailorable channel size, promising surface chemistries and remarkably robust stability suitable for aqueous separation. Due to a significantly decreased nanochannel size, cross-linking of TU (thiourea) molecule significantly improved monovalent salt rejection (95.6% for NaCl), outperforming existing state-of-the-art GO-based, commercial organic nanofiltration and emerging two-dimensional MoS2 membranes, while moderately decreasing water permeability. In comparison, the GOF membranes cross-linked with MPD (m-phenylenediamine) exhibited a simultaneous increase in permeability and rejection for both salts and micropollutants (21.0% and 53.3% enhancement for chloramphenicol (CAP) solution), breaking their conventional trade-off issue. Cross-linking mechanism indicates that more robust nanochannels were formed by stronger covalent bonds via dehydration condensation between amine (TU/MPD) and carboxyl groups (GO), and nucleophilic addition between amine (TU/MPD) and epoxy groups (GO). Molecule/ion separation mechanism involved size sieving (steric hindrance), electrostatic interaction, Donnan effect, and partial dehydration effect. This work provides a novel protocol for rationally designing size and surface chemistry of highly robust GO nanochannels at a subnanometer level to construct water-stable functional GOF membranes with enhanced sieving performance for water treatment applications.-
dc.languageeng-
dc.publisherAmerican Chemical Society. The Journal's web site is located at http://pubs.acs.org/journal/esthag-
dc.relation.ispartofEnvironmental Science & Technology-
dc.rightsThis document is the Accepted Manuscript version of a Published Work that appeared in final form in Environmental Science & Technology. copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acs.est.0c05387-
dc.titleCross-linked graphene oxide framework membranes with robust nano-channels for enhanced sieving ability-
dc.typeArticle-
dc.identifier.emailTang, C: tangc@hku.hk-
dc.identifier.authorityTang, C=rp01765-
dc.description.naturepostprint-
dc.identifier.doi10.1021/acs.est.0c05387-
dc.identifier.pmid33185431-
dc.identifier.scopuseid_2-s2.0-85096550581-
dc.identifier.hkuros326735-
dc.identifier.volume54-
dc.identifier.issue23-
dc.identifier.spage15442-
dc.identifier.epage15453-
dc.identifier.isiWOS:000596728600070-
dc.publisher.placeUnited States-

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