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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.<\/jats:p>","DOI":"10.1021\/acs.est.0c05387","type":"journal-article","created":{"date-parts":[[2020,11,13]],"date-time":"2020-11-13T10:16:06Z","timestamp":1605262566000},"page":"15442-15453","source":"Crossref","is-referenced-by-count":153,"title":["Cross-linked\nGraphene Oxide Framework Membranes with\nRobust Nano-Channels for Enhanced Sieving Ability"],"prefix":"10.1021","volume":"54","author":[{"given":"Baoqiu","family":"Yuan","sequence":"first","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mingxin","family":"Wang","sequence":"additional","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bo","family":"Wang","sequence":"additional","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fenglin","family":"Yang","sequence":"additional","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3085-0789","authenticated-orcid":true,"given":"Xie","family":"Quan","sequence":"additional","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7932-6462","authenticated-orcid":true,"given":"Chuyang Y.","family":"Tang","sequence":"additional","affiliation":[{"name":"The University of Hong Kong , , ,","place":["Pokfulam, Hong Kong, China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1409-0994","authenticated-orcid":true,"given":"Yingchao","family":"Dong","sequence":"additional","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2020,11,13]]},"reference":[{"issue":"7315","key":"2026081418144809600_cit1","doi-asserted-by":"publisher","first-page":"555","DOI":"10.1038\/nature09440","article-title":"Global threats to human water security\nand river biodiversity","volume":"467","author":"Vorosmarty","year":"2010","journal-title":"Nature"},{"issue":"22","key":"2026081418144809600_cit2","doi-asserted-by":"publisher","first-page":"12961","DOI":"10.1021\/acs.est.9b02966","article-title":"An Evidence\nSynthesis of Pharmaceuticals\nand Personal Care Products (PPCPs) in the Environment: Imbalances\namong Compounds, Sewage Treatment Techniques, and Ecosystem Types","volume":"53","author":"Meyer","year":"2019","journal-title":"Environ. 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