Confined assembly of ultrathin nanoporous nitrogen-doped graphene nanofilms with dual metal coordination chemistry

Summary: Graphene oxide (GO) nanosheets with unique structure have received much attention in providing opportunity for high-performance membranes in separation. However, the rational design of ultrathin graphene membranes with controlled structures remains a big challenge. Here, we report a methodo...

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Main Authors: Zehai Xu, Yufan Zhang, Xu Zhang, Qin Meng, Yujie Zhu, Chong Shen, Yinghua Lu, Guoliang Zhang, Congjie Gao
Format: Article
Language:English
Published: Elsevier 2021-06-01
Series:iScience
Subjects:
Online Access:http://www.sciencedirect.com/science/article/pii/S2589004221005447
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author Zehai Xu
Yufan Zhang
Xu Zhang
Qin Meng
Yujie Zhu
Chong Shen
Yinghua Lu
Guoliang Zhang
Congjie Gao
author_facet Zehai Xu
Yufan Zhang
Xu Zhang
Qin Meng
Yujie Zhu
Chong Shen
Yinghua Lu
Guoliang Zhang
Congjie Gao
author_sort Zehai Xu
collection DOAJ
description Summary: Graphene oxide (GO) nanosheets with unique structure have received much attention in providing opportunity for high-performance membranes in separation. However, the rational design of ultrathin graphene membranes with controlled structures remains a big challenge. Here, we report a methodology to synthesize dual metal-coordinated ultrathin nanoporous graphene nanofilms by tailoring well-aligned nanocrystals as building blocks on heteroatom-doped GO nanosheets with tunable architectures. Manipulation of metal nitrate as bifunctional dopants realizes N-doping of graphene oxide and preferential growth of α-Mn2O3 nanocrystals. Generation of Mn-O-C bond during cross-linking greatly strengthens the stability of membranes for long-term steady operation. Meanwhile, because of spatial confinement effects and high binding energy, N-doped reduced GO nanosheets are desirable supports to construct numerous Mn-N-C bonds, thus generating artificial nanopores to significantly increase nanochannels for ultrafast mass transport. Moreover, the size-selective permeability of ultrathin nanoporous GO-based nanofilms can be optimized by managing the types of metal source for target coordination.
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spelling doaj.art-815dafe7b7d64b7cbb3ce15c5e0068592022-12-21T20:32:47ZengElsevieriScience2589-00422021-06-01246102576Confined assembly of ultrathin nanoporous nitrogen-doped graphene nanofilms with dual metal coordination chemistryZehai Xu0Yufan Zhang1Xu Zhang2Qin Meng3Yujie Zhu4Chong Shen5Yinghua Lu6Guoliang Zhang7Congjie Gao8Center for Membrane and Water Science, Institute of Oceanic and Environmental Chemical Engineering, State Key Lab Breeding Base of Green Chemical Synthesis Technology, Zhejiang University of Technology, Hangzhou 310014, P. R. ChinaCollege of Engineering, Carnegie Mellon University, Pittsburgh, PA 15213, USACenter for Membrane and Water Science, Institute of Oceanic and Environmental Chemical Engineering, State Key Lab Breeding Base of Green Chemical Synthesis Technology, Zhejiang University of Technology, Hangzhou 310014, P. R. ChinaCollege of Chemical and Biological Engineering, State Key Laboratory of Chemical Engineering, Zhejiang University, Hangzhou 310027, P. R. ChinaCenter for Membrane and Water Science, Institute of Oceanic and Environmental Chemical Engineering, State Key Lab Breeding Base of Green Chemical Synthesis Technology, Zhejiang University of Technology, Hangzhou 310014, P. R. ChinaCollege of Chemical and Biological Engineering, State Key Laboratory of Chemical Engineering, Zhejiang University, Hangzhou 310027, P. R. ChinaCollege of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, P. R. ChinaCenter for Membrane and Water Science, Institute of Oceanic and Environmental Chemical Engineering, State Key Lab Breeding Base of Green Chemical Synthesis Technology, Zhejiang University of Technology, Hangzhou 310014, P. R. China; Corresponding authorCenter for Membrane and Water Science, Institute of Oceanic and Environmental Chemical Engineering, State Key Lab Breeding Base of Green Chemical Synthesis Technology, Zhejiang University of Technology, Hangzhou 310014, P. R. China; Hangzhou Water Treatment Technology Development Center, National Engineering Research Center for Liquid Separation Membrane, Hangzhou 310012, ChinaSummary: Graphene oxide (GO) nanosheets with unique structure have received much attention in providing opportunity for high-performance membranes in separation. However, the rational design of ultrathin graphene membranes with controlled structures remains a big challenge. Here, we report a methodology to synthesize dual metal-coordinated ultrathin nanoporous graphene nanofilms by tailoring well-aligned nanocrystals as building blocks on heteroatom-doped GO nanosheets with tunable architectures. Manipulation of metal nitrate as bifunctional dopants realizes N-doping of graphene oxide and preferential growth of α-Mn2O3 nanocrystals. Generation of Mn-O-C bond during cross-linking greatly strengthens the stability of membranes for long-term steady operation. Meanwhile, because of spatial confinement effects and high binding energy, N-doped reduced GO nanosheets are desirable supports to construct numerous Mn-N-C bonds, thus generating artificial nanopores to significantly increase nanochannels for ultrafast mass transport. Moreover, the size-selective permeability of ultrathin nanoporous GO-based nanofilms can be optimized by managing the types of metal source for target coordination.http://www.sciencedirect.com/science/article/pii/S2589004221005447ChemistryChemical engineeringOrganic chemistry
spellingShingle Zehai Xu
Yufan Zhang
Xu Zhang
Qin Meng
Yujie Zhu
Chong Shen
Yinghua Lu
Guoliang Zhang
Congjie Gao
Confined assembly of ultrathin nanoporous nitrogen-doped graphene nanofilms with dual metal coordination chemistry
iScience
Chemistry
Chemical engineering
Organic chemistry
title Confined assembly of ultrathin nanoporous nitrogen-doped graphene nanofilms with dual metal coordination chemistry
title_full Confined assembly of ultrathin nanoporous nitrogen-doped graphene nanofilms with dual metal coordination chemistry
title_fullStr Confined assembly of ultrathin nanoporous nitrogen-doped graphene nanofilms with dual metal coordination chemistry
title_full_unstemmed Confined assembly of ultrathin nanoporous nitrogen-doped graphene nanofilms with dual metal coordination chemistry
title_short Confined assembly of ultrathin nanoporous nitrogen-doped graphene nanofilms with dual metal coordination chemistry
title_sort confined assembly of ultrathin nanoporous nitrogen doped graphene nanofilms with dual metal coordination chemistry
topic Chemistry
Chemical engineering
Organic chemistry
url http://www.sciencedirect.com/science/article/pii/S2589004221005447
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