Bottom-up synthesis of graphene films hosting atom-thick molecular-sieving apertures
Incorporation of a high density of molecular-sieving nanopores in the graphene lattice by the bottom-up synthesis is highly attractive for high-performance membranes. Herein, we achieve this by a controlled synthesis of nanocrystalline graphene where incomplete growth of a few nanometer-sized, misor...
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| Published in | Proceedings of the National Academy of Sciences - PNAS Vol. 118; no. 37; pp. 1 - 10 |
|---|---|
| Main Authors | , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Washington
National Academy of Sciences
14.09.2021
|
| Series | Membrane Separations Science Special Feature |
| Subjects | |
| Online Access | Get full text |
| ISSN | 0027-8424 1091-6490 1091-6490 |
| DOI | 10.1073/pnas.2022201118 |
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| Abstract | Incorporation of a high density of molecular-sieving nanopores in the graphene lattice by the bottom-up synthesis is highly attractive for high-performance membranes. Herein, we achieve this by a controlled synthesis of nanocrystalline graphene where incomplete growth of a few nanometer-sized, misoriented grains generates molecular-sized pores in the lattice. The density of pores is comparable to that obtained by the state-of-the-art postsynthetic etching (1012 cm−2) and is up to two orders of magnitude higher than that of molecular-sieving intrinsic vacancy defects in single-layer graphene (SLG) prepared by chemical vapor deposition. The porous nanocrystalline graphene (PNG) films are synthesized by precipitation of C dissolved in the Ni matrix where the C concentration is regulated by controlled pyrolysis of precursors (polymers and/or sugar). The PNG film is made of few-layered graphene except near the grain edge where the grains taper down to a single layer and eventually terminate into vacancy defects at a node where three or more grains meet. This unique nanostructure is highly attractive for the membranes because the layered domains improve the mechanical robustness of the film while the atom-thick molecular-sized apertures allow the realization of large gas transport. The combination of gas permeance and gas pair selectivity is comparable to that from the nanoporous SLG membranes prepared by state-of-the-art postsynthetic lattice etching. Overall, the method reported here improves the scale-up potential of graphene membranes by cutting down the processing steps. |
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| AbstractList | The energy efficiency of gas separation is expected to benefit from the development of membranes yielding selective but large permeance. The ultimate limit of this is two-dimensional films hosting a high density of molecular-selective apertures (e.g., nanoporous single-layer graphene). Currently, pores are incorporated in single-layer graphene by postsynthetic etching route, and the direct bottom-up synthesis of nanoporous graphene, especially targeting a high pore density, remains a grand challenge attributing to a number of crystallization bottlenecks. We address this by increasing the density of molecular-sized intrinsic vacancy defects in graphene by developing crystallization conditions which promote the growth of misoriented grains, limiting the grains to a few nanometers in size and preventing a complete grain intergrowth while yielding mechanically robust films.
Incorporation of a high density of molecular-sieving nanopores in the graphene lattice by the bottom-up synthesis is highly attractive for high-performance membranes. Herein, we achieve this by a controlled synthesis of nanocrystalline graphene where incomplete growth of a few nanometer-sized, misoriented grains generates molecular-sized pores in the lattice. The density of pores is comparable to that obtained by the state-of-the-art postsynthetic etching (10
12
cm
−2
) and is up to two orders of magnitude higher than that of molecular-sieving intrinsic vacancy defects in single-layer graphene (SLG) prepared by chemical vapor deposition. The porous nanocrystalline graphene (PNG) films are synthesized by precipitation of C dissolved in the Ni matrix where the C concentration is regulated by controlled pyrolysis of precursors (polymers and/or sugar). The PNG film is made of few-layered graphene except near the grain edge where the grains taper down to a single layer and eventually terminate into vacancy defects at a node where three or more grains meet. This unique nanostructure is highly attractive for the membranes because the layered domains improve the mechanical robustness of the film while the atom-thick molecular-sized apertures allow the realization of large gas transport. The combination of gas permeance and gas pair selectivity is comparable to that from the nanoporous SLG membranes prepared by state-of-the-art postsynthetic lattice etching. Overall, the method reported here improves the scale-up potential of graphene membranes by cutting down the processing steps. Incorporation of a high density of molecular-sieving nanopores in the graphene lattice by the bottom-up synthesis is highly attractive for high-performance membranes. Herein, we achieve this by a controlled synthesis of nanocrystalline graphene where incomplete growth of a few nanometer-sized, misoriented grains generates molecular-sized pores in the lattice. The density of pores is comparable to that obtained by the state-of-the-art postsynthetic etching (1012 cm−2) and is up to two orders of magnitude higher than that of molecular-sieving intrinsic vacancy defects in single-layer graphene (SLG) prepared by chemical vapor deposition. The porous nanocrystalline graphene (PNG) films are synthesized by precipitation of C dissolved in the Ni matrix where the C concentration is regulated by controlled pyrolysis of precursors (polymers and/or sugar). The PNG film is made of few-layered graphene except near the grain edge where the grains taper down to a single layer and eventually terminate into vacancy defects at a node where three or more grains meet. This unique nanostructure is highly attractive for the membranes because the layered domains improve the mechanical robustness of the film while the atom-thick molecular-sized apertures allow the realization of large gas transport. The combination of gas permeance and gas pair selectivity is comparable to that from the nanoporous SLG membranes prepared by state-of-the-art postsynthetic lattice etching. Overall, the method reported here improves the scale-up potential of graphene membranes by cutting down the processing steps. Incorporation of a high density of molecular-sieving nanopores in the graphene lattice by the bottom-up synthesis is highly attractive for high-performance membranes. Herein, we achieve this by a controlled synthesis of nanocrystalline graphene where incomplete growth of a few nanometer-sized, misoriented grains generates molecular-sized pores in the lattice. The density of pores is comparable to that obtained by the state-of-the-art postsynthetic etching (1012 cm-2) and is up to two orders of magnitude higher than that of molecular-sieving intrinsic vacancy defects in single-layer graphene (SLG) prepared by chemical vapor deposition. The porous nanocrystalline graphene (PNG) films are synthesized by precipitation of C dissolved in the Ni matrix where the C concentration is regulated by controlled pyrolysis of precursors (polymers and/or sugar). The PNG film is made of few-layered graphene except near the grain edge where the grains taper down to a single layer and eventually terminate into vacancy defects at a node where three or more grains meet. This unique nanostructure is highly attractive for the membranes because the layered domains improve the mechanical robustness of the film while the atom-thick molecular-sized apertures allow the realization of large gas transport. The combination of gas permeance and gas pair selectivity is comparable to that from the nanoporous SLG membranes prepared by state-of-the-art postsynthetic lattice etching. Overall, the method reported here improves the scale-up potential of graphene membranes by cutting down the processing steps.Incorporation of a high density of molecular-sieving nanopores in the graphene lattice by the bottom-up synthesis is highly attractive for high-performance membranes. Herein, we achieve this by a controlled synthesis of nanocrystalline graphene where incomplete growth of a few nanometer-sized, misoriented grains generates molecular-sized pores in the lattice. The density of pores is comparable to that obtained by the state-of-the-art postsynthetic etching (1012 cm-2) and is up to two orders of magnitude higher than that of molecular-sieving intrinsic vacancy defects in single-layer graphene (SLG) prepared by chemical vapor deposition. The porous nanocrystalline graphene (PNG) films are synthesized by precipitation of C dissolved in the Ni matrix where the C concentration is regulated by controlled pyrolysis of precursors (polymers and/or sugar). The PNG film is made of few-layered graphene except near the grain edge where the grains taper down to a single layer and eventually terminate into vacancy defects at a node where three or more grains meet. This unique nanostructure is highly attractive for the membranes because the layered domains improve the mechanical robustness of the film while the atom-thick molecular-sized apertures allow the realization of large gas transport. The combination of gas permeance and gas pair selectivity is comparable to that from the nanoporous SLG membranes prepared by state-of-the-art postsynthetic lattice etching. Overall, the method reported here improves the scale-up potential of graphene membranes by cutting down the processing steps. |
| Author | (赵康宁), Kangning Zhao Oveisib, Emad Agrawal, Kumar Varoon Moradi, Mina Dakhchoune, Mostapha Goethem, Cédric Van Li, Shaoxian Boureaub, Victor Huang, Shiqi Hsu, Kuang-Jung Villalobos, Luis Francisco (沈悦卿), Yueqing Shen |
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| CitedBy_id | crossref_primary_10_1002_ange_202200321 crossref_primary_10_1016_j_carbon_2024_118866 crossref_primary_10_1038_s41563_022_01325_y crossref_primary_10_1103_PhysRevLett_131_168001 crossref_primary_10_1038_s41598_024_84308_0 crossref_primary_10_1002_anie_202200321 crossref_primary_10_1016_j_isci_2022_103832 crossref_primary_10_1021_acs_langmuir_3c00797 crossref_primary_10_1002_smll_202404087 crossref_primary_10_1016_j_seppur_2022_122919 crossref_primary_10_1021_acsnano_3c11885 crossref_primary_10_1021_accountsmr_2c00143 crossref_primary_10_1021_acsnano_2c03730 crossref_primary_10_1073_pnas_2106494118 |
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| Notes | ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 14 content type line 23 Author contributions: L.F.V., C.V.G., and K.V.A. designed research; L.F.V., C.V.G., K.-J.H., S.L., M.M., K.Z., M.D., S.H., Y.S., and E.O. performed research; L.F.V., C.V.G., K.-J.H., S.L., M.M., K.Z., M.D., S.H., Y.S., E.O., V.B., and K.V.A. analyzed data; and L.F.V., C.V.G., and K.V.A. wrote the paper. 1L.F.V. and C.V.G. contributed equally to this work. Edited by Manish Kumar, The University of Texas at Austin, Austin, TX, and accepted by Editorial Board Member Pablo G. Debenedetti March 28, 2021 (received for review December 1, 2020) |
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| Snippet | Incorporation of a high density of molecular-sieving nanopores in the graphene lattice by the bottom-up synthesis is highly attractive for high-performance... The energy efficiency of gas separation is expected to benefit from the development of membranes yielding selective but large permeance. The ultimate limit of... |
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| SubjectTerms | Apertures Chemical synthesis Chemical vapor deposition Crystal defects Density Etching Gas transport Graphene Lattice vacancies Membranes Nanocrystals Physical Sciences Polymers Pores Prepolymers Pyrolysis Selectivity Thick films |
| Title | Bottom-up synthesis of graphene films hosting atom-thick molecular-sieving apertures |
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