Carbon-doped metal oxide interfacial nanofilms for ultrafast and precise separation of molecules

Sengupta, Bratin; Dong, Qiaobei; Khadka, Rajan; Behera, Dinesh Kumar; Yang, Ruizhe; Liu, Jun; Jiang, Ji; Keblinski, Pawel; Belfort, Georges; Yu, Miao

doi:10.1126/science.adh2404

Carbon-doped metal oxide interfacial nanofilms for ultrafast and precise separation of molecules

Journal Article · 08 September 2023 · Science

DOI:https://doi.org/10.1126/science.adh2404· OSTI ID:2418180

^[1]; ^[2]; Khadka, Rajan ^[3]; ^[2]; ^[4]; ^[4]; ^[5]; Keblinski, Pawel ^[3]; ^[5]; ^[2]

Department of Chemical and Biological Engineering and RENEW Institute, University at Buffalo, Buffalo, NY 14260, USA.; OSTI
Department of Chemical and Biological Engineering and RENEW Institute, University at Buffalo, Buffalo, NY 14260, USA.
Department of Materials Science and Engineering, Rensselaer Polytechnic Institute, Troy, NY 12180, USA.
Department of Mechanical and Aerospace Engineering, University at Buffalo, Buffalo, NY 14260, USA.
Howard P. Isermann Department of Chemical and Biological Engineering and the Center of Biotechnology and Interdisciplinary Studies, Rensselaer Polytechnic Institute, Troy, NY 12180, USA.

Membranes with molecular-sized, high-density nanopores, which are stable under industrially relevant conditions, are needed to decrease energy consumption for separations. Interfacial polymerization has demonstrated its potential for large-scale production of organic membranes, such as polyamide desalination membranes. We report an analogous ultrafast interfacial process to generate inorganic, nanoporous carbon-doped metal oxide (CDTO) nanofilms for precise molecular separation. For a given pore size, these nanofilms have 2 to 10 times higher pore density (assuming the same tortuosity) than reported and commercial organic solvent nanofiltration membranes, yielding ultra-high solvent permeance, even if they are thicker. Owing to exceptional mechanical, chemical, and thermal stabilities, CDTO nanofilms with designable, rigid nanopores exhibited long-term stable and efficient organic separation under harsh conditions.

Research Organization:: Rensselaer Polytechnic Inst., Troy, NY (United States)

Sponsoring Organization:: USDOE Office of Fossil Energy (FE)

DOE Contract Number:: FE0031730; FG02-09ER16005

OSTI ID:: 2418180

Journal Information:: Science, Journal Name: Science Journal Issue: 6662 Vol. 381; ISSN 0036-8075

Publisher:: AAAS

Country of Publication:: United States

Language:: English

References (72)

Polyphenylsulfone-based solvent resistant nanofiltration (SRNF) membrane incorporated with copper-1,3,5-benzenetricarboxylate (Cu-BTC) nanoparticles for methanol separation Sani, N. A. A.; Lau, W. J.; Ismail, A. F. RSC Advances, Vol. 5, Issue 17 https://doi.org/10.1039/C4RA14284E	journal	January 2015
Realizing Mussel-Inspired Polydopamine Selective Layer with Strong Solvent Resistance in Nanofiltration toward Sustainable Reclamation Xu, Yanchao; You, Fangjie; Sun, Hongguang ACS Sustainable Chemistry & Engineering, Vol. 5, Issue 6 https://doi.org/10.1021/acssuschemeng.7b00871	journal	May 2017
Graphene membranes with tuneable nanochannels by intercalating self-assembled porphyrin molecules for organic solvent nanofiltration Gao, Tiantian; Huang, Liang; Li, Chun Carbon, Vol. 124 https://doi.org/10.1016/j.carbon.2017.08.042	journal	November 2017
Polymer nanofilms with enhanced microporosity by interfacial polymerization Jimenez-Solomon, Maria F.; Song, Qilei; Jelfs, Kim E. Nature Materials, Vol. 15, Issue 7 https://doi.org/10.1038/nmat4638	journal	May 2016
Fundamental transport mechanisms, fabrication and potential applications of nanoporous atomically thin membranes Wang, Luda; Boutilier, Michael S. H.; Kidambi, Piran R. Nature Nanotechnology, Vol. 12, Issue 6 https://doi.org/10.1038/nnano.2017.72	journal	June 2017
Simultaneous use of MOFs MIL-101(Cr) and ZIF-11 in thin film nanocomposite membranes for organic solvent nanofiltration Echaide-Górriz, Carlos; Navarro, Marta; Téllez, Carlos Dalton Transactions, Vol. 46, Issue 19 https://doi.org/10.1039/C7DT00197E	journal	January 2017
Surface modification methods of organic solvent nanofiltration membranes Amirilargani, M.; Sadrzadeh, M.; Sudhölter, E. J. R. Chemical Engineering Journal, Vol. 289 https://doi.org/10.1016/j.cej.2015.12.062	journal	April 2016
Crystalline 2D Covalent Organic Framework Membranes for High-Flux Organic Solvent Nanofiltration Shinde, Digambar B.; Sheng, Guan; Li, Xiang Journal of the American Chemical Society, Vol. 140, Issue 43 https://doi.org/10.1021/jacs.8b08788	journal	October 2018
Comparative performance assessment of flat sheet and hollow fiber DCMD processes using CFD modeling Yazgan-Birgi, Pelin; Hassan Ali, Mohamed I.; Arafat, Hassan A. Separation and Purification Technology, Vol. 212 https://doi.org/10.1016/j.seppur.2018.11.085	journal	April 2019
Molecular size-dependent subcontinuum solvent permeation and ultrafast nanofiltration across nanoporous graphene membranes Cheng, Chi; Iyengar, Sathvik Ajay; Karnik, Rohit Nature Nanotechnology, Vol. 16, Issue 9 https://doi.org/10.1038/s41565-021-00933-0	journal	July 2021
Electropolymerization of robust conjugated microporous polymer membranes for rapid solvent transport and narrow molecular sieving Zhou, Zongyao; Li, Xiang; Guo, Dong Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-19182-1	journal	October 2020
MOF nanoparticles of MIL-68(Al), MIL-101(Cr) and ZIF-11 for thin film nanocomposite organic solvent nanofiltration membranes Echaide-Górriz, Carlos; Sorribas, Sara; Téllez, Carlos RSC Advances, Vol. 6, Issue 93 https://doi.org/10.1039/C6RA17522H	journal	January 2016
Membrane Separation in Organic Liquid: Technologies, Achievements, and Opportunities Liang, Bin; He, Xiao; Hou, Junjun Advanced Materials, Vol. 31, Issue 45 https://doi.org/10.1002/adma.201806090	journal	December 2018
Realizing small-flake graphene oxide membranes for ultrafast size-dependent organic solvent nanofiltration Nie, Lina; Goh, Kunli; Wang, Yu Science Advances, Vol. 6, Issue 17 https://doi.org/10.1126/sciadv.aaz9184	journal	April 2020
Visualization and analysis of atomistic simulation data with OVITO–the Open Visualization Tool Stukowski, Alexander Modelling and Simulation in Materials Science and Engineering, Vol. 18, Issue 1 https://doi.org/10.1088/0965-0393/18/1/015012	journal	December 2009
Fungal Cell Wall‐Graphene Oxide Microcomposite Membrane for Organic Solvent Nanofiltration Zhang, Liyuan; Zhang, Mengchen; Liu, Gongping Advanced Functional Materials, Vol. 31, Issue 23 https://doi.org/10.1002/adfm.202100110	journal	March 2021
Fabrication and characterization of a novel nanofiltration membrane by the interfacial polymerization of 1,4-diaminocyclohexane (DCH) and trimesoyl chloride (TMC) Chen, Gui-E.; Liu, Yan-Jun; Xu, Zhen-Liang RSC Advances, Vol. 5, Issue 51 https://doi.org/10.1039/C5RA02560E	journal	January 2015
Cyclodextrin Films with Fast Solvent Transport and Shape-Selective Permeability Villalobos, Luis Francisco; Huang, Tiefan; Peinemann, Klaus-Viktor Advanced Materials, Vol. 29, Issue 26 https://doi.org/10.1002/adma.201606641	journal	April 2017
Effect of solvent properties on permeate flow through nanofiltration membranes. Part I: investigation of parameters affecting solvent flux Machado, Darı́o R.; Hasson, David; Semiat, Raphael Journal of Membrane Science, Vol. 163, Issue 1 https://doi.org/10.1016/S0376-7388(99)00158-1	journal	October 1999
Poly (maleic anhydride-alt-1-alkenes) directly grafted to γ-alumina for high-performance organic solvent nanofiltration membranes Amirilargani, Mohammad; Merlet, Renaud B.; Nijmeijer, Arian Journal of Membrane Science, Vol. 564 https://doi.org/10.1016/j.memsci.2018.07.042	journal	October 2018
Hydrocarbon ladder polymers with ultrahigh permselectivity for membrane gas separations Lai, Holden W. H.; Benedetti, Francesco M.; Ahn, Jun Myun Science, Vol. 375, Issue 6587 https://doi.org/10.1126/science.abl7163	journal	March 2022
Molecularly-porous ultrathin membranes for highly selective organic solvent nanofiltration Huang, Tiefan; Moosa, Basem A.; Hoang, Phuong Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-19404-6	journal	November 2020
Alginate-based membranes: Paving the way for green organic solvent nanofiltration Aburabie, Jamaliah H.; Puspasari, Tiara; Peinemann, Klaus-Viktor Journal of Membrane Science, Vol. 596 https://doi.org/10.1016/j.memsci.2019.117615	journal	February 2020
Highly porous nanofiber-supported monolayer graphene membranes for ultrafast organic solvent nanofiltration Shen, Liang; Shi, Qi; Zhang, Shengping Science Advances, Vol. 7, Issue 37 https://doi.org/10.1126/sciadv.abg6263	journal	September 2021
An overview of molecular layer deposition for organic and organic–inorganic hybrid materials: mechanisms, growth characteristics, and promising applications Meng, Xiangbo Journal of Materials Chemistry A, Vol. 5, Issue 35 https://doi.org/10.1039/C7TA04449F	journal	January 2017
Development of a ReaxFF Reactive Force Field for Titanium Dioxide/Water Systems Kim, Sung-Yup; Kumar, Nitin; Persson, Petter Langmuir, Vol. 29, Issue 25 https://doi.org/10.1021/la4006983	journal	June 2013
Synergistic effects in combined fouling of a loose nanofiltration membrane by colloidal materials and natural organic matter Li, Qilin; Elimelech, Menachem Journal of Membrane Science, Vol. 278, Issue 1-2 https://doi.org/10.1016/j.memsci.2005.10.045	journal	July 2006
Nanoscale control of internal inhomogeneity enhances water transport in desalination membranes Culp, Tyler E.; Khara, Biswajit; Brickey, Kaitlyn P. Science, Vol. 371, Issue 6524 https://doi.org/10.1126/science.abb8518	journal	January 2021
Hydrophobic polyamide nanofilms provide rapid transport for crude oil separation Li, Siyao; Dong, Ruijiao; Musteata, Valentina-Elena Science, Vol. 377, Issue 6614 https://doi.org/10.1126/science.abq0598	journal	September 2022
Controlling the Selectivity of Conjugated Microporous Polymer Membrane for Efficient Organic Solvent Nanofiltration He, Xiao; Sin, Haksong; Liang, Bin Advanced Functional Materials, Vol. 29, Issue 32 https://doi.org/10.1002/adfm.201900134	journal	June 2019
Solvent transport in organic solvent nanofiltration membranes Silva, Pedro; Han, Shejiao; Livingston, Andrew G. Journal of Membrane Science, Vol. 262, Issue 1-2 https://doi.org/10.1016/j.memsci.2005.03.052	journal	October 2005
Membrane selectivity in the organic solvent nanofiltration of trialkylamine bases Patterson, Darrell A.; Yen Lau, Lay; Roengpithya, Chayaporn Desalination, Vol. 218, Issue 1-3 https://doi.org/10.1016/j.desal.2007.02.020	journal	January 2008
In-situ interfacial formation of TiO 2 /polypyrrole selective layer for improving the separation efficiency towards molecular separation Cheng, Xiquan; Ding, Shangang; Guo, Jiang Journal of Membrane Science, Vol. 536 https://doi.org/10.1016/j.memsci.2017.04.057	journal	August 2017
Sub-10 nm polyamide nanofilms with ultrafast solvent transport for molecular separation Karan, S.; Jiang, Z.; Livingston, A. G. Science, Vol. 348, Issue 6241 https://doi.org/10.1126/science.aaa5058	journal	June 2015
VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data Momma, Koichi; Izumi, Fujio Journal of Applied Crystallography, Vol. 44, Issue 6 https://doi.org/10.1107/S0021889811038970	journal	October 2011
Design of Three‐Dimensional Covalent Organic Framework Membranes for Fast and Robust Organic Solvent Nanofiltration Shi, Xiansong; Zhang, Zhipeng; Yin, Congcong Angewandte Chemie International Edition, Vol. 61, Issue 36 https://doi.org/10.1002/anie.202207559	journal	July 2022
Mechanisms of solute rejection in solvent resistant nanofiltration: the effect of solvent on solute rejection Darvishmanesh, Siavash; Degrève, Jan; Van der Bruggen, Bart Physical Chemistry Chemical Physics, Vol. 12, Issue 40 https://doi.org/10.1039/c0cp00230e	journal	January 2010
Lysozyme Membranes Promoted by Hydrophobic Substrates for Ultrafast and Precise Organic Solvent Nanofiltration Wu, Ming-Bang; Yang, Facui; Yang, Jing Nano Letters, Vol. 20, Issue 12 https://doi.org/10.1021/acs.nanolett.0c03632	journal	November 2020
Role of Magnesium in Soda-Lime Glasses: Insight into Structural, Transport, and Mechanical Properties through Computer Simulations Pedone, Alfonso; Malavasi, Gianluca; Menziani, M. Cristina The Journal of Physical Chemistry C, Vol. 112, Issue 29 https://doi.org/10.1021/jp8016776	journal	June 2008
Facile pore size tuning and characterization of nanoporous ceramic membranes for the purification of polysaccharide Chen, Xianfu; Qi, Ting; Zhang, Yun Journal of Membrane Science, Vol. 597 https://doi.org/10.1016/j.memsci.2019.117631	journal	March 2020
Micromechanism of oxygen transport during initial stage oxidation in Si(100) surface: A ReaxFF molecular dynamics simulation study Sun, Yu; Liu, Yilun; Chen, Xuefeng Applied Surface Science, Vol. 406 https://doi.org/10.1016/j.apsusc.2017.01.302	journal	June 2017
On the contact area for nanoindentation tests with Berkovich indenter: case study on soda-lime glass Gong, Jianghong; Miao, Hezhuo; Peng, Zhijian Materials Letters, Vol. 58, Issue 7-8 https://doi.org/10.1016/j.matlet.2003.09.026	journal	March 2004
Tailoring TiO2 membranes for nanofiltration and tight ultrafiltration by leveraging molecular layer deposition and crystallization Wu, Shanshan; Wang, Zhaogen; Xiong, Sen Journal of Membrane Science, Vol. 578 https://doi.org/10.1016/j.memsci.2019.02.037	journal	May 2019
Na ⁺ -gated water-conducting nanochannels for boosting CO ₂ conversion to liquid fuels Li, Huazheng; Qiu, Chenglong; Ren, Shoujie Science, Vol. 367, Issue 6478 https://doi.org/10.1126/science.aaz6053	journal	February 2020
Stress evolution during the oxidation of silicon nanowires in the sub-10 nm diameter regime Kim, Byung-Hyun; Ariesto Pamungkas, Mauludi; Park, Mina Applied Physics Letters, Vol. 99, Issue 14 https://doi.org/10.1063/1.3643038	journal	October 2011
Molecular Separation with Organic Solvent Nanofiltration: A Critical Review Marchetti, Patrizia; Jimenez Solomon, Maria F.; Szekely, Gyorgy Chemical Reviews, Vol. 114, Issue 21 https://doi.org/10.1021/cr500006j	journal	October 2014
In situ growth of a tubular MoS₂ membrane on a ceramic tube with improved organic solvent nanofiltration performance Liu, Tongtong; Qin, Zhenping; Liu, Qiaohong Materials Chemistry Frontiers, Vol. 5, Issue 7 https://doi.org/10.1039/D1QM00104C	journal	January 2021
Ultrathin graphene-based membrane with precise molecular sieving and ultrafast solvent permeation Yang, Q.; Su, Y.; Chi, C. Nature Materials, Vol. 16, Issue 12 https://doi.org/10.1038/nmat5025	journal	November 2017
Nanofiltration-based diafiltration process for solvent exchange in pharmaceutical manufacturing Sheth, Jignesh P.; Qin, Yingjie; Sirkar, Kamalesh K. Journal of Membrane Science, Vol. 211, Issue 2 https://doi.org/10.1016/S0376-7388(02)00423-4	journal	January 2003
High Flux Thin Film Nanocomposite Membranes Based on Metal–Organic Frameworks for Organic Solvent Nanofiltration Sorribas, Sara; Gorgojo, Patricia; Téllez, Carlos Journal of the American Chemical Society, Vol. 135, Issue 40 https://doi.org/10.1021/ja407665w	journal	September 2013
Precise Molecular Sieving Architectures with Janus Pathways for Both Polar and Nonpolar Molecules Liu, Jiangtao; Hua, Dan; Zhang, Yu Advanced Materials, Vol. 30, Issue 11 https://doi.org/10.1002/adma.201705933	journal	January 2018
Swelling of 9 polymers commonly employed for solvent-resistant nanofiltration membranes: A comprehensive dataset Kappert, Emiel J.; Raaijmakers, Michiel J. T.; Tempelman, Kristianne Journal of Membrane Science, Vol. 569 https://doi.org/10.1016/j.memsci.2018.09.059	journal	January 2019
TiO2 nanofiltration membranes prepared by molecular layer deposition for water purification Song, Zhuonan; Fathizadeh, Mahdi; Huang, Yi Journal of Membrane Science, Vol. 510 https://doi.org/10.1016/j.memsci.2016.03.011	journal	July 2016
Ultrafast Viscous Permeation of Organic Solvents Through Diamond-Like Carbon Nanosheets Karan, S.; Samitsu, S.; Peng, X. Science, Vol. 335, Issue 6067 https://doi.org/10.1126/science.1212101	journal	January 2012
Reduced Graphene Oxide Membranes for Ultrafast Organic Solvent Nanofiltration Huang, Liang; Chen, Ji; Gao, Tiantian Advanced Materials, Vol. 28, Issue 39 https://doi.org/10.1002/adma.201601606	journal	August 2016
Amidoxime-functionalized polymer of intrinsic microporosity (AOPIM-1)-based thin film composite membranes with ultrahigh permeance for organic solvent nanofiltration Jin, Yehao; Song, Qiangqiang; Xie, Na Journal of Membrane Science, Vol. 632 https://doi.org/10.1016/j.memsci.2021.119375	journal	August 2021
Polyamide nanofiltration membrane with highly uniform sub-nanometre pores for sub-1 Å precision separation Liang, Yuanzhe; Zhu, Yuzhang; Liu, Cheng Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15771-2	journal	April 2020
Pore engineering of ultrathin covalent organic framework membranes for organic solvent nanofiltration and molecular sieving Shinde, Digambar B.; Cao, Li; Wonanke, A. D. Dinga Chemical Science, Vol. 11, Issue 21 https://doi.org/10.1039/D0SC01679A	journal	January 2020
N -Aryl–linked spirocyclic polymers for membrane separations of complex hydrocarbon mixtures Thompson, Kirstie A.; Mathias, Ronita; Kim, Daeok Science, Vol. 369, Issue 6501 https://doi.org/10.1126/science.aba9806	journal	July 2020
Thin-Film Nanocomposite Membrane with the Minimum Amount of MOF by the Langmuir–Schaefer Technique for Nanofiltration Navarro, Marta; Benito, Javier; Paseta, Lorena ACS Applied Materials & Interfaces, Vol. 10, Issue 1 https://doi.org/10.1021/acsami.7b17477	journal	December 2017
Microporous membranes comprising conjugated polymers with rigid backbones enable ultrafast organic-solvent nanofiltration Liang, Bin; Wang, Hui; Shi, Xinghua Nature Chemistry, Vol. 10, Issue 9 https://doi.org/10.1038/s41557-018-0093-9	journal	July 2018
Finely Tuned Submicroporous Thin‐Film Molecular Sieve Membranes for Highly Efficient Fluid Separations Ali, Zain; Ghanem, Bader S.; Wang, Yingge Advanced Materials, Vol. 32, Issue 22 https://doi.org/10.1002/adma.202001132	journal	April 2020
Ultrathin 2D‐Layered Cyclodextrin Membranes for High‐ Performance Organic Solvent Nanofiltration Huang, Tiefan; Puspasari, Tiara; Nunes, Suzana P. Advanced Functional Materials, Vol. 30, Issue 4 https://doi.org/10.1002/adfm.201906797	journal	November 2019
Size and Shape of Protein Molecules at the Nanometer Level Determined by Sedimentation, Gel Filtration, and Electron Microscopy Erickson, Harold P. Biological Procedures Online, Vol. 11, Issue 1 https://doi.org/10.1007/s12575-009-9008-x	journal	May 2009
Ultrathin Single Bilayer Separation Membranes Based on Hyperbranched Sulfonated Poly(aryleneoxindole) Joseph, Nithya; Thomas, Joice; Ahmadiannamini, Pejman Advanced Functional Materials, Vol. 27, Issue 9 https://doi.org/10.1002/adfm.201605068	journal	January 2017
Aligned macrocycle pores in ultrathin films for accurate molecular sieving Jiang, Zhiwei; Dong, Ruijiao; Evans, Austin M. Nature, Vol. 609, Issue 7925 https://doi.org/10.1038/s41586-022-05032-1	journal	August 2022
Scaling up nanoporous graphene membranes Mi, Baoxia Science, Vol. 364, Issue 6445 https://doi.org/10.1126/science.aax3103	journal	June 2019
Observations on solvent flux and solute rejection across solvent resistant nanofiltration membranes Gibbins, Emma; D' Antonio, Marco; Nair, Dinesh Desalination, Vol. 147, Issue 1-3 https://doi.org/10.1016/S0011-9164(02)00557-X	journal	September 2002
Oxidation of Silicon Carbide by O ₂ and H ₂ O: A ReaxFF Reactive Molecular Dynamics Study, Part I Newsome, David A.; Sengupta, Debasis; Foroutan, Hosein The Journal of Physical Chemistry C, Vol. 116, Issue 30 https://doi.org/10.1021/jp306391p	journal	July 2012
LAMMPS - a flexible simulation tool for particle-based materials modeling at the atomic, meso, and continuum scales Thompson, Aidan P.; Aktulga, H. Metin; Berger, Richard Computer Physics Communications, Vol. 271 https://doi.org/10.1016/j.cpc.2021.108171	journal	February 2022
PACKMOL: A package for building initial configurations for molecular dynamics simulations Martínez, L.; Andrade, R.; Birgin, E. G. Journal of Computational Chemistry, Vol. 30, Issue 13 https://doi.org/10.1002/jcc.21224	journal	October 2009
Interlayered thin-film nanocomposite membrane with synergetic effect of COFs interlayer and GQDs incorporation for organic solvent nanofiltration Li, Shuxuan; Yin, Yating; Liu, Shaoxiao Journal of Membrane Science, Vol. 662 https://doi.org/10.1016/j.memsci.2022.120930	journal	October 2022

Similar Records

Solvent Transport in Disordered and Dynamic Membrane Pores: Implications for Reverse Osmosis and Nanofiltration Membranes

Journal Article · 2025 · Environmental Science & Technology · OSTI ID:2587308

Ultrathin-film composite (uTFC) membranes based on amorphous perfluoropolymers for liquid separations

Journal Article · 2022 · Journal of Membrane Science · OSTI ID:2418815

Robust natural nanocomposites realizing unprecedented ultrafast precise molecular separations

Journal Article · 2020 · Materials Today · OSTI ID:1619147

Related Subjects

Science & Technology - Other Topics

Carbon-doped metal oxide interfacial nanofilms for ultrafast and precise separation of molecules

Citation Formats

References (72)

Similar Records

Related Subjects