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Affiliations

1 †MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, Guangzhou 510275, China.

2 ‡Van't Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, 1098 XH Amsterdam, The Netherlands.

Chun-Ting He et al.

J Am Chem Soc .

2015 .

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1 †MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, Guangzhou 510275, China.

2 ‡Van't Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, 1098 XH Amsterdam, The Netherlands.

Starov VM.
Starov VM.
Adv Colloid Interface Sci. 2004 Nov 29;111(1-2):3-27. doi: 10.1016/j.cis.2004.07.007.
Adv Colloid Interface Sci. 2004.

PMID: 15571660

Tian J, Lu C, He CT, Lu TB, Ouyang G.
Tian J, et al.
Talanta. 2016 May 15;152:283-7. doi: 10.1016/j.talanta.2016.02.007. Epub 2016 Feb 2.
Talanta. 2016.

PMID: 26992522

Bhadra BN, Seo PW, Khan NA, Jhung SH.
Bhadra BN, et al.
Inorg Chem. 2016 Nov 7;55(21):11362-11371. doi: 10.1021/acs.inorgchem.6b01882. Epub 2016 Oct 20.
Inorg Chem. 2016.

PMID: 27763765

Van der Perre S, Van Assche T, Bozbiyik B, Lannoeye J, De Vos DE, Baron GV, Denayer JF.
Van der Perre S, et al.
Langmuir. 2014 Jul 22;30(28):8416-24. doi: 10.1021/la501594t. Epub 2014 Jul 7.
Langmuir. 2014.

PMID: 24963698

Zhang JP, Chen XM.
Zhang JP, et al.
J Am Chem Soc. 2008 May 7;130(18):6010-7. doi: 10.1021/ja800550a. Epub 2008 Apr 3.
J Am Chem Soc. 2008.

PMID: 18386891

Gao M, Wang J, Rong Z, Shi Q, Dong J.
Gao M, et al.
RSC Adv. 2018 Nov 27;8(69):39627-39634. doi: 10.1039/c8ra08460b. eCollection 2018 Nov 23.
RSC Adv. 2018.

PMID: 35558014
Free PMC article.

Cao LM, Zhang J, Zhang XF, He CT.
Cao LM, et al.
Chem Sci. 2022 Jan 19;13(6):1569-1593. doi: 10.1039/d1sc05983a. eCollection 2022 Feb 9.
Chem Sci. 2022.

PMID: 35282621
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Wang C, Zhou DD, Gan YW, Zhang XW, Ye ZM, Zhang JP.
Wang C, et al.
Natl Sci Rev. 2020 May 8;8(3):nwaa094. doi: 10.1093/nsr/nwaa094. eCollection 2021 Mar.
Natl Sci Rev. 2020.

PMID: 34691585
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Krishna R, van Baten JM.
Krishna R, et al.
ACS Omega. 2021 Jun 2;6(23):15499-15513. doi: 10.1021/acsomega.1c02136. eCollection 2021 Jun 15.
ACS Omega. 2021.

PMID: 34151128
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Krishna R, van Baten JM.
Krishna R, et al.
ACS Omega. 2020 Oct 22;5(43):28393-28402. doi: 10.1021/acsomega.0c04491. eCollection 2020 Nov 3.
ACS Omega. 2020.

PMID: 33163823
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Porous materials combining high hydrophobicity, large surface area, as well as large and uniform pore size are very useful but rare. The nanoporous zeolitic metal azolate framework, RHO-[Zn(eim)2] (MAF-6, Heim = 2-ethylimidazole), is an attractive candidate but thought to be unobtainable/unstable. In this work, the supramolecular isomerism of [Zn(eim)2] is thoroughly studied using a rapid solution mixing reaction of [Zn(NH3)4](OH)2 and Heim, which enables MAF-6 with high crystallinity, purity, and thermal/chemical stabilities to be synthesized in large quantity. Gas and vapor adsorption isotherms, gas chromatography, and water contact angle measurements, as well as transient breakthrough and molecular dynamics simulations show that MAF-6 exhibits large surface area (langmuir surface area 1695 m(2) g(-1)), pore volume (0.61 cm(3) g(-1)), pore size (d = 18.4 Å), and aperture size (d = 7.6 Å) with high hydrophobicity on both the internal pore and external crystal surfaces. It can barely adsorb water or be wetted by water (contact angle 143°) but readily adsorb large amounts of organic molecules including methanol, ethanol, mesitylene, adamantane, C6-C10 hydrocarbons, xylene isomers, and saturated/unsaturated analogues such as benzene/cyclohexene/cyclohexane or styrene/ethylbenzene. It can also separate these organic molecules from each other as well as from water by preferential adsorption/retention of those having higher hydrophobicity, lipophilicity, or oil/water partition coefficient. These properties are very different with other porous materials such as SOD-[Zn(mim)2] (Hmim = 2-methylimidazole, MAF-4/ZIF-8) with a hydrophobic pore surface but a hydrophilic crystal surface and small aperture size.

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1 Department of Chemical and Biomolecular Engineering, National University of Singapore, 10 Kent Ridge Crescent, Singapore 119620.

Xiao Ying Bao et al.

J Phys Chem B .

2005 .

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1 Department of Chemical and Biomolecular Engineering, National University of Singapore, 10 Kent Ridge Crescent, Singapore 119620.

Bao XY, Li X, Zhao XS.
Bao XY, et al.
J Phys Chem B. 2006 Feb 16;110(6):2656-61. doi: 10.1021/jp0561120.
J Phys Chem B. 2006.

PMID: 16471868

Cho EB, Kim D, Jaroniec M.
Cho EB, et al.
Langmuir. 2007 Nov 6;23(23):11844-9. doi: 10.1021/la701948g. Epub 2007 Oct 6.
Langmuir. 2007.

PMID: 17918981

Kubo S, Kosuge K.
Kubo S, et al.
Langmuir. 2007 Nov 6;23(23):11761-8. doi: 10.1021/la701556y. Epub 2007 Oct 13.
Langmuir. 2007.

PMID: 17935361

Wang W, Lofgreen JE, Ozin GA.
Wang W, et al.
Small. 2010 Dec 6;6(23):2634-42. doi: 10.1002/smll.201000617. Epub 2010 Oct 18.
Small. 2010.

PMID: 20957618

Review.

Sun J, Bao X.
Sun J, et al.
Chemistry. 2008;14(25):7478-88. doi: 10.1002/chem.200800823.
Chemistry. 2008.

PMID: 18668502

Review.

Siefker J, Karande P, Coppens MO.
Siefker J, et al.
Expert Opin Drug Deliv. 2014 Nov;11(11):1781-93. doi: 10.1517/17425247.2014.938636. Epub 2014 Jul 12.
Expert Opin Drug Deliv. 2014.

PMID: 25016923
Free PMC article.

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In this article, we report a systematic investigation on the morphologies of SBA-15 type large-pore periodic mesoporous organosilicas templated by the block copolymer P123. By tuning synthetic parameters such as stirring, acidity, reaction ratio, reaction duration, and autoclaving, a wide spectrum of unique primary particle morphologies, such as the spindle-, pearl-, diamond-, rod-, and platelike particles, and nanoparticles has been prepared. These primary particles were found to self-assemble in solution to form various large hierarchical macrostructures, such as mesostructured necklaces and cobweb-supported necklaces. The assembling process was elucidated with the information observed at different stages of reaction. Stirring, reaction duration, and autoclaving were identified to be the key factors affecting the efficiency and degree of the self-assembly process. A nucleation-accretion mechanism for the formation of various PMO primary particles was proposed by examining the relation between the external morphologies and the underlying mesostructure.

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