Design of carbon–ceramic composite membranes with tunable molecular cut-offs from a carboxylic benzoxazine ligand chelated to silica–zirconia

Lawal, Sulaiman Oladipo; Nagasawa, Hiroki; Tsuru, Toshinori; Kanezashi, Masakoto

doi:10.1039/d2me00078d

Cited by 3 publications

(15 citation statements)

References 47 publications

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“…In our previous work, the successful formation of a polybenzoxazine-modified SiO 2 -ZrO 2 was established [ 25 ]. The resin of a SiO 2 -ZrO 2 and polybenzoxazine inorganic-organic hybrid was formed from vinyl trimethoxysilane (VTMS), zirconium n-butoxide (ZrTB), and a benzoxazine compound 3-(3-oxo-1,4-benzoxazin-4-yl) propanoic acid (BZPA) precursors.…”

Section: Resultsmentioning

confidence: 99%

“…The SiO 2 -ZrO 2 -polybenzoxazine resin cured at 200 °C was pyrolyzed to form carbon-SiO 2 -ZrO 2 . The inert calcination of the SiO 2 -ZrO 2 -polybenzoxzine resin resulted in a decomposition of the polymer chain into a sp 2 type of carbon and the ceramic transformation of the -C-Si-O-Zr- phase to form a carbon-SiO 2 -ZrO 2 composite [ 25 ]. Figure 4 a shows the thermogravimetric (TG) profile of SiO 2 -ZrO 2 -polybenzoxzine decomposition under an inert atmosphere.…”

Section: Resultsmentioning

confidence: 99%

“…The rate of weight loss beyond 500 °C became slight until 1000 °C was reached. In this range of temperatures, weight loss could be attributed to the process of carbonization whereby carbon was converted into sp 2 from sp 3 forms [ 25 , 29 , 30 ].…”

Section: Resultsmentioning

confidence: 99%

“…Therefore, the fabrication of a hydrothermally stable and molecular sieving carbon-SiO 2 -ZrO 2 membrane required a better carbon precursor. In a more recent work, we studied the novel use of a traditional thermosetting group of organic compounds known as benzoxazines as the chelating ligand for the modification and carbonization of the SiO 2 -ZrO 2 network [ 25 ]. A carboxylic benzoxazine (3-(3-oxo-1,4-benzoxazin-4-yl) propanoic acid) possessing a hydroxylated nucleophilic carboxyl group was specifically chosen as the chelating ligand.…”

Section: Introductionmentioning

confidence: 99%

“…This enabled the formation of a composite SiO 2 -ZrO 2 -polybenzoxazine resin material that was used to fabricate thin carbon-SiO 2 -ZrO 2 membranes with molecular sieving performances that could be tuned via pyrolysis temperature. H 2 /SF 6 and H 2 /CH 4 selectivity ranged from 10 2 to 10 4 and from 10 to 10 2 , respectively, depending on pyrolysis temperatures that ranged between 300 and 850 °C [ 25 ]. The wide range of the pyrolysis temperature for this SiO 2 -ZrO 2 -polybenzoxazine (SZ-PB) resin presented an opportunity for the fabrication of carbon–ceramic composite membranes at higher than the application temperatures that are usually required for a stable performance.…”

Section: Introductionmentioning

confidence: 99%

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Hydrothermal Stability of Hydrogen-Selective Carbon–Ceramic Membranes Derived from Polybenzoxazine-Modified Silica–Zirconia

et al. 2022

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This work investigated the long-term hydrothermal performance of composite carbon-SiO2-ZrO2 membranes. A carbon-SiO2-ZrO2 composite was formed from the inert pyrolysis of SiO2-ZrO2-polybenzoxazine resin. The carbon-SiO2-ZrO2 composites prepared at 550 and 750 °C had different surface and microstructural properties. A carbon-SiO2-ZrO2 membrane fabricated at 750 °C exhibited H2 selectivity over CO2, N2, and CH4 of 27, 139, and 1026, respectively, that were higher than those of a membrane fabricated at 550 °C (5, 12, and 11, respectively). In addition to maintaining high H2 permeance and selectivity, the carbon-SiO2-ZrO2 membrane fabricated at 750 °C also showed better stability under hydrothermal conditions at steam partial pressures of 90 (30 mol%) and 150 kPa (50 mol%) compared with the membrane fabricated at 500 °C. This was attributed to the complete pyrolytic and ceramic transformation of the microstructure after pyrolysis at 750 °C. This work thus demonstrates the promise of carbon-SiO2-ZrO2 membranes for H2 separation under severe hydrothermal conditions.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Hydrothermal Stability of Hydrogen-Selective Carbon–Ceramic Membranes Derived from Polybenzoxazine-Modified Silica–Zirconia

et al. 2022

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Rational design of defect-free carbon-silica-zirconia ceramic membrane derived from crosslinked organic structure for highly efficient gas separation

Niu,

Moriyama,

Nagasawa

et al. 2024

Journal of Membrane Science

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A Brief Overview of the Microstructural Engineering of Inorganic–Organic Composite Membranes Derived from Organic Chelating Ligands

Lawal

Kanezashi

2023

Membranes

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This review presents a concise conceptual overview of membranes derived from organic chelating ligands as studied in several works. The authors’ approach is from the viewpoint of the classification of membranes by matrix composition. The first part presents composite matrix membranes as a key class of membranes and makes a case for the importance of organic chelating ligands in the formation of inorganic–organic composites. Organic chelating ligands, categorized into network-modifying and network-forming types, are explored in detail in the second part. Four key structural elements, of which organic chelating ligands (as organic modifiers) are one and which also include siloxane networks, transition-metal oxide networks and the polymerization/crosslinking of organic modifiers, form the building blocks of organic chelating ligand-derived inorganic–organic composites. Three and four parts explore microstructural engineering in membranes derived from network-modifying and network-forming ligands, respectively. The final part reviews robust carbon–ceramic composite membranes as important derivatives of inorganic–organic hybrid polymers for selective gas separation under hydrothermal conditions when the proper organic chelating ligand and crosslinking conditions are chosen. This review can serve as inspiration for taking advantage of the wide range of possibilities presented by organic chelating ligands.

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Design of carbon–ceramic composite membranes with tunable molecular cut-offs from a carboxylic benzoxazine ligand chelated to silica–zirconia

Abstract: Carbon molecular sieve and composite carbon molecular sieving membranes are fabricated via the traditional methods of pyrolyzing polymers or by using preceramic composite polymers bearing macromolecular structures. Scant attention is...

Cited by 3 publications

References 47 publications

Hydrothermal Stability of Hydrogen-Selective Carbon–Ceramic Membranes Derived from Polybenzoxazine-Modified Silica–Zirconia

Hydrothermal Stability of Hydrogen-Selective Carbon–Ceramic Membranes Derived from Polybenzoxazine-Modified Silica–Zirconia

Rational design of defect-free carbon-silica-zirconia ceramic membrane derived from crosslinked organic structure for highly efficient gas separation

A Brief Overview of the Microstructural Engineering of Inorganic–Organic Composite Membranes Derived from Organic Chelating Ligands

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