Solution-mediated transformation of natural zeolite to ANA and CAN topological structures with altered active sites for ethanol conversion

Mutjalin Limlamthong; Minseong Lee; Bunjerd Jongsomjit; Isao Ogino; Shusheng Pang; Jungkyu Choi; Alex C.K. Yip

doi:10.1016/j.apt.2021.09.018

Solution-mediated transformation of natural zeolite to ANA and CAN topological structures with altered active sites for ethanol conversion

Mutjalin Limlamthong, Minseong Lee, Bunjerd Jongsomjit, Isao Ogino, Shusheng Pang, Jungkyu Choi, Alex C.K. Yip

Department of Chemical and Biological Engineering

Research output: Contribution to journal › Article › peer-review

5 Citations (Scopus)

Abstract

In this study, one-pot syntheses of cancrinite (CAN) and analcime (ANA) frameworks from mordenite (MOR) natural zeolite were performed for the first time. The effects of the synthesis gel composition and alkalinity on the phase formation and crystallinity of the product were investigated. All studied zeolites were evaluated for their catalytic activities in ethanol conversion reactions from 473 K to 673 K and at 1 atm. The results suggested that the formation pathways of CAN and ANA are highly dependent on the alkalinity of the synthesis solution and the type of starting material regardless of synthesis template. The use of natural MOR zeolite (MOR_NZ) in the synthesis can contribute to highly crystalline ANA structures comparable to the ANA products obtained from fumed silica and sodium aluminate (NaAlO₂). The quantity and locations of the acidic-cationic dual active sites of the proton-form product zeolites are suitable for synthesizing acetaldehyde from ethanol with over 90% product selectivity. However, further development of synthesis procedures to enhance the surface area is needed to improve the ethanol conversion of the resulting zeolites. This work provides a new perspective on highly crystalline and pure-phase zeolitic structural formations from natural zeolite and their potential application in ethanol conversion.

Original language	English
Pages (from-to)	4155-4166
Number of pages	12
Journal	Advanced Powder Technology
Volume	32
Issue number	11
DOIs	https://doi.org/10.1016/j.apt.2021.09.018
Publication status	Published - 2021 Nov

Bibliographical note

Funding Information:
The authors are grateful to the Center of Excellence on Catalysis and Catalytic Reaction Engineering at Chulalongkorn University for granting us access to their research facilities when our lab in New Zealand was closed during the COVID-19 lockdown. We also thank Lynne Clucas and Uthaiwan Limtrakul for collecting the ICP-OES and TGA data, respectively. The authors would like to acknowledge Blue Pacific Minerals Ltd. (New Zealand) for supplying the natural zeolite for our study. This project was supported by the Ministry of Business, Innovation & Employment in New Zealand under the MBIE Endeavour “Smart Ideas” grant (grant number UOCX1905).

Funding Information:
The authors are grateful to the Center of Excellence on Catalysis and Catalytic Reaction Engineering at Chulalongkorn University for granting us access to their research facilities when our lab in New Zealand was closed during the COVID-19 lockdown. We also thank Lynne Clucas and Uthaiwan Limtrakul for collecting the ICP-OES and TGA data, respectively. The authors would like to acknowledge Blue Pacific Minerals Ltd. (New Zealand) for supplying the natural zeolite for our study. This project was supported by the Ministry of Business, Innovation & Employment in New Zealand under the MBIE Endeavour ?Smart Ideas? grant (grant number UOCX1905).

Publisher Copyright:
© 2021 The Society of Powder Technology Japan

Keywords

Acetaldehyde production
Analcime zeolite
Cancrinite zeolite
Ethanol conversion
Natural mordenite zeolite

ASJC Scopus subject areas

General Chemical Engineering
Mechanics of Materials

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10.1016/j.apt.2021.09.018

Cite this

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title = "Solution-mediated transformation of natural zeolite to ANA and CAN topological structures with altered active sites for ethanol conversion",

abstract = "In this study, one-pot syntheses of cancrinite (CAN) and analcime (ANA) frameworks from mordenite (MOR) natural zeolite were performed for the first time. The effects of the synthesis gel composition and alkalinity on the phase formation and crystallinity of the product were investigated. All studied zeolites were evaluated for their catalytic activities in ethanol conversion reactions from 473 K to 673 K and at 1 atm. The results suggested that the formation pathways of CAN and ANA are highly dependent on the alkalinity of the synthesis solution and the type of starting material regardless of synthesis template. The use of natural MOR zeolite (MORNZ) in the synthesis can contribute to highly crystalline ANA structures comparable to the ANA products obtained from fumed silica and sodium aluminate (NaAlO2). The quantity and locations of the acidic-cationic dual active sites of the proton-form product zeolites are suitable for synthesizing acetaldehyde from ethanol with over 90% product selectivity. However, further development of synthesis procedures to enhance the surface area is needed to improve the ethanol conversion of the resulting zeolites. This work provides a new perspective on highly crystalline and pure-phase zeolitic structural formations from natural zeolite and their potential application in ethanol conversion.",

keywords = "Acetaldehyde production, Analcime zeolite, Cancrinite zeolite, Ethanol conversion, Natural mordenite zeolite",

author = "Mutjalin Limlamthong and Minseong Lee and Bunjerd Jongsomjit and Isao Ogino and Shusheng Pang and Jungkyu Choi and Yip, {Alex C.K.}",

note = "Funding Information: The authors are grateful to the Center of Excellence on Catalysis and Catalytic Reaction Engineering at Chulalongkorn University for granting us access to their research facilities when our lab in New Zealand was closed during the COVID-19 lockdown. We also thank Lynne Clucas and Uthaiwan Limtrakul for collecting the ICP-OES and TGA data, respectively. The authors would like to acknowledge Blue Pacific Minerals Ltd. (New Zealand) for supplying the natural zeolite for our study. This project was supported by the Ministry of Business, Innovation & Employment in New Zealand under the MBIE Endeavour “Smart Ideas” grant (grant number UOCX1905). Funding Information: The authors are grateful to the Center of Excellence on Catalysis and Catalytic Reaction Engineering at Chulalongkorn University for granting us access to their research facilities when our lab in New Zealand was closed during the COVID-19 lockdown. We also thank Lynne Clucas and Uthaiwan Limtrakul for collecting the ICP-OES and TGA data, respectively. The authors would like to acknowledge Blue Pacific Minerals Ltd. (New Zealand) for supplying the natural zeolite for our study. This project was supported by the Ministry of Business, Innovation & Employment in New Zealand under the MBIE Endeavour ?Smart Ideas? grant (grant number UOCX1905). Publisher Copyright: {\textcopyright} 2021 The Society of Powder Technology Japan",

year = "2021",

month = nov,

doi = "10.1016/j.apt.2021.09.018",

language = "English",

volume = "32",

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journal = "Advanced Powder Technology",

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T1 - Solution-mediated transformation of natural zeolite to ANA and CAN topological structures with altered active sites for ethanol conversion

AU - Limlamthong, Mutjalin

AU - Lee, Minseong

AU - Jongsomjit, Bunjerd

AU - Ogino, Isao

AU - Pang, Shusheng

AU - Choi, Jungkyu

AU - Yip, Alex C.K.

N1 - Funding Information: The authors are grateful to the Center of Excellence on Catalysis and Catalytic Reaction Engineering at Chulalongkorn University for granting us access to their research facilities when our lab in New Zealand was closed during the COVID-19 lockdown. We also thank Lynne Clucas and Uthaiwan Limtrakul for collecting the ICP-OES and TGA data, respectively. The authors would like to acknowledge Blue Pacific Minerals Ltd. (New Zealand) for supplying the natural zeolite for our study. This project was supported by the Ministry of Business, Innovation & Employment in New Zealand under the MBIE Endeavour “Smart Ideas” grant (grant number UOCX1905). Funding Information: The authors are grateful to the Center of Excellence on Catalysis and Catalytic Reaction Engineering at Chulalongkorn University for granting us access to their research facilities when our lab in New Zealand was closed during the COVID-19 lockdown. We also thank Lynne Clucas and Uthaiwan Limtrakul for collecting the ICP-OES and TGA data, respectively. The authors would like to acknowledge Blue Pacific Minerals Ltd. (New Zealand) for supplying the natural zeolite for our study. This project was supported by the Ministry of Business, Innovation & Employment in New Zealand under the MBIE Endeavour ?Smart Ideas? grant (grant number UOCX1905). Publisher Copyright: © 2021 The Society of Powder Technology Japan

PY - 2021/11

Y1 - 2021/11

N2 - In this study, one-pot syntheses of cancrinite (CAN) and analcime (ANA) frameworks from mordenite (MOR) natural zeolite were performed for the first time. The effects of the synthesis gel composition and alkalinity on the phase formation and crystallinity of the product were investigated. All studied zeolites were evaluated for their catalytic activities in ethanol conversion reactions from 473 K to 673 K and at 1 atm. The results suggested that the formation pathways of CAN and ANA are highly dependent on the alkalinity of the synthesis solution and the type of starting material regardless of synthesis template. The use of natural MOR zeolite (MORNZ) in the synthesis can contribute to highly crystalline ANA structures comparable to the ANA products obtained from fumed silica and sodium aluminate (NaAlO2). The quantity and locations of the acidic-cationic dual active sites of the proton-form product zeolites are suitable for synthesizing acetaldehyde from ethanol with over 90% product selectivity. However, further development of synthesis procedures to enhance the surface area is needed to improve the ethanol conversion of the resulting zeolites. This work provides a new perspective on highly crystalline and pure-phase zeolitic structural formations from natural zeolite and their potential application in ethanol conversion.

AB - In this study, one-pot syntheses of cancrinite (CAN) and analcime (ANA) frameworks from mordenite (MOR) natural zeolite were performed for the first time. The effects of the synthesis gel composition and alkalinity on the phase formation and crystallinity of the product were investigated. All studied zeolites were evaluated for their catalytic activities in ethanol conversion reactions from 473 K to 673 K and at 1 atm. The results suggested that the formation pathways of CAN and ANA are highly dependent on the alkalinity of the synthesis solution and the type of starting material regardless of synthesis template. The use of natural MOR zeolite (MORNZ) in the synthesis can contribute to highly crystalline ANA structures comparable to the ANA products obtained from fumed silica and sodium aluminate (NaAlO2). The quantity and locations of the acidic-cationic dual active sites of the proton-form product zeolites are suitable for synthesizing acetaldehyde from ethanol with over 90% product selectivity. However, further development of synthesis procedures to enhance the surface area is needed to improve the ethanol conversion of the resulting zeolites. This work provides a new perspective on highly crystalline and pure-phase zeolitic structural formations from natural zeolite and their potential application in ethanol conversion.

KW - Acetaldehyde production

KW - Analcime zeolite

KW - Cancrinite zeolite

KW - Ethanol conversion

KW - Natural mordenite zeolite

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DO - 10.1016/j.apt.2021.09.018

M3 - Article

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SN - 0921-8831

VL - 32

SP - 4155

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JO - Advanced Powder Technology

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Solution-mediated transformation of natural zeolite to ANA and CAN topological structures with altered active sites for ethanol conversion

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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