Downsizing AFX Zeolite Crystals to Nanoscale by a Postmilling

Apr 22, 2016 - Synopsis. We applied a postmilling recrystallization method for reducing the AFX aluminosilicate zeolite crystal sizes to the nanoscale...
1 downloads 15 Views 3MB Size
Subscriber access provided by University of Pennsylvania Libraries

Article

Downsizing AFX zeolite crystals to nanoscale by post-milling recrystallization method Hiroki Yamada, Takayuki Iida, Zhendong Liu, Yusuke Naraki, Koji Ohara, Shinji Kohara, Tatsuya Okubo, and Toru Wakihara Cryst. Growth Des., Just Accepted Manuscript • DOI: 10.1021/acs.cgd.6b00365 • Publication Date (Web): 22 Apr 2016 Downloaded from http://pubs.acs.org on April 26, 2016

Just Accepted “Just Accepted” manuscripts have been peer-reviewed and accepted for publication. They are posted online prior to technical editing, formatting for publication and author proofing. The American Chemical Society provides “Just Accepted” as a free service to the research community to expedite the dissemination of scientific material as soon as possible after acceptance. “Just Accepted” manuscripts appear in full in PDF format accompanied by an HTML abstract. “Just Accepted” manuscripts have been fully peer reviewed, but should not be considered the official version of record. They are accessible to all readers and citable by the Digital Object Identifier (DOI®). “Just Accepted” is an optional service offered to authors. Therefore, the “Just Accepted” Web site may not include all articles that will be published in the journal. After a manuscript is technically edited and formatted, it will be removed from the “Just Accepted” Web site and published as an ASAP article. Note that technical editing may introduce minor changes to the manuscript text and/or graphics which could affect content, and all legal disclaimers and ethical guidelines that apply to the journal pertain. ACS cannot be held responsible for errors or consequences arising from the use of information contained in these “Just Accepted” manuscripts.

Crystal Growth & Design is published by the American Chemical Society. 1155 Sixteenth Street N.W., Washington, DC 20036 Published by American Chemical Society. Copyright © American Chemical Society. However, no copyright claim is made to original U.S. Government works, or works produced by employees of any Commonwealth realm Crown government in the course of their duties.

Page 1 of 22

Crystal Growth & Design

1 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Downsizing AFX zeolite crystals to nanoscale by post-milling recrystallization method

Hiroki Yamada1, Takayuki Iida1, Zhendong Liu1, Yusuke Naraki2, Koji Ohara3, Shinji Kohara4, Tatsuya Okubo1 and Toru Wakihara1*

1) Department of Chemical System Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan 2) Inorganic Materials Research Laboratory, Tosoh Corporation, 4560 Kaiseicho, Shunan, Yamaguchi 746-8501, Japan 3) JASRI/SPring-8, Kouto 1-1-1, Sayo-cho, Sayo-gun Hyogo 679-5198, Japan 4) National Institute for Materials Science, Kouto 1-1-1, Sayo-cho, Sayo-gun, Hyogo 679-5148, Japan

*Corresponding author: Toru Wakihara Department of Chemical System Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan Tel: +81-3-5841-7368; Fax: +81-3-5800-3806; E-mail: [email protected]

ACS Paragon Plus Environment

Crystal Growth & Design

Page 2 of 22

2 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Abstract Downsizing zeolites to obtain nanosized crystals for circumventing problems regarding molecular diffusion is a critical method for enhancing their functionalities, and therefore, such approach has been a focus of great attention. Here we applied the post-milling recrystallization method for reducing the AFX aluminosilicate zeolite crystal sizes to the nanoscale. Highly crystalline AFX zeolite particles with crystal sizes smaller than 100 nm were obtained by the post-milling recrystallization method using the supernatant solution acquired during the preparation of the ingredient raw crystals used for the milling. The prepared AFX zeolite nanocrystals were found to possess better ion-exchange performance than micrometer-sized counterparts highlighting the improved accessibility of the cations inside the micropores.

ACS Paragon Plus Environment

Page 3 of 22

Crystal Growth & Design

3 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Introduction Zeolites are crystalline microporous aluminosilicate materials that have been widely used as catalysts, adsorbents, and ion-exchangers because of their favorable features such as ordered micropore structures, high hydrothermal stabilities, and large ion-exchange capacities1,2. Reduction of the zeolite crystal size down to the nanoscale (