Atom-Selective Analyses Reveal the Structure-Directing Effect of Cs Cation on the Synthesis of Zeolites

被引:4
|
作者
Yamada, Hiroki [1 ,2 ]
Horikawa, Hirofumi [1 ]
Anand, Chokkalingam [1 ]
Ohara, Koji [2 ,3 ]
Ina, Toshiaki [2 ]
Machida, Akihiko [4 ]
Tominaka, Satoshi [5 ]
Okubo, Tatsuya [1 ]
Liu, Zhendong [1 ,6 ,7 ]
Iyoki, Kenta [1 ]
Wakihara, Toru [1 ,6 ]
机构
[1] Univ Tokyo, Dept Chem Syst Engn, Tokyo 1138656, Japan
[2] Japan Synchrotron Radiat Res Inst JASRI, Sayo, Hyogo 6795198, Japan
[3] Shimane Univ, Fac Mat Energy, 1060 Nishi Kawatsu Cho, Matsue, Shimane 6908504, Japan
[4] Natl Inst Quantum Sci & Technol, Synchrotron Radiat Res Ctr, Sayo, Hyogo 6795148, Japan
[5] Natl Inst Mat Sci NIMS, Int Ctr Mat Nanoarchitecton WPI MANA, Ibaraki 3050044, Japan
[6] Univ Tokyo, Inst Engn Innovat, Sch Engn, Tokyo 1138656, Japan
[7] Tsinghua Univ, Dept Chem Engn, State Key Lab Chem Engn, Beijing 100084, Peoples R China
关键词
PAIR DISTRIBUTION FUNCTION; ALUMINOSILICATE ZEOLITES; HYDROTHERMAL SYNTHESIS; CRYSTALLIZATION; PRECURSORS; MECHANISM; EVOLUTION; ZEOTYPES; ORDER; FAU;
D O I
10.1021/acs.jpclett.3c00432
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
To understand the crystallization mechanism of zeolites, it is important to clarify the detailed role of the structure-directing agent, which is essential for the crystallization of zeolite, interacting with an amorphous aluminosilicate matrix. In this study, to reveal the structure directing effect, the evolution of the aluminosilicate precursor which causes the nucleation of zeolite is analyzed by the comprehensive approach including atom-selective methods. The results of total and atom-selective pair distribution function analyses and X-ray absorption spectroscopy indicate that a crystalline-like coordination environment gradually forms around Cs cations. This corresponds to the fact that Cs is located at the center of the d8r units in the RHO structure whose unit is unique in this zeolite, and a similar tendency is also confirmed in the ANA system. The results collectively support the conventional hypothesis that the formation of the crystalline like structure before the apparent nucleation of the zeolite.
引用
收藏
页码:3574 / 3580
页数:7
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