首页|Phosphotungstic acid immobilized on amino-functionalized TS-1 zeolite as a solid acid catalyst for the synthesis of tributyl citrate

Phosphotungstic acid immobilized on amino-functionalized TS-1 zeolite as a solid acid catalyst for the synthesis of tributyl citrate

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The amino-functionalization of TS-1 zeolite followed by immobilization of phosphotungstic acid (HPW) was presented to prepare a strong solid acid catalyst for the synthesis of bio-based tributyl citrate from the esterification of citric acid and n-butanol.γ-Aminopropyltriethoxysilane (APTES) was first grafted on the TS-1 zeolite via the condensation reactions with surface hydroxyl groups, and subsequently the HPW was immobilized via the reaction between the amino groups and the protons from HPW-forming strong ionic bonding. The Keggin structure of HPW and MFI topology of TS-1 zeolite were well maintained after the modifications. The amino-functionalization generated abundant uniformly distributed active sites on TS-1 for HPW immobilization, which promoted the dispersity, abundance, as well as the stability of the acid sites. The tetrahedrally coordinated framework titanium and non-framework titania behaved as weak Lewis acid sites, and the protons from the immobilized HPW acted as the moderate or strong Brønsted acid sites. An optimized TBC yield of 96.2％ (mol) with a conversion of -COOH of 98.1％ (mol) was achieved at 150 °C for 6 h over the HPW immobilized on amino-functionalized TS-1. The catalyst exhibited good stability after four consecutive reaction runs, where the activity leveled off at still a relatively high level after somewhat deactivation possibly caused by the leaching of a small portion of weakly anchored APTES or HPW.

Amino-functionalizationPhosphotungstic acidTS-1 zeoliteEsterificationTributyl citrate

Pei Li、Bianfang Shi、Junyao Shen、Ran Cui、Wenze Guo、Ling Zhao、Zhenhao Xi

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State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China

Key Laboratory of Smart Manufacturing in Energy Chemical Process, Ministry of Education, East China University of Science and Technology, Shanghai 200237, China

National Natural Science Foundation of ChinaProgram of Shanghai Academic/Technology Research LeaderKey Research and Development Program of Xinjiang Uygur Autonomous Region

2197808921XD14330002022B01032-1

2024

10.1016/j.cjche.2024.03.010

中国化学工程学报(英文版)
中国化工学会

中国化学工程学报(英文版)

CSTPCDEI
影响因子：0.818
ISSN：1004-9541
年,卷(期)：2024.70(6)
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