Controllable creating mesoporous coordination unsaturated sites in UiO-66 single crystals for efficient conversion of hydrogen sulfide into polysulphur - Details

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Abstract：

We　report　herein　a　facile　pyrolysis　etching　strategy　for　the　fabrication　of　UiO-66-xs　single　crystals　with　tunable　coordination　unsaturated　zirconium　sites　(Zr-CUS)　as　well　as　interconnected　mesoporosity.　The　synthesis　is　realized　by　having　pristine　UiO-66-xs　subjected　to　thermal　treatment,　which　results　in　the　selective　decomposition　of　thermal-sensitive　organic　linkers　and　hence　the　creation　of　permanent　mesoporosity,　leaving　abundant　Zr-CUS　with　enhanced　degree　of　exposure.　The　prepared　hierarchically　porous　UiO-66-xs　(HP-UiO-66-xs)　were　innovatively　applied　for　mild　oxidation　of　H2S　into　polysulphur,　achieving　near　100　%　H2S　conversion　and　polysulphur　selectivity　in　a　wide　range　of　temperatures.　The　superior　activities　can　be　well　maintained　in　a　continuous　test　of　over　50　h.　The　Zr-CUS　of　HP-UiO-66-xs　effectively　activate　H2S　and　O2　via　the　“adsorption　dissociation　tandem　hydrogen　transfer”　mechanism,　and　the　abundant　mesochannels　ensure　efficient　transport　of　reactants　and　bulky　products　in　and　out　HP-UiO-66-xs,　leading　to　catalytic　activities　superior　to　those　of　traditional　H2S　selective　oxidation　catalysts.　©　2023　Elsevier　B.V.

Keyword：

Coordination unsaturated degree H2S selective oxidation Mass transportation Mesoporous metal organic frameworks Polysulphur catalytic synthesis

Community：

[ 1 ] [Zhang G.]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fujian, Fuzhou, 350002, China
[ 2 ] [Liu F.]State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Hubei, Wuhan, 430071, China
[ 3 ] [Liu F.]University of Chinese Academy of Sciences, Beijing, 100049, China
[ 4 ] [Qu Y.]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fujian, Fuzhou, 350002, China
[ 5 ] [Zheng Y.]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fujian, Fuzhou, 350002, China
[ 6 ] [Zheng Y.]Qingyuan Innovation Laboratory, Fujian, Quanzhou, 362801, China
[ 7 ] [Cao Y.]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fujian, Fuzhou, 350002, China
[ 8 ] [Cao Y.]Qingyuan Innovation Laboratory, Fujian, Quanzhou, 362801, China
[ 9 ] [Liu F.]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fujian, Fuzhou, 350002, China
[ 10 ] [Liu F.]Qingyuan Innovation Laboratory, Fujian, Quanzhou, 362801, China
[ 11 ] [Liang S.]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fujian, Fuzhou, 350002, China
[ 12 ] [Liang S.]Qingyuan Innovation Laboratory, Fujian, Quanzhou, 362801, China
[ 13 ] [Xiao Y.]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fujian, Fuzhou, 350002, China
[ 14 ] [Xiao Y.]Qingyuan Innovation Laboratory, Fujian, Quanzhou, 362801, China
[ 15 ] [Yi X.]State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Hubei, Wuhan, 430071, China
[ 16 ] [Zheng A.]State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Hubei, Wuhan, 430071, China
[ 17 ] [Zheng A.]University of Chinese Academy of Sciences, Beijing, 100049, China
[ 18 ] [Zheng A.]Interdisciplinary Institute of NMR and Molecular Sciences, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan, 430081, China
[ 19 ] [Au C.]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fujian, Fuzhou, 350002, China
[ 20 ] [Jiang L.]National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fujian, Fuzhou, 350002, China
[ 21 ] [Jiang L.]Qingyuan Innovation Laboratory, Fujian, Quanzhou, 362801, China

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Chemical Engineering Journal

ISSN： 1385-8947

Year： 2024

Volume： 479

1 3 . 4 0 0

JCR@2023

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SCOPUS Cited Count： 4

ESI Highly Cited Papers on the List： 0 Unfold All

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