Synergic catalysis of W and Ni originating from substitution of trivacant phosphotungstate for the selective oxidation of aniline to azoxybenzene

Sheng Cai ¹Xiao-Yuan Wu ²Weiming Wu ²Sa-Sa Wang ²Can-Zhong Lu³

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作者信息

1. CAS Key Laboratory of Design and Assembly of Functional Nanostructures,and Fujian Provincial Key Laboratory of Nanomaterials,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,China;College of Chemistry and Materials Science,Fujian Normal University,Fuzhou 350117,China
2. CAS Key Laboratory of Design and Assembly of Functional Nanostructures,and Fujian Provincial Key Laboratory of Nanomaterials,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,China
3. CAS Key Laboratory of Design and Assembly of Functional Nanostructures,and Fujian Provincial Key Laboratory of Nanomaterials,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,China;College of Chemistry and Materials Science,Fujian Normal University,Fuzhou 350117,China;Xiamen Institute of Rare Earth Materials,Chinese Academy of Sciences,Xiamen 361021,China;University of Chinese Academy of Sciences,Beijing 100049,China
折叠

Abstract

Partial substitution of polyoxometalate(POM)is an efficient route to modulate the catalytic property of maternal POM.In this work,a new Keggin type POM involving {Ni6} cluster,{[Ni(H2O)2(Dach)2][Ni(Dach)2]2}{[Ni6Cl(μ-OH)3(H2O)(Dach)3(WO4)(PW9O34)][Ni6(μ-OH)3(H2O)2(Dach)3(WO4)(PW9O34)]}Cl-27H2O,(1,Dach=1,2-diaminocyclohexane)was synthesized.Compounds 1 shows excellent catalytic performance in the selective oxidation of aniline to azoxybenzene(AOB)in water.The apparently different results from that with the matrix {PW9O34}({PW9})suggest the successful regulation of the catalytic property of {PW9} by the introduction of the {Ni6} cluster into the skeleton.The experimental results indicate that the highlighted performance of 1 is contributed by the synergy of W and Ni sites,which are respectively responsible for the oxidation and condensation steps in the production of AOB.The good selectivity to AOB is essentially attributed to the effective modulation of the reaction rates of oxidation and condensation steps by W and Ni sites,respectively.

Key words

Polyoxometalate/{Ni6} cluster/Modulated catalytic property/Aniline oxidation/Azoxybenzene

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基金项目

国家自然科学基金(21773247)

国家自然科学基金(22275185)

国家自然科学基金(21521061)

国家自然科学基金(21875252)

福建省自然科学基金(2006L2005)

出版年

2024

中国化学快报(英文版)

中国化学会

中国化学快报(英文版)

CSTPCDCSCD

影响因子：0.771

ISSN：1001-8417

参考文献量42

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