Citation: Sheng Cai, Xiao-Yuan Wu, Weiming Wu, Sa-Sa Wang, Can-Zhong Lu. Synergic catalysis of W and Ni originating from substitution of trivacant phosphotungstate for the selective oxidation of aniline to azoxybenzene[J]. Chinese Chemical Letters, ;2024, 35(2): 108324. doi: 10.1016/j.cclet.2023.108324 shu

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

Sheng Cai ^{a, b} ,
Xiao-Yuan Wu ^a ,
Weiming Wu ^a ,
Sa-Sa Wang ^{a, *,} ,
Can-Zhong Lu ^{a, b, c, d, *,}

a.
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
b.
College of Chemistry and Materials Science, Fujian Normal University, Fuzhou 350117, China
c.
Xiamen Institute of Rare Earth Materials, Chinese Academy of Sciences, Xiamen 361021, China
d.
University of Chinese Academy of Sciences, Beijing 100049, China

wss@fjirsm.ac.cn

czlu@fjirsm.ac.cn

Received Date: 10 January 2023
Revised Date: 23 February 2023
Accepted Date: 8 March 2023
Available Online: 15 March 2023

Figures(5)

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.
- Polyoxometalate,
- {Ni₆} cluster,
- Modulated catalytic property,
- Aniline oxidation,
- Azoxybenzene
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