▎ 摘　　要

"Click reactions" are widely used for the synthesis and modification of new materials due to their fascinating advantages (e.g., highly efficient and selective, mild reaction conditions, and lack of side reactions). Redox-active metal-substituted polyoxotungstates (MSPs) were covalently immobilized on a graphene surface by using a "click" reaction between the azido group of K1.5Cs5.5[gamma-SiW10O39Cu2(N-3)(2)] (SiW10Cu2(N-3)(2)) and the alkynyl groups on functionalized graphene. This novel strategy allowed for controllable formation of interfacial catalysts (SiW10Cu2/GO) with a single MSP molecule being loaded on the surface of graphene. This interfacing between a single polyoxometalate (POM) molecule and graphene results in several advantages combined with redox properties and higher thermal stability due to the POMs, electronic band structure of graphene, special hydrophobic environment, and single molecular dispersing sites. This SiW10Cu2/GO catalyst exhibited excellent stability and highly efficient reactivity or selectivity for dismutation of H2O2 and oxidation of 2-chloroethyl ethyl sulfide (CEES). SiW10Cu2/GO was active for evolving oxygen from H2O2 dismutation at a rate of 1.35 x 10(-1) mu mol s(-1), which was much higher than that by using its parent SiW10Cu2(N-3)(2) (1.89 X 10(-2) mu mol s(-1)) and similar to that of the reported [Ru-4(mu-OH)(2)(mu-O)(4)(H2O)(4)][gamma- SiW10O36](2)(10-) (1.24 X 10(-1) mu mol s(-1)) catalyst. Therefore, this activity permitted it to mimic catalase (H2O2 -> H2O + O-2) as an inorganic synzyme at 27 degrees C. The simultaneous generation of O-2 and highly selective detoxification of CEES to nontoxic sulfoxide CEESO demonstrated the potential for personnel protection against chemical warfare agents. Moreover, SiW10Cu2/GO exhibited higher activity for the oxidation of CEES to sulfide CEESO with higher selectivity in the presence of O-2. Furthermore, recycling and leaching experiments indicated that no significant leaching of POMs was observed from graphene. In addition, the produced CEESO did not aggregate on the catalyst hybrids.