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A novel organic–inorganic hybrid,Na[PMo8ⅥMo4ⅤO40Zn4][H2bpz]2(NJNU-L1,H2bpz= 3,3′,5,5′-tetramethyl-4,4′-bipyrazole),based on ε-Zn Keggin units {ε-PMo8ⅥMo4ⅤO40Zn4},have been successfully synthesized under hydrothermal conditions by controlling the pH values,which presents interesting structural characteristics,high chemical stability,and proton-conducting properties.