摘要
Formic acid(FA),which is obtainable through CO_(2)hydrogenation with green hydrogen or biomass conversion,has been used as a prospective liquid organic hydrogen carrier(LOHC)because of the abundant advantages of renewability,wide availability,stability,and high volumetric capacity(53 g H_(2)/L).The development of highly efficient catalytic systems to achieve enhanced catalytic activity is attractive but still challenging.Herein,ultrafine and highly dispersed PdAu nanoclusters(NCs)anchored on amino-modified reduced graphene oxide(ArGO)were successfully synthesized via a facile impregnation-reduction method and applied as a catalyst toward formic acid dehydrogenation(FAD).Benefiting from the promoting effect of amino groups,the strain and ligand effect in the alloy,and the Mott–Schottky effect between PdAu NCs and ArGO,the resultant PdAu/ArGO affords an ultrahigh activity under visible light irradiation with an exceptional turnover frequency value of 10,699.5 h^(-1)at 298 K without any additives,more than 2.6times improvement than that under dark,which is the highest among all reported catalysts under the same conditions.This study provides a green and convenient strategy for developing more efficient and sustainable FAD catalysts and promotes the effective utilization of FA as a prospective renewable LOHC.
基金
financially supported by the National Natural Science Foundation of China(Nos.22162014 and 22162013)
Department of Science and Technology of Jiangxi Province(Nos.20212ACB204009,20212BCJL23059 and 20232ACB214002)。
