Co_(3)O_(4) has been widely explored in electrocatalytic 5-hydroxymethyl-furfural(HMF) oxidation. However,the poor intrinsic ability has seriously limited its electrochemical ability. Heteroatom-doping is an efficient...Co_(3)O_(4) has been widely explored in electrocatalytic 5-hydroxymethyl-furfural(HMF) oxidation. However,the poor intrinsic ability has seriously limited its electrochemical ability. Heteroatom-doping is an efficient method to enhance the electrocatalytic ability of catalyst by regulating electronic structure. Herein,we have modulated the electronic structure of Co_(3)O_(4) by high valance Mo^(6+)-doping. With the introduction of Mo^(6+), the content of Co^(2+) was increased and metal-oxygen bond was strength. Electrochemical results suggested that the electrocatalytic ability of Co_(3)O_(4) towards HMF oxidation has been dramatically improved and reaction kinetics has been fasten. Theoretical calculations demonstrated that the surrounding cobalt sites after Mo^(6+)-doping with assembled electron has a strong adsorption ability towards HMF molecule leading to more favourable oxidation of HMF. Post characterizations demonstrated pristine Co_(3)O_(4) structure was kept after electrolysis cycles and CoOOH active species were formed. This work provides a valuable reference for developing efficient heteroatom-doped electrocatalysts for HMF oxidation.展开更多
基金supported by National Natural Science Foundation of China (Nos. 92061201, 21825106, 22102155 and 32072304)the China Postdoctoral Science Foundation (Nos. 2021M692909 and 2022T150587)+1 种基金the Program for Innovative Research Team (in Science and Technology) in Universities of Henan Province and Zhengzhou University (No. 19IRSTHN022)the Key Scientific and Technological Project of Henan Province (No. 2021102210027)。
文摘Co_(3)O_(4) has been widely explored in electrocatalytic 5-hydroxymethyl-furfural(HMF) oxidation. However,the poor intrinsic ability has seriously limited its electrochemical ability. Heteroatom-doping is an efficient method to enhance the electrocatalytic ability of catalyst by regulating electronic structure. Herein,we have modulated the electronic structure of Co_(3)O_(4) by high valance Mo^(6+)-doping. With the introduction of Mo^(6+), the content of Co^(2+) was increased and metal-oxygen bond was strength. Electrochemical results suggested that the electrocatalytic ability of Co_(3)O_(4) towards HMF oxidation has been dramatically improved and reaction kinetics has been fasten. Theoretical calculations demonstrated that the surrounding cobalt sites after Mo^(6+)-doping with assembled electron has a strong adsorption ability towards HMF molecule leading to more favourable oxidation of HMF. Post characterizations demonstrated pristine Co_(3)O_(4) structure was kept after electrolysis cycles and CoOOH active species were formed. This work provides a valuable reference for developing efficient heteroatom-doped electrocatalysts for HMF oxidation.
基金supported by the National Natural Science Foundation of China(92061201,21825106,22102155,and 32072304)China Postdoctoral Science Foundation(2021M692909 and 2022T150587)+1 种基金the Program for Innovative Research Team(in Science and Technology)in Universities of Henan Province and Zhengzhou University(19IRSTHN022)the Key Scientific and Technological Project of Henan Province(2021102210027)。
