Interface engineering of 2D NiFe LDH/NiFeS heterostructure for highly efficient 5-hydroxymethylfurfural electrooxidation  

作　　者：Lili Wang Ya Yan Rulin Li Xujie Han Jiahui Li Ting Ran Jialu Li Baichuan Xiong Xiaorong Song Zhaohui Yin Hong Wang Qingjun Zhu Bowen Cheng Zhen Yin 

机构地区：[1]State Key Laboratory of Separation Membranes and Membrane Processes,School of Chemistry,Tiangong University,Tianjin 300387,China [2]School of Chemical Engineering and Technology,Tiangong University,Tianjin 300387,China [3]College of Chemical Engineering and Materials Science,Tianjin University of Science and Technology,Tianjin 300457,China [4]State Key Laboratory of Biobased Fiber Manufacturing Technology,Tianjin University of Science and Technology,Tianjin 300457,China [5]School of Materials Science and Engineering,Tiangong University,Tianjin 300387,China [6]Deutsches Elektronen-Synchrotron DESY,Platanenallee 6,Zeuthen 15738,Germany [7]Department of Chemistry and The Center for the Science of Materials Berlin,Humboldt-Universitäzu Berlin,Berlin 12489,Germany

出　　处：《Chinese Chemical Letters》2024年第9期514-520,共7页中国化学快报（英文版）

基　　金：supported by the National Natural Science Foundation of China(Nos.51908408,21872104);Natural Science Foundation of Tianjin for Distinguished Young Scholar,China(No.20JCJQJC00150)。

摘　　要：The electrochemical oxidation of 5-hydroxymethylfurfural(HMF)to valuable chemicals is an efficient way to upgrade biomass molecules and replace traditional catalytic synthesis.It is crucial to develop efficient and low-cost earth-abundant electrocatalysts to enhance catalytic performance of HMF oxidation.Herein,a new type of two-dimensional(2D)hybrid arrays consisting of Ni Fe layered double hydroxides(LDH)nanosheets and bimetallic sulfide(Ni Fe S)is constructed via interface engineering for efficient electrocatalytic oxidation of HMF to 2,5-furandicarboxylic acid(FDCA).The preparation process of 2D Ni Fe LDH/NiFeS with ultrathin heterostructure involves in anchoring a Co-based metal-organic framework(Co MOF)as template onto the carbon cloth(CC)via in-situ growth,formation of NiFe LDH on the surface of Co MOF and subsequent partial sulfidation.The electrocatalyst of Ni Fe LDH/Ni Fe S exhibits outstanding performance towards HMF oxidation,about 98.5%yield for FDCA and 97.2%Faraday efficiency(FE)in the alkaline electrolyte with 10 mmol/L HMF,as well as excellent stability retaining 90.1%FE for FDCA after six cycles test.Moreover,even at an HMF concentration of 100 mmol/L,the yield and FE for FDCA remain high at 83.6%and 93.6%,respectively.These findings highlight that 2D heterostructure containing abundant interfaces between Ni Fe LDH nanosheets and Ni Fe S can enhance the intrinsic activity of LDH and thus promote the oxidation reaction kinetics.Additionally,the synergistic effect of the bimetallic Ni Fe compounds also improved the selectivity of HMF conversion to FDCA.Our present work demonstrates that constructing 2D ultrathin heterostructure of Ni Fe LDH/Ni Fe S is a facile strategy via interface engineering to enhance the intrinsic activity of LDH electrocatalysts,which would open new avenues toward low-cost and advanced 2D nanocatalysts for sustainable energy conversion and electrochemical valorization of biomass derivatives.

关 键 词：Electrocatalytic oxidation Interface engineering 2D ultrathin heterostructure Layered double hydroxides 5-HYDROXYMETHYLFURFURAL 

分 类 号：O643.36[理学—物理化学] TQ251.11[理学—化学] TK6[化学工程—有机化工]