Carbon Fiber Supported Binary Metal Sulfide Catalysts with Multi-Dimensional Structures for Electrocatalytic Nitrogen Reduction Reactions Over a Wide pH Range  

作　　者：Tianyi Zhang Wei Zong Yue Ouyang Yue Wu Yue-E Miao Tianxi Liu 

机构地区：[1]State Key Laboratory for Modification of Chemical Fibers and Polymer Materials,College of Materials Science and Engineering,Innovation Center for Textile Science and Technology,Donghua University,2999 North Renmin Road,Shanghai 201620,People’s Republic of China [2]Research Center for Analysis and Measurement,Donghua University,Shanghai 201620,People’s Republic of China [3]Key Laboratory of Synthetic and Biological Colloids,Ministry of Education,School of Chemical and Material Engineering,Jiangnan University,Wuxi 214122,People’s Republic of China

出　　处：《Advanced Fiber Materials》2021年第4期229-238,共10页先进纤维材料（英文）

基　　金：support from the Natural Science Foundation of Shanghai(20ZR1401400,18ZR1401600);Shanghai Scientific and Technological Innovation Project(18JC1410600).

摘　　要：Green and environmentally friendly electrocatalytic nitrogen(N_(2))fixation to synthesize ammonia(NH3)is recognized as an effective method to replace the traditional Haber-Bosch process.However,the difficulties in N_(2) adsorption and fracture of hard N≡N bond still remain major challenges in electrocatalytic N_(2) reduction reactions(NRR).From the perspectives of enhancing N_(2) adsorption and providing more catalytic sites,two-dimensional(2D)FeS_(2) nanosheets and three-dimensional(3D)metal organic framework-derived ZnS embedded within N-doped carbon polyhedras are grown on the carbon cloth(CC)template in this work.Thus,a composite NRR catalyst with multi-dimensional structures,which is signed as FeS_(2)/ZnS-NC@CC,is obtained for using over a wide pH range.The uniform distribution of hollow ZnS-NC frameworks and FeS_(2) nanosheets on the surface of CC largely increase the N_(2) enrichment efficiency and offer more active sites,while the CC skeleton acts as an independent conductive substrate and S-doping helps promote the fracture of N≡N bond during the NRR reaction.As a result,the FeS_(2)/ZnS-NC@CC electrode achieves a high Faraday efficiency of 46.84%and NH3 yield of 58.52μg h^(−1) mg^(−1) at-0.5 V vs.Ag/AgCl in 0.1 M KOH.Furthermore,the FeS_(2)/ZnS-NC@CC electrode displays excellent NRR catalytic activity in acidic and neutral electrolytes as well,which outperforms most previously reported electrocatalysts including noble metals.Therefore,this work provides a new way for the design of multi-dimensional electrocatalysts with excellent electrocatalytic efficiency and stability for NRR applications.

关 键 词：Multi-dimensional structure Heteroatom doping Carbon fiber cloth Electrocatalytic nitrogen reduction 

分 类 号：O64[理学—物理化学]