V_(2)O_(3)/VN electrocatalysts with coherent heterogeneous interfaces for selecting low-energy nitrogen reduction pathways  

作　　者：Tae-Yong An Chengkai Xia Minyeong Je Hyunjung Lee Seulgi Ji Min-Cheol Kim Subramani Surendran Mi-Kyung Han Jaehyoung Lim Dong-Kyu Lee Joon Young Kim Tae-Hoon Kim Heechae Choi Jung Kyu Kim Uk Sim 

机构地区：[1]Hydrogen Energy Technology Laboratory,Korea Institute of Energy Technology(KENTECH),Naju,Republic of Korea [2]School of Chemical Engineering,Sungkyunkwan University(SKKU),Suwon,Republic of Korea [3]Materials&Chemistry Group,Institute of Inorganic Chemistry,University of Cologne,Cologne,Germany [4]Department of Polymer Engineering,Graduate School,Alan G.MacDiarmid Energy Research Institute&School of Polymer Science and Engineering,Chonnam National University,Gwangju,Republic of Korea [5]Research Institute,NEEL Sciences,Jeollanamdo,Republic of Korea [6]Department of Materials Science and Engineering,Chonnam National University,Gwangju,Republic of Korea [7]Department of Chemistry,Xi’an Jiaotong-Liverpool University,Suzhou,China

出　　处：《SusMat》2024年第4期90-103,共14页可持续发展材料（英文）

基　　金：National Research Foundation of Korea,Grant/Award Numbers:2022R1A2C1012419,2022R1A2C1011559,2022R1C1C1007004。

摘　　要：Electrochemical nitrogen reduction reaction(NRR)is a sustainable alterna-tive to the Haber-Bosch process for ammonia(NH3)production.However,the significant uphill energy in the multistep NRR pathway is a bottleneck for favorable serial reactions.To overcome this challenge,we designed a vanadium oxide/nitride(V_(2)O_(3)/VN)hybrid electrocatalyst in which V_(2)O_(3)and VN coex-ist coherently at the heterogeneous interface.Since single-phase V_(2)O_(3)and VN exhibit different surface catalytic kinetics for NRR,the V_(2)O_(3)/VN hybrid elec-trocatalyst can provide alternating reaction pathways,selecting a lower energy pathway for each material in the serial NRR pathway.As a result,the ammo-nia yield of the V_(2)O_(3)/VN hybrid electrocatalyst was 219.6µg h^(-1)cm^(-2),and the Faradaic efficiency was 18.9%,which is much higher than that of single-phase VN,V_(2)O_(3),and VNxOy solid solution catalysts without heterointerfaces.Density functional theory calculations confirmed that the composition of these hybrid electrocatalysts allows NRR to proceed from a multistep reduction reaction to a low-energy reaction pathway through the migration and adsorption of interme-diate species.Therefore,the design of metal oxide/nitride hybrids with coherent heterointerfaces provides a novel strategy for synthesizing highly efficient elec-trochemical catalysts that induce steps favorable for the efficient low-energy progression of NRR.

关 键 词：coherent heterogeneous interfaces green ammonia synthesis hybrid electrocatalyst low-energy progression nitrogen reduction reaction(NRR) vanadium oxide/nitride(V_(2)O_(3)/VN) 

分 类 号：O64[理学—物理化学]