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

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SusMat 2024年第4期4卷 90-103页

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 Hydrogen energy Technology Laboratory Korea Institute of Energy Technology(KENTECH)NajuRepublic of Korea School of Chemical Engineering Sungkyunkwan University(SKKU)SuwonRepublic of Korea Materials&Chemistry Group Institute of Inorganic ChemistryUniversity of CologneCologneGermany Department of Polymer Engineering Graduate SchoolAlan G.MacDiarmid Energy Research Institute&School of Polymer Science and EngineeringChonnam National UniversityGwangjuRepublic of Korea Research Institute NEEL SciencesJeollanamdoRepublic of Korea Department of Materials Science and Engineering Chonnam National UniversityGwangjuRepublic of Korea Department of Chemistry Xi’an Jiaotong-Liverpool UniversitySuzhouChina

Electrochemical nitrogen reduction reaction(NRR)is a sustainable alterna-tive to the Haber-Bosch process for ammonia(NH3)***,the significant uphill energy in the multistep NRR pathway is a bottleneck for favorable serial *** 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 *** 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 *** 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 *** 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 ***,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)

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