Advancing sustainable ammonia synthesis with the magnetic La-doped Ti_(3)C_(2)O_(2) MXenes  

作　　者：Koua Alain Jesus Koua Jiahe Peng Neng Li 

机构地区：[1]State Key Laboratory of Silicate Materials for Architectures,School of Materials Science and Engineering,Wuhan University of Technology,Hubei,430070,China [2]Shenzhen Research Institute of Wuhan University of Technology,Shenzhen,518000,Guangdong,China

出　　处：《Progress in Natural Science:Materials International》2024年第6期1184-1193,共10页自然科学进展·国际材料(英文版)

基　　金：supported by the Guangdong Basic and Applied Basic Research Foundation(No.2022A1515011303);the Basic Research Program of Shenzhen(No.JCYJ20190809120015163);the Central Government Guides Local Science and Technology Development Funds to Freely Explore Basic Research Projects(2021Szvup106);Natural Science Fund for Distinguished Young Scholars of Hubei Province(No.2020CFA087);the State Key Laboratory of Refractories and Metallurgy,Wuhan University of Science and Technology(No.G201605);Fundamental Research Funds for the Central Universities(No.WUT35401053-2022)

摘　　要：Developing an easy ammonia(NH_(3))production method to circumvent the demanding conditions of the HaberBosch process is a significant stride towards self-sufficiency in NH_(3)production and environment preservation.In pursuit of this goal,we carried out a theoretical approach to investigate the electrocatalytic N_(2)reduction reaction(eN_(2)RR)using the magnetic La-doped Ti_(3)C_(2)O_(2)(La-Ti_(3)C_(2)O_(2))MXene electrocatalyst.The first principle calculations of the DFT,conducted using the Vienna Ab-Initio Storage Package(VASP)were instrumental in assessing the performance of ferromagnetic(FM)and antiferromagnetic(AFM)configurations of La-Ti_(3)C_(2)O_(2).While Ti_(3)C_(2)O_(2)reveals limitations in eN_(2)RR efficiency attributed to its suboptimal surface reactivity,both FM and AFM structures of La-Ti_(3)C_(2)O_(2)exhibit enhanced electronic properties,enabling improved electron transfer features.La-Ti_(3)C_(2)O_(2)demonstrates heightened N_(2)adsorption capabilities and reduced energy barriers for transitional species towards NH_(3)production,presenting superior performance to Ti_(3)C_(2)O_(2).The density of states(DOS)analysis of La-Ti_(3)C_(2)O_(2)provided outcomes supporting the AFM as the credible magnetic configuration,a statement reinforced by the superior N_(2)conversion performance in the AFM structure compared to FM.During this process of eN_(2)RR,a study focused on the favorable pathway with less energy consumption is directed.

关 键 词：Ammonia production Electrocatalytic N2RR Magnetic MXene DFT calculations 

分 类 号：TQ113.2[化学工程—无机化工] O643.36[理学—物理化学]