Charge-redistribution in bimetallic oxides buried in microporous curled carbon for efficient nitrate electroreduction to ammonia

作     者：Lituo Liu Hongliang Dong Sina Huang Nana Gao Leiqian Zhang Li-Ming Yang Jingwen Ba Johan Hofkens Markus Antonietti Tianxi Liu Feili Lai Zhihong Tian 刘利拓;董洪亮;黄思娜;高娜娜;张镭骞;杨利明;巴静雯;Johan Hofkens;Markus Antonietti;刘天西;赖飞立;田志红

作者机构：Engineering Research Center for NanomaterialsHenan UniversityKaifeng 475004China Center for High Pressure Science and Technology Advanced ResearchShanghai 201203China Key Laboratory of Theoretical Chemistry of EnvironmentMinistry of EducationSchool of ChemistrySouth China Normal UniversityGuangzhou 510006China Key Laboratory of Synthetic and Biological ColloidsMinistry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi 214122China School of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China Department of ChemistryKU LeuvenCelestijnenlaan 200FLeuven 3001Belgium Department of Colloid ChemistryMax Planck Institute of Colloids and InterfacesPotsdam 14476Germany State Key Laboratory of Metal Matrix CompositesSchool of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China 

出 版 物：《Science China Materials》 (中国科学(材料科学)(英文版))

年 卷 期：2025年第68卷第2期

页      面：472-482页

核心收录：

学科分类：081702[工学-化学工艺] 08[工学] 0817[工学-化学工程与技术] 0805[工学-材料科学与工程（可授工学、理学学位）] 080502[工学-材料学] 

基　　金：supported by the National Natural Science Foundation of China(52373205 and 52003251) Henan Center for Outstanding Overseas Scientists(GZS_(2)022014) 

主　　题：carbon-based nanocomposites bimetallic catalyst molten-salt strategy electrocatalytic nitrate reduction ammonia 

摘      要：Electrochemical reduction from nitrate into ammonia is a chance for nitrate removal from drinking water,while at higher concentrations,this 8-electron reduction process could even become relevant for energy storage,high conversions and low onset potentials ***,we report the synthesis and analysis of a NiFe_(2)O_(4)/C-MS hybrid system made by a molten-salt strategy where the Ni-Fe oxide spinel nanoparticles act as the active center for electrochemical nitrate(NO_(3)−)reduction reaction,while the microporous carbon serves as a conductive support to form a cohesive electrode *** NiFe_(2)O_(4)/C-MS catalyst achieves a maximum NH3 yield rate of 5.4 mg mgcat.^(−1)h^(−1)and Faradaic efficiency of 98%at−0.6 V versus reversible hydrogen *** NiFe_(2)O_(4)nanoparticles buried into microporous carbon,the onset potential decreases *** propose that this reduction originates from charge redistribution in NiFe_(2)O_(4)in the electronic heterojunction with carbon,while enhanced electrolyte diffusion in microporous carbon facilitates high conversion *** functional theory calculations clarify the low energy barrier on NiFe_(2)O_(4),highlighting the essential role of Ni in activating Fe *** COMSOL Multiphysics simulations demonstrate that the microporous curled carbon accelerates NO_(3)−transport and enhances adsorption on the reactive *** work offers insights for designing carbon-based nanocomposites for efficient nitrate reduction electrocatalysis.