Guanine-derived F,N co-doped carbon-shell encapsulated iron carbide nanoparticles for enhanced CO_(2)electroreduction activity  

作　　者：Shuo Chen Lishun Pei Ying Peng Xuefei Zhang Zailai Xie 

机构地区：[1]Key Laboratory of Advanced Carbon-Based Functional Materials(Fujian Province University),Fuzhou University,Fuzhou 350016,China

出　　处：《Nano Research》2024年第6期4744-4752,共9页纳米研究（英文版）

基　　金：the financial support from the National Natural Science Foundation of China(Nos.22072018 and 22372039);the Natural Science Foundation of Fujian Province of China(No.2021J06010).

摘　　要：The development of highly selective,cost-effective,and energy-efficient electrocatalysts is critical for carbon dioxide reduction reaction(CO_(2)RR)to produce high-value products.Herein,we propose a facile strategy to obtain F,N co-doped carbon-coated iron carbide(Fe3C)nanoparticles by using biomolecule guanine and hexadecafluorophthalocyanine iron as raw materials.Remarkably,this method involves only one-step pyrolysis and does not require any guiding agent or sacrificial template.Benefiting from the advantageous surface microenvironment adjustments achieved through graphitic N(GN)and F co-doping,Fe3C@NF-G-1000 demonstrates exceptional efficacy in the electroreduction of CO_(2)to carbon monoxide(CO)with an impressive Faradic efficiency(FEco)up to 98%at the potential of−0.55 V(vs.reversible hydrogen electrode(RHE)).Furthermore,it delivers a remarkable current density of up to−43 mA·cm^(−2)and exhibits virtually no current attenuation over a span of 20 h within the flow cell.Insights from density functional theory(DFT)calculations reveal that the composite structure of GN and F co-doped graphitic layer and Fe3C exhibits different electron density distributions from that of iron carbide nanoparticles.This is attributed to the synergistic effect of the composite structure leading to the enrichment of electrons in the graphite layer on the surface,which contributes to the stability of the key reaction intermediate*COOH,thus,resulting in an enhanced catalytic activity and efficiency.Overall,this work introduces a new and promising approach to the design of green and low-cost carbon-coated metal materials for CO_(2)reduction reactions.

关 键 词：GUANINE F N co-doped carbon dioxide reduction reaction(CO_(2)RR) Fe-based catalyst 

分 类 号：TQ426[化学工程]