高等学校化学学报2024,Vol.45Issue(10) :12-20.DOI:10.7503/cjcu20240203

镍/氮共掺杂自支撑泡沫碳电极的构建及电催化CO2还原性能

Construction of Ni/N Co-doped Self-supported Carbon Foam Electrodes for Electrocatalytic CO2 Reduction

朱佳佳 芮家亮 石文文 甘铠宁 李宏强 何孝军
高等学校化学学报2024,Vol.45Issue(10) :12-20.DOI:10.7503/cjcu20240203

镍/氮共掺杂自支撑泡沫碳电极的构建及电催化CO2还原性能

Construction of Ni/N Co-doped Self-supported Carbon Foam Electrodes for Electrocatalytic CO2 Reduction

朱佳佳 1芮家亮 1石文文 1甘铠宁 1李宏强 1何孝军1
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作者信息

  • 1. 安徽工业大学化学与化工学院,煤清洁转化与高值化利用安徽省重点实验室,马鞍山 243002
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摘要

以沥青为碳源、聚氨酯泡沫为模板,通过浸渍、固化和碳化等步骤制备了一系列镍/氮共掺杂自支撑泡沫碳电极,采用扫描电子显微镜、透射电子显微镜、氮气吸附-脱附分析、拉曼光谱和X射线光电子能谱等手段对材料进行了表征.结果表明,制备的泡沫碳电极为三维大孔骨架结构,表面具有缺陷位和Ni-N配位结构,通过改变碳化温度可调控N含量,进而实现对Ni-Nx活性位含量的调控.将该泡沫碳电极作为电还原CO2的自支撑电极,可得到H2/CO摩尔比稳定可控的合成气.在-0.9~-1.3 V(vs.RHE)电位窗口内,H2/CO摩尔比可从1/2调整至2/1.反应10 h后,在900 ℃下得到的泡沫碳电极的电流密度为5.7 mA/cm2,H2/CO摩尔比约为1/1.

Abstract

A series of nickel/nitrogen co-doped self-supported carbon foam electrodes were prepared by impregna-tion,curing and carbonization using asphalt as the carbon source and polyurethane foam as the template,and then characterized by scanning electron microscopy,transmission electron microscopy,N2 adsorption-desorption analysis,Raman spectroscopy and X-ray photoelectron spectroscopy.The results show that the prepared carbon foam electrodes possess a three-dimensional macroporous skeleton structure.Moreover,their surface is abundant in defect sites and Ni-N coordination structures.The content of N species can be regulated by varying the carbonization temperature,thereby enabling the regulation of the content of Ni-Nx active sites.The carbon foam electrodes were directly used as a self-supported electrode for the electroreduction of CO2,and a syngas with a stable and controllable H2/CO molar ratio could be obtained.The H2/CO molar ratio can be tuned from 1/2 to 2/1 within the potential window of-0.9~-1.3 V(vs.RHE).In addition,the current density of the carbon foam electrode obtained at the carbonization temperature of 900 ℃ can be maintained at 5.7 mA/cm2 after a sustained reaction for 10 h,and the H 2/CO molar ratio can be maintained at about 1/1.

关键词

电催化CO,还原/自支撑电极/合成气/泡沫碳

Key words

Electrocatalytic CO2 reduction/Self-supported electrode/Syngas/Carbon foam

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基金项目

国家自然科学基金(22108003)

安徽省高校优秀青年科研项目(2023AH030026)

安徽工业大学大学生创新创业训练项目(S202210360206)

出版年

2024
高等学校化学学报
中华人民共和国教育部委托 吉林大学和南开大学

高等学校化学学报

CSTPCD北大核心
影响因子:1.067
ISSN:0251-0790
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