首页|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

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

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

Electrocatalytic CO2 reductionSelf-supported electrodeSyngasCarbon foam

朱佳佳、芮家亮、石文文、甘铠宁、李宏强、何孝军

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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

电催化CO,还原 自支撑电极 合成气 泡沫碳

国家自然科学基金安徽省高校优秀青年科研项目安徽工业大学大学生创新创业训练项目

221080032023AH030026S202210360206

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
年,卷(期):2024.45(10)