高效光催化二氧化碳还原钴单原子催化剂的多尺度结构工程
Multiscale structural engineering of cobalt single-atom catalyst for highly efficient photocatalytic CO2 reduction
王榆惠 1郑天宇 1金昱丞 1孙婷婷 1丁旭 1王萧 1徐清梅 1李彤轩 1张少龙 2姜建壮1
作者信息
- 1. Beijing Advanced Innovation Center for Materials Genome Engineering,Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials,Department of Chemistry and Chemical Engineering,School of Chemistry and Biological Engineering,University of Science and Technology Beijing,Beijing 100083,China
- 2. College of Chemistry and Environmental Engineering,Shenzhen University,Shenzhen 518060,China
- 折叠
摘要
人工光合作用将二氧化碳转化为增值化学品和燃料,在克服全球环境能源危机方面具有巨大潜力.然而,由于CO2的热力学稳定性和动力学滞后性,开发高效的CO2RR光催化剂是一个巨大的挑战.本文在微介孔氮掺杂碳(0.8-Co-ISAS/MMNC-900)上制备了一种具有高度分散Co单原子位的分级多孔钴单原子光催化剂,该催化剂显著促进了CO2-to-CO的光还原.0.8-Co-ISAS/MMNC-900催化剂的CO生成速率高达7261 μmol g-1 h-1,CO选择性高达90.1％,并且在四次循环测试中表现出良好的稳定性.实验数据和理论结果表明,分层多孔结构可以促进电荷分离引起的外部局部电场的形成,Co隔离的单原子位和微介孔构型协同作用,促进光激发电子积累、CO2吸附活化和*COOH中间体的形成.本研究通过多尺度多孔结构工程,提出了一种合成CO2还原光催化剂的新策略.
Abstract
Artificial photosynthesis,which converts CO2 into value-added chemicals and fuels,is of enormous potential in overcoming both global environmental problems and en-ergy crisis.However,the development of CO2 photoconver-sion catalysts with high efficiency remains a great challenge due to the thermodynamic stability and dynamics sluggishness of CO2.Herein,a superior hierarchical porous cobalt single-atom photocatalyst featuring highly dispersed Co isolated single atomic sites on micro-mesoporous nitrogen-doped carbon(0.8-Co-ISAS/MMNC-900)is developed and char-acterized,which significantly boosts the photoreduction of CO2-to-CO.The 0.8-Co-ISAS/MMNC-900 catalyst achieves a high 7261 μmol g-1 h-1 CO formation rate,an impressive 90.1％CO selectivity,as well as an decent stability during four times cycling test,indicating a boosted CO2 photoconversion property.Experimental data and theoretical results reveal that the hierarchically porous structure can promote the formation of exterior local electric field caused by charge separation as well as the synergic role of Co ISASs and micro-mesoporous configuration can facilitate photo-excited electron accumula-tion,CO2 adsorption and activation,and*COOH inter-mediate formation.This work develops a novel strategy to synthesize superior photocatalysts for CO2 reduction through multiscale porous structural engineering.
关键词
micro-mesoporous structure/single-atom catalysts/cobalt/photocatalytic CO2 reduction/CO selectivityKey words
micro-mesoporous structure/single-atom catalysts/cobalt/photocatalytic CO2 reduction/CO selectivity引用本文复制引用
基金项目
国家自然科学基金(11293064)
国家自然科学基金(22001015)
中央高校基本科研业务费专项(2050205)
出版年
2024
NETL
NSTL
万方数据