Liu Yuxuan, Tan Yufan, Zhang Keyi, Guo Tianqi, Zhu Yao, Cao Ting, Lv Haiyang, Zhu Junpeng, Gao Ze, Zhang Su, Liu Zheng, Liu Juzhe
State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing 100012, China.
The Key Laboratory of Resources and Environmental System Optimization, Ministry of Education, College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, China.
Molecules. 2024 Nov 25;29(23):5561. doi: 10.3390/molecules29235561.
The catalyst is the pivotal component in CO electroreduction systems for converting CO into valuable products. Carbon-based single-atom materials (CSAMs) have emerged as promising catalyst candidates due to their low cost and high atomic utilization efficiency. The rational design of the morphology and microstructure of such materials is desirable but poses a challenge. Here, we employed different Mg(OH) templates to guide the fabrication of two kinds of amorphous nitrogen-doped carbon nanosheet-supported Fe single atoms (FeSNC) with rough and flat surface structures. In comparison to flat FeSNC with saturated FeN sites, the rough FeSNC (R-FeSNC) exhibited unsaturated FeN sites and contracted Fe-N bond length. The featured structure endowed R-FeSNC with superior capacity of catalyzing CO reduction reaction, achieving an exceptional CO selectivity with Faradaic efficiency of 93% at a potential of -0.66 V vs. RHE. This study offers valuable insights into the design of CSAMs and provides a perspective for gaining a deeper understanding of their activity origins.
催化剂是将一氧化碳电还原为有价值产物的系统中的关键组件。碳基单原子材料（CSAMs）因其低成本和高原子利用效率，已成为有前景的催化剂候选材料。合理设计此类材料的形态和微观结构是可取的，但也具有挑战性。在此，我们采用不同的氢氧化镁模板来指导制备两种具有粗糙和平坦表面结构的非晶态氮掺杂碳纳米片负载铁单原子（FeSNC）。与具有饱和铁氮位点的平坦FeSNC相比，粗糙FeSNC（R-FeSNC）表现出不饱和铁氮位点和收缩的铁-氮键长。这种独特结构赋予R-FeSNC卓越的催化一氧化碳还原反应能力，在相对于可逆氢电极（RHE）为-0.66 V的电位下，实现了93%的法拉第效率下的优异一氧化碳选择性。这项研究为碳基单原子材料的设计提供了有价值的见解，并为更深入理解其活性起源提供了一个视角。
