Boosting electrocatalytic activity for CO2 reduction on nitrogen-doped carbon catalysts by co-doping with phosphorus

掺杂剂 兴奋剂 催化作用 法拉第效率 电催化剂 氮气 碳纤维 电化学 过渡金属 化学工程 密度泛函理论 无机化学 材料科学 化学 纳米技术 电极 计算化学 物理化学 有机化学 光电子学 复合材料 工程类 复合数
作者
Shuo Chen,Tian‐Fu Liu,Samson O. Olanrele,Zan Lian,Chaowei Si,Zhimin Chen,Bo Li
出处
期刊:Journal of Energy Chemistry [Elsevier BV]
卷期号:54: 143-150 被引量:50
标识
DOI:10.1016/j.jechem.2020.05.006
摘要

Electrochemical reduction of CO2 (CERR) to value-added chemicals is an attractive strategy for greenhouse gas mitigation, and carbon recycles utilization. Conventional metal catalysts suffered from low durability and sluggish kinetics impede the practical application. On the other hand, doped carbon materials recently demonstrate superior catalytic performance in CERR, which shows the potential to diminish the problems of metal catalysts to some extent. Herein, we present the design and fabrication of nitrogen (N), phosphorus (P) co-doped metal-free carbon materials as an efficient and stable electrocatalyst for reduction of CO2 to CO, which exhibits an excellent performance with a high faradaic efficiency of 92% (−0.55 V vs. RHE) and up to 24 h stability. A series of characterizations including TEM and XPS verified that nitrogen and phosphorous are successfully incorporated into the carbon matrix. Moreover, the comparisons between co-doping and single doping catalysts reveal that co-doping can significantly increase CERR performance. The improved catalytic activity is attributed to the synergetic effects between nitrogen and phosphorous dopants, which effectively modulate properties of the active site. The density functional theory (DFT) calculations were also performed to understand the synergy effects of dopants. It is revealed that the phosphorous doping can significantly lower the Gibbs free energy of COOH* formation. Moreover, the introduction of the second dopants phosphorous can reduce the reaction barrier along the reaction path and cause polarization of density of states at the Fermi level. These changes can greatly enhance the activity of the catalysts. From a combined experimental and computational exploration, current work provides valuable insights into the reaction mechanism of CERR on N, P co-doped carbon catalysts, and the influence from synergy effects between dopants, which paves the way for the rational design of novel metal-free catalysts for CO2 electro-reduction.
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