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在硫添加的中孔碳上,高选择性氧电还原到过氧化

Juan Du¹, Yicheng Liu¹, Ming Sun¹

¹College of Chemical and Pharmaceutical Engineering, Hebei University of Science and Technology, 26 Yuxiang Street, Shijiazhuang, 050018, P.R. China.

Angewandte Chemie (International ed. in English)

|April 9, 2025

概括

工程化硫合的半孔碳球作为高选择性的无金属电催化剂,用于两电子氧降解反应. 这些催化剂实现了高效的过氧化生产效率和活性,为传统材料提供了具有成本效益的替代品.

科学领域:

材料科学材料科学材料科学
电化学电化学电化学
催化剂是一种催化剂.

背景情况:

无金属电催化剂对于可持续能源应用至关重要.
为选择性二电子氧降解反应 (2e^--ORR) 到过氧化 (H₂O₂) 开发有效的催化剂仍然是一个挑战.

研究的目的:

为了设计和合成新型的,用硫合的 mesoporous carbon spheres (S-mC) 作为先进的电催化剂.
评估S-mC对2e^--ORR到H₂O₂的性能,重点关注选择性和活动.

主要方法:

垂直对齐的圆柱形半孔碳球的建筑设计.
碳矩阵的原子级硫化.
在两电子氧降解反应中进行电化学性能测试.
在现场光谱表征和密度函数理论 (DFT) 计算.

主要成果:

在2e-ORR中,S-mC催化剂表现出异常的H₂O₂选择性 (>99%) 和活性 (-3.5 mA cm^-2).
优化的S-mC在流细胞中实现了高H₂O₂的25molg_{催化剂^-1 h^-1的产量.}
独特的sp²/sp³混合碳网络和S诱导的电荷再分配创造了电子缺陷热点,稳定了OOH中间体.

结论:

S-mC的协同结构和电子特性使得选择性H₂O₂生产的金属类催化效率成为可能.
硫兴奋剂和中孔结构控制为开发强大的,经济高效的碳基电催化剂提供了有前途的战略.
这项工作为氧气高效电催化转化为过氧化开辟了新的途径.

关键词:

在H2O2中,H2O2是H2O的.顺序的垂直中位孔有序的.含有S-的碳.两个电子的氧气还原.

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