Yan Minmin, Wei Zengxi, Gong Zhichao, Johannessen Bernt, Ye Gonglan, He Guanchao, Liu Jingjing, Zhao Shuangliang, Cui Chunyu, Fei Huilong
State Key Laboratory for Chemo/Biosensing and Chemometrics, and College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, China.
Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology and School of Chemistry and Chemical Engineering, Guangxi University, Nanning, 530004, China.
Nat Commun. 2023 Jan 23;14(1):368. doi: 10.1038/s41467-023-36078-y.
Selective two-electron (2e) oxygen reduction reaction (ORR) offers great opportunities for hydrogen peroxide (HO) electrosynthesis and its widespread employment depends on identifying cost-effective catalysts with high activity and selectivity. Main-group metal and nitrogen coordinated carbons (M-N-Cs) are promising but remain largely underexplored due to the low metal-atom density and the lack of understanding in the structure-property correlation. Here, we report using a nanoarchitectured SbS template to synthesize high-density (10.32 wt%) antimony (Sb) single atoms on nitrogen- and sulfur-codoped carbon nanofibers (Sb-NSCF), which exhibits both high selectivity (97.2%) and mass activity (114.9 A g at 0.65 V) toward the 2e ORR in alkaline electrolyte. Further, when evaluated with a practical flow cell, Sb-NSCF shows a high production rate of 7.46 mol g h with negligible loss in activity and selectivity in a 75-h continuous electrolysis. Density functional theory calculations demonstrate that the coordination configuration and the S dopants synergistically contribute to the enhanced 2e ORR activity and selectivity of the Sb-N moieties.
选择性双电子（2e）氧还原反应（ORR）为过氧化氢（HO）的电合成提供了巨大机遇，其广泛应用取决于能否找到具有高活性和选择性的经济高效催化剂。主族金属与氮配位的碳材料（M-N-Cs）很有前景，但由于金属原子密度低以及对结构-性能相关性缺乏了解，在很大程度上仍未得到充分探索。在此，我们报道利用纳米结构的SbS模板在氮硫共掺杂的碳纳米纤维（Sb-NSCF）上合成高密度（10.32 wt%）的锑（Sb）单原子，该材料在碱性电解质中对2e ORR表现出高选择性（97.2%）和质量活性（在0.65 V时为114.9 A g）。此外，在实际流动池中进行评估时，Sb-NSCF在75小时的连续电解中显示出7.46 mol g h的高生产率，活性和选择性损失可忽略不计。密度泛函理论计算表明，配位构型和S掺杂剂协同作用，提高了Sb-N部分的2e ORR活性和选择性。
