苏州大学王炯团队报道了Silicalite-1沸石的电子传递特性研究及其潜在的电催化应用。相关研究成果于2024年10月30日发表在国际顶尖学术期刊《美国化学会杂志》。

开发高性能电催化剂对于可再生能源的可持续转化和储存至关重要。Silicalite-1（S-1）沸石被认为有望构建具有均匀和精确孔隙率，以及即使在极端电势下也具有稳定结构骨架的电催化剂。然而，其电化学性质仍然知之甚少，特别是关于内部孔道的作用。

该文利用经典氧化还原探针，研究了S-1沸石上的内外球电子转移（ISET/OSET）路线。结果首次表明，S-1沸石孔内的ISET动力学比外表面更快，通过微孔尺度通道和端羟基进行了优化。相反，OSET的动力学并不完全取决于S-1沸石的孔隙率和表面性质。

这些电化学见解进一步引发了锂离子掺入S-1沸石的快速ISET动力学，用于氧还原的电催化。它在中性溶液中对H₂O₂的生产表现出85%的高选择性，在流动池中配置时的产量为9.2 mol gcat^-1 h^-1。

附：英文原文

Title: To Investigate Electron Transfer Properties on Silicalite-1 Zeolite for Potential Electrocatalytic Applications

Author: Yingying Jin, Xichen Yin, Guanghua Yu, Qiming Sun, Jiong Wang

Issue&Volume: October 30, 2024

Abstract: To develop high-performance electrocatalysts is critical to sustainable conversion and storage of renewable energy. Silicalite-1 (S-1) zeolite is considered promising for constructing electrocatalysts featuring uniform and precise porosity and a stable structural skeleton even at extreme potentials. However, its electrochemical properties remain poorly understood, particularly regarding the roles of internal pore channels. Herein, inner- and outer-sphere electron transfer (ISET/OSET) routes on the S-1 zeolite were investigated by classical redox probes. The results for the first time revealed that the ISET kinetics inside the pores of S-1 zeolite is more rapid than that on external surfaces, optimized by microporous scale channels and terminated hydroxyl groups. Conversely, the kinetics of the OSET did not closely depend on the porosity and surface properties of the S-1 zeolite. These electrochemical insights further initiated a lithium-ion-incorporated S-1 zeolite with rapid ISET kinetics for electrocatalysis of oxygen reduction. It demonstrated a high performance of 85% selectivity for H2O2 production in a neutral solution and a yield of 9.2 mol gcat–1 h–1 when configured in a flow cell.

DOI: 10.1021/jacs.4c10258

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.4c10258