期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 318, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2022.121859
关键词
Metal-organic frameworks; Lattice distortion; Electron-donating effect; Photocatalysis; H2O2 generation
资金
- National Natural Science Foundation of China (NSFC) [51908218, 22075085, 22173069, 21905092]
- Shanghai Science and Technology Foundation [19JC1412100]
- Research Project of Shanghai Science and Technology Commission [21ZR1467800]
- Fundamental Research Funds for the Central Universities
This study found that partial replacement of formate by methoxy in UIO-66-NH2 can significantly enhance the production of H2O2. The introduction of methoxy induces lattice distortion and changes the proton donor for the protonation of OOH* intermediate, lowering the kinetic energy barrier. Methoxy groups also have an electron-donating effect, contributing to enhanced light harvesting and charge separation. The selectivity of the methoxy-functionalized UIO-66-NH2 for 2e-ORR is also improved.
Semiconducting metal-organic frameworks (MOFs) are emerging photocatalysts for H2O2 production via the two-electron oxygen reduction (2e-ORR) process. Whether and how the functional groups on MOF nodes affect the 2e-ORR mechanism and performance remain largely unexplored. Herein, we report that partial replacement of formate (-COO-) by methoxy (-OMe) coordinated Zr-oxo cluster in UIO-66-NH2 significantly enhances the H2O2 production. The introduction of -OMe groups induces lattice distortion in UIO-66-NH2, resulting in the change of proton donor for the protonation of OOH* intermediate from -COOH to -NH3+ with a lowered kinetic energy barrier. The -OMe groups with electron-donating effect contribute to promoted light harvesting and charge separation. The 2e-ORR selectivity of -OMe functionalized UIO-66-NH2 is also enhanced, evidenced by rotating ring-disk electrode test and theoretical calculation. As a result, an improved photocatalytic ability is achieved with an H2O2 yield of 312.9 mM g(-1) h(-1), similar to 4.7 times higher than that of the original UIO-66-NH2.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据