Covalent Immobilization of Molecular Complexes on Metal-Organic Frameworks Towards Robust and Highly Efficient Heterogeneous Water Oxidation Catalysts

Authors

Xiangming Liang, Lanzhou University
Sizhou Yang, Marquette University
Junyi Yang, Lanzhou University
Wanjun Sun, Lanzhou University
Xiangyang Li, Lanzhou University
Baochun Ma, Lanzhou University
Jier Huang, Marquette UniversityFollow
Jiangwei Zhang, Chinese Academy of Sciences
Lele Duan, Southern University of Science and Technology
Yong Ding, Lanzhou University

Document Type

Article

Publication Date

8-2021

Publisher

Elsevier

Source Publication

Applied Catalysis B: Environmental

Source ISSN

0926-3373

Abstract

The major challenges to practical implementation of efficient noble metal based molecular water oxidation catalysts are their stability and recycle ability. Herein, noble metal Ru based molecular water oxidation catalysts were covalently anchored in MOFs through “amide bond” as bridges, which leads to the formation of high-efficiency and robust heterogeneous catalysts for water oxidation reaction. We show that the efficiency for Ce^IV-driven water oxidation was significantly enhanced by 120 times when the Ru molecules were immobilized on the frameworks of MIL-101(Cr). The relationship between recycle stability and the structure of the Ru complexes covalently anchored in MOFs was carefully studied by recycle tests and various characterization methods. [Ru(terpy)(pic)₂(H₂O)]²⁺ was directly certified as real catalytic species instead of the original complex [Ru(terpy)(pic)₂Cl]⁺ by the X-ray absorption spectroscopy and control experiments. The synthetic method of hybrid catalysts offers a good strategy for enhancing water oxidation activity and stability of molecular catalysts.

Comments

Accepted version. Applied Catalysis B: Environmental, Vol. 291 (2021, August): 120070. DOI. © 2021 Elsevier. Used with permission.

Recommended Citation

Liang, Xiangming; Yang, Sizhou; Yang, Junyi; Sun, Wanjun; Li, Xiangyang; Ma, Baochun; Huang, Jier; Zhang, Jiangwei; Duan, Lele; and Ding, Yong, "Covalent Immobilization of Molecular Complexes on Metal-Organic Frameworks Towards Robust and Highly Efficient Heterogeneous Water Oxidation Catalysts" (2021). Chemistry Faculty Research and Publications. 1052.
https://epublications.marquette.edu/chem_fac/1052