Issue 34, 2024

Transition metal chalcogenide nanoparticle embedded metal–organic framework nanosheets for high-performance H2O2 electrosynthesis

Abstract

The rational design of high-performance two-electron oxygen reduction reaction (2e-ORR) electrocatalysts is of great significance for sustainable H2O2 production. Herein, we report the synthesis of a transition-metal chalcogenide@metal–organic framework (TMC@MOF) composite material as an efficient 2e-ORR electrocatalyst. Through a partial conversion route using NiFe-MOF nanosheets as precursors, the Ni ions are partially converted into NiS2 nanoparticles, which are embedded in the MOF skeleton with partially preserved crystalline structure and in situ generated mesopores. Experimental and theoretical results demonstrate that the interaction between NiS2 and retained MOFs regulates the electronic structure of Ni sites in NiS2 toward optimized adsorption of oxygen intermediates, enhancing the 2e-ORR selectivity. Additionally, the ultrasmall NiS2 nanoparticles (grain size < 10 nm) expose abundant active sites, and the created mesopores facilitate the mass transfer. Collectively, excellent 2e-ORR performances are achieved with a high selectivity of 96% and a high H2O2 production rate of 4.2 mol gcat−1 h−1. The proposed partial sulfidation strategy paves the way for the design of advanced MOF-based composite materials for various applications.

Graphical abstract: Transition metal chalcogenide nanoparticle embedded metal–organic framework nanosheets for high-performance H2O2 electrosynthesis

Supplementary files

Article information

Article type
Paper
Submitted
06 May 2024
Accepted
23 Jul 2024
First published
26 Jul 2024

J. Mater. Chem. A, 2024,12, 22557-22564

Transition metal chalcogenide nanoparticle embedded metal–organic framework nanosheets for high-performance H2O2 electrosynthesis

X. Zhang, C. Zhang, Y. Zou, T. Bao, J. Wang, S. Y. Al-Qaradawi, N. K. Allam, C. Yu and C. Liu, J. Mater. Chem. A, 2024, 12, 22557 DOI: 10.1039/D4TA03151B

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