Issue 27, 2023

Multi-interfacial engineering of an interlinked Ni2P–MoP heterojunction to modulate the electronic structure for efficient overall water splitting

Abstract

Exploring efficient and cost-efficient bifunctional electrocatalysts is crucial for H2 production via overall water splitting. Multi-interface engineering is a promising strategy to overcome the intrinsic activity limitation of electrocatalysts by the ensemble effect and electron effect but it is challenging. Herein, we elaborately designed and synthesized a multi-interface-coupled heterojunction composed of Ni2P and MoP encapsulated by N-doped carbon (Ni2P–MoP@NC), which possesses an adjustable electronic structure based on “d-electron complementation” to achieve effective HER and OER catalysis. A post-synthetic modification strategy anchoring Ni2+ ions on the phosphomolybdic acid (PMo12)-organic supramolecular via the multiple linkages of organic ligands is proposed, which ensures the construction of multiple hetero-interfaces electrocatalyst by means of the natural quasi-interfaces of {PMo12-organic ligand-Ni}. The organic ligands also play a crucial role in the size control of Ni2P–MoP nanoparticles (ca. 7 nm). Experimental characterization combined with theoretical calculations reveal that the heterojunction triggers the electron redistribution, thereby facilitating water dissociation and optimizing H* adsorption energy to boost the HER, and balancing the adsorption energies of oxygenated intermediates to lower the thermodynamic barrier for the OER. Consequently, Ni2P–MoP@NC exhibits excellent HER and OER activity with low overpotentials of 69 and 249 mV at 10 mA cm−2 in alkaline media. The alkali-electrolyzer assembled by Ni2P–MoP@NC requires a low voltage of 1.54 V to achieve 10 mA cm−2 with good durability. This work proposes a new route to design various multi-touch heterojunctions constructed using other early and late transition metals.

Graphical abstract: Multi-interfacial engineering of an interlinked Ni2P–MoP heterojunction to modulate the electronic structure for efficient overall water splitting

Supplementary files

Article information

Article type
Paper
Submitted
26 mars 2023
Accepted
12 juin 2023
First published
13 juin 2023

J. Mater. Chem. A, 2023,11, 15033-15043

Multi-interfacial engineering of an interlinked Ni2P–MoP heterojunction to modulate the electronic structure for efficient overall water splitting

W. Zhang, H. Yan, Y. Liu, D. Wang, Y. Jiao, A. Wu, X. Wang, R. Wang and C. Tian, J. Mater. Chem. A, 2023, 11, 15033 DOI: 10.1039/D3TA01789C

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