Multiple-Strategy Design of MOF-Derived N, P Co-Doped MoS2 Electrocatalysts Toward Efficient Alkaline Hydrogen Evolution and Overall Water Splitting

• Published in: ACS applied materials & interfaces Vol. 15; no. 45; pp. 52506 - 52518
• Main Authors: Ding, Pengbo, Wang, Tian, Chang, Pu, Guan, Lixiu, Liu, Zongli, Xu, Chao, Tao, Junguang
• Format: Journal Article
• Language: English
• Published: American Chemical Society 01.11.2023
• Subjects: Energy, Environmental, and Catalysis Applications; phase engineering; metal−organic framework (MOF); electrocatalysts; hydrogen evolution reaction (HER); MoS2
• ISSN: 1944-8244; 1944-8252
• DOI: 10.1021/acsami.3c11802

The multiple strategy design is crucial for enhancing the efficiency of nonprecious electrocatalysts in hydrogen evolution reaction (HER). In this work, we successfully synthesized N, P-codoped MoS2 nanosheets as highly efficient catalysts by integrating doping effects and phase engineering using a porous metal–organic framework (MOF) template. The electrocatalysts exhibit excellent bifunctional activity and stability in alkaline media. The N, P codoping induces electron redistribution to enhance conductivity and promote the intrinsic activity of the electrocatalysts. It optimizes the H* adsorption free energy and the dissociative adsorption energy, resulting in significant enhancement of HER activity. Moreover, the porous MOF structure exposes a large number of electrochemically active sites and facilitates the diffusion of ions and gases, which improve charge transfer efficiency and structural stability. Specifically, at a current density of 10 mA cm–2, the overpotential of the HER is only 32 mV, with a Tafel slope of 47 mV dec–1 and Faradaic efficiency as high as 98.51% (at 100 mA cm–2). Only a 338 mV overpotential is required to achieve a current density of 50 mA cm–2 for oxygen evolution reaction (OER), and a potential of 1.49 V (at 10 mA cm–2) is sufficient to drive overall water splitting. Further experimental measurements and first-principles calculations evidence that the exceptional performance is primarily attributed to the dual functionality of N and P dopants, which not only activate additional S sites but also initialize the phase transition of 2H to 1T-MoS2 to facilitate the rapid charge transfer. Through in-depth exploration of the combined design of multiple strategies for efficient catalysts, our work paves a new way for the development of future efficient nonprecious metal catalysts.