1. Engineering interfacial sulfur migration in transition-metal sulfide enables low overpotential for durable hydrogen evolution in seawater.
- Author
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Li, Min, Li, Hong, Fan, Hefei, Liu, Qianfeng, Yan, Zhao, Wang, Aiqin, Yang, Bing, and Wang, Erdong
- Subjects
NITROGEN ,SULFUR ,HYDROGEN evolution reactions ,SEAWATER ,SULFUR cycle ,OVERPOTENTIAL ,DENSITY functional theory - Abstract
Hydrogen production from seawater remains challenging due to the deactivation of the hydrogen evolution reaction (HER) electrode under high current density. To overcome the activity-stability trade-offs in transition-metal sulfides, we propose a strategy to engineer sulfur migration by constructing a nickel-cobalt sulfides heterostructure with nitrogen-doped carbon shell encapsulation (CN@NiCoS) electrocatalyst. State-of-the-art ex situ/in situ characterizations and density functional theory calculations reveal the restructuring of the CN@NiCoS interface, clearly identifying dynamic sulfur migration. The NiCoS heterostructure stimulates sulfur migration by creating sulfur vacancies at the Ni
3 S2 -Co9 S8 heterointerface, while the migrated sulfur atoms are subsequently captured by the CN shell via strong C-S bond, preventing sulfide dissolution into alkaline electrolyte. Remarkably, the dynamically formed sulfur-doped CN shell and sulfur vacancies pairing sites significantly enhances HER activity by altering the d-band center near Fermi level, resulting in a low overpotential of 4.6 and 8 mV at 10 mA cm−2 in alkaline freshwater and seawater media, and long-term stability up to 1000 h. This work thus provides a guidance for the design of high-performance HER electrocatalyst by engineering interfacial atomic migration. Stable and efficient hydrogen production from seawater remains challenging. Here the authors engineer sulfur migration in NiCoS electrocatalyst via N-doped carbon encapsulation, generating S vacancies and S doped CN active sites at the interface that improves electrocatalytic hydrogen evolution activity and durability in both alkaline freshwater and seawater. [ABSTRACT FROM AUTHOR]- Published
- 2024
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