ArticleProceedings of the National Academy of Sciences of the United States of America2023
Unveiling the structural transformation and activity origin of heteroatom-doped carbons for hydrogen evolution.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2023. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 9 papers.
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9 citing papers in PubMed.
- Biowaste-Derived Catalysts for Sustainable Electrochemical Water Splitting: A Pathway to Circular Bioeconomy.ChemSusChem · 2026Review
- Multidimensional design of carbon-supported Ru-based catalysts: a journey to hydrogen evolution reaction performance breakthroughs.Chemical science · 2026Review
- Implantable bioelectronic devices for photoelectrochemical and electrochemical modulation of cells and tissues.Nature reviews bioengineering · 2025Article
- A novel electrodeposited nanocatalyst of nickel nanoparticles and reduced graphene oxide doped with halogens for hydrogen evolution reaction.Scientific reports · 2025Article
- A New Doped Graphene-Based Catalyst for Hydrogen Evolution Reaction Under Low-Electrolyte Concentration and Biomass-Rich Environments.Energy & fuels : an American Chemical Society journal · 2025Article
- Vanadium-regulated nickel phosphide nanosheets for electrocatalytic sulfion upgrading and hydrogen production.Chemical science · 2025Article
- Electrochemically synthesized HNature communications · 2024Article
- Dual-strategy engineered nickel phosphide for achieving efficient hydrazine-assisted hydrogen production in seawater.Chemical science · 2024Article
- Recent Advances in Mechanistic Understanding of Metal-Free Carbon Thermocatalysis and Electrocatalysis with Model Molecules.Nano-micro letters · 2024Review
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6 authors.
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Abstract
Heteroatom-doped carbon materials have been widely used in many electrocatalytic reduction reactions. Their structure-activity relationships are mainly explored based on the assumption that the doped carbon materials remain stable during electrocatalysis. However, the structural evolution of heteroatom-doped carbon materials is often ignored, and their active origins are still unclear. Herein, taking N-doped graphite flake (N-GP) as the research model, we present the hydrogenation of both N and C atoms and the consequent reconstruction of the carbon skeleton during the hydrogen evolution reaction (HER), accompanied by a remarkable promotion of the HER activity. The N dopants are gradually hydrogenated and almost completely dissolved in the form of ammonia. Theoretical simulations demonstrate that the hydrogenation of the N species leads to the reconstruction of the carbon skeleton from hexagonal to 5,7-topological rings (G5-7) with thermoneutral hydrogen adsorption and easy water dissociation. P-, S-, and Se-doped graphites also show similar removal of doped heteroatoms and the formation of G5-7 rings. Our work unveils the activity origin of heteroatom-doped carbon toward the HER and opens a door to rethinking the structure-performance relationships of carbon-based materials for other electrocatalytic reduction reactions.
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