Leveraging Curvature on N–Doped Carbon Materials for Hydrogen Storage

Rice, Peter S.; Lee, Gabriel; Schwartz, Brayden; Autrey, Tom; Ginovska, Bojana

doi:10.1002/smll.202310162

Leveraging Curvature on N–Doped Carbon Materials for Hydrogen Storage

Journal Article · Sun Jan 14 00:00:00 EST 2024 · Small

DOI:https://doi.org/10.1002/smll.202310162· OSTI ID:2409379

^[1]; Lee, Gabriel ^[1]; Schwartz, Brayden ^[1]; ^[1]; ^[1]

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Carbon sorbent materials have shown great promise for solid-state hydrogen (H₂) storage. Modification of these materials with nitrogen (N) dopants has been undertaken to develop materials that can store H₂ at ambient temperatures. In this work density functional theory (DFT) calculations are used to systematically probe the influence of curvature on the stability and activity of undoped and N-doped carbon materials toward H binding. Specifically, four models of carbon materials are used: graphene, [5,5] carbon nanotube, [5,5] D_5d-C₁₂₀, and C₆₀, to extract and correlate the thermodynamic properties of active sites with varying degrees of sp² hybridization (curvature). From the calculations and analysis, it is found that graphitic N-doping is thermodynamically favored on more pyramidal sites with increased curvature. In contrast, it is found that the hydrogen binding energy is weakly affected by curvature and is dominated by electronic effects induced by N-doping. These findings highlight the importance of modulating the heteroatom doping configuration and the lattice topology when developing materials for H₂ storage.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; AC05-76RL01830

OSTI ID:: 2409379

Alternate ID(s):: OSTI ID: 2282188

Report Number(s):: PNNL-SA--191964

Journal Information:: Small, Journal Name: Small Journal Issue: 25 Vol. 20; ISSN 1613-6810

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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