Modulating the Electronic Structure and Basal-Plane Adsorption of Janus CrSSe through Mechanochemical Activation
- 1Federal University of ABC , , , ,
Abstract
Mechanochemical activation offers a reversible and chemically noninvasive route to tune the basal-plane reactivity of two-dimensional catalysts. Here, spin-polarized density functional theory calculations are employed to investigate strain- and curvature-engineered Janus CrSSe for the hydrogen evolution reaction, comparing H* adsorption on the CrSSe-S and CrSSe-Se surfaces and extending the analysis to zigzag CrSSe-NT(n,0) nanotubes. HER-relevant H adsorption thermodynamics are evaluated within the computational hydrogen electrode framework using the adsorption free energy, ΔGads, and the H* binding energy, Eb. Pristine 2D CrSSe exhibits strongly non-thermo-neutral H* adsorption with a pronounced polarity dependence. In-plane strain markedly reconstructs the electronic structure, with biaxial tension inducing metallicity and spin polarization and driving ΔGads close to thermo-neutral values. Curvature introduces an additional polarity-dependent degree of freedom: S-terminated nanotubes exhibit spin-polarized metallic behavior, whereas Se-terminated nanotubes remain semiconducting and converge to zero-net-spin states. A pronounced structural–magnetic crossover between CrSSe-NT-S(20,0) and (21,0) is accompanied by an abrupt change in H* binding, revealing a direct coupling between curvature, magnetism, and chemisorption. Moderate axial tensile strain of 3–5% further tunes this curvature-dependent adsorption response and brings ΔGads closer to the thermo-neutral regime over a broad range of nanotube diameters. Overall, these results establish strain, curvature, and Janus polarity as coupled physical descriptors for controlling the electronic, magnetic, and hydrogen adsorption properties of CrSSe nanostructures.
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BibTeX
@article{quispe2026modulating,
title = {{Modulating the Electronic Structure and Basal-Plane Adsorption of Janus CrSSe through Mechanochemical Activation}},
author = {Juan Gomez Quispe and Pedro Alves da Silva Autreto},
journal = {ACS Omega},
year = {2026},
month = oct,
doi = {10.1021/acsomega.6c04409},
url = {https://pubs.acs.org/acsodf/article/11/41/62744/5445763/Modulating-the-Electronic-Structure-and-Basal},
note = {CC BY 4.0},
}
RIS
TY - JOUR
TI - Modulating the Electronic Structure and Basal-Plane Adsorption of Janus CrSSe through Mechanochemical Activation
AU - Juan Gomez Quispe
AU - Pedro Alves da Silva Autreto
PY - 2026
DA - 2026/10/07
JO - ACS Omega
DO - 10.1021/acsomega.6c04409
UR - https://pubs.acs.org/acsodf/article/11/41/62744/5445763/Modulating-the-Electronic-Structure-and-Basal
AB - Mechanochemical activation offers a reversible and chemically noninvasive route to tune the basal-plane reactivity of two-dimensional catalysts. Here, spin-polarized density functional theory calculations are employed to investigate strain- and curvature-engineered Janus CrSSe for the hydrogen evolution reaction, comparing H* adsorption on the CrSSe-S and CrSSe-Se surfaces and extending the analysis to zigzag CrSSe-NT(n,0) nanotubes. HER-relevant H adsorption thermodynamics are evaluated within the computational hydrogen electrode framework using the adsorption free energy, ΔGads, and the H* binding energy, Eb. Pristine 2D CrSSe exhibits strongly non-thermo-neutral H* adsorption with a pronounced polarity dependence. In-plane strain markedly reconstructs the electronic structure, with biaxial tension inducing metallicity and spin polarization and driving ΔGads close to thermo-neutral values. Curvature introduces an additional polarity-dependent degree of freedom: S-terminated nanotubes exhibit spin-polarized metallic behavior, whereas Se-terminated nanotubes remain semiconducting and converge to zero-net-spin states. A pronounced structural–magnetic crossover between CrSSe-NT-S(20,0) and (21,0) is accompanied by an abrupt change in H* binding, revealing a direct coupling between curvature, magnetism, and chemisorption. Moderate axial tensile strain of 3–5% further tunes this curvature-dependent adsorption response and brings ΔGads closer to the thermo-neutral regime over a broad range of nanotube diameters. Overall, these results establish strain, curvature, and Janus polarity as coupled physical descriptors for controlling the electronic, magnetic, and hydrogen adsorption properties of CrSSe nanostructures.
SN - 2470-1343
ER -