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Guiding Successive Mo 4d–S 3p Orbital Hybridization in MoS2 via Dual-Confinement Engineering for Efficient Pseudocapacitive Storage
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DOI：10.1002/aenm.71344.png)
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Abstract
En 中文
The pseudocapacitive performance of MoS2 is intrinsically hampered by its poor electronic conductivity and inert basal planes, primarily arising from weak Mo 4d–S 3p orbital hybridization. Herein, we present a dual-confinement strategy that simultaneously modulates orbital hybridization via lattice-confined Mn doping and interlayer-confined ethylene glycol (EG), yielding a Mn- and EG-co-engineered MoS2 architecture (denoted as Mn-EG-MoS2). Microscopic characterization and theoretical calculations reveal that Mn substitution reconstructs the local Mo–S coordination, enhancing both Mo 4d–S 3p and Mn 3d–S 3p hybridization, thereby activating the basal plane sites and reinforcing Mo–S–Mn bonding in Mn-EG-MoS2. Simultaneously, EG incorporation expands the interlayer spacing and promotes dynamic orbital coupling across layers, effectively enhancing electron-ion transport kinetics. Consequently, the Mn-EG-MoS2 electrode delivers a high areal capacitance of 757.5 mF cm−2 at 5 mA cm−2 and good cycling stability. Furthermore, asymmetric supercapacitors assembled with a PVP-MnO2 cathode achieve a high energy density of 164.00 µWh cm−2 at 9.77 mW cm−2, superior cycling stability retaining 90.06% of their initial capacitance after 5000 cycles at 30 mA cm−2, and robust mechanical flexibility. This work establishes an effective design strategy by tuning orbital-level interactions via dual-confinement engineering for developing high-performance layer-structured materials.
Keywords:
confinement engineering
d-p orbital hybridization
pseudocapacitive storage
supercapacitors
transition metal sulfides
Journal
IF:
26
Papers:
1.0W
Citations:
15.7W
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