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Charge-Buffered Sulfidation Stabilized Bδ− in 1T MoS2: Orbital Alignment for Efficient Alkaline Hydrogen Production
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DOI：10.1002/adma.202509904.png)
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Abstract
En 中文
The sp3 hybridization of surface sulfur in metallic phase molybdenum disulfide (1T MoS2) is identified as the intrinsic bottleneck for alkaline hydrogen production (HER), where their electron-saturated nature elevates the kinetic barrier for water dissociation. To overcome this limitation, a charge-buffered sulfidation strategy is reported to stabilize anionic boron (Bδ−) within 1T MoS2. By employing molybdenum aluminum boride as the precursor, the Bδ− dopants can be efficiently preserved via the topological confinement imposed by Mo─B─Mo network. This approach also maintains the 1T phase integrity through Al-mediated electron compensation. Theoretical and experimental analyses reveal that Bδ− substitution generates vertically oriented empty pz orbitals through sp2 hybridization, which elevates orbital energy to align with molecular orbitals of water, significantly reducing the O─H cleavage barrier by over 80% compared to 1T MoS2. Concurrently, the B─Mo─S networks upshift adjacent sulfur 3p band centers to optimize the hydrogen adsorption path. These dual functionalities endow the pz-functionalized 1T MoS2 with a low overpotential of −30 mV at 10 mA cm−2, and high-current operation of 1 A cm−2 at 1.779 V in an anion-exchange membrane electrolytic cell. This work not only establishes orbital alignment as a transformative design principle for advanced electrocatalysts, but also paves a novel synthetic pathway for 1T transition metal disulfides.
Keywords:
1T molybdenum disulfide
alkaline hydrogen evolution reaction
anionic boron doping
charge-buffered sulfidation
empty pz orbital
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