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250811s2025 xx |||||o 00| ||eng c |
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|a 10.1002/adma.202509904
|2 doi
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|a pubmed25n1527.xml
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|a (DE-627)NLM390968722
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|a (NLM)40787930
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|a eng
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|a Dai, Liming
|e verfasserin
|4 aut
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|a Charge-Buffered Sulfidation Stabilized Bδ- in 1T MoS2
|b Orbital Alignment for Efficient Alkaline Hydrogen Production
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|c 2025
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|a Text
|b txt
|2 rdacontent
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|a ƒaComputermedien
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|2 rdamedia
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|a ƒa Online-Ressource
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|a Date Revised 11.08.2025
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|a published: Print-Electronic
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|a Citation Status Publisher
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|a © 2025 Wiley‐VCH GmbH.
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|a 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
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|a Journal Article
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|a 1T molybdenum disulfide
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|a alkaline hydrogen evolution reaction
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|a anionic boron doping
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|a charge‐buffered sulfidation
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|a empty pz orbital
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|a Fang, Chenchen
|e verfasserin
|4 aut
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1 |
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|a Zhang, Xiaoyuan
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Wang, Yaya
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Gao, Rui
|e verfasserin
|4 aut
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| 700 |
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|a Huang, Ying
|e verfasserin
|4 aut
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| 700 |
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|a Zhang, Lin
|e verfasserin
|4 aut
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| 700 |
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|a Xue, Liang
|e verfasserin
|4 aut
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|a Xiong, Pan
|e verfasserin
|4 aut
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|a Fu, Yongsheng
|e verfasserin
|4 aut
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|a Sun, Jingwen
|e verfasserin
|4 aut
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|a Zhu, Junwu
|e verfasserin
|4 aut
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| 773 |
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|i Enthalten in
|t Advanced materials (Deerfield Beach, Fla.)
|d 1998
|g (2025) vom: 11. Aug., Seite e09904
|w (DE-627)NLM098206397
|x 1521-4095
|7 nnas
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| 773 |
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|g year:2025
|g day:11
|g month:08
|g pages:e09904
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|u http://dx.doi.org/10.1002/adma.202509904
|3 Volltext
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