期刊
SMALL
卷 18, 期 4, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202105642
关键词
hydrogen evolution reaction; in-plane heterostructures; large current density; metal phosphides
类别
资金
- National Science Foundation of China [12074116, 52172197]
- Youth 1000 Talent Program of China, Undergraduate Scientific Research Innovation Project of China [202110542037]
- Science and Technology Innovation Platform [2018RS3070, 2019RS1032]
- Hundred Youth Talents Programs of Hunan Province
- Hunan Normal University [2021133, 21CSZ004, 21CSZ029]
- Hunan Joint International Laboratory of Advanced Materials and Technology for Clean Energy [2020CB1007]
This study introduces a novel strategy to integrate phosphorus-rich NiP2 and phosphorus-poor Ni5P4 into in-plane heterostructures, effectively enhancing the hydrogen-evolving activity of nickel phosphides by modulating their electronic structure and utilizing phosphorus atoms as active sites. The NiP2/Ni5P4 hybrid exhibits outstanding catalytic performance, surpassing most earth-abundant electrocatalysts and comparable to platinum catalysts in terms of hydrogen evolution efficiency.
The catalytic hydrogen-evolving activities of transition-metal phosphides are greatly related to the phosphorus content, but the physical origin of performance enhancement remains ambiguous, and tuning the catalytic activity of nickel phosphides (NiP2/Ni5P4) remains challenging due to unfavorable H* adsorption. Here, a strategy is introduced to integrate P-rich NiP2 and P-poor Ni5P4 into in-plane heterostructures by anion substitution, in which P atoms at the in-plane interfaces perform as active sites to adsorb H* and thus facilitate the hydrogen evolution reaction (HER) process via modulating the electronic structure between NiP2 and Ni5P4. Consequently, the NiP2/Ni5P4 hybrid exhibits an outstanding hydrogen-evolving activity, requiring only 30 and 76 mV to afford 10 and 100 mA cm(-2) in acid, respectively. It surpasses most of the earth-abundant electrocatalysts thus far, and is comparable to Pt catalysts (30/72 mV at 10/100 mA cm(-2)). Particularly, it can run smoothly at large current density and only requires 247 mV to reach 2000 mA cm(-2). Detailed theoretical calculations reveal that its exceptional activity stems from the moderate overlap of density states between P 2p and H 1s orbitals, thus optimizing the H*-adsorption strength. This work highlights a new avenue toward the fabrication of robust non-noble electrocatalysts by constructing in-plane heterojunctions.
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