Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 296, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120336
Keywords
Molybdenum carbide; Polyoxometalates precursor; In-situ confined carburization; Atomically dispersed Ni; Electrocatalytic hydrogen evolution
Funding
- National Natural Science Foundation of China [21878336]
- Shandong Provincial Natural Science Foundation, China [ZR2018MB035]
- Fundamental Research Funds for the Central Universities [19CX02008A, 20CX02213A]
- PetroChina Innovation Foundation [2019D-5007-0401]
- Taishan Scholars Program of Shandong Province [tsqn201909065]
- Applied Basic Research Projects of Qingdao [19-6-2-27-cg]
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A novel supramolecular-confinement pyrolysis strategy was proposed to construct ultrafine Ni-Mo2C nanoparticles uniformly distributed on N,P co-doped carbon (NPC). The Ni-Mo2C/NPC material exhibited remarkable electrocatalytic activity for hydrogen evolution reaction, showing great potential for clean energy conversion. The study demonstrated the development of high-active HER catalytic sites through atomic-scale catalyst design, providing opportunities for fabricating low-cost and efficient catalysts.
Herein, a novel supramolecular-confinement pyrolysis strategy was proposed to construct ultrafine Ni-Mo2C nanoparticles uniformly distributed on N,P co-doped carbon (NPC) by using polyoxometalate supramolecular aggregate as precursor. Ni-Mo2C/NPC exhibits remarkable electrocatalytic activity for hydrogen evolution reaction (HER) in both acidic and alkaline conditions, as well as superior long-term durability. Combining EXAFS with DFT calculations, we demonstrate that Ni species were atomically dispersed and anchored by Mo2C lattice and P atoms from NPC, thus defining Mo(C)-Ni-P active sites, which enhance the intrinsic catalytic activity of Mo2C by atomic-scale Ni doping and Ni-P catalyst-substrate chemical coupling. The Mo(C)-Ni-P sites have optimal hydrogen adsorption free energies and can precisely regulate and activate the neighboring C, leading to excellent HER performance. This work developed a bottom-up polyoxometalate-based supramolecular approach for in-situ assembly of high-active HER catalytic sites, which will provide opportunities to design and fabricate low-cost and efficient atomic-scale catalysts for clean energy conversion.
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