期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 291, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120100
关键词
Interface optimization; H2O dissociation; pH-universal catalyst; Stability
资金
- National Natural Science Foundation of China [51972011, 51622204]
This study introduces two-dimension monolayer Ti3C2 MXene sheets to support PtNi octahedrons, enhancing the activity and stability of PtNi nanoparticles in alkaline electrolyte. The resulting PtNi@Ti3C2 MXene exhibits excellent mass activity and stability, outperforming commercial Pt/C catalysts and other recent Pt-based alkaline HER catalysts. Interface interactions between PtNi and Ti3C2 MXene contribute to the improved performance by promoting stability and maintaining activity through interfacial electron transfer.
It remains a great challenge to balance the activity and stability of platinum and Pt-based hydrogen evolution reaction (HER) catalysts in alkaline electrolyte. Herein, two-dimension monolayer Ti3C2 MXene sheets were introduced to support PtNi octahedrons (PtNi@Ti3C2 MXene), which optimizes the activity and stability of PtNi nanoparticles (NPs) through interface interactions between PtNi and Ti3C2 MXene. It shows a small overpotential of 36 mV with a Tafel slope of 59 mV dec-1 at 10 mA cm-2 in 1 M KOH. It also exhibits excellent mass activity of 6.31 mA mu gPt-1 at an overpotential of 70 mV, which is -7.1 times that of commercial Pt/C and better than many recent reported Pt-based alkaline HER catalysts. Meanwhile, the PtNi@Ti3C2 MXene gives an increased overpotential of -4 mV while the PtNi gives -25 mV during a long-time continuous CV cycles. A series of characterizations disclose these interfaces could promote the stability by alleviating the Ni atoms dissolution from surficial PtNi through uniformly lattice strain dispersion of PtNi. Simultaneously, they could keep the activity by interfacial electron transfer from PtNi to Ti3C2 MXene demonstrated both by experimental tests (UPS, electrostatic potential and charge density distribution) and DFT calculation. It could decrease the energy barrier of H2O adsorbing and dissociating into hydrogen intermediates, further accelerating the recombination of hydrogen intermediates to H2. Under acidic and neutral medium, the electrocatalyst also exhibits improved HER performance compared to its counterparts. This work provides an interface optimization route for developing highefficiency pH-universal especially alkaline HER electrocatalysts.
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