| Citation: |
Songliang Liu, Shuli Yin, Lin Cui, Hongjie Yu, Kai Deng, Ziqiang Wang, You Xu, Liang Wang, Hongjing Wang. Interface engineering-inspired electron regulation in Pt/Pd hetero-metallene for methanol-assisted hydrogen evolution[J]. Energy Lab, 2023, 1(1): 220005. doi: 10.54227/elab.20220005
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Interface engineering-inspired electron regulation in Pt/Pd hetero-metallene for methanol-assisted hydrogen evolution
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Abstract
The small molecule oxidation reaction instead of oxygen evolution reaction coupled with hydrogen evolution reaction can greatly reduce the reaction overpotential of electrochemical water splitting, which is a very efficient and energy-saving hydrogen evolution strategy. Herein, we report an interface engineering constructed two-dimensional ultrathin curled Pt/Pd hetero-metallene for efficient electrocatalytic hydrogen evolution assisted by methanol. The thin-sheet structure of Pt/Pd hetero-metallene provides a large specific surface area and exposes numerous surface atoms that could act as reactive sites, thus accelerating the reaction mass transfer process. More importantly, the constructed Pt/Pd hetero-metallene possesses abundant Pt/Pd heterointerface, which can maximize the strong metal-metal interaction and increase the utilization of metal atoms, thereby optimizing the adsorption and activation of reactants during the reaction. Pt/Pd hetero-metallene can produce hydrogen stably and efficiently in 1 M KOH + 1 M CH3OH, and the voltage only needs 0.83 V at @100 mA cm−2 when used in electrocatalytic hydrogen evolution, which is much lower than the voltage required for the traditional electrochemical water splitting process (1.94 V). This work not only provides a powerful approach to rational design and construction of hetero-metallene through interface engineering, but also builds a bridge between hetero-metallene and methanol-assisted hydrogen evolution.
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References
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Songliang Liu, Shuli Yin, Lin Cui, Hongjie Yu, Kai Deng, Ziqiang Wang, You Xu, Liang Wang, Hongjing Wang. Interface engineering-inspired electron regulation in Pt/Pd hetero-metallene for methanol-assisted hydrogen evolution[J]. Energy Lab, 2023, 1(1): 220005. doi: 10.54227/elab.20220005
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Figure 1.
a Schematic illustration for the synthesis of the Pt/Pd hetero-metallene. b HAADF-STEM and c and d TEM images of the Pt/Pd hetero-metallene. e False-color HRTEM image of the Pt/Pd hetero-metallene. f The particle size distribution of figure 1d. The insets in e display the lattice fringes and corresponding atomic absorption intensity profile of the square region.
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Figure 2.
a HRTEM image of the Pt/Pd hetero-metallene. b HAADF-STEM and EDS mapping images of the Pt/Pd hetero-metallene.
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Figure 3.
a XRD patterns of the Pd metallene and Pt/Pd hetero-metallene. b XPS survey spectrum of the Pt/Pd hetero-metallene. c Pt 4f XPS spectra of the Pt/Pd hetero-metallene. d Pd 3d XPS spectra of Pt/Pd hetero-metallene and Pd metallene. e Bader charge of the Pt/Pd hetero-metallene. Negative and positive charge are indicated by red and blue balls, respectively. f Electron density difference on the Pt/Pd hetero-metallene. g, h and i Main side view, side view and top-view of electron density difference on the Pt/Pd hetero-metallene, respectively. The charge accumulation and depletion are indicated by cyan and yellow area, respectively. The isosurface level is 0.007 e Å−3.
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Figure 4.
a Mass-normalized and b ECSA-normalized CVs of MOR for various catalysts recorded at a scan rate of 50 mV s−1 with 1 M KOH + 1 M CH3OH. c Comparison of mass activities and specific activities for various catalysts. d Chronoamperometric curves for various catalysts recorded at −0.2 V in 1 M KOH + 1 M CH3OH.
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Figure 5.
a HER polarization curves for various catalysts in 1 M KOH and b the comparison of overpotentials at 10 mA cm−2. c Tafel slope plots for various catalysts. d HER polarization curves for the Pt/Pd hetero-metallene in 1 M KOH with and without 1 M CH3OH. e HER polarization curves for the Pt/Pd hetero-metallene before and after 5000 cycles in 1 M KOH. f Chronopotentiometry curves for the Pt/Pd hetero-metallene at a constant cathodic current density of 10 mA cm−2 in 1 M KOH for 15 h.
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Figure 6.
a Schematic illustration for two-electrode CH3OH-assisted water splitting system. b LSV curves of the Pt/Pd hetero-metallene as anode and cathode in 1 M KOH with and without 1 M CH3OH. c LSV curves of various catalysts in 1 M KOH + 1 M CH3OH in a two-electrode system. d LSV curves of Pt/Pd hetero-metallene || Pt/Pd hetero-metallene in 1 M KOH with different CH3OH concentrations and e corresponding voltages at 100 mA cm−2. f Chronopotentiometry curves of Pt/Pd hetero-metallene || Pt/Pd hetero-metallene at a constant current density of 10 mA cm−2 in 1 M KOH + 1 M CH3OH for 25 h.
