Electrochemically formed PtFeNi alloy nanoparticles on defective NiFe LDHs with charge transfer for efficient water splitting

doi:10.1016/S1872-2067(21)63926-8

Abstract

Abstract:

Efficient and stable bifunctional electrocatalysts for water splitting is essential for producing hydrogen and alleviating huge energy consumption. Meanwhile, charge transfer engineering is an efficient approach to modulate the localized electronic properties of catalysts and tune the electrocatalytic performance. Herein, we tactfully fabricate PtFeNi alloys/NiFe layered double hydroxides (LDHs) heterostructure by an easily electrochemical way with a small amount of Pt. The experimental and theoretical results unravel that the charge transfer on the alloy clusters modulated by the defective substrates (NiFe LDHs), which synergistically optimizes the adsorption energy of the reaction intermediates. The electrocatalyst exhibits an ultra-low overpotential of 81 and 243 mV at the current density of 100 mA cm^-2for hydrogen evolution and oxygen evolution, respectively. Furthermore, the overall water splitting indicates that PtFeNi alloys/NiFe LDHs presents an ultra-low overpotential of 265 and 406 mV to reach the current density of 10 and 300 mA cm^-2, respectively. It proves that the PtFeNi alloys/NiFe LDHs catalyst is an excellent dual-function electrocatalyst for water splitting and promising for industrialization. This work provides a new electrochemical approach to construct the alloy heterostructure. The prepared heterostructures act as an ideal platform to investigate the charge re-distribution behavior and to improve the electrocatalytic activity.

Key words: Hydrogen evolution reaction, Oxygen evolution reaction, Overall water splitting, Alloy heterostructure, Layered double hydroxides

Gen Huang, Yingying Li, Ru Chen, Zhaohui Xiao, Shiqian Du, Yucheng Huang, Chao Xie, Chungli Dong, Haibo Yi, Shuangyin Wang. Electrochemically formed PtFeNi alloy nanoparticles on defective NiFe LDHs with charge transfer for efficient water splitting[J]. Chinese Journal of Catalysis, 2022, 43(4): 1101-1110.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63926-8

https://www.cjcatal.com/EN/Y2022/V43/I4/1101

Figures/Tables 6

Fig. 1. (a) Schematic representation for the synthesis process of PtFeNi alloys on defective LDHs; SEM image of NiFe LDHs (b) and NiFe LDHs-Ar (c); TEM image of NiFe LDHs (d) and NiFe LDHs-Ar (e); (f) TEM image and the inset HR-TEM image of PtFeNi/NiFe LDHs; (g) EDS mapping image of PtFeNi alloys on NiFe LDHs for PtFeNi/NiFe LDHs-2500.

Fig. 2. (a) Pt 4f XPS spectrum of PtFeNi/NiFe LDHs-2500; (b) Pt L3-edge XANES spectra of PtFeNi/NiFe LDHs-2500, Pt foil and PtO2; (c) the k2-weighted Fourier transform EXAFS spectra of Pt for PtFeNi/NiFe LDHs-2500, Pt foil and PtO2; (d) the Fe 2p XPS spectrum of PtFeNi/NiFe LDHs-2500; (e) Fe K-edge XANES spectra of PtFeNi/NiFe LDHs-2500, Fe foil, α-Fe2O3 and FeO; (f) the k2-weighted Fourier transform EXAFS spectra of PtFeNi/NiFe LDHs-2500, Fe foil, FeO and Alfa-Fe2O3.

Fig. 3. Polarization curves (a) and Tafel plots (b) of the NiFe LDHs-Ar, 20% Pt/C, PtFeNi/NiFe LDHs-2500 and PtFeNi/NiFe LDHs-3500 for the HER; (c) the electrochemical impedance spectroscopy of PtFeNi/NiFe LDHs-2500 and NiFe LDHs-Ar; (d) the initial and after i~t 24 h stability test (the internal illustration) polarization curves of the PtFeNi/NiFe LDHs-2500 for the HER performed at current density of -75 mA cm-2(-0.3 V vs. RHE).

Fig. 4. (a) Polarization curves of NiFe LDHs-Ar, PtFeNi/NiFe LDHs-2500, 20% Pt/C and commercial IrO2 for OER; (b) the cyclic voltammetry of PtFeNi/NiFe LDHs-2500 between 1.23?1.47 V; (c) the electrochemical impedance spectroscopy of NiFe LDHs-Ar and PtFeNi/NiFe LDHs-2500 under OER condition; (d) the initial and after i~t 24 h stability test (the internal illustration) polarization curves of the PtFeNi/NiFe LDHs-2500 for the OER performed at current density of 100 mA cm-2(1.65 V vs. RHE).

Fig. 5. Schematic diagram of overall water splitting (a) and the polarization curves (b) of IrO2 (+) || 20% Pt/C (-) and PtFeNi/NiFe LDHs-2500 (+) & (-) of overall water splitting.

Fig. 6. Optimized structure (a) and schematic diagram (b) of differential charge density of PtFeNi alloy/NiFe LDHs. Iso-surface value is 0.004 e/bohr3. (Yellow and cyan regions represent electron accumulation and depletion, respectively; for the spheres in model, light purple is nickel, brown is iron, gray is platinum, red is oxygen and white is hydrogen); (c) Bader charge analysis of PtFeNi alloy/NiFe LDHs ( The positive values means the atom gets electron) and (d) (PDOS (the Fermi level is set to 0 eV); (e) free energy diagram of HER at Fe, Ni and Pt active sites and (f) OER at different potentials on the active sites of Fe on PtFeNi alloy/NiFe LDHs.

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