A MOF derived hierarchically porous 3D N-CoPx/Ni2P electrode for accelerating hydrogen evolution at high current densities

doi:10.1016/S1872-2067(21)63982-7

Abstract

Abstract:

Hydrogen evolution reaction is a critical reaction in water splitting for hydrogen production. However, developing effective and stable non-noble-metal electrocatalysts which work well at high current densities demanded by industry still remain great challenge. Herein, taking advantage of the highly tunable metal-organic framework (MOF) templates, nitrogen doped binary transition metal phosphides electrocatalysts (N-CoP_x/Ni₂P) with three-dimensional (3D) conductive network structure were successfully synthesized. The 3D open porous channels could expose more catalytically active sites; nitrogen doping and the synergistic effect between CoP and Ni₂P can increase the electron density of Co atoms at active sites, further optimizing the Gibbs free energy of hydrogen (ΔG_H*) and water (ΔG_H2O*). As a result, the obtained N-CoP_x/Ni₂P catalyst exhibits extraordinary electrocatalytic activity in a wide pH range. Especially, it requires an extremely low overpotential of 152 mV to deliver a high current density of 650 mA cm^-2in alkaline media. This work may shed some light on the rational design of cheap electrocatalysts and electrode materials that work well at high current densities.

Key words: Hydrogen evolution reaction, MOF templates, N-CoP_x/Ni₂P, Three-dimensional conductive network, High current density

Lan Wang, Ning gong, Zhou Zhou, Qicheng Zhang, Wenchao Peng, Yang Li, Fengbao Zhang, Xiaobin Fan*. A MOF derived hierarchically porous 3D N-CoP_x/Ni₂P electrode for accelerating hydrogen evolution at high current densities[J]. Chinese Journal of Catalysis, 2022, 43(4): 1176-1183.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63982-7

https://www.cjcatal.com/EN/Y2022/V43/I4/1176

Figures/Tables 5

Scheme 1. Schematic illustration shows the fabrication process for N-CoPx/Ni2P nanowall through converting the Co-MOF upon phosphorization.

Fig. 1. (a,b) SEM images of the Co-MOF/NF; SEM (c) and TEM (d-g) images of the N-CoPx/Ni2P; (h-k) EDS elemental mappings of N-CoPx/Ni2P.

Fig. 2. High resolution XPS spectra of Co 2p (a), Ni 2p (b), P 2p (c), and N 1s (d) for N-CoPx/Ni2P and CoPx/Ni2P.

Fig. 3. (a,b) HER polarization curves and the corresponding Tafel plots of N-CoPx/Ni2P, CoPx/Ni2P and Ni2P in 0.5 mol/L H2SO4, 1.0 mol/L PBS and 1.0 mol/L KOH with iR-corrected; (c) The corresponding HER overpotential required for j = 10, 100, 200 mA cm-2; (d) The corresponding Cdl values. (e) iR-corrected polarization curves recorded before and after 10000 accelerated degradation test CV cycles; (f) Time dependence of the current density for N-CoPx/Ni2P at static overpotentials of 63 mV (in 0.5 mol/L H2SO4), 80 mV (in 1.0 mol/L PBS) and 53 mV (in 1.0 mol/L KOH) for 24 h; (g) TOFs for Ni2P, CoPx/Ni2P, and N-CoPx/Ni2P at an overpotential of 100 mV in 1.0 mol/L KOH; (h) Theoretical and measured amount of H2 during electrolysis at 30 mA cm-2in 1.0 mol/L KOH; (i) Comparison of the overpotential and Tafel slope of N-CoPx/Ni2P with other recently reported TMP catalysts in 1.0 mol/L KOH.

Fig. 4. (a) iR-corrected HER polarization curves of N-CoPx/Ni2P in 0.5 mol/L H2SO4, 1.0 mol/L PBS and 1.0 mol/L KOH at high current density 650 mA cm-2; (b) Time dependence of the current density (200 mA cm-2) for N-CoPx/Ni2P at static overpotentials of 138 mV (in 0.5 mol/L H2SO4), 264 mV (in 1.0 mol/L PBS) and 134 mV (in 1.0 mol/L KOH) for 24 h; (c) Top view of the optimized heterogeneous structure of H and H2O adsorption on N-CoP/Ni2P surface. Color denotation: pink (Co), brown (Ni), blue (P), cyan-blue (N), red (O) and white (H); (d) The calculated HER free-energy; (e) Water adsorption energy.

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A MOF derived hierarchically porous 3D N-CoP_x/Ni₂P electrode for accelerating hydrogen evolution at high current densities

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