A co-coordination strategy to realize janus-type bimetallic phosphide as highly efficient and durable bifunctional catalyst for water splitting

doi:10.1016/j.jmst.2020.10.009

Abstract

Abstract:

In this work, a Janus-type dual-ligand metal-organic frameworks derived bimetallic (Fe, Co)P nanoparticles embedded carbon nanotube (CNT) skeleton (DLD-FeCoP@CNT) is presented and synthesized via a facile “co-coordination synthesis” strategy. The DLD-FeCoP@CNT hybrid shows much better performances for OER and HER with much lower Tafel slope of 39.6 (57.1) mV dec^-1, an overpotential of 286 (166) mV @10 mA cm^-2 and better stability for OER (HER) in 1 M KOH. Being both cathode and anode for water splitting, it requires only a low voltage of 1.67 V to obtain 10 mA cm^-2 with nearly 100% faradaic efficiency, which is close to Pt/C//RuO₂ cell. Density functional theory calculations based on the bimetallic phosphide (Fe_0.3Co_0.7P) model reveal that, compared with the monometallic FeP or CoP, the enhanced catalytic activities of Fe_0.3Co_0.7P is mainly manifested in its free energy of H adsorption ($\Delta {{G}^{{{\text{H}}^{*}}}}$) closer to zero, larger binding strength for H₂O and higher electrical conductivity.

Key words: Bimetallic phosphide, Bifunctional catalyst, Overall water splitting, DFT calculation

Bin Wang, Yuanfu Chen, Qi Wu, Yingjiong Lu, Xiaojuan Zhang, Xinqiang Wang, Bo Yu, DongXu Yang, Wanli Zhang. A co-coordination strategy to realize janus-type bimetallic phosphide as highly efficient and durable bifunctional catalyst for water splitting[J]. J. Mater. Sci. Technol., 2021, 74: 11-20.

Figures/Tables 8

Fig. 1. Schematic illustration of the preparation of Co-Fe-PBA/CNT and CoFeP/CNT.

Fig. 2. (a) XRD pattern, (b) Raman spectrum and (c) EDS spectrum of the DLD-FeCoP@CNT.

Fig. 3. (a) SEM image, (b) TEM, (c, d) HRTEM images, (c1-c2, d1-d2) zoomed views of the areas marked in the (c) and (d), respectively, (e-j) elemental mapping of the DLD-FeCoP@CNT.

Fig. 4. XPS spectra of the DLD-FeCoP@CNT: (a) C 1s, (b) P 2p, (c) Co 2p and (d) Fe 2p.

Fig. 5. (a) Polarization curves and (b) Tafel plots. The comparison of OER activity (c) overpotential at 10 mA cm-2 and (d) Tafel slope of the DLD-FeCoP@CNT, SLD-CoP@CNT, SLD-FeP@CNT and RuO2 in 1 M KOH.

Fig. 6. (a) Polarization curves and (b) Tafel plots. The comparison of HER activity (c) overpotential at 10 mA cm-2 and (d) Tafel slope of the DLD-FeCoP@CNT, SLD-CoP@CNT, SLD-FeP@CNT and Pt/C in 1 M KOH.

Fig. 7. DFT calculations of CoP, FeP and Fe-CoP for HER: (a) atomic structure of a model Fe-doped CoP (111) surface, (b) HER free energy diagrams for the P-, Co- and Fe-sites on pristine and Fe-doped CoP (111) surfaces and FeP (011) surface, (c) spin-polarized density of states of plots. The Fermi level (dashed line) is set as zero.

Fig. 8. Performance of overall water electrolysis: (a) polarization curves of the DLD-FeCoP@CNT for HER and OER, (b) polarization curves of water electrolysis respectively using the DLD-FeCoP@CNT, SLD-CoP@CNT, SLD-FeP@CNT and commercial material as electrocatalysts both for HER and OER in a two-electrode configuration with a scan rate of 1 mV s-1, (c) the theoretical and experimental H2 or O2 vs time of the DLD-FeCoP@CNT at 1.67 V vs RHE, (d) chronoamperometry (i-t) curves of the DLD-FeCoP@CNT based electrode during overall water splitting at the applied potential of 1.74 V. The inset digital photographs in (c) and (d) are the corresponding partially amplified of glassy carbon electrode for observation of the gas evolution from the electrodes during water electrolysis. The inset plots in (d) is the curves of the raw DLD-FeCoP@CNT and electrolyte immersion treated DLD-FeCoP@CNT for water electrolysis.

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