Hierarchical NiMoP2-Ni2P with amorphous interface as superior bifunctional electrocatalysts for overall water splitting

doi:10.1016/j.jmst.2020.09.046

Abstract

Abstract:

Producing highly efficient bifunctional catalyst for the generation of hydrogen and oxygen through overall water splitting is an emerging direction in electrocatalysis. Herein, a dandelion-like hierarchical NiMoP₂-Ni₂P (nanowire/nanoparticle) heterostructure was synthesized for efficient electrochemical water splitting. The NiMoP₂-Ni₂P heterostructures grown on carbon cloth as a freestanding integrated electrode exhibited excellent oxygen evolution reaction (OER) activity and hydrogen evolution reaction (HER) activities with low overpotentials (258 mV and 53 mV to reach 10 mA cm^-2 for the OER and HER, respectively), and small Tafel slope (45 mV dec^-1 and 58 mV dec^-1 for the OER and HER, respectively). Moreover, the NiMoP₂-Ni₂P heterostructure can act as both anode and cathode catalysts for overall water splitting with low overall potential of 1.48 V at 10 mA cm^-2. Density functional theory (DFT) combined with structural probes suggests that the amorphous heterogeneous interfaces play an essential role in enhanced catalytic performance.

Key words: Bimetallic phosphide, Amorphous interface, Adsorption energy, Hydrogen evolution reaction, Oxygen evolution reaction, Water splitting

Gaoqi Tian, Songrui Wei, Zhangtao Guo, Shiwei Wu, Zhongli Chen, Fuming Xu, Yang Cao, Zheng Liu, Jieqiong Wang, Lei Ding, Jinchun Tu, Hao Zeng. Hierarchical NiMoP₂-Ni₂P with amorphous interface as superior bifunctional electrocatalysts for overall water splitting[J]. J. Mater. Sci. Technol., 2021, 77: 108-116.

Figures/Tables 8

Fig. 1. Schematic illustration of the synthesis process for NiMoP2-Ni2P/CC and the design of NiMoP2-Ni2P/CC electrocatalysts as a bifunctional catalyst for OER and HER.

Fig. 2. (a) XRD patterns of NiMoP2-Ni2P/CC heterostructure. (b-d) High-resolution XPS spectra of the (b) Ni 2p, (c) Mo 3d, and (d) P 2p of NiMoP2-Ni2P/CC heterostructures and NiMoP2/CC.

Fig. 3. (a, b) SEM images of NiMo(OH)x/CC, and (c, d) NiMoP2-Ni2P/CC. (e) TEM micrographs of NiMoP2-Ni2P/CC. (f) HRTEM image of NiMoP2-Ni2P/CC. (g) HRTEM image of partial region enlarged in (f). (h) STEM and EDX elemental mapping images of Ni, Mo and P for NiMoP2-Ni2P/CC.

Fig. 4. (a) LSV polarization curves of OER and HER for Pt-C/CC, NiMoP2-Ni2P/CC, NiMoP2/CC, Ni2P/CC, NiMo(OH)x/CC, carbon fibers; (b) the histogram of OER overpotential and Tafel plots for NiMoP2-Ni2P/CC, NiMoP2/CC, Ni2P/CC, NiMo(OH)x/CC; (c) the histogram of HER overpotential and Tafel plots for Pt-C/CC, NiMoP2-Ni2P/CC, NiMoP2/CC, Ni2P/CC, NiMo(OH)x/CC, carbon fibers. (d) OER and (e) HER chronoamperometry curves of NiMoP2-Ni2P/CC for 20 h at 10 mA cm-2, 30 mA cm-2, 50 mA cm-2, respectively.

Fig. 5. (a) LSV polarization curves of the NiMoP2-Ni2P/CC (+) // NiMoP2-Ni2P/CC (-) couple, (b) chronoamperometry curve of NiMoP2-Ni2P/CC for 20 h.

Table 1. Comparisons of the water splitting activities of various bifunctional catalysts (η: overpotential at the current density of 10 mA cm-2).

Catalysts	η(V)	Electrolyte
NiMoP₂-Ni₂P/CC (This work)	1.48	1.0 M KOH
Ni₁Mo₁P NSs@MCNTs [29]	1.60	1.0 M KOH
MoP@Ni₃P/NF [62]	1.67	1.0 M KOH
Ni₂P nanoparticles [63]	1.63	1.0 M KOH
Ni₅P₄[64]	1.70	1.0 M KOH
NiS@Ni₂P₂S₆/NF [65]	1.64	1.0 M KOH
MoP/Ni₂P/NF [66]	1.55	1.0 M KOH
Co₅Mo₁P NSs@NF\|\|Co₅Mo₁O NSs@NF [67]	1.57	1.0 M KOH
MoNiN [6]	1.563	1.0 M KOH
N-NiMoO₄/NiS₂nanowires/nanosheets [14]	1.60	1.0 M KOH
Ni₂P/Cu₃P [38]	1.60	1.0 M KOH
MoS₂-Ni₃S₂particles [40]	1.56	1.0 M KOH

Fig. 6. (a-c) The schematic diagram of the NiMoP2, Ni2P, and NiMoP2-Ni2P crystal structures; (d) distribution of the charge density on the interface of the heterostructure; (e) the density of state (DOS) results of heterostructures and single phases; (f) the calculated free energy diagram for the HER on various atoms of NiMoP2-Ni2P/CC different position and various atoms of NiMoP2, Ni2P.

Table 2. The value of electron transfer for Ni, Mo elements on the amorphous interface.

Atom	NiMoP₂ electrons value (eV)	NiMoP₂-Ni₂P electrons value (eV)	Electrons transfer value (eV)
Ni	9.9139	9.9879	0.0740
Mo	5.5409	5.3798	-0.1611

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Hierarchical NiMoP₂-Ni₂P with amorphous interface as superior bifunctional electrocatalysts for overall water splitting

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