Metal/antiperovskite metal nitride composites Ag/AgNNi3 as novel efficient electrocatalysts for hydrogen evolution reaction in alkaline media

doi:10.1016/j.jmst.2021.09.059

Abstract

Abstract:

Searching for effective hydrogen evolution reaction (HER) electrocatalysts is crucial for water splitting. Transition metal nitrides (TMNs) are very attractive potential candidates since of high electrical conductivity, robust stability, element rich and high activity. Antiperovskite metal nitrides provide chemical flexibility since two different types of transition metal elements are contained, allowing partial substitution both for A- and M-sites. Herein, we report a novel antiperovskite metal nitride Ag_xNi_1-_xNNi₃ (0 ≤ x ≤ 0.80) thin film used as highly effective HER electrocatalysts. Pure phase antiperovskite nitride can be successfully obtained for Ag_xNi_1-_xNNi₃ with x less than 0.80. The Ag_0.76Ni_0.24NNi₃ towards HER shows an overpotential of 122 mV at 10 mA cm^-2 in alkaline media. Furthermore, considering the role of Ag for adsorbing hydroxyl groups, chemical engineering has been carried out for designing metal/antiperovskite nitride Ag/Ag_xNi_1-_xNNi₃ composite electrocatalysts. The 0.18 Ag/Ag_0.80Ni_0.20NNi₃ electrocatalyst shows a mere 13 and 81 mV of overpotential to reach 1 and 10 mA cm^-2, respectively, showing high durability in alkaline media. These results will provide a novel type of HER catalysts based on antiperovskite metal nitrides and a strategic design for metal/antiperovskite metal nitride composite electrocatalysts for HER in alkaline media.

Key words: Hydrogen evolution reaction, Antiperovskite, Metal nitride, Composite catalyst

Lili Zhu, Bingbing Yang, Ziqiang Wu, Changdian Li, Han Li, Hui Li, Yanan Huang, Xiaoguang Zhu, Xuebin Zhu, Yuping Sun. Metal/antiperovskite metal nitride composites Ag/AgNNi₃ as novel efficient electrocatalysts for hydrogen evolution reaction in alkaline media[J]. J. Mater. Sci. Technol., 2022, 112: 222-229.

Figures/Tables 7

Fig. 1. (a) A scheme for the fabrication of the AgxNi1-xNNi3 (0 ≤ x ≤ 0.80) on the ITO substrates by CSD. (b) A physical picture for the thin film of AgxNi1-xNNi3 (0 ≤ x ≤ 0.80), the area of the film is 1 cm × 1 cm. (c) The unit cell structure of the antiperovskite nitride AgxNi1-xNNi3 (0 ≤ x ≤ 0.80).

Fig. 2. (a) XRD patterns of Ag0.57Ni0.43NNi3, Ag0.76Ni0.24NNi3, 0.08 Ag/Ag0.80Ni0.20NNi3, 0.18 Ag/Ag0.80Ni0.20NNi3 and 0.25 Ag/Ag0.80Ni0.20NNi3. (b-d) AFM images of Ag0.57Ni0.43NNi3, 0.18 Ag/Ag0.80Ni0.20NNi3 and 0.25 Ag/Ag0.80Ni0.20NNi3, respectively.

Fig. 3. TEM (a) and HRTEM (b) results of Ag0.76Ni0.24NNi3. TEM (c, d), HRTEM (e), HAADF-STEM (f) and EDX element mapping (g-j) results of 0.18 Ag/Ag0.80Ni0.20NNi3.

Fig. 4. Electrocatalytic HER performances for all prepared samples measured in 1 mol L-1 KOH electrolyte. (a) LSV results for Ag0.57Ni0.43NNi3, Ag0.76Ni0.24NNi3, 0.08 Ag /Ag0.80Ni0.20NNi3, 0.18 Ag/Ag0.80Ni0.20NNi3, 0.25 Ag/Ag0.80Ni0.20NNi3 and the commercial 20 wt.% Pt/C at a scan rate of 5 mV s-1. (b) Tafel plots derived from the LSV curves. (c) Comparisons of the ƞonset, ƞ10, ƞ50 and Tafel slope. (d) Cdl results for the estimation of ESCA. (e) EIS of 0.18 Ag/Ag0.80Ni0.20NNi3 at different overpotentials and the inset is the equivalent electrical circuit to model HER process. (f) LSV results of 0.18 Ag/Ag0.80Ni0.20NNi3 before and after 3000 CV cycles, and the inset is the chronoamperometry results for the 0.18 Ag/Ag0.80Ni0.20NNi3 at the overpotential of 81 mV for 12 h. All results are collected without iR compensation.

Table 1. Values of Cdl and ESCA for all derived Ag/AgxNi1-xNNi3 (0 ≤ x ≤ 0.80).

Catalysts	C_dl (mF cm^-2)	ESCA (cm²)
Ag_0.57Ni_0.43NNi₃	1.15	28.75
Ag_0.76Ni_0.24NNi₃	0.96	24.00
0.08 Ag/Ag_0.80Ni_0.20NNi₃	1.25	31.25
0.18 Ag/Ag_0.80Ni_0.20NNi₃	3.98	99.50
0.25 Ag/Ag_0.80Ni_0.20NNi₃	0.82	20.50

Table 2. Summary of HER activities of all derived Ag/AgxNi1-xNNi3 (0 ≤ x ≤ 0.80).

Catalysts	ƞ_onset(mV)	ƞ₁₀(mV)	ƞ₅₀(mV)	Tafel(mV dec^-1)	ESCA(cm²)	R_ct(Ω)	j₀(μA cm^-2)
Ag_0.57Ni_0.43NNi₃	30	135	385	81	28.75	3.68	0.11
Ag_0.76Ni_0.24NNi₃	36	122	263	78	24.00	2.26	0.12
0.08 Ag/Ag_0.80Ni_0.20NNi₃	15	85	194	62	31.25	6.17	0.15
0.18 Ag/Ag_0.80Ni_0.20NNi₃	13	81	171	59	99.50	1.31	0.30
0.25 Ag/Ag_0.80Ni_0.20NNi₃	92	162	258	62	20.50	3.62	0.01

Fig. 5. (a) XRD patterns of the pristine 0.18 Ag/Ag0.80Ni0.20NNi3 sample and the 0.18 Ag/Ag0.80Ni0.20NNi3 sample after stability test. (b, c) SEM results of the pristine 0.18 Ag/Ag0.80Ni0.20NNi3 and the 0.18 Ag/Ag0.80Ni0.20NNi3 sample after stability test, the red circles mark the particles. (d) Dissociation mechanism for H2O bonded to metal atom Ag and ANNN. (e) Schematic illustration of the electrocatalytic process during the alkaline HER process.

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Metal/antiperovskite metal nitride composites Ag/AgNNi₃ as novel efficient electrocatalysts for hydrogen evolution reaction in alkaline media

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