磷化镍/氮硫双掺杂石墨烯复合材料的制备及电催化析氢性能

doi:10.7503/cjcu20200161

摘要/Abstract

摘要：

采用水热法合成了具有高活性的磷化镍纳米晶(Ni₂P), 并合成了氮、硫共掺杂石墨烯负载磷化镍纳米催化剂(Ni₂P/NSRGO). 对该催化剂的结构和形貌进行了表征, 并研究其电催化析氢性能. 电化学测试结果表明, Ni₂P/NSRGO复合电催化剂的析氢性能优于Ni₂P/RGO催化剂, 具有较小的Tafel斜率(35 mV/dec)、较低的过电位(η₁₀=140 mV)和良好的稳定性.

关键词: 析氢反应, 电催化剂, 磷化镍纳米晶, 氮硫双掺杂

Abstract:

Developing new type of electrolyzed water catalysts is very important. In this work, nickel phosphide nanocrystals supported on N, S co-doped reduced graphene oxide(Ni₂P/NSRGO) as a high activity catalyst was synthesized by the simple hydrothermal process. The graphene can anchor nickel phosphide and improve catalytic performance. The results of electrochemical test showed that the Ni₂P/NSRGO composite electrocatalyst showed better hydrogen evolution performance than Ni₂P/NRGO and Ni₂P/RGO catalysts, indicating the addition of N and S has a positive effect on the improvement of hydrogen evolution performance. The Ni₂P/NSRGO nanocrystals catalyst shows excellent performance with a small Tafel slope of 35 mV/dec, longterm durability and a low overpotential(η₁₀=140 mV) in 0.5 mol/L H₂SO₄ for the hydrogen evolution reaction(HER).

Key words: Hydrogen evolution reaction, Electrocatalyst, Nickel phosphide nanocrystal, Nitrogen-sulfur double-doping

中图分类号:

O646
O613.6

TrendMD:

赵国庆, 袁钊, 王连, 郭卓. 磷化镍/氮硫双掺杂石墨烯复合材料的制备及电催化析氢性能. 高等学校化学学报, 2020, 41(7): 1575.

ZHAO Guoqing, YUAN Zhao, WANG Lian, GUO Zhuo. Preparation of Ni₂P/N, S co-Doped Reduced Graphene Oxide Composites and Their Electrocatalytic Properties for Hydrogen Evolution^†. Chem. J. Chinese Universities, 2020, 41(7): 1575.

图/表 8

Scheme 1 Schematic illustration of experimental procedures of NSRGO(A) and NixP/NSRGO(B)

Fig.1 XRD patterns of GO(a), NSRGO(b) and RGO(c)(A) and Ni2P/RGO-1(a), Ni2P/RGO-2(b), Ni2P/RGO-3(c), Ni2P/RGO-4(d) and Ni2P/NSRGO-2(e)(B)

Fig.2 SEM images of RGO(A), NSRGO(B), Ni2P(C), Ni2P/RGO-1(D), Ni2P/RGO-2(E), Ni2P/RGO-3(F), Ni2P/RGO-4(G) and Ni2P/NSRGO-2(H, I) catalysts

Fig.3 TEM images of Ni2P/RGO-2(A), Ni2P/NSRGO-2(B, C) and HRTEM image of Ni2P/NSRGO-2(D) catalysts

Fig.4 XPS survey spectra(A), and high resolution spectra of C1s(B), Ni2p(C), P2p(D), N1s(E) and S2p(F) of Ni2P/RGO-2 and Ni2P/NSRGO-2

Fig.5 LSV polarzation curves(A), Tafel plots(B), EIS(C) and histograms(D) for different electrocatalysts a. RGO; b. NSRGO; c. Ni2P/RGO-1; d. Ni2P/RGO-2; e. Ni2P/RGO-3; f. Ni2P/RGO-4; g. Ni2P/NSRGO-2. Inset of (C): the equivalent circuit diagram used to fit the impedance spectra.

Table 1 Comparison of Ni2P-based HER electrocatalysts in acidic media

Catalyst	Electrolyte	η₁₀/mV	Tafels lope/(mV·dec^-1)	Ref.
Ni₂P@C/G	0.5 mol/L H₂SO₄	285	44	[23]
Ni2P/NRGO	0.5 mol/L H₂SO₄	80	93.1	[24]
Ni₂P/NPPC	0.5 mol/L H₂SO₄	159	74	[25]
Ni₂P/CC	0.5 mol/L H₂SO₄	119	50	[26]
Ni₂P/C	0.5 mol/L H₂SO₄	94	113.2	[27]
NFP@NG	0.5 mol/L H₂SO₄	250	91	[28]
Ni₂P/Ni	0.5 mol/L H₂SO₄	140	68	[29]
Ni₂P@C-400	0.5 mol/L H₂SO₄	186	85	[30]
Ni₂P/NSRGO-2	0.5 mol/L H₂SO₄	140	35	This work

Fig.6 LSV polarization curves of Ni2P/NSRGO-2 after initial and 1000 cycles(A) and timing current test(B)

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