氮/硫双掺多孔碳负载Fe9S10纳米粒子的氧还原电催化性能

doi:10.7503/cjcu20170728

摘要/Abstract

摘要：

通过简单热解后酸刻蚀方法制备了一种新型的氮/硫双掺的多孔碳负载Fe₉S₁₀纳米粒子(Fe₉S₁₀/NSPC)复合材料. 采用X 射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)和X射线光电子能谱(XPS)等方法对催化剂的结构形貌和化学成分进行了表征, 用旋转圆盘(RDE)和旋转环盘(RRDE)技术对其氧还原催化性能进行了探究. 结果表明, Fe₉S₁₀/NSPC-900(900 ℃为热解温度)在碱性介质中展现出了较高的氧还原催化活性及良好的稳定性和优异的抗甲醇性能.

关键词: Fe₉S₁₀纳米粒子, 氮/硫双掺多孔碳, 氧还原反应, 电催化剂

Abstract:

A novel hybrid material(Fe₉S₁₀/NSPC) comprising of Fe₉S₁₀ nanocrystals and nitrogen/sulphur-codoped porous carbon(NSPC) was synthesized via a facile pyrolysis procedure followed by an acid leaching process. X-Ray diffraction(XRD), scanning electron microscope(SEM), transmission electron microscope(TEM) and X-ray photoelectron spectroscopy(XPS) techniques were used to characterized the crystal phase structure, morphology and chemical composition of the as-obtained catalysts, respectively. In addition, rotating disk electrode(RDE) and rotating ring-disk electrode(RRDE) techniques were conducted to evoluate the electrocatalytic activity of the catalysts for oxygen reduction reaction(ORR). The results show that the Fe₉S₁₀/NSPC-900(where 900 ℃ represents the pyrolysis temperature) exhibits high ORR activity, good stability and excellent methanol resistance in an alkaline medium.

Key words: Fe₉S₁₀ nanocrystals, N, S-Codoped porous carbon, Oxygen reduction reaction, Electrocatalyst

中图分类号:

O646

TrendMD:

王秀利, 何兴权. 氮/硫双掺多孔碳负载Fe₉S₁₀纳米粒子的氧还原电催化性能. 高等学校化学学报, 2018, 39(7): 1524.

WANG Xiuli, HE Xingquan. Electrocatalytic Performance of Fe₉S₁₀ Nanoparticles Loaded Nitrogen and Sulphur Codoped Porous Carbon for Oxygen Reduction Reaction^†. Chem. J. Chinese Universities, 2018, 39(7): 1524.

图/表 11

Fig.1 SEM images of Fe9S10/NSC-900(A) and Fe9S10/NSPC-900(B)

Fig.2 TEM(A, C) and HRTEM(B, D) images of Fe9S10/NSC-900(A, B) and Fe9S10/NSPC-900(C, D)

Fig.3 XRD patterns of Fe9S10/NSC-900(A) and Fe9S10/NSPC-T(T=700, 800, 900, 1000 ℃)(B)

Fig.4 XPS survey spectra(A) and high-resolution XPS spectra of N1s(B), S2p(C) and Fe2p(D) of Fe9S10/NSPC-900

Fig.5 Nitrogen adsorption-desorption isotherms(A) and pore size distribution(B) of Fe9S10/NSPC-T and Fe9S10/NSC-900

Table 1 Structural parameters of different catalysts

Sample	Surface area/(m²·g^-1)	Pore volume, V/(cm³·g^-1)	Pore diameter, D/nm
Fe₉S₁₀/NSPC-700	208.1	0.55	10.60
Fe₉S₁₀/NSPC-800	331.3	0.68	8.24
Fe₉S₁₀/NSPC-900	398.9	1.64	16.48
Fe₉S₁₀/NSPC-1000	187.4	0.44	9.40
Fe₉S₁₀/NSC-900	261.9	0.65	9.96

Fig.6 Raman spectra of Fe9S10/NSPC-T[T=700 ℃(a), 800 ℃(b), 900 ℃(c), 1000 ℃(d)] and Fe9S10/NSC-900(e)

Fig.7 CV curves of Fe9S10/NSPC-900 in N2, O2 saturated 0.1 mol/L KOH at a scan rate of 100 mV/s(A), LSV curves of Fe9S10/NSPC-900 at different rotation in O2 saturated 0.1 mol/L KOH with a scan rate of 10 mV/s(B), LSV polarization curves of Fe9S10/NSPC-T(C) and Fe9S10/NSC-900, Fe9S10/NSPC-900, NSPC-900 and Pt/C(D)

Fig.8 Corresponding K-L plots of ORR for Fe9S10/NSPC-900 catalyst(A) and tafel plots of Fe9S10/NSPC-900 and Pt/C in 0.1 mol/L KOH(B)

Fig.9 Rotating ring disk electrode(RRDE) measurements of Fe9S10/NSPC-900(a) and Pt/C(b) in 0.1 mol/L KOH(A), peroxide percentage and electron transfer number(inset) of Fe9S10/NSPC-900(a) and Pt/C(b) at different potentials(B)

Fig.10 Chronoamperometric curves of Fe9S10/NSPC-900(a) and Pt/C(b) in 0.1 mol/L KOH solution saturated with O2 at a rotation speed of 1600 r/min(A) and chronoamperometric response for ORR on Fe9S10/NSPC-900(a) and Pt/C(b) with the scan rate of 10 mV/s in 0.1 mol/L KOH solution saturated with O2 with 3 mol/L methanol added after 300 s(B)

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氮/硫双掺多孔碳负载Fe₉S₁₀纳米粒子的氧还原电催化性能

Electrocatalytic Performance of Fe₉S₁₀ Nanoparticles Loaded Nitrogen and Sulphur Codoped Porous Carbon for Oxygen Reduction Reaction^†

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