Synthesis of Hollow PtNi/Graphene Cellular Monolith Catalysts and Their Electrochemical Performance†

doi:10.7503/cjcu20160264

Abstract

Abstract:

Hollow platinum nickel/graphene cellular monolith(PtNi/GCM) electrocatalysts were synthesized via a two-step method of sonochemical-assisted reduction and gelatinization reaction. X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS), scanning electronic microscopy(SEM) and transmission electron microscopy(TEM) were employed to characterize the structures, compositions and morphologies of as-prepared catalysts. The activity and stability of the catalysts for oxygen reduction reaction(ORR) were studied with electrochemical workstation and rotating disk electrode(RDE). The results show that different molar ratios of Pt to Ni in the precursor have great influence on the porous structure, particle morphology and dispersion of the catalyst. In particular, the PtNi/GCM electrocatalyst that was prepared with Pt/Ni molar ratio of 1∶1 in the precursor has the desirable structure and was uniformly distributed. The PtNi/GCM showed the excellent electrocatalytic activities and durability toward ORR. The mass and specific activities at half-wave potential of 0.494 V were 1.09 A/mg_Pt and 1.02 mA/cm², respectively, which were 5.4 and 3.5 times those of commercial Pt/C(0.20 A/mg_Pt and 0.29 mA/cm²).

Key words: Graphene cellular monolith, PtNi nanoparticles, Hollow structure, Oxygen reduction reaction, Electrocatalyst

CLC Number:

O646
O613

TrendMD:

XU Kai,LI Yi,ZHAO Nan,DU Wenxiu,ZENG Weiwei,GAO Shuai,CHENG Xiaonong,YANG Juan. Synthesis of Hollow PtNi/Graphene Cellular Monolith Catalysts and Their Electrochemical Performance^†[J]. Chem. J. Chinese Universities, 2016, 37(8): 1476.

Figures/Tables 10

Fig.1 Schematic showing the synthesis mechanism of alloyed PtNi nanoparticles supported by GCM using sonochemical-assisted synthesis and gelatinization method

Fig.2 XRD patterns of Pt/GCM(a), PtNi/GCM(b), PtNi2/GCM(c) and PtNi3/GCM(d)

Fig.3 C1s XPS spectra of PtNi/rGO(A) and PtNi/GCM(B), Pt4f(C) and Ni2p(D) XPS spectra of PtNi/GCM Inset of (A) shows the C1s XPS of GO.

Fig.4 SEM images of Pt/GCM(A,B), PtNi/GCM(C,D), PtNi2/GCM(E,F) and PtNi3/GCM(G,H)

Fig.5 Nitrogen adsorption-desorption isotherms(A) and pore size distributions(B) of PtNi/GCM(a) and PtNi3/GCM(b)

Fig.6 TEM images of Pt/GCM(A,B), PtNi/GCM(C,D), PtNi2/GCM(E,F), and PtNi3/GCM(G,H) Inset of (D) is HRTEM image of single PtNi.

Fig.7 CVs(A) and ORR polarization curves(B) of PtNi/GCM(a) and commercial Pt/C(b) catalysts

Fig.8 Comparison of ORR mass activity(A) and specific activity(B) of the PtNi/GCM and ommercial Pt/C catalysts

Fig.9 ORR polarization curves of commercial Pt/C(A) and PtNi/GCM(B) catalysts before(a) and after(b) 30000 potential cycles

Table 1 Comparison of durability(after 30000 cycles) of PtNi/GCM and commercial Pt/C catalysts

Catalyst	Onset potential/V		Half-wave potential/V		Mass activity/(A·mg^-1 Pt)		Specific activity/(mA·cm^-2)
Catalyst	Initial	Final	Initial	Final	Initial	Final	Initial	Final
PtNi/GCM	0.606	0.588	0.551	0.490	0.2311	0.1014	0.2164	0.0950
Pt/C	0.574	0.537	0.494	0.354	0.1999	0.0347	0.2854	0.0495

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