Promoted Formic Acid Electrooxidation Using PdNx/C Catalyst Prepared with Hyperbranched Polymer†

doi:10.7503/cjcu20190116

Abstract

Abstract:

Nitrogen-doped PdN_x/C(x denoted as the amine-terminate and palladium molar ratio) catalyst derived from hyperbranched polymer was prepared via in-situ polymerization, and the electrocatalytic oxidation of formic acid was investigated. The morphology and surface electronic state of the catalytically active component Pd were investigated by transmission electron microscopy(TEM), high resolution transmission electron microscopy(HRTEM), X-ray photoelectron spectroscopy(XPS) and X-ray diffraction(XRD). The results indicate that the Pd nanoparticles remain an average size of 2 nm using polymer modification, and maintain high dispersion, with surface Pd mainly presenting as Pd(0). Compared with the Pd/C catalyst, the Pd unit mass specific activity of PdN₂₀/C for formic acid electrooxidation was increased by 10.9%.

Key words: Formic acid, Fuel cell, Electrooxidation, Pd, Hyperbranched polymer

CLC Number:

O646.21

TrendMD:

YU Yancun, WANG Xian, GE Junjie, LIU Changpeng, XING Wei. Promoted Formic Acid Electrooxidation Using PdN_x/C Catalyst Prepared with Hyperbranched Polymer^†[J]. Chem. J. Chinese Universities, 2019, 40(7): 1433.

Figures/Tables 7

Fig.1 XRD patterns of the PdN20/C(a) and unreduced PdN20/C(b) catalysts

Fig.2 TEM images(A―C) and size distribution histograms(D―F) of PdNx/C with different molar ratio of amine-terminate group to Pd(A, D) PdN10/C; (B, E) PdN20/C; (C, F) PdN30/C.

Fig.3 SEM image(A) and element mapping profiles(B—D) of PdN20/C (B) C; (C) N; (D) Pd.

Fig.4 XPS spectra of Pd3d(A) and N1s of PdN20/C(B)

Fig.5 CV curves for the PdNx/C catalysts in an aqueous solution of 0.5 mol/L H2SO4+0.5 mol/L HCOOH at a scan rate of 20 mV/s

Table 1 Comparison of selected N-containing monomer for formic acid electrooxidation

N-containing monomer	w(Pd)(%)		ECSA/(m²·g^-1)	Peak current/mA
N-containing monomer	Nominal	ICP	ECSA/(m²·g^-1)	Peak current/mA
AEPZ	20	21.13	205.1	506.9
ED	20	19.57	187.3	498.6
DAPD	20	20.79	196.5	464.3

Fig.6 Chronoamperometric curves at 0.2 V on the PdN20/C catalyst in an aqueous solution of 0.5 mol/L H2SO4+0.5 mol/L HCOOH

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