Fabrication of amorphous PdNiCuP nanoparticles as efficient bifunctional and highly durable electrocatalyst for methanol and formic acid oxidation

doi:10.1016/j.jmst.2021.12.047

Abstract

Abstract:

Highly active and durable electrocatalytic materials towards small molecules electro-oxidation reaction are critical to the large-scale commercial applications of direct liquid fuel cells. Unfortunately, current nanocrystalline electrocatalysts normally suffer from low catalytic efficiency, severe CO poisoning and rapid activity decay. Herein, we report a novel amorphous PdNiCuP catalyst synthesized with laser liquid ablation as a potential settlement to this issue. The as-obtained amorphous PdNiCuP catalyst exhibits enhanced electrocatalytic performance with the mass activity of 1.61 A mg^-1 and 737.8 mA mg^-1 towards methanol oxidation reaction (MOR) and formic acid oxidation reaction (FAOR), respectively. Moreover, amorphous PdNiCuP displays excellent operation stability and CO-poisoning resistance in both alkaline and acidic medium. P was proposed to play the decisive role for forming the amorphous structure and maintaining the catalytic stability in MOR and FAOR processes. This work provided insights for the ration design of active and durable amorphous electrocatalysts applied in direct liquid fuel cells.

Key words: Laser ablation, Amorphous catalyst, Anti-poisoning, Stable, Methanol oxidation, Formic acid oxidation

Yunwei Liu, Chang Liu, Zelin Chen, Xuerong Zheng, Rui Jiang, Xing Tong, Yida Deng, Wenbin Hu. Fabrication of amorphous PdNiCuP nanoparticles as efficient bifunctional and highly durable electrocatalyst for methanol and formic acid oxidation[J]. J. Mater. Sci. Technol., 2022, 122: 148-155.

Figures/Tables 6

Fig. 1. Schematic illustration for the synthesis of PdNiCuP-A.

Fig. 2. Characterizations on PdNiCuP-A and PdNiCuP-C NPs. (a) low-magnification and amplified TEM image of PdNiCuP-A NPs. (b, c) HRTEM images of PdNiCuP-A and corresponding FFT (Fast Fourier Transform, inset) pattern. (d) Elemental mapping images of Pd, Ni, Cu, and P on PdNiCuP-A NPs. (e) low-magnification and amplified TEM image of PdNiCuP-C. (f) HRTEM image of PdNiCuP-C NPs. (g) XRD patterns of PdNiCuP-A and PdNiCuP-C. High resolution XPS spectra of (h) Pd 3d, (i) Ni 2p, (j) Cu 2p, and (k) P 2p in PdNiCuP-A and PdNiCuP-C NPs.

Fig. 3. Electrochemical measurements of PdNiCuP-A, PdNiCuP-C and Pd/C. (a) CV curves recorded in 1 M KOH solution. (b) CV curves recorded in 1 M KOH solution + 1 M CH3OH solution. (c) Specific and mass activities of PdNiCuP-A, PdNiCuP-C and Pd/C toward electrocatalytic MOR. (d) Stability of MOR catalysis of PdNiCuP-A, PdNiCuP-C and Pd/C in 1000 CVs cycles between -0.8 to 0.3 V vs. SCE. (e, f) Comparison of the MOR activity and durability with other reported results. (g) CV curves of PdNiCuP-A, PdNiCuP-C and Pd/C recorded in a 0.5 M H2SO4 solution. (h) FAOR CV curves of PdNiCuP-A, PdNiCuP-C and Pd/C recorded in 0.5 M H2SO4 + 1 M HCOOH solution. (i) Stability of FAOR catalysis of PdNiCuP-A, PdNiCuP-C and Pd/C in 100 CVs cycles between -0.3 to 1.0 V vs. SCE. All CV tests are performed in N2-saturated solution at a scan rate of 50 mV s-1.

Table 1. Summary of the MOR and FAOR results of PdNiCuP-A, PdNiCuP-C and Pd/C.

Sample	MOR				FAOR
	ECSA (m² g^-1)	Specific activity (mA cm^-2)	Mass activity (A mg^-1)	Stability (%)	ECSA (m² g^-1)	Specific activity (mA cm^-2)	Mass activity (mA mg^-1)	Stability (%)
PdNiCuP-A	65.95	2.49	1.61	77.4	27.61	3.12	737.8	53.1
PdNiCuP-C	58.08	2.47	1.51	17.6	26.33	1.90	577.6	36.6
Pd/C	50.35	0.99	0.5	28.2	15.50	2.43	377.6	27.8

Fig. 4. Cyclic voltammograms of CO-stripping on (a) PdNiCuP-A, (b) PdNiCuP-C and (c) commercial Pd/C catalysts in 1 M KOH and (d) PdNiCuP-A, (e) PdNiCuP-C and (f) commercial Pd/C in 0.5 M H2SO4 solution at a scan rate of 50 mV · s-1.

Fig. 5. XPS spectra of (a) Pd 3d, (b) Ni 2p, (c) Cu 2p, and (d) P 2p in PdNiCuP-A and (e) Pd 3d, (f) Ni 2p, (g) Cu 2p, and (h) P 2p in PdNiCuP-C NPs after 500 and 1000 CV cycles. (i) Schematic illustration of the CO tolerance abilities for the PdNiCuP-A, PdNiCuP-C and commercial Pd/C catalysts. (j) Schematic illustration of the enhanced anti-CO poisoning property for amorphous structure.

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