多孔氮化钛载体上铂催化剂的原子层沉积制备及其催化氧气还原性能

doi:10.3866/PKU.WHXB201906070

Abstract

Abstract:

The exploitation of high-performing stable oxygen reduction reaction (ORR) electrocatalysts is critical for energy storage and conversion technologies. The existing high-efficiency electrocatalysts applied to the ORR are mainly based on Pt and its alloys. Moreover, carrier catalysts are the most widely used in actual electrocatalysis. A suitable carrier not only improves the utilization rate of precious metals and the service life of the catalyst, but also serves as a co-catalyst to ameliorate the catalytic activity through a synergistic effect in the reaction. Therefore, research into Pt-based electrocatalysts mainly focuses on the precious metal Pt and the carrier. With the aim of improving the activity and durability of Pt-based catalysts for the ORR, one-dimensional porous titanium nitride (TiN) nanotubes with a large specific surface area as well as good conductivity, electrochemical stability, and corrosion resistance were prepared in this study, and then, Pt nanoparticles were deposited on the TiN-support by atomic layer deposition (ALD). ALD is a novel and simple method for the preparation of films or nanoparticles with fine control of the thickness or size, respectively. The results of X-ray diffraction (XRD) and high-resolution transmission electron microscopy (HR-TEM) experiments confirmed that the Pt nanoparticles obtained by ALD (ALD-Pt/TiN) were face-centered cubic (fcc) crystals with a uniform size and were highly dispersed on the surface of TiN. X-ray spectroscopy (XPS) measurements verified that the binding energy of Pt 4f in ALD-Pt/TiN was positively shifted by 0.33 eV with respect to that of the Pt/C catalyst, indicating strong electronic interactions between the ALD-Pt nanoparticles and the TiN carriers. Linear sweep voltammetry (LSV) and cyclic voltammetry (CV) analyses revealed that ALD-Pt/TiN possessed high activity for the ORR and favorable durability. The onset potential and diffusion-limiting current density of ALD-Pt/TiN were similar to those of commercial Pt/C, while the half-wave potential was 20 mV higher than that of commercial Pt/C, indicating better electrocatalytic performance of the designed material. Furthermore, the electrocatalytic mechanism and kinetics for ALD-Pt/TiN were investigated by rotating ring-disc electrode (RRDE) experiments. The results suggested that the electron transfer number of the ALD-Pt/TiN catalyst was about 3.93, indicating that the ORR on the electrode was dominated by an efficient four-electron pathway. At the same time, the peroxide content was only 5%. The results of accelerated durability testing (ADT) showed that ALD-Pt/TiN had better ORR stability than Pt/C. This excellent electrocatalytic performance was probably due to the high dispersibility of the Pt nanoparticles deposited by ALD, good conductivity and corrosion resistance of TiN, and strong interactions between ALD-Pt and the TiN support. This work provides a reliable strategy for the design of new electrocatalytic materials with high activity and stability. Future research will focus on the strong interactions between ALD-Pt and the TiN carriers.

Key words: Porous Titanium Nitride, Platinum nanoparticles, Atomic layer deposition, Electrocatalysis, Oxygen reduction reaction

Xiaolong Tang,Shenghui Zhang,Jing Yu,Chunxiao Lü,Yuqing Chi,Junwei Sun,Yu Song,Ding Yuan,Zhaoli Ma,Lixue Zhang. Preparation of Platinum Catalysts on Porous Titanium Nitride Supports by Atomic Layer Deposition and Their Catalytic Performance for Oxygen Reduction Reaction[J]. Acta Physico-Chimica Sinica 2020, 36(7), 1906070. doi: 10.3866/PKU.WHXB201906070

Figures/Tables 7

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Preparation of Platinum Catalysts on Porous Titanium Nitride Supports by Atomic Layer Deposition and Their Catalytic Performance for Oxygen Reduction Reaction

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