Synergistic Pt-WO3 Dual Active Sites to Boost Hydrogen Production from Ammonia Borane

Wenyao Chen; Wenzhao Fu; Gang Qian; Bingsen Zhang; De Chen; Xuezhi Duan; Xinggui Zhou

doi:10.1016/j.isci.2020.100922

Synergistic Pt-WO₃ Dual Active Sites to Boost Hydrogen Production from Ammonia Borane

iScience. 2020 Mar 27;23(3):100922. doi: 10.1016/j.isci.2020.100922. Epub 2020 Feb 19.

Authors

Wenyao Chen¹, Wenzhao Fu¹, Gang Qian¹, Bingsen Zhang², De Chen³, Xuezhi Duan⁴, Xinggui Zhou¹

Affiliations

¹ State Key Laboratory of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, China.
² Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua Road, Shenyang 110016, China.
³ Department of Chemical Engineering, Norwegian University of Science and Technology, 7491 Trondheim, Norway.
⁴ State Key Laboratory of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, China. Electronic address: xzduan@ecust.edu.cn.

Abstract

Development of synergistic heterogeneous catalysts with active sites working cooperatively has been a pursuit of chemists. Herein, we report for the first time the fabrication and manipulation of Pt-WO₃ dual-active-sites to boost hydrogen generation from ammonia borane. A combination of DFT calculations, structural characterization, and kinetic (isotopic) analysis reveals that Pt and WO₃ act as the active sites for ammonia borane and H₂O activation, respectively. A trade-off between the promoting effect of WO₃ and the negative effect of decreased Pt binding energy contributes to a volcano-shaped activity, and Pt/CNT-5W delivers a 4-fold increased activity of 710.1 mol_H2·mol_Pt^-1·min^-1. Moreover, WO₃ is suggested to simultaneously act as the sacrificial site that can divert B-containing by-products away from Pt sites against deactivation, yielding an increase from 24% to 68% of the initial activity after five cycles. The strategy demonstrated here could shed a new light on the design and manipulation of dual-active-site catalysts.

Keywords: Catalysis; Inorganic Chemistry; Nanomaterials.