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Angew Chem Int Ed Engl. 2016 Sep 19;55(39):11950-4. doi: 10.1002/anie.201604021. Epub 2016 Aug 17.

Cux Co1-x O Nanoparticles on Graphene Oxide as A Synergistic Catalyst for High-Efficiency Hydrolysis of Ammonia-Borane.

Angewandte Chemie (International ed. in English)

Kun Feng, Jun Zhong, Binhua Zhao, Hui Zhang, Lai Xu, Xuhui Sun, Shuit-Tong Lee

Affiliations

  1. Institute of Functional Nano and Soft Materials Laboratory (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, 215123, China.
  2. Institute of Functional Nano and Soft Materials Laboratory (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, 215123, China. [email protected].
  3. Institute of Functional Nano and Soft Materials Laboratory (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, 215123, China. [email protected].
  4. Institute of Functional Nano and Soft Materials Laboratory (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, 215123, China. [email protected].

PMID: 27532345 DOI: 10.1002/anie.201604021

Abstract

Ammonia-borane (AB) is an excellent material for chemical storage of hydrogen. However, the practical utilization of AB for production of hydrogen is hindered by the need of expensive noble metal-based catalysts. Here, we report Cux Co1-x O nanoparticles (NPs) facilely deposited on graphene oxide (GO) as a low-cost and high-performance catalyst for the hydrolysis of AB. This hybrid catalyst exhibits an initial total turnover frequency (TOF) value of 70.0 (H2 ) mol/(Cat-metal) mol⋅min, which is the highest TOF ever reported for noble metal-free catalysts, and a good stability keeping 94 % activity after 5 cycles. Synchrotron radiation-based X-ray absorption spectroscopy (XAS) investigations suggested that the high catalytic performance could be attributed to the interfacial interaction between Cux Co1-x O NPs and GO. Moreover, the catalytic hydrolysis mechanism was studied by in situ XAS experiments for the first time, which reveal a significant water adsorption on the catalyst and clearly confirm the interaction between AB and the catalyst during hydrolysis.

© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Keywords: graphene oxide; heterogeneous catalysis; hydrogen storage; hydrolysis mechanism; nanoparticles

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