Volume 60, Issue 6 pp. 3290-3298
Research Article

Exploiting Ru-Induced Lattice Strain in CoRu Nanoalloys for Robust Bifunctional Hydrogen Production

Dr. Weidong Li

Dr. Weidong Li

Green Catalysis Center, and College of Chemistry, Zhengzhou University, Zhengzhou, 450000 China

College of Materials Engineering, Henan International Joint Laboratory of Rare Earth Composite Material, Henan University of Engineering, Zhengzhou, 451191 China

These authors contributed equally to this work.

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Dr. Yunxuan Zhao

Dr. Yunxuan Zhao

Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190 China

These authors contributed equally to this work.

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Dr. Yuan Liu

Dr. Yuan Liu

Green Catalysis Center, and College of Chemistry, Zhengzhou University, Zhengzhou, 450000 China

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Mingzi Sun

Mingzi Sun

Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong SAR, China

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Prof. Geoffrey I. N. Waterhouse

Prof. Geoffrey I. N. Waterhouse

School of Chemical Sciences, The University of Auckland, Auckland, 1142 New Zealand

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Prof. Bolong Huang

Corresponding Author

Prof. Bolong Huang

Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong SAR, China

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Prof. Kan Zhang

Prof. Kan Zhang

MIIT Key Laboratory of Advanced Display Material and Devices, School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing, 210094 China

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Prof. Tierui Zhang

Prof. Tierui Zhang

Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190 China

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Prof. Siyu Lu

Corresponding Author

Prof. Siyu Lu

Green Catalysis Center, and College of Chemistry, Zhengzhou University, Zhengzhou, 450000 China

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First published: 26 October 2020
Citations: 364

Graphical Abstract

Ultra-low Ru induced CoRu nanoalloy lattice strain for robust hydrogen evolution reaction (HER) and hydrolysis of ammonia borane (AB) bifunctional hydrogen production is introduced. The CoRu0.5/CQDs displayed excellent stability during each reaction, including seven alternating cycles of HER and AB hydrolysis.

Abstract

Designing bifunctional catalysts capable of driving the electrochemical hydrogen evolution reaction (HER) and also H2 evolution via the hydrolysis of hydrogen storage materials such as ammonia borane (AB) is of considerable practical importance for future hydrogen economies. Herein, we systematically examined the effect of tensile lattice strain in CoRu nanoalloys supported on carbon quantum dots (CoRu/CQDs) on hydrogen generation by HER and AB hydrolysis. By varying the Ru content, the lattice parameters and Ru-induced lattice strain in the CoRu nanoalloys could be tuned. The CoRu0.5/CQDs catalyst with an ultra-low Ru content (1.33 wt.%) exhibited excellent catalytic activity for HER (η=18 mV at 10 mA cm−2 in 1 M KOH) and extraordinary activity for the hydrolysis of AB with a turnover frequency of 3255.4 molurn:x-wiley:14337851:media:anie202013985:anie202013985-math-0001  mol−1(Ru) min−1 or 814.7 molurn:x-wiley:14337851:media:anie202013985:anie202013985-math-0002  mol−1(cat) min−1 at 298 K, respectively, representing one of the best activities yet reported for AB hydrolysis over a ruthenium alloy catalyst. Moreover, the CoRu0.5/CQDs catalyst displayed excellent stability during each reaction, including seven alternating cycles of HER and AB hydrolysis. Theoretical calculations revealed that the remarkable catalytic performance of CoRu0.5/CQDs resulted from the optimal alloy electronic structure realized by incorporating small amounts of Ru, which enabled fast interfacial electron transfer to intermediates, thus benefitting H2 evolution kinetics. Results support the development of new and improved catalysts HER and AB hydrolysis.

Conflict of interest

The authors declare no conflict of interest.

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