4.8 Article

Modulating the Acidic Properties of Mesoporous Mox-Ni0.8Cu0.2O Nanowires for Enhanced Catalytic Performance toward the Methanolysis of Ammonia Borane for Hydrogen Production

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 14, Issue 24, Pages 27979-27993

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c06234

Keywords

hydrogen evolution; ammonia borane; methanolysis; acid sites; nanowires

Funding

  1. Major and Special Project in the Field of Intelligent Manufacturing of the Universities in Guangdong Province [2020ZDZX2067]
  2. National Natural Science Foundation of China [21975056, 52002079]
  3. Science & Technology project of Huizhou City [2020SD0404032]
  4. Natural Science Foundation of Huizhou University [20180927172750326, HZU202004, HZU202052]
  5. Professorial and Doctoral Scientific Research Foundation of Huizhou University [2018JB036, 2019JB023, 2019JB034, 2020JB046]

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In this study, uniform Mox-Ni0.8Cu0.2O nanowires were successfully fabricated as catalysts for ammonia borane (AB) methanolysis. The acidity of the catalysts' surface was flexibly modulated, leading to high catalytic activity. The relationship between the quantity of moderated acid sites and the activity of AB methanolysis was determined for the first time, and a plausible mechanism for the reaction was proposed.
Rational construction of inexpensive, highly efficient, and stable catalysts for ammonia borane (AB) methanolysis is in high demand but still remains a great challenge. In this work, we have successfully fabricated uniform Mox-Ni0.8Cu0.2O nanowires using a simple hydrothermal method followed by a post-calcination treatment and flexibly modulated the acidity of their surface by changing the amount of Mo introduced into Ni0.8Cu0.2O. The Mo0.1-Ni0.8Cu0.2O catalyst displayed strong catalytic activity toward AB methanolysis with an ultrahigh turnover frequency of 46.9 molH2 molcat. -1 min-1, which is even higher than some noble metal catalysts. In this work, an equation regarding the relationship between the quantity of moderated acid sites of catalysts and its corresponding activity toward AB methanolysis was first determined. A plausible mechanism for AB methanolysis catalyzed by Mox- Ni0.8Cu0.2O was proposed, and the benefits of the introduction of MoO3 to Ni0.8Cu0.2O for enhancing the catalytic performance were also discussed. These findings can form a basis for the rational construction of inexpensive catalysts with robust performance toward AB methanolysis for hydrogen production.

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