Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 117, Issue 47, Pages 29442-29452Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.2015897117
Keywords
LOHCs; methanol dehydrogenation; metal-support interaction; transition metal; BN
Categories
Funding
- Office of Science, Office of Basic Energy Sciences, of the US Department of Energy (DOE) [DE-AC0205CH11231]
- DOE through Hydrogen Materials Advanced Research Consortium, Energy Materials Network
- US DOE, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office [DE-AC02-05CH11231]
- Advanced Light Source, a DOE Office of Science User Facility [DE-AC0205CH11231]
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Employing liquid organic hydrogen carriers (LOHCs) to transport hydrogen to where it can be utilized relies on methods of efficient chemical dehydrogenation to access this fuel. Therefore, developing effective strategies to optimize the catalytic performance of cheap transition metal-based catalysts in terms of activity and stability for dehydrogenation of LOHCs is a critical challenge. Here, we report the design and synthesis of ultrasmall nickel nanoclusters (-1.5 nm) deposited on defect-rich boron nitride (BN) nano sheet (Ni/BN) catalysts with higher methanol dehydrogenation activity and selectivity, and greater stability than that of some other transition-metal based catalysts. The interface of the twodimensional (2D) BN with the metal nanoparticles plays a strong role both in guiding the nucleation and growth of the catalytically active ultrasmall Ni nanoclusters, and further in stabilizing these nanoscale Ni catalysts against poisoning by interactions with the BN substrate. We provide detailed spectroscopy characterizations and density functional theory (DFT) calculations to reveal the origin of the high productivity, high selectivity, and high durability exhibited with the Ni/BN nanocatalyst and elucidate its correlation with nanocluster size and support-nanocluster interactions. This study provides insight into the role that the support material can have both regarding the size control of nanoclusters through immobilization during the nanocluster formation and also during the active catalytic process; this twofold set of insights is significant in advancing the understanding the bottom-up design of highperformance, durable catalytic systems for various catalysis needs.
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