Journal
ACS CATALYSIS
Volume 6, Issue 5, Pages 3128-3135Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.6b00715
Keywords
Ru-Ni alloy; titania; dehydrogenation; ammonia-borane; hydrogen
Categories
Funding
- Japan Society for the Promotion of Science (JSPS) [26220911, 25289289, 26630409, 26620194]
- Ministry of Education, Culture, Sports, Science and Technology of Japan (MEXT)
- MEXT program Elements Strategy Initiative to Form Core Research Center
- Grants-in-Aid for Scientific Research [16K14478, 26220911] Funding Source: KAKEN
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Highly dispersed monometallic Ru nanoparticles can be successfully synthesized on TiO2 supports for effective hydrogen production from ammonia-borane (NH3 center dot BH3; AB). The choice of support material and reduction methods were confirmed to significantly influence the size of the Ru nanoparticles, and smaller sizes of Ru nanoparticles with a mean diameter of 1.7 nm could be formed on a TiO2 support material by H-2 reduction at 200 degrees C. The catalytic activity of the Ru nanoparticles can be significantly enhanced by alloying with Ni atoms, whereby a significantly high total turnover number (TTO) of approximately 153000 over 8 h was achieved with an excellent turnover frequency (TOF) of 914 min(-1) and an activation energy of 28.1 kJ mol(-1). Detailed characterization by means of TEM, EDX, H-2-TPR, and in situ XAFS measurements revealed that a synergistic alloying effect originates from the random distribution of Ru-Ni nanoparticles with a mean diameter of 2.3 nm and plays a crucial role in the exceptional catalytic performance. This catalytic system has particular potential for industrial application in fuel cells due to advantages such as the facile preparation method, the use of relatively cheap metals, and the exceptionally high catalytic activity.
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