Journal
ACS APPLIED NANO MATERIALS
Volume 4, Issue 6, Pages 6030-6044Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsanm.1c00871
Keywords
hydrogen spillover; noble metal nanoparticles; MOF nanocubes; ZIF-67 hydrogenolysis; heterogeneous catalysis
Funding
- National Research Foundation (NRF), Prime Minister's Office, Singapore, under its Campus for Research Excellence and Technological Enterprise (CREATE) program
- National University of Singapore under its Flagship Green Energy Program (GEP)
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Different metal nanoparticles supported on ZIF-67 were studied for their hydrogen spillover abilities through analyzing the hydrogenolysis of ZIF-67, providing a method for systematically comparing their performance.
The hydrogen spillover phenomenon offers a great potential for enhanced performance in heterogeneous catalysis involving hydrogenation. Despite this, the current applications of hydrogen spillover are usually only for demonstrative purposes and the appropriate metal elements are often chosen by trial-and-error screening. Therefore, herein we systematically study and rigorously compare the hydrogen spillover abilities of various metal nanoparticles (NPs) supported on ZIF-67 nanocubes (NCs) by analyzing the hydrogenolysis of ZIF-67 at elevated temperatures. In this investigation, we make our ultimate efforts to ensure that all factors influencing the hydrogen spillover and thus hydrogenolysis are constant, which is crucial to objectively compare the hydrogen spillover abilities of the studied metals. Finally, a controllable synthetic procedure is devised to anchor presynthesized 2 nm metal NPs onto the exterior surfaces of ZIF-67 NCs. On the basis of this protocol, we have successfully determined the relative ability of hydrogen spillover for a series of 2 nm noble metal NPs: Pt > Ir > Ru > Rh. It is important to recognize that the ZIF-67 NCs serve effectively as a detector (or a receiver) of the dissociated hydrogen, which can measure the amount of hydrogen atoms produced during the hydrogen spillover. Therefore, the findings of this study could guide the rational choice of metal materials in other catalytic hydrogenation reaction systems. Moreover, the hydrogen spillover abilities of a wide variety of metal elements with defined particle sizes can also be determined via devising similar procedures in future investigations.
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