Optimizing the surface distribution of acid sites for cooperative catalysis in condensation reactions promoted by water

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Li, Gengnan
Wang, Bin
Kobayashi, Takeshi
Pruski, Marek
Resasco, Daniel E.
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Iowa State University Digital Repository, Ames IA (United States)
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Ames National Laboratory

Ames National Laboratory is a government-owned, contractor-operated national laboratory of the U.S. Department of Energy (DOE), operated by and located on the campus of Iowa State University in Ames, Iowa.

For more than 70 years, the Ames National Laboratory has successfully partnered with Iowa State University, and is unique among the 17 DOE laboratories in that it is physically located on the campus of a major research university. Many of the scientists and administrators at the Laboratory also hold faculty positions at the University and the Laboratory has access to both undergraduate and graduate student talent.

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Nature accomplishes catalytic process with exquisite control by altering the distribution of active sites in a confining pocket and by regulating the structure of occluded solvents. In such systems, the ubiquitous water may influence reaction rates and selectivity by stabilizing reaction intermediates and transition states via a network of H bonds. Inspired by nature, here we aim at providing quantitative support and mechanistic insight into the role of water-promoting C–C bond formation on an acid catalyst by combining spectroscopic analysis, catalytic reaction measurements, and theoretical calculations. This set of experimental and computational studies reveals that the interaction between water and polar species on the surface generates diverse environments surrounding the active sites that facilitate the reaction. These findings provide an extra dimension for tailoring catalytic phenomena in industrially relevant reactions.
This is a manuscript of an article published as Li, Gengnan, Bin Wang, Takeshi Kobayashi, Marek Pruski, and Daniel E. Resasco. "Optimizing the surface distribution of acid sites for cooperative catalysis in condensation reactions promoted by water." Chem Catalysis 1, no. 5 (2021): 1065-1087. DOI: 10.1016/j.checat.2021.08.005. Copyright 2021 Elsevier Inc. DOE Contract Number(s): SC0018284; AC02-07CH11358. Posted with permission.