Asset Details
Do you wish to reserve the book?
The shape of water in zeolites and its impact on epoxidation catalysis
Hey, we have placed the reservation for you!
By the way, why not check out events that you can attend while you pick your title.
Oops! Something went wrong.
Looks like we were not able to place the reservation. Kindly try again later.
Are you sure you want to remove the book from the shelf?
The shape of water in zeolites and its impact on epoxidation catalysis
Do you wish to request the book?
The shape of water in zeolites and its impact on epoxidation catalysis
Please be aware that the book you have requested cannot be checked out. If you would like to checkout this book, you can reserve another copy
We have requested the book for you!
Your request is successful and it will be processed during the Library working hours. Please check the status of your request in My Requests.
Oops! Something went wrong.
Looks like we were not able to place your request. Kindly try again later.
Journal Article
The shape of water in zeolites and its impact on epoxidation catalysis
2021
Overview
Solvent structures that surround active sites reorganize during catalysis and influence the stability of surface intermediates. Within zeolite pores, H
2
O molecules form hydrogen-bonded structures that differ substantially from bulk H
2
O. Here, we show by spectroscopic measurements and molecular dynamics simulations that H
2
O molecules form bulk-like three-dimensional structures within 1.3 nm cages, whereas H
2
O molecules coalesce into oligomeric one-dimensional chains when the pore diameter falls below 0.65 nm. The differences between these solvent structure motifs provide opportunities to manipulate enthalpy–entropy compensation relationships and greatly increase the rates of catalysis. We describe how the reorganization of these pore-size-dependent H
2
O structures during alkene epoxidation catalysis gives rise to entropy gains that increase the turnover rates by up to 400-fold. Collectively, this work shows that solvent molecules form distinct structures with a highly correlated motion within microporous environments, and the reorganization of these structures may be controlled to confer stability to the desired reactive intermediates.
Solvent structuring affects the energy landscape of catalytic reactions, but the quantitative understanding of such effects remains difficult. Now, the structure of water within the micropores of different zeolites is disclosed together with the effects that its reorganization has over alkene epoxidation catalysis.
