We have located links that may give you full text access.
Entropy-Driven Direct Air Electrofixation.
Angewandte Chemie 2024 March 18
According to the rule of chemical thermodynamics, the catalytic activation of small molecules (like N2 in air and CO2 in flue gas) generally exhibits a negative activity dependence on O2 owning to the competitive oxygen reduction reaction (ORR). Nevertheless, some catalysts can show positive activity dependence for N2 electrofixation, an important route to produce ammonia under ambient condition. Here we report that the positive activity dependence on O2 of (Ni0.20Co0.20Fe0.20Mn0.19Mo0.21)3S4 catalyst arises from high-entropy mechanism. Thorough experimental and theoretical studies, we demonstrate that under the reaction condition in the mixed N2/O2, the adsorption of O2 on high-entropy catalyst contributes to activating N2 molecules characteristic of elongated N≡N bond lengths. As comparison to the low- and media-entropy counterparts, high entropy can play the second role of attenuating competitive ORR by displaying a negative exponential entropy-ORR activity relationship. Accordingly, benefiting from the O2, the system for direct air electrofixation has demonstrated an ammonia yield rate of 47.70 μg h-1 cm-2, which is even 1.5 times of pure N2 feedstock (31.92 μg h-1 cm-2), overtaking all previous reports for this reaction. We expect the present finding providing an additional dimension to high entropy that leverages systems beyond the constraint of traditional rules.
Full text links
Related Resources
Trending Papers
Autoimmune Hemolytic Anemias: Classifications, Pathophysiology, Diagnoses and Management.International Journal of Molecular Sciences 2024 April 13
Executive Summary: State-of-the-Art Review: Unintended Consequences: Risk of Opportunistic Infections Associated with Long-term Glucocorticoid Therapies in Adults.Clinical Infectious Diseases 2024 April 11
Clinical practice guidelines on the management of status epilepticus in adults: A systematic review.Epilepsia 2024 April 13
Finerenone: From the Mechanism of Action to Clinical Use in Kidney Disease.Pharmaceuticals 2024 March 27
Get seemless 1-tap access through your institution/university
For the best experience, use the Read mobile app
All material on this website is protected by copyright, Copyright © 1994-2024 by WebMD LLC.
This website also contains material copyrighted by 3rd parties.
By using this service, you agree to our terms of use and privacy policy.
Your Privacy Choices
You can now claim free CME credits for this literature searchClaim now
Get seemless 1-tap access through your institution/university
For the best experience, use the Read mobile app