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- Title
Descriptor‐Based Volcano Relations Predict Single Atoms for Hydroxylamine Electrosynthesis.
- Authors
Yang, Rong; Wang, Yuting; Li, Hongjiao; Zhou, Jin; Gao, Zeyuan; Liu, Cuibo; Zhang, Bin
- Abstract
Hydroxylamine (NH2OH) is an important feedstock in fuels, pharmaceuticals, and agrochemicals. Nanostructured electrocatalysts drive green electrosynthesis of hydroxylamine from nitrogen oxide species in water. However, current electrocatalysts still suffer from low selectivity and manpower‐consuming trial‐and‐error modes, leaving unclear selectivity/activity origins and a lack of catalyst design principles. Herein, we theoretically analyze key determinants of selectivity/activity and propose the adsorption energy of NHO (Gad(*NHO)) as a performance descriptor. A weak *NH2OH binding affinity and a favorable reaction pathway (*NHO pathway) jointly enable single‐atom catalysts (SACs) with superior NH2OH selectivity. Then, an activity volcano plot of Gad(*NHO) is established to predict a series of SACs and discover Mn SACs as optimal electrocatalysts that exhibit pH‐dependent activity. These theoretical prediction results are also confirmed by experimental results, rationalizing our Gad(*NHO) descriptor. Furthermore, Mn−Co geminal‐atom catalysts (GACs) are predicted to optimize Gad(*NHO) and are experimentally proved to enhance NH2OH formation.
- Subjects
ELECTROSYNTHESIS; HYDROXYLAMINE; ATOMS; VOLCANOES; ELECTROCATALYSTS; CATALYSTS
- Publication
Angewandte Chemie, 2024, Vol 136, Issue 14, p1
- ISSN
0044-8249
- Publication type
Academic Journal
- DOI
10.1002/ange.202317167