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Linear Adsorption Enables NO Selective Electroreduction to Hydroxylamine on Single Co Sites |
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| Authors: | Jin Zhou Shuhe Han Rong Yang Tieliang Li Wenbin Li Dr Yuting Wang Prof Yifu Yu Prof Bin Zhang |
| Institution: | 1. School of Chemical Engineering and Technology, Tianjin University, 300072 Tianjin, China
These authors contributed equally to this work.;2. Institute of Molecular Plus, Department of Chemistry, School of Science, Tianjin University, 300072 Tianjin, China These authors contributed equally to this work.;3. Institute of Molecular Plus, Department of Chemistry, School of Science, Tianjin University, 300072 Tianjin, China;4. School of Chemical Engineering and Technology, Tianjin University, 300072 Tianjin, China |
| Abstract: | Hydroxylamine (NH2OH), a vital industrial feedstock, is presently synthesized under harsh conditions with serious environmental and energy concerns. Electrocatalytic nitric oxide (NO) reduction is attractive for the production of hydroxylamine under ambient conditions. However, hydroxylamine selectivity is limited by the competitive reaction of ammonia production. Herein, we regulate the adsorption configuration of NO by adjusting the atomic structure of catalysts to control the product selectivity. Co single-atom catalysts show state-of-the-art NH2OH selectivity from NO electroreduction under neutral conditions (FE : 81.3 %), while Co nanoparticles are inclined to generate ammonia (FE : 92.3 %). A series of in situ characterizations and theoretical simulations unveil that linear adsorption of NO on isolated Co sites enables hydroxylamine formation and bridge adsorption of NO on adjacent Co sites induces the production of ammonia. |
| Keywords: | Co Single Atom Electrocatalysis Hydroxylamine Linear Adsorption NO Reduction |