Cavity Confinement to Create Multi‐Dimensional Functional Partition Iron Sites Synergistically Promotes Multi‐Scenario Ammonia Synthesis
Rui Bai, Qiao Ye, Yaling Jiang, Yicheng Zhang, Cuiyu Li, Jiajia Wang, Haijian Wang, Yanjuan Zhao, Zhuo Zhao, Ying Zhao, Chunli Zhang, Xingye Zhao, Yijing Feng, Yan Zhao, Haibo Zhang, Xue Zhao, Zhong JinABSTRACT
Electrocatalytic ammonia synthesis centered on nitrate reduction constitutes a vital component of the future green synthesis pathway from nitrogen to nitrogen oxides to ammonia. However, catalyst development often overlooks the critical coordination between the intricate reaction process and the distribution of catalyst functions. In this study, supramolecular encapsulation technology was employed to immobilize low‐boiling‐point ferrocene, followed by thermal conversion to fabricate iron‐based carbon materials (SAFe/Fex/Fe 3 C) endowed with distinct functional partitions and hierarchical dimensions. Utilizing SAFe/Fex/Fe 3 C as the cathode yielded a significantly enhanced ammonia yield rate and Faradaic efficiency (FE) at current levels within this field, with FE approaching nearly 100%. This work realized the efficient and stable conversion of NO 3 − to NH 3 in multiple scenarios, forming demonstration applications of air‐to‐nitrogen oxide‐to‐liquid ammonia fertilizer, ammonia production, and energy conversion; The important mechanism of multi‐site synergistic relay in SAFe/Fex/Fe 3 C to promote NO 3 − to NH 3 in multi‐scenario was revealed, and the importance of different distribution of active sites in the catalyst to promote multi‐reaction coexistence and multi‐proton/electron‐dependent electrochemical nitrate reduction reaction for ammonia synthesis was confirmed.