期刊論文
| 學年 | 114 |
|---|---|
| 學期 | 1 |
| 出版（發表）日期 | 2025-12-23 |
| 作品名稱 | Ampere-Level Membrane-Free Bipolar Ammonia Electrosynthesis with Faradaic Efficiency Exceeding 100% on a Surface-Reconstructed NiFe-Hydroxide |
| 作品名稱（其他語言） | |
| 著者 | Yimeng Cai; Yanghua Li; Hsiao-Tsu Wang; Guangyu Chen; Yibing Yang; Cheng-You Lee; Chi-Feng Lee; Shuwen Zhao; Linjie Zhang; Jing Mao; Lili Han |
| 單位 | |
| 出版者 | |
| 著錄名稱、卷期、頁數 | Angewandte Chemie International Edition 65(6), e21629 |
| 摘要 | Awaking the force of materials for specific efficacy by precise electronic modulation remains a fundamental challenge in catalysis. Herein, we transform ordinary NiFe-layered double hydroxide (NiFe-LDH) into a high-performance NO3−-to-NH3 electrocatalyst via cathodic electrochemical restructuring, which effectively induces oxygen vacancy (Ov) clusters preferentially localized around low-valence Ni sites. The resultant restructured NiFe-LDH (NiFe-LDH-R) demonstrates excellent concentration-universal NH3 electrosynthesis activity in 1 M KOH, notably sustaining high Faradaic efficiencies (FEs, 88.5%–95%) across a broad potential range and attaining an ampere-level current density (−1.46 A cm−2) together with a remarkable yield rate of 104.1 mgNH3 h−1 cm−2. In situ spectroscopic analyses reveal boosted hydrogenation kinetics and a thermodynamically favorable NOH pathway for NiFe-LDH-R, which is further decoded by theoretical calculations indicating that synergized Ov/Fe and low-valence Ni sites, respectively enhance NO3− adsorption and directional active hydrogen (*H) supply, thus streamlining overall energy barriers. Moreover, a new-style membrane-free bipolar electrosynthesis system is established, which enables unprecedent NH3 FEs exceeding 100% and scalable NH3 valorization into 4.1 g of methenamine. This study rekindles power of electrochemical restructuring in catalyst advance and pioneers a new paradigm for energy-efficient electrochemical NH3 production and fixation. |
| 關鍵字 | Ammonia synthesis; Ampere-level; Membrane-free; Nitrate reduction; Oxygen vacancy |
| 語言 | en |
| ISSN | 1433-7851; 1521-3773 |
| 期刊性質 | 國外 |
| 收錄於 | SCI |
| 產學合作 | |
| 通訊作者 | |
| 審稿制度 | 否 |
| 國別 | GBR |
| 公開徵稿 | |
| 出版型式 | ,電子版,紙本 |
| 相關連結 |
機構典藏連結 ( http://tkuir.lib.tku.edu.tw:8080/dspace/handle/987654321/129456 ) |