期刊論文
| 學年 | 113 |
|---|---|
| 學期 | 1 |
| 出版（發表）日期 | 2025-01-21 |
| 作品名稱 | Unlocking high-current-density nitrate reduction and formaldehyde oxidation synergy for scalable ammonia production and fixation |
| 作品名稱（其他語言） | |
| 著者 | Linjie Zhang; Yimeng Cai; Yanghua Li; Chen Sun; Yi Xiao; Yibing Yang; Dechao Chen; Dongdong Xiao; Chi-Feng Lee; Yunjian Wang; Shiqiang Feng; Hsiao-Tsu Wang; Yu-Cheng Shao; Ting-Shan Chan; Hirofumi Ishii; Nozomu Hiraoka; Xiuyun Wang; Jun Luo; Lili Han |
| 單位 | |
| 出版者 | |
| 著錄名稱、卷期、頁數 | Energy & Environmental Science 18(6), p.2804-2816 |
| 摘要 | Nitrate electroreduction to ammonia holds great promise in sustainable green ammonia synthesis, yet faces a dearth of competent electrocatalysts adapted to varying nitrate concentration, and inadequate ammonia fixation. Herein, we present a high-performance Ag single-atom-decorated Cu2O nanowire catalyst (Ag1@Cu2O) that exhibits concentration-universal high-rate nitrate reduction, achieving >90% to near-unity ammonia faradaic efficiency (FE) across nitrate concentrations from 0.01 to 0.5 M. Notably, at 0.5 M nitrate concentration, it attains a two-ampere-level current density (2.3 A cm⁻²) at −1 V vs. RHE, resulting in a leading ammonia yield rate of 184.4 mgNH3 h⁻¹ cm⁻². In situ studies combined with theoretical calculations elucidate an Ag–Cu inter-site synergistic catalytic mechanism, in which single-atom Ag serves as an accelerator for active hydrogen generation and stabilization on Cu sites to boost the hydrogenation kinetics of N-containing intermediates, thus smoothing the energy barriers for ammonia production via the favorable *NHO pathway. Additionally, Ag1@Cu2O demonstrates near-unity formate FE for formaldehyde oxidation, reaching a 300 mA cm⁻² current density at a mere 0.31 V vs. RHE. Motivated by this exceptional bifunctionality, we demonstrate an innovative tandem electrochemical–chemical strategy for upgrading ammonia into high-value ammonium formate by coupled electrolysis of nitrate reduction and formaldehyde oxidation, followed by straightforward chemical combination and isolation. In practice, membrane electrode assembly (MEA) electrolysis at 1.6 V for 100 h successfully outputs 10.7 g of high-purity ammonium formate. Furthermore, the commonality of this strategy is validated by application to various nitrate/aldehyde pairs. This work blazes a new trail for scalable, cost- and energy-efficient green ammonia production and fixation from nitrate reduction. |
| 關鍵字 | |
| 語言 | en |
| ISSN | 1754-5692; 1754-5706 |
| 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/987654321/129458 ) |