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Selective conversion of N2 to NH3 on highly dispersed RuO2 using amphiphilic ionic liquid-anchored fibrous carbon structure
Journal of Energy Chemistry ( IF 14.0 ) Pub Date : 2021-09-10 , DOI: 10.1016/j.jechem.2021.09.004
Kahyun Ham 1, 2, 3 , Muhammad Salman 4 , Sunki Chung 1, 2, 3 , Minjun Choi 1, 2 , HyungKuk Ju 3, 5 , Hye Jin Lee 4 , Jaeyoung Lee 1, 2, 3
Affiliation  

Ammonia (NH3) plays a key role in the agricultural fertilizer and commodity chemical industries and is useful for exploring hydrogen storage carriers. The electrochemical nitrogen reduction reaction (NRR) is receiving attention as an environmentally sustainable NH3 synthesis replacement for the traditional Haber–Bosch process owing to its near ambient reaction conditions (<100 °C and 1 atm). However, its NH3 yield and faradaic efficiency are extremely low because of the sluggish kinetics of N≡N bond dissociation and the hindrance from competitive hydrogen evolution. To overcome these challenges, we herein introduce a dual-functionalized ionic liquid (1-(4-hydroxybutyl)-3-methylimidazolium hydroxide [HOBIM]OH) for a highly dispersed ruthenium oxide electrocatalyst to achieve a biased NRR. The observed uniform distribution of RuO2 on the carbon fiber and increase in the surface area for N2 adsorption by limiting proton access can be attributed to the presence of imidazolium ions. Moreover, extensive N2 adsorption contributes to enhanced NRR selectivity with an NH3 yield of 3.0 × 10−10 mol cm−2 s−1 (91.8 μg h−1 mg−1) and a faradaic efficiency of 2.2% at −0.20 VRHE. We expect our observations to provide new insights into the design of effective electrode structures for electrochemical NH3 synthesis.



中文翻译:

使用两亲离子液体锚定的纤维碳结构在高度分散的 RuO2 上将 N2 选择性转化为 NH3

氨 (NH 3 ) 在农业肥料和商品化学工业中起着关键作用,可用于探索储氢载体。由于其接近环境反应条件(<100 °C 和 1 atm),电化学氮还原反应 (NRR) 作为传统 Haber-Bosch 工艺的环境可持续 NH 3合成替代品而受到关注。然而,其 NH 3由于 N≡N 键解离的缓慢动力学和竞争性析氢的阻碍,产率和法拉第效率极低。为了克服这些挑战,我们在此引入了一种双官能化离子液体(1-(4-羟基丁基)-3-甲基咪唑氢氧化物 [HOBIM]OH),用于高度分散的氧化钌电催化剂,以实现偏置 NRR。观察到的 RuO 2在碳纤维上的均匀分布和通过限制质子进入而增加的 N 2吸附表面积可归因于咪唑鎓离子的存在。此外,广泛的 N 2吸附有助于提高 NRR 选择性,NH 3产率为 3.0 × 10 -10 mol cm -2s -1 (91.8 μg h -1 mg -1 ) 和在 -0.20 V RHE 时的法拉第效率为 2.2% 。我们希望我们的观察能够为电化学 NH 3合成的有效电极结构的设计提供新的见解。

更新日期:2021-09-10
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