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Three‐Phase Electrolysis by Gold Nanoparticle on Hydrophobic Interface for Enhanced Electrochemical Nitrogen Reduction Reaction
Advanced Science ( IF 14.3 ) Pub Date : 2020-10-12 , DOI: 10.1002/advs.202002630
Junchang Zhang 1, 2 , Bo Zhao 3 , Wenkai Liang 3 , Genshu Zhou 4 , Zhiqiang Liang 3 , Yawen Wang 3 , Jiangying Qu 1 , Yinghui Sun 5 , Lin Jiang 3
Affiliation  

Electrochemical nitrogen reduction reaction (NRR) provides a facile and sustainable strategy to produce ammonia (NH3) at ambient conditions. However, the low NH3 yield and Faradaic efficiency (FE) are still the main challenges due to the competitive hydrogen evolution reaction (HER). Herein, a three‐phase electrocatalyst through in situ fabrication of Au nanoparticles (NPs) located on hydrophobic carbon fiber paper (Au/o‐CFP) is designed. The hydrophobic CFP surface facilitates efficient three‐phase contact points (TPCPs) for N2 (gas), electrolyte (liquid), and Au NPs (solid). Thus, concentrated N2 molecules can contact the electrocatalyst surface directly, inhibiting the HER since the lowered proton concentration and overall enhancing NRR. The three‐phase Au/o‐CFP electrocatalyst presents an excellent NRR performance with high NH3 yield rate of 40.6 µg h−1 mg−1 at −0.30 V and great FE of 31.3% at −0.10 V versus RHE (0.1 m Na2SO4). The N2‐bubble contact angle result and cyclic voltammetry analysis confirm that the hydrophobic interface has a relatively strong interaction with N2 bubble for enhanced NRR and weak electrocatalytic activity for HER. Significantly, the three‐phase Au/o‐CFP exhibits excellent stability with a negligible fluctuation of NH3 yield and FE in seven‐cycle test. This work provides a new strategy for improving NRR and simultaneously inhibiting HER.

中文翻译:

金纳米颗粒在疏水界面上的三相电解增强电化学氮还原反应

电化学氮还原反应(NRR)提供了一种在环境条件下生产氨(NH 3)的简便且可持续的策略。然而,由于竞争性析氢反应(HER),低NH 3产率和法拉第效率(FE)仍然是主要挑战。本文设计了一种通过原位制造位于疏水性碳纤维纸(Au/o-CFP)上的金纳米颗粒(NP)的三相电催化剂。疏水性 CFP 表面有利于 N 2(气体)、电解质(液体)和 Au NP(固体)的高效三相接触点 (TPCP) 。因此,浓缩的N 2分子可以直接接触电催化剂表面,由于质子浓度降低而抑制HER,并总体增强NRR。三相Au/o-CFP电催化剂表现出优异的NRR性能,与RHE(0.1 m Na)相比,在-0.30 V时NH 3产率高达40.6 µg h -1 mg -1,在-0.10 V时FE高达31.3% 2 SO 4 )。N 2气泡接触角结果和循环伏安分析证实疏水界面与N 2气泡具有相对较强的相互作用,从而增强了NRR,而对HER的电催化活性较弱。值得注意的是,三相Au/o-CFP表现出优异的稳定性,在七次循环测试中NH 3产率和FE的波动可以忽略不计。这项工作为改善NRR并同时抑制HER提供了新策略。
更新日期:2020-11-19
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