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,Advanced Science

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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
Advanced Science ( IF 15.1 ) 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

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。

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Three‐Phase Electrolysis by Gold Nanoparticle on Hydrophobic Interface for Enhanced Electrochemical Nitrogen Reduction Reaction

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.

更新日期：2020-11-19

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