g-C3N4纳米片/CuFeO2纳米复合材料中的氧空位和p-n异质结用于在环境条件下增强光催化N2对NH3的固定,New Journal of Chemistry

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g-C3N4纳米片/CuFeO2纳米复合材料中的氧空位和p-n异质结用于在环境条件下增强光催化N2对NH3的固定
New Journal of Chemistry ( IF 2.7 ) Pub Date : 2022-11-02 , DOI: 10.1039/d2nj02850f
Sattam Fahad Almojil ₁ , Abdulaziz Ibrahim Almohana ₁ , Abdulrhman Fahmi Alali ₁ , El-Awady Attia _{2,

3} , Kamal Sharma ₄ , Mohamed A. Shamseldin ₅ , Azheen Ghafour Mohammed ₆ , Yan Cao ₇

Affiliation

光催化固氮过程与太阳能一起是现有工业氨生产方法的一种有前途的替代策略。尽管条件温和且成本低廉，但令人不满意的收益率阻碍了其广泛发展。在此背景下，我们使用简单的水热法制备了具有不同重量百分比的 CuFeO _{2的 gC}₃ N ₄纳米片/CuFeO ₂光催化剂的 ap-n 异质结，并评估了其光催化固氮性能。使用 XRD 数据确定平均微晶尺寸、晶格应变和位错密度。使用 FESEM、TEM 和 HRTEM 图像的形态评估表明存在 CuFeO ₂剥离的gC ₃ N ₄纳米片上的纳米颗粒。gC ₃ N ₄纳米片/CuFeO ₂ 15（15是指CuFeO ₂的重量百分比）纳米复合材料实现了最佳产铵（4560 μmol g ^-1 L ^{-1 ），分别是纯gC}₃的4.3和2.5倍N ₄纳米片和CuFeO ₂，分别。可接受性能的重要因素之一与纳米复合材料结构中的氧空位有关，这已通过 XPS 和 EPR 分析得到证实。 [三键，长度为 m-dash]

氧空位允许氮分子的化学吸附和活化，并通过破坏 N N 三键导致异常高的氨生产效率。此外，通过电化学分析研究了匹配的能带结构、p-n异质结形成和电荷载流子的分离，这些是提高光催化活性的其他重要因素。纳米复合材料的光学性质证实了与CuFeO _{2偶联后的gC}₃ N _4纳米片能够吸收更多的光，这有利于光催化活性。然而，在较高重量百分比的 CuFeO ₂下纳米粒子的聚集降低了活性位点，从而降低了光催化活性。基于所获得的结果和所制备的光催化剂在连续用于固氮后的稳定性，预计将有未来的发展。

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Oxygen vacancy and p–n heterojunction in a g-C3N4 nanosheet/CuFeO2 nanocomposite for enhanced photocatalytic N2 fixation to NH3 under ambient conditions

The process of photocatalytic nitrogen fixation alongside solar energy is a promising alternative strategy to existing industrial methods of ammonia production. Despite the mild and low-cost conditions, dissatisfactory yield rates have prevented its widespread development. In this context, we have fabricated a p–n heterojunction of g-C₃N₄ nanosheets/CuFeO₂ photocatalysts with different weight percentages of CuFeO₂ using a simple hydrothermal method and evaluated its photocatalytic performance for nitrogen fixation. The average crystallite size, lattice strain, and dislocation density were determined using XRD data. Morphological assessment using FESEM, TEM, and HRTEM images showed the presence of CuFeO₂ nanoparticles on the exfoliated g-C₃N₄ nanosheets. The g-C₃N₄ nanosheet/CuFeO₂15 (15 refers to the weight percentage of CuFeO₂) nanocomposite achieved optimal ammonium production (4560 μmol g⁻¹ L⁻¹), which was 4.3 and 2.5 times higher than that of pure g-C₃N₄ nanosheets and CuFeO₂, respectively. One of the important factors of an acceptable performance is related to oxygen vacancies in the nanocomposite structure, which was confirmed by XPS and EPR analyses. Oxygen vacancies allow the chemisorption and activation of nitrogen molecules and result in the unusually high efficiency of ammonia production by breaking the N [triple bond, length as m-dash]

N triple bond. Also, the matched energy band structure, p–n heterojunction formation, and separation of charge carriers, which are other important factors for improving photocatalytic activity, were investigated by electrochemical analyses. The optical properties of the nanocomposite confirmed that the g-C₃N₄ nanosheets after coupling with CuFeO₂ were able to absorb more light, which was in favor of photocatalytic activity. However, the aggregation of nanoparticles at higher weight percentages of CuFeO₂ reduced the active sites and subsequently the photocatalytic activity. Based on the obtained results and the stability of the prepared photocatalyst after successive use in nitrogen fixation, it is expected to undergo future development.

更新日期：2022-11-02

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