Surface Lattice Oxygen Activation by Nitrogen-Doped Manganese Dioxide as an Effective and Longevous Catalyst for Indoor HCHO Decomposition,ACS Applied Materials & Interfaces

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Surface Lattice Oxygen Activation by Nitrogen-Doped Manganese Dioxide as an Effective and Longevous Catalyst for Indoor HCHO Decomposition
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-06-02 , DOI: 10.1021/acsami.1c04369
Jinwei Chen _{1,

2} , Haiyan Tang ₁ , Meng Huang ₁ , Yong Yan ₁ , Jin Zhang ₁ , Honggang Liu ₁ , Jie Zhang ₁ , Gang Wang ₁ , Ruilin Wang _{1,

2}

Affiliation

Oxygen vacancy plays an important role in catalytic oxidation of formaldehyde (HCHO), but the inherent drawback of its thermodynamic instability causes the deactivation of catalysts. Hence, improving the thermodynamic stability of oxygen vacancy is a crux during HCHO oxidation. Here, a novel and simple nitrogen doping of MnO₂/C catalyst is designed for HCHO oxidation at room temperature. The surface lattice oxygen of MnO₂ will be activated by nitrogen-doping, which acts as active sites for HCHO oxidation and solves the thermodynamic instability issue of oxygen vacancy. Furthermore, carbon is doped with nitrogen to promote electron transfer and accelerate the HCHO oxidation process. Therefore, the catalytic activity and stability of the catalyst can be significantly promoted, which can completely remove ∼1 ppm HCHO in the tank within 3 h, and remains highly active after 5 cycles at room temperature (RH = 55%). In addition, the excellent removal performance over the prepared catalyst is also attributed to abundant surface oxygen species, amorphous crystallinity, and low reduction temperature. In situ diffuse reflectance infrared Fourier transform spectrometry (DRIFTS) and density functional theory (DFT) calculations reveal the reaction mechanism of HCHO. This strategy provides crucial enlightenment for designing novel Mn-based catalysts for application in the HCHO oxidation field.

中文翻译：

掺氮二氧化锰的表面晶格氧活化作为室内 HCHO 分解的有效且持久的催化剂

氧空位在甲醛（HCHO）的催化氧化中起着重要作用，但其热力学不稳定性的固有缺点导致催化剂失活。因此，提高氧空位的热力学稳定性是 HCHO 氧化过程中的关键。在这里，设计了一种新型且简单的氮掺杂 MnO ₂ /C 催化剂，用于室温下的 HCHO 氧化。MnO ₂的表面晶格氧将通过氮掺杂激活，作为 HCHO 氧化的活性位点并解决氧空位的热力学不稳定性问题。此外，碳掺杂氮以促进电子转移并加速 HCHO 氧化过程。因此，可以显着提高催化剂的催化活性和稳定性，可以在 3 小时内完全去除罐中约 1 ppm 的 HCHO，并在室温（RH = 55%）下循环 5 次后仍保持高活性。此外，所制备的催化剂优异的去除性能也归功于丰富的表面氧物种、无定形结晶度和较低的还原温度。原位漫反射红外傅里叶变换光谱 (DRIFTS) 和密度泛函理论 (DFT) 计算揭示了 HCHO 的反应机理。

更新日期：2021-06-16

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