Fe₁/G上NO的还原反应

Yang, W.; Gao, Z.; Liu, X.; Ma, C.; Ding, X.-L.; Yan, W., Directly Catalytic Reduction of NO without NH₃ by Single Atom Iron Catalyst: A DFT Calculation, Fuel, 243, 262-270, 2019.

一氧化氮（NO）是一类重要的大气污染物，其排放受到严格的控制。NH₃选择性催化还原NO技术成熟、高效，但仍存在一些缺陷（氨泄漏、二次微粒形成、设备腐蚀等）。本文选择石墨烯的单缺陷位负载Fe₁（Fe/SV-G）作为催化剂，通过通过密度泛函理论计算，详细研究了NO分子在其上的还原反应过程。研究发现，可以在较低能垒的情况下实现NO→ N₂O→ N₂的还原过程，且两步反应均为放热反应。对于反应产生的吸附态氧原子，推测可与尾气中的CO反应去除，从而实现催化循环。该理论研究结果可为无氨脱硝除提供新的思路。

图 Fe₁/G上NO的还原反应机理

这方面的系列工作如下：

1.    Gao, Z.-Y.; Yang, W.-J.; Ding, X.-L.; Lv, G.; Yan, W.-P., Support Effects on Adsorption and Catalytic Activation of O₂ in Single Atom Iron Catalysts with Graphene-Based Substrates, Phys. Chem. Chem. Phys. 20, 7333-7341 (2018).

2.    Yang, W.; Gao, Z.; Liu, X.; Li, X.; Ding, X.-L.; Yan, W., Single-Atom Iron Catalyst with Single-Vacancy Graphene-Based Substrate as a Novel Catalyst for NO Oxidation: A Theoretical Study, Catal. Sci. Technol. 8, 4159-4168 (2018).

3.    Gao, Z.-Y.; Sun, Y.; Li, M.-H.; Yang, W.-J.; Ding, X.-L., Adsorption Sensitivity of Fe Decorated Different Graphene Supports toward Toxic Gas Molecules (CO and NO), Appl. Surf. Sci. 456, 351-359 (2018).

4.    Gao, Z.; Yang, W.; Ding, X.; Lv, G.; Yan, W., Support Effects in Single Atom Iron Catalysts on Adsorption Characteristics of Toxic Gases (NO₂, NH₃, SO₃ and H₂S), Appl. Surf. Sci. 436, 585-595 (2018).

5.    Yang, W.; Gao, Z.; Ding, X.; Lv, G.; Yan, W., The Adsorption Characteristics of Mercury Species on Single Atom Iron Catalysts with Different Graphene-Based Substrates, Appl. Surf. Sci. 455, 940-951 (2018).

6.    Yang, W.; Gao, Z.; Liu, X.; Ding, X.-L.; Yan, W., The Adsorption Characteristics of As₂O₃, Pb⁰, PbO and Pbcl₂ on Single Atom Iron Adsorbent with Graphene-Based Substrates, Chem. Eng. J. 361, 304-313 (2019).

7.    Yang, W.; Gao, Z.; Liu, X.; Ma, C.; Ding, X.-L.; Yan, W., Directly Catalytic Reduction of NO without NH₃ by Single Atom Iron Catalyst: A DFT Calculation, Fuel 243, 262-270 (2019).