Selective Catalytic Reduction of NO xby Methanol on Metal-Free Zeolite with Brønsted and Lewis Acid Pair
Selective Catalytic Reduction of NO xby Methanol on Metal-Free Zeolite with Brønsted and Lewis Acid Pair
复制标题
布伦斯特德和路易斯酸对在无金属沸石上通过甲醇选择性催化还原 NO x
DOI：
10.1021/acscatal.1c05624
复制
发表时间：
2022
期刊：
影响因子：
12.9
通讯作者：
Chen H.
中科院分区：
文献类型：
--
作者：
Han F.;Sun H.;Zhao Z.;Xu Y.;Dong H.;Liu W.;Sun L.;Wang Z.;Hou G.;Kitano M.;Li W.;Shen M.;Chen H.
钒基催化剂上的氨选择性催化还原脱硝技术（NH3-SCR）目前在世界范围内广泛应用于工业废气处理，而废催化剂的处置面临着有毒钒带来的高度环境风险。本文提出了一种环境友好的脱硝方法，即以甲醇代替NH3，以H-FER沸石为催化剂，采用甲醇-选择性催化还原法（CH 3OH-SCR）。这种具有布朗斯特酸和刘易斯酸对的无金属沸石显示出比大多数研究的贵金属催化剂（Ag/Al 2 O3）高几乎4倍的活性。此外，它显示出与钒基催化剂上的NH3-SCR的最新技术相当的脱NOx效率，以及具有工业应用潜力的良好稳定性。傅里叶变换红外光谱（FT-IR），原位核磁共振，和理论计算表明，固体酸物种是高活性的CH 3OH-SCR反应。提出了一种基于Si-O（H）-Al位和相邻骨架外铝（EFAL）物种之间协同催化效应的反应机理。
The selective catalytic reduction deNOxtechnology by ammonia (NH3-SCR) on vanadium-based catalysts is now being used worldwide for industrial exhaust treatment, while the disposal of spent catalysts faces a high level of environmental risk posed by poisonous vanadium. We present here an environmentally friendly deNOxmethod with pure H-FER zeolite as the catalyst using methanol as a reductant instead of NH3(CH3OH-SCR). This metal-free zeolite with Brønsted and Lewis acid pairs shows almost 4 times higher activity than the most investigated precious metal catalyst (Ag/Al2O3). Furthermore, it shows a comparable deNOxefficiency with state-of-the-art of NH3-SCR on vanadium-based catalysts, as well as good stability with potential for industrial application. Operando Fourier transform infrared (FT-IR), in situ NMR, and theoretical calculations demonstrated that solid acid species are highly active for the CH3OH-SCR reaction. A reaction mechanism based on a synergistic catalytic effect between Si–O(H)–Al sites and neighboring extra-framework aluminum (EFAL) species has been proposed.