原位掺杂衍生物MnOx/Mn-ZrO2-C的高效降解

IF 3.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis Pub Date : 2025-05-29 DOI:10.1016/j.mcat.2025.115243

Qiuju Qin , Chaolian Zhu , Donghai Mo , Zhengjun Chen , Lihui Dong , Bin Li , Liya Zhou

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引用次数: 0

摘要

MnOx具有良好的低温降解NOx活性，但其较差的SO2耐受性限制了其应用。本文提出了一种原位掺杂热解氧化Mn(NO3)2/ uuo -66衍生碳（MnOx/Mn-ZrO2- c）原位构建MnOx负载在Mn掺杂ZrO2载体上的方法，其中Mn取代Zr修饰ZrO2的电子结构。具有丰富表面氧和酸位的MnOx/Mn-ZrO2-C具有优异的活性和较好的抗SO2能力。一系列表征结果表明，Mn掺杂调节了载流子ZrO2的电子结构，增强了MnOx、碳和Mn-ZrO2之间的相互作用，导致Mn和Zr周围的电子云密度增加，从而使MnOx/Mn-ZrO2- c上的Mn和Zr表现出较差的亲硫性。这些发现强调了利用多管齐下的效应来制造高活性和耐硫的NH3-SCR催化剂的好处。

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In situ doping derivative construction of MnOx/Mn-ZrO2-C for efficient degradation of NOx

MnO_x exhibits excellent low temperature activity for degradation NO_x, but its poor SO₂ tolerance restrains its application. Herein, an in situ construction method for MnO_x loading on Mn-doped ZrO₂ carrier with carbon (MnO_x/Mn-ZrO₂-C) derived from Mn(NO₃)₂/UIO-66 by in situ doped pyrolysis–oxidation, in which Mn replaces Zr to modify the electronic structure of the ZrO₂. The MnO_x/Mn-ZrO₂-C with abundant surface oxygen and acid sites showed excellent activity and better SO₂ resistance. A series of characterization results indicated that Mn doping modulates the electron structure of carrier ZrO₂ and enhances the interactions among MnO_x, carbon, and Mn-ZrO₂, resulting in increasing the electron cloud density around Mn and Zr, and consequently, the Mn and Zr on the MnO_x/Mn-ZrO₂-C exhibit poorer sulfiphilic. These findings emphasize the benefits of utilizing a multipronged effect to fabricate highly active and sulfur-resistant NH₃-SCR catalysts.

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来源期刊

Molecular Catalysis Chemical Engineering-Process Chemistry and Technology

CiteScore

6.90

自引率

10.90%

发文量

700

审稿时长

40 days

期刊介绍： Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods