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Confining shell-sandwiched Ag clusters in MnO_(2)-CeO_(2)hollow spheres to boost activity and stability of toluene combustion

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Nano Research 2022年第8期15卷 7042-7051页

作者： Menglan Xiao Xueqin Yang Yue Peng Yucong Guo Yuechang Wei Maofa Ge Xiaolin Yu State Key Laboratory for Structural Chemistry of Unstable and Stable Species Beijing National Laboratory for Molecular Sciences(BNLMS)CAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China College of Forestry Henan Agricultural UniversityZhengzhou 450002China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China School of Environment Tsinghua UniversityBeijing 100084China State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing 102249China University of Chinese Academy of Sciences Beijing 100049China

Supported noble metal catalysts have the promising application in volatile organic compounds(VOCs)catalytic combustion but suffer from the deactivation due to noble metal sintering at high temperatures.Herein,we report the construction of shellsandwiched MnO_(2)-Ag-CeO_(2)hollow spheres with remarkable sintering resistance and high activity in toluene combustion.Ag clusters were sandwiched between outer MnO_(2)and inner CeO_(2)shell to enlarge and stabilize metal–support active interface.The unique hollow structure could alter the electronic states of catalysts sites and increase the adsorbed site of reactant molecules.Meanwhile,Mn–Ag–Ce multi-interfaces in MnO_(2)-Ag-CeO_(2)could facilitate the sustainable activation and the stable release of oxygen species via a tandem transfer.The oxygen species at Ag–Mn interface perimeter were instantly replenished by Ag–Ce interface to accelerate a deep oxidation of intermediates,guaranteeing the opening of benzene ring to generate maleic anhydride.This investigation provides a promising method for constructing efficient and sintering-resistant cluster catalysts for VOCs oxidation.

关键词： hollow spheres multi-interfaces toluene combustion active lattice oxygen

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toluene combustion over Pd-Ce_(0.4)Zr_(0.6)O_2 Directly Washcoated Monolithic Catalysts

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Journal of Rare Earths 2007年第6期25卷 715-720页

作者：赵雷洪张庆豹罗孟飞滕波涛谢云龙 Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces Institute of Physical Chemistry Zhejiang Normal University

A Ce0.4Zr0.6O2 washcoat was prepared using an impregnation method, which acted as a host for the active Pd component to prepare a Pd-Ce0.4Zr0.6O2/substrate monolithic catalyst for toluene combustion. The catalyst was characterized by scanning electron microscopy （SEM）, Raman spectroscopy, Brunauner-Emmett-Teller （BET）, and carbon monoxide tonperature-programmed reduction （CO-TPR）. It was found that the washcoat had strong vibration-shock resistance according to an ultrasonic test. The Pd-Ce0.4Zr0.6O2/substrate monolithic catalyst calcined at 400 ℃ showed 95% toluene conversion at a temperature as low as 210 ℃. Furthermore, the lowest temperature for 95% toluene conversion was increased by 40℃ after the catalyst calcined at 900℃, indicating that the catalyst had good thermal stability. The results revealed that the developed catalyst in this study was promising for eliminating volatile organic compounds （VOCs）.

关键词： toluene combustion monolithic catalyst volatile organic compounds rare earths

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Catalytic combustion of toluene over Pd-based monolithic catalysts with a novel washcoat Ce_(0.8)Zr_(0.15)La_(0.05)O_δ

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Journal of Rare Earths 2009年第5期27卷 733-738页

作者：岳雷赵雷洪张庆豹张甜罗孟飞 Zhejiang Key Laboratory for Reactive Chemistry on Solid Surface Institute of Physical ChemistryZhejiang Normal University

Two novel washcoats Ce0.8Zr0.15La0.05Oδ and Ce0.8Zr0.2O2 was prepared by an impregnation method, which acted as a host for the active Pd component to prepare Pd/Ce0.8Zr0.15La0.05Oδ/substrate and Pd/Ce0.8Zr0.2O2/substrate monolithic catalysts for toluene combustion. The washcoats was characterized by X-ray diffraction (XRD), Raman spectroscopy, Brunauner-Emmett-Teller (BET), and H2-temperature-programmed reduction (H2-TPR). The result indicated that both the washcoats had strong vibration-shock resistance according to ultrasonic test. Doping La3+ into CeO2-ZrO2 solid solution could generate more oxygen vacancies, and could inhibit the sinter of CeO2-ZrO2 solid solution when calcined at high temperatures (800, 900 and 1000 °C). The washcoat Ce0.8Zr0.15La0.05Oδ had much better redox properties. The reductive temperature of Ce4+ species shifted to low temperature by 60 °C when the washcoats calcined at high temperatures (800, 900 and 1000 °C). The Pd/Ce0.8Zr0.15La0.05Oδ/substrate monolithic catalyst calcination at 500 °C had the best catalytic activity and the 95% toluene conversion at a temperature as low as 190 °C. When calcined at low temperature (500 and 700 °C), the catalytic activity has little improvement, however, when calcined at high temperature, the catalytic activity of Pd/Ce0.8Zr0.15La0.05Oδ/substrate monolithic catalysts had significant improvement. As catalyst washcoat, the Ce0.8Zr0.15La0.05Oδ had better thermal stability than the washcoat Ce0.8Zr0.2O2, the developed Pd/Ce0.8Zr0.15La0.05Oδ/ substrate monolithic catalyst in this work was promising for eliminating Volatile organic compounds.

关键词： toluene combustion monolithic catalyst volatile organic compounds CeO2-ZrO2 La3+ rare earths

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Pd/silicalite-1: An highly active catalyst for the oxidative removal of toluene

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Journal of Environmental Sciences 2022年第6期34卷 209-219页

作者： Linke Wu Jiguang Deng Yuxi Liu Lin Jing Xiaohui Yu Xing Zhang Ruyi Gao Wenbo Pei Xiuqing Hao Ali Rastegarpanah Hongxing Dai Beijing Key Laboratory for Green Catalysis and Separation Key Laboratory of Beijing on Regional Air Pollution ControlKey Laboratory of Advanced Functional MaterialsEducation Ministry of ChinaLaboratory of Catalysis Chemistry and NanoscienceDepartment of Environmental Chemical EngineeringSchool of Environmental and Chemical EngineeringFaculty of Environment and LifeBeijing University of TechnologyBeijing 100124China

Catalytic combustion is thought as an efficient and economic pathway to remove volatile organic compounds, and its critical issue is the development of high-performance catalytic materials. In this work, we used the in situ synthesis method to prepare the silicalite-1(S-1)-supported Pd nanoparticles(NPs). It is found that the as-prepared catalysts displayed a hexagonal prism morphology and a surface area of 390-440 m^(2)/g. The sample(0.28Pd/S-1-H)derived after reduction at 500°C in 10 vol% H_(2)showed the best catalytic activity for toluene combustion(T50%= 180℃ and T90%= 189℃ at a space velocity of 40,000 m L/(g·hr), turnover frequency(TOFPd) at 160℃ = 3.46 × 10^(-3)sec^(-1), and specific reaction rate at 160℃ = 63.8μmol/(gPd·sec)), with the apparent activation energy(41 k J/mol) obtained over the bestperforming 0.28Pd/S-1-H sample being much lower than those(51-70 k J/mol) obtained over the other samples(0.28Pd/S-1-A derived from calcination at 500℃ in air, 0.26Pd/S-1-im derived from the impregnation route, and 0.27Pd/ZSM-5-H prepared after reduction at 500℃ in 10 vol% H_(2)). Furthermore, the 0.28Pd/S-1-H sample possessed good thermal stability and its partial deactivation due to CO_(2) or H_(2)O introduction was reversible, but SO_(2) addition resulted in an irreversible deactivation. The possible pathways of toluene oxidation over 0.28Pd/S-1-H was toluene → p-methylbenzoquinone → maleic anhydride, benzoic acid, benzaldehyde → carbon dioxide and water. We conclude that the good dispersion of Pd NPs, high adsorption oxygen species concentration, large toluene adsorption capacity, strong acidity,and more Pd~0 species were responsible for the good catalytic performance of 0.28Pd/S-1-H.

关键词： Silicalite-1 Hexagonal prism shape Supported palladium catalyst Volatile organic compound toluene combustion

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