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formaldehyde oxidation on Pd/USY catalysts at room temperature: The effect of acid pretreatment on supports

Journal of Environmental Sciences 2023年第3期125卷 811-822页

作者： Xiaofeng Liu Chunying Wang Yumin Chen Qi Qin Yaobin Li Hong He Center for Excellence in Regional Atmospheric Environment Key Laboratory of Urban Pollutant ConversionChinese Academy of SciencesInstitute of Urban EnvironmentXiamen 361021China University of Chinese Academy of Sciences Beijing 100049China Zhejiang Key Laboratory of Urban Environmental Processes and Pollution Control Chinese Academy of SciencesNingbo Urban Environment Observation and Research Station-NUEORSNingbo 315800China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-environmental SciencesChinese Academy of SciencesBeijing 100085China Xiamen Key Laboratory of Materials for Gaseous Pollutant Control Chinese Academy of SciencesInstitute of Urban EnvironmentXiamen 361021China

The complete catalytic oxidation of formaldehyde (HCHO) to CO_(2)and H_(2)O at room temperature is a green route for indoor HCHO *** is an excellent carrier material for HCHO oxidation due to its large surface area,intricate pores and high adsorption ***,the zeolite-supported noble metal catalysts have currently shown relatively low activity especially at room *** this work,we present a facile acid treatment strategy for zeolite catalysts to improve the hydroxyl concentration and further enhance their catalytic activity for HCHO *** tests illustrated that HCHO could be completely oxidized to CO_(2)and H_(2)O at a nearly 100%conversion rate with a weight hourly space velocity (WHSV) of 150,000 mL/(g·hr) at 25℃,when the support of Pd/USY catalysts was pretreated by hydrochloric acid with a concentration of 0.20 mol/*** characterization results revealed that the active hydroxyl groups originated from the dealumination in the acid treatment play a key role in the HCHO oxidation *** deduced reaction mechanism suggests that bridging hydroxyl groups may oxidize HCHO to dioxymethylene(DOM) species and terminal hydroxyl groups are responsible for the transformation of DOM groups to formate (HCOO) species.

关键词： formaldehyde oxidation USY zeolite Acid treatment Hydroxyl groups

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Light-enhanced metal-support interaction for synergetic photo/thermal catalytic formaldehyde oxidation

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Journal of Materials Science & Technology 2023年第36期167卷 74-81页

作者： Jiawei Ye Linxi Wang Bicheng Zhu Bei Cheng Rongan He Laboratory of Solar Fuel Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430078China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Hunan Key Laboratory of Applied Environmental Photocatalysis Changsha UniversityChangsha 410022China

The strong metal-support interaction(SMSI)plays a pivotal role in regulating electronic properties and activating surface oxygen *** this work,we report light-irradiation-modulated SMSI for enhanced formaldehyde(HCHO)***,the SMSI between Pt nanoparticles(NPs)and Bi_(2)MoO_(6)cre-ated surface-active oxygen at Pt-Bi_(2)MoO_(6)interfaces to activate HCHO to dioxymethylene(DOM).Notably,light irradiation boosted the SMSI and catalytic ***,photogenerated holes in Bi_(2)MoO 6 im-proved HCHO adsorption and activation,while photogenerated electrons migrated from Bi_(2)MoO_(6)to Pt NPs to promote O_(2)adsorption and activation,accelerating the oxidation of DOM to CO_(2)and H_(2)*** light-modulated SMSI and the synergy between photocatalysis and thermocatalysis lead to enhanced cat-alytic oxidation activity,providing a practical strategy for indoor volatile organic compound(VOC)de-composition under ambient conditions.

关键词： formaldehyde oxidation Strong metal-support interaction Photocatalysis Photo-thermal synergy Electron transfer

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Catalytic activities and mechanism of formaldehyde oxidation over gold supported on MnO2 microsphere catalysts at room temperature

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Frontiers of Environmental Science & Engineering 2016年第3期10卷 447-457页

作者： Guanglong PANG Donghui WANG Yunhong ZHANG Chunyan MA Zhengping HAO Institute of Chemical Physics School of Chemistry Beijing Institute of Technology Beijing 100081 China Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing 100085 China Research Institute of Chemical Defense Beijing 100191 China

MnO2 microspheres with various surface structures were prepared using the hydrothermal method, and Au/MnO2 catalysts were synthesized using the sol-gel method. We obtained three MnO2 microspheres and Au/MnO2 samples： coherent solid spheres covered with wire-like nanostructures, solid spheres with nanosheets, and hierarchical hollow microspheres with nanoplatelets and nanorods. We investigated the properties and catalytic activities of formaldehyde oxidation at room temperature. Crystalline structures of MnO2 are the main factor affecting the catalytic activities of these samples, and γ- MnO2 shows high catalytic performance. The excellent redox properties are responsible for the catalytic ability of γ-MnO2. The gold-supported interaction can change the redox properties of catalysts and accelerate surface oxygen species transition, which can account for the catalytic activity enhancement of Au/MnO2. We also studied intermediate species. The dioxymethylene （DOM） and formate species formed on the catalyst surface were considered intermediates, and were ultimately transformed into hydrocarbonate and carbonate and then decomposed into CO2. A proposed mechanism of formaldehyde oxidation over Au/MnO2 catalysts was also obtained.

关键词： MnO2 microspheres Au/MnO2 formaldehyde oxidation γ-MnO2

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The effect of hydrogen reduction of α-MnO_(2) on formaldehyde oxidation: The roles of oxygen vacancies

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Chinese Chemical Letters 2023年第3期34卷 171-174页

作者： Liping Zhou Chunying Wang Yaobin Li Xiaofeng Liu Hua Deng Wenpo Shan Hong He College of Resources and Environmental Sciences Fujian Agriculture and Forestry UniversityFuzhou 350002China Center for Excellence in Regional Atmospheric Environment Key Laboratory of Urban Pollutant ConversionInstitute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China Zhejiang Key Laboratory of Urban Environmental Processes and Pollution Control Ningbo Urban Environment Observation and Research StationInstitute of Urban EnvironmentChinese Academy of SciencesNingbo 315800China State Key Joint Laboratory of Environment Simulation and Pollution Control Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China

A series of α-MnO_(2) catalysts with various Mn valence states were treated by hydrogen reduction for different periods of time. Their catalytic capacity for formaldehyde(HCHO) oxidation was evaluated. The results indicated that hydrogen reduction dramatically improves the catalytic performance of α-MnO_(2) in HCHO oxidation. The α-MnO_(2) sample reduced by hydrogen for 2 h possessed superior activity and could completely oxidize 150 ppm HCHO to CO_(2) and H_(2)O at 70℃. Multiple characterization results illustrated that hydrogen reduction contributed to the production of more oxygen vacancies. The oxygen vacancies on the catalyst surface enhanced the adsorption, activation and mobility of O_(2) molecules, and thereby enhanced HCHO catalytic oxidation. This study provides novel insight into the design of outstanding MnO_x catalysts for HCHO oxidation at low temperature.

关键词： Hydrogen reduction α-MnO_(2) formaldehyde oxidation Oxygen vacancies

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Gold stabilized on various oxide supports catalyzing formaldehyde oxidation at room temperature

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Chinese Journal of Catalysis 2016年第10期37卷 1729-1737页

作者：陈冰冰朱晓兵王宜迪于丽梅石川大连理工大学化学学院精细化工国家重点实验室辽宁大连116024 大连理工大学等离子体物理化学实验室辽宁大连116024

Gold stabilized on reducible oxide （CeO2 and FeOx） and irreducible oxide （γ‐Al2O3, SiO2, and HZSM‐5） were prepared by deposition precipitation method and tested for catalytic oxidation of formaldehyde （HCHO） at room temperature under high GHSV of 600000 ml/（g＆#183;s）. Au/γ‐Al2O3 cata‐lyst showed distinctive catalytic performance, presenting the highest initial HCHO conversion and stability. Correlating the reaction rate with Au particle size, there is a linear relationship, suggesting that the smaller Au particle size with higher dispersion possesses high reactivity for HCHO oxida‐tion. All the catalysts deactivated at high GHSV （600000 ml/（g＆#183;s））, but in a quite different rate. Re‐ducible oxide （CeO2 and FeOx） could stabilize gold through O linkage and therefore exhibits a better stability for HCHO oxidation reaction. However, the aggregation of gold particles occurred over Au/SiO2 and Au/HZSM‐5 catalysts, which result in the fast deactivation. Therefore, our results sug‐gest that the reducibility of the supports for Au catalysis has no direct influence on the activity, but affects the catalytic stability.

关键词： Gold catalyst Oxide support formaldehyde oxidation Reducibility Catalytic stability

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Ag-Based Catalysts in Different Supports: Activity for formaldehyde oxidation

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Advances in Materials Physics and Chemistry 2022年第8期12卷 163-176页

作者： Rached Ousji Zouhaier Ksibi Abdelhamid Ghorbel Céline Fontaine Laboratory of Materials Chemistry and Catalysis Faculty of Sciences of Tunis University of Tunis El Manar Tunis Tunisia Institute of Chemistry of Poitiers: Materials and Natural Resources (IC2MP) University of Poitiers Poitiers France

Through the impregnation method, Ag catalysts with different support (such as TiO2 and γ-Al2O3) were prepared and then tested for catalytic oxidation of formaldehyde (HCHO) at low temperatures. The Ag/TiO2 catalyst exhibited strong catalytic performance, converting HCHO to CO2 and H2O at around 95°C. However, the Ag/Al2O3 catalysts showed much lower activity and reached 100% conversion at 125°C. The Ag-based catalysts were next characterized by several methods (XRD, TEM, FT-R, BET and H2-TPR). Results of characterization revealed that support dramatically impacts the size and dispersion of Ag particles. The XRD analysis showed the existence of different peaks of the silver on the surface of Al2O3 in the contrast with TiO2 no specific peaks exist. Therefore, the size of the Ag particles and their dispersion are the most important factors that affect their catalytic performance for formaldehyde oxidation. In terms of catalytic performance for HCHO oxidation, the Ag/TiO2 catalyst possesses the best Ag dispersion, as well as the smallest Ag particle size.

关键词： formaldehyde oxidation TiO2 Al2O3 Silver (Ag) Impregnation Sol-Gel

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Preparation of birnessite-supported Pt nanoparticles and their application in catalytic oxidation of formaldehyde

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Journal of Environmental Sciences 2012年第6期24卷 1117-1124页

作者： Linlin Liu Hua Tian Junhui He Donghui Wang Qiaowen Yang Functional Nanomaterials Laboratory and Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and Chemistry(TIPC)Chinese Academy of SciencesBeijing 100190China School of Chemical&Environmental Engineering China University of Mining&TechnologyBeijing 100083China Research Institute of Chemical Defense Beijing 100083China

Flaky and nanospherical birnessite and birnessite-supported Pt catalysts were successfully prepared and characterized by means of Xray diffraction （XRD）,transmission electron microscopy （TEM）,energy dispersive spectroscopy （EDS） and N2 *** of the birnessite morphology and Pt reduction method on the catalytic activity for the complete oxidation of formaldehyde （HCHO） were *** was found that flaky birnessite exhibited higher catalytic activity than nanospherical *** promoting effect of Pt on the birnessite catalyst indicated that the reduction method of the Pt precursor greatly influenced the catalytic *** birnessite-supported Pt nanoparticles reduced by KBH 4 showed the highest catalytic activity and could completely oxidize HCHO into CO2 and H2O at 50℃,whereas the sample reduced using H2-plasma showed lower activity for HCHO *** differences in catalytic activity of these materials were jointly attributed to the effects of pore structure,surface active sites exposed to HCHO and the dispersion of Pt nanoparticles.

关键词： birnessite manganese oxide noble metals formaldehyde oxidation

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Low-temperature catalytic oxidation of formaldehyde over Co_3O_4catalysts prepared using various precipitants

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Chinese Journal of Catalysis 2016年第6期37卷 947-954页

作者：范泽云张志翔房文健姚鑫邹谷初上官文峰上海交通大学燃烧与环境技术研究中心上海200240

Co3O4 catalysts prepared with different precipitants（NH3·H2O,KOH,NH4HCO3,K2CO3 and KHCO3）were investigated for the oxidation of formaldehyde（HCHO）.Among these,KHCO3-precipitated Co3O4（KHCO3-Co） was the most active low-temperature catalyst,and was able to completely oxidize HCHO at the 100-ppm level to CO2 at 90℃.In situ diffuse reflectance infrared spectroscopy demonstrated that hydroxyl groups on the catalyst surface were regenerated by K~＋ and CO3^（2-）,thus promoting the oxidation of ***,H2-temperature programmed reduction and X-ray photoelectron spectroscopy showed that employing KHCO3 as the precipitant increased the Co^3＋/Co^2＋molar ratio on the surface of the Co3O4 catalyst,thus further promoting *** characterization revealed that catalysts precipitated with carbonate or bicarbonate reagents exhibited greater specific surface areas and pore ***,these data suggest that the high activity observed during the Co3O4 catalyzed oxidation of HCHO can be primarily attributed to the presence of K~＋ and CO3^（2-） on the Co3O4 surface and the favorable Co^3＋/Co^2＋ ratio.

关键词： formaldehyde oxidation Catalysis Cobalt oxide Precipitation method Potassium ion

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Density functional theory calculations on single atomic catalysis:Ti-decorated Ti3C2O2 monolayer(MXene)for HCHO oxidation

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Chinese Journal of Catalysis 2020年第10期41卷 1633-1644页

作者： Junhui Zhou Guanlan Liua Quanguo Jiang Weina Zhao Zhimin Ao Taicheng An Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control Guangzhou Key Laboratory Environmental Catalysis and Pollution ControlSchool of Environmental Science and EngineeringInstitute of Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006GuangdongChina The College of Mechanics and Materials Hohai UniversityNanjing 211100JiangsuChina

formaldehyde(HCHO) is a common indoor pollutant, long-term exposure to HCHO may harm human health. Its efficient removal at mild conditions is still challenging. The catalytic oxidation of HCHO molecules on a single atomic catalyst, Ti-decorated Ti3C2O2(Ti/Ti3C2O2) monolayer, is investigated by performing the first principles calculations in this work. It demonstrates that Ti atoms can be easily well dispersed at the form of single atom on Ti3C2O2 monolayer without aggregation. For HCHO catalytic oxidation, both Langmuir-Hinshelwood(LH) and Eley-Rideal(ER) mechanisms are considered. The results show that the step of HCHO dissociative adsorption on Ti/Ti3C2O2 with activated O2 can release high energy of 4.05 e V based on the ER mechanism, which can help to overcome the energy barrier(1.04 e V) of the subsequent reaction steps. The charge transfer from *OH group to CO molecule(dissociated from HCHO) not only promotes *OH group activation but also plays an important role in the H2 O generation along the ER mechanism. Therefore, HCHO can be oxidized easily on Ti/Ti3C2O2 monolayer, this work could provide significant guidance to develop effective non-noble metal catalysts for HCHO oxidation and broaden the applications of MXene-based materials.

关键词： formaldehyde oxidation MXene Ti/Ti3C2O2 monolayer Single atomic catalysts Non-noble metal catalyst

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Top-down synthesis strategies: Maximum noble-metal atom efficiency in catalytic materials

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Chinese Journal of Catalysis 2017年第9期38卷 1588-1596页

作者： Yaxin Chen Zhiwei Huang Xiao Gu Zhen Ma Jianmin Chen Xingfu Tang Institute of Atmospheric Sciences Shanghai Key Laboratory of Atmospheric Particle Pollution & Prevention (LAP3) Department of Environmental Science & Engineering Fudan University Shanghai 200433 China Department of Applied Physics Chongqing University Chongqing 401331 China Jiangsu Collaborative Innovation Center of Atmospheric Environment and Equipment Technology (CICAEET) Nanjing University of Information Science & Technology Nanjing 210044 Jiangsu China

Top‐down synthesis has been used to prepare catalytic materials with nanometer sizes,but fabricating atomically dispersed metal catalysts remains a challenge because surface single metal atoms are prone to aggregation or coalescence.A top‐down strategy is used to synthesize atomically dispersed metal catalysts,based on supported Ag *** changes of the geometric and electronic structures of the Ag atoms during the top‐down process are studied using the in situ synchrotron X‐ray diffraction technique,ex situ X‐ray absorption spectroscopy,and transmission electron *** experimental results,coupled with the density functional theory calculations,demonstrate that the electronic perturbation of the Ag frontier orbitals,induced by the Ag‐O interactions at the perimeter of the metal‐support interface,is the driving force of the top‐down *** top‐down synthesis has two important functions:to increase the number of catalytic active sites and to facilitate the study of complex reaction mechanisms(e.g.,formaldehyde oxidation)by developing single‐site model catalysts.

关键词： Top‐down synthesis Atomic dispersion Catalytic active site Electronic metal‐support interaction formaldehyde oxidation

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