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Materials · 2024 ·Vol. 17 ·期 9 ·2103 · IF 3.1

Catalytic Oxidation of Chlorobenzene over Amorphous Manganese-Chromium Catalysts Supported by UiO-66-Derived ZrOx

Pengfei Zhu,Qiaosen Yuan,Na Li,Zhaoxia Hu,Shouwen Chen

The development of efficient catalysts with longevity to remove chlorobenzene is challenging due to Cl poisoning. Herein, a series of Mn-Cr/ZrOxcatalysts supported by Zr-based metal-organic framework (UiO-66)-derived ZrOxwas prepared and investigated for chlorobenzene (CB) catalytic oxidation. MnCr/ZrOx-M prepared via a wet impregnation method presented an amorphous structure, indicating the homogeneous dispersion of Cr and Mn, which improved acid and redox properties. 40Mn7Cr3/ZrOx-M exhibited the best catalytic activity for chlorobenzene oxidation with T90of 293 °C, which is mainly due to the strong interaction between manganese and chromium promoted by the large specific surface area of the ZrOxsupport. Furthermore, 40Mn7Cr3/ZrOx-M presented excellent stability for chlorobenzene oxidation.

研究领域: 环境科学 · 催化化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

Impact of Cu content on the activity of TiO2-based catalysts for toluene oxidation

Yaqi Wu,Jianhua Qian,Jinjuan Xing,Junhua Li,He Huang,Yanan Wang,Jiasheng Xu

Toluene is one of the most toxic contaminants in industrial waste gases, it can enter the body through the respiratory system and skin. Long-term exposure to it can lead to skin inflammation and neurasthenia, and even cause lesions in organs. Over the years, catalytic oxidation technology has been extensively employed to the remove of toluene, and oxides, especially copper oxide, is considered to be an effective catalyst technology and has been extensively studied. In this work, we introduced CuO as an active species to investigate the impact of Cu content in TiO 2 @CuO (TC-x, x=1, 2, 3, and 5) catalyst on the activity, reusability, and stability of toluene oxidation. The result demonstrated that the addition of Cu species, facilitating the generation of active oxygen obviously reduced the complete oxidation temperature of toluene. Among them, TC-3 catalyst exhibited the highest activity (T 50 = 234 ℃, T 90 = 289 ℃, and T 100 = 310 ℃, with C toluene =1000 ppm, WHSV=20,000 mL/ (g h)), great reusability, and stability for toluene degradation. According to the in-situ DRIFTS, the ultimate degradation products of toluene were CO 2 and H 2 O, which were clean and free of secondary pollution.

CAS / MDL: 6046-93-1 6153-56-6
研究领域: 环境科学 · 催化化学
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Journal of Energy Chemistry · 2014 · IF 0

Efficient oxidation of ethylbenzene catalyzed by cobalt zeolitic imidazolate framework ZIF-67 and NHPI

Hongyan Li,Hong Ma,Xinhong Wang,Jin Gao,Chen Chen,Song Shi,Minjie Qu,Na Feng,Jie Xu

Efficient catalytic oxidation of ethylbenzene to acetophenone was realized using the catalytic system of cobalt zeolitic imidazolate framework ZIF-67/N-hydroxyphthalimide (NHPI) under mild conditions. 95.2% conversion of ethylbenzene with 90.3% selectivity to acetophenone could be obtained at 373 K under 0.3 MPa O 2 for 9 h. The results show that there exists synergetic effect between ZIF-67 and NHPI. 1-Phenylethyl hydroperoxide (PEHP) was generated via a radical process involving the hydrogen abstraction from ethylbenzene by phthalimide N-oxyl, and subsequently effectively decomposed to acetophenone by ZIF-67.

CAS / MDL: 693-98-1
研究领域: 催化化学 · 材料科学
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CHEMICAL PAPERS · 2017 ·Vol. 72 ·期 1 ·51-56 · IF 1.258

The Cu(I)- and HNO3-catalyzed oxidation of substituted toluenes to the benzoic acid based on NO x recycling

Wei Mengyi,Qian Chao,Chen Xinzhi

Based on the recycling of NO x , the Cu(I)- and HNO 3 -catalyzed oxidation of 2-chloro-4-(methylsulfonyl)toluene to 2-chloro-4-(methylsulfonyl)benzoic acid has been developed with an excellent yield of 84.2% and a purity of 99.7%. The optimized reaction conditions (160 °C, oxygen pressure 1.5 MPa, HNO 3 concentration 25 wt%, HNO 3 : substrate 0.5:1) use 1.0 mol% CuI as catalyst. The dosage of HNO 3 in the new process is only 25% of the stoichiometric amount and 12.5% of the amount of the traditional process. The NO x emission is 5% amount of the traditional process. The oxidation of several additional toluene derivatives with comparable yields demonstrates the generality to these reaction conditions.

研究领域: 化学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Unraveling the importance between electronic intensity and oxygen vacancy on photothermocatalytic toluene oxidation over CeO2

Ying-juan Hao,Yue-guang Ma,Xiao Zhang,Jianjun Li,Saifei Wang,Xuemin Chen,Fa-tang Li

Developing low-temperature, high-efficiency and anti-poisoning catalysts is crucial for VOCs removal. CeO 2 materials with different electron density are prepared via regulation on facets and oxygen vacancies. It reveals that high electron density of materials plays a decisive role in the production of reactive oxygen species, reducibility of surface lattice oxygen and improvement of photothermocatalytic activity for toluene oxidation compared with highly concentrated oxygen vacancies and large special surface area. Photothermocatalytic conversion rate for 1500 ppm of toluene over the optimized defective CeO 2 could reach 93 % at 145 °C under the gas hourly space velocity of 60,000 mL·g −1 ·h −1 . H 2 -TPR result shows that excessive oxygen vacancies are detrimental to the appearance of mobile reactive oxygen species due to the strong chemical interaction and the escape probability of surface lattice oxygen of CeO 2 . It is also found that the decrement of electron density of the recovered sample can account for the slight catalyst deactivation, accompanied by the increasement of bulk oxygen vacancies in the recovered sample, exclusive of disappearance of surface oxygen vacancies, aggregations and deposition of organic carbon. This work provides an insight into the design of high-efficiency non-noble catalysts applied to VOCs removal.

研究领域: 环境科学 · 催化材料
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Photothermal catalytic oxidation of toluene with enhanced efficiency over constructed CuMn2O4/Mn2O3 heterojunction catalyst

Linfeng Nie,Shuangde Li,Shaohua Chai,Ning Han,Yunfa Chen

Photothermal catalyst oxidation of VOCs is a hot issue in the air purifier field due to the reducing of secondary energy consumption. Herein, we reported a photothermal catalyst CuMn 2 O 4 /Mn 2 O 3 with heterojunction for catalytic oxidizing toluene with high efficiency through sol–gel method followed different calcination temperature. Under the irradiation of 700 mW/cm 2 Xe lamp simulated sun light, the CuMn 2 O 4 /Mn 2 O 3 catalyst exhibited excellent full spectrum light absorption capacity, photo-thermal conversion ability and toluene conversion performance with a 90% toluene conversion (T = 233 °C, WHSV = 30,000 mL/g·h), together with a good catalytic stability. The excellent performance can be attributed to the synergistic effect of abundant oxygen vacancies, Mn 3+ active sites and heterojunctions between CuMn 2 O 4 and Mn 2 O 3 due to the XPS, H 2 -TPR, UPS characterizations.

CAS / MDL: 13778-31-9
研究领域: 环境科学 · 催化化学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2019 · IF 3.375

Role of Mineral Nutrients in Plant-Mediated Synthesis of Three-Dimensional Porous LaCoO3

Kuncan Wang,Junjie Huang,Wen Li,Jiale Huang,Daohua Sun,Xuebin Ke,Qingbiao Li

With the assistance of plant extracts, the facile synthesis of three-dimensional (3D) porous LaCoO3 perovskite is reported at a lower calcination temperature of 500 °C. The formation mechanism is carefully studied by investigating the different roles of organic and inorganic components in Cacumenplatycladi extract. The results indicate that organic components (mainly phenolic acids) function as the similar complex species of citric acid, while the mineral nutrients (Na+, K+, Ca2+, and Mg2+) together with NO3– serve as combustion-aid agents even with trace amounts. Moreover, the biosynthesized LaCoO3 has a high surface area of 32.5 m2 g–1 and exhibits excellent catalytic performance for benzene oxidation. Benzene of 1000 ppm can achieve a stable conversion above 90% at 285 °C in a continuous run for 80 h (weight-hourly space velocity (WHSV) = 40 000 mL g–1 h–1). It can be attributed to the bio-LaCoO3 with more electrophilic adsorption of oxygen species and 3D porous structure.

研究领域: 材料科学 · 环境科学
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JOURNAL OF CATALYSIS · 2023 · IF 7.3

Electron donation promotes the dual activation of lattice oxygen and molecular oxygen: The Pt-Pd/CeO2 catalyst efficiently catalyzes toluene

Lei Wang,Yonggang Sun,Yulong Ma,Min Xu,Juan Zhang,Yingbo Zhu,Jie Ding,Li Zhu,Jing Ma,Wenxin Ji,Liqiong Wang,Yuanyuan Li

Dual activation of molecular and lattice oxygen is an important step in the catalytic oxidation of volatile organic compounds. Herein, CeO 2 was derived from MOF as an electron donor support to develop a co-catalyst with Pt-Pd alloy nanoparticles (Pt-Pd/CeO 2 ). The Prepared Pt-Pd/CeO 2 exhibits excellent catalytic activity towards toluene oxidation, showing a turnover frequency (TOF 0.26 s −1 ) higher than those of Pt/CeO 2 (0.05 s −1 ) and Pd/CeO 2 (0.02 s −1 ). Several in situ experimental techniques and density functional theory calculations have revealed that the introduction of Pd valence electrons can intensify the electronic metal-support interactions (EMSIs) effects of Pt-Pd/CeO 2 catalysts, which can weaken the Ce-O bond, thereby promoting the production and circulation of lattice oxygen and oxygen vacancies, and modulating the d -band centre to enhance the adsorption and activation of reactants. This study presents a comprehensive investigation of toluene oxidation on alloy-supported catalysts, providing practical guidance for designing reliable catalysts suitable for industrial applications.

CAS / MDL: 16774-21-3 110-17-8
研究领域: 催化化学 · 环境科学 · 材料科学
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2021 ·Vol. 28 ·期 28 ·37592-37602 · IF 4.223

The improved activity of Co3O4 nanorods using silver in the catalytic oxidation of toluene

Li Tao,Zhao Jinxian,Quan Yanhong,Luo Dongmou,Miao Chao,Ren Jun

Co 3 O 4 nanorods with diameters of ~0.15 μm and lengths of ~1 μm were prepared using a hydrothermal method via the assembly of microcrystals and tested in the catalytic oxidation of toluene. The catalytic performance of Co 3 O 4 nanorods was improved by the addition of Ag at various concentrations, and the 7% Ag/Co 3 O 4 catalyst achieves a toluene conversion of 90% at 256 °C with a space velocity of 78,000 mL g −1 h −1 , which is much lower than that of the pristine Co 3 O 4 (269 °C). The addition of Ag promoted the activation of the surface oxygen species and the formation of more oxygen vacancies, improving the relative low-temperature reducibility of Co 3 O 4 , which is favorable for toluene oxidation. Moreover, the 7% Ag/Co 3 O 4 catalyst showed an excellent stability for toluene oxidation at 250 and 260 °C for 50 h under the same conditions.

研究领域: 材料科学 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

A novel CeO2 nanowire catalyst prepared by the freeze-drying method with significantly improved catalytic performance for toluene oxidation

Huiao Liu,Yan Li,Ziying Hu,Xinhui Hao,Hongpeng Jia,Jing Chen,Can-Zhong Lu

A wire like CeO 2 catalyst (CeO 2 -w) was obtained after the calcination of the precursor at 400 °C, which was prepared by the freeze-drying method for the first time. It shows good performance for catalytic oxidation of toluene with T 90 of 220 °C, which is much better than the CeO 2 catalysts with other structures prepared by the different methods. The good performance of CeO 2 -w is due to the bigger pore volume, more active oxygen species, more oxygen vacancies, better low temperature reducibility, higher surface area normalized reaction rates and lower E a value. Additionally, the CeO 2 -w catalyst exhibits good water resistance and catalyst stability. In situ DRIFTS indicates the catalytic oxidation of toluene on CeO 2 -w undergoes the progress of toluene → benzaldehyde → benzoic acid → maleic acid → CO 2 and H 2 O. This work affords a new idea to prepare high active CeO 2 nanowire catalysts for catalytic oxidation of toluene, and open an efficient way for the construction of CeO 2 based composite catalysts for VOCs degradation.

研究领域: 材料科学 · 环境科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Weakened Mn–O bond in Mn–Ce catalysts through K doping induced oxygen activation for boosting benzene oxidation at low temperatures

Xi Chen,Xiaoyan Wang,Ziliang Jia,Chao Yang,Zhihong Liu,Yuexing Wei,Mengxue Wang,Meisheng Liang

K-doped Mn–Ce solid solution catalysts were synthesized using a combination of coprecipitation and hydrothermal methods, demonstrating excellent performance in benzene oxidation. The catalyst K 1 Ce 5 Mn 5 exhibited comparable activity to noble metal catalysts, achieving a 90 % benzene conversion at approximately 194 ℃. Durable tests under dry and moist conditions revealed that the catalyst could maintain its activity for 50 h at 218 ℃ and 236 ℃, respectively. Characterization results indicated that the catalyst’s enhanced activity resulted from the weakened Mn–O bonding caused by the introduction of K + , facilitating the activation of oxygen and its involvement in the reaction. CeO x , the main crystalline phase of Mn–Ce solid solutions, provided abundant oxygen vacancies for capturing and activating oxygen molecules for the weakened Mn–O structures. This conclusion was further supported by partial density of state analysis from density functional theory computations, revealing that the introduction of K + weakened the orbital hybridization of Mn3d and O2p. Finally, in situ diffuse reflectance infrared Fourier-transform spectroscopy ( in situ DRIFTS) studies on Ce 5 Mn 5 and K 1 Ce 5 Mn 5 catalysts suggested that the introduction of K + promoted the conversion of adsorbed benzene. Furthermore, intermediate products were transformed more rapidly for K 1 Ce 5 Mn 5 compared to Ce 5 Mn 5 .

CAS / MDL: 10294-41-4 10377-66-9
研究领域: 催化化学 · 环境科学 · 材料科学
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Molecular Catalysis · 2024 · IF 3.9

Unveiling the crucial active sites responsible for CO, n-heptane, and toluene oxidation over Pt/ZrO2 catalyst

Wen-Xia Zhang,Xi Zhao,Lin-Ya Xu,Shuang Xia,Yu-Fen Zhou,Chong-Lai Chen,Hai-Hua He,Meng-Fei Luo,Jian Chen

The surface Pt species and adsorbed oxygen on the Pt/ZrO 2 catalyst were successfully modulated by altering the preparation methods, resulting in distinct catalytic behaviors for CO, n-heptane, and toluene oxidation. The Pt/ZrO 2 catalyst was initially prepared via wetness impregnation and subsequently reduced in an H 2 atmosphere to obtain the Pt/ZrO 2 -R catalyst. In contrast, the Pt/ZrO 2 -E catalyst was synthesized using ethanol solvent (also serving as a reducing agent) instead of water during wetness impregnation. Moreover, the pre-prepared Pt nanoparticles were loaded onto the ZrO 2 surface using polyvinylpyrrolidine (as a protective and structure directing agent) dissolved in ethanol solvent to fabricate the Pt/ZrO 2 -EP catalyst. Among these catalysts, the Pt/ZrO 2 -R exhibits superior catalytic activity towards CO oxidation due to its abundant metallic Pt species. It is found that activity of Pt/ZrO 2 catalyst for n-heptane oxidation is positively correlated with its surface adsorbed oxygen concentration, thus the highest activity is achieved over the Pt/ZrO 2 -EP catalyst possessing a higher concentration of surface adsorbed oxygen species. Unlike CO and n-heptane oxidation, toluene oxidation activity is affected by multiple factors, it is primarily promoted by synergistic catalysis between metallic Pt species (Pt 0 ) and surface adsorbed oxygen species over the Pt/ZrO 2 -EP catalyst. Our preliminary findings underscore that precise modulation of sensitive active sites on surfaces plays a critical role in specific catalytic reactions.

CAS / MDL: 9003-39-8
研究领域: 催化化学 · 材料科学 · 环境科学
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