Materials
·
2024
·Vol. 17
·期 9
·2103
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IF 3.1
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
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2023
·
IF 2.8
Zhong Zhihao,Liu Yalan,Liu Shantang
To develop and design highly efficient composite oxide nanoparticles for the combustion of chlorinated volatile organic compounds (CVOCs), a series of Co 3 O 4 /In 2 O 3 catalysts were synthesized and tested for the catalytic oxidation of chlorobenzene (CB) as a typical example for CVOCs. The catalytic performance of as-prepared samples manifested that In x Co 1 O y nanorods catalysts with an appropriate proportion of In/Co exhibited superior catalytic activity better than that of pure Co 3 O 4 nanorods, indicating that the strong interactions between cobalt oxide and indium oxide assisted the degradation of CB. To understand the synergistic mechanism, a series of experimental characterization have been employed to explore the physicochemical properties of the catalysts. The result indicates that the introduction of In 2 O 3 increases the Co 3+ contents and the mobility of surface oxygen species, which synergistically contribute to the degradation process of chlorobenzene. Furthermore, the intermediates that appeared in the process of CB degradation on the In 3 Co 1 O y catalyst have been monitored by in situ DRIFTS. The detailed reaction mechanism is established by the analysis of the intermediates. Graphical Abstract
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
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2015
·
IF 3.615
Jian Wang,Xue Wang,Xiaolong Liu,Junlin Zeng,Yangyang Guo,Tingyu Zhu
In this article, we present a detailed study combining the kinetic studies and in-situ FTIR experiments to investigate the oxidation behavior of chlorobenzene over V 2 O 5 /TiO 2 catalysts. The catalytic data show the 3–5 wt.% V 2 O 5 /TiO 2 catalysts are best fit for the oxidation of chlorobenzene. The calculated apparent reaction orders are about 0.6 and 0.2, respectively. The results of in-situ FTIR provided mechanism insights into the catalytic reaction, which supports the following proposal: (i) a nucleophilic substitution on V O species and (ii) attacking by surface oxygen through a electrophilic substitution, then (iii) followed by the cracking of ring structure, and further oxidation of the resulting species to form final products. The above results further suggest that the nucleophilic substitution process and surface reaction are kinetically significant steps for chlorobenzene oxidation, determining the overall rate of the reaction. Furthermore, 1,2-dichlorobenzene, 1,3-dichlorobenzene and 1,2,4-trichlorobenzene as additional reactants were tested together with chlorobenzene in binary mixtures to examine their competition reactions.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Mengxue Wang,Ziliang Jia,Xintong Ji,Yuxuan Zhou,Shuning Li,Miao Wang,Meisheng Liang,Xi Chen
Compared to noble metal catalysts at the nanoscale, single-atom catalysts are more likely to be poisoned then lead to the loss of activity during the catalytic oxidation of chlorinated volatile organic compounds (CVOCs) due to their unique coordination environment. Additionally, the commonly used low loading single-atom catalysts often suffer from limited active sites and low catalysts activities. Therefore, it is of great significance to synthesize stable and high-loading single-atom catalysts for CVOCs oxidation. In this study, a highly loaded (2.4 wt%) atomically dispersed 4RuCeO 2 -AA catalyst was synthesized through defect designing for the catalytic combustion of chlorobenzene (CB). By introducing defect sites on the CeO 2 supports using ascorbic acid, more atomically dispersed Ru were strongly anchored, significantly increasing the number of active sites and oxygen vacancies. With the same noble metal contents, the 4RuCeO 2 -AA catalyst exhibited superior performance in both CO 2 selectivity (99.6 % at 240 °C) and catalytic stability (no decay for 20 h). This enhanced performance can be attributed to the high dispersion of RuO x , strong Ru-O-Ce bonding energy, and an increased of chemically adsorbed oxygen, as well as the presence of strong Brønsted acid sites.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 22
·10820-10828
·
IF 3.925
Die Hu,Weiquan Li,Ke Yin,Bichun Huang
Mn/TiO2 catalysts were synthesized using a deposition–precipitation method. Ru-doped Mn/TiO2 catalysts were prepared by an incipient-wetness impregnation method. To investigate the interaction between Ru and Mn species, the catalytic performance of Mn/TiO2 and Ru–Mn/TiO2 catalysts in the catalytic oxidation of chlorobenzene (CB) was evaluated. The physicochemical properties of the catalysts were characterized by XRD, HRTEM, XPS, EPR, H2-TPR, O2-TPD and so on. The results showed that the 0.8% Ru-10% Mn/TiO2 catalyst exhibited the best catalytic activity with 99% CB conversion at 250 °C and showed an excellent CO2 yield (95% at 300 °C) and stability. In comparison with the 10% Mn/TiO2 catalyst, the T90 of the Ru–Mn/TiO2 catalyst decreased by 60 °C, which was attributed to the interaction between Ru and Mn species at the interfaces of Ru/Mn. The Ru species increased the concentration of Mn4+ and Ru4+ and reduced the H2 reduction temperature, which was conducive to improving the redox performance of the catalysts. Ru species were highly dispersed on the Mn/TiO2 catalyst surfaces, forming a large number of Ru/Mn interfaces. The interaction between Ru and Mn species at the interfaces of Ru/Mn promoted the formation of oxygen vacancies and surface reactive oxygen species, thus enhancing the catalytic activity.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Ziying Hu,Jing Chen,Dongxu Yan,Yan Li,Hongpeng Jia,Can-Zhong Lu
Chlorinated volatile organic compounds (CVOCs) existing widely in the industries are harmful to the environment and human’s health. It is urgent to develop highly efficient catalysts for their combustion. Herein, a series of porous MnO x/ Co 3 O 4 nanocomposites are synthesized by the pyrolysis of Mn@Co-ZIF-67 precursors, in which the Mn ions are introduced by impregnation method. XRD, Raman, ICP-OES, BET, SEM, TEM, XPS, O 2 -TPD, and H 2 -TPR have been performed to investigate the as-prepared catalysts’ physicochemical properties. The optimal catalyst MnO x /Co 3 O 4 -4h exhibits 90% and 100% chlorobenzene (CB) conversion (1000 ppm, Air, WHSV = 60,000 mL/(g h)) at 334 °C and 350 °C, respectively. And the better catalytic performance over MnO x /Co 3 O 4 -4h compared with the pure Co 3 O 4 and other MnO x /Co 3 O 4 nanocomposites mainly ascribes to its porous structures, homogeneous dispersion, optimal Mn/Co molar ratio, more lattice defects, and higher surface O Latt /O Ads ratio. Meanwhile, MnO x /Co 3 O 4 -4h displays high stability and resistance to moisture. Main intermediates have been further investigated by in situ DRIFT, and the degradation mechanism has been proposed according to the analysis of intermediates.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Sciences
·
2016
·
IF 2.208
Zhuowei Cheng,Zhiqi Gu,Jianmeng Chen,Jianming Yu,Lingjun Zhou
The photocatalytic oxidation of gaseous chlorobenzene (CB) by the 365 nm-induced photocatalyst La/N–TiO 2 , synthesized via a sol–gel and hydrothermal method, was evaluated. Response surface methodology (RSM) was used to model and optimize the conditions for synthesis of the photocatalyst. The optimal photocatalyst was 1.2La/0.5N–TiO 2 (0.5) and the effects of La/N on crystalline structure, particle morphology, surface element content, and other structural characteristics were investigated by XRD (X-ray diffraction), TEM (Transmission Electron Microscopy), FTIR (Fourier transform infrared spectroscopy), UV–vis (Ultraviolet–visible spectroscopy), and BET (Brunauer Emmett Teller). Greater surface area and smaller particle size were produced with the co-doped TiO 2 nanotubes than with reference TiO 2 . The removal of CB was effective when performed using the synthesized photocatalyst, though it was less efficient at higher initial CB concentrations. Various modified Langmuir-Hinshelwood kinetic models involving the adsorption of chlorobenzene and water on different active sites were evaluated. Fitting results suggested that competitive adsorption caused by water molecules could not be neglected, especially for environments with high relative humidity. The reaction intermediates found after GC–MS (Gas chromatography–mass spectrometry) analysis indicated that most were soluble, low-toxicity, or both. The results demonstrated that the prepared photocatalyst had high activity for VOC (volatile organic compounds) conversion and may be used as a pretreatment prior to biopurification.
研究领域:
环境科学
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材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2025
·
IF 7.5
Yan Tan,Xiao Liu,Yujia Zhang,Yiyang Rong,Xueying Wu,Ting Liu,Zizhen Ma,Huawei Zhang
In the current study, catalytic oxidation technology is among the most widely used methods for removing chlorinated volatile organic compounds (CVOCs). This article details the preparation of the Ag-Mn@ZSM-5 catalyst, which was prepared via the hydrothermal approach, followed by the incorporation of nano-Ag. The focus of the study is the catalytic oxidation of chlorobenzene (CB). Experimental results indicate that the hydrothermally synthesized nano-silver modified Ag-Mn@ZSM-5 catalyst, exhibiting a T90 of 290 °C, demonstrates superior performance compared to the Ag-Mn/ZSM-5 catalyst prepared via the traditional impregnation method, which has a T90 of 365 °C. As the operating airspeed increased from 7000 h −1 to 42000 h −1 , the removal efficiency of CB consistently remained above 90%, with stability maintained over a duration of 30 h. Furthermore, the catalyst exhibited excellent water resistance during a 12 h switching water test. Based on the characterization results, after loading Ag, the ratio of Mn 4+ and Mn 3+ on the surface of the Ag-Mn@ZSM-5 catalyst increases, the reducibility is enhanced, and the surface adsorbed oxygen species is increased, which is conducive to improving the catalytic activity. In addition, the Ag-Mn@ZSM-5 catalyst possesses an optimal pore structure, the proportion of mesoporous is 79.06%, suitable redox capacity, abundant acidic sites, and features a compact crystal stacking structure, which results in remarkable stability, catalytic activity, and space velocity resistance of the catalyst. These advantageous properties facilitate the adsorption and deep oxidation of CB. This study presents promising prospects for industrial applications and aims to offer innovative strategies for the treatment of chlorine-containing waste gases.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Shuai Yang,Yifeng Chen,Haiwei Guo,Xunzhu Jiang,Jiawen Ma,Xinyang Li,Zhao Chen,Xiaodong Ma
The current catalysts for polychlorinated aromatics (PCAs) oxidation showed either poor low-temperature catalytic activity, low mineralization ability or bad stability, and developing oxygen vacancies enriched catalysts with abundant acid sites is a potential solution for the above drawbacks. Herein, oxygen vacancies enriched Nb-WO X were developed for o -DCB ( o -dichlorobenzene, a PCAs model compound) oxidation, and they showed notably better low-temperature catalytic activity with T 50% <350 °C than did commercial WO 3 (T 50% >400 °C) under the WHSV of 36000 mL g −1 h −1 . Nb-WO X supported Ru exhibited even lower T 50% (173 °C) and T 90% (238 °C), as well as high CO X yield with >99% ratio of CO 2 to CO and good stability (>99% conversion for 500 mins) when with 1.5 wt% Ru loading at 300 °C. The above phenomenon was attributed to the abundant oxygen vacancies and acid sites in Nb-WO X that contributed to the better redox property, stronger interaction with Ru species and the removal of accumulated chloride. The o -DCB oxidation mechanism revealed that the higher CO 2 ratio to CO on Ru/Nb-WO X arose from the deep oxidation of CO byproducts. The work described here will instruct us to degrade PCAs effectively through catalysts design.
研究领域:
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
Tungsten
·
2025
·
IF 11.2
Qian Qi-Ling,Zeng Zhen-Yun,Chen Wan-Ting,Cheng Yu,Zhang Jia,Li Chuan-Hua,Qian Guang-Ren
The promoter is very important for effective catalysts, and the relationship among active species, promoter, and support is a hot topic in the field of catalysis. This work aims to investigate the influence of the promoter on the formation of effective active species. For this purpose, V was leached out from V-loaded TiO 2 (V/Ti) step by step, and the loaded V was classified into different species based on their performances in the catalytic oxidation of chlorobenzene. As a result, when V/Ti was co-doped with Mo or W, the chlorobenzene conversion rate was increased from 48.1% to 54.0% (Mo) or 61.0% (W) at 210 °C. The enhancement was attributed to the redistribution of V species. Specifically, 7.8% of V was “Inactive” V on V/Ti. This “Inactive” V was transformed into an “Active” species. At the same time, “Highly-active V” amounts were increased from 86.0% (V 3.3 /Ti) to 88.1% (WV 3.3 /Ti) and 87.1% (MoV 3.3 /Ti). According to the mechanism investigation, when W and Mo coexisted with V during the synthesis, V 3+ was oxidized into V 5+ , which is easily invaded into the TiO 2 , created more strong acidic sites, and activated more active lattice oxygens. These are all in favor of the effective catalytic oxidation of chlorobenzene. The new understanding of the promoter effect will help to produce a more effective catalyst using the same amount of active species. Graphical abstract
研究领域:
催化化学
·
材料科学
·
环境化学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Tong Chen,Rong Wang,Chen Sun,Debao Kong,Shengyong Lu,Xiaodong Li
In this study, a series of metal-organic frameworks (MOFs) derived binary porous MnCeO x catalysts were synthesized via solvothermal method for chlorobenzene (CB) oxidation . Compared with the catalysts from co-precipitation and sol-gel method, Mn1Ce1-MOF catalyst presented the best performance with T 90% at 242 °C and highest CO x yield of 94.6% at 400 °C, owing to its micropore-enriched structure, higher lattice oxygen ratio and better surface reducibility. The HCl selectivity of Mn1Ce1-MOF reached 91.3% at 400 °C. The gaseous byproducts over Mn1Ce1-MOF catalyst were identified and the degradation pathway of CB was proposed. The catalytic activity of Mn1Ce1-MOF catalyst at 300 °C could stabilize over 75% for 40 h. The oxidation of Mn 3+ and chlorine species adsorption were considered to be the main reasons for the catalyst inactivation. This work provides a highly-efficient MOFs templated porous metal oxide for tail gas purification.
研究领域:
催化
·
环境化学
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）