Catalysts
·
2019
·Vol. 9
·期 9
·726
·
IF 3.444
Jian Wang,Hainan Zhao,Jianfei Song,Tingyu Zhu,Wenqing Xu
Manganese oxide catalysts, including γ-MnO2, Mn2O3and Mn3O4, were synthesized by a precipitation method using different precipitants and calcination temperatures. The catalytic oxidations of benzene and 1,2-dichloroethane (1,2-DCE) were then carried out. The effects of the calcination temperature on the catalyst morphology and activity were investigated. It was found that the specific surface area and reducibility of the catalysts decreased with the increase in the calcination temperature, and both the γ-MnO2and Mn3O4were converted to Mn2O3. These catalysts showed good activity and selectivity for the benzene and 1,2-DCE oxidation. The γ-MnO2exhibited the highest activity, followed by the Mn2O3and Mn3O4. The high activity could be associated with the large specific surface area, abundant surface oxygen species and excellent low-temperature reducibility. Additionally, the catalysts were inevitably chlorinated during the 1,2-DCE oxidation, and a decrease in the catalytic activity was observed. It suggested that a higher reaction temperature could facilitate the removal of the chlorine species. However, the reduction of the catalytic reaction interface was irreversible.Keywords:benzene;1,2-Dichloroethane;catalytic oxidation;manganese oxide catalysts
研究领域:
环境科学
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催化化学
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DOI
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 14
·3417
·
IF 4.2
Pengfei Zhu,Zhaoxia Hu,Shouwen Chen
The development of economical catalysts that exhibit both high activity and durability for chlorinated volatile organic compounds (CVOCs) elimination remains a challenge. The oxidizing and acidic sites play a crucial role in the oxidation process of CVOCs; herein, praseodymium (Pr) was introduced into CrOx catalysts via in situ pyrolysis of MIL-101(Cr). With the decomposition of the ligand, a mixed micro-mesoporous structure was formed within the M-Cr catalyst, thereby reducing the contact resistance between catalyst active sites and the 1,2-dichloroethane molecule. Moreover, the synergistic interaction between chromium and praseodymium facilitates Oβspecies and acidic sites, significantly enhancing the low-temperature catalytic performance and durability of the M-PrCr catalyst for 1,2-dichloroethane (1,2-DCE) oxidation. The M-30PrCr catalyst possess enhanced active oxygen sites and acid sites, thereby exhibiting the highest catalytic activity and stability. This study may provide a novel and promising strategy for practical applications in the elimination of 1,2-DCE.
研究领域:
环境科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2024
·Vol. 14
·期 5
·3033-3043
·
IF 3.9
Xinhong Huang,Yan Liang,Jinhu Yun,Feishu Cao,Tian Xie,Hainong Song,Shuangfei Wang
1,2-Dichloroethane (1,2-DCA) is a typical organic chlorinated compound largely utilized in chemical manufacturing and industrial production and also a common pollutant in organically contaminated sites. The adsorption of 1,2-DCA on soil grains significantly influences its environmental fate and removal process. This study investigated the influence of fulvic acid (FA) and humic acid (HA) on the adsorption–desorption of 1,2-DCA in solid–liquid interfaces in water or constructed porous media. Experimental findings demonstrated the influence of organic matter on the adsorption of 1,2-DCA at the solid–water interface. 1,2-DCA adsorption increased in the FA or HA-treated soils when organic matter was present on the solid surfaces. The 1,2-DCA adsorption in the mixture of FA and HA was slightly lower than that in single organic acids, depending on the binding of FA and HA to the soil grains/colloids. Basic conditions reduced the adsorption of 1,2-DCA on soils, whereas acidic conditions enhanced adsorption due to the increased interactions via adsorption sites and hydrogen bonds. Conversely, the presence of organic matter in solutions (liquid phase in constructed porous media) will reduce the adsorption of 1,2-DCA on solid surfaces and increase the transport in the model aquifer. The combination of FA, HA, and rhamnolipids is helpful for the removal of 1,2-DCA from solid surfaces. Additionally, because of the enhanced desorption, the risk of 1,2-DCA contamination in groundwater can be increased when the organic matter or surfactant is present in the liquid phase if the eluent is not collected. This study helps to better understand the cooperative interaction of soil organic matter and chlorinated hydrocarbons at solid–water interfaces and the environmental fate and potential removal strategies of chlorinated hydrocarbons in contaminated sites.
研究领域:
环境科学
·
土壤学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Quan Zhang,Wei Huang,Wenhao Cui,Xingzong Dong,Guangye Liu,Yunpeng Xu,Zhongmin Liu
The acidity and porosity of zeolite catalysts are crucial parameters affecting the catalytic performance. In this work, alkali treatment and metal species loading were used to modify the porosity and acidity of ZSM-5 zeolite to prepare an efficient catalyst for the 1,2-dichloroethane cracking reaction. After optimization, the highly active catalyst Zn (1%) /ZSM-5-120 was obtained, and 78% conversion of EDC and 99% selectivity toward VCM could be achieved under the conditions of 300 °C and 3.0 h −1 (WHSV). A detailed investigation was conducted on the effects of acidity, texture properties and metal species loaded on ZSM-5 zeolite on the 1,2-dichloroethane cracking reaction.
研究领域:
化学工程
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催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Yujie Liu,Yuting Jiang,Yan Meng,Weini Xiong,Ziling Yuan,Ruihua Liu,Chao Yang
Because the interactions among contaminants may lead to enhanced toxicity, combined pollution caused by the co-presence of multiple contaminants has increasingly gained public concern. p -Nitrophenol (PNP) and 1,2-dichloroethane (1,2-DCA) are frequently co-detected in groundwater. To completely eliminate PNP, 1,2-DCA and intermediates from polluted sites, in this study, a novel degrader KTU-PDG was created by functional assembly of PNP and 1,2-DCA biodegradation pathways in a robust chassis Pseudomonas putida KT2440. Cell growth assay indicated that PNP or 1,2-DCA can be metabolized as a sole carbon source by strain KTU-PDG for cell proliferation. Stable isotope analysis indicated that strain KTU-PDG possesses the capability of co-mineralizing PNP and 1,2-DCA to CO 2 in mineral salt medium. In wastewater bioremediation, the strain KTU-PDG was proven to be capable of co-mineralizing PNP and DCA and maintained high cell viability during bioremediation. Herein, we demonstrate for the first time co-mineralization of PNP and 1,2-DCA by a single strain. Moreover, green fluorescent protein (GFP)-labeling of strain KTU-PDG facilitates estimation of viable cell number and real-time monitoring of cellular activity and transfer by autofluorescence in the environment. These merits of strain KTU-PDG highlight great potential of this degrader for in situ bioremediation of sites co-contaminated with PNP and 1,2-DCA. More importantly, this strategy of multi-pathways assembly in an optimal chassis shows good potential for the clean-up of combined pollution caused by other organic pollutants.
研究领域:
环境科学
·
微生物学
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DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2023
·
IF 5.9
Xin Ning,Heming Wang,Ganghua Zhou,Longyun Zhang,Yanju Yang,Jingya Sun,Xiaozhi Wang
Ni catalysts decorated with trace Rh supported on γ-Al2O3 were prepared by the co-impregnation method. To obtain the Ni–Rh nanoparticles with different nanostructures and chemical compositions, bimetallic catalysts with varied Ni/Rh molar ratios were prepared. For comparison, monometallic Ni/γ-Al2O3 and Rh/γ-Al2O3 catalysts were also prepared by the impregnation method. The selective gas phase catalytic hydrodechlorination of 1,2-dichloroethane to ethylene was used to evaluate catalytic performances of the catalysts. The catalysts were characterized by X-ray diffraction, N2 adsorption, X-ray photoelectron spectroscopy, H2 temperature-programmed reduction, transmission electron microscopy–energy-dispersive X-ray, and CO chemisorption. It was found that the introduction of Rh to Ni catalyst facilitated the generation of spillover hydrogen which could enhance the ability of the Ni catalyst for H2 activation. In bimetallic catalysts, there was an intimate interaction between Ni and Rh, and isolated Rh sites were formed due to the dilution effect of Ni. Accordingly, compared with the monometallic Ni catalyst for gas phase catalytic hydrodechlorination of 1,2-dichloroethane, the bimetallic Ni–Rh(800)/γ-Al2O3 catalyst exhibited markedly higher 1,2-dichloroethane conversion (37%) and comparable selectivity to ethylene (95%). The findings in this study indicate that Ni–Rh/γ-Al2O3 with trace Rh can be used as a promising catalyst for highly effective and selective catalytic hydrodechlorination of chlorinated hydrocarbons.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2019
·
IF 5.108
Xin Ning,Yuhan Sun,Heyun Fu,Xiaolei Qu,Zhaoyi Xu,Shourong Zheng
Metal-organic frameworks (MOFs) have received significant attention as promising precursors or sacrificial templates in the preparation of porous carbon supported catalysts. In this study, N-doped porous carbon supported Ni catalysts (denoted as Ni/NC) were prepared using furfuryl alcohol (FA) loaded Ni-MOF-74 as the precursor followed by NH 4 OH treatment and pyrolysis under N 2 atmosphere. For comparison purpose, Ni catalysts supported on porous carbon (denoted as Ni/C) were also prepared by direct pyrolysis of Ni-MOF-74. The selective gas phase catalytic hydrodechlorination of 1,2-dichloroethane to ethylene was carried out to evaluate the catalytic performances of the catalysts. It was found that for Ni catalysts prepared at the same pyrolysis temperature, Ni particle sizes in Ni/NC catalysts were significantly smaller (20–40% smaller) than that of Ni/C. This reflected that pre-modification of Ni-MOF-74 using FA and NH 4 OH could effectively increase Ni dispersion in Ni catalysts derived from Ni-MOF-74. Moreover, Ni/NC had a markedly stronger ability to form spillover H 2 owing to the enhanced metal-support interactions by N-doping. Accordingly, Ni/NC catalysts exhibited much higher catalytic activities than Ni/C catalysts. The turnover frequencies of Ni/NC catalysts were found to be 1.22–1.65 times higher than Ni/C catalysts. Increasing pyrolysis temperature led to decreased catalytic activities of both Ni/C and Ni/NC catalysts, due to the aggregation of Ni particles at higher treatment temperature. The findings from this study demonstrate that the MOF-mediated synthesis method offers a promising way to prepare Ni-based catalysts for catalytic hydrodechlorination of chlorinated hydrocarbons .
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2021
·Vol. 331
·期 1
·365-373
·
IF 1.371
Li Chunhui,He Hui,He Mingjian,Gao Yang,Zhang Meng,Jiao Caishan
A detailed extraction equilibrium study is experimentally performed to understand the extraction mechanisms of Ce(IV) by 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (C 4 mimNTf 2 ) in 1,2-dichloroethane. Further, the influence of adding TBP on the distribution ratio is investigated and demonstrated. The ceric aqueous chemistry in the nitric acid solution and slope analysis are combined to reveal the extraction mechanism. The monovalent anionic complex HCe(NO 3 ) 6 − is the dominant species, which extracted by C 4 mimNTf 2 . Importantly, this study demonstrates the antagonistic effect between TBP and C 4 mimNTf 2 on the extraction process.
研究领域:
化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Processes
·
2021
·Vol. 9
·期 1
·119
·
IF 2.847
Yu Huang,Shiyue Fang,Mingjiao Tian,Zeyu Jiang,Yani Wu,Chi He
Developing economical and robust catalysts for the highly selective and stable destruction of chlorinated volatile organic compounds (CVOCs) is a great challenge. Here, hollow nanosphere-like VOx/CeO2catalysts with different V/Ce molar ratios were fabricated and adopted for the destruction of1,2–dichloroethane (1,2–DCE). The V0.05Ce catalyst possessed superior catalytic activity, reaction selectivity, and chlorine resistance owing to a large number of oxygen vacancies, excellent low-temperature redox ability, and chemically adsorbed oxygen (O−and O2−) species mobility. Typical chlorinated byproducts (CHCl3, CCl4, C2HCl3,and C2H3Cl3) derived from the cleavage of C–Cl and C–C bonds of 1,2–DCE were detected, which could be effectively inhibited by the abundant acid sites and the strong interactions of VOxspecies with CeO2. The presence of water vapor benefited the activation and deep destruction of 1,2–DCE over V0.05Ce owing to the efficient removal of Cl species from the catalyst surface.Keywords:catalytic destruction;1,2–dichloroethane;VOx/CeO2;chlorinated byproduct inhibition;reaction mechanism
研究领域:
环境科学
·
催化化学
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产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Tian Xie,Zhi Dang,Qian Zhang,Lili Su,Yongxin Zhou,Shudi Li,Jian Zhang,Ronghai Zhang,Changjun Liao,Guining Lu
1,2-Dichloroethane (1,2-DCA) is a common compound found in groundwater contaminated with organics. This compound is difficult to remove from groundwater and has the potential to inflict significant harm on human health and the environment. This study used sodium persulfate (Na 2 S 2 O 8 ) activated by sodium hydroxide (NaOH) to remove 1,2-DCA from aqueous solutions. Density functional theory was employed to calculate the potential energy surface of the reactants, intermediates, transient states, and products to thoroughly analyze the degradation pathways. The computations were performed in combination with in situ remediation of a 1,2-DCA plume from a point source to verify the industrial applicability of the technology . The results showed the 1,2-DCA removal efficiency was impacted considerably by the Na 2 S 2 O 8 dosage and the dosing sequence of Na 2 S 2 O 8 and NaOH, with the mean removal ratio reaching 96.24%. A free radical reaction was the main pathway of 1,2-DCA degradation; superoxide radical (O 2 •– ) existed stably and played a key role in the reaction, and the main transformation proceeded via a vinyl chloride intermediate. The maximum removal of 1,2-DCA reached 91.79% in the in situ remediation. The developed technology exhibits important advantages in enabling flexible control over chemical dosages, long durations of effective activity, and rapid full-cycle remediation.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Sciences
·
2025
·
IF 6.3
Xiaonan Guo,Yuanzhe Yu,Runduo Zhang,Shuting Wei,Bin Kang,Ying Wei,Jingbo Jia,Zhou-jun Wang
The Ru-based catalysts with different preparation methods or supports were achieved and applied in efficiently catalytic elimination of 1,2-dichloroethane (1,2-DCE). It was firstly found that the redox ability and chlorine resistance of the catalyst could be improved by regulating the interaction between Ru and supports. Compared with other supports and conventionally impregnated methods, the Ru@ZSM-5 catalyst synthesized by the in-situ encapsulation strategy exhibited an excellent low-temperature catalytic performance ( T 50 = 262°C, T 90 = 327°C), superior stability in long-term test as well as ideal target products. The acidity, specific surface area, and interaction with precious metals of the supports have significant influences on the catalytic activity, and the Ru clusters inside the pore structures are more closely bound to the framework Al species, which promotes the oxidation behavior. The encapsulation strategy also significantly improves the Ru dispersion thereby facilitates oxygen activation as well as Cl-containing volatile organic compounds (CVOCs) deep oxidation, and preserves large amounts of Brønsted acid sites to optimize the hydrolysis mechanism for purification of CVOCs. Subsequently, the synergistic effect between metal redox and acidity is greatly optimized, thus extremely promoting the catalytic efficiency of 1,2-DCE 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
ACS Applied Nano Materials
·
2021
·
IF 5.097
Yiman Zhang,Shiying Fan,Xinyong Li,Liang Wang,Zhifan Yin,Penglei Wang,Moses O. Tadé,Shaomin Liu
The application of carbon-based materials as electrocatalysts for electrochemical dechlorination of chlorinated volatile organic compounds (Cl-VOCs) has stirring extensive concern. However, the relationship between morphology and activity toward carbon-based materials is often overlooked by researchers. Herein, a unique three-dimensional (3D) sea-urchin-like carbon nanosphere containing a hollow interior self-assembled from 1D carbon nanorods (SS-CNRs) has been successfully fabricated. It can be achieved through morphology-preserved thermal conversion of a 3D metal–organic framework (MOF) superstructure, which possesses an identical sea-urchin-like nanostructure consisting of 1D MOF nanorods (SS-MOFNRs). The as-prepared SS-CNRs can be utilized as an efficient cathode catalyst for electrocatalytic dechlorination of 1,2-dichloroethane (1,2-DCA) to selectively produce highly valuable ethylene. Benefiting from the peculiar sea-urchin-like morphology and the void-confinement effect induced by the hollow structure, the SS-CNRs are endowed with an abundant electrode–electrolyte contact area to accelerate the electron transfer. As a result, the as-synthesized catalyst exhibits outstanding electrocatalytic dechlorination performance of 1,2-DCA with high ethylene yield, selectivity, reusability, and stability, where the Faradaic efficiency of ethylene is up to 55% at −2.75 V (vs SCE). This work provides a promising prospect for the rational morphological engineering of carbon-based nanometer materials and the effective transformation of Cl-VOCs to value-added ethylene in a friendlier manner.
研究领域:
材料科学
·
环境科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）