SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Meiling Li,ShanShan Mao,Xin Zhou,Hao Wang
The efficient separation of ethylene (C 2 H 4 ) from ethane/ethylene (C 2 H 6 /C 2 H 4 ) mixtures, achieved via a single-step selective adsorption process, represents a promising yet challenging goal. Notably, the pursuit of adsorbents that combine high adsorption capacity with low adsorption heat is paramount, as these attributes directly correlate with superior separation efficiency and minimized regeneration energy. In this study, we present the selective adsorption of C 2 H 6 over C 2 H 4 by a V-MOF (V-TBAPy), constructed from [V( μ 2 -O)O 4 ] n secondary building units. The pore surface of V-TBAPy is characterized by a high density of aromatic rings and oxygen atoms, which facilitates targeted adsorption of C 2 H 6 through C-H···π and C-H···O interactions. V-TBAPy adsorbs up to 102.6 cm 3 /g of C 2 H 6 at 298 K and 1 bar, with a selectivity of 1.66 for an equimolar C 2 H 6 /C 2 H 4 binary mixture. Importantly, the adsorption heat for C 2 H 6 on V-TBAPy is as low as 22.7 kJ/mol, enabling energy-efficient regeneration. Breakthrough experiments have confirmed the efficacy of V-TBAPy in achieving one-step purification of C 2 H 6 /C 2 H 4 mixtures in conditions mimicking industrial settings.
研究领域:
材料科学
·
化学工程
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DOI
高影响因子
Catalysis Science & Technology
·
2024
·
IF 4.4
Shan Hu,Yunfei Gao,Lu Ding,Xueli Chen,Weitong Pan,Fuchen Wang
Hydroformylation is an important reaction for aldehyde synthesis and requires ethylene and syngas (CO + H2) with the feedstocks. While these feedstocks are typically synthesized separately, it would be highly desirable to directly convert abundant ethane into ethylene and syngas in a single step. In this work, we loaded B2O3 onto perovskite La0.8Sr0.2FeO3 (LSF) and formed a core–shell structured catalyst, with B2O3 and Sr3B2O6 being the shell and LSF being the core. The shell structure can substantially inhibit deep oxidation of ethane into CO2 and the optimized La0.8Sr0.2FeO3@20B2O3 can achieve 69.2% ethane conversion and 88.8% ethylene + syngas selectivity at 700 °C with good stability, with a ratio of CO/H2 close to 1 : 1. The effects of reaction temperature, space velocity, B2O3 loading, and La/Sr were also investigated. This catalyst marks a promising progress for the direct oxidation of ethane and has good potential for industrial applications.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Qian Bao,Yi Yang,Dahang Shen,Feiyang Ye,Jiageng Yu,Osama Alam,Wei Wang
Decabromodiphenyl ethane (DBDPE), a key alternative to deca-BDE (BDE-209), has been ubiquitous in the receiving ecosystem. However, little is known about its uptake process and fate in plants. Here, the plant absorption, distribution, and metabolism of 14C-DBDPE under two distinct exposure pathways (i.e., soil-root and airborne dust-leaf) were investigated with three vegetables (cherry radish, water spinach, and eggplant). DBDPE was absorbed and primarily accumulated in directly exposed roots and leaves, with translocation factors to other tissues of 0.04–0.77 and 0.73–12.80 × 10–3, respectively. DBDPE in exposed leaves was more difficult to transport as most DBDPE did not enter the interior of the leaves but was stored in waxes (>90%). Furthermore, DBDPE within leaves was found to enter mostly through waxy layer penetration (>97%). The majority of 14C-DBDPE was localized in cell walls (52.6 and 75.6%, respectively) and organelles (22.7 and 45.5%, respectively) of exposed tissues, substantially restricting its in-plant translocation. Debrominated products were detected in exposed roots, but barely found in exposed leaves, as most DBDPE was blocked by the waxy layer. Moreover, DBDPE was stable in soils and dust without degradation. Our findings contribute to a deeper understanding of the environmental fate of DBDPE in soil-plant and airborne dust-plant systems.
研究领域:
环境科学
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植物学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Lina Dai,He Wang,Yanduo Liu,Liru Cui
Direct light-driven methane selective conversion into useful chemicals remains a major challenge due to the need for photocatalysts with high photoactivity and selectivity in activating inert C-H bonds. In this study, we have developed highly photoactivity and selective photocatalytic CH 4 oxidation into C 2 H 6 using Ag-Mg tandem sites co-modified ultrathin ZnO hybrid photocatalysts in a flow reactor. Our system achieves an C 2 H 6 production rate of over 1860 μmol/g/h with 93 % selectivity, which is significantly higher than the efficiency of state-of-the-art photocatalytic systems. Various in-situ characterizations and theoretical studies reveal that the Ag-Mg tandem sites co-modified leads to enhanced photogenerated charge separation efficiency, while maintaining high ethane production rate owing to the strong selective adsorption capacity for methane and oxygen of the doped Mg sites and oxygen vacancy. Furthermore, the Ag nanoparticles cocatalyst can facilitate the removal of activated CH 4 in the form of methyl radicals in the gas phase, thereby promoting C 2 H 6 formation and inhibiting CH 4 overoxidation to produce CO 2 . Overall, these findings provide novel insights into the photocatalytic conversion of CH 4 on Ag/Mg-ZnO. These results offer valuable possibilities for developing more effective catalysts for the conversion of CH 4 to higher value-added products.
研究领域:
材料科学
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能源化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Qianqian Li,Hairong Yue,Changjun Liu,Kui Ma,Shan Zhong,Bin Liang,Siyang Tang
Transformation from photocatalytic oxidative dehydrogenation of ethane (PODHE) to photocatalytic dehydrogenation of ethane (PDHE) is an attractive process. A series of Pd/TiO 2 photocatalysts with different Pd loading amount were synthesized by photochemical deposition. And the Pd particle sizes varied from 1 nm to 4 nm. PDHE happened instead of POHDE over Pd particles smaller than 3 nm. The best PDHE performance (H 2 , 799.4; C 2 H 4 , 614.9, in micromoles per gram of catalyst) was obtained over 0.5 wt.% Pd/TiO 2 catalyst. And it was 3 times of it of PODHE over 1 wt.% Pd/TiO 2 . Reducing the Pd particle size of Pd/TiO 2 would increase Pd 0 /Pd 2+ and lower the valence band and conductive band of Pd/TiO 2 , which affect the catalytic behaviors. Detailed formation of products was investigated in this work.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Guangzhi Xu,Mingzhen Shi,Ping Zhang,Zhuoheng Tu,Xingbang Hu,Xiaomin Zhang,Youting Wu
The separation of ethylene (C 2 H 4 ) and ethane (C 2 H 6 ) is crucial for the production of down-stream chemicals in petrochemical industry. However, the currently used technologies still suffer from high energy intensity and contamination of volatile organic compounds (VOCs), stimulating researches on screening greener separation media and methods. Developed in this work were deep eutectic solvents (DESs) containing tetrabutylammonium chloride (TBACl) and n -decanoic acid (DA) for absorption separation of C 2 H 4 and C 2 H 6 . Chemical structures of DESs were confirmed using NMR and FT-IR spectroscopy, and their densities, viscosities as well as the thermal decomposition temperatures were measured. C 2 H 4 solubilities in these DESs were found to be higher than 0.0632 mol/kg at 313 K and 1.0 bar, higher than most ionic liquids reported so far. Importantly, tunable C 2 H 4 /C 2 H 6 selectivities ranging from 0.86 to 1.31 were achieved via altering the ratio of compositions in DESs, while the absolute C 2 H 4 solubilities remained almost unchanged, which was attributed to the change in free volume and better affinity of DA and TBACl for C 2 H 4 . The Henry’s constants ( H m ), enthalpy changes (Δ sol H ), Gibbs free energy changes (Δ sol G ) and entropy changes (Δ sol S ) for the dissolution of C 2 H 4 and C 2 H 6 in the DESs were calculated through thermodynamic analysis. In addition, quantum chemical calculations elucidated the origin of the different dissolution behaviors of the two gases in DESs. Furthermore, energy-efficient regeneration of DESs could be carried out by only depressurizing without heating, and no visible decrease in separation performance was observed after ten consecutive absorption–desorption cycles. Overall, the findings in this work may provide utility guidance for designing absorbents targeting separation of C 2 H 4 /C 2 H 6 with variable composition.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
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IF 8.3
Yong Wang,Xuanyu Zhao,Shaoxiong Han,Yongzhen Wang
The development of efficient technology for natural gas separation in industrial processes has become imperative. In this regard, the exploration of novel and effective adsorbents has gained significant attention. One promising approach is the metal regulation of metal–organic frameworks (MOFs), particularly heterometallic MOFs, which offer greater potential for gas separation due to their diverse composition. This study presents the synthesis of a series of iron- and vanadium-based heterometallic MOFs (MIL-126), featuring interpenetrated structures, and investigates their adsorption performance for methane (CH4), ethane (C2H6), and propane (C3H8). Experimental results reveal that the choice of metal combinations within the MOF framework significantly influences the adsorption performance of MIL-126. Notably, heterometallic MIL-126(Fe/Ni) exhibits a stronger binding affinity for C3H8, with an impressive uptake of 177 cm3/g. The C3H8/CH4 ideal adsorbed solution theory selectivity of MIL-126(Fe/Ni) surpasses that of MIL-126(Fe) by a factor of 7, reaching a value of 853, second only to the highest reported value. Furthermore, MIL-126(Fe/Ni) exhibits remarkable potential for the recovery of pure CH4 from the equimolar C3H8/CH4 mixture, with the amount of pure CH4 approaching the maximum reported value for MOFs. Insights from isosteric heat at zero loading and Henry’s coefficients indicate that the transformation of metal types leads to a change in the interaction energy between C3H8 and the framework. Furthermore, breakthrough experiments validate the effective separation capability of MIL-126(Fe/Ni) for CH4/C2H6/C3H8 mixtures. These findings underscore the remarkable potential of heterometallic MOFs in constructing a wide range of new MOFs with tailorable properties, thereby enhancing their gas separation performance.
研究领域:
材料科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Shao-Min Wang,Fei Wang,Yong-Li Dong,Mohana Shivanna,Qiubing Dong,Xuan-Tong Mu,Jingui Duan,Qingyuan Yang,Michael J. Zaworotko,Qing-Yuan Yang
The separation of ethane (C 2 H 6 ) from ethylene (C 2 H 4 ) is one of the most challenging and important tasks in chemical industry. Herein we report two interpenetrated diamondoid ( dia ) coordination networks, Dia-4-M [M(pba) 2 ] (pba = 4-(4-pyridyl)benzoate); M = Ni or Co), that can directly capture ethane from ethane-ethylene mixtures with reverse C 2 H 6 /C 2 H 4 separation. Both materials not only exhibit ultra-high C 2 H 6 uptake (100 cm 3 g −1 for Dia-4-Ni ; 103 cm 3 g −1 for Dia-4-Co ) but also display good C 2 H 6 /C 2 H 4 selectivity (1.76 for Dia-4-Ni ; 2.04 for Dia-4-Co ). Such C 2 H 6 /C 2 H 4 separation performance was confirmed by dynamic breakthrough experiments. Dia-4-M could extract low concentrated of C 2 H 6 from C 2 H 6 /C 2 H 4 mixture (v(C 2 H 6 )/v(C 2 H 4 ) = 1:9 and 1:15) and produce high purity (99.9%) of C 2 H 4 under ambient conditions. The mechanism for selective C 2 H 6 /C 2 H 4 separation was clarified through Grand Canonical Monte Carlo (GCMC) simulations and Density functional theory (DFT) calculations. Overall, this research demonstrates that Dia-4-M has a significant potential as effective C 2 H 6 -selective adsorbents for the purification of ethylene in practice.
研究领域:
化学工程
·
材料科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yan Zhang,Shangyong Zhou,Xing Liu,Peixin Zhang,Zhihong Yan,Jianguo Hu,Ziqi Wei,Lihua Chen,Jun Wang,Shuguang Deng
Efficient separation of ethane (C 2 H 6 ) from ethylene (C 2 H 4 ) using C 2 H 6 -selective adsorbents is more efficient but challenging due to their similar physical and chemical properties. Herein, we report a Zn (II) cluster-based metal-organic framework, Zn 4 O(NTB) 2 , with suitable cavity pockets and favorable adsorption sites for the reverse capture of C 2 H 6 from C 2 H 6 /C 2 H 4 mixtures. Both high C 2 H 6 uptake (2.83 mmol g −1 ) and C 2 H 6 /C 2 H 4 selectivity (2.06) at 273 K and 1 bar was achieved, outperforming many top-ranking C 2 H 6 -selective adsorbents. Moreover, dispersion-corrected density functional theory (DFT) and grand canonical Monte Carlo (GCMC) simulation revealed that C H···O and C H···π interactions are formed with C 2 H 6 in the suitable pockets with saturated Zn clusters and nonpolar pore surfaces. Dynamic breakthrough experiments demonstrated its practical separation performances with various gas-mixture compositions and those containing water vapor.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Qingrong Wu,Guilin Li,Yanyan Cheng,Bangyu Fan,Yinge Bai,Nian Zhang,Zhongzhi Wang,Xiangping Zhang,Suojiang Zhang
Efficient purification of ethylene (C 2 H 4 ) from ethane (C 2 H 6 ) is one of the seven chemical separations which can change the world. Chemical absorption is considered as the most promising method for C 2 H 4 /C 2 H 6 separation. However, the two critical separation properties of absorbent, the solubility and selectivity, are always trade-offs, which are still needed to both promote and balance in the viewpoint of industrial application. Herein, a series of novel silver-containing protic imidazolium ionic liquids (SPILs), with high chemical activity for efficient C 2 H 4 absorption, have been designed and synthesized. The physical properties of the prepared silver-containing ionic liquids (SILs) were first characterized. Then the separation performances of C 2 H 4 /C 2 H 6 by SPILs and silver-containing aprotic ionic liquids (SAILs) were carefully compared. The C 2 H 4 /C 2 H 6 selectivity of SPILs (16.73) was eight times higher than the value of the latter. Then, the C 2 H 4 absorption mechanism was confirmed by density functional theory (DFT) calculations. The charge density of Ag + was greater and the Gibbs free energy (ΔG) of C 2 H 4 absorption was more negative in [Bim] n [Ag(NTf 2 ) n+1 ]. The proposed SPILs, [Bim] 1.5 [Ag(NTf 2 ) 2.5 ], had a high C 2 H 4 /C 2 H 6 selectivity of 41.2 and C 2 H 4 solubility of 1.86 mol C 2 H 4 /mol Ag + , which were the highest value of ionic liquids (ILs) absorption reported so far. The [Bim] 1.5 [Ag(NTf 2 ) 2.5 ] exhibited excellent reversibility after five absorption–desorption cycles. An absorbent designed strategy of SPILs was proposed with enhanced solubility and selectivity for C 2 H 4 /C 2 H 6 separation.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
AICHE JOURNAL
·
2024
·Vol. 70
·期 7
·e18443
·
IF 3.5
Kang Wang,Yao Jiang,Mingming Xu,Dongdong Zheng,Shaojun Jia,Peng Cui
Separation of CH 4 from natural gas is an essential but extremely challenging process in the petrochemical industry. Here, we tailored a MOF-based adsorbent with partitioned aliphatic pore spaces through the simultaneous incorporation of the aliphatic sites and the symmetrically matched partition agent. The resulting adsorbent demonstrates exceptional adsorption capacity for C 3 H 8 and C 2 H 6 compared to CH 4 , along with remarkably competitive adsorption selectivities for C 3 H 8 /CH 4 and C 2 H 6 /CH 4 . Breakthrough experiments further support the excellent dynamic separation efficiency of the adsorbent for the purification of CH 4 from natural gas. Moreover, detailed density functional theory calculations and molecular simulations elucidate the synergistic interactions between the aliphatic sites and the partitioned pore spaces within the adsorbent, which promote the stronger binding affinities for C 3 H 8 and C 2 H 6 over CH 4 .
研究领域:
材料科学
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化学工程
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能源技术
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产品关联
DOI
高影响因子
JOURNAL OF SOILS AND SEDIMENTS
·
2025
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IF 3
Jin Meiqing,Sun Yuanchao,Chai Bing,Wang Minghu,Wu Yuping,Wu Weihong,Zhou Qingwei,Qiu Linlin,Du Jia,Fu Li
Purpose Decabromodiphenyl ethane (DBDPE) and lead (Pb), two prevalent contaminants in e-waste dismantling areas, pose significant threats to soil ecosystem health. However, the ecotoxicological effects of their co-exposure on soil invertebrates remain poorly characterized. Methods Avoidance behavior, survival rate, and growth-inhibition assays were performed to assess the combined toxic effects of DBDPE and Pb on earthworm ( Eisenia fetida ) in an artificial soil system over exposure periods of 7–21 d. Responses from multiple biochemical biomarkers, including superoxide dismutase (SOD), catalase (CAT), malondialdehyde (MDA), glutathione S-transferase (GST), and acid phosphatase (ACP) were also measured, and the data were integrated by the biomarker response index (BRI). Interaction between Pb and DBDPE on BRI was further analyzed by calculation of effect addition index (EAI). Results Avoidance behavior emerged as the most sensitive endpoint and exhibited concentration-dependent escalation under co-exposure conditions. While individual exposure to DBDPE (0–0.75 mg/kg) induced negligible impacts on growth and mortality, its combination with Pb (1000 mg/kg) resulted in significant synergistic effects. Similarly, biochemical biomarkers—including SOD, CAT, MDA, GST, and ACP—showed markedly greater alterations in co-exposure groups compared to single DBDPE treatments. The BRI revealed only slight alterations in biological health across most treatments. The EAI values indicated that antagonistic effects dominated the interaction between DBDPE and Pb. Conclusion Our findings demonstrated significant variation in biomarker sensitivity to pollutant exposure. Notably, short-term sub-lethal co-exposures may elicit synergistic effects on avoidance, growth, and mortality, revealing a time-concentration toxicity dependency. These results provide novel insights into the interaction between heavy metals and organo-pollutants and highlight the ecological hazards posed by emerging brominated flame retardants (e.g., DBDPE) in heavy metal-contaminated soil systems.
研究领域:
环境科学
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毒理学
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产品关联
DOI
高影响因子