JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Xincheng Zhang,Changqing He,Muhmmad Youssef Muhmmad Mostafa,Waseem Akram,Lin He,Hong Sui,Xingang Li
Separation of oil-water emulsions co-stabilized by solid particles and natural interfacially-active components has always been a challenge in petroleum and coal industry. Herein, we constructed and synthesized an interfacially-active nonionic material by esterification and polymerization, which contains multiple oxygen-containing groups (-COOH, -C-O, -COOR) and aromatic rings. The lab bottle tests show that this polymer (1000 mg/L) could completely break the silica-asphaltene co-stabilized water-in-heavy oil emulsions at 60 °C within 45 min, much faster and higher than those of commercial and reported demulsifers (>75 °C, >90 min). Mechanistic study by interfacial characterization and molecular dynamics simulation shows that this newly synthesized polymer possesses multiple hydrogen bonding sites and delocalized π bonds. These functional groups and active sites play the vital role in reconstructing and breaking the interfacial film by non-covalent interactions reconstruction, repelling the coated heavy fractions (e.g., asphaltenes) from the fine solids surface. The introduction of aromatic rings with delocalized π bonds into the polymer provides it with a solubilizing effect on asphaltene and promotes the dispersion of asphaltene aggregation, enhancing the demulsification efficiency. In addition, these hydrogen bonding sites can also build connecting bridges between emulsified droplets, facilitating the coalescence of them. This work would provide insights for developing efficient functional materials for low-carbon separation of complex emulsions in industry, including oily sludges, water-in-oil emulsions.
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
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Xiangyu Yan,Daohao Li,Lixue Zhang,Xiaojing Long,Dongjiang Yang
Oxygen-containing groups (OCGs) modified carbon materials can affect the microstructure and chemical composition, which is important for oxygen reduction to hydrogen peroxide (ORHP). Thus, exploring the relationship between structure and activity of OCG-containing electrodes is of great significance. In this work, we synthesized OCGs modified pyrene-based organic molecules as electrocatalysts for ORHP. Their electrocatalytic performance are correlated with types and locations of the modified OCGs. Particularly, the Pyr-2OMe with better absorption of O 2 exhibits high H 2 O 2 selectivity. DFT calculations reveal that the carbon atoms attached OCGs are the catalytic active sites. More importantly, the groups on one side of the molecules ( Pyr-2OMe , Pyr-2OH , and Pyr-2CO ) with large dipole moments exhibit superior catalytic activity. Thus, for the first time we find that the asymmetrically local charge redistribution of these catalysts can promote ORHP process. This work paves an alternative way to supply constructive information for understanding the structure and selectivity correlations.
研究领域:
电化学
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材料科学
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催化
✓ 已验证
DOI
高影响因子
ChemistrySelect
·
2025
·Vol. 10
·期 26
·e00237
·
IF 2
Xiaoyue Li,Zhiyuan Wang,Tao Zhang,Yang Dong,Enqi Sun,Tianbo Fan,Hongfan Guo
Graphical Change from none to one hundred percent just by a simple calcination : Directly using graphene to support gold nanoparticles gives no catalytic activity. But if the graphene support just undergoes a very simple thermal treatment for removing some oxygen-containing groups on it, a full conversion can be obtained within only half hour. Graphene is a promising support material for gold (Au) catalysts and its surface functional groups may play important roles in Au catalysis. By using alcohol oxidation with molecular oxygen as the probe, this work reveals that the oxygen-containing groups on the graphene support significantly affect the Au catalysis. The carbonyl groups can totally deactivate the catalysts. Just by thermally treating the graphene at suitable conditions to remove the carbonyl groups, the catalytic performance of the Au catalysts can be greatly improved. Even a full conversion can be obtained in a very short reaction time (just 0.5 h), when the oxygen content of the graphene support decreases from the initial 6.67% to 2.58% with the almost disappearance of C═O groups. The mechanism is also analyzed. Despite poisoning the present catalytic reaction, the Au-support interaction elucidated in this work may be beneficial to some other catalytic reactions with different reaction mechanism. Thus, this work helps to enhance the catalytic activity of graphene-supported Au catalysts, according to the applied catalytic reactions.
研究领域:
催化
·
纳米材料
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表面化学
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材料科学
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化学反应工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Qifan Wu,Bin Zhang,Chao Zhang,Xiangchun Meng,Xinluona Su,Shan Jiang,Ruhui Shi,Yan Li,Weiwei Lin,Masahiko Arai,Haiyang Cheng,Fengyu Zhao
The selectivity of 3-nitrostyrene (NS) hydrogenation over 0.5 wt-% Pt catalysts supported on carbon materials can be switched simply by changing reduction temperature. When the reduction temperature was 150 °C, 1-ethyl-3-nitrobenzene (ENB) was mainly produced in a selectivity of 93% at a conversion of 95% (at 100 °C). When the reduction was conducted at a higher temperature of 450 °C, in contrast, the main product was switched to 3-aminostyrene (AS) in a selectivity of 96% at a conversion of 91%. That is, the Pt/C catalysts reduced at low and high temperatures could preferentially catalyze the hydrogenation of vinyl and nitro groups of NS, respectively. This switching of the product selectivity may be ascribed to actions of surface oxygen-containing functional groups and surface hetero P species. The quantity and nature of these surface species were examined in detail by a few different methods. For the low-temperature reduced catalyst, surface acidic groups present close to Pt nanoparticles (∼2 nm) would interact with the nitro group of a NS molecule and make its vinyl group more likely to interact with the surface active metal species of Pt nanoparticles; this facilitates the hydrogenation of the latter and produces ENB selectively. For the high-temperature reduced catalyst, however, P species would interact with Pt and form Pt-PO x complex, on which a NS molecule is likely to be adsorbed with its nitro group, facilitating the selective production of AS via its hydrogenation. It is demonstrated that surface functional groups and surface hetero atoms (like P), in addition to main active metal species (like Pt), should have direct actions in the catalysis for such a catalyst that exposes a larger quantity of surface functional groups and/or hetero atoms compared to the number of supported metal nanoparticles .
研究领域:
催化
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化学工程
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Lei Zeng,Yun Zhao,Xinghang Jia,Yabin Jiang,Limin Huang
Graphitic carbon nitride (g-C 3 N 4 ) is a remarkable metal-free photocatalyst which is widely used for photocatalytic reductive reaction due to its suitable potential of conduction band, but also suffers from intrinsically weak photocatalytic oxidation ability. Here, by simply refluxing g-C 3 N 4 in H 2 O 2 , oxygenous groups are introduced into g-C 3 N 4 . The resultant oxygenous groups modified g-C 3 N 4 (g-C 3 N 4 (H 2 O 2 )) exhibits significantly improved hydrophilic ability and photocatalytic oxidative ability. It is well evidenced that valence band position is positive shifted significantly by introduction of surface oxygenous groups. However, the photocatalytic activity for oxygen evolution is not improved obviously, suggesting that the driving force for water oxidation is not increased simultaneously. Luckily, the photocatalytic oxidative activity of the modified g-C 3 N 4 (include oxygen evolution, pollutant degradation and antibacterial property) could be further improved after forming TiO 2 -containing nanocomposites during the H 2 O 2 reflux treatment with the addition of tertrabutyl titanate (g-C 3 N 4 /TiO 2 (H 2 O 2 ) due to much increased driving force and accelerated charge migration. Herein, a facile and simple method is proposed to engineer the band structure of g-C 3 N 4 for improving its photocatalytic oxidative ability, which expand the application of carbon nitride.
研究领域:
材料科学
·
环境科学
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化学
·
光催化
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Kaizheng Feng,Zhenzhen Wang,Rong Guo,Jingyuan Ma,Guancheng Wang,Qianqian Li,Haoan Wu,Ming Ma,Xingfa Gao,Yu Zhang
Despite of the rapid development of nanozymology, the long-term catalysis of nanozymes, which reflects their hidden catalytic mechanism and sustainability is still overlooked. Herein, we systematically investigate the prolonged catalase (CAT)-like activity of nanozymes prepared by flow chemistry. Through a rational control on the reaction conditions in micro-channel, fast synthesis of a library of common CAT-like nanozymes, including Prussian blue (PB), manganese Prussian blue (Mn-PB), Fe 3 O 4 , CeO 2 , Pt, and Au is realized. The mass production capability of the developed synthetic device is validated with a high yield of 60.5 g uniform PB nanozymes in 115 min. A precise definition of s nano value is then proposed, quantitively expressing the long-term catalytic behavior of the as-prepared nanozymes with self-increasing or self-depleting activity. Taking Mn-PB, Fe 3 O 4, and Pt as representative models, the irreversible oxidation effect of H 2 O 2 is demonstrated to endow them with abundant oxygenated groups during the prolonged catalysis and regulate their reaction energy profiles, thus varying their catalytic activities. Our results reveal the superiority of flow synthesis for the nanozymes preparation and the guiding significance of long-term catalysis for the mechanism study and the efficient application of nanozymes.
研究领域:
纳米酶学
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催化化学
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材料化学
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流动化学
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纳米材料
·
酶模拟
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）