APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Houhong Song,Xian Zhou,Xiaofeng Gao,Hantao Gong,Hao Teng,Yongkang Huang,Ziyu Song,Lili Lin,Siyu Yao
Treating and recycling high concentration acetic acid in the exhaust water has long posed a challenge in industry. These wastes containing acetic acid are typically processed via basic neutralization, characterized by high acidity and resistance to degradation, which can bring potential economic burden and environmental hazards. Here we report a new photocatalytic conversion route for addressing high concentrations of acetic acid. This process transforms acetic acid into valuable succinic acid through dehydrogenative coupling. Additionally, the photocatalytic conversion of acetic acid exhibits structure sensitivity when employing Pt cocatalysts of varying sizes. Through inhibiting the undesirable H termination of active free radicals over small Pt atoms and clusters, the rate of undesired decarboxylation reactions can be decreased by 75 %. This effectively enhances the selectivity of the coupling product succinic acid by 2.1 times, achieving a succinic acid formation rate of 7.28 mmol/(g cat •h). This work offers a theoretical guidance for searching value-added reaction pathways of acetic acid, thereby establishing an innovative approach for high concentration exhaust acetic acid treatment and converting low value monocarboxylic molecules into valuable diacid polymerization monomers under a mild and green condition.
研究领域:
环境科学
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化学工程
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催化科学
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产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2024
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IF 8.4
Yanshao Yang,Yuzhang Zhu,Youjing Zhao,Zejun Song,Di Zhu,Min Wang,Jian Jin,Wangxi Fang
Facilitated transport membranes (FTMs) constitute a promising group of membranes to achieve high precision ion separation, especially for ions with similar sizes and charges. Gelation is an effective means to improve the performance of FTMs by balancing the transport carrier mobility and stability in the membrane. Here, the phenomenon of gelation induced ion selectivity enhancement and its relation to transport resistance were systematically investigated, leading to the development of gelatinous FTMs designed for highly selective ion separation. The ion transport resistance across the FTM was regulated by controlling the degree and proportion of gelation. Interestingly, gelatinous FTMs with increased transport resistance exhibit a reduced passage of most ion species but favor the transport of ion species with a smaller size. By adjusting the extent of gelation, the membrane’s Li/K separation factor reached 150, more than three times incremented from a control membrane with only liquid phase carriers. Moreover, the negative impact of increased transport resistance on ion transport rate was offset by reducing the gel layer thickness, so that high ion selectivity was achieved while maintaining fast ion transport. Therefore, highly selective FTMs can be obtained by gelation induced ion transport behavior manipulation, and this work serves as a demonstration on designing high-performance lithium selective FTMs via gelation.
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Xianni Song,Xinhua Xu,Donglei Wu,Haijiao Xie
Sulfoxides are widely recognized as probes for identifying and evaluating the generation and contribution of high-valent metals in advanced oxidation processes. However, this paper was surprising to find that the presence of sulfoxides selectively enhanced the degradation of specific pollutants in the Fe(II)/PS system. Represented by methyl phenyl sulfoxide (PMSO), scavenging experiments for active species showed that the presence of PMSO transformed the mechanism from radical dominated (55.60 %) to nonradical dominated (60.91 %), greatly improving the anti-interference ability of the system. Determining the concentration of Fe(Ⅱ) and total iron (Fe tot ) in solution revealed that the presence of PMSO improved the utilization efficiency of Fe(II) and PS by enhancing the redox reaction between Fe(II) and PS, and resulted in the generation of Fe(IV) more favorably than the generation of SO 4 ·− and ·OH. Additionally, comparing the proven high-valent iron dominated Fe(II)/PI system with the free radical dominated Fe(II)/PS system of this paper, it was revealed that the selectively enhanced oxidation of PMSO specifically targets the free radical dominated system. Experiments have shown that the degradation of acetaminophen, ibuprofen, phenol, and p-chlorophenol was enhanced by PMSO, while the degradation of norfloxacin, primidone, chloramphenicol, sulfamethoxazole, p-nitrophenol, benzoic acid, and nitrobenzene was inhibited. Based on density functional theory (DFT) calculations, PMSO has a selectively enhanced degradation effect for organic pollutants with ionization potential (IP) below 8.66 eV, and vice versa, it has an inhibitory effect. The present study provides new insights into the contribution of sulfoxide to the assessment of high-valent metals and sheds new light on the mechanism of active species.
研究领域:
环境科学
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化学
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产品关联
DOI
高影响因子
LANGMUIR
·
2024
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IF 3.7
Hongyan Yu,Yongxue Chen,Zhenyu Wen,Rensheng Wang,Sisi Jia,Wenjie Zhu,Yanping Song,Huanhuan Sun,Bingbing Liu
Pressure-induced surface-enhanced Raman spectroscopy (PI-SERS) has garnered significant attention as a subfield of SERS detection due to its capacity to regulate the band gap between molecules and substrates through pressure modulation. Currently, SERS detection primarily focuses on single molecules at atmospheric pressure with limited investigations conducted under high pressure conditions. Herein, we employed rose-shaped MoS2 nanoflowers as the SERS substrate and realized selective PI-SERS enhancement of R6G molecules in the binary (MV+R6G) and ternary (MV+R6G+RhB) systems. The MoS2 demonstrated an exceptionally low SERS detection limit of 5 × 10–6 M in binary and ternary systems with equimolar amounts of molecules. High-pressure experimental results indicate that MoS2 displays selective enhancement for R6G molecules, as evidenced by the comparison of the PI-SERS peak intensity ratio between MoS2 and the probe molecules. The proposed enhancement mechanism in binary and ternary SERS systems under high pressure involves pressure-induced changes in both the band structures of the MoS2 substrate and molecules, thereby influencing their charge transfer dynamics. Consequently, this approach holds great promise for practical applications in complex SERS systems operating under extreme conditions.
研究领域:
材料科学
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光谱学
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化学
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产品关联
DOI
PubMed
高影响因子
Advanced Materials Interfaces
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2023
·Vol. 10
·期 12
·2202524
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IF 5.4
Lei Wang,Xianying Bai,Yawei Gu,Xinxin Shi,Shilong Wang,Jingxian Hua,Rujing Hou,Chongqing Wang,Yichang Pan
2D metal–organic frameworks are attractive filler in mixed matrix membranes (MMMs) due to the high aspect ratio and contact opportunity at the filler–polymer interface. However, their alignment in polymer matrix remains a challenge to fully play their functions. Herein, to our best knowledge, for the first time, the facile synthesis of KAUST-7-NH 2 (KAUST, King University of Science and Technology) nanoplate is reported with 1D channels with an aspect ratio greater than 30. The nanoplates are incorporated and aligned in the 4,4′-(hexafluoroisopropylidene) diphthalic anhydride-2,4-diaminomesitylene (6FDA-DAM) polymer matrix under the shear force with a filler loading up to 50 wt%. The large difference in adsorption abilities between CO 2 and CH 4 from the (001)-oriented KAUST-7-NH 2 nanoplate-based MMMs and the favorable interaction at the filler–polymer interface contribute to the excellent CO 2 /CH 4 separation performance. The resultant membranes show CO 2 /CH 4 selectivity with 66.2% enhancement (surpassed 2008 Robeson upper bound), antiplasticization up to 17 bar, and long-term stability up to 240 h indicating its good potential for natural gas treatment.
研究领域:
材料科学
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化学工程
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环境科学
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产品关联
DOI
高影响因子
ACS Applied Nano Materials
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2023
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IF 5.9
Jingwen Feng,Jinjuan Gao,Wen Yang,Yaru Li,Jian Shi,Cong Liu,Mingshun Jiang,Shouzhen Jiang
Two-dimensional (2D) metal–organic frameworks (MOFs) have promising applications in surface plasmon resonance (SPR) sensing for their intriguing exciton migration and visible light-near infrared absorption properties. In this study, an effective biosensing structure comprising 2D Cu-TCPP MOF nanosheet-capsulated Au film was developed, such that lower molecular-weight dopamine with small changes of refractive index can be identified on the fiber-optic platform. The large areas of ultrathin 2D Cu-TCPP MOF nanosheets were well prepared, the experimental results indicated that the sensitivity (48%) and figure of merit (18%) were increased notably compared with the bare Au film. Moreover, the finite element method was adopted to numerically analyze and verify the excellent charge-transfer ability of MOF nanosheets and the bidirectional gain properties between MOF nanosheets and Au films. Furthermore, the sensitivity [1.24 nm/log(M)] and selectivity of the dopamine were significantly enhanced with a low limit of detection of 1.50 × 10–13 M and linear response with a wide range of concentrations from 5 × 10–12 M to 5 × 10–7 M through ssDNA surface modification and conformation amplification. As revealed by the above-mentioned results, the Cu-TCPP/Au/SMF biosensor can serve as a promising nanoplatform for clinical diagnosis and medical assessment.
研究领域:
材料科学
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生物医学工程
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光学传感
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产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2021
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IF 7.46
Yiran Zhang,Bang Xiao,Lin Yang,Anqi Jiao,Ke Li,Chunping Wu,Reggie Zhan,Zhen Huang,He Lin
YSZ-based mixed-potential sensors with double-sensing electrodes were fabricated for ammonia (NH 3 ) detection. ZnO and LaCoO 3 nanoparticles prepared by flame spray pyrolysis (FSP) method were used as the sensing materials. The sensing responses of ZnO and LaCoO 3 sensing electrodes can be overlapped based on the double-sensing-electrode structure, thereby significantly enhancing the sensitivity compared with the traditional mixed-potential sensors using Pt reference electrode. The sensitivities of this sensor reached up to -102.85, -75.312, -70.165, -48.616 mV/decade to 10–50 ppm NH 3 at 450, 475, 500, 525 ℃ , respectively. Moreover, the NO 2 interference effects on NH 3 detection of ZnO and LaCoO 3 electrodes were opposite and can be counteracted based on the double-sensing-electrode structure, eliminating most of the cross-sensitivity to NO 2 . The double-sensing-electrode sensor exhibited good performance under CO, CH 4 , NO, NO 2 interference, oxygen fluctuation, and humidity variations, and showed good long-term stability. The results of sensing performance exhibited the sensors with double-sensing electrodes have a great potential for application on SCR system of diesel engines. In further studies, each sensing electrode can be optimized respectively and the sensitivity and selectivity of NH 3 sensors could be enhanced to a higher level.
研究领域:
传感器学
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材料科学
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环境监测
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能源工程
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气体传感
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纳米材料
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催化化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）