MICROPOROUS AND MESOPOROUS MATERIALS
·
2018
·
IF 3.649
Tongtong Wang,Xuedan Song,Qunxing Luo,Xiaodong Yang,Siying Chong,Jie Zhang,Min Ji
In terms of ‘green chemistry’ and ‘atom economy’, the cycloaddition of CO 2 to yield cyclic carbonate without any additive is an eco-friendly way to utilize CO 2 . Unfortunately, the low CO 2 capture quantity of common catalysts limited its catalytic efficiency. Herein, a novel acid-base bifunctional catalyst was successfully prepared by immobilizing ionic liquid on MIL-101-NH 2 (IL/MIL-101-NH 2 ) and tested for propylene carbonate (PC) rapid and facile synthesis from CO 2 and propylene oxide (PO). The synergetic interaction between Lewis base with strong CO 2 chemical capture capacity and Brønsted acid with strong hydrogen bond donor leads to the high catalytic efficiency of IL/MIL-101-NH 2 for carbonate synthesis from CO 2 and PO without any additive. The immobilization mode between MIL-101-NH 2 and IL is energetically supported by the density functional theory (DFT) calculations. This design idea of specific catalyst and the acid-base synergetic strategy provides new insights into the design of powerful catalyst systems for the CO 2 conversion.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2016
·
IF 3.926
Saichai Lin,Ning Gan,Yuting Cao,Yinji Chen,Qianli Jiang
In this paper, a novel dispersive solid phase extraction (dSPE) adsorbent based on aptamer-functionalized magnetic metal-organic framework material was developed for selective enrichment of the trace polychlorinated biphenyls (PCBs) from soil sample. Firstly, we developed a simple, versatile synthetic strategy to prepare highly reproducible magnetic amino-functionalized UiO-66 (Fe 3 O 4 @PDA@UiO-66-NH 2 ) by using polydopamine (PDA) as covalent linker. Then amino-functionalized aptamers which can recognize 2,3′,5,5′-tetrachlorobiphenyl (PCB72), 2′,3′,4′,5,5′-pentachlorobiphenyl (PCB106) were covalent immobilized on UiO-66-NH 2 through coupling reagent of glutaraldehyde. Aptamer-functionalized adsorbent (Fe 3 O 4 @PDA@UiO-66-Apt) can specifically capture PCBs from complex matrix with high adsorption capacity based on the specific affinity of aptamer towards target. Moreover, the adsorbent can be easily isolated from the solution through magnetic separation after extraction. Afterwards, the detection was carried out with gas chromatography tandem mass spectrometry (GC–MS). The selective dSPE pretreatment coupled with GC–MS possessed high selectivity, good binding capacity, stability, repeatability and reproducibility for the extraction of PCBs. Furthermore, the adsorbent possessed good mechanical stability which can be applied in replicate at least for 60 extraction cycles with recovery over 80%. It provided a linear range of 0.02–400 ng mL −1 with a good correlation coefficient (R 2 = 0.9994–0.9996), and the limit of detection was found to be 0.010–0.015 ng mL −1 . The method was successfully utilized for the determination of PCBs in soil samples.
研究领域:
环境科学
·
分析化学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 11
·1-10
·
IF 6.408
Fan Ru,Tian Jinrong,Wang Huili,Wang Xuedong,Zhou Peipei
By employing NH 2 -MIL-88 as a template, we synthesized the intermediate Fe@CN under high-temperature calcination and further fabricated the FeS 2 @CN nanocomposites in the presence of sulfur powder. Under varying temperatures (300–600 °C) and Fe@CN-to-S ratios (1:3–6), FeS 2 @CN 500-5 nanocomposites had the highest peroxidase-mimetic activity. Under optimized conditions (incubation temperature 40 °C; solution pH 4.0 and nanocomposite concentration 10 μg/mL; 652-nm absorption), the Michaelis-Menten constant ( K m ) of FeS 2 @CN was much lower than that of horseradish peroxidase (HRP), therefore demonstrating that it had a higher affinity for both chromogenic substrates than conventional HRP. The limits of detection for H 2 O 2 and glucose were 0.15 and 0.30 μmol/L, respectively, and the recoveries for glucose were 91.8–103% with RSDs <5.2%. The novelty of this study lies in (1) the FeS 2 @CN was confirmed to possess stronger enzyme-mimetic activity than its precursors (NH 2 -MIL-88 and Fe@CN); (2) the enhanced activity resulted from the unsaturated sites of N and S doping and the plentiful defects on the porous carbon surface; and (3) free radical trapping experiments evidenced that •OH played a major role in the catalytic reaction, while h + and •O 2 − simultaneously participated in the catalytic process. These convincing performance metrics lead us to postulate that the FeS 2 @CN-based colorimetric biosensor provides a promising approach for several real-world applications, such as point-of-care diagnosis and workplace health evaluations. Graphical abstract
研究领域:
生物化学
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分析化学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2021
·
IF 3.498
Meimei Zhou,Wei Zou,Xuemei Zhu,Huachen Ma,Pengbo Wang,Jiaxin Shang,Pingping Luo
UIO-66-NH 2 was successfully deposited on electrospun polyacrylonitrile (PAN) nanofibers treated by thermal oxidative stabilization (TOS) via a simple and effective in situ growth method. Owing to the formation of acridone rings, naphthyridinering rings and hydronaphthyridine rings during the TOS process, the thermally stabilized electrospun PAN (TSPAN) nanofibers were greatly improved in stability and heat resistance and could provide adequate nucleation points for MOFs growth, indicating an ideal MOFs deposition support without additional surface modifications. The results demonstrated that UIO-66-NH 2 crystals distributed relatively uniform and dense on the TSPAN nanofibers with mass loading up to 28.1 wt%. Compared with powdered UIO-66-NH 2 , the formed UIO-66-NH 2 @TSPAN nanofibers showed enhanced visible light driven photocatalytic activity towards reduction of Cr(VI) due to the improvement of visible light response, more excellent photothermal conversion ability and the increase of exposed active sites. The photocatalytic reduction rate of Cr(VI) over UIO-66-NH 2 @TSPAN was up to 93% within 180 min and the rate constant (k = 0.1362) was 2.3 times that of powdered UIO-66-NH 2 (k = 0.00576). Significantly, the mechanical flexibility and structural stability endowed the nanofibrous photocatalyst easy operation and outstanding reusable capability. The photocatalytic activity for Cr(VI) reduction still preserved 90% after five cycles. This work proposes a facile strategy for preparation of free-standing MOFs nanofibers and provides MOFs-based photocatalysts a new opportunitie for broad applications in water treatment.
研究领域:
材料科学
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环境催化
·
纳米材料
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光化学
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水处理技术
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 12
·期 2
·1218-1232
·
IF 11.9
Zi-Yang Zhang,Hao Tian,Han Jiao,Xin Wang,Lei Bian,Yuan Liu,Nithima Khaorapapong,Yusuke Yamauchi,Zhong-Li Wang
The electrochemical CO2 reduction reaction (CO2RR) for high value-added multi-carbon product (C2+) production over copper oxide-based catalysts is an important way to realize the carbon cycle. However, developing effective reaction interfaces and microenvironments to improve the Faraday efficiency (FE) and current density of C2+ remains a major challenge. Herein, we construct Cu0–Cu+–NH2 composite interfaces with the assistance of SiO2. Using Cu2O nanoparticles as a model catalyst, a layer of porous SiO2 is first coated on the surface of the particles, and then, a silane coupling agent containing –NH2 is bonded on the surface of SiO2. The strong interaction between SiO2 and Cu2O at the interface induces the oxidation effect of low valent Cu, and even under the CO2RR, part of Cu+ is reduced to Cu0 and part of Cu+ still maintains positive valence, forming the interface of Cu0–Cu+. SiO2 also acts as a bridge between copper species and –NH2 to create a Cu catalyst–NH2 group interface. With the help of the synergistic effect of the composite interfaces, the optimized Cu2O@SiO2–NH2 catalyst achieves a FE of 81.2% for C2+ products with a current density of 292 mA cm−2 at −1.7 V versus a reversible hydrogen electrode. In situ Raman and attenuate total reflectance-infrared absorption spectroscopy spectra show that the interaction between surface –NH2 and CO2 molecules enhances the adsorption and activation process of CO2 and promotes the formation of CO intermediates (*CO). On the Cu0–Cu+ interface, the C–C coupling process between *CO is accelerated, and the two interfaces synergistically promote the generation of C2+ products. This work provides a new strategy for constructing composite interfaces to improve the CO2RR to C2+ products.
研究领域:
电化学
·
材料科学
·
催化
·
可持续能源
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2025
·
IF 8.1
Si-yuan He,Wei Wen,Peng Wu,Zhe Meng
Developing a green and efficient technology for decomposing aflatoxin B 1 (AFB 1 ) and ochratoxin A (OTA) in grains has important theoretical value and application prospects for ensuring food safety. A dual Z-scheme ternary heterojunction photocatalyst, Sr 2 MgSi 2 O 7 :Eu 2+ ,Dy 3+ /BiVO 4 /NH 2 -UiO-66 (SBN), was prepared via a self-assembling hydrothermal approach. The SBN heterojunction photocatalyst exhibits round-the-clock photocatalytic activity due to the intrinsic light source of Sr 2 MgSi 2 O 7 : Eu 2+ , Dy 3+ (SMS). Dual Z-scheme mechanism was proposed and validated through detailed analysis of quenching experiments, ESR spectra, band arrangement, and charge transfer processes. The dual Z-scheme mechanism not only promotes the effective transfer and separation of photo generated charge carriers during charge carrier transport, but also maintains significant reduction and oxidation potentials. SBN photocatalyst exhibits stable and persistent photocatalytic performance, significantly enhancing the degradation efficiency of AFB 1 and OTA under all-weather conditions. Experimental data shows that the removal rate of AFB 1 increased from 69.60 % after 60 min of illumination to 83.9 % after 4 h of turning off the light source; At the same time, the removal rate of OTA increased from 64.8 % to 78.1 %. •O 2 − and •OH were identified as key active species in photocatalytic reactions. Based on the analysis of AFB 1 and OTA degradation intermediates and the prediction of degradation sites using density functional theory (DFT), degradation pathways for AFB 1 and OTA were proposed. Collectively, these findings suggest a highly promising practical approach for the detoxification of mycotoxins in grain commodities.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
·
IF 11.2
Haoyuan Zheng,Yuxiao Jia,Chen Jin,Hang Che,Chia-TseLee,Guang Liu,Li Wang,Yuyuan Zhao,Shixuan He,Haizhen Liu,Xinhua Wang,Yifeng Yu,Mi Yan
The magnesium based metal hydrogen storage composite system Mg(NH 2 ) 2 -2LiH has a theoretical hydrogen storage capacity of 5.6 wt.% and is a promising hydrogen storage material for vehicles. However, its application is limited due to serious thermodynamic and kinetic barriers. Introducing efficient catalysts is an effective method to improve the hydrogen storage performance of Mg(NH 2 ) 2 -2LiH. This article investigates for the first time the use of nano rare earth oxide CeO 2 (∼44.5 nm) as an efficient modifier, achieving comprehensive regulation of the hydrogen storage performance of Mg(NH 2 ) 2 -2LiH composite system through oxygen vacancy driven catalysis. The modification mechanism of nano CeO 2 is also systematically studied using density functional theory (DFT) calculations and experimental results. Research has shown that the comprehensive hydrogen storage performance of the Mg(NH 2 ) 2 -2LiH-5 wt.% CeO 2 composite system is optimal, with high hydrogen absorption and desorption kinetics and reversible performance. The initial hydrogen absorption and desorption temperatures of the composite system were significantly reduced from 110/130°C to 65/80°C, and the release of by-product ammonia was significantly inhibited. Under the conditions of 170°C/50 min and 180°C/100 min, 4.37 wt.% of hydrogen can be rapidly absorbed and released. After 10 cycles of hydrogen release, the hydrogen cycle retention rate increased from 85% to nearly 100%. Further mechanistic studies have shown that the nano CeO 2− x generated in situ during hydrogen evolution can effectively weaken the Mg–N and N–H bonds of Mg(NH 2 ) 2 , exhibiting good catalytic effects. Meanwhile, oxygen vacancies provide a fast pathway for the diffusion of hydrogen atoms in the composite system. In addition, nano CeO 2− x can effectively inhibit the polycrystalline transformation of the hydrogen evolving product Li 2 MgN 2 H 2 in the system at high temperatures, reducing the difficulty of re-hydrogenation of the system. This study provides an innovative perspective for the efficient modification of magnesium based metal hydrogen storage composite materials using rare earth based catalysts, and also provides a reference for regulating the comprehensive hydrogen storage performance of hydrogen storage materials using rare earth catalysts with oxygen vacancies.
研究领域:
材料科学
·
催化
·
氢气存储
·
纳米技术
✓ 已验证
DOI
高影响因子
JOURNAL OF RARE EARTHS
·
2024
·
IF 5.2
Haoyuan Zheng,Yuxiao Jia,Chen Jin,Hang Che,Chia-Tse Lee,Zhenke Chen,Guang Liu,Li Wang,Shixuan He,Xinhua Wang,Haizhen Liu,Mi Yan
The Mg(NH 2 ) 2 -2LiH composite system is a promising vehicle-mounted hydrogen storage material, but its application is limited due to serious thermodynamic and kinetic barriers. Adding additives can effectively optimize their hydrogen absorption and desorption kinetics and thermodynamic performance. In this work the comprehensive hydrogen storage performance of Mg(NH 2 ) 2 -2LiH with extremely small nano rare earth borides is improved, and a series of characterization methods and density functional theory (DFT) calculation systems was combined to study its hydrogen storage improvement mechanism. The research results show that the method of adding 5 wt% molten salt to prepare nano CeB 6 (24.5 nm) can significantly reduce the initial hydrogen absorption/release temperature of Mg(NH 2 ) 2 -2LiH from 110/130 to 45/90 °C, inhibit the generation of ammonia by-products, and improve hydrogen purity. Under low-temperature hydrogen absorption conditions at 120 °C, the improved sample can absorb 2.81 wt% hydrogen gas, with a hydrogen absorption capacity more than 3.5 times of the unmodified sample. The amount of hydrogen released at 150 °C reaches 3.35 wt%, which is more than twice that of the pristine sample, demonstrating excellent hydrogen absorption and release kinetics performance. After 10 consecutive hydrogen cycles, 4.64 wt% hydrogen can still be released, and the cycle retention rate can be increased from 85% before improvement to nearly 100%, demonstrating good reversibility. Mechanism studies show that nano CeB 6 can effectively weaken the Mg–N and N–H bonds of Mg(NH 2 ) 2 and inhibit the polycrystalline transformation of the hydrogen evolution product Li 2 MgN 2 H 2 at high temperatures. It can also provide nucleation active sites for hydrogen absorption and desorption in the material, making the system possess superior hydrogen absorption and desorption performance and cycling stability. This study provides new insights into the role of rare earth borides in Mg(NH 2 ) 2 -2LiH hydrogen storage materials, both experimentally and theoretically.
研究领域:
材料科学
·
化学工程
·
物理化学
·
理论化学
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 55
·期 34
·16171-16183
·
IF 3.553
Liu Shengjun,Zou Qichao,Ma Yan,Sun Wen,Li Yu,Zhang Jian,Zhang Cheng,He Lifang,Sun Yudie,Chen Qian,Liu Bo,Zhang Hexin,Zhang Kui
Metal–organic frameworks (MOFs) are a new type of porous crystal materials that have been widely used in various fields. Owing to their adjustable porous structure, MOF photocatalysts with high catalytic activity have become a research hotspot. In this study, NH 2 -MIL-125/CoS x samples were investigated as a novel visible light-responsive catalyst for the removal of organic dye. The NH 2 -MIL-125/CoS x -20 composites showed the best photodegradation efficiency, where photodegradation of the rhodamine B reached 95.4% in 45 min. CoS x was able to effectively extend the wavelength absorption range of NH 2 -MIL-125 and effectively separate the photogenerated electrons and holes and that could lead to the improved photocatalytic performance of the composites. The reactive superoxide radical ( · O 2− ) was identified as the main active species using reactive species capture experiments, and a reasonable photocatalytic mechanism was proposed. This paper is intended to guide the development of organic–inorganic hybrid materials for environmental remediation.
研究领域:
材料科学
·
环境科学
·
化学
·
纳米技术
✓ 已验证
DOI
高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Zhiyong Bai,Lehui Liu,Zhoubin Lin,Kang Min Ok
A novel guanidinium-templated ultraviolet (UV) nonlinear optical zinc carbonate crystal, [C(NH2)3]2Zn(CO3)2 (GZCO), has been synthesized in a closed system at low temperatures. GZCO crystallizing in the tetragonal noncentrosymmetric nonpolar space group, P41212 exhibits a three-dimensional anionic framework constructed by interconnected [Zn6C6O32] 12-membered ring channels with inorganic CO3 triangles and ZnO4 tetrahedra. Notably, the anhydrous GZCO shows a very high thermal stability among guanidine-based hybrid NLO materials benefiting from the confinement effect of the organic cations within inorganic channels. The UV–visible transmittance spectrum reveals that GZCO has a short UV cutoff edge of 210 nm, corresponding to the large band gap of 5.9 eV. GZCO exhibits a mild second-harmonic generation efficiency of 0.5 × KH2PO4 with type-I phase-matching behavior.
研究领域:
材料科学
·
光学
·
化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Qianqian Huang,Yun Hu,Yun Pei,Jinhui Zhang,Mingli Fu
TiO 2 @NH 2 -MIL-125, composite photocatalysts with close interfacial contact between NH 2 -MIL-125 and TiO 2 , were successfully synthesized via an in-situ solvothermal method for formaldehyde (HCHO) removal under UV irradiation. Samples were characterized by using a variety of analytical techniques. The results showed that TiO 2 particles were highly dispersed on the surface of NH 2 -MIL-125, and there was a strong electronic interaction (Ti-N-C) between elements of the composite. TiO 2 @NH 2 -MIL-125 exhibited significantly enhanced photocatalytic performance for HCHO removal compared to pure TiO 2 and NH 2 -MIL-125 that was ascribed to the synergistic combination of high adsorption capacity of NH 2 -MIL-125, high dispersion of TiO 2 and efficient interfacial charge transfer between TiO 2 and NH 2 -MIL-125. Furthermore, the HCHO removal rate over the composite remained at 90% after 122 h of continuous photocatalytic reaction, indicating the high stability of the catalyst. This work provides new insights that will be helpful in the further development of photocatalysts for indoor air purification.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Zhikun Huang,Haojie Yu,Li Wang,Xiaowei Liu,Shuning Ren,Jinyi Liu
Designing graphitic carbon nitride (CN) based heterostructured photocatalysts with high catalytic activity is highly desired for peroxymonosulfate (PMS) activation to degrade organic pollutants from water. Herein, a novel heterostructured composite (U-F@CN) consisting of ferrocene-modified Uio-66-NH 2 (U-F) and CN was synthesized. The U-F@CN exhibited superior photocatalytic performance to degrade bisphenol A (BPA) in the presence of PMS under visible light. The experimental results indicated that BPA could be removed entirely by U-F@CN within 60 min under visible light irradiation. In addition, the outstanding photocatalytic activity could be maintained at high level in a wide pH range, appropriate temperature region and natural water condition. Benefiting from the good chemical stability, outstanding optical property and in-situ generation of interfacial heterojunction of U-F@CN, the interfacial transport of photogenerated charges could follow the Z-scheme mechanism, which can accelerate the charge separation and transport to yield abundant reactive active species (ROS) to efficiently active PMS and under visible light. This work provides a novel approach to design CN-based heterostructured photocatalysts with high stability and superior photocatalytic activity for environmental remediation.
研究领域:
材料科学
·
环境科学
·
化学
·
光催化
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）