JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Tian Tian,Xuefeng Hu,Yao Huang,Huixian Du,Chao Wang,Mina Yang
The widespread utilization of fossil fuels has resulted in a significant increase in CO 2 emissions, leading to a variety of environmental issues. The photocatalytic conversion of CO 2 into fuel presents an effective solution to both the energy crisis and environmental warming. Therefore, the selection of a suitable catalyst is paramount. However, traditional photocatalysts often encounter challenges such as rapid electron-hole recombination and limited exposure of active sites. To improve these limitations, this study introduces AFM-X, a heterojunction catalyst composed of Au/Fe 3 O 4 /MIL-101(Fe)-X, which facilitates the formation of open metal sites (OMS) that enhance the effective separation of photogenerated carriers. In AFM-X, OMS function as Lewis acid sites, thereby enhancing CO 2 adsorption. The presence of Au nanoparticles (NPs) introduces additional active sites for CO 2 reduction. The synergistic effect between OMS and Au NPs increases the catalyst’s active sites, while the heterojunction construction promotes electron transfer, thereby enhancing CO 2 photocatalytic reduction efficiency. The CO generation rate of AFM-2 reached 98.8 μmol g −1 h −1 , surpassing those of FM, MIL-101(Fe), Fe 3 O 4 , and Au NPs, by 4.1, 6.3, 6.2, and 3.2 times, respectively. Furthermore, AFM-2 maintains stable performance over a 40 h cycle test. In-situ DRIFTS spectroscopy reveals that CO 2 reduction occurs through two parallel pathways. This study offers new insights into the design of composite photocatalytic materials, highlighting the effectiveness of OMS Lewis acid sites in significantly enhancing the photocatalytic reduction of CO 2 .
研究领域:
环境科学
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材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Xiaowu Liang,Pengfei Wang,Congli Li,Min Yuan,Qi Shi,Jinxiang Dong
CO is an important raw material and the separation of CO/N 2 in blast furnace gas can supply an abundant source of CO. Metal organic frameworks (MOFs) containing open metal sites are capable of selectively binding to CO over N 2 . However, the open metal sites easily bind to guest molecules during the preparation and activation process. In this study, typical MOFs containing open metal sites (Co-MOF-74) were used to investigate the activation behavior and corresponding CO/N 2 adsorptive separation performance. To characterize the removal and decomposition of guest molecules, TG-MS and NMR analysis of MOF-74 prepared under different activation conditions were performed. During the heat and vacuum process, the guest H 2 O and methanol (MeOH) molecules in Co-MOF-74 were first removed at 150 °C under vacuum. The aim of high temperature activation at 300 °C is the decomposition of a small amount of bind N,N-dimethylformamide (DMF) and terminal ligands occupying the open metal sites in Co-MOF-74. In addition, H 2 O molecules occupy the open metal sites of Co-MOF-74 during the filtration and MeOH wash steps under air, which is accompanied by the removal of a portion of DMF. The CO adsorption (298 K and 1 bar) and the CO/N 2 selectivity (Ideal adsorbed solution theory: 50:50, v/v) of Co-MOF-74 activated at 300 °C was 6.07 mmol/g and 384, respectively, which was higher than that of the other activated Co-MOF-74 samples and was attributed to the effective removal of guest molecules. Our results may guide the activation of MOFs, which contain open metal sites.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
LANGMUIR
·
2012
·
IF 4.186
Yan-Yan Fu,Cheng-Xiong Yang,Xiu-Ping Yan
Metal–organic frameworks (MOFs) with open metal sites have great potential for enhancing adsorption separation of the molecules with different polarities. However, the elution and separation of polar compounds on such MOFs packed columns using nonpolar solvents is difficult due to too strong interaction between polar compounds and the open metal sites. Here, we report the control of the coordination status of the open metal sites in MOFs by adjusting the content of methanol (MeOH) in the mobile phase for fast and high-resolution separation of polar compounds. To this end, high-performance liquid chromatographic separation of nitroaniline, aminophenol and naphthol isomers, sulfadimidine, and sulfanilamide on the column packed with MIL-101(Cr) possessing open metal sites was performed. The interaction between the open metal sites of MIL-101(Cr) and the polar analytes was adjusted by adding an appropriate amount of MeOH to the mobile phase to achieve the effective separation of the polar analytes due to the competition of MeOH with the analytes for the open metal sites. Fourier transform infrared spectra and X-ray photoelectron spectra confirmed the interaction between MeOH and the open metal sites of MIL-101(Cr). Thermodynamic parameters were measured to evaluate the effect of the content of MeOH in the mobile phase on the separation of polar analytes on MIL-101(Cr) packed column. This approach provides reproducible and high performance separation of polar compounds on the open metal sites-containing MOFs.
研究领域:
材料科学
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分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2025
·
IF 5.5
Jing Chen,Jiawen Li,Huanhuan Wang,Xincun Dou,Baiyi Zu
How to modulate the open metal sites (OMS) for enhancing the luminescence emerges as a significant issue to explore in the exploration of high-performance metal-organic frameworks (MOFs) for photoluminescence (PL) sensing and X-ray detection. Here, by efficiently extending the conjugation of the ligand, nanoscale Zr-ADIP, which has eight OMS per Zr cluster, was first synthesized and demonstrated to have enhanced PL and X-ray excited luminescence (XEL) performance. Furthermore, a modulator tuning strategy was adopted to occupy the OMS, which has been proven to be efficient for engineering the unoccupied electronic levels, promoting the relaxation of the excited electrons, and enhancing the PL efficiency. It is found that with benzoic acid as the modulator, the optimal nanoscale Zr-ADIP-BzOH exhibits superior performance with an X-ray detection limit of 0.53 μGy s–1, which is 10 times lower than the minimum X-ray dose rate requirement for medical X-ray imaging. The superior XEL performance of Zr-ADIP-BzOH has been further proven to be effective in the tentative monitoring of the morphology of a mature pearl in a clam sample by constructing a condensed film device. We expect that the proposed OMS introduction and modulator tuning strategy would offer insights for the structural design and performance enhancement of luminescent MOFs.
研究领域:
材料科学
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光学
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医学影像
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Xintong Li,Xianglin Wang,Min Li,Junhong Luo,Yongtao An,Peilong Li,Jiangfeng Song,Changan Chen,Xingwen Feng,Shuai Wang
Deuterium has numerous applications in industry and scientific research. However, the conventional methods for separation hydrogen isotopes face the problems of low selectivity and high energy consumption. Recently, microporous material adsorption separation technology provides an efficient way for the separation of hydrogen isotopes. Herein, we prepared the metal bistriazolate framework Ni 2 Cl 2 BBTA, featuring a high density of coordinatively unsaturated Ni 2+ sites. Interactions between the open metal sites and hydrogen render this material excellent separation ability for the capture of D 2 from the hydrogen isotopes mixture, with the D 2 over H 2 selectivity up to 4.5 at 77 K and 4.0 at 87 K respectively. Notably, recycle experiments show that this material has great potential in the application of hydrogen isotope separation, owing to its good structural stability and reusability .
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2017
·
IF 6.065
Songjian Zhao,Jian Mei,Haomiao Xu,Wei Liu,Zan Qu,Yong Cui,Naiqiang Yan
Metal-organic frameworks (MOFs) adsorbent Mil-101(Cr) was introduced for the removal of elemental mercury from sintering flue gas. Physical and chemical characterization of the adsorbents showed that MIL-101(Cr) had the largest BET surface area, high thermal stability and oxidation capacity. Hg 0 removal performance analysis indicated that the Hg 0 removal efficiency of MIL-101(Cr) increased with the increasing temperature and oxygen content. Besides, MIL-101(Cr) had the highest Hg 0 removal performance compared with Cu-BTC, UiO-66 and activated carbon, which can reach about 88% at 250 °C. The XPS and Hg-TPD methods were used to analyze the Hg 0 removal mechanism; the results show that Hg 0 was first adsorbed on the surface of Mil-101(Cr), and then oxidized by the open metal site Cr 3+ . The generated Hg 2+ was then combined surface adsorbed oxygen of adsorbent to form HgO, and the open metal site Cr 2+ was oxidized to Cr 3+ by surface active oxygen again. Furthermore, MIL-101(Cr) had good chemical and thermal stability.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Caijiao Yu,Yueyao Liang,Xiangyu Guo,Zhihua Qiao,Chongli Zhong
Metal-organic framework (MOF)-mixed matrix membranes (MMMs) have the potential to overcome the trade-off limitations between gas separation performance and large-scale fabrication. However, most conventional MOF MMMs are used for CH 4 /N 2 separation systems, the preparation of MOF-MMMs with high permeance and good selectivity for N 2 /CH 4 separation has rarely been reported. Here in, we propose supported thin MOF-MMMs with abundant open metal sites to preferentially adsorb N 2 and improve the N 2 /CH 4 separation performance. The formation of the selectivity layer with abundant open metal sites was realized through dual-induction mechanism of in-situ Co 2+ ion doping and polydimethylsiloxane (PDMS) solution post-modification. The introduction of Co 2+ ions restricted the coordination of Zn-N and increased the number of open metal sites in the ZIF layer during its formation. The post-treated PDMS solution with weak acid could further induce the formation of open metal sites. Meanwhile, the electron paramagnetic resonance and synchrotron radiation-based XAFS results also confirmed that the number of open metal sites in the separation layer increased gradually with the in-situ Co 2+ ion decoration and PDMS solution post-modification. In addition, the PDMS also could repair the intercrystalline defects of the MOF membranes and reduce their non-selectivity area. Therefore, the synthesized ZIF-8 MMMs showed a high N 2 permeance of 1367 GPU and a moderate N 2 /CH 4 selectivity of up to 6.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2020
·
IF 3.421
Houxiao Wu,Yinuo Yuan,Yongwei Chen,Daofei Lv,Shi Tu,Ying Wu,Zhong Li,Qibin Xia
CO2 capture and storage technologies have been adopted to eliminate anthropogenic CO2 emission. Compared with other methods, adsorptive separation technology using excellent adsorbents has attracted extensive attention for its operational flexibility and energy-efficient characteristics. Herein, we present a copper-based metal–organic framework, MOF-11, exhibiting highly efficient CO2/N2 (15:85, v/v) separation performance. There are two kinds of channels with different pore chemistries in the framework, in which dense Cu open metal sites (OMS) were found in channel I, while channel II had a narrower pore window size and was mainly decorated with −CH2 moieties from the organic ligands. At 298 K, the CO2 uptake value of MOF-11 was 4.63 mmol/g at 100 kPa and 2.92 mmol/g at 15 kPa, respectively, which was superior to many other reported MOF adsorbents. Molecular simulation indicated that CO2 dominantly occupied channel I due to the strong electrostatic interactions with the dense Cu OMS in channel I. In comparison, more N2 molecules were adsorbed into channel II through multiple weak van der Waals interactions with −CH2 moieties. Such a pore system gives MOF-11 high CO2/N2 selectivity (ca. 116 at 298 K). Moreover, the dynamic separation of CO2/N2 mixture gases on MOF-11 was further investigated by cyclic breakthrough experiments.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Zhong Li,Wenzhe Sun,Chong Chen,Qirui Guo,Xue Li,Mengwei Gu,Nengjie Feng,Jing Ding,Hui Wan,Guofeng Guan
Targeting CO 2 capture at low pressure due to the partial pressure of CO 2 in flue gases (0.01 MPa–0.02 MPa), a facile method was constructed to build functional UiO-66 structure via mixing ligands of terephthalic acid and 1,2,4-benzenetricarboxylic acid. The free -COOH from 1,2,4-benzenetricarboxylic acid could graft quantitative and dispersive deep eutectic solvents onto UiO-66 with reserved open metal sites for CO 2 adsorption. Compared to 1,3,5-benzenetricarboxylic acid, mixing ligands by 1,2,4-benzenetricarboxylic acid preserved the stability of UiO-66 structure, which was more suitable for CO 2 capture from flue gases. The active -NH 2 and -OH groups from incorporated DES synergized with the intrinsic open metal sites to enhance the CO 2 uptake at low pressure and improve adsorption selectivity of CO 2 /N 2 . At 298 K, the CO 2 uptake of DES@UiO-66-COOH(0.05) was increased by 26% at 1 bar and 50% at 0.15 bar compared to UiO-66. In addition, the selectivity of CO 2 /N 2 for DES@UiO-66-COOH(0.05) was 24.7 times as high as UiO-66 at low pressure. The strong interaction between guest CO 2 and modified UiO-66 was confirmed by higher isosteric heats of adsorption (Q st ) for DES-appended UiO-66. Even so, the sample could be regenerated at 373 K and vacuum, and could be recycled without drop of CO 2 uptake after 6 times.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2017
·Vol. 2018
·期 2
·194-202
·
IF 2.444
Zhong Li,Xue Li,Chong Chen,Lijin Zhou,Qirui Guo,Dashui Yuan,Hui Wan,Jing Ding,Guofeng Guan
Graphical A facile route is applied to fabricate Zr–TCPP MOFs with incorporated open metal sites M 3+ (Fe 3+ and Al 3+ ) to enhance CO 2 uptake through strong interaction between central M 3+ and CO 2 molecules. Moreover, the CO 2 uptake on Zr–TCPP MOFs with extra Al 3+ ions is higher than that with extra Fe 3+ ions, and is ascribed to the higher isosteric heat of CO 2 adsorption. Developing adsorption materials to capture CO 2 at low pressure has attracted great attention due to the low CO 2 partial pressure in fuel gases. Herein, zirconium-based metal–organic frameworks (PCN-X) are successfully synthesized and open metal sites (Fe 3+ and Al 3+ ) are incorporated into the PCN-X MOFs. The results indicate that the CO 2 adsorption capability is enhanced through the strong interaction between extra open metal centers and CO 2 molecules at low pressure. Meanwhile, the CO 2 adsorption capacity of PCN-X with incorporated Al 3+ is higher than with incorporated Fe 3+ , which can be attributed to the higher isosteric heat of CO 2 adsorption. The adsorption kinetics further indicate the faster CO 2 transmission on PCN-X with extra Al 3+ than with extra Fe 3+ . Besides, modified PCN-X, treated by some inorganic acids, exhibits favorable chemical stability, which is suitable for CO 2 capture from acidic fuel gases.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Functional Materials Letters
·
2024
·
IF 1.2
Jianhang Hai,Shuli Wei,Jie Zou,Lele Wang,Yunqing Lu,Jin Wang
In this work, we activate metal-organic frameworks (MOFs) by applying the general vacuum heating (VH) method or the solvent exchange (SE) method, and encapsulate PSt into the MOF channels by the in-situ polymerization. For the SE method, methanol is optimal to exchange the DMF molecules inside MOF. The effectiveness of these two activation methods is compared. The results show that the MOF activated via the SE method has a higher specific surface area and a larger pore volume than the MOF activated via the general VH method. Also, the SE method is more efficient for the removal of DMF from the MOF channels, and leaves more open metal sites. Specifically, the amounts of loaded monomers inside the MOF activated via the SE method and the general VH method are 4.58 and 2.67 mmol/cm 3 . Furthermore, the MOF activated via the SE method has better retention of the channel structure and more free volume in the channels. This can increase the mobility of the monomers. As a consequence, the conversion rate of 47.57% from St to PSt is achieved in the MOF activated via the SE method, which is 50.21% higher than that obtained via the general VH method.
研究领域:
材料化学
·
纳米多孔材料
·
高分子科学
·
配位化学
·
功能材料
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Fang Zheng,Lidong Guo,Rundao Chen,Feng Zhou,Zhiguo Zhang,Qiwei Yang,Yiwen Yang,Qilong Ren,Zongbi Bao
The separation of hexane isomer mixtures into their individual components is one of the most important while challenging industrial process to produce high-octane gasoline. Herein robust M(pz)[Ni(CN) 4 ], termed MpzNi (M = Co, Ni, pz = pyrazine) that can realize efficient separation of ternary mixtures into the pure, individual components. As optimal pore channels with double-accessible open metal sites providing the adsorbate-dependent affinity differences for molecular exclusion behavior via temperature programming, CopzNi reached optimum performance with not only exceptional selectivity of linear/monobranched alkanes and monobranched/dibranched alkanes, but also notably higher adsorption capacity than those of the previously reported adsorbents. Breakthrough experiments with equimolar ternary C6 alkane isomers and binary branched mixtures confirmed CopzNi can highly capture n -hexane and 2-methylpentane from their mixtures. The excellent separation efficiency, lower-energy regeneration, scalability, recyclability as well as high stability render the CopzNi a benchmark candidate for implementation in the current separation processes.
研究领域:
化学工程
·
材料科学
·
分离技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）