Nanomaterials
·
2023
·Vol. 13
·期 14
·2072
·
IF 5.3
Xu Zhang,Bo Tian,Zhiheng Ma,He Wang,Zhixuan Cheng,Jiaqiang Xu
As a volatile air pollutant, formaldehyde can enter people’s living environment through interior decoration, furniture and paint, causing serious harm to human health. Therefore, it is necessary to develop a sensor for the real-time detection of formaldehyde in low concentrations. According to the chemical interaction between amino groups and formaldehyde, a MIL-101(Cr) aminated-material-based formaldehyde cantilever sensor was prepared, of which ethylenediamine- functionalized MIL-101(Cr) named ED-MIL-101(Cr)) showed the best gas sensing performance. Using quasi-in situ infrared spectroscopy, ED-MIL-101(Cr) was found bound to formaldehyde through a Schiff base. The adsorption enthalpy of formaldehyde-bound ED-MIL-101(Cr) was −52.6 kJ/mol, which corresponds to weak chemical adsorption, so the material showed good selectivity. In addition, ED-MIL-101(Cr) has the most active sites, so its response value to formaldehyde is larger and it takes longer to reach saturation adsorption than bare MIL-101(Cr). Through the research on the gas sensing performance of functionalized MIL-101(Cr) material, we found that it has a strong application potential in the field of formaldehyde monitoring, and the material performance can be quantitatively and accurately evaluated through combining calculation and experimentation for understanding the gas sensing mechanism.
研究领域:
材料科学
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环境科学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 26
·11164-11171
·
IF 3.288
Zhuo Wang,Jin Liu,Zhen Li,Xianbiao Wang,Ping Wang,Di Wang,Fengjun Zhang
A crosslinkable UIO-66 type MOF material denoted UIO-66-DETA composed of Zr(IV) metal ions and 2,5-diallyl ether terephthalic acid (DETA) was synthesized, and then by initiating double bond crosslinking, a new crosslinking MOF material denoted UIO-66-DETA-CL was obtained. UIO-66-DETA and UIO-66-DETA-CL were characterized by FTIR spectroscopy, PXRD, 1H solid-state NMR spectroscopy, SEM, nitrogen sorption, thermogravimetric analysis and hydrogen storage tests to analyze their structure and properties. The results showed that a crosslinked structure has been formed, and UIO-66-DETA-CL can maintain its structure below 340 °C, compared with UIO-66-DETA; its carbon residual rate is improved, which shows that the crosslinking modification enhances the thermal stability. Meanwhile, the hydrogen uptake capacity of UIO-66-DETA-CL reaches 5.36 wt% at 77 K and 4 MPa. Furthermore, the hydrogen adsorption enthalpy of UIO-66-DETA-CL (ΔHUIO-66-DETA-CL) calculated using the Arrhenius equation reaches −0.889 kJ mol−1, which is significantly improved by crosslinking modification. The crosslinked structure changes the pore size and increases the active adsorption sites in organic ligands. The framework of UIO-66-DETA-CL can provide more polar charges to cause some hydrogen molecules to be negatively charged because of a small HOMO–LUMO gap, and a lower LUMO energy level of UIO-66-DETA-CL enables stronger negative charge acceptability. Therefore, crosslinking modification enhances the material's hydrogen storage capacity. This result provides a new idea for the crosslinking modification of MOFs.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2019
·
IF 6.393
Dan Zhang,Yu Fan,Gaojie Li,Wei Du,Runlong Li,Yiming Liu,Zhixuan Cheng,Jiaqiang Xu
A series of zeolitic imidazolate frameworks (ZIFs) were synthesized by a facile and environmental friendly biomimetic method. The textural properties of the ZIFs were characterized by PXRD, FESEM, TEM and FT-IR spectra. These results showed ZIF 90 having typical rhombic dodecahedron crystals with a diameter of 800–1200 nm. Furthermore, the presence of rich aldehyde groups is confirmed through chemical analysis. Gas-sensing tests of quartz crystal microbalance (QCM) transducers based on ZIFs were investigated. The results showed that ZIF-90 based sensors exhibited excellent sensing performance towards low concentration of acetone vapor, such as high sensitivity (the frequency shift was 95 Hz @ 1 ppm), fast response (the response/recovery time was 12 s/17 s, respectively) and good selectivity. On the basis of temperature-varying experimental method, a moderate adsorption enthalpy (the value of ΔH θ was −57.93 kJ/mol) was obtained, indicating the existence of weak and reversible chemisorption between ZIF-90 and acetone molecules. The value of adsorption enthalpy (ΔH = −60.10 kJ/mol) obtained from Density functional theory is in close agreement with the experimental results.
研究领域:
材料科学
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化学工程
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传感器技术
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产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2025
·Vol. 12
·期 12
·4007-4018
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IF 6.4
Hong-Juan Lv,Yunhui Zhai,Ying-Ying Xue,Jiao Lei,Wenyu Yuan,Quan-Guo Zhai
Adsorption-based separation techniques are pivotal in the purification of C2H2, leveraging their eco-friendly and energy-efficient attributes. However, the reusability of adsorbents is highly restricted by the trade-off between adsorption capacity and adsorption enthalpy, which is required to be urgently addressed. Herein, we demonstrated that the implantation of distortable ligands with functional groups is efficient in solving the above issue. The functional groups provided binding sites for C2H2 adsorption, while the distortable ligands optimized the pore structures to reduce adsorption enthalpy, thus balancing the trade-off between adsorption capacity and enthalpy. A series of ultra-microporous MOFs was successfully constructed by employing different pyridine ligands. The adsorption capacity of SNNU-504 after optimization was effectively enhanced, while the adsorption enthalpy hardly increased due to the adjustable ligand torsion angle. Breakthrough experiments and GCMC simulations further verified the potential C2H2/CO2 separation applications.
研究领域:
材料科学
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化学工程
·
吸附技术
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分离科学
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纳米多孔材料
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 6
·1788-1798
·
IF 6.177
Jing Zhao,Yanzhuo Zhang,Hucheng Zhang,Haiyan Wang,Jianji Wang
Hydrogen spillover is an important theme for hydrogen storage and H-involving catalytic reactions. This work shows that catalytic reactivity and selectivity can be revealed by differentiating the energetic characteristics of spilled H species. With the assistance of Ti, F and C in MXenes, Pd1.8Ni@Ti3C2Tx presents a high capacity for spillover hydrogen storage at ambient temperatures, and the rich oxygenated groups act as the main carriers of hydrogen spillover around metal nanoparticles. Thermodynamic analysis reveals that the catalytic performances are energetically dominated by the adsorption enthalpies of the active spilled H species rather than the amount of spillover hydrogen, and can be tuned by alloying and surface modification. The ideas are verified from the excellent catalysis, chemoselectivity and stereoselectivity of Pd1.8Ni@Ti3C2Tx in semihydrogenations. The strategy of maximizing catalytic performances is applicable to other Pd-based bimetals@Ti3C2Tx, such as Pd2.6Co@Ti3C2Tx and Pd1.5Fe@Ti3C2Tx, and provides new energetics perspectives to understand the catalytic mechanism in spillover-involving chemical procedures.
研究领域:
催化
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材料科学
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化学工程
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Kai Zong,Dongshun Deng
In this study, we proposed a robust and efficient accelerator-silicic acid (SA) to support metal chlorides (MCl x ) as adsorbents for NH 3 adsorption and separation. Their structures and NH 3 adsorption performance were systematically investigated. Results revealed that SA with abundant hydroxyl group could dissociate and immobilize MCl x to realize synergistic M x + –NH 3 coordination and Cl - –NH 3 hydrogen bonding. Meanwhile, the interactions between the MCl x and SA significantly reduced the desorption energy of the adsorbent. The outstanding LiCl-3@SA composite demonstrated remarkable NH 3 adsorption capacity of 17.20 mmol NH 3 /g-adsorbents at 30 °C and 1.0 bar and adsorption enthalpy of −50.23 kJ/mol. Present work provided valuable information on deep understanding of MCl x −porous support interactions and strategy to design efficient composites for NH 3 capture.
研究领域:
化学工程
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
POLYMER
·
2017
·
IF 3.684
Hongyan Yao,Na Zhang,Kunzhi Shen,Ningning Song,Kaixiang Shi,Shiyang Zhu,Yunhe Zhang,Shaowei Guan
A dianhydride monomer 2, 5-bis(3, 4-dicarboxyphenoxy)-4′-phenylethynyl biphenyl (PEPHQDA) containing a chain extendable phenylethynyl pendant group has been successfully synthesized via successive nucleophilic substitution , Sonogashira cross-coupling, hydrolysis and dehydration reactions. A flexible microporous polyimide network has been prepared based on the use of triamine (TAPOB), affording hyperbranched polyimide, followed by the curing of phenylethynyl groups to give network structure. Specifically microporous features such as a well-defined surface morphology , microporous structure and nanometer-sized pore channels have been introduced to the flexible polyimide networks through this two-step pathway. This network exhibit a BET surface area (322 m 2 g −1 ) as well as a comparable CO 2 uptake (1.25 mmol g −1 at 273 K and 1 bar) and enthalpy of adsorption (30.3 kJ mol −1 ) to that of other microporous polyimides derived from rigid tridimensional monomers.
研究领域:
高分子科学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2018
·
IF 5.667
Yansi Cao,Yu Fan,Zhiheng Ma,Zhixuan Cheng,Qun Xiang,Zhiming Duan,Jiaqiang Xu
There is an urgent need for effective and portable gas sensors toward organophosphorus (OP) vapors in the areas of anti-terrorism and pesticides residue monitoring. Herein, we report a series of urea-functionalized SBA-15 (UXs/SBA-15: U1/SBA-15, U2/SBA-15 and U3/SBA-15) prepared by post-grafting methods and their applications in trace-level dimethyl methylphosphonate (DMMP, lab simulate of toxic OP agents) sensing by means of quartz crystal microbalance (QCM) transducers. U3/SBA-15 based QCM sensors exhibited excellent responses and remarkable selectivity toward DMMP vapors. A frequency shift (Δ F ) of −50 Hz was achieved when the DMMP vapors reached 30 ppb. And the limit of detection (LOD) of QCM sensor modified with U3/SBA-15 was found at 12.25 ppb. Moreover, the simulated adsorption enthalpies (Δ H ) of UXs and DMMP molecules were calculated with Gaussian 09 to investigate the sensing mechanism. The results indicated the existence of chemisorption between UXs and DMMP molecules caused by hydrogen-bonding interactions, among which a minimum Δ H (−71.96 kJ mol −1 ) between U3 and DMMP molecule was found, resulting a maximum response to DMMP compared with U1-DMMP (−52.53 kJ mol −1 ) and U2-DMMP (−57.01 kJ mol −1 ). Therefore, the well-defined UXs/SBA-15 lead to a great potential on the detection of OP vapors.
研究领域:
材料科学
·
化学传感
·
分析化学
·
环境监测
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Wei Li,Xiaoxiao Xia,Song Li
Exploring high-performing adsorption-driven heat pumps (AHPs) remains a challenging task owing to the low working capacity, high regeneration temperature, and low energy efficiency of conventional adsorbents. Quick discovery of the novel promising adsorbents could help to improve the coefficient of performance of AHPs for heating (COPH) and cooling (COPC). Herein, we reported an approach to identify the high-performing covalent–organic frameworks (COFs) for heating, cooling, and ice making by high-throughput computational screening based on grand canonical Monte Carlo simulations and, for the first time, machine learning. It was demonstrated that compared with metal–organic frameworks (MOFs), COFs were more suitable adsorbents of AHPs for cooling because of their weak interaction toward ethanol that favors stepwise adsorption. Structure–property relationship analysis revealed that the average enthalpy of adsorption commensurate with the enthalpy of evaporation will benefit the performance of AHPs besides the high working capacity and low step positions of adsorption isotherms. In order to reduce the computational cost of screening, a random forest model was developed to successfully predict the COPC of both COFs and MOFs.
研究领域:
材料科学
·
热能工程
·
计算化学
·
机器学习
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）