Science China-Materials
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2021
·Vol. 64
·期 8
·2008-2016
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IF 8.273
Wen Xin,Lin Chensheng,Luo Min,Fan Huixin,Chen Kaichuang,Ye Ning
[PO 4 ] 3− possesses small microscopic second-order susceptibility and polarizability anisotropy, which inherently result in weak second-harmonic generation (SHG) and small birefringence. Herein, a new noncentrosymmetric phosphate, [C(NH 2 ) 3 ] 3 PO 4 ·2H 2 O, was successfully designed and synthesized by a solution evaporation method. [C(NH 2 ) 3 ] 3 PO 4 ·2H 2 O without metal ions is composed of planar conjugated guanidine cations and PO 4 tetrahedrons, which are connected by hydrogen bonds, forming a three-dimensional network. Physical property measurements indicate that the title compound displays an SHG response of 1.5 × KH 2 PO 4 (KDP) and a larger birefringence (0.055@546.1 nm) compared with most reported ultraviolet nonlinear optical phosphates. Furthermore, first-principles calculations reveal that the π-conjugated planar [C(NH 2 ) 3 ] + cations and [PO 4 ] 3− groups are responsible for its excellent linear and NLO properties.
研究领域:
材料科学
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光学工程
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无机化学
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晶体工程
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非线性光学
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ELECTROCHIMICA ACTA
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2026
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IF 5.6
Yuan Jin,Yanhong Zhang,Fuzhi Li,Guangli Li
To address microfibrillated cellulose (MFC) separator shortcomings in lithium-ion flux homogenization and dendrite growth due to uneven ion distribution, this study developed a UiO-66-MFC composite separator with 20-30% loading. The hierarchical pores (0.8-1.2 nm micropores and 2-50 nm mesopores) enable selective Li + screening and rapid transport, while MFC's hydroxyl groups form hydrogen bonds with amino groups of UiO-66-NH 2 , enhancing mechanical strength to 16 MPa at a 20% loading. Density functional theory (DFT) calculations further reveal a strong interaction between -NH 2 and PF 6 - , with a binding energy reaching -8.622 keV. This interaction effectively restricts the migration of PF 6 - , promotes the desolvation process of lithium salts, accelerates Li⁺ transport, and fosters more uniform lithium deposition behavior. The electrochemical test results indicate that the 20% UiO-66-NH 2 /MFC separator demonstrates the most favorable overall performance. After cycling for 1000 h at a current density of 1 mA cm -2 , the overpotential of the Li/Li symmetrical battery remains stable at ± 0.10 V, suggesting effective inhibition of lithium dendrite growth. When paired with the LiFePO 4 cathode, the battery exhibits a capacity retention rate exceeding 90% after 100 cycles, while the coulombic efficiency approaches 100%. This study significantly improves the ion conduction and interface stability of the separator by optimizing the MOF ratio, thereby offering a novel strategy for the material design of high-safety and long-life lithium-ion batteries. This MOF-incorporated MFC strategy significantly enhances separator ion conduction and stability, offering a novel approach for safe, long-life lithium-ion batteries.
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JOURNAL OF CHROMATOGRAPHY A
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2026
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IF 4
Xueyun Wei,Lanrui Yang,Zhuomin Zhang,Gongke Li
Trace disinfection by-products (DBPs) in aquatic products may have serious impact on human health via direct or indirect consumption. However, the accurate and sensitive quantification of trace chlorophenol DBPs in complex aquatic products still remains a great challenge. In this work, the defective MIL-101(Fe)-NH 2 enrichment medium was prepared for developing a selective membrane solid phase extraction (M-SPE) technology for quantifying trace chlorophenol DBPs in fish, coupled with high performance liquid chromatography-ultraviolet-visible spectroscopy (HPLC-UV). The established analytical method showed good selectivity, sensitivity and accuracy, achieving the limits of detection from 0.03 to 0.15 ng/mL and the recovery from 80.0% to 117%, achieving sensitivity comparable to that of HPLC-mass spectrometry (MS)-based methods. The validated method was successfully applied to quantify chlorophenol DBPs in grass carp and crucian carp, offering a selective and sensitive alternative for monitoring chlorophenol DBPs in fish, with practical advantages for routine analysis via compatibility with widely available HPLC-UV.
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ChemNanoMat
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2023
·Vol. 9
·期 5
·e202300051
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IF 3.8
Qiankun Xu,Yaru Li,Wen Ji,Jun Mei,Xianbiao Wang
Graphical TiO 2 hollow sphere/UiO-66-NH 2 heterostructures were successfully synthesized by an adsorption-induced in-situ solvothermal growth strategy. The integration of TiO 2 and UiO-66-NH 2 could construct a type-II heterojunction to broaden the absorption range of light and suppress the recombination of photoproduced electrons and holes, thus boosting the photoreduction activity toward Cr(VI) of TiO 2 /UiO-66-NH 2 . Water contamination caused by highly toxic Cr(VI) should be resolved imminently with a more efficient photocatalytic approach. The interaction between photocatalyst heterostructure is critical for charge separation which largely affects the photocatalytic efficiency. Herein, TiO 2 hollow sphere/UiO-66-NH 2 (TiO 2 /UiO-66-NH 2 ) heterostructures were successfully synthesized by an adsorption-induced in-situ solvothermal growth strategy. The UiO-66-NH 2 particles were well dispersed on TiO 2 hollow spheres by solvothermal treatment of Zr 4+ adsorbed TiO 2 hollow spheres with NH 2 -BDC ligand. The photocatalytic activities of TiO 2 /UiO-66-NH 2 heterostructures were investigated by reduction of Cr(VI) with visible light irradiation. With the introduction of UiO-66-NH 2 , the reduction efficiency toward Cr(VI) by TiO 2 /UiO-66-NH 2 heterostructures reached 89% after 180 min of irradiation, which is much higher than those of TiO 2 hollow spheres (10%) and UiO-66-NH 2 crystals (29%). Moreover, the TiO 2 /UiO-66-NH 2 heterostructures display good regeneration ability and can still maintain 70% of Cr(VI) removal ability after four cycles. The integration of TiO 2 and UiO-66-NH 2 could construct a type-II heterojunction to broaden the absorption range of light and suppress the recombination of photoproduced electrons and holes. As a result, such unique composite structure significantly enhance the photocatalytic performance towards Cr(VI) reduction. This work not only inspires a new approach for in-situ solvothermal synthesis of semiconductor@MOFs composites, but provides a novel photocatalyst for highly efficient removal of Cr(VI) from wastewater.
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ACS Applied Materials & Interfaces
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2023
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IF 9.5
Dianfa Zhao,Jie Liu,Yunshan Zhou,Lijuan Zhang,Yuxu Zhong,Yang Yang,Baoquan Zhao,Mengru Yang,Yong’an Wang
It is very important to establish a sustained-release pralidoxime chloride (2-PAM) drug system with brain targeting function for the treatment of neurotoxicant poisoning. Herein, Vitamin B1 (VB1), also known as thiamine, which can specifically bind to the thiamine transporter on the surface of the blood–brain barrier, was incorporated onto the surface of MIL-101-NH2(Fe) nanoparticles with a size of ∼100 nm. Pralidoxime chloride was further loaded within the interior of the above resulted composite by soaking, and a resulting composite drug (denoted as 2-PAM@VB1-MIL-101-NH2(Fe)) with a loading capacity of 14.8% (wt) was obtained. The results showed that the drug release rate of the composite drug was increased in PBS solution with the increase of pH (2–7.4) and a maximum drug release rate of 77.5% at pH 4. Experiments on the treatment of poisoning by gavage with the nerve agent sarin in mice combined with atropine revealed that sustained release of 2-PAM from the composite drug was achieved for more than 72 h. Sustained and stable reactivation of poisoned acetylcholinesterase (AChE) was observed with an enzyme reactivation rate of 42.7% in the ocular blood samples at 72 h. By using both zebrafish brain and mouse brain as models, we found that the composite drug could effectively cross the blood–brain barrier and restore the AChE activity in the brain of poisoned mice. The composite drug is expected to be a stable therapeutic drug with brain targeting and prolonged drug release properties for nerve agent intoxication in the middle and late stages of treatment.
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TALANTA
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2023
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IF 6.1
Qingying Wang,Lianfang Chen,Xiaoyan Cui,Jie Zhang,Yaohui Wang,Xiupei Yang
Herein, a covalent organic framework (COF) was grown on a magnetic metal-organic framework (MOF) by a solvothermal method for the efficient extraction of bisphenols (BPs). The magnetic solid-phase extraction (MSPE) of four bisphenols (bisphenol A, bisphenol B , bisphenol AF and bisphenol C) was carried out without adjusting the pH and salt concentration. When 30 mg Fe 3 O 4 @NH 2 -MIL-88(Fe)@TpPa was used to adsorb for 25 min, 6 mL methanol was used to elute for 20 min, and the extract was detected by high-performance liquid chromatography (HPLC). The proposed method has a low detection limit of 0.011–0.036 ng mL −1 , a wide linear range of 0.05–100 ng mL −1 , and a correlation coefficient (R 2 ) of 0.9980–0.9998. The intra-day and inter-day precisions are 0.74–2.54% and 1.68–3.72%, respectively. Bisphenol A was determined by applying the proposed method to the determination of actual milk samples. The standard addition experiment showed that the relative recovery of the four bisphenols was 85.70–119.7%. Pseudosecond-order, first-order, Langmuir and Freundlich models were applied to explore the adsorption characteristics of Fe 3 O 4 @NH 2 -MIL-88(Fe)@TpPa. In general, the established Fe 3 O 4 @NH 2 -MIL-88(Fe)@TpPa-MSPE-HPLC-UV method exhibits attractive sensitivity, simple manipulation, and excellent reusability, and it has excellent prospects for the detection of trace BPs in complex milk matrices.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2023
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IF 6.1
Kunpeng Liu,Nan Wang,Jianhua Li,Fanglin Du,Baorong Hou,Ruiyong Zhang
Electrochemical two-electron water oxidation reaction (2e − WOR) to produce H 2 O 2 has been widely concerned. However, four-electron competition reaction causes the large overpotential and low production rates of 2e − WOR, which restrict its’ development and application. Herein, we prepared N-TiO 2 derived from NH 2 -MIL-125 by the hydrothermal combined with calcination method. We found that N-TiO 2 as photoanode exhibited the well properties of photoelectrocatalysis water oxidation, which gave an overpotential of 630 mV at 1 mA cm −2 . The overpotentials of N-TiO 2 was approximately 130 mV (at 1 mA cm −2 ) lower than NH 2 -MIL-125, and even lower than the previous reported TiO 2 , which may attribute to the increased oxygen vacancy with the calcination process and N doping. In addition, we investigated the degradation performance of the prepared catalysts to degrade methylene blue by photoelctrocatalysis on-site the preparation of H 2 O 2 . It was shown that N-TiO 2 performed high degradation efficiency (∼91%) and excellent stability. The possible mechanism was speculated due to the increased oxygen vacancy and N doping. This work provides a new idea for photoelectrocatalysis water oxidation materials and points out a new way for on-site H 2 O 2 production for direct use.
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Journal of Materials Chemistry A
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2022
·Vol. 10
·期 44
·23666-23674
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IF 14.511
Mingna Chu,Yang Li,Ximing Chen,Guangyao Hou,Yan Zhou,Hongjun Kang,Wei Qin,Xiaohong Wu
Solar-driven carbon dioxide (CO2) reduction into valuable chemicals or feedstock is of great significance for the sustainable development of the environment and energy. Herein, we presented a photo-induced reduction method to synthesize catalysts by anchoring Zn single atoms (SAs) on UiO-66-NH2. Impressively, UiO-66-NH2-0.7Zn SAs had excellent performance in converting CO2 to carbon monoxide (CO), which was about a 5-fold improvement compared to pristine UiO-66-NH2 without a photosensitizer or hole sacrificial agent under UV-vis light. The remarkable photocatalytic CO2 reduction performance was attributed to the built-in electric field construction by anchoring highly dispersed Zn SAs on UiO-66-NH2. The built-in electric field could effectively promote the separation of photogenerated charges and activate CO2. Density functional theory (DFT) calculations revealed that low-coordination Zn–N2 sites could dramatically enhance the formation of COOH*, which was the rate-limiting step for CO generation. This study created a new opportunity to develop high-efficiency photocatalysts containing single-atom sites for photocatalytic CO2 reduction.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2022
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IF 3.898
Xueting Liu,Chunhui Hu,Jingjing Wu,Peng Cui,Fengyu Wei
In this study, a series of metal–organic frameworks (MOFs) NH 2 -UiO-66- x HAc catalysts were synthesized by solvothermal method using acetic acid (HAc) as a modulator, and were applied to the cycloaddition of CO 2 and epichlorohydrin (EPIC) under ambient pressure. Influences of the modulation by HAc on morphologies and structures of the MOFs are demonstrated via PXRD, FESEM, FTIR, N 2 adsorption–desorption, XPS and 1 H NMR characterizations. The results show that the MOFs containing mesoporous pores can be prepared by adjusting the concentration of HAc. By optimizing the amount of HAc added, the specific surface area of NH 2 -UiO-66-8HAc is as high as 879.17 m 2 ·g −1 , which is 28.3% higher than that of the original MOFs. And the evaluation of catalytic performance showed that HAc modulation enhanced the activity of NH 2 -UiO-66- x HAc under mild conditions. The exposure of Lewis acid sites, increased specific surface area and porosity via the modulation of HAc defective ligand can be supposed the key factors to determine the enhanced catalytic activities. In addition, considering the influence of gas concentration on the reaction, the concept of TOP (Turnover of Pressure, defined as the mass of conversions of a unit mass catalyst under unit pressure and unit time) was first proposed in this article.
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JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Zhihong Lin,Ziyi Yuan,Kaifang Wang,Xuezhong He
Novel mixed matrix membranes (MMMs) with superior CO 2 /N 2 separation properties are of great importance for post-combustion CO 2 capture from flue gas . Metal-organic frameworks (MOFs) as one of the most attractive porous fillers for MMMs fabrication, are considered to provide a solid molecular sieving mechanism for enhancing CO 2 /N 2 selectivity. However, it causes the reduction in gas permeability and limits its further industrialization. Herein, we proposed a new strategy for filler functionalization by doping silver ions (Ag + ) into UiO-66-NH 2 nanoparticles through the double-solvent method and used for the preparation of advanced MMMs. The double-solvent method is benefits for the enrichment of Ag + in the hydrophilic pores of UiO-66-NH 2 . As a result, the prepared novel MMMs called Ag + @UiO@PIM-1 with the polymers of intrinsic microporosity (PIMs) as polymer matrix , show outstanding CO 2 permeability. According to the mixed gases (CO 2 /N 2 = 10:90) permeation experiments under 25 °C and 2 bar, the membrane with 30%Ag + @10%UiO loading achieves more than 65% increase in CO 2 /N 2 selectivity (∼30) and 120% in CO 2 permeability (>15,000 Barrer) compared to the pristine PIM-1 membrane. By optimizing the Ag + doping amount and Ag + @UiO loading content, the separation performance exceeds the 2019 CO 2 /N 2 upper bound. To figure out the separation mechanism, the pore texture properties and CO 2 affinity of the functional filler (Ag + @UiO) together with the membrane structure were characterized by XPS , PXRD , SEM, gas sorption , etc. The synergistic mechanisms by combing CO 2 facilitated transport and molecular sieving from pore regulation were identified to enable advanced CO 2 /N 2 membrane separation .
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COLLOIDS AND SURFACES B-BIOINTERFACES
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2023
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IF 5.8
Ke Cai,Wei Pi,Jiangyang Qin,Chenxi Peng,Dandan Wang,Yingying Gu,Yong Mei
In this study, an electrochemical immunosensor was constructed to detect the cytokeratin 19 fragment antigen 21-1 (CYFRA 21-1) in human serum. CYFRA 21-1 is the most sensitive tumor marker of non-small cell lung cancer (NSCLC), its content in normal human serum should be less than 3.3 ng/mL. When lung cancer cells dissolve or die, a myriad of CYFRA 21-1 is released into a tumor patient’s blood circulation , and its serum content elevates strikingly. Consequently, detecting CYFRA 21-1 by an electrochemical biosensor is expected to provide a new method for the early detection and prevention of lung cancer. In this study, a composite of UiO-66-NH 2 and carboxylated multi-walled carbon nanotubes (CMWCNTs) was used as the substrate material of a sensor; the resulting sensor had a large specific surface area and strong electrical conductivity . Moreover, gold nanoparticles (AuNPs) were used to bind to antibodies through an Au-S bonds. Also, a supersensitive detection of CYFRA 21-1 was achieved through the specific bindings of antigens and antibodies. Under optimal detection conditions, the change of current signal intensity of the immunosensor was proportional to the logarithm of CYFRA 21-1 concentration and had a linear relation in the range of 0.005–400 ng/mL, while the detection limit was 1.15 pg/mL (S/N = 3). The proposed immunosensor had high precision, stability, and selectivity . More importantly, the sensor was been successfully applied to detect CYFRA 21-1 in human serum with high recovery, providing a new method for early screening and dynamic monitoring of lung cancer.
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ENVIRONMENTAL RESEARCH
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2023
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IF 8.3
Chunyan Hu,Jinke He,Jianjun Liang,Tao Lin,Qiuliang Liu
A novel photo-Fenton catalyst α-Fe 2 O 3 @g-C 3 N 4 @NH 2 -MIL-101(Fe) (FGN) with dual Z-scheme heterojunction was successfully prepared by hydrothermal method to degrade tetracycline (TC). The preparation conditions were optimized by orthogonal test, and the successful synthesis was confirmed by characterization analyses. The prepared FGN showed better light absorption performance, higher photoelectrons-holes separation efficiency, lower photoelectrons transfer resistance, and higher specific surface area and pore capacity compared with α-Fe 2 O 3 @g-C 3 N 4 and α-Fe 2 O 3 . The effects of experimental conditions on the catalytic degradation of TC were investigated. The degradation rate of 10 mg/L TC could reach 98.33% within 2 h when the dosage of FGN was 200 mg/L, and the degradation rate could remain 92.27% after 5 times of reuse. Furthermore, the XRD spectra and XPS spectra of FGN before and after reuse were compared to explore the structural stability and catalytic active sites of FGN, respectively. According to the identification of oxidation intermediates, three degradation pathways of TC were proposed. Through H 2 O 2 consumption experiment, radical-scavenging experiments, EPR results, the mechanism of the dual Z-scheme heterojunction was proved. The improved performance of FGN was attributed to the dual Z-Scheme heterojunction effectively promoting the separation of photogenerated electrons from the holes and accelerating the electrons transfer , and the increase of the specific surface area.
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