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APPLIED ORGANOMETALLIC CHEMISTRY · 2018 ·Vol. 33 ·期 1 ·e4580 · IF 3.581

Effective removal of 2,4,6-trinitrophenol over hexagonal metal–organic framework NH2-MIL-88B(Fe)

Hongxu Guo,Baitong Niu,Xuemin Wu,Yi Zhang,Shaoming Ying

A nanostructured organic–inorganic framework, hexagonal NH 2 -MIL-88B, has been prepared through a facile one-pot reflux reaction and then it was characterized using various techniques. The as-prepared sample with high specific surface area (414 m 2 g −1 ) showed excellent adsorption for 2,4,6-trinitrophenol (TNP) in the liquid phase. Detailed studies of the adsorption kinetics, adsorption mechanism, adsorption isotherm, activation energy and various thermodynamic parameters were conducted. The adsorption mechanism of NH 2 -MIL-88B for TNP may be ascribed to hydrogen bond interaction, and the complexation between ─OH in TNP and unsaturated Fe(III) on the surface of NH 2 -MIL-88B. The maximum adsorption capacity of NH 2 -MIL-88B for TNP based on the Langmuir isotherm was 163.66 mg g −1 . The as-prepared NH 2 -MIL-88B adsorbent seems to be a promising material in practice for TNP removal from aqueous solution.

研究领域: 材料科学 · 环境科学
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Processes · 2024 ·Vol. 12 ·期 9 ·1879 · IF 2.8

Bimetallic Fe, Co-Modified TiO2 Derived from NH2-MIL-125(Ti) as an Efficient Photocatalyst for N2 Fixation

Huiying Yang,Xiangchao Meng

The conversion of nitrogen (N2) and water (H2O) into NH3by photocatalysis under ambient conditions has been considered an environmentally friendly strategy. However, developing effective catalysts for N2fixation is still challenging. Herein, we report a bimetallic JH Fe, Co/TiO2derived from NH2-MIL-125(Ti) by the fast Joule heating (FJH) method for visible–light–driven catalytic N2fixation. It was found that the photocatalytic N2reduction efficiency of bimetallic FC@TiO2-JH was improved, enabling an NH3yield rate of 110.14 µmol g−1h−1without any sacrificial agents. Furthermore, the rate was higher than those of Fe@TiO2-JH and Co@TiO2-JH, suggesting that the synergistic effect between Fe and Co broke the electronic equilibrium and increased the center of its d-band, enhancing electronic feedback to the antibonding π* orbitals of N2while weakening the bonding energy of N≡N. Meanwhile, the rate was about 2.75 times higher than that of FC@TiO2-TF, which was calcined in a tube furnace. It is assumed that FJH might lead to the formation of lattice defects, leading to localized charge deficiency, enhanced carrier separation, and transport. Thus, doping of Fe and Co synergistically interacted with the defects produced from FJH, facilitating the photocatalytic reduction process. As detected, it had a greater ability to separate hole–electron pairs and transferred electrons to adsorbed N2at faster rates. Our work demonstrates a prospective strategy for designing bimetallic catalysts derived from NH2-MIL-125(Ti) for N2fixation.

CAS / MDL: 5593-70-4
研究领域: 材料科学 · 环境科学 · 催化化学
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Nano Research · 2024 · IF 9.5

Amino-modified UiO-66-NH2 reinforced polyurethane based polymer electrolytes for high-voltage solid-state lithium metal batteries

Huang Danru,Wu Lin,Kang Qi,Shen Zhiyong,Huang Qiaosheng,Lin Wenjie,Pei Fei,Huang Yunhui

Solid-state polymer electrolytes (SPEs) are candidate schemes for meeting the safety and energy density needs of advanced lithium-based battery because of their improved mechanical and electrochemical stability compared to traditional liquid electrolytes. However, low ionic conductivity and side reactions occurring in traditional high-voltage lithium metal batteries (LMBs) hinder their practical applications. Here, amino-modified metal-organic frameworks (UiO-66-NH 2 ) with abundant defects as multifunctional fillers in the polyurethane based SPEs achieve the collaborative promotion of the mechanical strength and room temperature ionic conductivity. The surface modified amino groups serve as anchoring points for oxygen atoms of polymer chains, forming a firmly hydrogen-bond interface with polycarbonate-based polyurethane frameworks. The rich interfaces between UiO-66-NH 2 and polymers dramatically decrease the crystallization of polymer chains and reduce ion transport impedance, which markedly boosted the ionic conductivity to 2.1 × 10 −4 S·cm −1 with a high Li + transference numbers of 0.71. As a result, LiFePO 4 ∣SPEs∣Li cells exhibit prominent cyclability for 700 cycles under 0.5 C with 96.5% capacity retention. The LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622)∣SPEs∣Li cells deliver excellent long-term lifespan for 260 cycles with a high capacity retention of 91.9% and high average Coulombic efficiency (98.5%) under ambient conditions. This simple and effective hybrid SPE design strategy sheds a milestone significance light for high-voltage Li-metal batteries.

研究领域: 材料科学 · 电化学 · 能源存储
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Journal of Environmental Chemical Engineering · 2024 · IF 7.4

Facile preparation of UiO-66-NH2-coated mesh membrane with underwater superoleophobicity for high efficiency oil-water separation

Yongbo He,Mengqi Liu,Linzhi Zhai,Hongshuang Li,Peng Song,Xiufang Zhu,Yubin Tang

The metal organic framework (MOF) polycrystalline membranes on stainless steel mesh (SSM) are urgently required for effective oil-water separation, but the affordable preparation still remains a challenge. Herein, we report a series of UiO-66-NH 2 /SSM films, which are developed by a rational ‘seeding-assisted secondary growth’ method. Results depict that the proposed method greatly shortens the synthesis time, and helps to achieve a continuous and uniform modification of UiO-66-NH 2 on SSM, and hence contributes to a superior hydrophilicity and superoleophobicity for UiO-66-NH 2 /SSM with minimum water contact angle of 32° and maximum underwater oil contact angle of 150°, respectively. Specifically, the UiO-66-NH 2 /SSM-600–2 has total permeation fluxes and separation efficiencies of ca. 8.4×10 4 L·m −2 ·h −1 and 100% for the n-hexane-, petroleum ether- and chloroform-water emulsions (1% volume ratio), which exceed numerous polycrystalline membranes reported so far. It also exhibits a great durability with only 0.1% loss of separation efficiency after 8 cycles. Furthermore, outstanding acid-resistivity and salt-tolerance are also presented. Our work supplies a new strategy to construct UiO-66-NH 2 /SSM, and the decent properties confirm a huge potential for practical use in oil-water separation.

CAS / MDL: 10312-55-7 10026-11-6
研究领域: 材料科学 · 环境工程
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Particuology · 2024 · IF 4.1

UiO-66-NH2 nanoparticles supported on layered double hydroxides as an excellent adsorbent for levofloxacin capture

Yan Li,Heng Lin,Qiaolan Yu,Na Ma,Wei Dai

The adsorption performances of individual adsorbent such as UiO-66-NH 2 and MgAl-layered double hydroxides (MgAl-LDH) toward levofloxacin (LVX) is less satisfactory due to the disappointing uptake capacity and adsorption efficiency. Herein, a 3D flower-like composite adsorbent prepared via iterative hydrothermal synthesis method anchoring UiO-66-NH 2 nanoparticles onto the MgAl-LDH surface. Attributed to the synergistic effects of UiO-66-NH 2 , and MgAl-LDH, the MgAl-LDH@UiO-66-NH 2 exhibits an outstanding adsorption performance toward LVX. Typically, the maximum LVX uptake capacity over MgAl-LDH@UiO-66-NH 2 reached 268 mg/g, which was higher than that of the individual adsorption materials UiO-66-NH 2 (41 mg/g), MgAl-LDH (140 mg/g), and some adsorbents reported in previous literature. The rapid adsorption process can reach equilibrium within 20 min, which conformed well to the pseudo-second-order kinetics and the Langmuir isotherm model. Adsorption thermodynamic result also indicated that the adsorption was spontaneous and exothermic, simultaneous coexisting physical and chemical adsorption interactions. Importantly, the MgAl-LDH@UiO-66-NH 2 still maintained excellent adsorption capacity with a slightly decrease after fifth cycle, exhibiting a remarkable reuse and stable performances. This work provides a highly novel strategy to prepare recyclable composite adsorbent for the LVX capture from aqueous solution.

研究领域: 环境科学 · 材料科学
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Inorganic Chemistry Frontiers · 2022 ·Vol. 9 ·期 23 ·6067-6074 · IF 7.779

[C(NH2)3]2S2O8: combining delocalized and localized π-conjugate units to achieve strong optical anisotropy

Man Zhang,Bingbing Zhang,Daqing Yang,Ying Wang

A new birefringent crystal [C(NH2)3]2S2O8 was obtained by combining the π-conjugated [C(NH2)3] cation and the [S2O8] groups with localized O–O π-bonds. Optical measurements show that the UV cutoff wavelength of [C(NH2)3]2S2O8 is 222 nm, and its birefringence is 0.102 at 546 nm. The calculated results show that its large birefringence is attributed to the synergistic effect of the [C(NH2)3] and [S2O8] units, which is the first case among known birefringent crystals. These results provide new insights into the design of superior birefringent materials.

研究领域: 材料科学 · 光学
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

High-Efficient removal of mercury in water by the flexible NH2-MIL-53(Al): Exploiting the gate opening effect

Meipeng Jian,Xiaoqin Yang,Congxin Huang,Chaochun Tang,Xiwang Zhang,Ruiping Liu,Haiyan Li

Flexible metal–organic frameworks (MOFs) with the gate opening feature can optimize the removal efficiency on the adsorption behavior by accommodating to the specific target molecules. In this study, a flexible MOF denoted as NH 2 -MIL-53(Al) was investigated to remove Hg(II) from water, in which the adsorption capacities of large-pore NH 2 -MIL-53(Al) (NH 2 -MIL-53(Al)-LP) for Hg(II) reached 433.20 mg/g, which is about 4 times higher than narrow-pore NH 2 -MIL-53(Al) (112.75 mg/g). Further, the kinetic experiment also revealed that nearly 90 % Hg(II) can be captured within 60 min for NH 2 -MIL-53(Al)-LP. Advanced characterizations and density functional theory calculations demonstrated that the strong coordination of the amino and oxygen centers on NH 2 -MIL-53(Al)-LP to Hg(II). Importantly, molecular dynamic simulation verified the gate opening effect of NH 2 -MIL-53(Al)-LP, as the faster diffusivity of Hg(II) ions in NH 2 -MIL-53(Al)-LP was observed. This work provides another opportunity in designing the pore geometry of porous materials for water remediation.

研究领域: 环境科学 · 材料科学
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Journal of the Taiwan Institute of Chemical Engineers · 2022 · IF 5.477

Defect-rich covalently-crosslinked UiO-66(Zr)-NH2/PVC adsorption ultrafiltration membrane for effective phosphate ions removal from water

Yong Pan,Feng Liu,Yong Zhou,Chen Zhu,Haixia Pang,Baoming Xu

Background Phosphorus in wastewater is a major environmental concern. Very small phosphorus inputs in the environment can cause algal blooms that can deplete the dissolved oxygen and decrease the water quality, leading to eutrophication. Furthermore, some algal blooms produce toxins and bacterial growth that can cause human illness through exposure to contaminated water. Therefore, It is necessary to remove phosphorus before it is discharged to the environment. Methods adsorbent enhanced adsorptive ultrafiltration (UF) has recently emerged as an advanced ion recovery technology with membrane filtration function and adsorption function, and is very effective in removing cationic bisphosphate and anionic phosphate. Significant findings Herein, a novel defect-rich and covalently-crosslinked octanoic acid (OA)-UiO-66(Zr)-NH 2 /PVC adsorption ultrafiltration membrane are designed for removal of phosphate ions in water. The OA-UiO-66-NH 2 /PVC-33 membrane achieved the adsorption capacity (∼30 mgg −1 ) and higher removal efficiency (∼90%). The OA-UiO-66(Zr)-NH 2 /PVC ultrafiltration membrane exhibited a higher water flux of 266.9 L/(m 2 ·h·bar) compared to those of pristine PVC and UiO-66-NH 2 /PVC. Filtration and cyclic stability experiments reveal that OA-UiO-66(Zr)-NH 2 /PVC membrane can maintain a high retention capacity and exhibit excellent regeneration performance after 5 cycles.

研究领域: 环境科学 · 材料科学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2024 · IF 7.7

Construction of greenly biodegradable bacterial cellulose/UiO-66-NH2 composite separators for efficient enhancing performance of lithium-ion battery

Shuaitian Jia,Zan Chen,Yinhui Li,Claudia Li,Cuijia Duan,Kang Hui Lim,Sibudjing Kawi

The disposal of waste lithium batteries , especially waste separators, has always been a problem, incineration and burial will cause environmental pollution, therefore, the development of degradable and high-performance separators has become an important challenge. Herein, UiO-66-NH 2 particles were successfully anchored onto bacterial cellulose (BC) separators by epichlorohydrin (ECH) as a crosslinker, then a BC/UiO-66-NH 2 composite separator was prepared by vacuum filtration. The ammonia groups (−NH 2 ) from UiO-66-NH 2 can form hydrogen bonds with PF 6 − in the electrolyte, promoting lithium-ion transference. Additionally, UiO-66-NH 2 can store the electrolyte and tune the porosity of the separator. The lithium ion migration number (0.62) of the battery assembled with BC/UiO-66-NH 2 composite separator increased by 50 % compared to the battery assembled with commercial PP separator (0.45). The discharge specific capacity of the battery assembled with BC/UIO-66-NH 2 composite separator after 50 charge and discharge cycles is 145.4 mAh/g, which is higher than the average discharge specific capacity of 114.3 mAh/g of the battery assembled with PP separator. When the current density is 2C, the minimum discharge capacity of the battery assembled with BC/UiO-66-NH 2 composite separator is 85.3 mAh/g. The electrochemical performance of the BC/UiO-66-NH 2 composite separator is significantly better than that of the commercial PP separator. In addition, -NH 2 can offer a nitrogen source to facilitate degradation of the BC separators, whereby the BC/UiO-66-NH 2 composite separator could be completely degraded in 15 days.

研究领域: 材料科学 · 环境科学 · 能源科学
✓ 已验证 DOI PubMed 高影响因子
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MICROCHEMICAL JOURNAL · 2024 · IF 4.9

A novel electrochemical ammonia sensor based on Pt NPs@MIL101(Cr)-NH2 for chemical leaks detection at room temperature

Li Gong,Siwei Jin,Renlong Liu,Zuohua Liu,Yijiao Zhang,Li Zhang,Tengda Zhao,Huanbao Fa,Wei Yin

Achieving the real-time, low-cost, portable and accurate NH 3 detection is of great importance in industry owing to the toxicity of NH 3 . In this paper, Pt NPs@MIL-101-NH 2 composites modified screen-printed electrodes (SPEs) were prepared by solvothermal method and ionic liquids [BMIM][BF 4 ] were used as electrolytes. Finally, the prepared Pt NPs@MIL-101-NH 2 /SPEs were combined with a miniature electrochemical workstation to construct a novel electrochemical NH 3 sensor. The experimental results showed that Pt NPs@MIL-101-NH 2 has excellent adsorption capacity for NH 3 , and the sensor has good linearity in the range of 0.7–600 ppm with low limit of detection (0.58 ppm) and fast response time for 10 ppm NH 3 (8.0 s). Furthermore, this sensor also possesses excellent stability, reproducibility, anti-interference and accuracy. The synthesized Pt NPs@MIL-101-NH 2 nanocomposite was proved to be an excellent candidate for constructing high-performance NH 3 sensor for industry.

CAS / MDL: 174501-65-6
研究领域: 材料科学 · 环境监测 · 工业安全
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CRYSTENGCOMM · 2024 ·Vol. 26 ·期 38 ·5431-5439 · IF 2.6

One-step synthesis of pure-phase amino-functionalized zirconium-based capsule ZrC-1-NH2 for photocatalytic degradation of tetracycline

Ting-Ting Xu,De-Sheng Wei,Shuang-Bao Li,Yu-Teng Zhang,Nan Lv

Although the fundamental configuration (tetrahedron-type and capsule-type) of Zr-MOCs is well understood, the synthesis of amino-functionalized Zr-based capsule (denoted as ZrC-1-NH2) based on 2-aminoterephthalic acid remains a considerable challenge. Fortunately, we obtained single crystals under solvothermal conditions and further achieved the rapid synthesis of ZrC-1-NH2 with pure phase and high yield using a microwave-assisted solvothermal method. In addition, ZrC-1-NH2 was utilized as a photocatalyst to perform the degradation of tetracycline (TC) in water. The degradation efficiency of 92.3% was achieved at the optimal conditions, and the main active free radical was determined as ·O2− according to the trapping agent experiment and EPR results. Furthermore, the possible degradation pathway of TC was proposed.

研究领域: 材料科学 · 环境科学 · 化学
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MATERIALS RESEARCH BULLETIN · 2014 · IF 1.968

Designed synthesis of multifunctional Fe3O4@SiO2–NH2@CS–Co(II) towards efficient oxidation of ethylbenzene

Shi Li,Shang-Ru Zhai,Qing-Da An,Ming-Hui Li,Yu Song,Xiao-Wei Song

The preparation of Co(II) supported magnetic heterogeneous catalyst, i.e. Fe 3 O 4 @SiO 2 –NH 2 @CS–Co, and its efficient and selective catalytic properties toward the oxidation of ethylbenzene to acetophenone are presented. The materials were characterized by various physicochemical techniques such as scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, vibrating sample magnetometer, elemental analysis, inductively coupled plasma-atomic emission spectrometer and X-ray photoelectron spectroscopy, etc. The reaction conditions were thoroughly investigated and highly improved catalytic performance (82.5% conversion of ethylbenzene and 80.1% selectivity to acetophenone) was gained under more mild reaction conditions of lower temperature (70   °C), shorter reaction period (60   min) and cheaper and greener oxygen source (H 2 O 2 ). More importantly, it could be reused successively at least 10 times when more than 80% of its catalytic activity maintained.

研究领域: 材料科学 · 催化化学 · 环境化学
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