Inorganic Chemistry Frontiers
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2022
·Vol. 9
·期 11
·2725-2733
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IF 7.779
Shouxin Bao,Mingyang Lv,Chen Zhao,Ping She,Zhenyu Lei,Xiaowei Song,Mingjun Jia
Metal–organic frameworks (MOFs) have shown excellent adsorption and degradation performance towards different kinds of dyes but suffer problems in the desorption process, where adsorbates cannot be completely removed and may cause energy waste or secondary pollution by the repeated washing with eluent, as well as their relatively weak stability in aqueous solutions. Thus, it is very attractive to integrate MOFs with active ingredients to prepare MOF-based composites with dye adsorption and degradation ability. The reported fabrication method of MOF@TiO2 usually involves high crystallization temperature or contains acid or base additives, which are unfriendly to MOF structures. Here, we report the design of MOF@TiO2 core–shell nanostructures via a surfactant-free amorphous TiO2 coating followed by water-assisted crystallization at a low temperature (100 °C) below the decomposition temperature of most MOFs. Owing to the mild crystallization conditions, MOF cores are maintained and TiO2 shells crystallize to an active anatase phase. The obtained MOF@TiO2 core–shell nanostructures showed excellent dye removal efficiency and stability for anionic dyes, which can remove 98% dye after five adsorption and photodegradation cycles due to the synergistic effect of MOF cores and TiO2 shells. The design concept and synthetic strategy via the water-assisted crystallization method for labile MOF materials encapsulated in functional TiO2 shells may be used to construct other multifunctional MOF core–shell nanostructures, broadening their applications in diverse fields.
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CARBON
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2022
·
IF 11.307
Xue Zhang,Xuelei Tian,Chang Liu,Jing Qiao,Wei Liu,Jiurong Liu,Zhihui Zeng
Metal-organic frameworks (MOFs) have attracted more and more attentions for preparing electromagnetic wave (EMW) absorption materials because of the porous structure , high specific surface area, and designable configuration. Herein, a series of MOF-74 derived nanocomposites were synthesized by hydrothermal process and subsequent carbonization . The EMW absorption performance and the functions of each component were investigated in depth. Moreover, the inherent EMW absorption mechanisms were comprehensively revealed. Benefiting from the synergistic effect of constituents and microstructure, the MnCo-MOF-74 derived MnO/Co/C nanocomposites delivered a minimum reflection loss value of −68.89 dB at the thickness of 2.64 mm and an effective absorption band of 5.3 GHz at the thickness of 2.3 mm. The high EMW absorption performance was ascribed to the optimized impedance matching and multiple attenuation mechanisms including interfacial and dipole polarization loss, magnetic loss, conductive loss, and multiple scatterings capability. This study shed light on exploring high-efficiency MOF-based EMW absorption materials with rational design of components and structure.
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CERAMICS INTERNATIONAL
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2022
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IF 5.532
Meng Wang,Panpan Zhou,Tong Feng,Zhi Song,Qingguo Ren,Huidong Gu,Xueqing Shi,Qitu Zhang,Lixi Wang
Benefiting from its large specific surface area, abundant defects and functional groups, two-dimensional (2D) laminated Ti 3 C 2 T x MXene is a kind of electromagnetic wave (EMW) absorber with great potential. However, the impedance mismatch caused by the excessive conductivity, inappropriate permittivity and lack of magnetic loss seriously hinders the application of MXene to EMW absorption. Herein, multidimensional hierarchical Ni/TiO 2 /C nanocomposites composed of three-dimensional (3D) hydrangea-like Ni/C microspheres and well-arranged 2D carbon sheets embedded with TiO 2 nanoparticles were successfully fabricated from a Ni-based trimellitic acid framework (Ni-BTC) and Ti 3 C 2 T x MXene via facile in-situ solvothermal assembly and annealing processes. As expected, excellent EMW absorption properties were obtained only by changing the annealing temperature. The minimum reflection loss ( RL min ) value of -45.6 dB and the effective absorption bandwidth (EAB) of 3.40 GHz (14.6–18.0 GHz) with a layer thickness of only 1.5 mm is obtained by annealing the sample at 700 °C. The outstanding ternary multilayer structure and the optimization of magnetoelectric synergy in impedance matching jointly create its remarkable EMW absorption performance. This work is expected to provide a simple and effective method to design MXene-based EMW absorbing materials possessing high absorption intensity, light weight, wide EAB and thin thickness.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Shaokang Jiang,Jian Wang,Zhou Zhu,Shuo Shan,Yilin Mao,Xin Zhang,Xibo Pei,Chao Huang,Qianbing Wan
Bio-MOF-1 is a kind of metal-organic frameworks (MOFs) with bio-derived constitution, self-fabricated by zinc-adeninate secondary building units (SBUs) and may theoretically be endowed with biocompatible behaviors. Its biological applications currently contain several small molecule drugs delivery and in vitro mineralization, yet the related evidence on its biosafety and biocompatibility is still in great need. With the aid of self-modified protocol to synthesize micro/nanoscale bio-MOF-1 (m/n-bio-MOF-1), this study aimed to implement a systematic evaluation based on a series of tests from different dimensions including cell proliferation , oxidative stress, apoptosis and animal experiment, etc. These in vitro & in vivo biosafety and biocompatibility tests are to provide fresh evidence and advice for further applications. The outcomes indicated a concentration-dependent trend that 50 and 20 μg/mL groups proved biofriendly, with n-bio-MOF-1 surpassing m-bio-MOF-1. In conclusion, this work provided systematic evidence for the biosafety of m/n-bio-MOF-1, paved the way for their further exploration, and appealed more emphasis on MOFs toxicity.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Minmin Gou,Ruili Guo,Hengheng Cao,Weifang Zhu,Fu Liu,Zhong Wei
Mixed matrix membranes (MMMs) for separating CO 2 /CH 4 mixture were prepared through incorporating Cu@Al(bpydc) into a Pebax polymer in which Cu@Al(bpydc) synthesized through a competitive coordination method achieved a controllable micro/mesopores structure and abundant functional sites for CO 2 . The hierarchical pores of Cu@Al(bpydc) provided multidimensional diffusion channels in the Pebax matrix, which increased the diffusion of CO 2 . In addition, the abundant chemical groups, such as the polar group COO – and nitrogen Lewis basic groups, created a microenvironment with multiple CO 2 affinity sites in the membrane, increasing the selectivity of CO 2 . A MMM loaded with 5 wt% Cu@Al(bpydc) exhibited excellent CO 2 separating property under wet mixed-gas test conditions. In particular, the CO 2 permeability and selectivity of the MMMs were increased by 92.90% and 27.10% respectively, compared with those of pure Pebax, showing exceptional potential for the separation and capture of CO 2 from biological natural gas.
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CHEMOSPHERE
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2022
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IF 8.943
Tao Zhang,Pan Wu,Gary Owens,Zuliang Chen
Since ofloxacin (OFX) is one of many common antibiotics, which effluxes into aquatic environment in relatively high concentration, it has become of significant environmental concern due to the potential for increased antibiotic resistance. In this study, an innovative functional Fe/Ni@ZIF-8 composite was successfully used for the Fenton-like oxidation of OFX, with a OFX removal efficiency >98% under optimal conditions. FTIR analysis confirmed that OFX removal occurred via adsorption to Fe/Ni@ZIF-8 by a combination of π-π bond intercalation and electrostatic interaction, while XPS revealed that the Fe/Ni NPs in Fe/Ni@ZIF-8 were also involved in oxidation. Furthermore, LC-MS analysis identified the presence of several OFX degradation products post exposure, which indicted that Fe/Ni NPs in Fe/Ni@ZIF-8 reacted with H 2 O 2 to form •OH, leading to Fenton-like oxidation of OFX. Thus overall, OFX removal by Fe/Ni@ZIF-8 involved both adsorption to ZIF-8 and Fenton-like oxidation by Fe/Ni NPs. A synergistic mechanism for OFX removal by Fe/Ni@ZIF-8 was thus proposed. The removal efficiency of the synthesized catalysts remained high (above 65%) even after a 5th reuse cycle, which reflected the high stability of Fe/Ni@ZIF-8. Overall, this study demonstrated that Fe/Ni@ZIF-8 had significant potential for the removal of OFX from wastewaters with a removal efficiency >90%.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Qiulin Li,Ke Zhang,Xiang Li,Jiaqi He,Yongbing Lou,Jinxi Chen
The creation of considerably effective electrocatalysts to reduce overpotentials is essential for speeding up the sluggish oxygen evolution reaction (OER) processes, which is imperatively required for the practical exploitation of electrochemical water-splitting. Herein, we prepared a unique composite structure, uniformly spherical Ni-MOF decorated with NiMoO 4 nanorods on Ni foam (NF), and assessed its performance toward oxygen evolution reaction. The synergistic effect between NiMoO 4 and Ni-MOF remarkably promoted the OER intrinsic activity. Moreover, introducing NiMoO 4 endowed the composite structure with enhanced electrical conductivity and exposed more active sites. The NiMoO 4 /Ni-MOF/NF electrode exhibited exceptional electrocatalytic activity in 1.0 M KOH aqueous solution, with a low overpotential of 218 mV to drive the current density of 10 mA cm −2 and a low Tafel slope (67.75 mV dec −1 ), surpassing the benchmark RuO 2 . The presented strategy opens a promising candidate for preparing novel non-precious metal OER electrocatalysts derived from MOF materials for sustainable energy applications.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Shaoxia Yang,Qing Wang,Huazhang Zhao,Daoqing Liu
The intrinsic properties of metal-based adsorbents originate from multiples factors such as surface functional groups, electronic and dimensional structures. However, the synthetic strategies are limited to top-down methods, which inhibited the improvement of adsorbent performance. Herein, Fe-Ce bimetal oxide composites are prepared by a bottom-up modified MOF template method. MOF template-directed nano rod-like morphology can expose more active sites and facilitate phosphate access to active sites. The introduction of citric acid effectively increased the amount of surface –OH groups and greatly improved the phosphate adsorption capacity. Furthermore, the Fe dopant enables the high Ce(III) fraction and generate magnetic property for Fe-Ce bimetal oxide composites, which are capable of enhancing the intrinsic phosphate adsorption performance. The results show that the optimized Fe-Ce bimetal adsorbent showed remarkably high phosphate adsorption capacity, achieving a maximum phosphate adsorption capacity of 357 mg g −1 by Langmuir model. High adsorption capacity and high magnetic separation efficiency characteristics make this adsorbent a promising material for phosphate treatment. The above results further prove the effectiveness of the bottom-up strategy in the design process of environmental functional materials.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Naseeb Ullah,Aymeric Ramiere,Waseem Raza,Pengfei Ye,Wei Liu,Xingke Cai,Zhengchun Peng,Ki-Hyun Kim
Chemical fixation of CO 2 with epoxides is an effective option to achieve sustainable synthesis of cyclic organic carbonates. Although metal–organic frameworks (MOFs) are promising catalysts for this reaction, their low stability in aqueous solutions makes this application infeasible. In an effort to overcome this limitation, cobalt-based metal–organic framework (Co(II)MOF) nanoribbons have been prepared by coordinating the Co(II) ions with a new ligand (C 16 H 12 N 4 O 4 ) full of oxygen and nitrogen moieties. Strong chemical interactions occur between the adsorbed CO 2 and oxygen/nitrogen atoms in this porous MOF structure. Co(II)-MOF nanoribbons with tetra- n -butylammonium bromide acted as cocatalysts with ∼97% yield of cyclic carbonate (reaction kinetic rate of 14.7 × 10 6 µmol g -1 h −1 ) upon the cycloaddition of epichlorohydrin (ECH) to CO 2 (>99% reaction selectivity under solvent-free reaction condition at 80 °C, 3 h and 1 MPa CO 2 pressure). This work may open a new avenue for chemical fixation of CO 2 by rational design of the components and morphology of MOF-based catalysts.
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MICROCHIMICA ACTA
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2022
·Vol. 189
·期 8
·1-11
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IF 6.408
Hu Xue,Tang Jianshe,Shen Yizhong
A tunable interaction between Fe-MOFs (MIL-53(Fe) and kojic acid (KA)-functional copper nanoclusters (Cu NCs) has been studied. When introducing MIL-53(Fe), the Fe–O bonds can be formed between the KA on the surface of Cu NCs and MIL-53(Fe), which will induce the electron transfer from Cu NCs to MIL-53(Fe) and fluorescence quenching of Cu NCs. By introducing S 2− it occupies the Fe-site of MIL-53(Fe) and impede the interaction between Cu NCs and MIL-53(Fe), rendering a “turn-on” fluorescence signal. Thus, the KA-Cu NC/MIL-53(Fe) pair is designed as fluorescence sensing for S 2− , which displays a low detection limit of 18.6 nM and a wide linear detection range from 0.05 to 5 µM by fitting the fluorescence intensity at maximum wavelength of 500 nm with excitation at 400 nm. It was also applied to monitor S 2− in water samples and food additives with satisfactory results, demonstrating the practicability and reliability of the sensing strategy based on the tuable MOF-Cu NC interactions. Graphical abstract
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LUMINESCENCE
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2022
·Vol. 37
·期 10
·1793-1799
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IF 2.613
Piaotong Liu,Rusi Hao,Wenliang Sun,Ziyi Lin,Tianfeng Jing
The increasing degradation of ecosystems due to heavy metal residues has led to environment and food contamination, prompting the development of convenient platforms for monitoring heavy metals. Here, a new dual-emission fluorescent sensor CuNCs@Tb@UiO-66-(COOH) 2 for the detection of copper ions (Cu 2+ ) has been synthesized using one-pot encapsulation of Tb(III) and glutathione-stabilized copper nanoclusters (CuNCs) into metal–organic frameworks (MOFs) UiO-66-(COOH) 2 . In this ratiometric sensor, the fluorescence intensity of Tb 3+ decreased significantly upon the addition of Cu 2+ , whereas that of CuNCs showed good stability, together with an apparent colour change. Therefore, ratiometric fluorescence detection of Cu 2+ can be accomplished by measuring the ratio of the fluorescence intensity at the 450 nm (F 450 ) wavelength of CuNCs to the 548 nm (F 548 ) emission of Tb 3+ in the fluorescence spectra of the CuNCs@Tb@UiO-66-(COOH) 2 suspension. Moreover, the obtained fluorescent probe showed good results in the detection of actual samples. This work can provide the basis of method for the exploration of ratiometric fluorescence and visual sensors of trace pollutants analysis in complicated samples.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Yu Tao,Baogang Yang,Fengyan Wang,Yanghao Yan,Xianyong Hong,Haihua Xu,Mingzhu Xia,Fengyun Wang
In this work, a facile and green method is applied to synthesize hydrophilic MOF-808(Zr) and modulate its defect content and particle size using different amounts of iron nitrate (denoted as F) to obtain serial XF-MOF-808 (“X” implied the dosage of used F). The development of additional adsorption sites and the fine-tune of pore and particle size based on MOF-808 significantly improved phosphate adsorption performance. In particular, the 0.5F-MOF-808 shows excellent adsorption capacity (305.5 mg/g) and rapid diffusion rate (37.51 mg/g·min 0.5 ) for phosphate at 298 K and initial pH = 6.5, outperforming pristine MOF-808 and most previously reported adsorbents. 0.5F-MOF-808 possesses a wide pH tolerance, outstanding reusability and excellent selectivity for phosphate adsorption from simulated wastewater, verified in environmental implication and regeneration experiments. Phosphate loaded on the adsorbent can be converted to struvite for agricultural fertilizer via a simple crystallization process. Compared to MOF-808, the exceptional sorption performance of 0.5F-MOF-808 is supported by decreased internal diffusion limitation, enlarged pore size and the development of new adsorption sites, which can be proved by advanced characterizations and batch adsorption experiments. This work presents a promising modification strategy of MOF materials for phosphate adsorption and recovery.
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