Advanced Materials Interfaces
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2018
·Vol. 5
·期 8
·1701548
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IF 4.834
Lin Liu,Yang Yan,Zihe Cai,Shengxuan Lin,Xiaobin Hu
Metal–organic frameworks (MOFs) and graphene aerogels (GAs) are both considered as good candidates for high-performance supercapacitors. In this work, a growth-oriented Fe-based MOF synergized with GA composite for supercapacitor is prepared. MIL-88-Fe is in situ grown at (002) lattice plane on the surface of graphene via a one-step solvothermal method. Long periodic hexagonal structure and electrophilicity of MOF provide strong p–π interaction with graphene sheets. By utilizing the abundant interspace of GA, the existence of MOF could affect the electric double-layer characteristics of composites. The MOF/GA composites have the advantages of high capacitive volume, fast charge/discharge rate, and reliable cycling stability. The specific capacitance is as high as 353 F g −1 at the scan rate of 20 A g −1 , and the retention ratio is 74.4% after 10 000 cycles.
研究领域:
材料科学
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能源存储
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JOURNAL OF COORDINATION CHEMISTRY
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2018
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IF 1.703
Yukun Liu,Guimei He,Yiyu Chen,Kang Tian,Feng Cao,Chi Zhang,Wenhua Zhu,Juan Wang
A series of heterometallic metal-organic frameworks (MOFs) employing pyridine-2,6-dicarboxylate and 1,10-phenanthroline as ligands have been synthesized hydrothermally. In isostructural compounds 1–3 [Ln(pydc)3Cu2(phen)4]·I·× H2O (Ln = La (1), Nd (2), Dy (3); x = 6, 5, 5), the metalloligand [Ln(pydc)3] assembles with [Cu(phen)2] units to construct a dodecanuclear cluster via Cu–O bonds and π–π interactions. The clusters are further stacked into three-dimensional supramolecular frameworks with nano-sized cavities. In [La(Hpydc)(pydc)2Zn(phen)3]·3H2O (4), the metalloligand [Ln(Hpydc)(pydc)2] assembles with [Zn(phen)3] units to construct a tetranuclear cluster via electrostatic interaction and π–π interaction. This work reveals that the changes of lanthanide metalloligands and the coordination pattern of 3d transition centers would result in significant variation in the final structures. The thermal, optical, and electrochemical properties have been well investigated.
研究领域:
材料科学
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化学
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COLLOIDS AND SURFACES B-BIOINTERFACES
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2023
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IF 5.8
Bin Cao,Mengyu Li,Ye Zhao,Huimin Zhou,Ting Tang,Mengran Li,Chuan Song,Wei Zhuang
In recent years, two-dimensional nanosheet metal-organic frameworks (2D MOFs) have been widely considered as promising carriers for enzyme immobilization owing to their large surface area, designable and tunable structures, and other properties that enhance enzyme loading and modulate interactions with enzymes. In this study, a series of ultrathin 2D M-TCPP (M = Co, Ni, Zn, Cu) nanosheets were synthesized employing a surfactant-assisted bottom-up approach, and the effect of solvent ratio on the morphology and properties of 2D MOFs was explored. After systematic characterization, Cu-based 2D MOFs with large specific surface areas and excellent water stability was selected as the carrier for the co-immobilization of glucose oxidase (GOx) and horseradish peroxidase (HRP). The effects of adsorption and covalent immobilization strategies on bis-enzyme loading and enzyme activity , as well as their applications in rapid glucose detection, were systematically investigated. The results showed that A-CTGH and C-CTGH owned enzyme loadings of 187.9 and 249.1 mg/g, respectively, and exhibited superior enzymatic activity when exposed to harsh environments compared to free enzymes. In addition, the covalently immobilized biocatalyst based on GOx demonstrated a more sensitive glucose detection performance, including a wide linear range from 5.0 to 16 μM with a detection limit of 0.6 μM.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2023
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IF 8.2
Yujiao Lin,Qingqing Wang,Yuhui Huang,Jian Du,Yi Cheng,Jie Lu,Yehan Tao,Haisong Wang
Water pollution remains a serious problem for aquatic organism and human beings. Developing an efficient material which can simultaneously remove and convert pollutants into low or no harmful compounds is an essential issue. Targeting at this goal, a multifunctional and amphoteric wastewater treatment material of Co-MOF and functionalized cellulose-based composite (CMC/SA/PEI/ZIF-67) was designed and prepared. Carboxymethyl cellulose (CMC) and sodium alginate (SA) were selected as support to construct an interpenetrating network structure and made it crosslinked with polyethyleneimine (PEI) for further in situ growth of ZIF-67 with good dispersion. The material was characterized using an appropriate set of spectroscopic and analytical techniques. When applied in the adsorption of heavy metal oxyanions with no adjustment of pH, the adsorbent could completely decontaminate Cr(VI) at both low and high initial concentrations with good reduction rates. The adsorbent maintained good reusability after five cycles. Meanwhile, the cobalt species of CMC/SA/PEI/ZIF-67 can activate peroxymonosulfate to generate high oxidizing substances (such as SO 4 ˉ · and ·OH ˉ radicals) to degrade cationic rhodamine B dye within 120 min, thus indicating the amphoteric and catalytic nature of our CMC/SA/PEI/ZIF-67 adsorbent. The mechanism of the adsorption and catalytic process was also discussed based with the assistance of different characterization analysis.
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ACS Applied Materials & Interfaces
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2023
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IF 9.5
Si-Yuan Fang,Ji-Lai Gong,Lin Tang,Juan Li,Meng Qin,Huai-Yang Zhou,Liang-Xiu Tang,Jun Zhao
A nanofiltration membrane functionalized with metal–organic frameworks (MOFs) is promising to enhance micropollutant removal and realize wastewater reclamation. However, the current MOF-based nanofiltration membranes still suffer from severe fouling problems with an indefinable mechanism when used for antibiotic wastewater treatment. Hence, we report a nature-inspired MOF-based thin-film nanocomposite (TFN-CU) membrane to explore its rejection and antifouling behavior. Compared with unmodified membranes, the optimal TFN-CU5 membrane (with 5 mg·mL–1 C-UiO-66-NH2) had high water permeance (17.66 ± 1.19 L·m–2·h–1·bar–1), exceptional rejection for norfloxacin (97.92 ± 2.28%) and ofloxacin (95.36 ± 1.03%), and excellent long-term stability for treating synthetic secondary effluent with antibiotic rejection over 90%. Furthermore, it also showed superior antifouling capability (flux recovery up to 95.86 ± 1.28%) in bovine serum albumin (BSA) filtration after fouling cycles. Deriving from the extended Derjaguin–Landau–Verwey–Overbeek (XDLVO) approach, the antifouling mechanism between BSA and the TFN-CU5 membrane was mainly attributed to the inhibited adhesion forces because the growing short-ranged acid–base interaction caused repulsive interfacial interactions. It is further revealed that BSA fouling behavior is slightly retarded under an alkaline environment, while strengthened in the presence of calcium ions and humic acid, as well as high ionic strength. In short, the nature-inspired MOF-based TFN membranes possess exceptional rejection and organic fouling resistance, giving insights into the design of antifouling membranes during antibiotic wastewater reclamation.
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RSC Advances
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2023
·Vol. 13
·期 22
·14980-14990
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IF 3.9
Xiaoyu Hu,Jinchuan Wang,Shangkun Li,Xuanhao Hu,Rongxing Ye,Linsen Zhou,Peilong Li,Changlun Chen
Extensive research has been devoted to developing metal nanoparticle (NP) doped porous materials with large hydrogen storage capacity and high hydrogen release pressure at ambient temperature. The ultra-sound assisted double-solvent approach (DSA) was applied for sample synthesis. In this study, tiny Pd NPs are confined into the pore space of HKUST-1, affording Pd@HKUST-1-DS with minimizing the aggregation of Pd NPs and subsequently the formation of Pd NPs on the external surface of HKUST-1. The experimental data reveal that the obtained Pd NP doped Pd@HKUST-1-DS possessed an outstanding hydrogen storage capacity of 3.68 wt% (and 1.63 wt%) at 77 K and 0.2 MPa H2 (and 298 K and 18 MPa H2), in comparison with pristine HKUST-1 and impregnated Pd/HKUST-1-IM. It is found that the storage capacity variation is not only ascribed to the different textural properties of materials but is also illustrated by the hydrogen spillover induced by different electron transport from Pd to the pores of MOFs (Pd@HKUST-1-DS > Pd/HKUST-1-IM), based on X-ray photoelectron spectroscopy and temperature desorption spectra. Pd@HKUST-1-DS, featuring high specific surface area, uniform Pd NP dispersion and strong interaction of Pd with hydrogen in the confined pore spaces of the support, displays the high hydrogen storage capacity. This work highlights the influence of spillover caused by Pd electron transport on the hydrogen storage capacity of metal NPs/MOFs, which is governed by both physical and chemical adsorption.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Peng Liu,Jianyue Yan,Hao Huang,Wenbo Song
Electrochemical reduction of nitrate to ammonia is an eco-friendly strategy to remove the nitrate pollution in waste effluents. Developing new-type electrocatalysts with high activity for NO 3 RR has attracted worldwide attention. Owing to the numerous active single-metal sites, electric conductivity and ordered in-plane porous structure, conductive metal–organic frameworks (cMOFs) are promising alternative to construct the next-generation NO 3 RR electrocatalysts. In this work, a bimetallic cMOF (Cu x Co y HHTP) is proposed for efficient NO 3 – electroreduction to ammonia and the synergy effect between different types of single-metal sites is also revealed. As the result, the optimal Cu 1 Co 1 HHTP exhibits an outstanding electrocatalytic activity with a high NH 3 yield rate of 299.9 μmol h −1 cm −2 and a large Faradic efficiency of 96.4%. Both theoretical and experimental results reveal that the Co sites can affect the electron structure of Cu sites in Cu 1 Co 1 HHTP slab and decrease the ΔG of potential determining step in NO 3 RR process. Moreover, the Co sites bring a higher selectivity to Cu active sites for reducing *NO 2 to *NO, rather than the desorption of NO 2 – . The bimetallic c-MOFs strategy will innovate the design concept of next-generation catalyst, paving the way to investigate catalytic mechanism of single-metal-atom and open up their application prospects.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Liming Dai,Chenchen Fang,Fanglei Yao,Xiaoyuan Zhang,Xuefeng Xu,Shangling Han,Jingyao Deng,Junwu Zhu,Jingwen Sun
In-situ generated hydroxides and oxyhydroxides have been gradually recognized as the real active sites of metal organic frameworks (MOFs) towards the oxygen evolution reaction (OER). Nevertheless, the fine phase evolution process is still less of concern and elusive. Herein, we successfully construct serious of Ni-MOFs with differing thickness ranging from 1 nm to 270 nm through a competitive coordination strategy. Utilizing the operando resonance spectroscopy, an accurate phase inversion behavior of the Ni-MOFs has been witnessed during the OER, and demonstrated as a thickness-dependent process. Ultrathin architecture is identified as a positive factor to promote the exchange between MOFs ligands and applied electrolyte during the electrochemical test. Hence, after removing most of the internal ligands, 2D MOFs favor to be transformed as β-NiOOH, which is more active than the generated γ-NiOOH in bulky system. The density function theory (DFT) calculation alongside with the in-situ electrochemistry tests further affirm the β/γ-NiOOH transformation behavior. This work offers a new understanding of the electrocatalytic mechanism from the view point of phase evolution in 2D MOFs.
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Applied Sciences-Basel
·
2023
·Vol. 13
·期 5
·3182
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IF 2.7
Chuning Zhang,Huaqiang Chu,Qian Ma,Yanyan Chen,Jianwei Fan
It is important to further enhance the performance of green and efficient non-homogeneous catalysts for advanced oxidation process of Peroxymonosulfate (PMS-AOP) for green treatment of industrial wastewater. In this paper, nitrogen–sulfur co-doped MOFs-derived carbon material (CoSN@C) was prepared by one-pot synthesis followed by carbonization, and its morphological structure was characterized by XRD and SEM. After pyrolysis, the CoSN@C still maintained the dodecahedral morphology and structure of ZIF-67. The synergistic effects of S and N significantly elevated the activation of PMS. The results show that the CoSN@C + PMS system can effectively activate PMS to degrade Rhodamine B (RhB), with a rate constant (1.85 min−1) four times higher than that of the CoN@C + PMS system (0.44 min−1). The optimal catalytic process parameters of material dosage, PMS concentration, temperature, pH, and other parameters were also investigated for the activation of PMS to remove Rhodamine B. The cyclic experiment shows that the CoSN@C has excellent recyclability and the degradation rate of RhB still reached 88.9% after four cycles. Radical capture experiments and EPR tests showed that the CoSN@C + PMS system generated a large amount of SO4·−and ·OH radicals adsorbed on the catalyst surface and a certain amount of singlet oxygen, and the free radical pathway and non-radical pathway worked together to degrade RhB efficiently and rapidly. While non-radical pathway with singlet oxygen as main reactive oxygen species played a key role in the CoN@C + PMS system. This work provides a new idea for the rational design of non-homogeneous catalysts for PMS-AOP system.Keywords:advanced oxidation process;peroxymonosulfate (PMS);non-homogeneous catalyst;MOFs
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BIOCHEMICAL ENGINEERING JOURNAL
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2022
·
IF 4.446
Jiabao Xv,Zeyang Zhang,Saizhao Pang,Jiahui Jia,Zixin Geng,Ruirui Wang,Peikun Li,Muhammad Bilal,Jiandong Cui,Shiru Jia
Immobilized carbonic anhydrase (CA, EC4.2.1.1) for CO 2 capture has been intensively investigated. Unfortunately, the immobilized CA usually shows low CO 2 capture efficiency due to lack of CO 2 capture function for the conventional CA supports. In this study, an acid-resistant metal-organic framework MOF-808 was first modified by co-deposition of PEI (polyethyleneimine) and PDA (polydopamine) (PEI/PDA-MOF-808). Subsequently, the PEI/PDA-MOF-808 with a large number of amino groups was used as the strengthening material of CO 2 capture to immobilize CA (CA@PEI/PDA-MOF-808). The resultant CA@PEI/PDA-MOF-808 showed a considerably improved CO 2 capture capacity compared with free CA and PEI/PDA-MOF-808. The amount of CaCO 3 produced by CA@PEI/PDA-MOF-808 was 11.0-fold and 2.5-fold higher than free CA and PEI/PDA-MOF-808, respectively. After 8 consecutive rounds of CO 2 conversion, the total production of CaCO 3 by CA@PEI/PDA-MOF-808 was 92-fold higher than free CA, reaching 294.0 mg. Furthermore, CA@PEI/PDA-MOF-808 displayed high thermostability , pH stability, storage stability, and reusability compared with free counterpart. After 1 h treatment at pH 3.0, CA@PEI/PDA-MOF-808 preserved 53.6% of its original activity while free CA was almost inactivated. In conclusion, this work provides a promising strategy for enzymatic CO 2 conversion.
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CHEMICAL PHYSICS LETTERS
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2022
·
IF 2.719
Peng Yong,Sheng Wang,Xu Zhang,Haibo Pan,Shuifa Shen
Shape controlled preparation and doping are important means to improve the gas sensitivity of metal oxide semiconductor materials. In this work, pure and Co-doped In 2 O 3 porous hollow hexagonal cylinders were successfully prepared using metal–organic frameworks (MOFs) MIL-68(In) as self-sacrificial template. The size of the MIL-68(In) hexagonal cylinder is uniform, and the In 2 O 3 obtained after pyrolysis better inherits the shape of the MIL-68(In), but becomes hollow, and the cylinder surfaces are porous. The product has a large specific surface area (46.52 m 2 /g), and the doping of Co significantly increases the oxygen vacancy of the material. The Co-doped sample obtained by pyrolysis at 500℃ has excellent gas sensing performances to ethanol gas, its sensitivity to 100 ppm ethanol gas at 210 ℃ is 14.6, response/recovery time is 21 s and 107 s, and the sensing selectivity to ethanol is also good.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Hao Guo,Junye Zhang,Fan Yang,Mingyue Wang,Tingting Zhang,Yanrui Hao,Wu Yang
Metal-organic frameworks (MOFs) have ordered porous structure and intriguing properties for supercapacitors , however, poor conductivity and cycle stability limits their application. To solve these problems, hence, a simple strategy is proposed, by which MOFs are in-situ grown in the porous conductive p-MXene substrate. And then, along with the introduction of CuS, the grown Ni-MOF is derived to Ni 3 S 4 , which is more stable and more electrochemically active. Due to higher contact area, excellent synergistic effect and more exposed active sites, the prepared sandwiched p-MXene@Ni 3 S 4 /CuS nanostructure displays a big specific capacitance (1917 F·g −1 ) and superior cycling performance (91.2%@30000). What’s more, the assembled p-MXene@Ni 3 S 4 /CuS//AC asymmetric device delivers a high energy density of 87.62 Wh·Kg −1 at the power density of 775.02 W·Kg −1 , suggesting that this material provides a brilliant candidate for energy storage.
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