ANALYTICA CHIMICA ACTA
·
2023
·
IF 6.2
Xiang Li,Xiaofeng Lu,Xiaojing Liang,Zhimin Yang,Shuai Wang,Yong Guo
Background Large accumulations of pesticide residues in the environment eventually enter the human body with food. Based on magnetic solid-phase extraction (MSPE) technology , it is possible to achieve efficient extraction of trace pesticide residues in foodstuffs, and the construction of MSPE adsorbents with excellent magnetic properties and many active sites is still one of the main research topics. Based on this, we developed a new strategy for the preparation of "MOF-on-MOF" composites, which were carbonized and used as adsorbents for the extraction of pesticide residues in cereals. Results A novel corn cob core-shell composite Fe 2 O 3 @C@ZIF-8 was created by embedding ZIF-8 onto the surface of Fe 2 O 3 @C derived from MIL-88A(Fe), and used for the extraction of benzoylurea insecticides(BUs) from cereals. The adsorption behaviour between Fe 2 O 3 @C@ZIF-8 and BUs was investigated by static and kinetic experiments and the adsorption mechanism was elaborated. For the trace analysis of BUs, a magnetic solid-phase extraction combined with high performance liquid chromatography-ultraviolet detector (HPLC-UV) approach was also developed. Under the optimized experimental conditions, the limits of detection and quantification were 0.015–0.03 μg L −1 and 0.05–0.1 μg L −1 , and the relative standard deviations for the intra-day and inter-day ranges were 1.82%–2.13 % and 3.85%–4.59 %, respectively. The spiked recoveries of the four cereals ranged from 82.72% to 104.45 %. After 10 cycles of use of Fe 2 O 3 @C@ZIF-8, the recoveries of BUs ranged from 77.90% to 96.74 %. Significance The analytical method based on Fe 2 O 3 @C@ZIF-8 as adsorbent has a low limit of detection, a wide linear range and is highly applicable to the analysis of real samples. In addition, the strategy developed in this study for the preparation of thermoplastic polymer-assisted "MOF-on-MOF" composites has promising applications.
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Journal of Environmental Sciences
·
2024
·
IF 5.9
Qiang Li,Qi Zhou,Yanling Wu,Yingxue Shi,Yingqi Liu,Hao Deng,Siwei Chen,Zhiheng Li,Erpeng Wang,Huayue Zhu,Qi Wang
Accelerating the separation of carriers in the heterojunction plays vital role in the photoelectrocatalytic (PEC) process, yet it remains a challenging undertaking. Herein, a MOF-on-MOF based dual S-scheme heterojunction (BiVO 4 /NH 2 -MIL-125(Ti)/NH 2 -MIL-53(Fe), denoted as BVO/NM125/NM53) was rationally designed and prepared for PEC removing and detoxification of organic contaminants (phenol, tetracycline hydrochloride, ciprofloxacin and norfloxacin). The S-scheme heterojunction was double confirmed by DFT calculation and XPS analysis. The charge transfer resistance of BVO/NM125/NM53 photoanode decreases to 1/11 of bare BiVO 4 photoanode. Meanwhile, the photocurrent density was 3 times higher, demonstrating a marked improvement in carrier separation efficiency due to dual S-scheme heterojunction. The photoanode achieved 94.3 % removal of phenol within 60 min and maintained stable performance over 10 consecutive cycles, demonstrating good PEC efficiency and structural stability. The BVO/NM125/NM53 photoanode also showed effectiveness in removing antibiotics, with chlorophyll fluorescence imaging confirming a significant reduction in the ecotoxicity of intermediates. For example, wheat seed germination, growth, chlorophyll and Carotenoid production were not affected, which was similar to that of deionized water. Radical trapping experiments and electron paramagnetic resonance (EPR) analysis identified •O 2 - and •OH as the primary active species. This work demonstrates the effectiveness of developing MOF-on-MOF heterojunctions for visible-light response and enhancing charge separation in PEC.
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Mengli Yan,Zhuo Liu,Shuang Li,Jianwang He,Yan Xu
Metal–organic frameworks (MOFs), known for their exceptional gas permeability and abundant active sites, are a class of porous coordination polymers that can serve as ideal candidates for constructing advanced gas sensors. However, the limitations of low electrical conductivity and inadequate stability under extreme conditions hinder their advancements in gas-sensing applications. Moreover, a single MOF structure occasionally demonstrates insufficient selectivity toward specific gases, failing to meet stringent sensing requirements. To overcome these challenges, this study innovatively constructs an MOF-on-MOF architecture by etching Ti-MOF into a hollow cage-like structure with l-glutamic acid and connecting it with Ni2+ ions to form Ni-MOF via peptide bonds. The approach not only enhances the specific surface area and pore structure of the material but also facilitates carrier transport rates at the interface by effectively linking the two MOFs. The resultant MOF-on-MOF structure exhibits remarkable selectivity and sensitivity in detecting triethylamine gas at a low operating temperature of 140 °C, along with exceptional reproducibility and long-term stability. This work demonstrates a novel amino acid-assisted feasible and simple method to construct MOF-on-MOF material, showcasing immense potential in high-performance gas detection applications.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Bing He,Ying-Jie Wang,Xuefeng Bai,He Bian,Yabo Xie,Rui Li,Jian-Rong Li
MOF-on-MOF composites are deemed promising candidates to accomplish synergistic CO 2 capture and photoreduction thanks to their plentiful active sites, extended light response range, timely separation of photoexcited electron-hole pairs, and large CO 2 adsorption capacities. Unfortunately, the controllable growth of the designed MOF-on-MOF heterostructure is challenging. Deficient interphase contact and the consequent mass transfer deprivation is one of the primary obstacles severely impairing the catalytic efficiency. Herein, the contact between two widely-employed MOFs of Ni-BDC and NH 2 -MIL-125 was significantly strengthened by exploiting a self-assembled array of Ni-BDC microsheets. In contrast to the spontaneously formed spheroidal aggregate, the loosely-packed array exhibits amplified accessible surfaces to interact with NH 2 -MIL-125, contributing to a radically improved interfacial built-in electric field and 7∼9 times rises in the product yields. Moreover, the preferably thin thickness of Ni-BDC microsheets prompts its macroscopic flexibility, permitting intensified deformation for enhanced interphase contact. Coupled with the additional contribution from its copious Lewis acid sites, the developed NH 2 -MIL-125@Ni-BDC array simultaneously converted CO 2 into CO and CH 4 at rates that cannot be matched by its isostructural Co counterpart with declined acidity and flexibility. This work innovatively reveals the immense importance of morphology tailoring and assembly tactic to interphase contact modulation and the upgrade of catalyst performances.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Xi Zhou,Shuai Zhang,Yan Liu,Jiashen Meng,Muxue Wang,Yaoji Sun,Linbo Xia,Zhaozhi He,Wenxin Hu,Lei Ren,Zhiwei Chen,Xingcai Zhang
Nanozymes with peroxidase-like activity have great application potential in combating pathogenic bacterial infections and are expected to become an alternative to antibiotics. However, the near-neutral pH and high glutathione (GSH) levels in the bacterial infection microenvironment severely limit their applications in antibacterial therapy. In this work, a metal–organic framework (MOF)-based cascade catalytic glutathione-depleting system named MnFe2O4@MIL/Au&GOx (MMAG) was constructed. The MMAG cascade-catalyzed glucose to provide H+ and produces a large amount of toxic reactive oxygen species. In addition, MMAG consumed GSH, which can result in bacterial death more easily. Systematic antibacterial experiments illustrated that MMAG has superior antibacterial effects on both Gram-positive bacteria and Gram-negative bacteria.
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Nano Research
·
2021
·Vol. 15
·期 4
·2961-2970
·
IF 8.897
Hu Qian,Xu Licong,Fu Kaixing,Zhu Feichao,Yang Taoyu,Yang Tao,Luo Jinming,Wu Minghua,Yu Deyou
Metal-organic frameworks (MOFs) are attractive for promising applications but plagued by difficult recovery and deployment due to their intrinsic nano/micro powder nature. Although significant efforts have been made to develop separable solid matrixes for MOF supporting, the poor loading stability and durability of MOFs still challenge their engineering applications. Here, we present a facile and effective approach to fabricate MOF-based melamine foams (MFs) (denoted as MOFiths) with ultrahigh loading stability and operation stability, easy separation, and high-efficient performance for versatile robust applications. By adopting our approach, numbers of typical fragile MOFs characterized with wide ranges of particle size (from ∼ nm to ∼ µm) can be precisely incorporated into MFs with controllable loading ratios (up to ∼ 1,600%). Particularly, the produced MOFiths show excellent capacities for the highly effective and durable water purifications and acetalization reactions. 100% of organic pollutants can be rapidly destructed within 10 min by MOFiths initiated Fenton or catalytic ozonation processes under five successive cycles while the maximum adsorption capacity of MOFiths toward Pb(II), Cd(II), and Cu(II) reaches to 422, 222, and 105 mg·g −1 , respectively. This study provides a critical solution to substantially facilitate the engineering applications of MOFs for long-term use in practice.
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Journal of Materials Chemistry C
·
2018
·Vol. 6
·期 30
·8105-8114
·
IF 5.976
Ping Gao,Xiang-Ying Sun,Bin Liu,Hui-Ting Lian,Xin-Qiang Liu,Jiang-Shan Shen
Developing a catalyst with a uniform and well-defined crystal structure is very important to establish a catalytic sensing system with high efficiency. In this work, Cu-BTC metal–organic frameworks (MOFs) without a crystalline CuO or Cu2O phase were successfully synthesized by using a low temperature synthesis method, and the as-prepared Cu-BTC MOFs were found to have outstanding catalytic activity towards the traditional oxidase substrate, o-phenylenediamine (OPD), to generate a colored and fluorescent product. The results of the kinetics analysis revealed that the catalytic behavior of Cu-BTC MOFs towards OPD could well follow the typical Michaelis–Menten equation, indicative of a strong affinity between Cu-BTC MOFs and OPD. On the basis of these findings, taken together the condensation reaction between the –CHO group of formaldehyde and the –NH2 group of OPD to form Schiff base compounds, a novel Cu-BTC MOF-based catalytic sensing system for detecting gaseous formaldehyde could be successfully established.
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ADVANCED ENGINEERING MATERIALS
·
2024
·Vol. 26
·期 14
·2400527
·
IF 3.4
Rongjuan Zhang,Qi Hu,Shaobo Yang,Song Yan,Yaxin Gu,Jiawei Ji,Zheng Zhou,Chaoze Liu,Xinran Li,Zihao Wang,Chengchun Tang
The arrival of the 5 G era has brought great benefits to our lives, but it has also brought problems such as electromagnetic radiation. Therefore, the demand for lightweight, high-performance microwave absorbing materials with wide effective bandwidth is increasing. Herein, MIL-53/g-C 3 N 4 is first synthesized from precursors of ferric chloride, terephthalic acid, and g-C 3 N 4 , and then thermally annealed at different temperatures to generate MOF-Fe@C nanocomposites. Heat treatment can effectively carbonize g-C 3 N 4 to amorphous carbon and reduce iron in MIL-53 to magnetic Fe and Fe 3 O 4 nanoparticles through carbon-thermal reduction reaction. The synergistic effect of dielectric loss of amorphous carbon and magnetic losses of magnetic particles enhances attenuation and improves impedance matching, enhancing microwave absorption. The RL min of MOF-Fe@C(4)-700 is as low as -72.78 dB at 9.44 GHz at a thickness of 3.18 mm and its effective absorption bandwidth is as broad as 4.88 GHz, covering most of X-band frequency range. The research introduces a novel technique for synthesizing absorbers with controllable electromagnetic characteristics by incorporating g-C 3 N 4 as carbon sources into MOF materials.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Yuping Gai,Wei Deng,Junbo Hu,Dan Li,Wenshuo Xie,Xiang Li,Jingjing Zhang,Dewu Long,Fei Jiang
The preparation of stable electrocatalyst for oxygen evolution reaction is of the utmost importance to realize high performance water decomposition reaction . Metal-organic framework (MOF) nanostructures have become promising materials. Herein, we report three kinds of electrocatalysts with different structures and properties for the oxygen evolution reaction, which were constructed by using different binding sites of three kinds of ligands following a mechanism which involved only *O and *OH species as intermediates. CoFeBTC-MOF shows excellent overpotential η = 261 mV at 10 mA cm −2 (1.481 V vs. RHE), Tafel slope of 59.29 mV dec −1 and pretty excellent stability (48 h of continuous testing), making it become one of the best acid-resistant catalysts for oxygen evolution reaction. The DFT calculations show that there are different ways to transfer electrons . In addition, the coupling effect between Co and Fe metals is the key to regulate the electrocatalytic activity , confirming the cooperative catalysis mechanism with a reduced energy barrier.
研究领域:
材料科学
·
电化学
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Yang Zhan,Shun-zhi Yu,Shao-hua Luo,Jian Feng,Qing Wang
Transition-metal sulfides (TMS) are one of the most promising cathode catalysts for Li–O2 batteries (LOBs) owing to their excellent stabilities and inherent metallicity. In this work, a highly efficient mode has been used to synthesize Co@CNTs [pyrolysis products of metal–organic frameworks (MOFs)]-derived CoS2(CoS)@NC. Benefiting from the special yolk–shell hierarchical porous morphology, the existence of Co–N bonds, and dual-function catalytic activity (ORR/OER) of the open metal sites contributed by MOFs, the CoS2@NC-400/AB electrode illustrated excellent charge–discharge cycling for up to nearly 100 times at a current density of 0.1 mA cm–2 under a limited capacity of 500 mA h g–1 (based on the total weight of CoS2@NC and AB) with a high discharge voltage plateau and a low charge cut-off voltage. Meanwhile, the average transferred electron number (n) is around 3.7 per O2 molecule for CoS2@NC-400, which is the chief approach for a four-electron pathway of the ORR under alkaline media. Therefore, we believe that the novel CoS2@NC-400/AB electrode could serve as an excellent catalyst in the LOBs.
研究领域:
材料科学
·
电化学
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yongjiang Shan,Mingliang He,Fei Zhang,Yifei Wang,Yuxin Liu,Yingdong Yang,Xingqian Wang,Xinkang Zhang,Yuqin Li,Zhipeng Wang,Xiangshu Chen
Well-intergrown MOF membranes were challenging to construct using the in-situ approach, due to the poor heterogeneous nucleation of MOF on the supports. Here, we described a technique to manufacture ZIF-8 membranes devoid of induced seeds using support modified by O 2 plasma for the first time. O 2 plasma can increase the number of oxygen-containing functional groups (–OH) on the support surface that could absorb zinc ions from synthesizing solution and offer heterogeneous nucleation sites for the formation of ZIF-8 membranes. The as-synthesized membrane exhibits outstanding gas permeation performance with a high hydrogen permeance of about 2.22 × 10 −7 mol·m −2 ·s −1 ·Pa −1 and a high H 2 /CH 4 ideal selectivity of 25.91. The separation factor of the equimolar H 2 /CO 2 and H 2 /CH 4 mixtures reached 8.72 and 31.03 at 298 K and 0.1 MPa, respectively. In addition, this new technique also allowed for the synthesis of ZIF-67 membranes, and the prepared membrane had an H 2 /CH 4 ideal selectivity of 14.92. This work develops a new route for the efficient fabrication of MOF membranes.
研究领域:
材料科学
·
化学工程
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 10
·106518
·
IF 4.386
Qingxiao Zhang,Pei Han,Hui Zhang,Jixin Yao,Xinyu Wang,Dongmeng Chen,Xueqin Zuo,Qun Yang,Shaowei Jin,Guang Li
The oxygen evolution reaction (OER) is a critical process in the operation of electrochemical water splitting. Metal-organic frameworks (MOFs) are applied in the field of OER electrocatalysis because of their unique structure, but the high impedance and unstable framework during pyrolysis remain unresolved. Here, MIL-88A (iron-based MOF) was modified by hydrolysis and loading Co(OH)2 to improve the catalytic activity. The electrochemical results showed that the Co(OH)2/MIL-88A achieved the optimized performance with the current density of 10 mA cm−2 at 278 mV (vs RHE). Density functional calculations (DFT) combined with characterization tests suggest that electrons transfer from Co(OH)2 to MIL-88A at the interface of the heterostructure, leading to a larger hole electron pair density. D-band theory calculations demonstrated that the synergistic effect of MIL-88A and Co(OH)2 in heterostructure strengthens the adsorption between active sites and adsorbate. The above proofs are the source of the excellent OER performance of the Co(OH)2/MIL-88A. The finding has certain reference significance for the heterogeneous treatment of iron-based MOF catalysts.
研究领域:
材料科学
·
电化学
·
催化科学
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