SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Shiyin Zhao,Yangke Long,Xuehua Shen,Shubin Wang,Yiping Su,Xuanjun Zhang,Zuotai Zhang
Peroxymonosulfate (PMS)-based Fenton-like reactions are widely used for wastewater remediation. Metal-free carbonaceous activators can avoid the secondary pollution caused by metal leaching but often suffer from insufficient activity due to limited active centers and mass transfer barriers. Here, we prepared a series of heteroatom (N, S, F)-doped, highly porous carbonaceous materials (UC- X , X = N, S, F) by pyrolyzing UiO-66 precursors assembled by various organic ligands. Density functional theory calculations showed that the heteroatoms modulated the electronic structures of the carbon plane. UC- X exhibited significantly enhanced PMS activation capability compared with the undoped counterpart, in the efficiency order of UC-N > UC-S > UC-F > UC. UC-N (calcined at 1000°C) showed the best PMS activation, exceeding that of commonly used carbocatalysts. The prominent performance of UC-N originated from its unique porous structure and homogeneously dispersed graphitic N moieties. Trapping experiments and electron spin resonance showed a nonradical degradation pathway in the UC-N/PMS system, through which organics were oxidized by donating electrons to UC-N/PMS* metastable complexes. This work not only reports a universal way to access high-performance, metal-free PMS activators but also provides insight into the underlying mechanism of the carbon-activated PMS process.
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DOI
PubMed
高影响因子
CATALYSIS TODAY
·
2020
·
IF 5.825
Yulong Gu,Wei Xu,Yinyong Sun
The development of active oxidative desulfurization (ODS) catalysts is of practical importance. Recently, MOF-808(Zr) has been attempted to use as ODS catalyst due to its various advantages. However, generally MOF-808(Zr) prepared by conventional method was less active in the oxidation reactions due to the lack of defect sites in the structure. In this contribution, we report that the catalytic oxidative performance of MOF-808(Zr) can be enhanced by acid treatment due to the formation of defect sites resulting from the partial removal of organic linkers in the structure. During the experiment, the effect of acid concentration, treatment time, the addition amount of oxidant and reaction parameters on the performance of MOF-808(Zr) was studied. The catalytic results show that MOF-808(Zr) treated with 0.4 M HCl for 1h can catalyze the oxidation of dibenzothiophene completely at 60°C in 15 min. The activity (mole number of converted DBT per hour per unit mass) is 70 mmol h −1 g −1 , which is much higher than that (45 mmol h −1 g −1 ) of parent MOF-808(Zr). In addition, the catalyst can be reused several times without obvious loss of catalytic performance.
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DOI
高影响因子
Nanoscale
·
2019
·Vol. 11
·期 14
·6970-6981
·
IF 6.97
Jian-Ping Song,Liang Wu,Wen-Da Dong,Chao-Fan Li,Li-Hua Chen,Xin Dai,Chao Li,Hao Chen,Wei Zou,Wen-Bei Yu,Zhi-Yi Hu,Jing Liu,Hong-En Wang,Yu Li,Bao-Lian Su
The lithium–selenium (Li–Se) battery has attracted growing interest recently due to its high energy density and theoretical capacity. However, the shuttle effect and volume change during cycling severely hinder its further application. In this work, we report a metal–organic framework (MOF)-derived nitrogen-doped core–shell hierarchical porous carbon (N-CSHPC) with interconnected meso/micropores to effectively confine Se for high-performance Li–Se batteries. The micropores were located at the ZIF-8-derived core and the ZIF-67-derived shell, while mesopores appeared at the core–shell interface after the pyrolysis of the core–shell ZIF-8@ZIF-67 precursor. Such a special hierarchical porous structure effectively confined selenium and polyselenides to prevent their dissolution from the pores and also alleviated the volume change. In particular, in situ nitrogen doping, which afforded N-CSHPC, not only improved the electrical conductivity of Se but also provided strong chemical adsorption on Li2Se, as confirmed by density functional theory calculations. On the basis of dual-physical confinement and strong chemisorption, Se/N-CSHPC-II (molar ratio of Co source to Zn source of 1.0 in the core–shell ZIF-8@ZIF-67 precursor) exhibited reversible capacities of up to 555 mA h g−1 after 150 cycles at 0.2 C and 462 mA h g−1 after 200 cycles at 0.5 C and even a discharge capacity of 432 mA h g−1 after 200 cycles at 1 C. Our demonstration here suggests that the carefully designed Se/C composite can improve the reversible capacity and cycling stability of Se cathodes for Li–Se batteries.
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DOI
高影响因子
Asia-Pacific Journal of Chemical Engineering
·
2022
·Vol. 17
·期 2
·e2739
·
IF 1.777
Yuan Wang,Shanshan Liu,Qirui Guo,Yidong Zhang
Conversion of biomass-derived furfural platform compound to value-added tetrahydrofurfuryl alcohol (THFL) molecule is a sustainable route, and an efficient nonnoble metallic catalyst is a key factor for this reaction. In this work, Ni@C@CNT composite as a highly effective catalyst for hydrogenation of furfural to tetrahydrofurfuryl alcohol was synthesized by one-step pyrolysis of Ni-centered metal organic framework (Ni-MOF) doping with carbon nanotube (CNT). For comparison, Ni@C catalyst derived directly from Ni-MOF was also synthesized. The characterization results show that the doping of CNT promotes high dispersion of active sites and formation of Ni 3 C phase which has Pt-like catalytic activity. Therefore, the obtained Ni@C@CNT exhibited excellent activity in furfural hydrogenation (99.1% furfural conversion and 94.7% THFL yield at 120°C, 4 h, 4-MPa initial hydrogen pressure). Ni@C@CNT also shows good stability in reuse test. Current work presents a facile method for preparation of nonnoble metallic catalysts with high efficiency.
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DOI
高影响因子
COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING
·
2022
·
IF 9.463
Mei Wan,Congling Shi,Xiaodong Qian,Yueping Qin,Jingyun Jing,Honglei Che,Fei Ren,Jian Li,Bin Yu
In this study, three-dimensional flower-like Ni-MOFs were fabricated and successfully functionalized on multi-terminal lamellar MXene (Ti 3 C 2 T x ) by solvothermal method, and their flame retardant application in thermoplastic polyurethanes (TPU) was investigated. As expected, the addition of Ni-MOF@Ti 3 C 2 T x can improve the flame retardancy and smoke suppression properties of TPU. The heat release rate, the smoke release rate, total smoke production, CO and CO 2 release of the composite with only 1 wt% MOF@Ti 3 C 2 T x were significantly reduced by 15%, 44%, 26%, 18%, and 8%, respectively. Furthermore, the carbon residues of TPU/Ni-MOF@Ti 3 C 2 T x composites were about 2–5 times that of pure TPU, indicating that the Ni-MOF@Ti 3 C 2 T x can inhibit the thermal degradation of TPU. The mechanism illustrated that the excellent fire safety properties of TPU/Ni-MOF@Ti 3 C 2 T x composites are due to the physical barrier, catalytical carbonization, and gas-phase flame retardant of Ni-MOF@Ti 3 C 2 T x . In this work, the dispersity, thermal stability, and flame retardancy of MXene were improved due to the modification of MXene with Ni-MOF by chemical bonding and physical adsorption, which can broaden the range of applications of MOFs .
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DOI
高影响因子
NANOTECHNOLOGY
·
2023
·Vol. 34
·期 49
·495706
·
IF 3.5
Ziran Zeng,Yunfan Li,Yilin Zhao,Jun Yuan,Longju Yi,Peilong Li,Gary J Cheng,Feng Liu
Due to the advantages of high porosity, excellent conductivity, and tunable morphology, carbonized metal-organic framework (C-MOF) is expected to become an ideal material for constructing high-performance flexible pressure sensor. Herein, to achieving the suitable morphology of C-MOF for piezoresistive sensors, a rapid thermal process (RTP) was used for carbonization of NiCo-MOF, and the petal-shaped NiCo alloy nanoparticles/nanoporous carbon composites (NiCo-NPCs) were obtained. Compared with NiCo-NPCs carbonized by common thermal process (CTP), NiCo-NPCs carbonized by RTP exhibit a modified morphology with smaller particle size and larger most frequent pore diameter. Due to the modified morphology, the piezoresistive sensor with RTP-carbonized NiCo-NPCs has a high sensitivity of 62.13 kPa–1 at 0–3 kPa, which is 3.46 times higher than that of the sensor with CTP-carbonized NiCo-NPCs. Meanwhile, the sensor shows an ultra-wide range of 1000 kPa, excellent cycle stability (>4000 cycles), and fast response/recovery time of 25/44 ms. Furthermore, the application of the sensor in dynamic loading test, airflow monitoring, voice recognition, and gesture detection demonstrates its great application prospects. In short, this work investigates the application of carbonized NiCo-MOFs in flexible pressure sensors, and provides a new strategy to improve the performance of piezoresistive sensors with porous carbon derived from MOFs.
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DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2019
·
IF 3.218
Xiaolong Tu,Yu Xie,Xue Ma,Feng Gao,Lei Gong,Dingwen Wang,Limin Lu,Guangbin Liu,Yongfang Yu,Xigen Huang
Metal–organic frameworks (MOFs) as porous materials have been widely used in electrochemical sensing field. Unfortunately, their low electrical conductivity and poor stability in the aqueous solution limit their application. To overcome these shortcomings, in this study, a novel reduced graphene oxide-encapsulated Ce-MOF (RGO@Ce-MOF) composite was synthesized by using a simple and green method. Ce-MOF and GO were firstly casted onto glassy carbon electrode, respectively, and then GO was reduced to RGO through electrochemical reduction strategy. The proposed encapsulated structure of RGO@Ce-MOF effectively improved the stability of Ce-MOF by preventing decomposition of MOF in solution. The combination of RGO and Ce-MOF can also significantly promote the conductivity of composite. Then, the obtained RGO@Ce-MOF composite was utilized as electrode material for the detection of dichlorophen (Dcp), a halogenated phenolic intermediate for synthesis of pesticide. The electrochemical properties of the proposed sensor were investigated by electrochemical techniques in detail. Benefiting from the synergy between Ce-MOF and RGO, the RGO@Ce-MOF can be used to detect Dcp with a wide linear range from 0.02 μM to 10 μM and a low detection limit of 0.007 μM (S/N = 3). Furthermore, the RGO@Ce-MOF electrode showed acceptable reproducibility and good selectivity. This method was applied to detect Dcp in the real samples with satisfying results.
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DOI
高影响因子
ChemSusChem
·
2023
·Vol. 16
·期 24
·e202300864
·
IF 8.4
Chen Zhang,Tingyu Su,Xinqi Zhang,Duoyong Zhang,Tao Xuan,Liwei Wang
Graphical A kind of ionic liquid, namely deep eutectic solvents, are introduced to load on the surface of porous MOF-808 core as membranes to construct porous core-membrane microstructured nanomaterials for CO 2 capture at room temperature with the sorption mechanism coupling of diffusion, physisorption, and chemisorption. It shows excellent development potential for future application in CO 2 capture. A series of porous core-membrane microstructured nanomaterials, constructed of a deep eutectic solvent (DES) membrane and porous MOF-808 core via liquid surface tensions and electrostatic interactions, are introduced for carbon dioxide capture with the sorption mechanism coupling diffusion, physisorption, and chemisorption. MOF-808 as the porous core considerably improves the diffusion interactions for DES membranes, hence significantly enhancing the sorption performance of DESs. Although the DES consisted by monoethanolamine and tetrapropylammonium chloride (MEA-TPAC-7) has the highest sorption capacity among all DESs, it is only 4.39 mmol g −1 at 2.4 bar and further attenuates by fastidious diffusion interactions when increasing viscosity or dose. The sorption capacities of DES@MOF-120 are 5.18 mmol g −1 at 3.0 bar and 4.78 mmol g −1 at 2.4 bar without apparent sorption hysteresis in pressure swing sorption, which are substantially improved contrasted to MEA-TPAC-7. The sorption isotherms are reconstructed via Sips models considering surface heterogeneity with regression correlation coefficients over 0.9454 to forecast maximum sorption capacity over 6.33 mmol g −1 .
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DOI
高影响因子
Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 14
·5159-5166
·
IF 8.262
Lijin Huang,Man He,Beibei Chen,Bin Hu
A facile preparation of magnetic MOF composites with flexible mercapto group pendants in their pores is realized through solvent-assisted ligand exchange (SALE) under mild conditions in water, and terephthalate in UIO-66 is replaced with mercaptoacetic acid (MAA). After the SALE processing, the crystallinity, porosity, and superparamagnetism of the mercapto functionalized magnetic Zr-MOF (MFC-S) are well maintained, and the obtained MFC-S exhibits a higher adsorption capacity (282 mg g−1) for Hg2+ than that of the magnetic Zr-MOF (MFC-O). Furthermore, the prepared MFC-S can be regenerated easily by liquid desorption after adsorption of metal ions and be reused more than 5 times without obvious decrease in removal performance. The proposed SALE method for the preparation of mercapto functionalized magnetic MOF composites (MFCs) is easy-to-operate and low cost, providing not only a reliable porous MFC platform for the removal of metal ions, but also a simple and efficient synthesis route for the preparation of functionalized MFCs which cannot be achieved through conventional approaches.
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2018
·
IF 6.578
Ke Chen,Kai Xu,Long Xiang,Xiao Dong,Yue Han,Chongqing Wang,Lin-Bing Sun,Yichang Pan
Mixed matrix membranes (MMMs) derived from metal-organic frameworks (MOFs) nanocrystals represent a promising alternative for overcoming the trade-off between permeability and selectivity derived from the pristine polymeric membrane . The selection of MOFs fillers are mainly focused on their diffusion-selectivity property for gas-pairs. However, the improvement of both gas-permeability and selectivity through addition of sorption-selective MOFs are rarely reported. Herein, the incorporation of CO 2 -philic KAUST-7 (also referred to as NbOFFIVE-1-Ni) nanocrystals makes the neat 6FDA-Durene polyimide membrane more permeable and more selective, surpassing the state-of-the-art 2008 Robeson upper bound for CO 2 /CH 4 . Nano-sized (~ 80 nm) KAUST-7 crystals with sharp particle size distribution were first fabricated through a co-solvent synthesis method. The explored gas transportation mechanism indicates that the improvement of CO 2 /CH 4 selectivity on MMMs are attributed to the significant raise of the sorption-selectivity rather than the diffusion-selectivity. The favorable interfacial interaction between the imide groups of the 6FDA and the H of the pyrazine in the KAUST-7 enhances plasticization resistance of the neat polymer membrane. The developed MMMs exhibit a promising application in CO 2 capture from natural- and bio-gas.
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DOI
高影响因子
JOURNAL OF APPLIED ELECTROCHEMISTRY
·
2019
·Vol. 49
·期 6
·563-574
·
IF 2.366
Zheng Sining,Wu Dan,Huang Limei,Zhang Mengxin,Ma Xiuling,Zhang Zhangjing,Xiang Shengchang
Abstract It is needed to speed up the development of a sensitive detection platform for simultaneous determination of dihydroxybenzene isomers with harmful properties. Here, two isomorphic Metal–organic frameworks (MOFs) [Zn(Trz)(R-BDC) 1/2 ] (FJU-40-R, R = H or NH 2 ; Trz = 1,2,4-Triazole; H-BDC = terephthalic acid) were selected to derive two N-doping porous carbon (NPC) materials. Further, a strategy for constructing electrochemical sensors for simultaneous determination of hydroquinone (HQ) and catechol (CT) was proposed by the MOF-derived NPC modifying glass carbon electrode (GCE). It was found that HQ and CT had good responses on NPC-FJU-40-H/GCE, but had no obvious responses on NPC-FJU-40-NH 2 /GCE. NPC-FJU-40-H/GCE displayed excellent reproducibility, stability, and anti-interference. Under the optimal conditions, the linear ranges of HQ and CT on NPC-FJU-40-H/GCE were 1 ~ 70 µmol L −1 and 1 ~ 100 µmol L −1 with the detection limits of 0.18 µmol L −1 for HQ and 0.31 µmol L −1 for CT, respectively. Although the porous carbon (PC) derived from MOFs has been applied in electrochemical sensing, the effect of the ligand functional groups of isomorphic MOFs on the electrochemical properties of the derived PC materials is still lack of relevant research. Our research provided an idea that the electrocatalysis properties of MOF-derived porous carbon materials could be tuned by changing the functional groups in ligands of isomorphic MOFs in electrochemical sensing field. Graphical abstract A feasible strategy was proposed by changing the ligands of the two isomorphic MOFs (FJU-40-H and FJU-40-NH 2 ) to tune the electrocatalysis properties of MOF-derived N-doped porous carbon materials for the simultaneous determination of dihydroxybenzene isomer.
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高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Zihui Yu,Yan Wang,Yaoming Zhang,Qihua Wang,Tianqiang Yin,Zhancheng Zhang,Gai Zhao,Meizhe Yu,Xianqiang Pei
Due to their unique organic–inorganic hybrid structures, metal–organic frameworks (MOFs) have shown increasing potential as fillers for polymer self-lubricating composites. In this study, a systematic investigation of three structurally different MOFs (ZIF-8, MOF-5, and UiO-66, each at 3 wt%) in polyimide (PI) composite coatings revealed that their incorporation enhanced the mechanical properties. Notably, UiO-66 exhibited the most pronounced reinforcement, attributable to its strong interfacial bonding with the resin matrix, which led to an 18.4% increase in tensile strength as well as corresponding enhancements in elastic modulus and hardness. To gain insight into the friction and wear mechanisms of MOFs/PI composite coatings, ball-on-disc tests were complemented by molecular dynamics (MD) simulations and density functional theory (DFT) calculations. This combined approach elucidated the role of MOFs at the frictional contact interface and their influence on transfer film formation. The conclusions regarding the intrinsic relationship between the structure of MOFs and their tribological mechanisms are of both theoretical and practical importance for developing PI composite coatings for self-lubricating bushings, bearing shells and sliders.
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