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Journal of Cleaner Production · 2023 · IF 11.1

Construction of MXene/MOFs nano-coatings on PU sponge with enhanced interfacial interaction and fire resistance towards efficient removal of liquid hazardous chemicals

Guojun Deng,Mengnan Sun,Yongqian Shi,Yuezhan Feng,Yuancai Lv,Longcheng Tang,Jiefeng Gao,Pingan Song

The leaked hazardous chemicals pose significant risks due to their harmful and combustible nature. Removing them from the environment has become an arduous task for both the industrial sector and academic community. In this paper, Ti 3 C 2 T x (MXene) nanosheets and metal-organic framework (ZIF-8 MOFs) functionalized polyurethane (PU) sponges (PU-Ti 3 C 2 T x -MOF sponges) were prepared by immersion coating and in-situ growth techniques. The as-prepared PU-Ti 3 C 2 T x -MOF sponge exhibited superior hydrophobicity with a water contact angle of 135°. Additionally, it demonstrated a higher adsorption capacity and rapid adsorption ability for liquid hazardous chemicals within 1 min, while still maintaining good reusability for adsorption. The PU-Ti 3 C 2 T x -MOF 2 sponge had the highest adsorption capacity of 48–91 times of its own mass for liquid hazardous chemicals. Furthermore, it demonstrated excellent reusability, maintaining its high adsorption capacity for oils and organic solvents even after being used 5 times. These results surpass previously reported data and highlight the superior capabilities of the PU-Ti 3 C 2 T x -MOF 2 sponge. Meanwhile, the PU-Ti 3 C 2 T x -MOF sponge maintained the excellent flame retardancy and compressibility . This work provides a new pathway for the design of functional polymer sponges and their potential application in rapid elimination of the leaked hazardous chemicals.

CAS / MDL: 10196-18-6
研究领域: 材料科学 · 环境科学
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DALTON TRANSACTIONS · 2019 ·Vol. 49 ·期 2 ·312-321 · IF 4.052

Chemical fixation of CO2 into cyclic carbonates catalyzed by bimetal mixed MOFs: the role of the interaction between Co and Zn

Yuanfeng Wu,Xianghai Song,Siquan Xu,Yuan Chen,Olayinka Oderinde,Lijing Gao,Ruiping Wei,Guomin Xiao

Bimetal mixed MOFs of [CoZn][(BDC)(DABCO)0.5] (CZ-BDO), [CoNi][(BDC)(DABCO)0.5] (CN-BDO), and [NiZn][(BDC)(DABCO)0.5] (NZ-BDO) were prepared under solvothermal conditions and further employed as highly active accelerants for converting carbon dioxide into cyclic carbonates. The characteristics of the bimetal compounds were revealed via various techniques, including ICP-OES, XRD, FT-IR, Raman, XPS, SEM, EDS maps, N2 adsorption, TG-DTG, and CO2/NH3-TPD. The catalytic results revealed that CZ-BDO is superior to the other samples for obtaining a satisfactory chloropropene carbonate (CPC) yield. The excellent catalytic activity may be owing to the presence of a solid solution within the Co and Zn bimetal sample, which provides synergistic catalysis in the carbon dioxide cycloaddition. In addition, the synergistic catalysis was further confirmed by the NH3-TPD profiles, whereby the amount of CZ-BDO basic sites was obviously enhanced compared to the other samples. Furthermore, DFT calculations were also performed to reveal the synergistic catalysis between Co and Zn for the coupling reaction. Additionally, when the coupling reaction was carried out at 100 °C for 5 h in the presence of 0.5 wt% epichlorohydrin (ECH) as a catalyst at 3.0 MPa, 99.31% conversion of ECH and 97.05% yield of CPC were obtained over the optimal CZ-BDO sample. Moreover, the bimetal sample can also efficiently convert other epoxides into the corresponding cyclic carbonates.

研究领域: 化学 · 材料科学
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NEW JOURNAL OF CHEMISTRY · 2022 ·Vol. 46 ·期 25 ·12372-12380 · IF 3.925

A series of novel Cu-based MOFs: syntheses, structural diversity, catalytic properties and mimic peroxidase activity for colorimetric detection of H2O2

Juan Chai,Luohao Yuan,Shiwei Wang,Tong Li,Mingxue Wu,Zhiwei Huang,Hongfeng Yin

Three metal–organic frameworks {[Cu6(L1)4(DMF)(H2O)2·5H2O]}n (1), {Cu3(L1)2(phen)2(H2O)}n (2) and {[Cu8(μ3-OH)3(L2)4(NO3)(H2O)5]·3H2O}n (3) utilizing nitrogen-containing heterocyclic carboxylate bifunctional ligands (L1 = 5-(4-carboxypyridin-3-yl)isophthalic acid and L2 = 2-(5-carboxypyridin-2-yl)terephthalic acid) were self-assembled hydrothermally and characterized. MOFs 1–3 possess 3D networks which consist of three different types of Cu clusters {Cu2O2(OCO)4}, {Cu2O2N4(OCO)2} and {Cu4O10(OCO)4}, respectively. MOFs 1–3 efficiently catalyze the oxidation of cycloalkanes under mild conditions. Besides, the synthesized MOFs 1–3 exhibited high peroxidase-like activity and could be utilized to catalyze the oxidation of 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulphonic acid ammonium salt) (ABTS) to produce green color in the presence of hydrogen peroxide (H2O2). The steady-state kinetics experiments of the oxidation of ABTS catalyzed by MOFs 1–3 were carried out, and the kinetic parameters were obtained. The results indicated that the affinity of MOFs 1–3 towards H2O2 and ABTS was higher than that of the natural horseradish peroxidase (HRP). The as-prepared MOF 1 can be applied for the colorimetric detection of H2O2 with a wide linear range of 0.5 to 200 μM and a limit of detection (LOD) of 0.097 μM. Therefore, the novel Cu-MOFs could be regarded as promising artificial enzyme mimics in catalysis, sensors and environment analysis.

研究领域: 材料科学 · 生物化学 · 分析化学
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MOLECULES · 2024 ·Vol. 29 ·期 21 ·4989 · IF 4.2

Two Co(II) Isostructural Bifunctional MOFs via Mixed-Ligand Strategy: Syntheses, Crystal Structure, Photocatalytic Degradation of Dyes, and Electrocatalytic Water Oxidation

Siyu Yue,Mengqi Tuo,Yemeng Sheng,Xinyu Guo,Jiufu Lu,Dong Wang

The solvothermal reactions involving cobalt ions with 5-methylisophthalic acid (H2MIP) and 1,3-bis(2-methylimidazol)propane (BMIP) yielded two cobalt(II) organic frameworks: {[Co4(MIP)4(BMIP)3]·1/2DMA}n(SNUT-31) and {[Co4(MIP)4(BMIP)3]·(EtOH)2·H2O]}n(SNUT-32) where DMA represents N,N-dimethylacetamide and EtOH signifies ethyl alcohol. Single-crystal X-ray diffraction analyses reveal thatSNUT-31andSNUT-32possess an isomorphic structure, featuring a unique 2-fold interpenetration of 3D frameworks in a parallel manner. Notably, bothSNUT-31andSNUT-32demonstrate remarkable performance in electrocatalytic oxygen evolution reactions and exhibit exceptional photocatalytic degradation capabilities against a model comprising three distinct dyes: rhodamine B, methyl orange, and methyl blue.

研究领域: 材料科学 · 环境科学 · 化学
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APPLIED ORGANOMETALLIC CHEMISTRY · 2024 · IF 3.7

A Microsphere Dual-Ligand MOFs Modified Carbon Paste Electrode and Its Application as Electrochemical Sensor for Bisphenol A and Metal Ions

Ganghui Wang,Han Wang,Huan Li,Panpan Chen,Hongxu Guo

This study introduces a new electrochemical sensor for bisphenol A (BPA) and metal ions utilizing a microsphere dual-ligand Ni-based MOFs modified carbon paste. The MOFs (Ni-bipy-btc) synthesized from dual-ligands were prepared via a hydrothermal method and characterized using X-ray diffraction (XRD), scanning electron microscope (SEM), FT-IR spectrometer, X-ray photoelectron spectrum (XPS), and specific surface area test (BET) analysis. The resulting MOFs exhibited promising performance as electrode materials for electrochemical sensors targeting the detection of BPA and heavy metal ions (Pb 2+ and Cu 2+ ). The linear range of the MOFs (Ni-bipy-btc)/CPE electrode for BPA detection ranged from 0.2 to 150 μM, with a detection limit of 0.045 μM, demonstrating robust immunity and stability. Additionally, the limit of detection for the MOFs (Ni-bipy-btc)/CPE electrode was found to be 4.3 and 9.5 nM for Pb 2+ and Cu 2+ ions, respectively, showcasing excellent stability and reproducibility. This study presents a straightforward approach for the highly sensitive electrochemical detection of BPA and heavy metal ions using a simple hydrothermal reaction method.

CAS / MDL: 80-05-7
研究领域: 分析化学 · 环境科学 · 材料科学
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RESEARCH ON CHEMICAL INTERMEDIATES · 2022 ·Vol. 48 ·期 6 ·2489-2507 · IF 3.134

MOFs-derived hierarchical porous carbon confining the monodisperse Ni and defective WOx for efficient and stable hydrogenolysis of cellulose to ethylene glycol

Shao Lingling,Zhou Jiancheng,Zhang Ming,Zhang Qianyi,Wang Nan,Zhu Fengfan,Wang Ke,Li Naixu

The one-pot catalytic conversion of cellulose into ethylene glycol (EG) is an attractive way of biomass utilization. However, low-cost, efficient, and stable catalysts are the premise and research challenges of industrial application. Herein, the magnetic recyclable W–Ni@C catalyst was synthesized by in-situ pyrolysis of Ni-MOFs impregnated with ammonium metatungstate. Compared with the Ni-W bimetallic catalysts prepared by the impregnation method and the sol–gel method, the W–Ni@C catalyst for cellulose hydrogenolysis reaction can achieve a higher ethylene glycol yield (67.1% vs 43.3% and 42.6%) and 100% of cellulose conversion rate. The uniformly dispersed Ni nanoparticles and abundant defective WO x were formed in a reductive atmosphere generated in pyrolysis of Ni-MOFs, which was indispensable for the hydrogenolysis of cellulose into EG. Besides, the hierarchical porous carbon derived from organic ligands in Ni-MOFs reduces the mass transfer resistance while confining Ni nanoparticles and WO x to prevent their leaching, effectively enhancing the stability of the W–Ni@C catalyst. Therefore, the remarkable catalytic performance, the simple and effective recovery method as well as satisfying stability would make W–Ni@C become a promising catalyst for the conversion of cellulose to EG. Graphical abstract

研究领域: 材料科学 · 催化化学 · 生物质转化
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CHEMOSPHERE · 2020 · IF 5.778

MOFs-derived magnetic C@Cu–Ni bimetal particles: An efficient peroxymonosulfate activator for 2,4,6-trichlorophenol degradation

Deyun Zhang,Yunong Li,Jing Guo,Lixiang Zhou,Yeqing Lan,Cheng Chen

In this study, magnetic Cu and Ni bimetallic particles embedded carbon sheets, namely as C@Cu–Ni, was derived via calcining a mixture of Cu-MOFs and Ni-MOFs (mass ratio = 4:6) under N 2 protection and served as a catalyst for the degradation of 2,4,6-trichlorophenol (2,4,6-TCP) by peroxymonosulfate (PMS). The results showed that more than 98.5% of 2,4,6-TCP (10 mg L −1 ) was rapidly decomposed at initial pH = 5, PMS = 1 mM and catalyst dosage = 0.1 g L −1 within 30 min, accompanied by 42.47% removal of total organic carbon (TOC). This fully confirmed that C@Cu–Ni possessed excellent catalytic performance for PMS activation . The radical quenching experiments and electron paramagnetic resonance (EPR) investigation testified that the reactive oxygen species (ROS) included SO 4 •− , • OH, O 2 •− radicals and singlet oxygen ( 1 O 2 ), which were responsible for the rapid degradation of 2,4,6-TCP. Among them, O 2 •− and 1 O 2 played a decisive role. Cyclic voltammograms (CV) and electrochemical impedance spectroscopy (EIS) revealed that C@Cu–Ni material possessed superior electrical conductivity and electron transfer , improving its catalytic activity . What is more, C@Cu–Ni displayed excellent stability and could be consecutively used for five times without any decline of catalytic performance. The main intermediates of the 2,4,6-TCP degradation were analyzed by high-performance liquid chromatography-mass spectrometry (HPLC-MS/MS) and possible pathways of 2,4,6-TCP degradation were further proposed. The extraordinary stability and superior catalytic activity of C@Cu–Ni coupled with its easy separation from wastewater due to magnetism suggest that the newly synthesized material may offer a promising alternative approach to efficiently degrade organic pollutants by PMS.

CAS / MDL: 554-95-0
研究领域: 环境科学 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Carbon nanotubes interpenetrating MOFs-derived Co-Ni-S composite spheres with interconnected architecture for high performance hybrid supercapacitor

Zhenlin Ma,Rong Zheng,Yu Liu,Yulong Ying,Weidong Shi

Recently, carbon nanotubes (CNT)-based interconnected architectures exhibit promising prospects in supercapacitors due to their flexibility and high electrical conductivity. Herein, a three-dimensional (3D) interconnected network structure combined with conductive carbon nanotubes interpenetrating MOFs-derived Co-Ni-S composite spheres (Co-Ni-S/CNTs) was synthesized. Such 3D interconnected architecture significantly leads to a favorable electronic structure, fast charge-transfer capacity, and more pseudocapacitive. The Co-Ni-S/CNTs-based hybrid electrode exhibits an extraordinary specific capacitance of 540.6C g −1 at 1 A g −1 and competitive rate performance (capacity retention rate of 69.9% when the current density increases to 10 times). Subsequently, a hybrid supercapacitor is assembled using Co-Ni-S/CNTs as the positive electrode and commercial activated carbon as negative electrode. The device delivers a high energy density of 63.5 W h kg −1 at 800 W kg −1 and keeps 83.0% initial capacitance retention after 10,000 cycles. The encouraging performances demonstrate the significant contribution of the 3D interconnected architecture for the future energy storage.

研究领域: 材料科学 · 能源存储
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Catalysis Science & Technology · 2020 ·Vol. 10 ·期 6 ·1699-1707 · IF 5.721

Lewis acid sites in MOFs supports promoting the catalytic activity and selectivity for CO esterification to dimethyl carbonate

Yu-Ping Xu,Zhi-Qiao Wang,Hong-Zi Tan,Kai-Qiang Jing,Zhong-Ning Xu,Guo-Cong Guo

CO esterification to dimethyl carbonate (DMC) is an attractive route, although the catalyst is the main problem restricting the industrialization of this route. Supported palladium catalysts have been often used for this route. However, the effect of the support is not always clear. In this work, we firstly introduced three metal–organic frameworks (MOFs) materials as catalyst supports, namely UiO-66, MIL-101 and MOF-5, and studied the effect of Lewis acid sites in the MOFs supports on the catalytic activity and selectivity for CO esterification to DMC. Interestingly, the Pd(II)/UiO-66 catalyst exhibits superior catalytic performance to the other catalysts, with 87.9% CO conversion and 98.5% DMC selectivity due to the abundant Lewis acid sites in UiO-66. It was proven that UiO-66 with more defects would have a large number of Lewis acid sites, and the catalytic performance was positively correlated with the number of Lewis acid sites in MOFs supports, which can be demonstrated by characterization by NH3-TPD, pyridine-IR, XPS and in situ DRIRS. The current work not only revealed the relationship between the Lewis acidity of the support and catalytic performance, but also promotes the development of practical catalysts for CO esterification to DMC.

CAS / MDL: 10026-11-6
研究领域: 化学工程 · 催化科学
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IONICS · 2024 ·Vol. 30 ·期 3 ·1723-1733 · IF 2.4

NiCo2S4/rGO composite electrode material derived from Co-based MOFs for hybrid supercapacitors

Zhao Ji-wei,Wei Zhi-qiang,Wang Can,Zhou Mei-pan,Lu Cheng-gong

The Co-based organic skeleton was combined with graphene oxide (GO) as a precursor, Ni 2+ hydrolysis etching was introduced, and finally, NiCo-LDH/GO was obtained. The final composite electrode material NiCo 2 S 4 /rGO was obtained by high-temperature vulcanization. The introduction of MOFs and rGO significantly increased the specific surface area of the material and made it have excellent electrochemical properties. The specific capacitance of the composite NiCo 2 S 4 /20rGO reaches an astonishing 272.5 mAh g −1 when the current density is 1 A g −1 . In addition, at a large current of 10 A g −1 , the specific capacitance of the material can also reach 139.5 mAh g −1 , and after a long cycle of 5000 cycles at such a current density, the capacity remains at the original 73.2%. With NiCo 2 S 4 /20rGO electrode material as the positive electrode and activated carbon as the negative electrode, the hybrid supercapacitor is assembled. At an energy density of 56.9 Wh kg −1 , its power density reaches an excellent 799 W kg −1 , and it still has a capacity retention rate of 74% at a current density of 10 A g −1 . The excellent properties of composites demonstrated in this work open up new possibilities for high-quality energy storage devices.

研究领域: 材料科学 · 电化学 · 储能 · 纳米技术 · 无机化学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Promoting the hole extraction and interfacial performance with MOFs derived Co3O4@NC for efficient carbon-based perovskite solar cells

Cong Geng,Peng Wei,Huamei Chen,Haichao Liu,Shenshen Zheng,Haobin Wang,Yahong Xie

Carbon-based perovskite solar cells (C-PSCs) facilitate modularization and commercialization due to their excellent thermal stability and low cost. However, C-PSCs show the poor performance that charge carrier extraction by the carbon electrode alone is not as efficient as in the case of conventional hole transport materials (HTMs) based PSCs. In this work, an inorganic hole buffer layer of nitrogen-doped carbon/Co 3 O 4 (Co 3 O 4 @NC) nanoparticles derived from MOFs is introduced to adjust energy alignment and passivate perovskite (PSK) grain boundaries (GBs). Moreover, a simple processing method on the Co 3 O 4 @NC nanoparticles manipulated by controllable ultraviolet/ozone (UVO) treatment is employed, to further improve the interfacial performance of MAPbI 3 /Co 3 O 4 @NC and reduce the hysteresis. Through interface engineering, it is found that Co 3 O 4 @NC inorganic hole buffer layer effectively promotes photo‐generated charge separation and extraction, and suppresses charge recombination at the MAPbI 3 /Carbon electrode (CE) interface, resulting in improved photovoltaic performance. Consequently, the optimal C-PSCs without encapsulation achieved a maximum PCE of 14.63%, which is 22.3% more efficient than the pristine device (11.96%), and exhibited outstanding long-term stability.

研究领域: 材料科学 · 能源技术 · 光电转换
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FUEL · 2022 · IF 8.035

Spherical NiCo-MOFs catalytic hydrogenolysis of lignin dimers and enzymatic lignin to value-added liquid fuels under nitrogen atmosphere

Minghao Zhou,Chengjun Tang,Jing Li,Haihong Xia,Peng Liu,Junming Xu,Changzhou Chen,Jianchun Jiang

Ni-based MOFs catalysts are promising candidates that can be used to achieve biomass valorization following the process of selective hydrogenolysis process. Here we report a spherical NiCo-based MOFs catalyst, which provides a larger BET surface to enhance 2-phenoxy-1-phenylethan-1-ol molecules enrichment and promote the hydrogenolysis on spherical NiCo-based MOFs catalyst surface. In addition, the synergistic interaction between Ni and Co species also shows great effect on catalytic hydrogenolysis of 2-phenoxy-1-phenylethan-1-ol molecules and enzymatic lignin. The yields of ethylcyclohexane and cyclohexanol are dramatically improved to more than 90 mol% over Ni3Co1-based MOFs catalyst under nitrogen atmosphere. Various lignin dimers derivatives are investigated over Ni3Co1-based MOFs catalyst, which indicates oxygen-containing functional groups played a critical role in the hydrogenolysis process. Isopropanol is used as solvent in the hydrogenolysis of 2-phenoxy-1-phenylethan-1-ol molecules and enzymatic lignin. 21% of H 2 is observed in the GC/MS, suggesting that it is a catalytic transfer hydrogenolysis process. Catalytic hydrogenolysis of enzymatic lignin is also carried out under 280 ℃ over optimal Ni3Co1-based MOFs catalyst for 6 h, giving highest lignin oil yield (75.6 wt%) and lower O/C ratio (0.17). This work can be extended to different biomass valorizations to promote the catalytic behavior of spherical MOFs catalysts.

研究领域: 催化化学 · 生物质能 · 材料科学
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