JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Yuwei Hu,Yijing Jiang,Lingyu Ni,Zhengjie Huang,Lei Liu,Qinfei Ke,He Xu
Due to the frequent spill accidents during crude oil exploration and transport, to rapidly cleanup crude oil and eliminate the environmental pollution of oil spill is in high demand. In this work, a three-dimensional graphene aerogel (MEGA) with high elasticity, photothermal conversion capacity and adsorption capacity was prepared for rapid removal of crude oil. The results showed that the as-prepared MEGA exhibited a layered structure, the octahedral HKUST-1 nanoparticles and hydrophobic polydimethylsiloxane (PDMS) coatings were uniformly deposited on the surface. Such a hierarchical micro-nano porous structure not only improved the aerogel’s hydrophobicity (water contact angle in air up to 152.7°), but also endowed it with strong oil adsorption capacity (41–118 times of its own weight). Especially, the MEGA showed excellent photothermal conversion capacity. Under light irradiation, its temperature raised to 80 ℃ from room temperature in 100 s. As a result, the adsorption for one drop of crude oil by MEGA was shortened from 5 h to 40 s, comparing with that in dark condition. In addition, the MEGA showed remarkable elasticity and mechanical stability, it could maintain more than 90% efficiency after 10 adsorption-compression cycles. This study suggests that the prepared MEGA has great potential for rapid removal of crude oil.
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Analytical Methods
·
2022
·Vol. 14
·期 41
·4095-4105
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IF 3.532
Qiao Gao,Yu Zhao,Jiyu Gong,Xin Chen,Wei Liu,Wenyi Gao
Adsorption and separation of dyes are extremely important as they damage the water environment and human health. ZIF-8 has the benefits of large specific surface area, explicit structure and a good confinement effect on POM, which can better facilitate the synergetic effect of POM and ZIF-8. Therefore, ZIF-8 was chosen as the support material to wrap H3PW12O40. In the present work, magnetic ZIF-8@H3PW12O40 composites were prepared by a facile impregnation synthesis strategy and applied to the adsorption of cationic dyes with methylene blue (MB) as a representative. Compared with the other three prepared materials, Fe3O4@ZIF-8@H3PW12O40 exhibited the best adsorption performance. The adsorption process conformed to the pseudo-second-order model and the Langmuir model, and the adsorption reaction was spontaneous with the maximum adsorption capacity of up to 431.03 mg g−1 within 20 min. The electrostatic attraction has been testified to be the major driving force of the adsorption process, and the material can still hold 90% of the max adsorption capacity after 5 cycles, which serve as the foundation for its further applications in the field of adsorption.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Daping Hu,Yuhang Jia,Fuyao Huang,Yuhong Long,Chunjin Ai,Pengcheng Du
Transition metal phosphides (TMPs) are considered excellent candidate electrode materials for supercapacitors (SCs) due to their high theoretical capacity. However, the severe performance degradation of TMPs, originating from poor conductivity and resulting volumetric expansion under electrochemical conditions, hinders the practical and large-scale application in supercapacitor electrodes. Herein, a robust heterostructure of nanoscale nickel phosphide encapsulated in carbon microsphere (Ni 2 P @ CM) is constructed through the carbonization of spherical Ni-MOF, and followed by subsequent low-temperature phosphorylation. The MOF-derived uniform carbon layer on the Ni 2 P surface provides massive electron transport channels and physically restricts the volumetric expansion during electrochemical reactions , facilitating the electrode reaction kinetics and further leading to a good capacitive performance in high capacitance (1622 F/g at 1 A/g), long-term cyclic stability (75.2% capacitance retention after 8000 cycles at 20 A/g), and high rate capability. Furthermore, asymmetric SCs based on Ni 2 P @ CM and AC exhibit a high capacitance of 135.4 F/g at 0.5 A/g, and a remarkable energy density of 47.46 Wh/kg at a power density of 0.397 kW/kg with the excellent cyclic property. These results demonstrate that the methodology is highly promising in the design and construction of Ni 2 P/carbon hybrid electrodes, revealing an attractive candidate electrode material in high-property energy-storage devices.
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Journal of Environmental Chemical Engineering
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2022
·
IF 7.968
Pan Ma,Meili Ding,Wei Rong,Xi Liu,Jianfeng Yao
The synergistic catalysis involving multiple active sites provides a promising method for improved catalytic activity . In this work, we developed a gentle acetic acid-assisted polyhydroxy acid modification strategy to regulate the coordination environment of a zirconium-based MOF , UiO-66. D -gluconic acid with multiple hydroxyl groups is selected to replace the acetic acid coordinated at the metal nodes of UiO-66 via competitive coordination, allowing for the coexistence of hydrogen bonding donors and Lewis acid sites. The effect of acetic acid and D -gluconic acid separately as modulator and modifier agent to produce linker defects on catalytic properties of UiO-66 was investigated in the cycloaddition of carbon dioxide (CO 2 ) with epichlorohydrin. It was demonstrated that the activity of UiO-66 can be tuned by the amount of D -gluconic acid. Remarkably, the resultant UiO-66-GA-1200, which is modified with 1200 μL of D -gluconic acid, achieves a high catalytic yield for CO 2 cycloaddition of epichlorohydrin under 1 bar CO 2 and 60 °C. In contrast of pure UiO-66, UiO-66-GA-1200 shows admirable catalytic activities (92–94% yield) even after exposure to humid environment or in simulated flue gas . This work provides a novel method for constructing MOF-based solid acid catalysts and casts a new light on the development of practical CO 2 utilization.
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Catalysis Science & Technology
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2022
·Vol. 12
·期 23
·7057-7064
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IF 6.177
Lin Cheng,Changchang Wu,Huifang Feng,Hong Liu
2D MOFs show great potential in photocatalysis owing to their ultrathin thickness, large surface area and highly accessible active sites. Nevertheless, studies applying 2D MOFs as photocatalysts are very limited, especially for photocatalytic CO2 reduction. In this paper, a novel 2D/2D Co-PMOF/GR heterojunction was successfully constructed by coupling a 2D cobalt porphyrin-based MOF (Co-PMOF) and graphene (GR). The resultant Co-PMOF/GR composites could efficiently reduce CO2 to CO and CH4 under visible-light illumination without any assistance of a sacrificial agent and photosensitizer. When the content of GR was 10 wt%, the Co-PMOF/GR composite presented an optimum catalytic performance. The maximum yields of CO and CH4 over the Co-PMOF/GR composite reached 20.25 and 1.61 μmol g−1 h−1, respectively, which were 2.84 and 2.44 times those over pristine Co-PMOF. The enhanced catalytic efficiency was due to the synergy of higher light harvesting, enhanced CO2 absorption and efficient charge migration within the conductive and intimate 2D heterostructure. This study offers a new idea for the fabrication of highly active 2D MOF-based photocatalysts for solar energy conversion.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2022
·
IF 10.319
Yaokun Fu,Lu Zhang,Yuan Li,Sanyang Guo,Zhichao Yu,Wenfeng Wang,Kailiang Ren,Qiuming Peng,Shumin Han
The introduction of the heterogeneous catalysts with high activity can significantly improve hydrogen storage performance of MgH 2 , therefore, in this paper, we synthesize a carbon-supported transition metal compound, FeCoS@C derivative from ZIF-67, by utilizing the in situ formed C dispersive multiphase Mg 2 Co, α-Fe, Co 3 Fe 7 , and MgS to implement catalysis to MgH 2 . Noteworthily, MgH 2 -FeCoS@C rapidly absorbs 6.78 wt% H 2 within 60 s at 573 K and can also absorb 4.56 wt% H 2 in 900 s at 473 K. Besides, the addition of FeCoS@C results in decreasing of the initial dehydrogenation temperatures of MgH 2 from 620 to 550 K. The dehydrogenation activation energy of MgH 2 decreases from 160.7 to 91.9 kJ mol –1 . Studies show that the Mg 2 Co, α-Fe, and Co 3 Fe 7 act as “hydrogen channels” to accelerate hydrogen transfer due to the presence of transition metals, and MgS with excellent catalytic effect formed from MgH 2 -FeCoS@C provides a strong and stable catalytic effect. Besides, the carbon skeleton obtained by the carbonization of ZIF-67 not only serves as a dispersion for the multiphase catalytic system, but also provides more active sites for the catalysts. Our study shows that the multiphase and multiscale catalytic system provides an effective strategy for improving the hydrogen storage performance of MgH 2 .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Pingping Tan,Rongwei Gao,Yawei Zhang,Ning Han,Yinzhu Jiang,Maowen Xu,Shu-Juan Bao,Xuan Zhang
Hydrogen production from water electrolysis is severely restricted by the poor reaction kinetics of oxygen evolution reaction (OER). In this work, a series of two-dimensional (2D) composites MOF/Ti 3 C 2 T x (the MXene phase) were fabricated by electrostatically directed assembly and used as catalysts for OER. The obtained composite materials exhibit enhanced electrocatalytic properties, thanks to the ultrathin 2D/2D heterostructure with abundant active sites in Co2Ni-MOF and the high electronic conductivity of Ti 3 C 2 T x . Among all the catalysts, Co2Ni-MOF@MX-1 achieved the best oxygen evolution performance with the lowest Tafel slope (51.7 mV dec −1 ) and the lowest overpotential (265 mV on carbon paper) at the current density of 10 mA cm −2 . These results demonstrated that the synthesis of 2D composite materials by electrostatically directed assembly could be a feasible and promising method for the preparation of 2D heterostructure catalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Xuan-Ting He,Bo-Yu Li,Jia-Xiang Liu,Wen-Quan Tao,Zhuo Li
The surface chemical composition and building unit structures of membrane are the key factors to realize highly-efficient oil–water separation. Here we report the synthesis of Cu-CAT-1 metal–organic frameworks (MOFs) with unique two-dimensional (2D) hierarchical structures grown directly on copper mesh (Cu-CAT-1@CM) for oil–water separation. The Cu-CAT-1@CM membrane with micro/nano- architecture exhibits robust superhydrophilicity and underwater superoleophobicity characteristics, allowing gravity-driven oil–water separation by achieving ultrahigh flux up to 329 kL∙m −2 ∙h −1 . The membrane shows excellent separation performances by testing various oils, particularly actual crude oil and xylene, which are considered as the notorious pollutants in the water. The residual oil contents of six samples are all less than 24.6 mg∙L -1 . The mechanism analysis demonstrated that the appropriate hierarchical structures of the membrane surface is the code for the extreme wettability that remarkably improved the separation efficiency. Moreover, such a membrane with high performance can be readily synthesized by electrochemical method at room temperature in only 20 min, which shows the advantages of facile and environmentally friendly fabrication process as well as low cost. Overall, the membrane with energy-saving of gravity-driven and ultra-high permeability allows the rapid separation of oil–water mixture, showing the potential applications for resolving the problem of oil pollution.
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ChemSusChem
·
2022
·Vol. 15
·期 19
·e202201386
·
IF 9.14
Zhenzhen Zhou,Xiao Liu,Jian-Gong Ma,Peng Cheng
Graphical It's a trap ! Through a new “ligand-in-dimer-trap” strategy, the host–guest composites featuring metal–organic framework-encapsulated binuclear NHC−Co complex ( Co 2 @MOF) is prepared and used as a double-sites catalyst, which combines and surpasses the advantages of homo- and heterogeneous catalysis and exhibits prime performance in converting CO 2 into widely used formamides under ambient conditions. Environmental problem caused by carbon emission is of widespread concern. Involving CO 2 as C 1 resource into chemical synthesis is one of the most attractive ways for carbon recycling. Herein, the first example of host–guest composites featuring metal–organic framework (MOF)-encapsulated binuclear N-heterocyclic carbene (NHC) complex, Co 2 @MIL101, was developed with the molecularly dispersed [Co(IPr)Br] 2 (μ-Br) 2 ( Co 2 ) loading in the cage of MIL-101(Cr) via a “ligand-in-dimer-trap” strategy, which was comprehensively investigated through various techniques including synchrotron X-ray absorption, electron microscopy, X-ray diffraction, solid-state nuclear magnetic resonance spectroscopy, and others. The noble-metal-free double-sites catalyst Co 2 @MIL101 exhibited promising stability, activity, efficiency, reusability, and substrate adaptability for converting CO 2 into various formamides with amines and hydrosilanes and achieved the best performance for one of the most useful formamides, N -methyl- N -phenylformamide (MFA), among the recyclable catalysts at ambient conditions, providing a reliable approach to successfully unify the advantages of both homo- and heterogeneous catalysts. Density functional theory calculations were applied to illustrate the superior activity of the binuclear NHC complex center as double-sites catalyst toward the activation of CO 2 .
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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Zheng Shen,Deyan Xu,Guangxian Wang,Lingjun Geng,Rui Xu,Guanjie Wang,Yemin Guo,Xia Sun
For the visual detection of four organophosphorus pesticides (OPs), a colorimetric aptasensor was developed based on aptamer-mediated bimetallic metal-organic frameworks (MOFs) nano-polymers. Fe-Co magnetic nanoparticles (MNPs) and Fe-N-C nanozymes were prepared based on pyrolytic reaction, and were labeled with broad spectrum aptamers and complementary chains of organophosphorus pesticides respectively. The hybridization of aptamers and complementary chains led to the formation of nano-polymers. In the presence of target pesticides, they competed with complementary chains for aptamers on Fe-Co MNPs, resulting in a large number of Fe-N-C nanozymes signal labels being released into the supernatant. Fe-N-C nanozymes showed similar activity to peroxidase and catalyzed the 3,3′,5,5′-tetramethylbenzidine-hydrogen peroxide (TMB-H 2 O 2 ) color system to turn the solution blue-green under mild conditions. The magnetic probes had good selectivity and sensitivity, and were easily separated by magnetic absorption . The sensor functioned well under optimal conditions, demonstrating good stability and specificity for four pesticides: phorate, profenofos , isocarbophos and omethoate, and the detection limits of four pesticides were as low as 0.16 ng/mL, 0.16 ng/mL, 0.03 ng/mL and 1.6 ng/mL respectively, and the recovery rate of OPs residue in vegetable samples was satisfactory. The work described here provided a simple, rapid and sensitive way to construct a biosensor .
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Minjun Liu,Ying Liu,Xinru Liu,Chengcheng Chu,Ducheng Yao,Shun Mao
Metal organic framework (MOF)-derived materials normally have three-dimensional (3D) structure, while little attention has been paid to two-dimensional (2D) MOF-derived materials with high catalytic activity. Nevertheless, the underlying agglomeration and metal leaching issues of 2D MOF-derived catalysts hinder their real applications. In this work, we report a bimetallic nanocomposite (Ni-Fe-C-600-acid/GO) derived from 2D Ni-Fe-MOF and graphene oxide (GO) network. Employing Ni(0) and Fe 3 O 4 as active site, the Ni-Fe-C-600-acid/GO shows high efficiency in peroxydisulfate (PDS) activation for the removal of p-chloroaniline (PCA), and the catalyst/PCA dosage ratio (0.8) is substantially lower than those of the previous studies (3.9–156.9). The prepared catalysts demonstrate high catalytic activity over a wide pH range of 3–9 and maintain high efficiency after five cycles with good tolerance to inorganic anions. The singlet oxygen is identified as the predominant active species and relatively weak contributions from sulfate free radicals and hydroxyl radicals are confirmed. This catalysis system presents new insights in 2D MOF-derived catalysts in advanced oxidation processes .
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Bingzhe Jia,Huailin Yang,Lei Wang,Zhiqi Zhao,Xinming Wu
Compared with most transition metal based electrode materials, 2D M n+1 X n T x has high conductivity and good solvent compatibility. However, its low energy density hinders its application as supercapacitior electrode for electrochemical energy storage applications. Herein, the interface-pillared of Fe-MOF (MIL-100(Fe)) onto Ti 3 C 2 T x MXene layer, which provide rich electrochemical active sites, is achieved, and the MOF nanospheres with MXene nanosheets are subsequently converser into three dimensional multilayer porous nanostructures through the chemical bond couping. Therefore, the MOF nanospheres are anchored between the nansheets of MXene, enabling the fast ion transportation in the three dimensional nanostructures. Menanwhile, the MOF nanospheres prevent the aggregation of MXene nanosheets, and the laminar structure is maintained for more redox reaction sites within the hybrid electrodes through fast charge–discharge cycles. As a result, the MIL-100(Fe)/Ti 3 C 2 T x MXene electrode displays superior energy density (85.53 Wh kg −1 ), which is much higher than the other MXene-based electrodes as far as we know. This design strategy of 2D hybrid electrodes opens up a new way for the commercial application of high perfermance supercapacitor.
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