JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2022
·Vol. 98
·期 4
·919-931
·
IF 3.709
Bixiu Song,Dajun Ren,Zhaobo Wang,Yongwei Huang,Xiaoqing Zhang,Shuqin Zhang,Xiangyi Gong,Wangsheng Chen
As a result of the poor mechanical properties of most metal–organic frameworks (MOFs), they are liable to dissociate in water and thus cannot maintain immobilized enzyme activity. In this paper, a magnetic porous carbon material (Fe-Cu-MPC) with good stability was prepared by high temperature carbonization using a bimetallic Fe-Cu-MOF precursor, and used to immobilize laccase by a simple and rapid adsorption-crosslinking method. Optimized by the response surface method, optimal conditions for the immobilization of laccase on Fe-Cu-MPC were obtained as follows: enzyme concentration 1.275 mg mL −1 , immobilization time 32 min, and pH 4.7. Under the optimal preparation conditions, the activity of the immobilized laccase obtained was 0.63 U mg −1 , with activity recovery of 63.13%. The enzyme loading was 189.03 mg g −1 and the immobilization yield was 74.13%. Compared with free laccase, Fe-Cu-MPC@Lac showed stronger tolerance to temperature and pH, and had better thermal stability and storage stability. The removal of BPA by immobilized laccase was studied, showing that the removal effect of Fe-Cu-MPC@Lac on BPA was much higher than that of free laccase. Within 5 h, the BPA removal amount of Fe-Cu-MPC@Lac (0.34 mmol g −1 ) was two-fold that of free laccase (0.14 mmol g −1 ), and the BPA removal rate reached 41.35% after ten cycles. Finally, based on the intermediates identified by gas chromatography–mass spectrometry, two possible degradation pathways of BPA were proposed. Studies have shown that Fe-Cu-MPC is an excellent carrier and Fe-Cu-MPC@Lac has great potential in the treatment of BPA containing wastewater. © 2022 Society of Chemical Industry (SCI).
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 23
·7057-7064
·
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.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2023
·
IF 4.6
Wei He,Yucheng Liu,Zhi Huang,Wenwen Tu,Rui Liu,Mingyan Chen
A novel superhydrophilic and underwater superoleophobic material (MOF-5/PDA/SSM) with high flux, outstanding oil/water separation performance and durability was prepared. The stainless steel mesh (SSM) was modified by MOF-5 crystals and PDA. The introduction of MOF-5 can improve the hydrophilicity of SSM and achieve high water flux at the same time. PDA is a substance with strong adhesion which can be used as an effective bonding intermediate. The preparation strategy includes the self-polymerization of dopamine and the deposition of cubic clusters on SSM via hydrothermal reaction . The MOF-5 particles on the mesh are cubic hexahedral crystal with a uniform size diameter, which can trap water in the rough microstructure, forming a strong hydration barrier layer or composite water-solid interface on its surface, hindering the penetration of oil. The super-hydrophilicity and underwater superoleophobicity of the modified meshes were introduced by pre-wetting surface. The FTIR, XRD , XPS and SEM characterizations demonstrated that the successfully growth of MOF-5 and a rough structure was obtained on the mesh. The special wetting and the robustness of the fabricated mesh led to the outstanding separation efficiency (up to 99.5%), excellent recyclability (about 20 cycles) and high water flux (53.9 k L m −2 h −1 ). The mesh also showed remarked water flux and various oil/water mixtures separation performance. Particularly, the successfully prepared materials were found to be significant stable under various physical and chemical extremes environments, including maintain UWOCA>150 under acid/alkali media, marvelous performance after 120 min of continuous separation and high anti-oil intrusion pressure. The combination of metal organic framework and stainless steel mesh may provide a candidate application to effective oil-water separation.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Guihua Xu,Qiaoning He,Kexin Huang,Ying Wang,Chun Pu,Ganggang Chang,Xiaoyu Yang
Benefiting from their unique properties including faster mass transfer, more exposed active sites and large molecule recognition, hierarchically porous metal–organic frameworks (HP-MOFs), in the form of ultrasmall nanoparticles (NPs) and having self-assembled interparticle mesopores, have garnered greater attention in recent years that given to typical MOFs. However, controllable synthesis of HP-MOFs on the nanoscale remains a significant challenge. Herein, for the first time, a facile top-down acid etching strategy was developed to fabricate a series of nanosized (∼15 nm) mesoporous MOF, HP-UiO-66-NH 2 (Hf). The sizes of mesopores in this material can be effectively tuned by simply controlling the concentration of propionic acid (PA) utilized in the preparation solution. Interestingly, the generated mesoporous HP-UiO-66-NH 2 (Hf) has excellent stability and can be readily constructed by using PA etching solution that has been recycled at least four times. Remarkably, HP-UiO-66-NH 2 (Hf) displays a high size-selectivity for adsorption of enzymes. Associated with its highly matched mesopore size, the nanocomposite generated by complexation with glucose oxidase (GOD), [email protected] 2 (Hf) has a higher catalytic activity and a significantly enhanced stability (recycled at least 7 times) in promoting oxidation of glucose compared to its MOF counterpart, [email protected] 2 (Hf) and native GOD .
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
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.
✓ 已验证
产品关联
DOI
高影响因子
CARBOHYDRATE POLYMERS
·
2022
·
IF 10.723
Yucheng Song,Hui Li,Tianhang Shan,Peipei Yang,Songwei Li,Zhong Liu,Chuntai Liu,Changyu Shen
In this study, a composite hydrogel with a low swelling ratio, excellent mechanical properties, and good U (VI) adsorption capacity was developed by incorporating a metal-organic framework (MOF) with a poly (acrylamide- co -acrylic acid)/chitosan (P(AM-co-AA)/CS) composite. The CS chain, which contains NH 2 , reduces the swelling ratio of the hydrogel to 4.17 after 5 h of immersion in water. The coordinate bond between the MOF and carboxyl group on the surface of P(AM-co-AA)/CS improves the mechanical properties and stability of P(AM-co-AA)/CS. The U(VI) adsorption capacity of P(AM-co-AA)/CS/MOF-808 is 159.56 mg g −1 at C 0 = 99.47 mg L −1 and pH = 8.0. The adsorption process is well fitted by the Langmuir isotherm and pseudo-second-order model. The P(AM-co-AA)/CS/MOF-808 also exhibits good repeatability and stability after five adsorption–desorption cycles. The uranium adsorption capacity of the developed adsorbent after one month in natural seawater is 6.2 mg g −1 , and the rate of uranium adsorption on the hydrogel is 0.21 mg g −1 day −1 .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Z.W. Zhu,Q.R. Zheng
Comparisons were made between the samples mechanochemically (MOF-5(M)) and solvothermally (MOF-5(S)) prepared for the development of efficient hydrogen storage medium. Synthesized samples were undergone structural characterization as well as adsorption equilibrium measurements of hydrogen at temperature-pressure range 77 K–87 K and 0.1–10 MPa. Grand Canonical Monte Carlo (GCMC) simulations were further conducted to study the behaviors of hydrogen molecules adsorbed on MOF-5. It shows that, besides the advantage of large scale synthesis and a lower cost, mechanochemical method respectively brings about 207% and 90.5% increments in the specific surface area and the maximum excess adsorption capacity of hydrogen at 77 K within pressure range 0–10 MPa. Results also reveal that the crystal within MOF-5(M) is regular and distributing uniformly with a mean size only one tenth of that of the MOF-5(S); at 77 K within pressure range 0–10 MPa, Toth equation can predict the adsorption equilibrium data of hydrogen on two MOF-5 samples with a mean relative error less than 1.5%. It suggests that MOF-5(M) is more promising for hydrogen storage by adsorption for practical applications.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Juan Li,Xiaolei Jiang,Mingyuan Zhu,Bin Dai
Oxidative desulfurization (ODS) is a promising technique for obtaining clean fuel. Designing and researching zirconium-based metal–organic frameworks (Zr-MOFs) with bimetallic catalytic sites are encouraging for its further development. In this study, Cu(Ⅰ)-MOF-808 was successfully synthesized through anchoring Cu + in MOF-808. Pyridine infrared spectrum (Py-IR) and NH 3 temperature programmed desorption (NH 3 -TPD) confirmed that Lewis (L) acid sites existed in the synthesized material. Cu(Ⅰ)-MOF-808 was applied into the ODS reaction, during the reaction process, L acid sites adsorbed sulfide, Cu + sustainably provided electron to H 2 O 2 to formed into •OH, with the synergistic effect of L acid sites and Cu + , 99.9 % of the dibenzothiophene was oxidated to dibenzothiophene sulfone in 120 min. In addition, the cyclic experiment indicated that the ODS performance of Cu(Ⅰ)-MOF-808 was maintained at 99.2 % after 12 times recycling. Powder X-ray diffraction (PXRD) spectra indicated the framework structure of the reused catalyst was stable, inductively coupled plasma optical emission spectrometer (ICP-OES) result displayed no metal ions (Zr, Cu) leaching after the ODS reaction, which also proved the catalytic stability of the Cu(Ⅰ)-MOF-808.
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 26
·39427-39440
·
IF 5.19
Wang Cheng,Li Airong,Ma Yuling,Qing Shenglan
Due to the increasingly serious environmental problems caused by the combustion of sulfides in fuel, deep desulfurization of fuel became particularly urgent. Herein, the catalyst (PMA@MOF-808) of the Zr-based metal–organic framework (MOF-808) encapsulating phosphomolybdic acid (PMA) was prepared via a one-pot hydrothermal method. Besides, the formate ions of PMA@MOF-808 were removed by posttreatment with methanol, resulting in formate-free PMA@MOF-808-H catalysts with unsaturated open metal sites. The as-synthesized catalysts were systematically characterized by XRD, FT-IR, SEM, BET, TGA, 1 H NMR and XPS. The catalysts were also applied in catalytic oxidation desulfurization of fuel. The results indicated that the introduction of PMA and the removal of formate ions can improve the desulfurization performance of catalysts. Formate-free 0.2-PMA@MOF-808-H catalyst can reach 100% desulfurization rate for DBT. Besides, the kinetic properties were studied, and the apparent activation energy was 29.34 kJ/mol. Graphical abstract
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yamin Chai,Yanjia Zhang,Lichun Wang,Yunzheng Du,Biao Wang,Nan Li,Mengya Chen,Lailiang Ou
Metal-organic framework (MOF)-based composite hydrogel microspheres (MOF/hydrogel) are one of the most promising adsorbents for high-efficiency wastewater treatment. However, conventional MOF/hydrogel synthesis methods involve simple blending, which inevitably results in poor particle-polymer matrix interactions and particle agglomeration. In this work, inspired by the symbiotic relationships in nature, we successfully constructed a three-dimensional zeolitic imidazolate framework-8 (ZIF-8)/polysaccharide (sodium alginate-kappa-carrageenan, SC) hydrogel beads, denoted a ZIF-8/SC, via phase inversion based on an in situ one-pot method for nanosized ZIF-8 assembly with polysaccharide matrices. Notably, our adsorbent demonstrated excellent mechanical performance with a stress and an elastic modulus of 1.14 MPa and 1.70 MPa respectively, as well as exhibited the good stability after immersed in water at room temperature for 7 days. Furthermore, benefiting from the uniform distribution and interfacial compatibility of ZIF-8, ZIF-8/SC exhibited a good adsorption capacity value of 2887 mg g −1 , resulting in better removal performance than most MOF-based or natural polymer-based ciprofloxacin adsorbents. Moreover, the adsorption processes followed the pseudo-second-order and Langmuir isotherm models. In addition, we fabricated a ZIF-8/SC column for practical dynamic separation, which could treat 1500 mL of CIP solution in tap water. The experimental characterization results revealed that the adsorption mechanism involved electrostatic, π-π stacking, and hydrogen-bonding interaction, as well as coordination effects between CIP and the adsorbent. This study could offer a promising strategy for designing uniform MOF-based composite hydrogel adsorbents for pharmaceutical wastewater treatment with appealing application prospects.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）