CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Cheng Liu,Mengning Chen,Yueling Chen,Qi Chen,Jionghua Wu,Sen Lin,Ling Wu,Jimmy C. Yu
This work develops a series of bimetallic MIL-68(InFe) MOF nanorods (NM(In 1-x Fe x )) mimicking the nitrogenase for biomimetic photocatalytic N 2 fixation. The partial substitution of In 3+ with Fe 3+ leads to the electron redistribution from In 3+ to Fe 3+ , generating electron-poor In 3+ (In (3+δ)+ ) sites and electron-rich Fe 3+ (Fe (3–δ)+ ) sites as an electron acceptor–donor combination to promote the N 2 activation by a π back-donation mechanism. The smaller size of the nanorods further provides more accessible active sites than the bulk counterpart. In cooperation with the H + released from the H 2 O, the activated N 2 molecules were reduced by photogenerated electrons to give NH 3 . The optimal sample NM(In 0.90 Fe 0.10 ) exhibited the highest NH 4 + production rate of 30.8 µmol·h −1 ·g −1 without any sacrificial agent, attributed to the presence of abundant In/Fe bimetallic sites for N 2 activation and enhanced charge mobility. This work provides new insights into rational design for artificial N 2 fixation systems by mimicking natural nitrogenase.
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ACS Applied Materials & Interfaces
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2024
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IF 8.3
Liwei Hou,Xinyue Xu,Zhoujun Zhong,Fengchun Tian,Li Wang,Yi Xu
The demand for the detection of ultralow concentrations of ammonia gas is growing. A bimetallic metal–organic framework (MOF) comprising Prussian blue analogs (PBAs) was used to achieve highly sensitive and stable detection of ammonia gas at room temperature in this study. First, PB was enriched by using ammonia for improved gas sensing properties. Second, a sensitive membrane with more vacancies was formed by partially replacing Fe3+ with Cu2+ through a cation-exchange strategy. Finally, a capacitive sensor was developed for ultralow-concentration ammonia detection using a Cu–Fe PBA sensitive membrane and interdigitated electrodes (IDEs). To investigate the adsorption efficiency of the designed composite sensitive film for ammonia, PBAs nanoparticles were deposited on a quartz microcrystal balance (QCM) via cyclic voltammetry and a hydrothermal method. Approximately 10 ppm of ammonia was adsorbed under 1 atm by the Cu–Fe PBA film prepared using a reaction time of 36 h, and the adsorption efficiency was measured to be 2.2 mmol g–1 using the QCM frequency response. The Cu–Fe PBAs were also tested using scanning electron microscopy, transmission electron microscopy, X-ray diffraction, and Brunauer–Emmett–Teller theory. The introduction of Cu2+ ions significantly increased the specific surface area of Cu–Fe PBAs MOF, and the number of adsorption sites for ammonia also increased; however, its skeleton structure remained similar to that of PB. Then, the capacitive sensor based on Cu–Fe PBA sensitive membrane and IDE was fabricated and the gas sensing detection device was established for ammonia detection. Overall, the developed capacitive sensor exhibits a linear response of 75–1000 ppb and a detection limit of 3.8 ppb for ultralow ammonia concentrations, which makes it superior to traditional detection methods and thus allows excellent application prospects.
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PubMed
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JOURNAL OF MEMBRANE SCIENCE
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2024
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IF 8.4
Jiangnan Wang,Long Li,Jinli Zhang,Xueqin Li
The chitosan (CS)-grafted UiO-66-NH 2 (U6N) (CSGUN) was synthesized and incorporated into Pebax matrix to fabricate mixed matrix membranes (MMMs) for boosting CO 2 transport. The excellent CO 2 separation performance was exhibited for MMMs due to the following reasons: U6N with the suitable porosity and abundant CO 2 transport carriers can provide a unique “expressway” for CO 2 to boost CO 2 transport through MMMs. The grafting CS in CSGUN can connect Pebax (regular roads) and U6N (expressway), acting as an “on-ramp” between them to enrich CO 2 and guide CO 2 through U6N in an orderly manner. Thus, the constructed “on-ramp” and “expressway” in MMMs can improve CO 2 separation performance. Furthermore, the CS-MOF networks were formed in MMMs through using CS molecular chains to connect U6N for enhancing CO 2 separation performance of MMMs. Therefore, Pebax/CSGUN MMMs exhibited the excellent CO 2 separation performance with the CO 2 permeability of 558 ± 7 Barrer and the CO 2 /CH 4 selectivity of 37.5 ± 0.7. The study indicated that MMMs with CS-MOF bridged networks had great potential for boosting CO 2 transport by combining “expressways” and “on-ramp”.
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RSC Advances
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2015
·Vol. 5
·期 110
·90265-90271
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IF 3.84
Lili Li,Xingyue Li,Lunhong Ai,Jing Jiang
The earth-abundant metal phosphides have emerged as new and active alternatives for the precious metal platinum to electrocatalyze the hydrogen evolution reaction (HER) via water splitting. In this study, we report on the straightforward and controllable synthesis of various nanostructured cobalt phosphide assemblies through the direct chemical transformation of a Co-containing metal–organic framework (ZIF-67-Co) under mild phosphorization conditions. The resulting CoP nanoparticle assemblies (NPAs) and nanorod assemblies (NRAs) can be selectively produced by rationally tuning the calcination atmosphere. The CoP NRAs were found to be highly active for electrocatalytic hydrogen generation, which exhibited better performance than that of the CoP NPAs, as evidenced by their relatively low onset overpotential (∼86 mV), small Tafel slope (∼69 mV dec−1) and long-term stability in acidic media.
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JOURNAL OF MEMBRANE SCIENCE
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2016
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IF 5.557
Xiao-Hua Ma,Zhe Yang,Zhi-Kan Yao,Zhen-Liang Xu,Chuyang Y. Tang
A novel positively charged nanofiltration (NF) membrane was fabricated by incorporating metal-organic frameworks (MOFs) into chitosan polymeric matrix for enhanced removal of multivalent cations. The synthesized MOFs, NH 2 -MIL-101(Al) and NH 2 -MIL-101(Cr), could be homogeneously dispersed in the chitosan polymeric matrix. The morphologies of MOFs had a significant influence on the permeability of NF membranes. NF membrane filled with NH 2 -MIL-101(Al) with rod-like structure attained two times higher flux but similar rejection compared with that filled with NH 2 -MIL-101(Cr) with grainy structure. The effect of MOF loadings (NH 2 -MIL-101(Al)) on the membrane performance were evaluated by XRD , FTIR and SEM. These positively charged MOF/chitosan NF membranes were able to reject up to 93.0% of MgCl 2 , and the salt rejection followed the order of MgCl 2 >CaCl 2 >NaCl>Na 2 SO 4 .
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NEW JOURNAL OF CHEMISTRY
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2024
·Vol. 48
·期 12
·5311-5325
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IF 2.7
Pengna Huang,Xianjin Qi,Xiaoxu Duan,Wenqi Jiang,Nina Yang,Gang Zhi,Jianhua Wang
The low adsorption capacity of metal–organic frameworks (MOFs) limits their practical application in high-arsenic wastewater for adsorption owing to their insufficient active sites and suboptimal pore structure. Accordingly, we employed a one-pot hydrothermal method to synthesise mixed-metal La/Zr-MOFs with complex pore structures. Notably, the material possesses both La-BDC and Zr-BDC morphology features and integrates the advantages of monometallic MOFs through a framework symbiotic structure. This complex pore structure promotes the migration and diffusion of arsenic ions in the pore channels, improving the adsorption kinetics. Moreover, mixed-metal functional centres can expose more active sites, which is conducive to enhancing adsorption capacity. Experiments showed that mixed-metal La/Zr-BDC-4 rapidly reached adsorption equilibrium in 60 min, corresponding to a maximum adsorption amount of 694 mg g−1. Batch adsorption experiments and X-ray photoelectron and Fourier-transform infrared spectroscopy analyses revealed that mixed-metal La/Zr-BDC-4 arsenates tend to form internal complexes with each other, suggesting that As(V) adsorption is an exothermic and spontaneous chemisorption process. After four adsorption–desorption cycles, the material maintained an arsenic removal rate of 85%, exhibiting its potential application in wastewater treatment. Therefore, the mixed-metal La/Zr-BDC-4 MOF is a promising material for wastewater treatment.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Shouxin Zhu,Can Sun,Zijie Fang,Mingli Qin,Zhexiao Zhu,Jingyi Qu,Hui Zheng
Facing the escalating issue of antibiotic pollution and the emergence of bacterial resistance in water ecosystems, photocatalytic technology has been widely studied as one of the efficient methods to remove antibiotics in aquatic ecosystem. Herein, the bimetallic organic framework materials Cu/Zn-BTC were synthesized with varying proportions of copper and zinc as metal joints and 1,3,5-phthalic acid as organic ligands. Subsequently, the zinc elements within the MOF were eliminated through high pyrolysis to obtain carbon materials derived from Cu/Zn-BTC (referred to as 1.3CZC, 1.4CZC, and 1.5CZC based on the copper-to-zinc ratio). Notably, the presence of different valence copper species facilitated to form type II heterojunction within MOF-derived carbon materials, where internal Cu 0 /Cu + species combined with oxygen vacancies to create localized bands that prolonged the lifetime of photogenerated carriers and enhanced photocatalytic activity. X-ray photoelectron spectroscopy, Brunauer-Emmett-Taylor and other characterization methods were used to analyze the difference in structure and performance of different catalysts. 1.4CZC showed excellent performance, upon exposure to visible light for 30 min, the removal rate of tetracycline significantly increased to an impressive 92.4 %, while extending the exposure time to 60 min further improved the removal rate of ciprofloxacin to approximately 82.6 %. It provides a highly efficient antibiotics removal pathway by MOF-derived carbon materials.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Dandan Hao,Ping Wang,Ju Liu,Huanhui Zhan,Tiantian Zhou,Bo Fu
MOF-199 is considered to be an excellent CO 2 adsorbent owing to its substantial specific surface area, suitable pore structure and abundant sorption sites. However, powdered MOF-199 is prone to agglomeration and has poor recyclability. Herein, we proposed a MOF-199-based adsorbent by combining the MOF synthesis process with traditional papermaking process. Through such a design, MOF-199 particles are adhered on the surface of wood pulp fiber. The sufficient hydroxyl groups and electrostatic forces of cellulose facilitates the homogeneous and tight adhesion of MOF crystals. The optimal MP-4 sample demonstrated a high CO 2 adsorption capacity (1.80 mmol·g ‐−1 at 25 °C) and good CO 2 /N 2 selectivity (30.06). Moreover, the composite sorbent can be easily regenerated. The adsorption mechanism was analyzed by the density functional theory approach. The simulation results showed that the carboxyl functional groups with a large number of oxygen atoms and active metal sites are the key to boost the CO 2 adsorption performance.
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
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2024
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IF 4.3
Tiantian Zhou,Ju Liu,Huanhui Zhan,Ping Wang,Kefan Chao,Muhua Chen,Junjie Zheng,Bo Fu
Herein, through in-situ growing BiVO 4 nanosheets on CAU-17 (Bi-based metal-organic framework) with a hydrothermal method , a BiVO 4 /CAU-17 Z-scheme heterojunction photocatalyst is fabricated. The composite manifest that the BiVO 4 is well dispersed on CAU-17 while CAU-17 surface transforms into a well-defined sheet-like morphology. As a result of the construction of Z-scheme heterojunction , in contrast to pure BiVO 4 and CAU-17, composites have excellent photodegradation ability for Rhodamine B (RhB) and Congo Red (CR), and achieve synergistic removal of pollutants in the RhB/CR binary system, indicating it has great potential in the treatment of dye wastewater. At the same time, it still maintains outstanding photocatalytic performance after five cycles of testing, demonstrating superior reusability and durability.
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JOURNAL OF RARE EARTHS
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2024
·
IF 5.2
Jinxiu Sheng,Xiao Liu,Fengyi Liu,Quanqing Xu,Aixin Zhu,Xufeng Zhang
Metal-organic frameworks (MOFs) usually exist in the state of powder or crystal. When they are exposed to hydrophilic solvents, their structure will change and become unstable. Therefore, it is a challenge to construct MOF materials with tunable mechanical properties. Herein, we report in-situ growth lanthanide metal-organic framework (LnMOF) in sodium alginate (SA) and polyvinyl alcohol (PVA) hydrogel matrix. The prepared composite hydrogel not only displays characteristic lanthanide narrow-band emission under ultraviolet light, but also demonstrates excellent mechanical properties. The addition of LnMOF significantly enhances the compressive strength of the hydrogel (from 0.75 to 7.32 MPa). Furthermore, the composite hydrogel shows highly selective recognition of glutaraldehyde and gaseous formaldehyde at room temperature. The detection limits (LOD) of SP-EuMOF for glutaraldehyde and formaldehyde are 0.27 and 0.22 ppm, respectively. Based on these results, the LnMOF composite hydrogel is deemed to have significant potential as a fluorescent sensor for both glutaraldehyde and formaldehyde detection.
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Journal of Cleaner Production
·
2025
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IF 10
Yating Ji,Weifeng Yang,Xiaoyan Li,Zhuizhui Fan,Bi Xu,Zaisheng Cai
Metal-organic frameworks (MOFs) have emerged as a favored component in composites owing to their high porosity and synthetic tunability. However, loading MOF powders into a polymer matrix to form composites often relies on organic solvents and rigorous manufacturing processes. Here, we propose a biomimetic mineralized molecular engineering strategy, enabling robust, large-scale fabrication of MOF-fabric composites without organic solvents. This strategy allows MOF nodes to be embedded between highly elastic state polymer molecular chains, achieving strong physical anchoring. The preparation process realizes a significant reduction in carbon emissions (30%–50%) and high production efficiency (10 kg/h) while maintaining excellent fixation fastness, including resistance to washing (over 25 times), rubbing (over 100 times), and light (over 12 h). Furthermore, the applications of MOF-fabric composites in personal protective equipment are demonstrated, including organic gas adsorption, UV protection, and antibacterial. Our work provides a sustainable pathway towards the practical application of MOF-fabric composites.
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
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2024
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IF 4.3
Mohan Huang,Kun Zhao,Shuangyan Liu,Ang Bian,Lu Jiang,Dawei He,Jiaqi He,Yongsheng Wang
The design and development of microwave-absorbing materials with excellent performance hold significant importance in both civil and military fields. The combination of magnetic loss materials and dielectric loss materials can achieve complementary performance effects and regulate impedance matching. In this paper, spindle-like α-Fe 2 O 3 was synthesized using MIL-88A as a template, which was then composited with Ti 3 C 2 T x phase possessing excellent electrical conductivity to obtain Fe 2 O 3 /Ti 3 C 2 T x composites. Ti 3 C 2 T x can provide good conductance loss and dipole polarization relaxation, while the incorporation of Fe 2 O 3 between the layers of Ti 3 C 2 T x not only triggers the interfacial polarization effect but also increases layer spacing, thereby enhancing multiple reflection effects. Furthermore, the magnetic-dielectric synergies further optimize the impedance matching. Through the combined action of multiple mechanisms, the Fe 2 O 3 /Ti 3 C 2 T x composites (with a mass ratio of 1:3 for Fe 2 O 3 and Ti 3 C 2 T x ) exhibit a minimum reflection loss of −34 dB and an effective absorption bandwidth of 1.53 GHz at a thickness of 3 mm, as well as an effective absorption bandwidth of 2.805 GHz at a thickness of 1.5 mm. This paper presents a reference strategy for constructing highly efficient microwave absorbers derived from Metal-organic frameworks (MOFs) and MXene based on their outstanding properties.
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