Materials Today Energy
·
2020
·
IF 5.604
Kuofeng Xu,Huayuan Bao,Chaoyun Tang,Kristina Maliutina,Fengjiao Li,Liangdong Fan
The development of non-platinum electrocatalysts for the quick oxygen reduction reaction (ORR) is highly desirable in electrochemical energy conversion technologies such as fuel cells and metal-air batteries. In this work, we synthesize Fe 3 O 4 /Fe–N–C-CNT (FeNC) using Fe 3+ adsorbed ZIF-8 as a chemical precursor that is obtained with a green and sustainable procedure. FeNC possesses impressive ORR activities, stability and selectivity over that of the commercial Pt/C electrocatalyst in alkaline media, and demonstrates a better peak power density of 118.05 mW cm −2 over that with Pt/C cathode and quicker reaction kinetics when integrated as air electrode catalyst into a primary zinc-air battery. In-depth investigation confirms that the presence of Fe 3 O 4 increases the wettability of carbon-based composite that promotes the adsorption of the dissolved O 2 in the electrolyte solution and extends the triple-phase boundary for ORR, and also protect the active site of Fe–N–C from poisoning. This work sheds light on a sustainable method to synthesize highly efficient non-precious metal-based electrocatalyst from metal-organic-framework precursors and understanding the reaction mechanism of the ORR process for efficient chemical energy to electricity conversion.
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Shan Peng,Haobo Ma,Xiaoyan Hao,Ruimeng Han,Xiaoyu Ji,Lei Wang,Yanyan Fang,Kyongjin Pang,Kwon Il-Ho,Xiaoxin Chen
Oil spills and micropollutants have become thorny environmental issues , posing serious threat to ecosystem and human health. To settle such dilemma, this study successfully constructed a robust and environmentally-friendly MOFs-COFs hybrid-based membrane (FS-50/COF(MATPA)-MOF(Zr)/PDA@PVDF) for the first time through solution synthesis and solvothermal method, combined with surface modification of FS-50 molecule. Importantly, we employed a simple two-step strategy to obtain the high-aspect-ratio MOFs fibers: (1) solvent regulation to generate smaller needle-like whiskers during the in-situ growth of MOFs on COFs; (2) high pressure induced directional crystallization in filtration process. The introduction of polydopamine (PDA) greatly improved the adhesion between coating and PVDF membrane. The in-situ growth of high length-diameter ratio MOFs fibers on blocky COFs greatly enhanced the specific surface area of MOFs-COFs hybrid, thus provided sufficient absorption sites. The functional groups of FS-50 endowed the hybrid membrane with superhydrophilicity and superoleophobicity, which facilitated to selectively penetrate water molecules and repel non-polar pollutants. The separation efficiency and decontamination mechanism of hybrid membrane to the simulated oily wastewater (containing various MPs , dyes, and pesticides) were investigated through experiments and theoretical calculations. The hybrid membrane could selectively and synchronously adsorb various dyes (20 mg/L–120 mg/L, almost 100% removal) and pesticides (10 mg/L for DIF and TET, adsorption rates 93.2% and 90.9%, respectively) from oil-water emulsion (50 mL). The large-scale coated sponge (6 cm × 4.5 cm × 3 cm) could quickly achieve separation of oil-water mixture (almost 100%) with a water permeability of more than 162 L m −2 ·h −1 ·bar −1 , and simultaneously remove various MPs (PP-2000, PP-100, PE-2000, PS-100, 0.2 g/300 mL for each), Sudan Ⅲ (C 0 = 200 mg/L), and DIF (C 0 = 10 mg/L) from a simulant oily wastewater (300 mL), with the removal rates of almost 100% for MPs, 99.7% for Sudan Ⅲ, and 95.8% for DIF. Furthermore, we elucidated the removal mechanism of pesticide and dyes through simulating the theoretical adsorption energy and potential adsorption sites. The hybrid membrane not only provides a promising candidate for the removal of multiple pollutants from oil-water emulsion, but also opens a new strategy for achieving efficient and clean aquatic environment restoration.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Guowen Qian,Yuqian Mao,Yang Shuai,Zhikui Zeng,Shuping Peng,Cijun Shuai
Bioceramics have been extensively used to improve osteogenesis of polymers because of their excellent bone-forming capabilities. However, the inadequate interfacial bonding between ceramics and polymers compromises their mechanical properties . In this study, zeolitic imidazolate framework-8 (ZIF-8) was grown in situ on strontium carbonate (SrCO 3 ) to construct a core–shell SrCO 3 @ZIF-8, which was then added to poly- l -lactic acid (PLLA) to print a SrCO 3 @ZIF-8/PLLA composite scaffold using selective sintering technology. First, ZIF-8 characterized by its multiple organic ligands, forms a robust interface with PLLA. Second, SrCO 3 characterized by its negative zeta potential in solution, exhibits the ability to adsorb positively charged zinc ions . This, in turn, promotes the in situ growth of ZIF-8 on SrCO 3 , eventually achieving perfect bonding between the second phase and the PLLA matrix. Our findings indicated that the composite scaffold exhibited the highest compressive strength (21.93 MPa) and significantly promoted the osteogenic differentiation of mouse mesenchymal stem cells. Moreover, the in vivo results established that the SrCO 3 @ZIF-8/PLLA scaffold significantly accelerated bone regeneration efficiency in rat femur defects. The prepared scaffold, with its favorable mechanical properties and osteogenic activity, shows considerable promise for applications in bone repair.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·
IF 19
Mengqiu Huang,Lei Wang,Ke Pei,Bangxin Li,Wenbin You,Liting Yang,Gang Zhou,Jincang Zhang,Chongyun Liang,Renchao Che
Heterogeneous interface regulation plays an important role in tailoring the intrinsic electromagnetic (EM) properties for obtaining excellent EM wave absorption, which still faces huge challenge. In this work, bi-metal MOFs-derived ZnFe 2 O 4 –ZnO-Fe@C (ZZFC) microspheres with custom-built heterogeneous interfaces are successfully fabricated via a confined growth strategy. Bi-metal Fe–Zn–ZIF with tailored coordination structure and chemical bonding are first selected as the precursor template. After undergoing the annealing process, the metal Fe 2+ host is converted into magnetic Fe nanoparticles (NPs). The Zn 2+ host is transformed into semiconductor zinc oxide (ZnO) with increasing (101) crystal-oriented growth. At the same time, metal hosts Fe 2+ and Zn 2+ are further reacted to synthesize the zinc ferrite (ZnFe 2 O 4 ). Formed Fe nanoparticles catalyze organic ligands to constitute graphitized carbon layers, which confine the further growth of ZnFe 2 O 4 , ZnO, and Fe NPs. Combined with the well impendence and synergy absorption mechanism (magnetic loss, interface polarization, and conduction loss), optimized magnetic–dielectric ZnFe 2 O 4 –ZnO-Fe@C microspheres exhibit outstanding EM wave absorption with the minimum reflection loss −66.5 dB at only 2.0 mm thickness. Bi-metal MOF-derived magnetic–dielectric absorption materials with tailored heterogeneous interfaces provide a new sight to design an efficient EM wave absorption system.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Huanggen Yang,Pei Zhang,Qi Zheng,Muhammad Usman Hameed,Saleem Raza
The presence of pollutants in drinking water has become a significant concern recently. Various substances, including activated carbon, membranes, biochar, etc., are used to remove these pollutants. In the present study, a new composite comprising cotton fabric and a mixture of Metal-Organic Frameworks (MOFs) was synthesized and used as an adsorbent for eliminating pollutants from wastewater. At first, the UiO-66 MOFs were prepared by a simple method of reacting Zirconium (IV) chloride (ZrCl 4 ) and p-Phthalic acid (PTA) after successful preparation of UiO-66 then modified its surface with amino functional groups by reacting with APTES to obtain UiO-66-NH 2 . Moreover, the cellulose cotton fabric (CF) surface was modified with Polydopamine (PDA) and obtained CF@PDA. Further, with the help of EDC-HCl and NHS, the UiO-66-NH 2 grafted on the surface of the CF@PDA and finally obtained CF@PDA/UiO-66-NH 2 . In addition, the adsorption study was performed toward RhB dye and Pb(II) metal ion pollutants. The maximum adsorption toward RhB dye was 68.5 mg/g, while toward Pb(II) metal ions was 65 mg/g. In addition, the kinetic study was also conducted and the result favoured the Pseudo-second order kinetic study. The adsorption isotherm was also studied and the Langmuir model was more fitted as compared with the Freundlich model. Moreover, the material has excellent regeneration and recycling ability after ten cycles. The significant adsorption ability, the novel combination of cotton and MOFs, and the recycling feature make our material CF@PDA/UiO-66-NH 2 a promising potential absorbent material for wastewater treatment and even in other important areas of water research.
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ChemNanoMat
·
2023
·Vol. 10
·期 3
·e202300499
·
IF 3.8
Xiaozhu Zhao,Zongxin Li,Fengchuan Guo,Naipu He,Wen Li,Xuerui Zhao
Graphical The morphology of micelles in surfactant-free emulsion was regulated by adjusting the oil-water ratio and concentration of amphiphilic copolymer. Subsequently, polymer micelles served as templates to direct the assembly of ZIF-8 crystals in the surfactant-free emulsion to fabricate polymer/ZIF-8 composite materials (ZIF-8@CSP) with various structures. An amphiphilic chitosan-g-poly N-(3-dimethylaminopropyl) methacrylamide (CS-g-PDMAPMA, CSP) was proposed and synthesized by reversible addition-fragmentation chain transfer polymerization (RAFT), and further employed as emulsifier to construct a surfactant-free emulsion. The morphology of micelles in surfactant-free emulsion was regulated by adjusting the oil-water ratio and concentration of amphiphilic copolymer. Subsequently, polymer micelles served as templates to direct the assembly of ZIF-8 crystals in the surfactant-free emulsion to fabricate polymer/ZIF-8 composite materials (ZIF-8@CSP) with various structures. Specifically, ZIF-8@CSP with various architectures such as spheres, rods, cubes, leaf-shaped flakes, cross-flowers and wrinkled cubes were obtained by varying the concentration of CSP, the addition sequence of ZIF-8 precursors and the ratio of oil-water.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Zhi Hu,Shucheng Liu,Nana Tang,Xuan Zhang,Jianming Pan
The main obstacles of recognition of flavoniods are low concentration and complexity of extract wastewater solutions. The structural and stability limitation of the sorbents is the significant reason for the difficulty in increasing the adsorption amount in the separation system. Hereon, a novel hierarchical-pore boronic acid-functionalized-MOFs based on macroporous organo/hydro copolymers (CPs@H-UiO-66-NH 2 @BA) were firstly fabricated through the triple sacrificial cross-linking strategy, which allowed the formation of multiple hydrogen bond networks (i.e. main crosslinked networks and weak crosslinked networks) at oil–water interface. Noticeably, the MOFs with polymer chain entanglement effects as a physical sacrificial cross-linking network, significantly enhancing the mechanical properties. The maximum equilibrium binding capacity of CPs@H-UiO-66-NH 2 @BA was 40.93 µmol g −1 for NRG at 308 K. Furthermore, it also showed superior regeneration capacity capability (only 7.81% loss) after six cycles. Meanwhile, they had a stronger selectivity towards NRG. It can effectively purify the low purity of the actual sample ground to 92.68%. It is anticipated that in-situ the introduction of nanoboronic-functionalized MOFs construction into copolymers would hold great promise in the selective capture of target flavonoids in actual samples.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Zhiyuan Liu,Linmeng Wang,Changan Wang,Rushuo Li,Peiyun Zhou,Hongyi Gao,Ge Wang
Strong metal-support interaction (SMSI) plays an important role in heterogeneous catalysis, but the influence of the chemical microenvironment of metal on it is often neglected. In this study, a mesoporous Ce-MOFs with pyridine N sites and open metal sites (OMS) were constructed, and highly dispersed Pt nanoclusters (NCs) and Pt-N x interface were subsequently introduced and constructed via SMSI effect for hydrogenation of dicyclopentadiene (DCPD). The spectroscopic results and density functional theory (DFT) computations demonstrate that pyridine N and OMS can regulate the SMSI effect between Ce-PyDC and Pt through Pt-N x interface and electronic interaction between Pt and OMS, which increase electron cloud density of Pt nanoclusters, promote DCPD adsorption, H 2 activation. The optimal Pt NCs@Ce-PyDC-3 can efficiently convert DCPD to tetrahydrodicyclopentadiene (THDCPD) at 50 °C, giving a 100 % DCPD conversion and 99 % THDCPD selectivity. This work provides an in-depth understanding of the correlation between the metal nanoparticle microenvironment and SISM effect.
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ANALYST
·
2018
·Vol. 144
·期 2
·649-655
·
IF 3.864
Siyuan Li,Song Yue,Chao Yu,Yiyu Chen,Dong Yuan,Qiubo Yu
In this study, a new, simple, and label-free electrochemical immunosensor was presented for the detection of nuclear matrix protein-22 (NMP-22). In order to accurately monitor very small amounts of NMP-22, it was advantageous to use highly efficient nanomaterials as signals. For this reason, we synthesized a chrysanthemum-like nanocomposite (Co-MOFs/CuAu NWs), using Co-based metal–organic frameworks (Co-MOFs) as carriers and copper gold nanowires (CuAu NWs) wrapped around their surface, which was applied for modifying a glassy carbon electrode (GCE). The Co-MOFs/CuAu NWs possessed outstanding catalytic capabilities, which served as signal materials and simultaneously carried the anti-NMP-22 antibody (Ab). When different concentrations of the NMP-22 antigen (Ag) were specifically attached to the immunosensor, the current responses decreased by varying degrees. The designed biosensor used the principle to establish a linear regression equation and achieve an accurate quantification of NMP-22. After optimization, the NMP-22 sensor exhibited a good linear response over a concentration range from 0.1 pg mL−1 to 1 ng mL−1, with a lower detection limit of 33 fg mL−1 (based on S/N = 3). The proposed biosensor demonstrated the advantages of ultra-sensitivity, high specificity and acceptable reproducibility, suggesting that the proposed strategy has the potential for the quantification of NMP-22 in human urine samples. Moreover, the novel nanocomposite Co-MOFs/CuAu NWs are promising materials for electrochemical sensors to detect other biomolecules.
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DALTON TRANSACTIONS
·
2018
·Vol. 47
·期 14
·5065-5071
·
IF 4.099
Junyi Yang,Xiao Feng,Guangnong Lu,Yulin Li,Chaochao Mao,Zhongliang Wen,Wenbing Yuan
The use of salts as grinding media to assist the mechanosynthesis, and the following one-pot mechanochemical post-synthesis, of hierarchically porous MOFs was carried out efficiently by ball milling. NaCl or KCl were used as a solid solvent to initially pre-grind with 1,3,5-benzenetricarboxylic acid (H3BTC) and copper acetate monhydrate, respectively, for 1 minute, then both mixtures were combined together for a further 20 minutes of grinding, and the resultant mixture was finally washed with ethanol and water to obtain the hierarchically micro-, meso- and macroporous HKUST-1 with a high yield. Moreover, the post-synthesis of these as-obtained hierarchically porous HKUST-1 was easily performed via grinding triethylenediamine (TED) with the above unwashed crude-products for 20 minutes. By adjusting the amount of NaCl and TED added, we simply fabricated the pore- and function-adjustable hierarchically porous HKUST-1. Furthermore, these as-obtained HKUST-1 products showed high performance in the capture of volatile iodine.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2025
·
IF 3.5
Peng Wang,Hongmei Qu,Xia Li,Ruyu Liu,Ruihan Dai,Yameng Li,Zhihua Zhang
To further enhance the performance of MOFs-based hydrogen sulfide (H 2 S) detection probes, we proposed a novel strategy for constructing for H 2 S detection. We have designed and synthesized a new reactive coumarin-based ligand (NTA) and directly prepared the MOFs-based fluorescent probe UiO-66-NTA using the new ligand. This approach overcame the issues of low grafting rates and uneven reactive sites associated with post synthetic modification (PSM) strategy prepared MOFs-based fluorescent probes. This construction strategy endowed MOFs with a greater number of active sites on their surfaces for H 2 S detection, thereby achieving superior sensing performance for H 2 S, which included an ultra-fast response time (5 s) and a low detection limit (0.063 μM). The rigid topological structure of the MOFs minimizes π-π interactions between fluorophores, conferring aggregation-induced emission (AIE) characteristics to the probe. To enhance the practical utility of the probe, a smartphone-assisted test strip sensing system was developed and successfully applied to the detection of real water samples. Additionally, the probe was integrated into the sodium alginate (SA) hydrogel to create a portable sensor UiO-66-NTA@SA for assessing the freshness of meat by detecting H 2 S.
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TALANTA
·
2016
·
IF 4.035
Jiping Ma,Zhidan Yao,Liwei Hou,Wenhui Lu,Qipeng Yang,Jinhua Li,Lingxin Chen
Magnetic metal-organic frameworks (MOFs, [MIL-101]) were prepared and used as magnetic solid-phase extraction (MSPE) adsorbents for preconcentration of four kinds of pyrazole/pyrrole pesticides (flusilazole, fipronil , chlorfenapyr , and fenpyroximate) in environmental water samples, followed by high-performance liquid chromatography-diode-array detector (HPLC-DAD) determination. Several variables affecting MSPE efficiency were systematically investigated, including amount of MIL-101, extraction time, sample pH, salt concentration, type of desorption solvent and desorption number of times. Under optimized conditions, excellent linearity was achieved in the range of 5.0–200.0 μg/L for flusilazole and fipronil, and 2.0–200.0 μg/L for chlorfenapyr and fenpyroximate, with correlation coefficients r >0.9911. Limits of detection and quantification were 0.3–1.5 μg/L and 1.0–5.0 μg/L, respectively. The intra-day and inter-day precision (relative standard deviation, n =6, %) at three spiked levels were 1.1–5.4% and 3.9–7.8% in terms of peak area, respectively. The method recoveries at three fortified concentration levels ranged from 81.8% to 107.5% for reservoir water samples, 81.0–99.5% for river water samples, and 80.2–106.5% for seawater samples. The developed MOFs based MSPE coupled with HPLC method proved to be a convenient, rapid and eco-friendly alternative to the sensitive determination of pyrazole/pyrrole pesticides with high repeatability and excellent practical applicability.
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