TALANTA
·
2024
·
IF 5.6
Yaofei Ren,Jialing Li,Weixuan Wu,Xin Yu,Mengying Tao,Yanhu Han,Yintong Lin,Zhongfeng Shi,Liqin Zhou,Zhenxia Zhao,Zhongxing Zhao
A novel “double chemical bonding” electrochemical peptide biosensor 2FcP-GA-GDY(Fe)@NMIL-B was developed for highly selective, ultrasensitive, and ultrastable identification of prostate-specific antigen (PSA). The C–Fe–O chemical bond linking Fe-Graphdiyne (Fe-GDY) with NH 2 -MIL88B(Fe) (NMIL88B) as the first chemical bonding of electrode carrier Fe-GDY@NH 2 -MIL88B(Fe) (GDY(Fe)@NMIL) significantly accelerates electron transport. With glutaraldehyde (GA) as a crosslinking agent, the Schiff-base –N C- formed by GDY(Fe)@NMIL nanocomposites links the two Fc molecules labeled peptides (2FcP) as the second chemical bonding, facilitating high-density attachment of peptides to the electrode carrier in a firm manner. When the PSA analyte is introduced to identify and cleave the specific peptide, the release of ferrocene from its head leads to a decrease in the electrical signal, enabling sensitive detection. The prepared sensing platform exhibits exceptional analytical performance for PSA with an extended linear response range from 10 fg mL −1 to 50 ng mL −1 . Additionally, the detection limit has been significantly reduced to an ultra-low level of only 0.94 fg mL −1 , surpassing those reported in most literature by several orders of magnitude. Moreover, the 2FcP-GA-GDY(Fe)@NMIL-B sensor has excellent selectivity and stability while also showcasing great potential for practical application of PSA detection in human serum using the standard addition method.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jingjing Tang,Hongchao Li,Xuan Zhang,Jieshu Qian,Bingcai Pan
Fe-based metal–organic frameworks (MOFs) have garnered significant attention as catalysts for heterogeneous Fenton reactions, while the limited efficiency of the Fe(III)/Fe(II) redox cycle hinders their widespread use in wastewater treatment. Herein, we successfully incorporated carbon nanotubes (CNTs) into MIL-101(Fe) to modulate the coordination environment of Fe for achieving better catalytic activity. The MIL-101(Fe)/CNTs/H 2 O 2 system shows outstanding performance in degrading various pollutants, with the catalytic activity of the MIL-101(Fe)/CNTs composites (98.8%) significantly surpassing that of MIL-101(Fe) alone (26.4%) or CNTs alone (3.5%). Multiple experimental findings suggest that this synergistic effect is primarily attributed to the C-O-Fe bridge bonds resulting from the interaction of surface carboxyl groups on CNTs with Fe in MIL-101(Fe). This unique coordination structure accelerates the redox cycle of Fe(III)/Fe(II), thereby promoting the generation of hydroxyl radicals (HO • ). Furthermore, the MIL-101(Fe)/CNTs composites demonstrate excellent reusability and stability, maintaining effectiveness over a wide pH range from 3.0 to 6.5. This study provides new insights into regulating the microstructure of Fe-based MOFs to enhance their Fenton catalytic activity.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2025
·
IF 6.2
Chunhua Li,Zhehang Tian,Guanqun Luan,Luqian Bao,Mengyao Cui,Yixin Ji,Xieyang Zhang
The extensive use of tetracyclines in livestock poses health risks due to their residues in animal-derived food; therefore, developing simple detection methods to replace complex traditional approaches is of paramount importance. Here, we developed a dual-ligand zinc-based metal–organic framework material, Zn-BTC-BDC-NH2 (denoted as ZTD), for the detection of tetracyclines. The intrinsic blue fluorescence of ZTD was quenched upon the introduction of tetracyclines due to electron transfer from −NH2 of ZTD to −CO– and −OH groups of tetracycline molecules; meanwhile, the new green fluorescence emission was generated through π–π stacking between aromatic rings and the formation of complexes between Zn2+ and C–O/C═O groups. In real food samples, ZTD exhibited recovery rates ranging from 93.62 to 110.66%, with detection limits as low as 0.011 μmol·L–1. Additionally, a ZTD fluorescence test paper was developed for portable detection. This study presents a novel tetracycline detection method, offering insights into multiligand metal–organic framework preparation and future sensing method design.
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FUEL
·
2024
·
IF 6.7
Junfeng Qin,Shijie Hu,Xiaohua Zhang,Min Hong,Cuicui Du,Jinhua Chen
Although Metal-organic frameworks (MOFs) have attracted extensive attention in energy-related fields, the direct application of MOF as bifunctional electrocatalysts for overall water electrolysis still remains a challenging topic. Herein, nickel foam (NF) self-supported hydrangea shaped NiRu bimetallic MOFs (NiRu-PTA/NF) prepared by a simple one-step hydrothermal method was directly used as bifunctional electrocatalyst, and exhibited highly-efficient hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) catalytic performances for alkaline freshwater/seawater overall splitting owing to the large active surface area, abundant active sites and high intrinsic activity attributed to the unique morphology, enriched oxygen vacancies and modulated electronic structure of the catalyst. Specifically, NiRu-PTA/NF needed only 16 mV overpotential to drive a HER current density of 10 mA cm −2 and 298 mV overpotential to drive a OER current density of 20 mA cm −2 in alkaline freshwater, much lower than those of Ni-PTA/NF ( η 10,HER = 162 mV, η 20,OER = 372 mV) and Ru-PTA/NF ( η 10,HER = 36 mV, η 20,OER = 335 mV). Furthermore, a two-electrode configured water electrolysis cell assembled with NiRu-PTA/NF as both cathode and anode required a very low cell voltage of 1.54 V to achieve an electrolytic current density of 10 mA cm −2 and were operated continuously for 200 h at various current densities including 10, 100 and 200 mA cm −2 . Additionally, the NiRu-PTA/NF-assembled electrolysis cell also displayed excellent seawater electrolysis performance. This study proposes an available strategy to design highly-efficient bifunctional catalysts for overall freshwater/seawater electrolysis based on electronic structure and oxygen vacancy modulation between bimetallic centers of MOFs, and extends their promising application prospects for industrially clean hydrogen production.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
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IF 11.2
Rong Liu,Yan Gao
Preparing metal-organic frameworks (MOFs) film in situ on the surface of the Ti-6Al-4V (TC4) titanium alloy is challenging owing to the dense and stable surface TiO 2 passive film. In this study, titanium-doped zirconium-based MOFs (Zr(Ti)-MOFs) film was constructed in situ on the TC4 alloy in one step at a low temperature and atmospheric pressure, with ZrCl 4 as the source of Zr metal ions. ZrCl 4 attacked and dissolved the TiO 2 film to form Zr-O-Ti bonds on the surface of TC4 to provide nucleation sites for further reactions. At the same time, Zr 4+ and dissolved Ti 4+ combined in solution to form Ti containing Zr-O cluster nodes, which aggregated and grafted to the Zr-O-Ti bonds on the substrate surface, and reacted with organic ligands (terephthalic acid) to form Zr(Ti)-MOFs film. The Ti 4+ dissolved from the TC4 participate in the Zr-MOFs formation, thereby changing the high temperature and high-pressure conditions required for the traditional preparation of Zr-MOFs (UiO-66). The in situ preparation of Zr(Ti)-MOFs on TC4 was achieved at 80°C under atmospheric pressure conditions. This study elucidated the growth mechanism of Zr(Ti)-MOFs on the TC4 surface, providing a reference for the design and in-situ preparation of multifunctional MOFs on the TC4 titanium alloy.
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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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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ya-Nan Yu,Wei-Min Ma,Jia-Xin Wu,Qian Zhang,Jie Zhou,Ke-Ke Jiang,Dan-Dan Wang,Yong-Kang Li,Yang-Min Ma,Zheng Yin
The radioactive iodine as highly harmful fission waste from nuclear power production features fifteen-million years radiation period and easy diffusion, yet its efficient treatment and sensing is greatly challenged by the operation concentration as low as several ppm in gaseous and aqueous medium. A (3,12)-connected and [Pb 6 ( µ 4 -O) 2 (COO) 8 ] based MOFs of [Pb 6 ( μ 4 -O) 2 (pia) 4 ]·4DMF ( 1 ) was rationally constructed as a multifunctional materials for iodine capture and sensing, which possesses the highest void fraction of 34.4 % among all known cluster based Pb-MOFs. Microwave-assistant solvothermal reaction facilitates gram-scale synthesis of 1 with yield of 82 % within 4 h. The 1D round channels sized at 1.0 nm coupled with high structure stability of the MOFs contribute to accommodate iodine. 1 can rapidly capture iodine vapor at 70 °C in 6 h with fully utilized nanopores, resulting in a high iodine packing density of 3.52 g cm −3 closely matching that of iodine single crystal. Particularly, the MOFs of 1 exhibits long-lasting adsorption to iodine vapor at extremely low concentration of 120 ppm, as well as efficient capture of I 2 in 1.0 × 10 -4 M aqueous solution with removal percentages of 67.1 % in only 20 min, driven by synergistic host–guest interactions. The MOFs is further discovered as a single-phase white-emitting phosphor with quite broad fluorescence spectrum covering the entire visible region, benefited from the multiple Pb···Pb interactions and change-transfer between the metal and ligand. White light emitting diodes can be created by coating commercial blue LEDs with phosphor 1 , generating pure white chromaticity coordinates of (0.313, 0.338), a near daylight color temperature of 6420 K, a high color rendering index of 85 and light maintenance up to 120 °C. The migration of iodine into the channels of 1 led to obvious fluorescence quenching. As the combined result, 1 presents a rare and instructive multifunctional MOFs that exhibiting efficient capture to low-concentration iodine in gaseous/aqueous condition and fluorescent detection to iodine.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Ximeng Liu,Jingwen Chen,Fan Xia,Jian Yang,Chun Feng,Jinlou Gu
The design and construction of MOFs with flower-like structure could afford sufficient space for the immobilization of guests with large size and interconnected transport channels for their mass diffusion although it remains a challenge. Herein, wrinkled Ce-based hierarchically porous UiO-66 (Ce-WUiO-66) with good crystallinity was successfully synthesized for the first time using bicontinuous emulsion composed of 1-heptanol, water and F127 (PEO 106 PPO 70 PEO 106 ) surfactant as a template. F127 played a key role in the formation of emulsions as a stabilizer, and meanwhile its PEO segments interacted with MOF precursors to guide the evolvement of crystallized pore walls. Through controlling the ratios of heptanol to water and the salinity, the distances of the pleat openings and the morphology of the resultant Ce-WUiO-66 were facilely regulated. In virtue of its highly open radial structure, Ce-WUiO-66 could serve as an ideal platform for loading multiple substances to build a cascade sensing system. As a proof of concept, we designed an amino acid (AA) cascade probe by co-immobilizing gold nanoclusters (AuNCs) and LAA oxidase into Ce-WUiO-66. The aggregation-induced-emission enhancement resulted from the encapsulation of AuNCs into Ce-WUiO-66 significantly improved the detection sensitivity and the detection limit of corresponding substrates reached as low as 10 -8 M. The proposed biphasic interface assembly strategy is hopefully to provide a new route for the rational design of MOFs with various open pore structure and broaden their potential applications with multiple large-size substances involved besides the currently exemplified cascade sensing platform.
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Frontiers in Chemistry
·
2025
·
IF 4.2
Xianbing Zhang,Yuheng Liu,Jiajia Yuan
Metal-organic frameworks (MOFs) are recognized as important Fenton-like materials for environmental remediation. However, their applications are often hindered by slow cycling between Fe (III) and Fe (II). This study aimed to address the slow Fe (III)/Fe (II) cycling limitation of Fe-MOFs through dual modification strategy: bimetallic modification and amino functionalization. A series of NH2-MOF(Fe, Co) catalysts with varying Fe/Co ratios were synthesized via a hydrothermal method and evaluated for sulfamethoxazole (SMX) degradation. The optimized NH2-MOF(Fe, Co) catalyst (Fe/Co ratio = 7:3) exhibited substantially enhanced catalytic performance, with SMX removal rate and rate constant in the H2O2 system being 3.2 and 43.5 times higher than those of the Fe-MOF/H2O2 system, respectively. The catalyst demonstrated robust performance across a wide pH range (3.05–7.00), addressing a common limitation of Fenton-like systems. Physicochemical characterization revealed that the enhanced performance was attributed to two key factors: the synergistic effect between Co and Fe in the bimetallic active center, and improved electron transfer to the central metal due to -NH2 functionalization. These modifications effectively addressed the Fe (III)/Fe (II) redox cycling limitation. The proposed reaction mechanism provides insights into SMX degradation pathways in the NH2-MOF(Fe, Co)/H2O2 system. This study presents an efficient and stable MOF-based Fenton-like catalyst with potential applications in wastewater treatment and environmental remediation.
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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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CRYSTENGCOMM
·
2024
·Vol. 26
·期 24
·3185-3193
·
IF 2.6
Wan-Ru Yan,Yu Xue,Mei-Chen Liu,Xiu Qiao,Chang-Yi Jing,Yue Yu,Xiao-Chun Yan,Jin-Zhi Wei,Hong Dong,Feng-Ming Zhang
Room temperature, rapid and large-scale preparation of 2D-metal organic frameworks (2D-MOFs) with high oxygen evolution reaction (OER) activity is still a challenge. Herein, a series of 2D NiCo-CAT MOFs were synthesized by a mild green electrochemical method with Ni and Co as metal sources and 2,3,6,7,10,11-hexahydroxytribenzene (HHTP) as the organic ligand. The synthesis conditions were fine-tuned by adjusting the solvent ratio, applied voltage, synthesis temperature, and reaction time. Electrochemical testing revealed that NiCo-CAT/CC exhibited a low overpotential of 307 mV at a current density of 10 mA cm−2, accompanied by a small Tafel slope of 61.03 mV dec−1 in a 1.0 M KOH solution (the dosage of Co2+ was 70 μmol). Further investigation shows that the rapid electron transfer, large electrochemical active area and exposure of more metal active sites in bimetallic NiCo-CAT enhanced the OER activity. This work has opened up a new pathway for the rapid preparation of OER catalysts using the electrochemical strategy, offering a green approach with short reaction times, low energy consumption, and high yields, making it ideal for future practical applications.
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Hongqi Liang,Fenglong Chen,Zhizhuo Liu,Litao Tian,Jingmei Xu
The design and preparation of low-cost and high-stability proton exchange membranes (PEMs) play an indispensable role in sustainable development and application expansion. In this study, sulfonic acid-amino difunctionalized hydrophilic metal–organic frameworks (MOFs) (named as TA-SNU6) were designed and synthesized as proton transport carriers to be incorporated into sulfonated poly(aryl ether ketone sulfone) (SPAEKS) to obtain high proton conductivity and single-cell performance. The experimental results show that abundant hydroxyl and acid–base groups significantly increase the proton transport efficiency in PEMs and improve the hydrophilicity and electrochemical performance of PEMs. The single-cell performance of the STSN-1% membrane was about 1.8 W cm–2. The proton conductivity was up to 190 mS cm–1, the mechanical properties were significantly improved, and the tensile strength reached 48 MPa. SPAEKS polymer with a specified degree of sulfonation was prepared by a stepwise polycondensation reaction, which showed excellent comprehensive properties after adding TA-SNU6 fillers. The STSN-1% composite membrane performs better than Nafion 211 and Nafion 117 in fuel cells. Therefore, it can be seen that this work has achieved certain results, which makes PEMs have excellent electrochemical performance, and provides a reference for the development of high-performance PEMs.
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