SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yubo Pan,Linrui Li,Baogang Yang,Guangwei Ji,Zhiren Zhao,Hongling Zhang,Fengyun Wang,Mingzhu Xia,Yu Tao
The rapid development of industries such as new energy and photovoltaic has led to the generation of a large amount of industrial fluorine wastewater, posing serious threats to water environment and human health. To address this issue, MOF-808 adsorbent was synthesized by controlling the synthesis conditions and modifying the ligand structure. Batch adsorption experiments were conducted by varying experimental conditions, including type of adsorbent, pH, wastewater concentration, adsorption time, temperature, and interfering anions. The adsorption behavior of MOF-808-AA towards fluoride ions was well fitted by the Elovich non-linear kinetic model, as well as the Freundlich and Temkin non-linear isotherm models, indicating that the adsorption behavior was influenced by multiple mechanisms other than just intraparticle diffusion. Thermodynamic results suggested a spontaneous exothermic monolayer chemical adsorption process. Under the conditions of pH 6.0 and T = 298 K, MOF-808-AA exhibited a maximum adsorption capacity of 84.65 mg/g for fluoride ions. Characterization techniques, as well as quantum chemical analysis was employed to analyze the adsorption behavior and predict the reaction sites. The potential mechanism can be summarized as the formation of new bonds between MOF-808-AA and the adsorbed fluoride ions, as well as the weak intermolecular interactions such as hydrogen bonding and vdW forces. Furthermore, MOF-808-AA demonstrated satisfactory reusability and excellent chemical stability during the cyclic process. These findings suggest the potential application of MOF-808-AA for removing fluoride ions from wastewater.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Lijun Liu,Luyang Zuo,Xuejing Zhai,Xiangping Xiao,Huitao Fan,Bo Li,Liya Wang
Photocatalytic water splitting is a commonly used pathway for hydrogen (H 2 ) production, and it is crucial to develop highly active ZnIn 2 S 4 (ZIS)-based photocatalytic systems. In recent years, metal-organic frameworks (MOFs) are also of great interest in the fields of energy production and environmental remediation. Therefore, this study primarily focuses on the fabrication of a series of heterojunction hexagonal prism-shaped Zr-based MOF@ZIS core-shell nanorods through a simple solvothermal method, in which ZIS nanosheets are highly distributed on the surface of the Zr-based MOF (NU-1000). The photocatalytic activities of the resulting materials were evaluated under visible light illumination (λ ≥ 400 nm) by combining different contents of NU-1000 with ZIS. The H 2 evolution results demonstrate that the optimal content of NU-1000 corresponds to a photocatalytic H 2 production rate of 8.53 mmol g −1 h −1 , which is 5.3 times higher than that of pure ZIS. The enhanced photocatalytic activity of the NU-1000@ZIS (NUZ) heterojunction can be attributed to the incorporation of the NU-1000, which provides abundant active sites due to its larger specific surface area. Additionally, the well-matched band structure between the NU-1000 and ZIS is beneficial to efficiently transfer and separate the photogenerated charge carriers. Furthermore, the NUZ core-shell nanorods exhibit excellent stability, offering a new approach for the fabrication of composite photocatalysts by combining MOF-based and ZIS in the field of photocatalytic H 2 production.
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CHEMOSPHERE
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2024
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IF 8.1
Guangli Yu,Fei Ni,Wenyue Niu,Yu Chen,Feng Zhang,Guo-Dong Li,Xingfei Song,Yajing Zhang,Kangjun Wang
Metal-organic frameworks (MOFs) recently gained immense popularity for the adsorption of organic impurities. In this work, the adsorptive separation of bisphenol A (BPA) from aqueous mixtures was explored utilizing three types of zirconium-based MOFs, namely MOF-808, UiO-66, and hierarchically porous UiO-66 (HP-UiO-66). The HP-UiO-66, which was etched by sodium acetate as the terminal ligand, generated large mesopores ranging from 40 to 300 Å due to the departure of partial linkers and metallic clusters. The adsorption ability for BPA increased significantly with the introduction of numerous mesopores onto the HP-UiO-66 framework, even though the surface area of HP-UiO-66 was lower compared to that of the pristine UiO-66 and MOF-808. The study revealed that the maximum adsorption capacities ( q ) for BPA by HP-UiO-66 reached up to 295.04 mg g −1 , which was about 88.5% and 17.4% higher in comparison to UiO-66 and MOF-808, respectively. Furthermore, the q value of HP-UiO-66 was also better than many other previously reported MOF adsorbents. The analysis of possible adsorption mechanisms indicated that physical pore-filling was anticipated as the principal mechanism, attributed to the larger window size and high mesopore surface area of HP-UiO-66. Furthermore, X-ray photoelectron and Fourier transform infrared spectroscopic measurements inferred that the synergetic effects of H-bonding and π-π interactions played crucial roles in BPA capture as well. Overall, this study revealed a structure–property relationship in the Zr-MOFs-based adsorbents and opened up a new avenue to exploit unique MOF platforms for the efficient removal of emerging contaminations in the future.
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REACTIVE & FUNCTIONAL POLYMERS
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2025
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IF 5.1
Shuxin Chen,Liting Wang,Wenxiang Ni,Hui Qiu
The self-assembly behavior of the MPNs-based adsorbent is substantially influenced by changes in solution pH. In this study, a highly negatively charged tannic acid‑zirconium (TA-Zr) macromolecular network has been successfully synthesized. As pH increases from 3 to 11, the coordination structure of TA with Zr(IV) changes from mono- to tri-complexation state, resulting in enhanced electronegativity and increased structural stability of tri-complex TA-Zr(9) due to its higher charge density. The TA dissolution experiments and zeta potential measurements confirm this conclusion. The tri-complex TA-Zr(11) underwent structural changes in its macromolecular network due to partial zirconium hydroxide formation under strongly alkaline conditions, as confirmed by X-ray photoelectron spectroscopy analysis, which in turn impacted its stability. Meanwhile, the adsorption capacity of TA-Zr materials for Pb(II) ion increases with the pH of the synthesis solution. XPS analysis suggested that the underlying adsorption mechanism involved ligand exchange between Pb(II) ion and phenolic hydroxyl groups on TA-Zr(9). After batch adsorption-regeneration cycles, TA-Zr(9) could be regenerated with an acidic solution while maintaining consistent Pb(II) ion removal efficiency. Furthermore, TA-Zr(9) effectively treated 12,150 bed volumes (BV) of synthetic water at pH 5.6, which is 18 times more than commercial D001. These results confirm that TA-Zr(9) shows great potential as an effective adsorbentfor Pb(II) removal in practical wastewater treatment, making it a promising candidate for water remediation.
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AICHE JOURNAL
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2024
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IF 3.5
Yanru Zhu,Zhen Zhang,Yunfei Zou,Jian Zhang,Zhe An,Xin Shu,Hongyan Song,Jing He
Catalytic conversion of biomass-derived 5-(hydroxymethyl)furfural (5-HMF) into carbon-increased hydrocarbons as drop-in energy-rich biofuels has received a great deal of concern for the development of sustainable chemical industry. Here, we demonstrate a one-pot conversion of 5-HMF into C 9 -alkanes on one single catalyst, acidic–basic layered double oxides (Mg(Al)(Zr)O) supported CuCo alloy. The well-defined multifunctional catalytic sites with harmonious combination carry out cascade catalysis, affording C 9 -alkanes (including 30% of more value-added branched-cycloalkanes) in 83% yield. The basic–acidic sites on Mg(Al)(Zr)O show high activity for aldol condensation of 5-HMF and acetone, producing 4-[5-(hydroxymethyl)-2-furanyl]-3-buten-2-one (HAc) in a yield of >99%. The engineered Co–Cu–Co linkages on supported CuCo perform efficient hydrodeoxygenation, affording C 9 -alkanes in a selectivity of 96% from HAc. C 9 -cycloalkanes are generated from the cyclization of the corresponding monohydric alcohol intermediates by the synergy of acidic and CuCo sites in the hydrodeoxygenation reaction.
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APPLIED SURFACE SCIENCE
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2024
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IF 6.3
Chunhua Li,Luqian Bao,Yubo Shi,Zhehang Tian,Yixin Ji,Mengyao Cui,Zhilei Zhao,Xianyou Wang
A hollow heterojunction of W-Zr-MOF-NH 2 @TpTt-COF (WZT) was fabricated by combining etched W-Zr-MOF-NH 2 with TpTt-COF. WZT, synthesized through acid etching and hydrothermal methods, showed better tetracycline degradation than pure W-Zr-MOF-NH 2 and pure TpTt-COF due to its larger specific surface area and more active sites. The surface of WZT contains abundant oxygen vacancies (OVs) that capture electrons, promoting the separation of photogenerated e - -h + pairs and increasing WZT’s photocatalytic activity. WZT (1:1, mass) showed 87% degradation of tetracycline under 300 W Xenon lamp irradiation. The results of cycling experiments demonstrated the high stability and reusability of WZT (1:1), making it feasible for production. The excellent photocatalytic degradation of tetracycline by WZT (1:1) originates from the formation of heterojunctions and the presence of surface OVs, which reduces the strong photogenerated e - -h + complexation efficiency. Possible photocatalytic degradation mechanisms are proposed while demonstrating the formation of Z-scheme heterojunction in WZT, which aligned with the experimental results of electron spin resonance (ESR). The tetracycline oxidative decomposition process involves the participation of •OH, 1 O 2 , • O 2 - , e - , and h + as proven by ESR and radical trapping experiments. This work proposes a research idea to prepare high-performance photocatalysts with MOF@COF type, featuring OVs-rich and Z-scheme heterojunctions.
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Carbon Capture Science & Technology
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2025
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IF 10.5
Xueyang Jiang,Xiaoshen Li,Shaohui Xiong,Wei Liu,Jiayan Yan,Xiang Duan,Song Song,Qingpeng Cheng,Ye Tian,Xingang Li
The hydrogenation of CO 2 to methanol using H 2 produced from renewable resources has been regarded as an effective way to mitigate CO 2 emissions. Unfortunately, how to obtain both high activity and methanol selectivity is still a trade-off challenge for catalyst development. Herein, we synthesize Co-In-Zr ternary metal oxide precursors via a simple hydrothermal method for hydrogenation of CO 2 to methanol. After reduction by H 2 , a part of Co and In cations could be reduced from the solid solution to generate CoIn alloy, simultaneously constructing oxygen vacancy rich environment on the catalyst surface. The increased concentration of surface oxygen vacancies can improve the adsorption and activation of CO 2 . Meanwhile, our findings show that the formed CoIn alloy significantly enhances the adsorption and dissociation of H 2 , thus accelerating successive hydroconversion of CO 2 and intermediates to methanol. The synergy of CoIn alloy and oxygen vacancies significantly boosts both activity and methanol selectivity. Under the conditions of 300 °C and GHSV of 30,000 ml g cat -1 h -1 , the catalyst with a Co: In: Zr molar ratio of 1: 2: 7 achieves the CO 2 conversion of 10.2 %, the methanol selectivity of 81.5 %, and especially the methanol time-space yield up to 860 mg g cat -1 h -1 , surpassing the majority of the state-of-the-art In-based catalysts. Moreover, the catalyst exhibits the excellent stability, maintaining the performance within 100 h. Our work provides insights into designing efficient none-noble-metal catalysts for CO 2 hydrogenation reactions.
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SENSORS AND ACTUATORS B-CHEMICAL
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2025
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IF 7.7
Xin Xie,Peng Chen,Jingxi Wang,Ding Wang,Daxiu Li,Beibei Kou,Wenjiao Zhou
Herein, a novel electrochemical biosensor on the basis of MB/AuNPs@Zr-MOF signal probe and enzyme-free cascade signal amplification was fabricated for the ultrasensitive detection of colorectal cancer (CRC)-associated miR-92a-3p. Impressively, compared with the traditional electrochemical probes, MB/AuNPs@Zr-MOF not only exhibits high loading for electroactive substances, but also shows enhanced electronic conductivity, thereby generating stable and high electrochemical signal. Meanwhile, under the assistance of the target-induced enzyme-free cascade signal amplification including multicomponent nuclease (MNAzyme) recycle catalytic and catalytic hairpin assembly (CHA), the sensitivity of proposed biosensor was further improved. Additionally, the DNA tetrahedral scaffold (TDNs) was served as an electrode support interface, which could greatly reduce the non-specific adsorption and improve the analytical performance. As a result, the developed biosensor enabled the miR-92a-3p with a detection limit as low as 0.36 fM. This work provided an efficient method to increase the sensitivity and the stability of electrochemical sensing platforms, showing great potential for the detection of biomarker and disease diagnosis.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yuanfang Song,Qi-an Zhang,Ying Li,Ao Tang
All‑iron redox flow batteries (AIRFBs) represent a compelling solution for grid-scale energy storage due to their cost-effectiveness, material abundance, and environmental compatibility. However, the limited electrochemical activity and sluggish reaction kinetics of conventional carbon felt electrodes at the negative side severely restrict the areal capacity and lifespan of AIRFBs. This study addresses these limitations through rational design of amorphous zirconium-based metal-organic framework (ZrATMP) catalysts synthesized via a single-step solvothermal process. The ZrATMP-modified carbon felt (Zr@CF) electrode with microporous structure provides abundant active sites and facilitates electrolyte transport, significantly enhancing the electrochemical activity of the electrode. Moreover, the composite electrode also effectively suppresses hydrogen evolution side reactions through elevated energy barriers while promoting uniform Fe deposition. Benefiting from the synergistic effects, the assembled full cell achieves stable operation over >300 h at 20 mA cm −2 /20 mAh cm −2 with 99 % Coulombic efficiency. More importantly, it also sustains unprecedented cyclability at 40 mAh cm −2 —a benchmark areal capacity demonstrating practical viability. This study establishes amorphous MOF catalysts for high-performance AIRFBs, resolving the critical trade-off between cycle longevity and energy density in flow battery systems.
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ACS Applied Materials & Interfaces
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2025
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IF 8.2
Lixin Ding,Qian Guo,Ya’nan Ren,Pei Wang,Yongxiang Pan,Jin Ding,Feng Wang,Zhi Yang,Hua Zhu
Extracellular vesicles (EVs) act as carriers that transfer molecules between donor and recipient cells, thereby altering the phenotype and function of the latter. EVs derived from mesenchymal stem cells (MSCs) inherit the homing ability of their parent cells to tumor sites. We speculate that MSC-derived EVs labeled with the isotope zirconium-89 ([89Zr]Zr) will accumulate within tumors and have the potential for tumor location via positron emission tomography (PET) imaging. Here, as a proof of concept, we used [89Zr]Zr-labeled human umbilical cord MSC (hucMSC)-derived EVs to characterize the homing of EVs to tumor regions via PET imaging. The uptake of [89Zr]Zr-DFO-hucMSC-EVs by 4T1, H292, and FaDu cells increased in a time-dependent manner. [89Zr]Zr-DFO-hucMSC-EVs were rapidly cleared from the blood circulation, showing a 2-phase exponential decay with a biodistribution half-life of 0.46 h and an elimination-phase half-life of 11.87 h. At 24 h postinjection, [89Zr]Zr-DFO-hucMSC-EVs were mainly distributed in the liver (10.39 ± 0.52%ID/g) and, to a lesser extent, in the spleen (9.87 ± 0.87%ID/g). PET imaging in tumor-bearing mouse models revealed persistently high tumor accumulation. The projected effective dose for an adult human female was low and was 0.084 mSv/MBq. There was no obvious normal tissue toxicity following the administration of excessive radioactivity. In summary, these studies demonstrate the potential feasibility of using the [89Zr]Zr-DFO-hucMSC-EV tracer for noninvasive visualization of tumor lesions.
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FUEL
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2025
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IF 7.5
Liang Chu,Zhaokun Wang,Zhaohui Liu,Teng Zhao,Liyan Wang,Mu Yang,Ge Wang
Host-guest catalysts are promising for tailored applications but require innovative synthesis strategies. Herein, we report the first ambient aqueous-phase synthesis of bimetallic Ce/Zr MOF-801, followed by acid post-treatment. Utilizing defect engineering, Ce species are preferentially exposed within the robust Zr-MOF-801 substrate. This structural modification substantially enhances the host–guest catalyst’s oxidative desulfurization (ODS) performance. We systematically investigate synthesis parameters, spatiotemporal yield, and defect characterization, and refines catalytic conditions. Post-acid-treated Ce/Zr-MOF-801-H displays augmented external surface area (189 m 2 g −1 ), and exposed acidic sites while upholding the outstanding intrinsic stability of the Zr-MOF-801 substrate. Under optimal conditions (60 °C, 6 min), Ce/Zr-MOF-801-H completely eliminates dibenzothiophene (1000 ppm S), with a turnover frequency of 39.3 h −1 and catalytic activity of 53.2 mmol g −1 h −1 , far surpassing Zr-UiO-66-H. It maintains a desulfurization rate of 96.6% after five cycles. FTIR spectroscopy, quenching experiments, and ESR spectroscopy reveal that the exposed Ce sites serve dual roles: (1) activating the substrate by reducing the electron density of sulfur atoms and (2) facilitating H 2 O 2 into hydroxyl and superoxide radicals, driving ODS. This strategy not only advances industrial ODS applications but also sheds light on the synthesis of MOF-based host–guest catalysts.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2025
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IF 8.5
Weibo Lu,Huangwei Ye,Yike Zhu,Yuhan Li,Huan Li,Qing Shen,Jian Chen
The non-destructive, real-time, and visual assessment of fish freshness is crucial for maintaining food quality and safeguarding public health. In this study, a pH-sensitive and colorimetric enhancement film was developed using a carboxymethyl cellulose/anthocyanin/metal-organic framework (CMC-BA-UIO). The concentration of UIO-66 in the film-forming solution significantly influences the mechanical properties and ammonia responsiveness of the indicator film, with the CMC-BA/2.5%UIO-66 variant exhibiting optimal performance. When utilized for real-time fish freshness monitoring at 4 °C, the CMC-BA/2.5%UIO-66 indicator film demonstrated a distinct color transition from purple to yellow, which exhibited a strong correlation with the rot index (TVB-N) of the fish. These findings indicate that the developed indicator film has potential applications in intelligent packaging for monitoring food shelf life, providing a visual alert to producers and consumers regarding food spoilage.
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