JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Xiangrong Li,Shaohua Xie,Dongman Hou,Wenliang Wang,Guoqiang Li
Indium nitride (InN) exhibited significant potential as a photoelectrode material for photoelectrochemical (PEC) water splitting, attributed to its superior light absorption, high electron mobility, and direct bandgap. However, its practical application was constrained by rapid carrier recombination occurring within the bulk and at the surface. To address these limitations, researchers developed InN/UiO-66 heterojunction photoelectrodes, which markedly enhanced PEC water splitting for hydrogen production. Functionalization of the UiO-66 metal–organic framework (MOF) with hydroxyl (–OH) groups optimized the bandgap and improved light absorption, facilitating efficient charge separation and transfer processes. The functionalization also mitigated surface defect states in the InN nanorods (NRs), which were a major source of photogenerated carrier recombination, thereby enhancing overall photocatalytic activity. Compared to pristine InN NRs, the optimized InN/UiO-66-(OH) 2 electrode achieved a photocurrent density of −0.42 mA cm −2 and an applied bias photon-to-current efficiency (ABPE) of 0.47 % at −0.5 V vs. reversible hydrogen electrode (RHE). Furthermore, the InN/Ag/UiO-66-(OH) 2 system demonstrated a hydrogen production rate of 1.82 μmol min −1 under AM 1.5G illumination, with excellent long-term stability. This study provided critical insights into the design of efficient and durable PEC photoelectrodes, achieved the highest hydrogen yield reported for indium-based photocathodes to date, and underscored the promise of InN-based materials for solar-driven hydrogen production in the context of clean energy applications.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2025
·Vol. 39
·期 4
·e70109
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IF 0
Yun Xiong,Yifan Shu,Shi Cai,Shengpeng Liu,Xiaoyu Wu
The efficient separation of gases under high-temperature industrial conditions is crucial for addressing global energy and environmental challenges, particularly in processes such as CO₂ capture in natural gas processing, power plant flue gas treatment, and cement plant emissions. However, conventional membranes often suffer from interfacial defects, low gas selectivity, and poor thermal stability, which limit their practical applications. In this study, we aimed to develop high-performance mixed matrix membranes (MMMs) to improve CO₂/CH₄ separation performance. Amino-functionalized UiO-66-NH₂ was incorporated into a polyimide (PI) matrix using a simple, scalable fabrication process involving phase inversion and thermal imidization, which ensured uniform dispersion of UiO-66-NH₂ particles and facilitated large-scale production of dense, defect-free membranes. At an optimal UiO-66-NH₂ loading of 2 wt%, the MMMs achieved a CO₂ permeability of 451 Barrer and a CO₂/CH₄ selectivity of 6.62 at 25°C and 0.1 MPa, representing improvements of 23.91% and 114.94%, respectively, compared to pure PI membranes. The performance enhancement was attributed to the increased free volume within the membrane and the strong Lewis acid–base interactions between the amino groups of UiO-66-NH₂ and CO₂ molecules. Long-term stability testing at 300°C demonstrated excellent thermal stability, with consistent gas separation performance maintained over 160 h, confirming the membranes' suitability for high-temperature industrial applications. Furthermore, the UiO-66-NH₂/PI MMMs achieved an excellent balance between high permeability and selectivity, outperforming both organic and inorganic membranes, as well as certain traditional MOF-based MMMs. These findings offer a promising strategy for the development of robust and sustainable MMMs for high-temperature industrial gas separation processes.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2024
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IF 3.9
Bo Zhao,Yao Yao,Kexin Huang,Jiaxin Li,Minjie Chen,Chao Liu,Hongjian Xu,Xinyu Zhao,Ganggang Chang
The selective hydrogenation of furfural (FFA) to furfuryl alcohol (FA) is regarded as attractive transformation to achieve the sustainable synthesis of value-added chemicals from biomass resources. However, the conventional supported catalysts are significantly restricted by their narrow pore size, ununiform dispersion and easy leaching or aggregation of catalytic sites. Herein, we designed hollow UiO-66-NH2 as the support to encapsulate Pd nanoparticles (Pd@H-UiO-66-NH2) to achieve the highly active and selective conversion of FFA to FA. Benefiting from the void-confinement effect and substrate enrichment of hollow structure, as well as the surface wrinkles, the as-prepared catalyst Pd@H-UiO-66-NH2 exhibited 96.8 % conversion of FFA with satisfactory selectivity reaching up to 92.4 % at 80 °C, 0.5 MPa H2 in isopropanol solvent within 6 h. More importantly, as-prepared Pd@H-UiO-66-NH2 catalyst exhibited excellent long-term stability, as well as good universality toward a series of hydrogenation of unsaturated hydrocarbons.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
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2024
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IF 1.5
Guo Dingge,Xiao Jing,Ning Yang,Yu Hongchao,Jin Tianxiang,Huang Bin,Qian Yong
The efficient removal of thorium from the environment is critical due to the risks it poses to organisms. Metal–organic frameworks are favored by scholars because of their potential to effectively adsorb a variety of heavy metal ions in wastewater treatment. In this work, the interaction of UiO-66-NH 2 surface with graphene, enhances adsorption capacity of MOFs. Optimal adsorption conditions have been identified, and a detailed adsorption mechanism has also been comprehensively discussed. The theoretical maximum adsorption capacity exhibited by UiO-66-GO is 119.57 mg g −1 . Moreover, it shows a fast adsorption rate and reached equilibrium within 20 min. The development of materials with good adsorption performance and fast adsorption for Th(IV) plays an important role in the development of Th(IV) adsorption in the future.
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Journal of Materials Chemistry A
·
2024
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IF 10.7
Ying Luo,Da Lei,Maohua Li,Yuansheng Ge,Jiguang Li,Baiyi Zu,Jun Yao,Xincun Dou
Metal organic frameworks (MOFs) have made great progress in the field of fluorescent sensing; however, whether the electronic structure and recognized sites can be adjusted by external functionalization still remains challenging. Here, by postmodifying 5-carboxyfluorescein (Flu), externally coupled orbitals were introduced into the electronic structure of UiO-66-OH, and thus an effective photo-induced energy transfer (PET) process was established in functionalized MOFs (UiO-66-Flu), resulting in the reduction of the intrinsic blue fluorescence. Due to the formation of the ester bond by effective incorporation of the surface –OH with Flu, the hydrazinolysis reaction triggered by hydrazine could happen and the Zr6O6 clusters could further reduce the reaction energy barrier through strong hydrogen bonding with hydrazine, resulting in a remarkably low limit of detection (LOD, 27.17 nM) and a fast response (4 s). Furthermore, with polyvinylidene fluoride (PVDF) as the dispersion medium, UiO-66-Flu was fabricated into a UiO-66-Flu/PVDF film sensor, enabling the rapid detection of gaseous hydrazine within 2 s in simulated practical scenarios. We expect that the present fluorescent ligand modifying concept will not only deepen the understanding of electronic structure engineering in functionalized MOF design, but also shine light on the exploration of high-performance MOF-based sensing strategies.
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Materials Today Chemistry
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2024
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IF 6.7
Deshuang Lu,Zhonghan Cheng,Nikom Klomkliang,Wanida Koo-amornpattana,Francis Verpoort,Somboon Chaemchuen
Organic linkers are typically controlled to create the micropore structure when synthesizing metal-organic frameworks (MOFs). However, developing a hierarchical pore structure is beneficial for improving the efficiency of MOFs in various applications. This study investigates a green strategy using a water modulator that competes with the terephthalic ligand to coordinate with zirconium clusters, thereby accessing open sites for hierarchical micro- and mesopores in UiO-66. Using a hydro-modulator induced the formation of a mesoporous structure and enhanced the hydrophilic properties of UiO-66-X due to the presence of hydroxyl groups. Also, model calculations using density functional theory (DFT) support the observed structural chemical geometry. The advantages of a hierarchical pore structure, increased hydrophilicity, and the presence of open sites in the robust structure of UiO-66-X led to a significant enhancement in both antibiotic adsorption and the catalytic activity of ring-opening epoxide reactions compared to the pristine microporous UiO-66. Therefore, utilizing water as a green modulator presents a simple and environmentally friendly approach to introducing hierarchical pore structures in MOFs. It offers a promising strategy for enhancing their performance across various applications.
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JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Jiajun Yu,Xiao Wang,Guanhong Lu,Haijiao Xie,Xiaofeng Xie,Jing Sun
The purification of oxygenated volatile organic compounds VOCs (OVOCs), important precursors of ozone and particulate matters, has triggered intensive research interests. UiO-66 with high photocatalytic activity have shown great potential. However, the lack of active sites severely limited the trapping and degradation of OVOCs. Herein, reo-UiO-66 with increased specific surface area, hierarchical porous structure and tunable acidic/basic sites was synthesized by simply adding water as the modulator. XRD, TGA and FTIR results confirmed the formation of reo-defects, which significantly affected the surface hydrophilicity and active sites of UiO-66. The adsorption of Lewis acidic acetaldehyde was enhanced by 265 times with coordinative unsaturated Zr acting as the dominant adsorption sites. The degradation efficiency of typical OVOCs (acetaldehyde and acetone) increased from 0% and 25% to 50% and 73%, respectively. This work provided a facile method to modulate the micro-environment in MOFs for the efficient capture and catalytic purification of OVOCs.
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FUEL
·
2024
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IF 6.7
Wenli Zhang,Yijie Zhou,Zhenzhen Wu,Cheng Pan,Qunpeng Cheng,Guozhi Fan
A porous sulfonic acid-functionalized zirconium-based metal–organic framework possessing both Lewis acid and Brønsted acid sites (UiO-66-SO 3 H) was synthesized and tested for the selective conversion of furfural (FUR) to isopropyl levulinate (IPL) through one-pot cascade reaction. UiO-66-SO 3 H exhibited excellent catalytic performance, and the conversion of FUR as well as the yield and selectivity of IPL reached 96.4 %, 86.0 %, and 89.2 %, respectively. UiO-66-SO 3 H could be simply recovered and reused, but the catalytic performance was significantly decreased. The FUR conversion and IPL yield dropped to 73.8 % and 65.1 %, respectively, after 1 cycle, and the reason for the decrease in the catalyst activity were also investigated. It was found that the decrease was mainly caused by the loss of some −SO 3 H groups, and the cyclic performance of UiO-66-SO 3 H could be restored by supplementing a small amount of BDC-SO 3 Na. A plausible mechanism for the selective synthesis of IPL from FUR was proposed, wherein both Lewis acid and Brønsted acid sites played important roles. This work provides guidance for the selective conversion of FUR into IPL, and the high-valued utilization of biomass and its derivatives.
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RSC Advances
·
2018
·Vol. 8
·期 18
·10009-10016
·
IF 2.936
Zichen Xu,Guoying Zhao,Latif Ullah,Meng Wang,Aoyun Wang,Yanqiang Zhang,Suojiang Zhang
A facile strategy for the synthesis of acidic ionic liquid based UiO-67 type MOFs was developed in this study. Brønsted acids (H2SO4, CF3SO3H and hifpOSO3H (hexafluoroisopropyl sulfuric acid)) were introduced into UiO-67–bpy (bpy = 2,2′-bipyridine-5,5′-dicarboxylic acid) frameworks by reacting with bipyridyl nitrogen to introduce the properties of an acidic ionic liquid into the frameworks. The prepared catalysts, denoted as UiO-67–HSO4, UiO-67–CF3SO3 and UiO-67–hifpOSO3, were characterized by XRD, SEM, FT-IR, EA, TGA and N2 adsorption–desorption studies. The relatively high surface area was still maintained and acidic active groups were uniformly dispersed in the frameworks. The catalytic performance of UiO-67–HSO4, UiO-67–CF3SO3 and UiO-67–hifpOSO3 was evaluated by the esterification of acetic acid with isooctyl alcohol. The prepared catalysts showed good catalytic activities in the esterification, of which UiO-67–CF3SO3 gave the maximum isooctyl alcohol conversion of 98.6% under optimized conditions. The catalyst could be reused five times without a significant decrease in the conversion of isooctyl alcohol, and almost no active species were leached, indicating the excellent stability and reusability of the catalyst. Our study provides one effective way to synthesize heterogeneous acidic ionic liquid catalysts consisting of isolated, well defined acidic groups that will probably attract interest in acid catalyst chemistry.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2024
·
IF 3.2
Yi Wang,Tao He,Siying Lv,Jing Yang,Shihai Cui
Novel type of micro mesoporous materials Co-doped NH 2 -UiO-66 had been successfully prepared. The properties of the material were understood through a series of characterization. When the dosage of Zr:Co is 2:1, the modified material showed specific surface area of 840.02 m 2 ∙g −1 , which is larger than the material without Co. Especially, the material was transformed from microporous NH 2 -UiO-66 to micro-mesoporous Co-doped NH 2 -UiO-66 through the adjustment of metal Co. The Co-doped nanocomposite was then applied to the adsorption of oxytetracycline. The effects of initial concentration, pH, humic acid and ionic strength on the adsorption were investigated. It was found that 50 mg∙L −1 oxytetracycline can be effectively adsorbed by Co-doped NH 2 -UiO-66 in pH 7. Further research showed that adsorption was pseudo-second-order kinetics and fitted Freundlich model with the maximum adsorption capacity 223.7 mg∙g −1 . In addition, the adsorption equilibrium time was only 2 h, which is shorter than the adsorption time of most adsorbents. The mechanism of pore adsorption, π-π interaction, hydrogen bonds and electrostatic interactions was deeply discussed. In conclusion, Co-doped NH 2 -UiO-66 was a fast and effective absorbent for the removal of oxytetracycline in aqueous solution.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2024
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IF 4.3
Ming-Qin He,Hong-Wei Li,Yuqing Wu
Nitrite is a commonly used food preservative and a water contaminant that has garnered significant attention due to its harmful effects on human health. Developing a simple and sensitive method for determining nitrite levels is crucial for safeguarding public health. In this paper, we present a novel ratiometric fluorescent nanosensor (CDs@UiO-66-NH 2 ), created by combining orange-red-emitting CDs with blue-emitting UiO-66-NH 2 . This ratiometric probe detects nitrite ions (NO 2 − ) based on the diazotization reaction between the amino group in UiO-66-NH 2 and the target NO 2 − , where the blue emission of UiO-66-NH 2 is quenched but the orange-red emission of CDs remains stable. The probe demonstrated a detection range of 0.5–20 μM with a limit of detection (LOD) of 0.157 μM for NO 2 − . Due to the probe’s distinct color changes in response to NO 2 − , RGB values can be easily read using a smartphone, enabling ultrasensitive visual detection of NO 2 − with an LOD of 0.76 μM. This sensor was successfully applied to detect NO 2 − in environmental water samples. Finally, a smartphone-based RGB reading method using CDs@UiO-66-NH 2 for visual quantitative detection of NO 2 − was proposed, broadening the application of CDs@UiO-66-NH 2 in environmental protection.
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BIOCHEMICAL AND BIOPHYSICAL RESEARCH COMMUNICATIONS
·
2024
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IF 2.5
Liuxuan Yang,Xianbin Liu,Jing Yang,Ke Wang,Zhenghao Ai,Jinlu Shang,Meiling Zhou
Acute pancreatitis (AP) is a severe inflammatory condition with a rising incidence and high mortality rates, especially in severe cases. Emodin (ED), known for its potent anti-inflammatory properties, holds promise in addressing AP. However, its clinical application is hindered by limitations such as low bioavailability and insufficient target specificity. Herein, we developed a novel drug delivery system using macrophage membrane-coated UiO-66-NH 2 nanoparticles loaded with ED (MVs-UiO-ED). UiO-66-NH 2 was successfully synthesized and characterized, revealing an octahedral structure with a suitable size distribution. The successful loading of ED onto UiO-66-NH 2 was confirmed by ultraviolet and infrared spectroscopy. Subsequently, MVs-UiO-ED was prepared by coating macrophage membrane-derived vesicles onto UiO-ED, resulting in a biomimetic delivery system. In vitro release studies demonstrated that MVs-UiO-ED exhibited a sustained-release profile, indicating its potential for prolonged drug circulation. An AP mouse model was established to evaluate the therapeutic efficacy of MVs-UiO-ED. Compared with the model group, MVs-UiO-ED significantly reduced serum levels of α-amylase and lipase, two indicators of pancreatitis severity. Furthermore, histopathological examinations revealed that MVs-UiO-ED ameliorated pancreatic tissue damage. This study underscores the potential of MVs-UiO-ED as an effective therapeutic approach for AP.
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