FUEL
·
2024
·
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.
研究领域:
化学工程
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催化科学
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可再生资源利用
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Keli Li,Mengli Li,Changsheng Su,Long Deng,Zheng Yan,Hongxia Shen,Yang Jiao,Xuebo Cao
Abundant porosity, sufficient active sites, and appropriate stability are crucial factors for metal–organic frameworks (MOFs) designed for photocatalysis. Herein, a controllable partial pyrolysis strategy was employed to synthesize hierarchically porous UiO-66-X (X denotes the mass ratio of H2BDC-NH2 in ligands) with adjustable coordinated unsaturated zirconium sites and interconnected mesoporous structure. By taking full advantage of linker instability in MOFs, which is usually viewed as an undesirable trait of MOFs, this controllable thermolysis involved heat treatment of the original UiO-66-X, leading to selective partial decomposition and permanent mesopores within the structure. Meanwhile, dangling functional amino groups could serve as anchoring sites for cocatalyst and CO2 molecules. Cu nanoclusters were successfully incorporated into hierarchically porous MOFs by a structure engineering approach, yielding a novel photocatalyst. A mutually active mechanism was put forward and illustrated in this work. Mechanistic investigation reveals that mesoporous structures in a catalyst not only offer three-dimensional (3D) interconnected gas transport channels but also provide sufficient space for accommodating the introduced Cu nanoclusters, which served as active sites and efficiently induced a CO2 photoreduction reaction. At the optimal ratio, the photocatalyst exhibited superior photocatalytic activity, achieving a CO yield of 121.64 μmol g–1 under 5 h of the stimulated solar irradiation without any photosensitizer.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Yujuan Xie,Jinghua Han,Fengchao Li,Lingfei Li,Zhenghao Li,Qian Li,Zhaoting Shang,Wangting Lu,Yazhen Wang,Fan Yu,Wei Yan,Yun Zheng,Jiujun Zhang
Introducing advanced conductive nanoparticles to combine with metal-organic frameworks (MOFs) as electrode is emergingly regarded as a practical and efficient approach to improve the capacitive performance of supercapacitors. Herein, a new MOF (ZrNi-UiO-66, Nickel-zirconium 1,4-dicarboxybenzene) is designed to combine with carbon quantum dots (CQDs) to form a composite electrode with high specific capacitance, in which the charge regulation is performed to facilitate the electronic conduction and transfer. Such constructed electrode delivers an enhanced electronic conductivity and an improved specific capacitance of 2468.75 F g −1 @ 1 A g −1 , which is four times of the contrast sample. Meanwhile, the assembled hybrid supercapacitor exhibits an increased energy density and power density, as well as a sustainable stability after 10,000 cycles with a retention rate of 91.6 %. Basing on the study of advanced characterizations and density functional theory (DFT) simulation, the mechanism of significantly improved specific capacitance can be elaborated as the promote electronic conduction caused from narrowed band gap from 3.9 eV or 0.41 eV–0.23 eV, and the increased charge accumulation at the Ni sites in designed MOFs. This work provides new insights for the design and construction of potential energy storage materials based on MOFs and/or advanced carbon-based materials.
研究领域:
材料科学
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能源存储
·
纳米技术
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Douhao Yang,Ruiting Jian,Jianjun Yan,Ao Zhang,Bowen Liu,Zhongwei Liu
Defect engineering has a great effect on the properties of metal–organic frameworks (MOFs). In this study, the defective UiO-66-NH2 MOFs are successfully prepared by a rapid Ar plasma modification method. At certain experimental conditions (15 W radio frequency input power, 20 Pa working pressure, and 120 s Ar plasma modification time), the afforded UiO-66-NH2 shows significant enhancement in photocatalytic reduction of Cr(VI), and a maximum reduction efficiency of 68.5% is obtained. Advanced characterizations show that the plasma treatment generates missing-linker defects within the UiO-66-NH2 structure, which can enhance the separation of photogenerated electrons and holes and improve the photoreduction capability. The findings not only contribute to a better understanding of the relationship between the structure and performance of MOFs but also provide a simple approach for defect engineering of MOFs.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
BIOCHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 3.8
Rui Zhao,Wenhui Yang,Pengyan Yang,Yunhan Cao,Fenghuan Wang
Carbonic anhydrase (CA) has been suggested as a biocatalyst for carbon dioxide capture since it could effectively catalyze the hydration of carbon dioxide. Metal-organic frameworks (MOFs) have attracted significant attention in the development of immobilized enzyme carriers due to their pore tunability and excellent stability. In this study, UiO-67 materials with varying defect degrees (DUiO-67) were prepared using the organic linker missing method to enhance the catalytic performance. The results indicated that both the defect degree and the pore size of DUiO-67 materials decreased with an increase in acetic acid equivalent. After CA immobilization, all DUiO-67 materials exhibited excellent thermal, pH and recycling stability. CA@DUiO-67–25 showed higher enzyme catalytic activity and conversion ability than the other materials. After 10 cycles, CA@DUiO-67–25 retained 57 % of its initial conversion capacity. The construction of defective MOFs provides a promising new strategy for CA immobilization to achieve the catalytic conversion of CO 2 .
研究领域:
材料科学
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生物催化
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2020
·Vol. 10
·期 25
·14778-14784
·
IF 3.119
Shujian Sun,Peisen Liao,Lihua Zeng,Lanqi He,Jianyong Zhang
Robust UiO-67 metal–organic framework nanoparticles have been precisely and uniformly anchored on the surface of a photonic crystal via metal–organic gelation, resulting in a nanoscale UiO-67 composite. Mott–Schottky measurements indicate that UiO-67/B is an n-type semiconductor with electron conduction, and the band gap significantly decreases with the assistance of the photonic crystal matrix with a band gap of 0.75 eV. Benefiting from the abundant photoelectrons trapped from the photonic crystal, good hydrogen evolution reaction performance is achieved under light irradiation. The current density increases from 3.2 to 7.0 mA cm−2 at −0.6 V (vs. RHE) for UiO-67/B. The optimized carrier density obtained from UiO-67/B is apparently increased 2.15 times under light irradiation for 30 min. This work provides a rational strategy to address the photo-capture and energy transfer issues of metal–organic frameworks under visible light irradiation for H2 production in artificial photosynthesis.
研究领域:
材料科学
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光化学
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能源转换
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DOI
高影响因子
PLASMA SCIENCE & TECHNOLOGY
·
2025
·
IF 1.8
Ruiting Jian,Qirui Zou,Jianjun Yan,Bowen Liu,Lijun Sang,Zhongwei Liu
Cr(VI), a hazardous heavy metal pollutant found in wastewater, exerts detrimental effects on biological system and the human body. Efficient photocatalytic reduction of Cr(VI) to Cr(III) using high-performance materials offers a viable approach for chromium decontamination. In the current work, the defective UiO-66-(OH)2 with enhanced photocatalytic activity was developed by the plasma treatment. These defects not only triggered an expansion in mesoporous domains and increased the BET surface area of the UiO-66-(OH)2 system, thereby exposing more adsorption and photocatalytically active sites, but also created additional electron migration pathways, enhancing the separation of photogenerated e-/h+ pairs. When subjected to an operating power of 15 W, chamber pressure at 20 Pa, and a 300-second treatment period, UiO-66-(OH)2 exhibited a removal efficiency of 83 %. This work explored a novel way for the construction of the defective MOFs and broadened the utilizationation of MOFs in the fields of photoreduction of heavy metal ions in water.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
高影响因子
MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 6
·1-10
·
IF 5.3
Ma Jinzhu,Shi Yu-e,Song Qian,Kou Shufang,Wang Zhenguang
Dual-emissive fluorescence probes were designed by integrating porphyrin into the frameworks of UiO-66 for ratiometric fluorescence sensing of amoxicillin (AMX). Porphyrin integrated UiO-66 showed dual emission in the blue and red region. AMX resulted in the quenching of blue fluorescence component, attributable to the charge neutralization and hydrogen bonds induced energy transfer. AMX was detected using (F 438 /F 654 ) as output signals. Two linear relationships were observed (from 10 to 1000 nM and 1 to 100 µM), with a limit of detection of 27 nM. The porphyrin integrated UiO-66 probe was used to detect AMX in practical samples. This work widens the road for the development of dual/multiple emissive fluorescence sensors for analytical applications, providing materials and theoretical supporting for food, environmental, and human safety. Graphical Abstract
研究领域:
分析化学
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食品安全
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Shenyi Tang,Chenglian Luo,Zhi Wang,Xinlei Liu
A defect-free and stable metal–organic framework (MOF) membrane is a promising candidate for the separation of methanol/methyl tertiary butyl ether (MeOH/MTBE) mixtures. In this work, a structural-integrity and low-thickness (∼400 nm) UiO-66 membrane was fabricated by regulating the metal ion/ligand molar ratio in the synthesis solution and optimizing the preparation process using the secondary growth method with safer and more environment-friendly Zr(n-OPr)4 metal source. Based on the effective pore size and inherent amphiphilic structure of UiO-66, the membrane exhibits exceptional pervaporation (PV) performance. For the separation of MeOH/MTBE (5:95 wt/wt %) mixtures, the membrane displays an outstanding separation performance with an average separation factor of 2.23 × 104 and an average total flux of 3.61 kg·m–2·h–1 at 40 °C, which is superior to most membranes reported for the PV separation of MeOH/MTBE mixtures. In addition, a 72 h PV process was used to further confirm the structural stability of the membrane.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2021
·
IF 5.097
Shilin Wang,Shuaikang Fan,Zhou Fang,Yue Hu,Mengyang Dong,Xinsheng Peng
Stimuli-responsive conductive MOF nanoporous materials have been considered to have great potential for photoelectric conversion, information processing, bioelectronics, and smart devices. However, light-regulating hydroxide ion conduction of MOFs is rarely reported. Herein, a reversible optical switch on hydroxide ion conduction has been achieved based on the intrinsic localized photothermal heating of NH2-UiO-66 nanoparticles. The amino group on the organic ligand of NH2-UiO-66 can build a hydrogen-bond network with water molecules to promote hydroxide ion transport in the nanochannel and cause an absorption band in the visible light region. Irradiated by visible light, NH2-UiO-66 nanoparticles can absorb light and convert it into heat, resulting in partial removal of water molecules in the nanopores and destroying the hydroxide ion transport path. Then, the hydroxide ion conductivity decreased by 2 orders of magnitude. When turning off the light, the hydroxide ion conductivity can restore quickly. This work will promote the development of remotely controlled hydroxide ion conductive smart devices.
研究领域:
材料科学
·
光电转换
·
智能设备
✓ 已验证
DOI
高影响因子
FOOD CHEMISTRY
·
2024
·
IF 8.5
Yiran Wang,Xiaolong Sun,Yufeng Zhou,Jiachen Liu,Huayue Zhu,Ru Jiang,Yingjie Miao,Yongqian Fu
Quercetin (QCT) is a flavonoid with significant health benefits, necessitating sensitive detection methods for food safety and quality control . This study presents a novel UiO-66-TCPP ratiometric fluorescent probe for the quantitative and visual detection of QCT. Under optimal conditions, the fluorescence intensity of UiO-66-TCPP decreased linearly with increasing QCT concentration, with a detection limit of 26 nM. The probe demonstrated high specificity, showing no significant interference from various substances and QCT analogues. Practical applicability was confirmed by testing artificially contaminated juice samples, achieving recovery rates between 98.0% and 104.8%. Furthermore, a paper-based sensor was developed by incorporating UiO-66-TCPP onto Whatman#1 chromatography paper . This sensor exhibited stable fluorescence and a reliable, sensitive visual response to QCT concentrations, detectable via a smartphone-based color recognizer application. The UiO-66-TCPP ratiometric fluorescent probe provides a sensitive, specific, and practical method for detecting QCT in food matrices, offering significant potential for both laboratory and on-site applications.
研究领域:
分析化学
·
食品安全
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Yating Xie,Nicui Yuan,Hongyang Liu,Lukai Luo,Jun Gong,Xiping Yin,Tengfei Li,Yonghua Zhou
Defect engineering by creating oxygen vacancies (OVs) and heterogeneous frustrated Lewis acid-base pairs (FLPs) emerged as an efficient strategy to enhance the selective conversion CO 2 to CH 4 . Considering the intrinsic FLPs contained in UiO-66-NH 2 (UNH for abbreviation), in this paper, the OVs was introduced therein by fabricating the Ce-doped UNH (denoted as UNH(Ce/Zr)) via one-step solvothermal route. The as-prepared UNH(Ce/Zr) catalyst exhibited the CH 4 yield of 31.02 μmol·g −1 ·h −1 accompanied with the CH 4 selectivity of 93 % and satisfying recycling stability. The XRD, SEM, FT-IR, XPS, TG, TPD and NH 3 in situ DRIFTS and in situ FT-IR characterization results justified that the UNH(Ce/Zr) possess the obviously increased OVs sites and enhanced Lewis acidic and basic properties. Additionally, the photoelectrochemical characterization results showed that UNH(Ce/Zr)−0.014 efficiently improved photogenerated electron-hole separation efficiency and charge transfer rate. It could be concluded that it was the cooperative action of OVs and FLPs that led to the high CH 4 selectivity and CH 4 yield.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）