RSC Advances
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2019
·Vol. 9
·期 65
·37733-37738
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IF 3.049
Yanghe Fu,Jieyu Wu,Rongfei Du,Ke Guo,Rui Ma,Fumin Zhang,Weidong Zhu,Maohong Fan
Defect engineering can be a promising approach to improve the photocatalytic performance of metal–organic frameworks (MOFs). Herein, a series of defective NH2-UiO-66(Zr) materials were synthesized via simply controlling the synthesis temperature, with concentrated HCl as the modulator and then these as-prepared samples were used to systematically investigate the effects of their structural defects on photocatalytic CO2 reduction. Remarkably, these MOFs with defects exhibit significantly enhanced activities in photocatalytic CO2 reduction, compared with the material without defects. The defect engineering creates active binding sites and more open frameworks in the MOF, and thus facilitates the photo-induced charge transfer and restrains the recombination of photo-generated charges efficiently. The current work provides an instructive approach to improve the photocatalytic efficiency by taking advantage of the structural defects in MOFs, and could also inspire more work on the design of advanced defective MOFs.
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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PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Qingqing Wang,Wei Zhou,Claudia Li,Sibudjing Kawi,Yinhui Li
The application of photocatalysts in environmental field has emerged as a prominent research topic. Nevertheless, the efficiency of photocatalysts is reduced as the recombination of photogenerated chargers significantly, restricting their extensive use in this domain. In the present study, photocatalysts composed of bismuth molybdate/NH 2 -UiO-66(Zr) (Bi 2 MoO 6 /NH 2 -UiO-66(Zr)) featuring Z-scheme heterojunctions were effectively synthesized using a two-step hydrothermal technique. These photocatalysts exhibit remarkable photocatalytic degradation under visible light conditions. Notably, the broad planar configuration of Bi 2 MoO 6 sheets improves the separation of the photogenerated charge carriers. NH 2 -UiO-66(Zr) layered atop Bi 2 MoO 6 sheets enhances the availability of catalytically active sites, reduces charge recombination, and promotes charge transfer through the interface. The kinetic rate constant for Bi 2 MoO 6 /NH 2 -UiO-66(Zr) is around 0.00329 L mg −1 min −1 , indicating the increase of 3.78 and 41.13 times compared with pure Bi 2 MoO 6 and NH 2 -UiO-66(Zr), respectively. The efficiency for photocatalytic degradation of tetracycline using Bi 2 MoO 6 /NH 2 -UiO-66(Zr) reaches 81.72 % under visible light. Importantly, this efficiency exhibits a reduction of 10 % after five recycling cycles, demonstrating notable stability. The photocatalytic mechanism involved in tetracycline degradation was uncovered through trapping experiments and EPR, indicating that it is predominantly facilitated by the active oxidation of ·O 2 - and ·OH. The intermediates of the photocatalytic process as well as the possible degradation pathways were discussed. The creation of Bi 2 MoO 6 sheets/NH 2 -UiO-66(Zr) heterojunction photocatalysts provides a fresh approach to the development of novel catalysts, which may lead to significant advancements in environmental remediation efforts.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
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2013
·Vol. 19
·期 42
·14279-14285
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IF 5.831
Dengrong Sun,Yanghe Fu,Wenjun Liu,Lin Ye,Dengke Wang,Lin Yang,Xianzhi Fu,Zhaohui Li
Graphical Higher CO 2 photoreduction activity than previously studied metal–organic framework (MOF) NH 2 -MIL-125(Ti) in the presence of triethanolamine (TEOA) as the sacrificial agent under visible light is exhibited by the amino-functionalized MOF NH 2 -Uio-66(Zr). The photoinduced electron transfer from 2-aminoterephthalate linkers to Zr oxo clusters was revealed for the first time by photoluminescence studies, and the generated Zr III was detected by ESR analysis (see figure). Metal–organic framework (MOF) NH 2 -Uio-66(Zr) exhibits photocatalytic activity for CO 2 reduction in the presence of triethanolamine as sacrificial agent under visible-light irradiation. Photoinduced electron transfer from the excited 2-aminoterephthalate (ATA) to Zr oxo clusters in NH 2 -Uio-66(Zr) was for the first time revealed by photoluminescence studies. Generation of Zr III and its involvement in photocatalytic CO 2 reduction was confirmed by ESR analysis. Moreover, NH 2 -Uio-66(Zr) with mixed ATA and 2,5-diaminoterephthalate (DTA) ligands was prepared and shown to exhibit higher performance for photocatalytic CO 2 reduction due to its enhanced light adsorption and increased adsorption of CO 2 . This study provides a better understanding of photocatalytic CO 2 reduction over MOF-based photocatalysts and also demonstrates the great potential of using MOFs as highly stable, molecularly tunable, and recyclable photocatalysts in CO 2 reduction.
研究领域:
材料科学
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环境科学
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DOI
PubMed
高影响因子
Journal of Physical Chemistry C
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2023
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IF 3.7
Huan-Yu Chen,Xing-Biao Liu,Qi-Xin Guan,Can-Jun Zou,Ping-Ping Fang
The detection of antibiotics has attracted great attention among scientists and health researchers in the past decades. However, it is still difficult to realize the sensitive and selective detection of antibiotics with similar structures. Herein, the antibiotic molecules of oxytetracycline (OTC) can be sensitively and selectively detected by surface-enhanced Raman spectroscopy (SERS) on NH2–UiO-66(Zr)@Au nanoparticles (NPs). The SERS substrate of NH2–UiO-66(Zr)@Au NPs realizes a detection sensitivity of 1 × 10–12 g·L–1 for 4-mercaptobenzoic acid, indicating its high SERS activity. A high detection sensitivity of 10–11 g·L–1 is obtained for OTC on such a SERS substrate. Besides the high sensitivity, NH2–UiO-66(Zr)@Au NPs can also selectively detect OTC from streptomycin sulfate, salicylic acid, and ofloxacin by SERS on NH2–UiO-66(Zr)@Au NPs, with a selective detection limit of 10–10 g·L–1. Furthermore, OTC can be selectively detected in a real sample of river water with a detection limit of 1.0 × 10–10 g·L–1. Therefore, this study provides an effective way to enrich and detect antibiotics in real samples in the environment.
研究领域:
分析化学
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环境科学
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材料科学
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纳米技术
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高影响因子
Desalination and Water Treatment
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2024
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IF 1
Honghuan Yin,Huaiwen Wang,Dongai Wang,Miaomiao Shi,Xi Xu,Jiaqi Yang
Developing low-cost and stable adsorbent is urgent and attractive to remove hazardous dye from water. In this study, zirconium based metal-organic framework (NH 2 -UiO-66) was grown on waste wool fibers and the fabricated composite adsorbent (NH 2 -UiO-66/wool) was used to remove anionic dye methyl orange (MO). After characterizing the adsorbents, we determined the effect of pH and initial concentration of MO on adsorption performance. Moreover, adsorption kinetics and isotherms were conducted to reveal the adsorption mechanism. The results showed that NH 2 -UiO-66/wool achieved the highest adsorption capacity at natural pH with the maximum adsorption of 61.0 mg/g adsorbent, which is higher than most biomass based adsorbents. Moreover, NH 2 -UiO-66/wool enabled a broad range of pH (3−11) and initial concentration of MO (10–50 mg/L). Adsorption kinetics and isotherms of NH 2 -UiO-66/wool fitted well with pseudo-second-order model and Langmuir mode, respectively. NH 2 -UiO-66/wool presented 40.3 times higher of kinetics constant than that of original wool in the presence of initial MO concentration of 10 mg/L due to the positive nature of NH 2 -UiO-66. Ultimately, NH 2 -UiO-66/wool presented excellent regeneration ability with 500 mg/L NaCl solution and regeneration efficiency remained 98% after 10 cycles. Overall, this work may provide new insights into the development of MOFs/wool adsorbents for enhanced dye removal.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
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2025
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IF 4.6
Mingming Dong,Shuyong Yang,Peng Zhou,Yue Gao,Anshun Wang,Shenghui Tu
The accumulation of antibiotics in aquatic ecosystems poses a serious threat to the environment and to human health. Tetracyclines (TC) account for a significant proportion of antibiotic residues worldwide. In order to overcome the limitations of conventional degradation methods, we created a three-component S-scheme heterojunction consisting of BiVO 4 /MWCNTs@NH 2 -UiO-66 (Zr) using a two-step solvothermal process. This synergistic integration utilises: (i) MWCNTs as electron transport bridges; (ii) NH 2 -UiO-66 (Zr) for high TC adsorption (surface area of 931.86 m 2 g −1 ); and (iii) BiVO 4 for visible light harvesting. This architecture broadens light absorption, reduces charge recombination and enables dual-pathway Reactive Oxygen Species (ROS) generation. Under visible light, the optimised catalyst achieves 95.2 % TC degradation within 90 min–7.73 times faster than pristine BiVO 4 (k = 0.02721 vs. 0.00352 L mg −1 ·min −1 ). Radical trapping and EPR analyses confirm ·O 2 − and h + as the dominant species, while LC-MS reveals three degradation pathways. With 85.3 % activity retention after five cycles, this work provides a blueprint for the design of efficient, antibiotic-mineralising photocatalysts.
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DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2022
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IF 3.898
Xueting Liu,Chunhui Hu,Jingjing Wu,Peng Cui,Fengyu Wei
In this study, a series of metal–organic frameworks (MOFs) NH 2 -UiO-66- x HAc catalysts were synthesized by solvothermal method using acetic acid (HAc) as a modulator, and were applied to the cycloaddition of CO 2 and epichlorohydrin (EPIC) under ambient pressure. Influences of the modulation by HAc on morphologies and structures of the MOFs are demonstrated via PXRD, FESEM, FTIR, N 2 adsorption–desorption, XPS and 1 H NMR characterizations. The results show that the MOFs containing mesoporous pores can be prepared by adjusting the concentration of HAc. By optimizing the amount of HAc added, the specific surface area of NH 2 -UiO-66-8HAc is as high as 879.17 m 2 ·g −1 , which is 28.3% higher than that of the original MOFs. And the evaluation of catalytic performance showed that HAc modulation enhanced the activity of NH 2 -UiO-66- x HAc under mild conditions. The exposure of Lewis acid sites, increased specific surface area and porosity via the modulation of HAc defective ligand can be supposed the key factors to determine the enhanced catalytic activities. In addition, considering the influence of gas concentration on the reaction, the concept of TOP (Turnover of Pressure, defined as the mass of conversions of a unit mass catalyst under unit pressure and unit time) was first proposed in this article.
研究领域:
化学
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材料科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.7
Haileyesus Hatano Haitosa,Osman Ahmed Zelekew,Pu Chen,Daniel Manaye Kabtamu,Weimao Yan,Hong Wang,Yi-nan Wu
Fluoroquinolone antibiotics like ciprofloxacin (CIP) pose environmental risks when released into water. Herein, a visible-light-active Fe-doped NH 2 -UiO-66(Zr)@AgI Z -scheme heterostructure was prepared via an ion exchange precipitation method. By varying AgI content, reduced particle size and enhanced charge separation for efficient photodegradation was achieved. The optimum composition (Fe-UNH@AgI-20) exhibited a 95.2 % degradation efficiency toward CIP after 60 min of visible-light irradiation. It also showed high removal efficiencies for tetracycline, lomefloxacin, and Rhodamine B. Reaction kinetics followed pseudo-first-order behavior, with rate constants significantly higher than those of pristine NH 2 -UiO-66(Zr) and AgI. The catalyst maintained 85.1 % activity after cycles, indicating good stability. Scavenger tests and electron paramagnetic resonance (EPR) analyses identified holes (h + ), superoxide radical (•O 2 − ), and hydroxyl radical (•OH) as key reactive species. Fe doping enhanced visible-light absorption and created defect sites, while AgI introduction promoted charge separation and suppressed AgI photocorrosion. Under irradiation, a small fraction of Ag + was reduced to metallic Ag, forming an electron bridge that switched the initial type-II heterojunction to a Z -scheme configuration. This Z-scheme mechanism efficiently separated carriers, facilitated generation of ROS, and enabled thorough mineralization of CIP; toxicity predictions showed most products were less mutagenic than CIP, confirming reduced ecological risk. The findings demonstrate that the Fe-doped NH 2 -UiO-66(Zr)@AgI heterostructure is a promising photocatalyst for antibiotic-contaminated wastewater remediation.
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PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2024
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IF 7.4
Zewan Qin,Qing Guan,Yating Lu,Yu Tian,Xia Yang
The naphthalene tetracarboxdiimide (NDI) modified NH 2 -UiO-66(Zr) and NH 2 -MIL-101(Cr) (NDI/UZr and NDI/MCr for short) metal organic frameworks (MOFs) materials with strong covalent bond O C–N–C O were designed and prepared by solvothermal method. The comprehensive physical and chemical properties of the materials were characterized, and the adsorption and photocatalytic properties of the materials were evaluated by using methylene blue (MB) and Cr(VI) in single and mixture system. When the initial concentration of MB was 50 mg·L −1 , the photocatalytic degradation rate constant of NDI/MCr(2:1) was 10.3 and 13.8 times higher than that of NH 2 -MIL-101(Cr) and NDI/UZr(2:1), respectively. Additionally, NDI/MCr(2:1) exhibited 1.6 times higher reaction rate constant than that of NDI/UZr(2:1) for the removal of 10 mg∙L −1 Cr(VI). The enhanced adsorption and photocatalytic ability over NDI/MOFs were attributed to the MOFs larger specific surface area and wider spectral response, and NDI showed high electron affinity, superior charge carrier transport properties. Free radical and electron capture experiments indicated that h + , •O 2 − , and e − were the main active species in the NDI/MOFs system. Among them h + and •O 2 − played an essential role in the removal of MB, while e − and •O 2 − contributed to the photocatalytic reduction of Cr(VI). The mechanism of the photocatalytic process was discussed in detail.
研究领域:
材料科学
·
环境工程
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化学工程
·
光催化
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高影响因子
危险品化学品经营许可证（带存储）