COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Lili Ma,Xueting Feng,Fanghui Cai,Chunyu Sun,Hanming Ding
Metal-organic frame materials are intensively investigated in catalysis due to their outstanding thermal stability, large specific surface area, and ultra-high porosity. In this work, a cobalt-doped zirconium-based metal-organic framework, Co-UiO-66, was synthesized by the hydrothermal approach. Co-UiO-66 could successfully activate peroxymonosulfate (PMS) ions to produce reactive oxygen species for the degradation of rhodamine B (RhB) when it was used as a Fenton-like catalyst. The catalyst with 4% Co in mass in UiO-66 (4% Co-UiO-66) showed the highest degradation efficiency. About 97.3% of RhB (50 ml of 30 mg L −1 ) was degraded in 45 min under simulated sunlight when 10 mg of 4% Co-UiO-66 was used. The degradation efficiency was much higher than that when pure UiO-66 was used. Furthermore, it was even slightly higher than when cobalt ions were used as the activator. The single-atomic dispersion and confinement effect in Co-UiO-66, as well as the strong absorption in the visible light region are responsible for the high catalytic efficiency.
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 6
·2567-2576
·
IF 4.569
Aijia Gao,Fangfang Li,Zhi Xu,Changchun Ji,Jing Gu,Ying-Hua Zhou
The development of heterogeneous catalysts for promoting epoxide cycloaddition with carbon dioxide is highly desirable for recycling CO2 and achieving the goal of carbon neutrality. Herein, we designed and synthesized Zr-based metal organic frameworks (MOFs) by implanting functional guanidyl into the framework via mixing different molar ratios of 4-guanidinobenzoic acid (Gua) with 1,4-benzenedicarboxylic acid (BDC). Consequently, a small sized Zr-MOF (∼350 nm) can be prepared by implanting Gua with 20% molar ligands, denoted as UiO-66-Gua0.2(s). Compared to large sized and different guanidyl Zr-MOFs, UiO-66-Gua0.2(s) exhibited an optimal activity on catalyzing epoxide cycloaddition with CO2 in the presence of the Bu4NBr cocatalyst. A yield of 97% for the product of chloropropene carbonate was achieved at 90 °C under 1 atm CO2. The great performance of UiO-66-Gua0.2(s) might be attributed to the synergistic effect of guanidyl groups as hydrogen-bond donors and Zr centers acting as Lewis-acidic sites. In addition, the heterogeneous catalyst of UiO-66-Gua0.2(s) exhibited a great versatility towards converting other epoxides and a satisfactory recyclability for five consecutive runs. Moreover, a plausible reaction mechanism has been proposed for UiO-66-Gua0.2(s) in promoting CO2 epoxide cycloaddition reactions.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2023
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IF 6.1
Qin Zhang,Lijiao Fan,Wenbin Liu,Yuming Xie,Jiangang Li,Guolin Huang
The core–shell structure UiO-66-NH 2 @Ni-MOF was prepared by in-diffusion growth of 2D Ni-MOF on UiO-66-NH 2 using PVP (polyvinylpyrrolidone) as a structural guide. It was applied to the adsorption of U(VI) in aqueous solution. The materials were characterized by powder X-ray diffraction (PXRD), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and energy dispersive spectrometer (EDS). The UiO-66-NH 2 @Ni-MOF adsorption to U(VI) was investigated experimentally. The study showed that the adsorption of U(VI) onto UiO-66-NH 2 @Ni-MOF was endothermic and spontaneous. At pH 5.00 and 308 K, the adsorption capacity was 581.40 mg/g according to Langmuir model. In addition, the adsorption process can be described by the pseudo-second-order kinetic model. The adsorption capacity was kept at 83.83% of its original one after five sorption–desorption cycles, a promising indication for repetitive usage.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Yunlong Li,Miao Liu,Yixian Liu,Lilong Zhou,Jilong Han,Zhengjie Li,Jimmy Yun,Runjing Liu
Two kinds of Ce-doped UiO-66 were synthesized by using CeCl 3 ·7H 2 O and (NH 4 ) 2 Ce(NO 3 ) 6 as cerium precursors, namely Ce(III)- and Ce(IV)-UiO-66. The effect of valence states of cerium precursors on adsorption performance towards Rhodamine B (RhB) was investigated for the first time. Ce atoms are in two valence states of +3 and + 4, where Ce 3+ ions turn their surfaces negatively charged. The higher cerium content (24.8%) and ratio of Ce 3+ /Ce 4+ ions (1.4:1) of Ce(IV)-UiO-66 made its surface more negatively charged, which is contributed to form stronger electrostatic interaction with cationic dyes. The adsorption amounts of RhB were 239.5 mg/g and 431.7 mg/g for Ce(III)- and Ce(IV)-UiO-66, which are 2.38 and 5.11 times higher than pristine UiO-66, respectively. The well-fit Langmuir model and pseudo-second-order model suggest a monolayer chemisorption process. The adsorption mechanism suggests that the electrostatic interaction and the complexation interaction between Ce 3+ and RhB are dominant factors affecting RhB adsorption. Since Ce 3+ severed as adsorption sites, the higher Ce content and stronger electrostatic interaction of Ce(IV)-UiO-66 together promoted its RhB adsorption than Ce(III)-UiO-66. The obtained results help to understand how the mixed-valences of incorporated metals affect the adsorption behaviors of bimetallic MOFs deeply.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Wenqian Zhao,Xu Zhang,Chang Li,Lusheng Xu,Qin Meng,Guoliang Zhang
Adding nanomaterials such as metal–organic frameworks (MOFs) into a polyamide (PA) layer to prepare forward osmosis (FO) membranes for efficient desalination has attracted great attention. However, rational design and preparation of high-quality MOF-based PA nanocomposite forward osmosis membranes still remain a big challenge. In this study, a polyamine (PA) forward osmosis (FO) membrane was fabricated via interfacial polymerization (IP) with the assistance of a UiO-66 nanocomposite interlayer to enhance desalination and antifouling performances. Polydopamine (PDA) and polyethyleneimine (PEI) were codeposited with UiO-66 and formed a hydrophilic nanocomposite intermediate layer. The substrate with the PDA/PEI/UiO-66 interlayer had better hydrophilicity, restricting the diffusion of m-phenylenediamine (MPD) and promoting the formation of a defect-free active layer. In addition, the PDA/PEI/UiO-66 interlayer not only provided additional water channels but also enhanced the interaction of the substrate and PA layer. The water flux of the PA-PDA/PEI/UiO-66 membrane reached 40.0 L m–2 h–1 with a low reverse salt flux (3.2 g m–2 h–1). Moreover, the PA-PDA/PEI/UiO-66(0.1) membrane also possessed excellent antifouling performances with a high flux recovery of 98% and a low total fouling rate of 17%, which were 18.4% higher and 43.3% lower than those of the pristine TFC membrane, respectively. These results presented that the codeposition of the PDA/PEI/MOF interlayer greatly improved the desalination and antifouling performances of the PA FO membrane.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 51
·111039-111050
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IF 5.8
Dong Shiwen,Liu Xuan,Kong Xianxian,Dong Feilong,Yu Yan,Wang Lizhang,Wang Da,He Zhiqiao,Song Shuang
Metal-organic frameworks (MOFs) and covalent organic frameworks (COFs) have been proved as efficient catalysts for photocatalytic hydrogen (H 2 ) evolution, thanks to their tunable functionalities, permanent porosity, excellent visible light response, and physicochemical stability. Herein, a series of photocatalysts (termed NUBC) was fabricated by loading different amounts of Zr-UiO-66-NH 2 (NU) onto a benzoic acid–modified covalent triazine–based framework (BC) based on post-synthetic covalent modification. The resulting NUBC catalysts exhibited a type-II Z-scheme heterojunction structure formed via the amide covalent bonds between the amine groups on NU and carboxyl groups on BC. The optimal loading of NU on BC is 30 wt.% (30NUBC) and the corresponding photocatalytic H 2 evolution rate was 378 μmol h −1 g −1 , almost 445 and 2 times than that of NU and BC, respectively. The synergistic effect between the type-II Z-scheme heterojunctions and amide bonds was conducive to boosting visible light harvesting and facilitating charge transportation and separation. Furthermore, the prepared NUBC catalysts show great reusability and stability. Overall, this work sheds light on the design of novel MOF/COF hybrid materials and provides a systematic exploration of their photocatalytic H 2 evolution properties.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jiayou Liu,Xiaoxiang Huang,Lizhen Hu,Penglei Liu,Liuhu Jia,Keiko Sasaki,Zhongchao Tan,Hesheng Yu
Simultaneous avoidance of secondary air pollution and catalyst deactivation remains a challenge for existing photocatalytic removal of nitric oxide (NO). Herein, a photocatalysis-adsorption (P-A) heterojunction is synthesized for eco-friendly NO removal by facilely grinding Pd single atoms (Pd 1 ) anchored g-C 3 N 4 (48CN/Pd) with UiO-66-NH 2 (UION). Under visible-light irradiation, the 40UION-CN/Pd composite shows 93.91 % of NO removal efficiency with only 2.73 % of NO 2 emissions and negligible catalyst deactivation. The DeNO x index increases remarkably from −0.66 for 48CN/Pd to 0.86 for 40UION-CN/Pd. Furthermore, the synthesized P-A heterojunction efficiently removes NO from real flue gases produced by a domestic coal-fired stove and from SO 2 -rich flue gases. The mechanism exploration based on experimental investigations and density functional theory (DFT) calculations reveals that UION captures the NO 2 selectively produced by 48CN/Pd, simultaneously suppressing NO 2 emissions and refreshing active sites for NO photooxidation. Moreover, the results of X-ray photoelectron spectroscopy (XPS), charge density difference calculation, energy-resolved distribution of electron traps (ERDT) and in-situ Kelvin probe force microscopy (KPFM) reveal that the built-in electric field and Type-II heterojunction formed between 48CN/Pd and UION promote the separation of photogenerated carriers, enhancing the catalytic activity of the composite. This work provides an innovative strategy to avoid NO 2 emission and catalyst deactivation during photocatalytic NO removal.
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CHEMOSPHERE
·
2023
·
IF 8.8
Xiule Wang,Fanyong Yan,Ying Chen,Xinyi Bai,Yang Fu
Metal organic frameworks (MOFs) possess a large surface area, inherent porosity and high crystallinity . Nevertheless, they lack electron acceptors, which limit the exploitation of their photocatalytic properties. Carbon dots (CDs) known for excellent optical properties can serve as localized electron acceptors. As a novel hybrid nanomaterial , the structure of CDs@MOFs effectively facilitates charge separation and carrier transfer, bring about a marked improvement of photocatalytic activity. In this study, yellow-emission carbon dots (YCDs) were encapsulated within zirconium-based metal organic framework (UiO-66) via a dynamic adsorption method. Compared with blue carbon dots (BCDs), the YCDs@UiO-66 exhibited superior degradation performance. It demonstrates that incorporation of YCDs broadens the UV absorption range of UiO-66, thereby enhancing light utilization. The degradation efficiency of YCDs@UiO-66 was 92.6%, whereas UiO-66 alone achieved only 63.1%. Notably, the results of the radical quenching experiment and electron paramagnetic resonance (EPR) revealed that h + and •O 2 − played a prominent role in the photodegradation of tetracycline hydrochloride (TCH). This study highlights that the introducing YCDs in MOFs-mediated photocatalytic reactions is a viable strategy to improve catalytic efficiency.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Siyu Liu,Jianhua Zu,Gang Han,Xiaohan Pan,Yi Xue,Jingjie Diao,Qing Tang,Mingjie Jin
137 Cs is a radioactive pollutant in the production of wastewater from nuclear power plants. In this study, a rapid and simple in-situ synthesis new method was employed to prepare a novel AMP-functionalized UiO-66 composite material for the selective capture of 137 Cs from low-level radioactive wastewater. Characterization techniques such as SEM-EDS, FTIR, XRD, TG, and BET were used to confirm the successful loading of AMP on the surface of UiO-66. UiO-66/AMP showed a good removal effect in pH4-11. At pH7, the effects of different parameters, such as the initial Cs concentration, the ratio of the amount of adsorbent to the volume of solution, and the adsorption time were investigated. The adsorption efficiency is 96.7%, the maximum adsorption capacity is 94.9 mg/g and has fast adsorption kinetics (90% Cs + removal within 5 min). The adsorption data conformed to the pseudo-second-order kinetic model and Langmuir isotherm model, suggesting a monolayer homogeneous adsorption process. XPS helps confirm that the adsorption mechanism is the ion exchange between Cs + and NH 4+ ions. Particularly, in the adsorption experiments of 137 Cs, UiO-66/AMP demonstrated good selectivity (K d Cs : 5.8 × 10 3 ∼ 1.26 × 10 4 mL/g) towards trace Cs + in a mixed ion solution with a molar ratio of 1 (Cs): 2.18 × 10 15 (Na): 4.6 × 10 14 (K): 2 × 10 14 (Mg): 2 × 10 14 (Ca), indicating its potential for selective capture of 137 Cs from low-level liquid waste (LLLW).
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Journal of Materials Chemistry A
·
2023
·Vol. 12
·期 6
·3565-3574
·
IF 11.9
Ling-Chan Tian,Geqian Fang,Yun Zhou,Wenjun Yu,Lin Li,Jin-Nian Hu,Haiyan Wang,Jin-Xia Liang,Chun Zhu,Xiaodong Wang,Jian Lin
Direct selective oxidation of methane (DSOM) to oxygenates under mild conditions is garnering increasing interest. UiO-66-H MOFs are effective for this reaction, while the active configuration of Zr-oxo nodes with adsorbed ˙OH species need further clarification from the atomic/molecular viewpoint. Here, we detect the evolution of the geometric and electronic structures of adsorbed oxygenic species on Zr-oxo nodes of UiO-66-H via the controlled ˙OH species. DFT calculations reveal a volcano-like curve relationship between the quantity of ˙OH species and the DSOM performance, which is further corroborated by experimental tests. Zroxo-˙OH is the main active configuration on Zr-oxo nodes of UiO-66-H at low ˙OH concentration, while it evolves to other oxygenic species (˙OOH, O2, and H2O) due to the self-reaction with the increase of ˙OH concentration, which leads to performance decrease. Furthermore, a critical descriptor of the p-band centers of O atoms in these oxygenic species on the Zr-oxo nodes is established, which can well represent the catalytic activity for the DSOM reaction.
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Biomaterials Science
·
2021
·Vol. 9
·期 7
·2647-2657
·
IF 6.843
Xiaojuan Wang,Xuejian Zhou,Kai Yang,Qiong Li,Rongxin Wan,Guoying Hu,Jin Ye,Yue Zhang,Jiahui He,Hanqing Gu,Yongfang Yang,Lei Zhu
In this study, UiO-66-NH2 metal–organic framework (MOF) nanoparticles with peroxidase and oxidase mimetic activities were incorporated into a chitosan (CS) matrix by a simple and environmentally friendly method. The UiO-66-NH2/CS composite membrane possesses the peroxidase mimicking activity in the presence of traces of H2O2, thus resulting in good antibacterial properties. Intriguingly, 30 min of UV pre-irradiation of the UiO-66-NH2/CS composite membrane, in the absence of H2O2, still leads to a good antibacterial activity. This was attributed to the oxidase mimetic activity and the peroxidase mimicking activity of UiO-66-NH2. In such a way, the side effects of direct exposure to UV irradiation and H2O2 can be avoided for wound-healing treatments. The antibacterial mechanism was further proved by antibacterial experiments, TMB·2HCl color development experiments, reactive oxygen species generation tests and electron spin resonance tests. As a potential medical antibacterial dressing, in vitro membranes were also investigated.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Jiali Tang,Yingbi Chen,Minghu Zhao,Shixing Wang,Libo Zhang
A novel metal-organic framework (UiO-66-PTC) for efficient removal of Pb 2+ ions from wastewater has been prepared by using 4-phenyl-3-thiosemicarbazide as the modifier. Various characterizations showed that UiO-66-PTC was successfully synthesized. The absorption results showed that the maximum adsorption capacity of Pb(II) is 200.17 mg/g at 303 K and optimal pH 5. The adsorption kinetic follows the pseudo-second-order model and the adsorption isotherms fit the Langmuir model. This shows that Pb(II) is a single-layer adsorption on the surface of the adsorbent and the rate-controlling step is chemical adsorption . The thermodynamic results show that the adsorption process can proceed spontaneously, belong to the exothermic reaction . The adsorbent can selectively uptake lead ions from wastewater containing multiple interfering ions. After four adsorption and desorption cycles, the adsorption efficiency is still high. The adsorption mechanism of Pb(II) on the adsorbent is mainly through the chelation of Pb(II) with N and S atoms. These results indicate that UiO-66-PTC is an effective material for efficiently and selectivity removal of Pb(II) from solution, which is of practical significance.
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