INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Jun-Qing Ye,Yan-Zi Dai,Shu-Ying Xu,Pin-Xi Wang,Zhong-Hua Sun,Jun-Feng Qian,Qian Liang,Ming-Yang He,Qun Chen
The construction of efficient photocatalysts for water splitting to enable H2 evolution is pivotal to alleviate energy issues and environmental concerns. In this work, carbon dots (CDs) were prepared by employing “green solvent” ionic liquids as carbon sources and then combined with Pt/NH2-MIL-125, resulting in the emergence of a high-efficiency photocatalyst termed CDs-Pt/NH2-MIL-125 for the first time. This composite photocatalyst exhibited outstanding photocatalytic activity in H2 production under visible light irradiation. Notably, the H2 production rate of CDs100-Pt/NH2-MIL-125 reaches up to 951.4 μmol/g/h, which was 3.1 times that of Pt/NH2-MIL-125. The characterization results indicate that CDs and Pt uniformly dispersed on the surface of NH2-MIL-125 and fabricated a synergistic compact structure, providing a high BET surface area (985 m2 g–1) and a suitable band gap. Furthermore, the distinctive embeddable-dispersed CDs and Pt, as dual cocatalyst, can harvest light and facilitate the transfer of photogenerated electrons, thereby significantly augmenting the exploitation of visible light. The plausible mechanism of photocatalytic H2 evolution over the CDs-Pt/NH2-MIL-125 catalyst was also discussed. This work introduces a promising strategy for designing high-performance CDs-MOFs-based photocatalysts, an innovative step toward achieving efficient photocatalytic water splitting for H2 production.
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Nanomaterials
·
2023
·Vol. 13
·期 14
·2072
·
IF 5.3
Xu Zhang,Bo Tian,Zhiheng Ma,He Wang,Zhixuan Cheng,Jiaqiang Xu
As a volatile air pollutant, formaldehyde can enter people’s living environment through interior decoration, furniture and paint, causing serious harm to human health. Therefore, it is necessary to develop a sensor for the real-time detection of formaldehyde in low concentrations. According to the chemical interaction between amino groups and formaldehyde, a MIL-101(Cr) aminated-material-based formaldehyde cantilever sensor was prepared, of which ethylenediamine- functionalized MIL-101(Cr) named ED-MIL-101(Cr)) showed the best gas sensing performance. Using quasi-in situ infrared spectroscopy, ED-MIL-101(Cr) was found bound to formaldehyde through a Schiff base. The adsorption enthalpy of formaldehyde-bound ED-MIL-101(Cr) was −52.6 kJ/mol, which corresponds to weak chemical adsorption, so the material showed good selectivity. In addition, ED-MIL-101(Cr) has the most active sites, so its response value to formaldehyde is larger and it takes longer to reach saturation adsorption than bare MIL-101(Cr). Through the research on the gas sensing performance of functionalized MIL-101(Cr) material, we found that it has a strong application potential in the field of formaldehyde monitoring, and the material performance can be quantitatively and accurately evaluated through combining calculation and experimentation for understanding the gas sensing mechanism.
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CHEMOSPHERE
·
2023
·
IF 8.8
Hao Li,Canyuan Lin,Ruhui Ma,Yuancai Chen
In this study, the selective adsorption of aromatic compounds on mesoporous MIL-53(Al) was investigated, and followed the order: Biphenyl (Biph) > Triclosan (TCS) > Bisphenol A (BPA) > Pyrogallol (Pyro) > Catechol (Cate) > Phenol (Phen), and exhibited high selectivity toward TCS in binary compounds. In addition to hydrophobicity and hydrogen bonding, π–π interaction/stacking predominated, and more evidently with double benzene rings. TCS-containing halogens could increase π interaction on the benzene rings via forming Cl–π stacking with MIL-53(Al). Moreover, site energy distribution confirmed that complementary adsorption mainly occurred in the Phen/TCS system, as evidenced by Δ Q pri (the decreased solid-phase TCS concentration of the primary adsorbate) < Q sec (the solid-phase concentrations of the competitor (Phen)) . In contrast , competitive sorption occurred in the BPA/TCS and Biph/TCS systems within 30 min due to Δ Q pri = Q sec , followed by substitution adsorption in the BPA/TCS system, but not for the Biph/TCS system, likely attributed to the magnitude of energy gaps (E g ) and bond energy of TCS (1.80 eV, 362 kJ/mol) fallen between BPA (1.74 eV, 332 kJ/mol) and Biph (1.99 eV, 518 kJ/mol) according to the density-functional theory of Gaussian models. Biph with a more stable electronic homeostasis than TCS lead to the occurrence of substitution adsorption in the TCS/BPA system, but not in the TCS/Biph system. This study provides insight into the mechanisms of different aromatic compounds on MIL-53(Al).
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ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Yu-Fei Li,Can-Jun Zou,Xing-Biao Liu,Feng Gan,Ping-Ping Fang
The detection of pharmaceuticals has been a matter of concern among scientists and health researchers in the past few decades. However, it is still difficult to realize the sensitivity and selectivity detection of pharmaceuticals with similar structures. Herein, the pharmaceutical molecules of 2-mercaptobenzimidazole (MBI) and 2-mercaptobenzothiazole (MBT) with so similar structures can be selectively detected by surface-enhanced Raman spectroscopy (SERS) taking advantage of the fingerprint identification on Au/MIL-101(Cr), with sensitive detection limits of 0.5 ng·mL–1 for MBI and 1 ng·mL–1 for MBT. MBI is selectively enriched by Au/MIL-101(Cr) from the mixture solution and detected by SERS below 30 ng·mL–1. MBI can also be selectively detected in the serum samples with a detection limit of 10 ng·mL–1. Density functional theory calculations combined with the SERS experiments explained that the high sensitivity and selectivity are caused by the intrinsic differences in Raman intensity and different adsorption energies from the pharmaceutical molecules adsorbed on Au/MIL-101(Cr), respectively. This study provides an effective way to enrich and detect pharmaceutical molecules with similar structures.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2019
·
IF 6.361
Zongchen Li,Xuemin Liu,Wei Jin,Qingsong Hu,Yaping Zhao
Arsenic species are regarded as typical water pollutants due to their toxicity. The chemical structures of arsenic species greatly influence their migration and transformation in the environment. Metal-organic frameworks (MOFs) are used as reliable adsorbents to control arsenic contamination, so it is urgently needed to study the effect of chemical structure of arsenic species during adsorption process. The adsorption behaviors of arsenate (As(V)) and its organic forms such as roxarsone (ROX), p-arsanilic acid (p-ASA) and dimethyl arsenate (DMA) by MIL-101(Fe), a type of highly porosity iron-based MOFs in aqueous environment were detailed investigated. The adsorption kinetics of those arsenic species on MIL-101(Fe) is rapid followed with pseudo-second-order kinetic model. MIL-101(Fe) exhibits excellent adsorption capacities for As(V), ROX, p-ASA and DMA with maximum adsorption capacities of 232.98, 507.97, 379.65 and 158.94 mg g −1 , respectively. The formed Fe O As inner-sphere coordination between arsenic species and the incomplete-coordinated cationic Fe in the MIL-101(Fe) cluster is the primary adsorption mechanism based on FTIR and XPS analysis. Substituent aromatic units in ROX and p-ASA strengthen the adsorption on MIL-101(Fe) through hydrogen bonds and π-π stacking interaction, resulting in higher adsorption capacities far beyond that of As(V) and DMA. The reusability of MIL-101(Fe) is limited by the strong Fe O As coordination. These results confirm MIL-101(Fe) a reliable adsorbent to control the aqueous arsenic species contamination and emphasize the significant role of the chemical structure of arsenic speciation on adsorption performances of MOFs.
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INORGANICA CHIMICA ACTA
·
2017
·
IF 2.002
Tian Zhao,Ling Yang,Peiyong Feng,Irina Gruber,Christoph Janiak,Yuejun Liu
MIL-101(Cr), one of the best investigated and widely used metal–organic frameworks, has been easily synthesized with particle diameters in the range from 387(28) nm to 90(10) nm by using acetic acid as a modulator . The particle size of MIL-101(Cr) decreased with increasing acetic acid concentration. The decrease of size in high concentration of acetic acid may be explained with the efficient suppression of the framework extension. In a selected condition, MIL-101(Cr) possessing an average diameter of about 90 nm can be prepared easily and reproducibly in gram-scale, with high BET-surface areas (3200–3500 m 2 /g) and fairly good yield (60–75%).
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RSC Advances
·
2017
·Vol. 7
·期 68
·42819-42825
·
IF 3.108
Yanghe Fu,Huan Yang,Rongfei Du,Gaomei Tu,Chunhui Xu,Fumin Zhang,Maohong Fan,Weidong Zhu
Co-doped NH2-MIL-125(Ti) catalysts [Co/NH2-MIL-125(Ti)] are developed for the photocatalytic reduction of CO2 upon visible-light irradiation. Compared with NH2-MIL-125(Ti), Co/NH2-MIL-125(Ti) exhibits a significantly enhanced activity in CO2 reduction, due to the fact that the doping of Co nanoparticles onto NH2-MIL-125(Ti) can promote the visible-light harvesting and electron transfer. In addition, when benzylic alcohols as electron donors, instead of triethanolamine (TEOA) which is often used as a sacrificial agent, are added into the reaction system, Co/NH2-MIL-125(Ti) can simultaneously catalyze CO2 reduction to formic acid (HCOOH) and the selective oxidation of the benzylic alcohols to the corresponding aldehydes, making the proposed process more economical and environment-friendly.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Yong Li,Xinyue Yang,Mengyao Wang,Deyun Yue,Jun Wu,Haojie Song
The pollutants present in wastewater can cause structural damage to evaporators, thereby reducing their evaporation efficiency and hindering the application of solar-driven water evaporation technologies. Here, the TiO 2 -based evaporator (CPM-Air) with highly efficient photodegradation and solar-powered water evaporation performance for simultaneous freshwater production and decontamination was prepared by pyrolysis NH 2 -MIL-125(Ti) grown on the surface of Carbon Felt (CF). The evaporation rate of CPM-Air evaporator reached 2.21 kg m -2 h −1 under 1.0 kW/m 2 , and high solar-vapor conversion efficiency of 102.20 %. Meanwhile, the Anatase TiO 2 obtained by carbonized NH 2 -MIL-125 (Ti) has more active sites for removal pollutants. CF as the catalytic promoter to accelerate electron transport, and improve the photogenerated electron-hole separation efficiency. The photothermal-photocatalytic synergy removal efficiency of high concentration (50 mg/L) CIP was 2 times higher than photocatalytic only. In addition, the CPM-Air evaporator has high water evaporation rate in different harsh environments, the 99.9 % of metal ions removal and excellent salt resistance. More importantly, the growth experiments on soybean indicated that the products of photothermal-photocatalytic synergy degradation CIP of CPM-Air evaporator was non-biotoxic. This study provides valuable insights into the potential of photothermal-photocatalytic synergy for sustainable water production.
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 20
·9185-9195
·
IF 2.7
Shikai Xue,Dongying Zhu,Qing Zuo,Shuangfeng Yang,Haiyan Wang,Qiujun Lu,Guoxing Yin,Guihua Ruan,Fuyou Du
A novel MIL-101(Fe)/ZnCrZr-LBMO heterojunction was successfully constructed and used for the removal of ciprofloxacin (CIP) in this work. The MIL-101(Fe)/ZnCrZr-LBMO composite exhibited significantly enhanced photocatalytic degradation activity, with reaction rates approximately 3.4 and 3.1 times faster than those observed with pristine MIL-101(Fe) and ZnCrZr-LBMO, respectively. The effect of different amounts of ZnCrZr-LBMO, sample pH, CIP concentration, inorganic cations, and anions on CIP removal was investigated, and the possible intermediates and degradation pathways of CIP were speculated. The·O2− radicals dominated CIP degradation, with minor contributions from 1O2, h+, and ·OH radicals. The composite exhibited high removal rates for CIP (94.7%), ofloxacin (86.8%), and tetracycline (96.3%), respectively, within 60 min of light irradiation, and excellent reusability, retaining over 85.1% CIP degradation rate after five cycles. Our work provides a new reference to construct highly efficient and easily recyclable MIL-101(Fe)/ZnCrZr-LBMO photocatalysts for the removal of antibiotic pollutants, promising advancements in real water treatment applications.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Wenjin Ni,Sicheng Zhang,Lingling Cheng,Tiejun Luo,Hongyun Yang,Tengfei Duan,Dejian Yan
Developing efficient photoanodes for water oxidation is highly promising due to their critical role in producing green H 2 and harnessing solar energy. Herein, a metal-organic framework (MOF)/photoanode was successfully constructed by coating TiO 2 nanorods with MIL-88(Fe) MOF for photoelectrochemical (PEC) water splitting. The results demonstrated that MIL-88(Fe) was uniformly and tightly coated on TiO 2 and functioned as a cocatalyst. The MIL-88(Fe) MOF provides a large surface area and more Fe-O active sites, contributing to high PEC activity by reducing electron/hole recombination and enhancing light response capability. Moreover, the photoanode also exhibited an improved charge conductivity. As a result, the MIL-88(Fe)/TiO 2 photoanode exhibited an excellent photocurrent density of 1.06 mA cm −2 at 1.23 V RHE , which is approximately 2.6 times higher than the pristine TiO 2 . Charge transfer kinetics analyses and electrochemical tests were carried out and revealed that the improved PEC performance was attributed to the introduction of MIL-88(Fe), which promoted charge separation-transfer. This research provided new insights into the design of efficient semiconductor/MOF composite photoanodes for PEC water oxidation.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2014
·
IF 2.129
Zhengjuan Sun,Yali Liu,Yuanfang Li
A novel and rapid spectrofluorometry method for the recognition of 6-mercaptopurine (6-MP) has been developed based on luminescent metal–organic frameworks Fe-MIL-88NH 2 as fluorescent probe. The strong fluorescence of Fe-MIL-88NH 2 at 430 nm could be quenched by 6-MP directly, and the Fe-MIL-88NH 2 shows high selectivity for 6-MP compared to other thiol-containing amino acids such as homocysteine (Hcy), cysteine (Cys), glutathione (GSH), etc. Under optimal conditions, the relative fluorescence intensity was linearly proportional to the concentration of 6-MP in the range of 5–600 μM with the detection limit at 1.17 μM (S/N = 3). Furthermore, the present approach has been successfully applied to the determination of 6-MP in human serum samples. The possible fluorescence quenching mechanism has also been investigated, where it is revealed that the quenching was attributed to competition of absorption of the light source energy as well as electron transfer between Fe-MIL-88NH 2 and 6-MP.
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ANALYTICAL CHEMISTRY
·
2025
·
IF 6.7
Chengzhuo Yu,Jin Xu,Li Xiong,Yarui Wang,Silong Wang,Fanglan Geng,Zesen Shang,Huasheng Wu,Lixia Zhao,Yawei Wang
Luminol-based chemiluminescence (CL) systems, as a powerful tool for bioanalysis, are limited owing to their weak CL intensity and self-decomposition of the classic oxidant H2O2. Herein, we introduced a new luminol CL enhancer, the natural light-driven photocatalyst MIL-100(Fe)/TiO2, for the selective determination of dopamine (DA). By employing MIL-100(Fe)/TiO2 for the first time as an efficient enhancer, the MIL-100(Fe)/TiO2-luminol CL intensity was 100 times higher than that of the classical H2O2-luminol system. The CL spectrum, UV–vis absorption spectroscopy, radical scavenger experiments, and electron spin resonance spectroscopy were utilized to investigate the possible CL mechanism of the MIL-100(Fe)/TiO2-luminol system. All of the results indicated that MIL-100(Fe)/TiO2 can generate reactive oxygen species under mild natural light, which could react rapidly with the luminol anion radical and result in direct CL emission. The sensitive plate for DA was developed based on its inhibiting effect on CL intensity, and the linear range between CL intensity and DA concentration was 100 nM–1000 μM with a detection limit of 16.7 μM (S/N = 3). This study successfully achieved a stable reactant that can directly trigger the CL of luminol without the need for additional oxidizing agents under mild natural light and offers new possibilities for photoinduced amplification technology.
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