APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
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IF 11.698
He Xiao,Wenyao Zhang,Qiushi Yao,Liulian Huang,Lihui Chen,Bruno Boury,Zhongwei Chen
Metal organic frameworks (MOFs) are exploited in many applications of materials science and very recently were investigated as precursors or reagents for material synthesis. In a new way different from previous approaches, here we introduce for the first time the synthesis of metal oxide M x O y in the presence of M-free MOF acting partially as a sacrificial template and as a provider of doping metal atom. We demonstrate this approach in the case of ZnO prepared by a simple hydrothermal method in the presence of a Zn-free MOF like MIL-53(Al) or MIL-125(Ti). The resulting ZnO show low content of Al or Ti < 2% and properties are significantly different depending on whether MIL-53(Al) or MIL-125(Ti) are used or if no MOF is present. The nature and presence of MOF has different major effects on the morphology, the specific surface area of as prepared ZnO and also on the oxygen defects in its crystal structure. Corroborating the XPS, UV–vis DRS, PL, EPR and DFT studies evidence the role of such O-defects on band gap narrowing for samples calcined at 400 °C. These exhibit high efficiency in photodegradation of methyl orange (MO) compared to ZnO prepared in MOF-free conditions or previous literatures. The kinetics of MO degradation is different depending on the morphology, the specific surface and oxygen defects. The present data open the door to a new approach of the synthesis of metal oxides and a control of their properties.
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MICROCHIMICA ACTA
·
2020
·Vol. 187
·期 8
·1-9
·
IF 6.232
Li Jingxian,Jiang Ding,Shan Xueling,Wang Wenchang,Chen Zhidong
A novel “off-on” electrochemiluminescence (ECL) aptasensor based on ECL resonance energy transfer (RET) system from 3,4,9,10-perylenetetracar-boxylic acid/the metal-organic frameworks NH 2 -MIL-125(Ti) (PTCA/NH 2 -MIL-125) to Au nanoparticles (Au NPs) was put forward for microcystin-LR (MC-LR) assay. The electrochemiluminescence (ECL) emission spectra of PTCA/NH 2 -MIL-125 show excellent spectral overlap with the UV-vis absorption spectrum of Au NPs. A linear response ranging from 10 fM (9.95 × 10 −6 μg L −1 ) to 0.1 μM (99.5 μg L −1 ) was obtained, and the detection limit was 3.6 fM (3.58 × 10 −6 μg L −1 ) under optimal conditions at a potential of − 1.6 V ( S/N = 3). Besides, the prepared ECL-RET MC-LR aptasensor exhibited good selectivity and stability.
Graphical abstract
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BIOSENSORS & BIOELECTRONICS
·
2021
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IF 10.618
Yukun Yang,Wenyan Yan,Xiaomin Wang,Ligang Yu,Jinhua Zhang,Baoqing Bai,Caixia Guo,Sanhong Fan
In this work, a molecularly imprinted photoelectrochemical (MIP-PEC) sensor based on a novel PEC composite of metal-organic frameworks (MOFs) and TiO 2 (NH 2 -MIL-125(Ti)–TiO 2 ) was established for the ultrasensitive and selective detection of oxytetracycline (OTC). This is the first attempt of applying MOFs in the construction of MIP-PEC sensor. The NH 2 -MIL-125(Ti)–TiO 2 was synthesized by a simple one-step solvothermal method and modified onto the surface of indium tin oxide (ITO) electrode as the photosensitive layer. Subsequently, molecularly imprinted polymer (MIP) was modified as recognition element by electropolymerization . The NH 2 -MIL-125(Ti)–TiO 2 showed an enhanced photocurrent response due to stronger light absorption capacity and matched energy band. Furthermore, MIP greatly improved the selectivity and sensitivity of the constructed PEC sensor. The photocurrent response of the MIP-PEC sensor was reduced after OTC recognition because the specific binding of OTC to the imprinted cavities blocked the electron transfer of the electrode. Under optimal experimental conditions, the MIP-PEC sensor exhibited a wide detection range from 0.1 nM to 10 μM with a low limit of detection (LOD) of 60 pM, as well as certain reproducibility, stability and good applicability in real samples. The proposed sensor provides ideas for the application of MOFs in the construction of PEC sensors and will offer an alternative method for the detection of other pollutants in the field of food safety.
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Journal of Environmental Sciences
·
2023
·
IF 6.9
Lei Zheng,Lixia Sun,Jiangbo Qiu,Junling Song,Luyi Zou,Yue Teng,Yongzhong Zong,Hongyan Yu
The coexistence of inorganic and organic contaminants is a challenge for real-life water treatment applications. Therefore, in this research, we used NH 2 -MIL-125(Ti) to evaluate the single adsorption of hexavalent chromium (Cr(VI)) or Rhodamine B (RhB) in an aqueous solution and further investigate simultaneous adsorption experiments to compare the adsorption behavior changes. The main influencing factors, for example, reaction time, initial concentration, reaction temperature, and pH were studied in detail. In all reaction systems, the pseudo-second-order kinetic and Langmuir isotherm models were well illuminated the adsorption progress of Cr(VI) and RhB. Thermodynamic studies showed that the adsorption process was spontaneous and endothermic. As compared to the single system, the adsorption capacity of Cr(VI) in the binary system gradually decreased as the additive amount of RhB increased, whereas the adsorption capacity of RhB in the binary system was expanded brilliantly. When the binary reaction system contained 100 mg/L Cr(VI), the removal rate of RhB increased to 97.58%. The formation of Cr(VI)-RhB and Cr(III)-RhB complexes was the cause that provided facilitation for the adsorption of RhB. These findings prove that the interactions during the water treatment process between contaminants may obtain additional benefits, contributing to a better adsorption capacity of co-existing contaminant.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Jian Wang,Changchun Chen,Zhihao Zhao,Cheng Cheng,Zhonghai Tang,Zhou Du,Yifeng Wang,Lin Pan
Considerable attentions are currently paid to water pollution, which seriously threats human health. Semiconductor catalysts with step-like (S-scheme) heterojunction are often used for degrading organic pollutants in water bodies due to their high carrier separation efficiency, high redox capacity, and broad light absorption capacity. In this paper, a novel S-scheme N-doped g-C 3 N 4 /NH 2 -MIL-125(Ti) heterojunction composite is synthesized for photodegradation of organic pollutants. The structural measurements indicate that the NH 2 -MIL-125(Ti) nanoparticles are intimately anchored on the surface of porous N-doped g-C 3 N 4 nanosheets . The experimental characterizations as well as the DFT theoretical calculation for samples demonstrate that the N-doped g-C 3 N 4 /NH 2 -MIL-125(Ti) composites not only bear larger specific surface area providing abundant reactive sites, but also improve the separation efficiency of photogenerated carriers during photodegradation. In addition, the degradation rate of RhB solution catalyzed by 25 wt% N-doped g-C 3 N 4 /NH 2 -MIL-125(Ti) (25 wt% NCM) attains the highest degradation rate (96.4%) under visible light irradiation. Moreover, the mineralization of RhB solution and intermediates produced in the degradation process are analyzed by total organic carbon (TOC) and high- performance liquid chromatography (HPLC) tests, respectively. Electron paramagnetic resonance (EPR) with free radical capture measurements show that the photodegradation of RhB is mainly ascribed to the superoxide radicals (·O 2 - ) and hole (h + ). This study provides an effective method to construct S-scheme heterojunction photocatalysts and apply them to wastewater treatment.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Syed Jalil Shah,Ruimeng Wang,Zhu Gao,Yaseen Muhammad,Hanzhuo Zhang,ZhengSheng Zhang,Zhe Chu,Zhongxing Zhao,Zhenxia Zhao
A novel strategy and design for ionic liquid (IL) assisted in-situ grafting of polyaniline (PANI) oligomers in NH 2 -MIL-125 was proposed to synthesize the defect-rich IL-PANI/NMIL(Ti) nanohybrids with an intimate interface for the superior photodegradation of CH 3 CHO. PANI was dissolved into small oligomers with the aid of IL [EMIM]BF 4 and was composited to NH 2 -MIL-125 by a strong interfacial connection through Ti-N bonds (XPS) with high dispersion and large surface area (BET = 1125 m 2 /g). Characterizations results showed that smart grafting of PANI-oligomers generated abundant defects (3.4-times, ESR) and intensified Lewis acid sites (1.2-times, CO-DRIFT) in IL-PANI/NMIL(Ti) compared to NH 2 -MIL-125. It promoted adsorptive interactions for aldehyde VOCs capturing, which in-turn increased the adsorption rate ( k a ) of CH 3 CHO. Smart grafting also improved the light absorption of IL-PANI/NMIL(Ti) from 500 to 800 nm, reduced band gap (1.7 eV), increased photo-current density (2.2-folds of pure MOF), enhanced O 2 − and OH radicals generation and improved e − /h + mobility. As a result, IL-PANI/NMIL(Ti) showed 11.4 and 4.2 times higher k a (0.262 min −1 ) of CH 3 CHO photodegradation kinetics than PANI and NH 2 -MIL-125, respectively, at 75% relative humidity (RH). The k a of CH 3 CHO degradation was steadily increased with increasing humidity (<80 RH%), indicating that H 2 O from humid air was beneficial for CH 3 CHO degradation. Furthermore, IL-PANI/NMIL(Ti) exhibited the excellent recycling stability compared to NH 2 -MIL-125, as only a 5% decrease in photocatalytic activity was observed after five cycling runs. Considering the excellent photostability and ultrafast photodegradation of CH 3 CHO, the current study opens up new perspectives in fabricating MOFs for a wide-range of practical applications.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Ziying Zhong,Xiaoshuo Zhang,Rui Dai,Chunfang Wang,Faqiong Zhao,Baizhao Zeng
In this work, layered Co-Ni bimetallic hydroxide was synthesized and combined with polyethyleneimine hydrogel (PEI@LDH) as substrate material, then the metal-organic framework MIL-125 loaded Ru(bpy) 3 2+ (MIL@Ru) was added as single luminophore, followed by electrochemical deposition of tetracycline (TC) imprinted copolymer of hydroquinone and o-phenylenediamine to construct an electrochemiluminescent (ECL) sensor for TC detection. The stable and sensitive luminophore MIL@Ru associating with co-reactant K 2 S 2 O 8 in the solution could cause a cathode ECL signal sensing TC, it could also associate with the immobilized co-reactant PEI hydrogel to produce a stable anode ECL signal acting as a reference. The LDH had catalysis and could efficiently amplify both anode and cathode ECL signals. Therefore, the constructed single luminophore based ratiometric ECL sensor displayed high selectivity, sensitivity and reproducibility. Under the selected testing conditions, the linear response range was 0.01 μmol L −1 to 1 mmol L −1 and the detection limit reached 8 nmol L −1 . Its good practicability was validated by determining TC in different actual samples. Hence, the ratiometric MIP-ECL sensor was quite promising.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Mazhar Khan,Zeeshan Akmal,Muhammad Tayyab,Seemal Mansoor,Dongni Liu,Ziwei Ye,Jinlong Zhang,Shiqun Wu,Lingzhi Wang
The rational design of heterojunction photocatalysts is crucial for enhancing CO 2 photoreduction efficiency, yet precisely channeling photogenerated electrons to the CO 2 adsorption sites remains an enormous challenge. In this work, we developed an organic-inorganic heterostructure with continuous inter- and intra-component electric fields. The integration of BiOBr with MIL-125 via chemical bonding established a heterojunction, where the built-in electric field between the two components facilitated the efficient transfer of photogenerated electrons from BiOBr to MIL-125. The intrinsic electric field of MIL-125 further drove the accumulation of photogenerated electrons at Ti sites. This tandem electric field effect, in conjunction with the CO 2 adsorption and activation at Ti sites, significantly enhanced the efficiency of CO 2 reduction within the heterojunction system. The optimized photocatalyst achieving CO production at a rate of 65.6 μmol g −1 h −1 with nearly 90 % selectivity without the use of sacrificial agents, exhibiting a remarkable 43-fold and 8-fold enhancement in activity compared to pristine MIL-125 and BiOBr, respectively. In-situ infrared spectroscopy and theoretical calculations confirmed the energy optimization effect of the heterostructure on CO 2 activation and the hydrogenation reaction, facilitating the formation of the key intermediate *COOH. This work elucidates the mechanism by which tandem built-in electric fields facilitate charge separation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Boyuan Tu,Kaifu Yu,Dengjiang Fu,Li Zhou,Ruixiang Wang,Xinying Jiang,Huanhuan Liu,Xin Cao,Xiang Gong,Rong He,Yongjian Tang,Tao Chen,Wenkun Zhu
Photo-assist uranium extraction from fluorine-containing uranium wastewater by building semiconductor-plasma material heterostructure is a forward-looking strategy, which not only effectively accelerates F-U separation via the LSPR effect but also impacts the intensity of binding between U (VI) and site. Here, we developed an amino-rich Ag-NWs/NH 2 -MIL-125(Ti) (AgNW/N-M(Ti)) hybrid nanowires with LSPR effect for photo-assist uranium extraction. Accordingly, the AgNW/N-M(Ti) hybrid nanowires presented 90.4% removal efficiency for U(VI) without a sacrificial agent at the U: F molar ratio of 1:20. By virtue of In-situ KPFM, we identify hot electrons generated over AgNW were transferred to amino-rich N-M(Ti) to efficiently reduce the U(VI) adsorbed on the N-M(Ti), which effectively enhances the excellent uranium removal performance of AgNW/N-M(Ti) hybrid nanowires. This strategy may open a paradigm for the development of advanced heterojunctions with the LSPR effect as catalysts for photo-assisted uranium extraction from fluorine-containing uranium wastewater.
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Sustainable Energy & Fuels
·
2024
·Vol. 8
·期 13
·2889-2899
·
IF 5
Jiaqi Wang,Hongyang Huo,Guozhe Sui,Shuang Meng,Dongxuan Guo,Shanshan Fu,Dantong Zhang,Xue Yang,Jinlong Li
The development of visible-light-active photocatalysts with high performance has been regarded as a promising way to address environmental wastewater issues. In this work, a highly efficient g-C3N4/CdS/TiO2 ternary Z-type heterojunction photocatalyst with a hollow structure has been fabricated using a step-by-step self-assembly strategy, which demonstrates excellent photocatalytic performance under visible light and removes various water-soluble organic pollutants effectively. The photocatalytic degradation efficiency of 20-g-C3N4/CdS/TiO2-10 against rhodamine B (RhB) is found to be 29.8 times higher than that of the pristine g-C3N4 within 90 minutes of visible light irradiation attributed to the active species of ˙O2− and h+. Liquid chromatography mass spectrometry results suggest that the degradation pathway of RhB involves main steps such as N-de-ethylation, chromophore cleavage, ring opening, and mineralization. A series of characterization analyses, combined with the observed enhanced photocatalytic performance, indicate that the g-C3N4/CdS/TiO2 ternary heterojunction benefits from the rapid transport and separation of photogenerated carriers facilitated by the formation of a heterointerface. Furthermore, the g-C3N4/CdS/TiO2 ternary heterojunction exhibits favorable stability, with 88.1% degradation efficiency after five cycles of degradation experiments. This work provides novel insights into the preparation and application of ternary heterojunctions with superior photocatalytic performance for eliminating organic pollutants from wastewater.
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OPTICAL MATERIALS
·
2022
·
IF 3.754
Yang Wang,Sheng Feng,Changchang Ma,Yun Zhou,Zhiwei Ye,Xiaojun Dai,Xun Cao
In this paper, a novel Mn-doped CdS@NH 2 -MIL-125(Ti) (MC@NT) photocatalytic composites was synthetized through hydrothermal method . Hydrogen desorption and tetracycline and oxytetracycline degradation were performed under visible light to test their photocatalytic activities . The composites were characterized by XRD , FTIR, SEM, TEM, XPS , UV–Vis diffuse reflectance spectroscopy (DRS), EPR , EIS, and transient photocurrent response. From the characterization consequence, it could be seen that Mn-doped CdS was tightly attached to the surface of tetragonal NT in the form of nanoparticles . The MC@NT composites exhibited more promising catalytic activity than pristine monomeric materials. The photocatalytic hydrogen evolution rate reached 3.61 mmol g −1 h −1 . Within 110 min, the degradation efficiencies of TC and OTC were 90% and 88%, respectively. The free radical trapping experiments proved that ·O 2 − and h + were decisive role for degrading pollutants in the degradation catalysis process. Radical trapping experiments and electron spin resonance (ESR) indicated that the Z-scheme heterojunction was formed between Mn-doped CdS and NT, leading to facilitate the migration and shift of photogenerated carriers and holes. Cycling experiments showed that the as-prepared composites have good stability and have good prospects for practical applications. We believe this work will offer new ideas on the future development of efficient heterojunction catalysts for light energy conversion and other applications.
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JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Shuang Luo,Xingyan Liu,Xiangjun Wei,Min Fu,Peng Lu,Xuan Li,Yiming Jia,Qiao Ren,Youzhou He
The novel bifunctional NH 2 -MIL-125/Co(dmgH) 2 composite catalysts with several different Co(dmgH) 2 contents that can simultaneously achieve photocatalytic NO removal and hydrogen production were first prepared by a simple and convenient method. The corresponding physical and chemical properties of the composite catalysts were characterized by SEM, XRD, ESR, in situ DRIFTS, etc. The characterization results indicated that the noble-metal-free Co(dmgH) 2 , which was much cheaper and more available than most noble-metals such as Pt, could be an effective co-catalyst to accelerate the separation of photogenerated electron-hole pairs, further eventually enhancing the photocatalytic efficiency. Under visible-light irradiation for half an hour, the NO removal ratio of NH 2 -MIL-125/Co(dmgH) 2 (3 wt%) increased by 22.7 % compared with the pristine NH 2 -MIL-125 without Co(dmgH) 2 loading. In addition, it was found that Eosin Y dye-sensitized NH 2 -MIL-125/Co(dmgH) 2 (3 wt%) was capable of promoting a hydrogen generation rate of 2195 μmol g −1 h -1 under visible light, which was 12.6 times greater than the original NH 2 -MIL-125. This strategy was expected as an available way to fabricate noble-metal-free molecular complexes with metal-organic frameworks (MOFs) to enhance the photocatalytic NO removal and hydrogen production performance simultaneously.
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