INDUSTRIAL CROPS AND PRODUCTS
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2023
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IF 5.9
Na Li,Huan Xia,Shiyuan Liu,Junjiang Teng,Yanbin Jiang
In order to improve the activity and reusability of β-xylosidase, the β-xylosidase mutant S160N-R333H (R333H) which could convert notoginsenoside R1 to ginsenoside Rg1 and xylose was immobilized on the metal-organic framework (MOF) UiO-66-NH 2 . The physical and biochemical properties of immobilized β-xylosidase ( [email protected] 2 ) were studied in detail. The results showed improved performances, i.e. the high immobilization yield of 93% and recovery activity of 192.8%, better stability under acidic or trypsin-containing conditions, the higher activity in the reaction containing ions , and the improved catalytic efficiency (was 1.37-fold than that of free R333H). Importantly, the ginsenoside Rg1 yields remained more than 80% after six recycles in McIlvaine buffer and pure water. The UiO-66-NH 2 could catalyze xylose dehydration to produce furfural and the yield reached 69%. Thus this study provides a promising method for production of bioactive or platform chemicals via continuous conversion of xyloylated substrates using nanocatalyst synthesized by β-xylosidase and MOF.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Baofang Zhang,Ziyu Zengcai,Wenting Lin,Meijin Zhang,Yunhong Pi,Tiejun Wang
Photothermal synergism can effectively activate methanol at low operating temperature and significantly reduce the activation energy of the reaction, achieving more efficiently H 2 release from methanol reforming. Here, a novel hierarchical heterojunction that integrating photo- and thermal-active Cu 2 O catalytic species with in-situ derived NH 2 -MIL-125@TiO 2 framework was specifically designed for photothermal-driven aqueous phase reforming of methanol into H 2 . The afforded Cu 2 O/NH 2 -MIL-125@TiO 2 realized an outstanding photothermal H 2 production activity (apparent quantum efficiency of 22.3 % at 365 nm), ca. 13-times higher than that of thermocatalytic condition. Interestingly, the photothermal effect did confer the Cu 2 O/NH 2 -MIL-125@TiO 2 with unexpected activity at low temperature subsided to 100 °C and accelerated the activation of MeOH/H 2 O with an obvious reduction of activation energy from 82.62 kJ·mol −1 to 52.40 kJ·mol −1 . The improvement of catalyst stability and the promotion of charge separation also contributed to a long-term photothermal H 2 evolution activity with average rate of 1.49x10 6 μmolg Cu -1 h −1 and a total turnover number (TON) up to 5971 in 63 h, almost 125-fold promotion compared with Cu 2 O.
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Analytical Methods
·
2023
·Vol. 15
·期 21
·2622-2630
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IF 3.1
Liangyun Yu,Liangju Sun,Qi Zhang,Jingjing Zhang,Bairen Yang,Mingquan Huang,Yawen Zhou,Baocai Xu,Xiaoya Hu
This study developed an electrochemical sensor for the determination of Mn2+ in Chinese liquor by modifying a glass carbon electrode with TiO2-NH2@COFDPTB, which was synthesized via the controllable growth of COFDPTB onto the surface of TiO2-NH2 using the Schiff-base condensation reaction between 2,5-dimethoxyterephthalaldehyde and 1,3,5-tris(4-aminophenyl)benzene. The morphological and structural characterization studies of the proposed TiO2-NH2@COFDPTB were carried out by SEM, TEM, HRTEM, EDX, BET, XRD and FTIR techniques. Owing to the excellent properties and the synergism between TiO2 and COFDPTB, the introduction of TiO2-NH2@COFDPTB improved the electrochemical response significantly. By optimizing the experimental parameters, the sensor exhibited good linearity in the range of 0.1–1.0 nM and 0.08–10 μM with a detection limit of 2.83 × 10−11 M and 9.50 × 10−9 M, respectively, showing competitive performance for Mn2+ determination. Besides, the proposed sensor was successfully applied to Mn2+ detection in liquor samples, suggesting its practical application performance.
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INORGANICA CHIMICA ACTA
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2022
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IF 3.118
Yan Wang,Wenpei Feng,Jinjun Li,Zhixiong You
Metal-organic frameworks (MOFs) have shown attractive advantages in adsorbing dyes from wastewater. However, their complex synthesis processes and poor stability have limited their applications. Herein, we proposed a novel two-step route to prepare NH 2 -MIL-53(Fe) at room temperature and investigated its dye adsorption performance. The prepared NH 2 -MIL-53(Fe) displayed high water stability in the pH range of 3–11. Moreover, NH 2 -MIL-53(Fe) showed a significantly higher adsorption capacity and faster adsorption rate towards congo red (CR) than the other selected dyes, with more than 99 % of CR being removed by NH 2 -MIL-53(Fe) within 20 min. The maximum adsorption capacity of NH 2 -MIL-53(Fe) for CR was 1877 mg·g −1 . Besides, the removal efficiency of CR could maintain higher than 80 % within the tested pH range (3 to 11), and removal efficiency was consistently higher than 95 % at different NaCl concentrations (0 to 0.4 M). The dynamic CR adsorption process matched the pseudo-second-order kinetic model and fitted well using the Langmuir model, suggesting that the adsorption of CR onto NH 2 -MIL-53(Fe) was a monomolecular-layer chemical adsorption process. More importantly, NH 2 -MIL-53(Fe) showed high removal efficiency and good reusability towards CR in both synthetic and model wastewater. Mechanistic studies suggested that the removal of CR was attributed to the synergistic effects of the π-π stacking interactions, hydrogen bonds and electrostatic interactions between CR and NH 2 -MIL-53(Fe). Overall, the present study provides a novel strategy for the facile synthesis of NH 2 -MIL-53(Fe), highlights the excellent adsorption performance and reusability towards CR and underlies the adsorption mechanisms involved.
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JOURNAL OF MOLECULAR LIQUIDS
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2023
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IF 6
Guohao Cheng,Xing Li,Zhao Li,Kaixin Zhao,Guifen Zhu
Benzydamine hydrochloride (BDH) is a kind of nonsteroidal anti-inflammatory drugs for the treatment of inflammation. However, research on removing BDH from the environment has not attracted attention. Herein, a green deep eutectic solvent (DES) as functional monomer and magnetic metal organic frameworks (MUiO-66-NH 2 ) as supporter help to form more effective recognition sites and easy separation properties in polymerization procedure of the surface imprinted polymer (DES-MMIP). The performance of novel DES-MMIP for the selective removal of the template (BDH) in water was characterized and evaluated. The equilibrium experiment results showed that the maximum adsorption capacity of BDH can reach 41.18 mg g −1 , and fast adsorption equilibrium was obtained within 30 min. Due to the participation of magnetic MUiO-66-NH 2 and DES, the prepared DES-MMIP had excellent separability, and the adsorption capacity towards template (BDH) was 1.4–2.6 times that of other commercial adsorbents (PS-DVB, HLB, silica and zeolite). The DES-MMIP combined with UV-via was successfully applied to remove BDH from eight environmental samples. Additionally, the DES-MMIP adsorbent can be reused 5 times and still maintain excellent recovery. This work provides a promising method for preparing an efficient adsorbent for the fast separation and selective removal of BDH in the environmental field.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 31
·14828-14839
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IF 3.3
Lin Dong,Yunlan Xu,Dengjie Zhong,Nianbing Zhong,Zhuofan Han,Yi Liu,Haixing Chang
The low electron–hole separation in the photoanode generally restricts the visible light response of photocatalytic fuel cell (PFCs). In this study, 5% NH2-MIL-125/g-C3N4/Bi2O3/Ti photoanode was synthesized and assembled with a PFC with Cu cathode to degrade rhodamine B and generate electricity. With visible light irritation, the maximum photocurrent density, maximum power density, and degradation rate of the PFC were 0.59 mA cm−2, 29.88 μW cm−2, and 97.48% (1 h), respectively. The major active species in the PFC were h+, ˙O2−, and ˙OH. The good performance of the PFC was ascribed to the formation of a double Z-type heterojunction in the 5% NH2-MIL-125/g-C3N4/Bi2O3/Ti photoanode so that the photoelectrons of NH2-MIL-125 and Bi2O3 directly combine with the photoholes of g-C3N4, making the photoholes of NH2-MIL-125 and Bi2O3 and the photoelectrons of g-C3N4 directly or indirectly involved in the RhB degradation process and generating electricity. Thus, the separation rate of the e−–h+ pairs in the photoanode and the capability of the PFC are greatly improved.
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MICROCHEMICAL JOURNAL
·
2023
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IF 4.8
Zongyan Lu,Hao Guo,Xiaoqin Wei,Lei Sun,Zhilan Pan,Bingqing Liu,Yinsheng Liu,Jiaxi Xu,Jiaying Tian,Wu Yang
In this article, a novel and simple electrochemical sensing platform has been developed for the simultaneous and sensitive determination of acetaminophen (ACOP) and 4-aminophenol (4-AP). The porous covalent organic frameworks (COFs) material with β-ketoenamine-linkage was successfully synthesized via 1,3,5-triformylphloroglucinol (TFP) and 2,6-diaminoanthraquinone (DAAQ) and named as TFP-DAAQ-COF. High conductivity walnut shells-derived carbon (WC), amine-functionalized multi-walled carbon nanotubes (NH 2 -MWCNTs) with multiple active sites and TFP-DAAQ-COF were combined to obtain composite materials, which were used to modify bare glass carbon electrodes (GCE) and realize the electrochemical analysis of ACOP and 4-AP. The experiments showed that the composite electrode had a strong synergistic effect and exhibited a good electrocatalytic oxidation ability for the two target analytes. The linearity ranges of ACOP and 4-AP were 0.5 ∼ 200 μM and 1.0 ∼ 250 μM, respectively and the detection limits (S/N = 3) were 0.12 μM and 0.18 μM. In addition, the sensor showed acceptable reproducibility, stability and excellent selectivity. The recovery was satisfactory, when it was used to analyze the contents of ACOP and 4-AP in real samples, indicating that the sensor was feasible in practical applications.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Rui Ji,Zhuzhu Zhang,Lechen Tian,Liujun Jin,Qingfeng Xu,Jianmei Lu
A novel BiOI-incorporated NH 2 -UiO-66 composite photocatalyst, NH 2 -UiO-66@BiOI, was prepared using an in-situ successive ion-insertion method. The in situ grown BiOI nanosheets exhibited an ultrathin structure and were uniformly dispersed on NH 2 -UiO-66. The formation of tight heterojunctions, characteristics of enhanced visible light absorption and availability of abundant exposed active sites facilitated the efficient activation of peroxymonosulfate and the rapid degradation of Bisphenol A in water (12 min). Surprisingly, the photocatalyst maintained a fast degradation rate of Bisphenol A under the interference of different conditions. The research explored the charge transfer pathways and radical species between the heterojunction components, indicating that the heterojunction type of the NH 2 -UiO-66@BiOI was Z-scheme. In addition, the degraded intermediate components and high mineralization rate indicated that Bisphenol A was deeply degraded. In conclusion, this study synthesized metal–organic framework-based photocatalysts through a simple preparation method, which has potential application value in the rapid degradation of bisphenol A.
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ACS Applied Materials & Interfaces
·
2022
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IF 10.383
Chuan Zhou,Bo Yuan,Shouxin Zhang,Guang Yang,Lin Lu,Heguo Li,Cheng-an Tao
Zirconium-based metal–organic frameworks (Zr-MOFs) have been considered as prospective materials for the degradation of nerve chemical warfare agents (CWAs) but show poor catalytic performance toward blister agents. Moreover, the powder issues and the poor adsorption capability also remain as the major challenges for the application of Zr-MOFs in practical CWA detoxification. Herein, a series of defected granular UiO-66-NH2 metal–organic gels are synthesized via adjusting the amount of added concentrated hydrochloric acid for the decontamination of 2-chloroethyl ethyl sulfide (2-CEES), a sulfur mustard simulant. The half-life of 2-CEES decontaminated by defected granular UiO-66-NH2 metal–organic gels can be shortened to 7.6 min, which is the highest reported value for MOFs under ambient conditions. The mechanism of decontamination is that the amino group on the linkers in UiO-66-NH2 MOGs undergoes a substitution reaction with 2-CEES to yield 2-(2-(ethylthio)ethylamino)terephthalic acid, which is less toxic and fixed in the frameworks. The recycling test corroborates that the granular UiO-66-NH2 xerogels possess good stability and reusability. Static adsorption and desorption tests show that UiO-66-NH2 xerogels possess a high 2-CEES vapor adsorption capacity of 802 mg/g after exposure for 1 d and only 28 wt % desorption capacity after air exposure for 7 d. The dual function of ultrafast degradation and high adsorption capability provide a firm foundation for using UiO-66-NH2 xerogels as a future protection media.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Youzhou He,Shuang Luo,Yuwei Tan,Mingzuo Chen,Haibo Zhou,Jianning Yu,Linjiang Pu,Yumin Huang,Min Fu,Xingyan Liu
Novel ionic state Co passivated carbon nanodots (Co-CDs) combined with NH 2 -MIL-125 as efficient photocatalysts Co-CDs/NH 2 -MIL-125 were fabricated in a convenient process for the first time. These materials exhibited excellent photocatalytic activity in both NO purification and hydrogen production under visible light irradiation. The NO purification rate of Co-CDs/NH 2 -MIL-125 increased to 46.6%, which was 20.2% and 13.4% higher than that of NH 2 -MIL-125 and CDs/NH 2 -MIL-125, respectively. Moreover, the hydrogen production efficiency of Co-CDs/NH 2 -MIL-125 reached 2261 μmol g −1 , which was 6.86 times and 3.54 times of the values for NH 2 -MIL-125 and CDs/NH 2 -MIL-125, respectively. The corresponding properties characterized by Mott-Schottky, UCPL , and in situ DRIFTS , indicated that the introduction of Co 2+ could not only passivate the CDs to further improve physicochemical properties, but also enhance the photocatalytic activity via the photosensitization and up-conversion effect. This research provides a promising strategy that adding active metal ions passivated CDs in the catalyst platform to improve photocatalytic performance.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Zhen-Peng Cui,Le-Xi Zhang,Heng Xu,Yan-Yan Yin,Bo Tang,Li-Jian Bie
Metal-organic frameworks (MOFs) have been proved to be outstanding candidates for humidity sensors, however, pure MOFs are still limited in hysteresis, integration, and intelligence. In this investigation, inspired by a single-site-ion strategy for catalysis, UiO-66-NH 2 is first grafted by 2, 6-DPA (2, 6-dipicolinic acid) molecules (named as U-DPA) and then combined by Zn (II) ions (noted as U-DPA-Zn). Taking advantage of electrolyte and MOF, U-DPA-Zn exhibits significantly enhanced humidity sensing performance than UiO-66-NH 2 and U-DPA. U-DPA-Zn possesses the highest sensitivity (S r = 8.07 × 10 3 ), the best linearity (R 2 = 0.994), the shortest response-recovery time (τ res = 2 s, τ rec = 105 s), the smallest hysteresis (ΔH = 1.81%), as well as good repeatability in a wide relative humidity (RH) range (11%-97%). Thanks to its excellent properties, U-DPA-Zn shows great potential in the field of monitoring human respiration (breath detection) and water evaporation on human skin (finger detection). Additionally, the humidity sensing mechanism is discussed based on complex impedance analysis, revealing the single Zn (II) make giant contribution to MOFs. This work provides an optional material for humidity sensors and further a new strategy to improve the humidity sensitivity of pure MOFs.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Jinchao Chen,Chunmei Gao,Shuangquan Zhao,Shenghui Liu,Shifeng Ji,Yunqing Xing,Tianyang Wu,Jinjian Wu,Hongyu Chen,Peng Zou,Jiaonan Cai
In this work, the NH 2 -MIL-125/F127/PES membranes with superior ultrafiltration , anti-fouling and self-cleaning were constructed via the RTIPS method. Characterizations showed the successful fabrication of NH 2 -MIL-125 with good photocatalysis activities, together with its stable anchoring in PES membrane. The loss of NH 2 -MIL-125 was suppressed by hydrogen bond between F127 and NH 2 -MIL-125, where hydrophilic F127 significantly boosted permeability and anti-fouling property. The permeability-selectivity trade-off effect was alleviated by NH 2 -MIL-125 with a regular size window. It was observed that the membranes prepared by the RTIPS method occurred a spongy-like cross-section and a porous surface, which imparted the membrane with improved ultrafiltration and mechanical properties over the finger-like cross-section and dense skin caused by the NIPS method. The optimal membranes exhibited decent permeability (1511 L/m 2 h), BSA rejection rate (85.3%) and high COD removal rate over the commercial membranes, whose flux recovery rate was up to 76.91% after two cycles under light irradiation by the synergistic effect of F127 and NH 2 -MIL-125. The membrane fouled with RhB exhibited excellent regeneration properties benefiting from the holes (h + ) and superoxide free radicals ( • O 2 − ), as well as reactive •OH. Overall, the membrane with F127 and NH 2 -MIL-125 presented a highly promising in improving ultrafiltration and self-cleaning via the RTIPS method.
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