DALTON TRANSACTIONS
·
2020
·Vol. 50
·期 1
·197-207
·
IF 4.174
Yan Zhao,Lei Li,Bo Ding,Xiu-Guang Wang,Zheng-Yu Liu,En-Cui Yang,Xiao-Jun Zhao
Decontamination of industrial wastewater containing toxic organic dye molecules and oxoanions is urgently desirable for environmental sustainability and human health. Water-stable porous metal–organic frameworks (MOFs) have emerged as highly efficient photocatalysts and/or adsorbents for water purification through controllable integration of the constitutive requirements. To reveal the inclusion anion effect of microporous MOFs on wastewater treatment, two isostructural MOFs incorporating positive charge and semiconductive characteristics, {[Cu(tpt)]·3H2O·0.5SO4}n (1) and {[Cu(tpt)]·2H2O·ClO4}n (2, tpt = 2,4,6-tris(4-pyridyl)-1,3,5-triazine), have been synthesized and employed as dual-functional materials for both dye photodegradation and oxoanion removal. The two MOFs possess the same 3-fold interpenetrating cationic backbones but are encapsulated by highly disordered sulfate or perchlorate in the open channels. These included anions have significantly tuned the hydrophilicity of the channels, extended the visible-light absorption, optimized the bandgap and decreased the conduction band potential. Under the low-energy irradiation of a 30 W LED lamp, MOF 1 has selectively and efficiently degraded rhodamine B compared to 2 with accelerated kinetics, resulting from the stronger reduction ability and less migration resistance of the photogenerated electrons. Instead, MOF 2 can quickly capture harmful MnO4− and Cr2O72− by exchanging with the entrapped ClO4−, with maximum adsorption amounts of 557 and 168 mg g−1, respectively, under ambient conditions. The improved decolorization of the aqueous solution over 2 benefits essentially from the shape and charge memory effect and the smaller hydration energy of ClO4− than SO42−. These interesting observations highlight the importance of the included anions inside the porous MOF semiconductors on wastewater treatment.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Qian Lei,Zhenting Zhao,Wenda Wang,Yong Chen,Jie Hu,Lin Chen
Ultrasensitive determination of Sudan I is critically important for food products due to its potential carcinogenicity. Herein, an electrochemical sensor was developed for Sudan I detection by using nanocomposites-based glassy carbon electrodes (GCE). Cobalt trioxides (Co 3 O 4 ) dodecahedron were initially derived from zeolitic imidazolate frameworks (ZIF) and interconnected by carbon nanotubes (CNTs). After that, the Co 3 O 4 -CNTs complexes were functionalized with platinum nanoparticles (PtNPs), giving rise to a hierarchic system (PtNPs@Co 3 O 4 -CNTs/GCE) ultrasensitive to the cooperative binding activity of Sudan I. The electrochemical responses of as-proposed PtNPs@Co 3 O 4 -CNTs/GCE sensors have been evaluated toward Sudan I detection under different optimum conditions. Especially, the obtained results demonstrated that the Pt 4.5 NPs@(Co 3 O 4 ) 1 -(CNTs) 1 /GCE sensor exhibits the superior electrochemical responses with high sensitivity (27870 μA·mM −1 ·cm −2 ), wide linear range (0.03 μM-100 μM) and low limit of detection (0.005 μM, S/N = 3). These results are promising for the development of high performance sensors of Sudan I which can be used for various food applications.
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JOURNAL OF MOLECULAR LIQUIDS
·
2021
·
IF 6.165
Fengxin Guo,Qiong Liu,Jiao Sha,Zidan Cao,Yuanhui Chong,Yu Li,Tao Li,Baozeng Ren
The solubility of amitriptyline hydrochloride (AMT) (Form I) in fourteen mono-solvents, including {methanol, 2-methoxyethanol, ethanol, 2-ethoxyethanol, n-propanol, 2-propoxyethanol, n-butanol, 2-butoxyethanol, n-octanol, n-hexanol, n-heptanol, n-pentanol, N-Methyl pyrrolidone (NMP), N,N-Dimethylformamide (DMF)} was determined under 0.1 MPa from 278.15 K to 323.15 K by laser detection method. The experimental results showed that as the temperature increasing, the solubility of AMT (Form I) gradually increased. The order of solubility of AMT (Form I) in fourteen mono-solvents at 298.15 K was: methanol (0.1753) > 2-methoxyethanol (0.1488) > 2-ethoxyethanol (0.1082) > 2-propoxyethanol (0.08140) > ethanol (0.07940) > 2-butoxyethanol (0.06600) > n-propanol (0.05720) > NMP (0.04480) > DMF (0.04230) > n-butanol (0.04050) > n-pentanol (0.03210) > n-hexanol (0.02700) > n-heptanol (0.02250) > n-octanol (0.004700). In addition, the Hansen solubility parameter (HSP) was applied to further discuss the miscibility of AMT (Form I) in the studied solvents. Molecular dynamics simulation explored the intermolecular interaction between solute and solvents. And the solvent effect of AMT (Form I) in the tested pure solvents was explained by the KAT-LSER model. The basic data of experimental solubility of AMT (Form I) were correlated with five thermodynamic models, including NRTL, λh, modified Apelblat, NRTL-SAC and two-Suffix Margules. Furthermore, the van't Hoff equation was applied to calculate the dissolution thermodynamic properties of AMT (Form I) in all tested solvents, including Δ dis H o , Δ dis S o and Δ dis G o .
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ACS Applied Energy Materials
·
2024
·
IF 5.4
Lei Zhou,Xin Wei,Junxiang Zhang,Xuecui Mei,Yun Li,Chaoyue Zheng,Furong Zhang,An Wen,Bin Wang
Sulfide solid electrolytes (SSEs) have some huge advantages in high room-temperature conductivity, good thermal stability, low interfacial resistance, etc. They are one of the ideal solid electrolytes for developing high energy density and high safety for all-solid-state lithium batteries (ASSLBs). However, the preparation of SSEs requires expensive Li2S as the raw material, whose high cost limits its practical application. Herein, a cost-effective SSE Li7.3P2.9S10.75X0.3 (X = F, Cl, Br, and I) was designed and prepared by using low-cost lithium and sulfur instead of expensive Li2S. Significantly, the cost of SSEs was reduced from $169.72 to $28.13 kg–1 based on replacing the Li2S strategy. Moreover, the prepared Li7.3P2.9S10.75X0.3 (X = F, Cl, Br, and I) solid electrolytes have a high ionic conductivity of 1.86–2.73 mS cm–1 at room temperature and a high voltage window of 5 V. On this basis, we assembled the all-solid-state lithium battery TiS2/Li7.3P2.9S10.75I0.3/Li–In, which presented a high initial discharge capacity of 219 mA h g–1 at room temperature and satisfactory cycle stability with a capacity retention of 86.7% after 100 cycles at 0.50 mA cm–2. This work provides an effective strategy for reducing the cost of SSEs, advancing the practical process of ASSLBs.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Menglu Wang,Bolong Liang,Shumin Lin,Zhe Zhao,Hongbin He,Xiliang Li,Shu-xuan Liang
The magnetic Fe 3 O 4 @ZIF-8 with high adsorption properties and easy separation were embedded in BiOX (X = Cl, Br, I) to synthesize Fe 3 O 4 @ZIF-8@BiOX using a simple one-pot solvothermal strategy. The crystal structure, surface morphology, photoelectric properties, thermal stability and magnetic response of the three materials were compared and analyzed, and the effect on the removal of OTC and Cr(VI) from single and coexisting systems by adsorption-photocatalysis is discussed. The results show Fe 3 O 4 @ZIF-8@BiOI has the highest separation efficiency of photogenerated carriers upon photoexcitation and stronger light absorption capacity, and exhibits better adsorption-photocatalytic activity than the other two materials in the photocatalytic reduction of Cr(VI) (68 % and 65 % removal for single and coexisting systems) and degradation of OTC (86 % and 59 % removal for single and coexisting systems). It is noteworthy that in the coexistence of Cr(VI) and OTC, a slight decrease of removal occurred, which could be due to a competitive effect between two pollutants being greater than the synergistic effect. ∙O 2 - is the main active substances in the adsorption-photocatalysis process. Finally, this work demonstrates the excellent adsorption and photocatalytic ability of Fe 3 O 4 @ZIF-8@BiOI for the simultaneous removal of Cr(VI) and OTC, which has great potential for practical wastewater treatment.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2024
·Vol. 416
·期 10
·2541-2551
·
IF 3.8
Niu Yanyan,Chen Yuxue,Zhou Juan,Sun Wei
In this study, an online electrochemistry coupling high-performance liquid chromatography-mass spectrometry (EC-HPLC-MS) technology has been developed for simulating metabolic reactions and rapid analysis of metabolites of flavone, quercetin, and rutin, which are not only widely present compounds with pharmacological activity in nature, but also have structural similarity and variability. The simulated metabolic processes of the substrates (phase I and phase II metabolism) were implemented on the surface of glassy carbon electrode (GCE) by using different electrochemical methods. After online chromatographic separation, the products were transmitted to a mass spectrometer for detection, in order to speculate relevant reaction pathways and structural information of the reaction product. The main metabolites, including methylation, hydroxylation, hydrolysis, and conjugation reaction products, had been successfully identified through the designed in situ hyphenated technique. Furthermore, compared with metabolites produced by in vitro incubation of rat liver microsomes, it was found that the products of electrochemical simulated metabolism were more abundant with diverse metabolic pathways. The results indicated that the proposed method exhibited advantages in the sample pretreatment process and detection cycle without compromising the reliability and accuracy of the results. Graphical
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Drug Testing and Analysis
·
2024
·
IF 2.6
Rui-Jia Chen,Zi-hua Zhang,Shenglan Yang,Shu-chen Yu,Jun-chang Wang,Ping-yong Liao,Ting-ting Qiu,Lu Xiao,Shang Xue,Hong Chen,Wen-bin Shao,Jian-wen Hu,Yun Lan,Xi-long Chen,Yue Xu,Tian-meng Zhou,Xue-jun Zhao,Wen-bin Liu
5F-MDMB-PICA, an indole-type synthetic cannabinoid (SC), was classified illicit globally in 2020. Although the extensive metabolism of 5F-MDMB-PICA in the human body warrants the development of robust analytical methods for metabolite detection and quantification, a current lack of reference standards for characteristic metabolites hinders such method creation. This work described the synthesis of 18 reference standards for 5F-MDMB-PICA and its possible Phase I metabolites, including three hydroxylated positional isomers R14 to R16 . All the compounds were systematic characterized via nuclear magnetic resonance, Fourier transform infrared spectroscopy, and high-resolution mass spectrometry. Furthermore, two methods were developed for the simultaneous detection of all standards using liquid chromatography–tandem mass spectrometry and ultra-performance liquid chromatography–quadrupole time-of-flight mass spectrometry. By comparison with authentic samples, R17 was identified as a suitable urine biomarker for 5F-MDMB-PICA uptake.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Lining Su,Guizhen Wang,Linlin Zhao,Yuan Deng,Yujing Guo,Yong Xiao,Huanwen Wang,Chuan Dong,Lifang Fan
Due to the urgent need for detecting trace amounts of 3,3′,4,4′-tetrachlorobiphenyl (PCB77) in the environment, we have developed an efficient and visible-driven photoelectrochemical (PEC) sensing platform based on carbon quantum dots (CQDs) modified titanium dioxide nanorods (TiO 2 NRs), coupling with exonuclease I (Exo I) assisted in target recycling for significant signal amplification. CQDs/TiO 2 NRs with high visible-light absorption ability and electron-hole separation efficiency is used as photoactive substrate for anchoring anti-PCB77 aptamer and its complementary DNA (cDNA). With the addition of PCB77, the specific interaction between PCB77 and its aptamer forces aptamer to separate from the electrode surface, resulting in an increase in photocurrent density. Adding Exo I in the test system, a self-catalytic target cycle was motivated, which significantly increased the PEC signal by more than twice, achieving signal amplification. The relationship between the photocurrent density changes and the concentrations of PCB77 are utilized to achieve quantitative detection of PCB77. The designed PEC sensing platform has good analytical performance with a detection limit as low as 0.33 pg L −1 , high selectivity and stability. Moreover, the PEC sensor is successfully used to evaluate the content of PBC77 in the environment samples. The established sensing platform provides a simple and efficient method for detecting trace amounts of PCB77 in the environment.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Chenglong Bao,Fengyu Wu,Fan Wang,Longyu Qiu,Menggang Li,Depeng Zhao,Yongsheng Yu,Weiwei Yang
The development of efficient heterogeneous catalysts for copper-catalyzed azide-alkyne cycloaddition (CuAAC) is crucial for overcoming the limitations of homogeneous systems, such as poor recyclability and catalyst leaching. In this study, we report the synthesis of nanosized hollow Cu(I)/Cu(II)-metal-organic frameworks (Nano-hollow Cu(I)/Cu(II)-MOF). The paddlewheel Cu(II) sites persist as robust structural nodes, while partial reduction engenders catalytically active planar tetranuclear Cu(I) sites strategically embedded within the framework. This unique architecture endowed Nano-hollow Cu(I)/Cu(II)-MOF with remarkable catalytic activity, achieving a turnover frequency (TOF) of 456.9 h −1 over 10 min for the CuAAC reaction between phenylacetylene and benzyl azide with a TOF 1.66-fold higher than the nanosphere control, underscoring the hollow structure's advantages. Moreover, the catalyst also demonstrated exceptional recyclability, maintaining a nearly constant catalytic conversion rate over 6 cycles. Theoretical calculations unveiled a dual‑copper synergistic mechanism, wherein coordinated charge redistribution mediated by both copper sites significantly lowered the activation barrier. The alkyne dehydrogenation is identified as the rate-determining step with a theoretical overpotential of 0.82 eV, which was pivotal for enhancing reaction efficiency. Beyond conventional catalysis, the Nano-hollow Cu(I)/Cu(II)-MOF exhibited versatile applicability, including rapid fluorescent molecule synthesis with a rate constant (k Flu ) of 0.1 min −1 and efficient DNA-templated ligation reactions with an apparent rate constant (k obs ) of 0.21 s −1 .
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Zeyan Yu,Shiyue Zhang,Jiyang Liu,Xiaofeng Dong
A homogeneous electrochemical aptasensor was developed for sensitive detection of aflatoxin B1 (AFB1) by integrating ultrasmall silica nanochannel film (SNF)-modified electrode, two-dimensional (2D) nanoprobes, and DNase I-assisted target recycling. The 2D nanoprobes (Ru(NH 3 ) 6 3+ /AFB1 Apt@GO) were prepared by co-loading cationic electrochemical probe Ru(NH 3 ) 6 3+ and AFB1 specific aptamers (AFB1 Apt) onto graphene oxide (GO) via π–π stacking and electrostatic interaction. SNF was rapidly formed on indium tin oxide (ITO) electrodes within 10 s. The resulting structure provided 2–3 nm nanochannels, which enabled the electrostatic enrichment of Ru(NH 3 ) 6 3+ . In addition, the 2D nanoprobes were unable to enter the ultrasmall nanochannels of the SNF due to size exclusion and thus could not access the underlying electrode surface. In the presence of AFB1, aptamer–target binding caused conformational changes and aptamer detachment, releasing Ru(NH 3 ) 6 3+ . The detached aptamer was digested by DNase I, triggering further Ru(NH 3 ) 6 3+ release as AFB1 participated in additional recognition cycles. The released Ru(NH 3 ) 6 3+ was electrostatically enriched at the electrode surface, amplifying the ECL signal. DNase I-assisted recycling enhanced the ECL response by 3-fold compared to the non-enzymatic system. Under optimized conditions, the aptasensor exhibited a linear detection range for AFB1 detection from 3.12 × 10 −4 to 312 ng/mL and a limit of detection of 302 fg/mL. The method was successfully applied to detect AFB1 in corn and peanut samples, offering a simple, rapid, and highly sensitive strategy for electrochemical toxin detection in food safety analysis.
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Small
·
2025
·
IF 12.1
Qiqiong Ren,Pei Wang,Nan Zhang,Guojun Zhou,Xian-Ming Zhang
Organic–inorganic hybrid materials face significant barriers to large-scale commercialization, primarily stemming from their intrinsic vulnerability to moisture-triggered hydrolytic degradation. Herein, an ultra-stable 2D copper(I) iodide, Cu 6 I 6 (26dmpz) 3 , is engineered through a synergistic waterproofing strategy that integrates atomic-level passivation and surface-interface hydrophobicity. N-metal coordination in Cu 6 I 6 (26dmpz) 3 (26dmpz = 2,6-dimethylpyrazine) passivates H-bond donors at atomic-level, blocking hydrolytic degradation induced by N─H···O interactions. Its methyl-dominated non-polar surface and “hydrogen-bond-free” contribute to low surface energy (37.68 mJ m −2 ) and polarity (4.09 mJ m −2 ), minimizing water adsorption, as corroborated by a 130.8° contact angle. The 2D corrugated groove structure creates a physical barrier against water penetration at solid–liquid interfaces. This endows Cu 6 I 6 (26dmpz) 3 with exceptional water stability, preserving its structure and luminescence after 30 days in water. Moreover, it shows bright orange–red emission (616 nm) with strong blue-light response, attributed to halide/metal-to-ligand charge transfer. The fabricated white LED exhibits an ultra-high color rendering index (CRI = 89.9), showing tremendous potential for high-quality solid-state lighting.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2025
·Vol. 27
·期 45
·24273-24283
·
IF 2.9
Jin Zou,Daoyun Zhu,Zhongfei Mu,Song Xu,Nurahmat Wali,Fugen Wu,Huafeng Dong,Xin Zhang,Xiao Wu,Yifei Luo,Yuchun Zhan
Near-infrared (NIR) spectroscopic technology has shown extensive application prospects. However, developing NIR phosphors with tunability and high thermal stability is a huge challenge. In this work, a highly promising phosphate compound, K3Ga2(PO4)3, has been successfully synthesized. When doped with Cr3+ ions, it is particularly noteworthy that Cr3+ exhibits highly efficient and thermally stable broadband NIR luminescence in the tetrahedral coordination environment. This unique property makes K3Ga2(PO4)3:Cr3+ a compelling candidate for advanced photonic applications. Therefore, studying the luminescent properties of Cr3+ rare earth ions doped into tetrahedral sites is of great significance. In the tetrahedral coordination environment of K3Ga2(PO4)3:Cr3+ ions exhibit broadband near-infrared emission spanning from 700 to 1100 nm (λem = 822 nm, FWHM = 124 nm) under 452 nm blue light excitation. Remarkably, the quantum efficiency reaches as high as 70.9%, demonstrating its exceptional potential for advanced photonic applications. In addition, the phosphors demonstrated exceptional thermal stability with near-zero thermal quenching. The NIR luminescence intensity at 373 K and 423 K retained 109.0% and 90.4% of its initial room-temperature value, respectively. This remarkable performance can be attributed to the material's ultra-wide band gap, and minimal electron–phonon coupling. The NIR pc-LED devices, fabricated by integrating the optimized K3Ga1.93(PO4)3:0.07Cr3+ phosphors with a blue LED chip (λex = 455 nm), achieved a near-infrared output power of 274 mW with a conversion efficiency of 5.42% under a driving current of 100 mA. Experimental results demonstrate that the fabricated NIR pc-LED exhibits significant potential for applications in night vision and vein imaging technologies. This study provides a strategic framework for designing high-performance NIR pc-LED devices, utilizing K3Ga2(PO4)3:Cr3+ as an efficient phosphor-converted light source, and offers valuable insights for practical implementation in advanced optical systems.
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