JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Senda Su,Xiaoman Li,Xu Zhang,Jingting Zhu,Guodong Liu,Mengyao Tan,Yingying Wang,Min Luo
The incorporation of polyoxometalates (POMs) in metal-organic frameworks (MOFs) with host-guest structure have proven to be effective strategy to rational design of heterogeneous catalysis. In this study, the Keggin-type POM@MIL-101(Cr) composite catalysts (PMo 12 , PW 12 and SiW 12 ) are synthesized for nitrogen fixation reaction without sacrificial agents at room temperature in the first time. The SiW 12 molecules are encapsulated in smaller cavities of MIL-101(Cr) by solvothermal method and in larger cavities by impregnation method, respectively. Solvothermal synthesized catalyst has a performance of 75.56 μmol·h −1 ·g -1 cat and TOF value of 1.95 h −1 , which are about 10 and 88 times than that of Na 4 SiW 12 O 40 . The excellent performance is ascribed to the synergistic effect of SiW 12 and MIL-101(Cr). The MIL-101(Cr) adsorbs a large amount of N 2 and generates sufficiently photogenerated electrons under sunlight irradiation, and electrons quickly transfer to the SiW 12 through hydrogen bonds. Moreover, the agglomeration effect of the homogeneous catalyst SiW 12 is weakened due to encapsulation with more exposed active sites. This work provides a feasible route to design and synthesize nanocomposite materials with exceptional performance for photocatalytic nitrogen fixation.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2019
·
IF 2.931
Fanglin Ming,Jingzhou Hou,Changjun Hou,Mei Yang,Xianfeng Wang,Jiawei Li,Danqun Huo,Qiang He
A novel, simple and low-cost nitrogen doped carbon dots (N-CDs) fluorescent sensor for sensitive detection of Cr (VI) was developed via one-step hydrothermal method using thymidine as carbon source. As-prepared N-CDs exhibited the ability of sensitive and selective detection of Cr (VI) through the inner filter effect (IFE). The performances of N-CDs were investigated with the characterization methods of transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). Under the optimized conditions, a good logarithm correlation between the fluorescence intensity of N-CD S and the concentration of Cr (VI) was obtained ranging from 0.1 μM to 430 μM (R 2 = 0.992), with a low detection limit (LOD; S/N = 3) of 1.26 nM. The fluorescent sensor showed good repeatability, reproducibility and stability. Furthermore, N-CDs fluorescent sensor had a good applicability for Cr (VI) detection in real water samples with acceptable recoveries, and the detection results were consistent with the inductively coupled plasma mass spectrometry (ICP-MS) results, indicating this fluorescent sensor has a great potential for the environmental monitoring.
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Inorganic Chemistry Frontiers
·
2019
·Vol. 6
·期 11
·3057-3062
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IF 5.934
Weixuan Zeng,Sheng Cao,Lulu Qiao,Anquan Zhu,Quanyin Ma,Xiewen Xu,Yi Chen,Jun Pan
In the present study, we report a one-step hydrothermal synthesis of visible-light response Cr-doped Sr2Ta2O7 nanosheets for photocatalytic hydrogen generation. It is discovered that the Cr ion is successfully doped into the Sr2Ta2O7 nanosheet crystal lattice and uniformly distributed without changing the crystal structure and morphology of the Sr2Ta2O7 host. Compared to pristine Sr2Ta2O7, the as-prepared Cr-doped Sr2Ta2O7 photocatalysts show enhanced photocatalytic activity for hydrogen generation under visible-light irradiation. The spectroscopy and Mott–Schottky results reveal that proper Cr doping can narrow the band gap of Sr2Ta2O7 as well as facilitate the separation of photo-generated electrons and holes, thus enhancing the photocatalytic performance under visible-light irradiation. This work provides a simple approach to fabricate visible-light active tantalum-based oxide photocatalysts.
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Nanoscience and Nanotechnology Letters
·
2019
·Vol. 11
·期 2
·229-233
·
IF 0
Zhao Tian,Yu Jun,He Ziyu,He Nongyue,Dong Ming,Chen Zhu,Chen Hong
The well investigated chromium-benzenedicarboxylate metal-organic framework (MOF), nano-sized MIL-101(Cr), was synthesized in this study by using tetramethylammonium hydroxide (TMAOH) or acetic acid (HAc) as modulator. The addition of TMAOH/HAc played a crucial role on particle size
and morphology of MIL-101(Cr). The obtained MIL-101(Cr) had average diameter of about ∼90 nm in selected condition, and possessed relatively high porosity (the BET surface area can up to 3500 m2/g). Furthermore, compared to bulk phase MIL-101(Cr), the nano-MIL-101(Cr) presented
significant improvement of catalytic activity in oxidation of indene.
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ANALYTICAL CHEMISTRY
·
2015
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IF 5.636
Juan Wei,Zheng Guo,Xing Chen,Dong-Dong Han,Xiang-Ke Wang,Xing-Jiu Huang
Detection of Cr(VI) by electrochemical methods generally focuses on noble-metal-modified electrodes in strong acid solution using voltammetric techniques. In this work, we report a new strategy to detect Cr(VI) as HCrO4– at pH 5.0 in drinking water using electrochemical impedance spectroscopy. The strategy is based on the high-affinity and specific binding of crown ethers (i.e., azacrown) to HCrO4–, which forms sandwich complexes between them via hydrogen bonds and moiety interactions with K+ captured by azacrown on its self-assembled Au electrode surface. This then blocks the access of redox probes (Fe(CN)63–/4–) to the self-assembled Au electrode, further resulting in an increase in the electron transfer resistance. This method offers a detection limit of 0.0014 ppb Cr(VI) with a sensitivity of 4575.28 kΩ [log c (ppb)]−1 over the linear range of 1–100 ppb (R2 = 0.994) at pH 5.0. In addition, the azacrown self-assembled Au electrode has good selectivity for Cr(VI) with good stability and low interferences. This approach can be performed on spiked Cr(VI) as well as real samples. To the best of our knowledge, this is the first example of electrochemical impedimetric sensing that allows ultrasensitive and ultraselective detection of Cr(VI).
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MOLECULES
·
2017
·Vol. 22
·期 4
·572
·
IF 2.861
Yun Zheng,Zihao Yu,Feng Lin,Fangsong Guo,Khalid A. Alamry,Layla A. Taib,Abdullah M. Asiri,Xinchen Wang
As a promising conjugated polymer, binary carbon nitride has attracted extensive attention as a metal-free and visible-light-responsive photocatalyst in the area of photon-involving purification of water and air. Herein, we report sulfur-doped polymeric carbon nitride microrods that are synthesized through thermal polymerization based on trithiocyanuric acid and melamine (TM) supramolecular aggregates. By tuning the polymerization temperature, a series of sulfur-doped carbon nitride microrods are prepared. The degradation of Rhodamine B (RhB) and the reduction of hexavalent chromium Cr(VI) are selected as probe reactions to evaluate the photocatalytic activities. Results show that increasing pyrolysis temperature leads to a large specific surface area, strong visible-light absorption, and accelerated electron-hole separation. Compared to bulk carbon nitride, the highly porous sulfur-doped carbon nitride microrods fabricated at 650 °C exhibit remarkably higher photocatalytic activity for degradation of RhB and reduction of Cr(VI). This work highlights the importance of self-assembly approach and temperature-control strategy in the synthesis of photoactive materials for environmental remediation.Keywords:carbon nitride;self-assembly;photocatalysis;pollutant degradation;Cr(VI) reduction
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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Xiaofeng Yi,Shurui Liu,Mingyu Luo,Qingbiao Li,Yuanpeng Wang
Microbe-photocatalyst biohybrids, integrating the optimal attributes of whole-cell catalysts and nanometer photocatalysts, have emerged as a promising strategy for environment-associated applications. However, few such biohybrids have been tested for complex pollution systems. Herein, we constructed an outer membrane photosensitized Geobacter sulfurreducens ( G. sulfurreducens )-CdS biohybrid, which enabled to generate stronger photocurrent in response to irradiation and meanwhile achieved an significant promotion for the redox transformation of Cr(VI) and tetracycline compared with that of bare G. sulfurreducens or CdS counterparts. Further analysis revealed that the outer membrane played a significant role in photoelectron transfer. Differential pulse voltammetry (DPV) tests demonstrated that CdS enhanced the catalytic activity of C-type cytochromes on the outer membrane under irradiation, resulting in the increase of electron-hole pairs separation efficiency. The possible degradation pathway of tetracycline was proposed based on determined intermediates, whose toxicities were well evaluated. Importantly, the toxicity of the final detected intermediates was apparently decreased. Overall, this work aims to explore the working mechanisms of the novel G. sulfurreducens -CdS biohybrid system and opens up a new avenue to purifying combined wastewater by microbe-photocatalyst biohybrids.
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Inorganics
·
2022
·Vol. 10
·期 3
·33
·
IF 3.149
Tian Zhao,Hexin Zhu,Ming Dong,Minmin Zou,Songfan Tang,Mingliang Luo,Xianggang Li
The chromium-benzenedicarboxylate metal–organic framework (MOF), MIL-101(Cr), is one of the most well-investigated and widely used prototypical MOFs. Regarding its synthesis, the use of a toxic modulator (usually HF) and high reaction temperature (220 °C) are the main factors hindering its further expansion of production and utilization. In fact, high quality MIL-101(Cr) crystals can be prepared at a much lower temperature (160 °C) with spherical morphology via an additive-free approach. Compared to traditional octahedral MIL-101(Cr), the spherical MIL-101(Cr) possesses higher adsorption performance toward dye molecules, including methyl orange (MO) and rhodamine B (RB). The results suggest that toxic additives and high reaction temperatures are not essential in the synthesis of MIL-101(Cr), and the fabrication of spherical MIL-101(Cr) may offer a facile and effective pathway for the large-scale industrial application of MIL-101(Cr).
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JOURNAL OF POROUS MATERIALS
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2025
·
IF 3.2
Li Jionghui,Zhang Weiquan,Chen Qing,Xiong Chunhua
Polyacrylonitrile-2-aminopyridine (PAN-TAP) is a novel chelating fiber rapidly prepared by microwave-assisted synthesis method. The optimal synthesis conditions are microwave power of 800 W, reaction at 140 ℃ for 20 min. Fourier transform infrared spectroscopy (FT-IR) shows nucleophilic addition reaction between cyanide and 2-aminopyridine in PAN fibers. thermogravimetric analysis (TGA) shows that the synthesized material is stable within 200 ℃. Scanning electron microscopy (SEM) shows that synthetic materials have a larger diameter and a very rough surface compared to PAN fibers. The synthesized materials were also characterized by elemental analysis, energy dispersive X-ray spectroscopy (EDS), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). Meanwhile, the adsorption characteristics and mechanism of PAN-TAP for Cr(Ⅵ) were evaluated. When the pH of the solution is 2, the adsorption capacity of Cr (Ⅵ) is the highest and it has good separation ability, with a maximum separation coefficient of β Cr/Ni = 357.75. The adsorption process conforms to the Langmuir isothermal adsorption model and the pseudo-second-order kinetic model, indicating that the adsorption mechanism is a chemisorption of monolayer adsorption. Cr(Ⅵ) is reduced to Cr(Ⅲ) by the amino groups on the fiber and then adsorbed. The maximum theoretical adsorption capacity is 287.1 mg/g (at 298 K), and the adsorption equilibrium can be reached within 1 h. The thermodynamic parameter Δ H > 20 kJ·mol − 1 indicates that adsorption is a spontaneous endothermic process. PAN-TAP fibers can be eluted with hydrochloric acid and reused. Overall, PAN-TAP is a cost-effective and rapid adsorbent, which has broad application prospects for the removal of Cr(Ⅵ) in water.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Liqing Zhang,Bo Li,Zhenye Jiang,Haoyuan Xu,Chengqian Li,Yonggang Wei,Hua Wang
Among many pollution sources, Cr(VI) has captured much attention because of its strong toxicity, bioaccumulation and carcinogenicity. In recent years, nanoscale magnesium oxide has shown great potential in removing Cr(VI) pollution in water by virtue of its excellent adsorption and environmental friendliness. In this study, a high‑magnesium slag produced during the nitric acid pressure leaching process of laterite nickel ore was utilized as raw material for nano MgO preparation. A nano MgO-based adsorbent material (T-MgO) was prepared via the modification of MgO by nano TiO 2 which was synthesized use low-grade titanium slag as titanium source. Adsorption results demonstrated that T-MgO exhibits rapid adsorption performance, reaching adsorption equilibrium within 60 min. The kinetic adsorption conforms to the pseudo-second-order (PSO) model, revealing a chemisorption-dominated mechanism. According to the Freundlich model analysis, saturated adsorption capacity of the T-MgO for Cr(VI) reached 241.53 mg/g. The T-MgO material also possesses excellent reusability and selectivity to Cr(VI) adsorption. Furthermore, an in-depth analysis was performed to elucidate the Cr(VI) removal mechanism. Cr(VI) existing as HCrO 4 − and Cr₂O₇ 2− species under pH = 2 is electrostatically adsorbed on the protonated active sites of T-MgO. With the participation of free electrons generated by the nano-TiO 2 semiconductor, Cr(VI) is reduced to low-toxicity Cr(III), forming Mg-O-Cr bonds. The study achieved the purposes of superior and economic removal of Cr(VI) and high value-added utilization of the magnesium and titanium secondary resources.
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Surfaces and Interfaces
·
2025
·
IF 6.3
Tang Xiaojing,Shakeel Zeb,Hao Li,Abdul Haleem,Zhong Hua
The removal of hexavalent chromium from wastewater is a pressing environmental challenge due to its high toxicity and strong mobility in aquatic systems. To address this issue, we engineered a three-dimensional porous biomonolith via redox cryopolymerization, leveraging the abundant functional groups and structural advantages of covalently crosslinked lignin and chitosan for efficient chromium adsorption. Remarkably, the developed biomonolith exhibited a high chromium adsorption capacity of 232.2 mg/g at pH 2, reaching 63.6% of equilibrium uptake within the first 30 min and achieving full equilibrium in 90 min. This enhanced performance stems from the synergistic effects of the material’s macroporous structure, which facilitates rapid chromium diffusion, and its multifunctional surface chemistry, featuring amine, amide, sulfonic, and oxygen-containing groups. These functional groups promote chromium adsorption through electrostatic interactions and partial reduction of Cr(VI) to Cr(III), as confirmed by X-ray photoelectron spectroscopy (XPS). The positively charged Cr(III) further strengthens electrostatic interactions with lignin’s oxygen-containing groups, enhancing adsorption. The chromium adsorption process followed the pseudo-second-order kinetic model (R² = 0.972) and the Freundlich isotherm (R² = 0.93), indicating chemisorption and surface complexation as the dominant mechanisms. The developed biomonolith exhibits enhanced selectivity, improved shelf stability, and excellent reusability for chromium adsorption. This lignin-based biomonolith presents a promising solution for Cr(VI) removal, offering significant potential for environmental applications and advancing research in sustainable wastewater treatment.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Mimi Sun,Jiahui He,Wanting Xiang,Wei Zou,Wenfei Song,Yating Xi,Jun Yan,Meimei Zhou,Pingping Luo
The design and construction of diverse heterojunction architectures have emerged as an effective strategy for enhancing the photocatalytic performance of semiconductors. In this study, ZIF-8/TiO 2 composite nanofibers were successfully fabricated by combining electrospinning technology with a facile in-situ solvothermal method, followed by ZIF-8 sulfurization to form ZnS/TiO 2 nanofiber heterostructures. Comprehensive characterization confirmed that ZIF-8 on the surface of TiO 2 nanofibers was completely converted into ZnS, establishing a robust and intimate interface with TiO 2 . The resulting ZnS/TiO 2 heterojunction exhibited remarkable photocatalytic reduction activity for Cr(VI), achieving 100% removal efficiency within 20 min under visible light irradiation. The photocatalytic reaction rate constant of the ZnS@TiO 2 nanofibers was approximately 10 and 319.5 times higher than those of pristine ZnS and TiO 2 nanofibers, respectively. This enhanced photocatalytic performance is attributed to the formation of the heterojunction, which effectively narrows the bandgap of the composite, optimizes photogenerated charge transfer pathways and significantly improves electron-hole pairs separation. Furthermore, mechanistic studies identified photogenerated electrons (e − ) and superoxide radicals ( O 2 − ) as the dominant active species involved in the photocatalytic reduction process. This work provides both fundamental understanding and practical methodology for developing high-performance TiO 2 -based photocatalytic systems, highlighting their potential for advanced water purification technologies.
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