WATER RESEARCH
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2025
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IF 12.4
Haokun Bai,Peike Cao,Lanlan Liang,Shuo Chen,Xie Quan
Metal atomic cluster (AC) catalysts exhibit remarkable catalytic activity in environmental catalysis owing to their tunable structural and electronic properties regulated by electronic metal-support interactions (EMSI). Nevertheless, the precise size control of metal AC remains challenging owing to their inherent aggregation tendency under harsh synthetic conditions. Herein, we propose a confined synthesis strategy for fabricating cobalt AC within the interlayer channels of a two-dimensional molybdenum disulfide membrane (CoAC@MoS 2 membrane) for peroxymonosulfate (PMS) activation. The interlayer confinement of MoS 2 nanosheets enforces the in-plane assembly of metal precursors, yielding ultrafine CoAC (2.1 nm) with excellent Fenton-like activity (0.733 min -1 ), outperforming unconfined Co nanoparticles (29.3 nm, 0.291 min -1 ). Experiments and density functional theory calculations reveal that electrons transfer from sulfur vacancy and Mo sites in MoS 2 to Co 3d orbitals, generating electron-rich Co sites with an upshifted d -band center, which optimizes PMS adsorption and electron transfer to generate SO 4 ⚫- and ⚫OH radicals. The as-prepared CoAC@MoS 2 membrane achieved a sulfamethoxazole degradation rate of 5.33 × 10 6 μmol g metal -1 s -1 , which was 1-2 orders of magnitude higher than state-of-the-art nanoconfined catalytic membranes, and also proved effective in treating secondary pharmaceutical wastewater. This work establishes a universal paradigm for size and electronic structure engineering of metal catalysts through spatial confinement, advancing the development of high-performance Fenton-like catalytic systems for sustainable water remediation.
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Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 13
·7644-7653
·
IF 10.733
Jingyi Wu,Na You,Xiongwei Li,Hongxia Zeng,Shuai Li,Zhigang Xue,Yunsheng Ye,Xiaolin Xie
This study introduces an improved design of interlayers to achieve a balance between high Li+ diffusion and polysulfide inhibition in lithium–sulfur batteries. The design involves encapsulating mesoporous SiO2 nanospheres in few-layer MoS2 nanosheets via a facile one-step self-assembly to form a core–shell nanocomposite (SiO2@MoS2). The SiO2@MoS2 layer overlaid on a sulfur cathode simultaneously intercepts polysulfides and ensures rapid Li+ diffusion. Few-layer MoS2 as the shell is capable of breaking up polysulfides by a catalytic reaction, while mesoporous SiO2 as the core allows for physiochemical adsorption of such species; moreover, the densely packed hermetic SiO2@MoS2 nanocomposite layer provides an additional physical shield against polysulfide diffusion, realizing the full protection of the whole cathode. At the same time, the high Li+ density in the nanolayered MoS2 shell and the additional Li+ pathways created by the mesoporous SiO2 core allow for fast Li+ diffusion. Thus, a pristine sulfur cathode battery with a SiO2@MoS2 interlayer exhibits an outstanding electrochemical performance with a negligible capacity decay of 0.028% per cycle over 2500 cycles. The core–shell design suggested in this study could be extended to other nanomaterials for the optimization of Li–S battery interlayers.
研究领域:
材料科学
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储能
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纳米技术
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电化学
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ANALYTICAL CHEMISTRY
·
2018
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IF 6.042
Hui Zhu,Hui Zhang,Yunsheng Xia
In this study, we present a simple but effective fluorescent system for highly sensitive and versatile sensing of 2,4,6-trinitrotoluene (TNT) using few layered planar MoS2 quantum dots (QDs) as reporters. Excitation-independent emitting MoS2 QDs were first fabricated by using the proposed ultrasonic–hydrothermal-based top-down method assisted by carbon-free hydroxylamine hydrochloride. The obtained pristine MoS2 QDs were then modified with cysteine for introducing amino groups as TNT binding sites. The as-prepared MoS2 QDs possess a planar structure, which can more adequately interact with flat aromatic TNT molecules due to π–π attraction and decreased steric effects, compared with traditional spherical/quasi-spherical QDs. As a result, they exhibit extremely high sensitivity for TNT sensing (1 nM and 2 ng for solution and substrate assay, respectively). The common ions containing in environmental water samples do not interfere with the sensing. Furthermore, the QDs-decorated test paper shows an instantaneous (within 1 min) response to trace amounts of deposited TNT, and the fluorescence quenching can even be well-visualized by the naked eye. Because of favorable analytical performances, the proposed MoS2 QDs-based TNT sensing system has potential applications in both environmental water monitoring and security screening.
研究领域:
环境化学
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纳米材料
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荧光传感
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安全检测
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分析化学
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Changhui Zhou,Jinhua Li,Yan Zhang,Jing Bai,Pengbo Wang,Bo Zhang,Lina Zha,Mingce Long,Baoxue Zhou
Sulfurous and nitrogenous oxides, including NO x and SO 2 , and the generated substances NO x - and SO 3 2- widely exist in air and water as pollutants and thus are difficult to control in the environment. In this study, we designed a novel photoelectrocatalytic (PEC) system for the efficient conversion of SO 2 and NO x in mixed gases and NO x - and SO 3 2- in wastewater to N 2 and SO 4 2- , respectively, by activating SO 3 2- to form SO 3 • - . The key ideas include the conversion of SO 3 2- from SO 2 and efficient activation of SO 3 2- into SO 3 • - and further conversion into SO 4 • - by the MoS 2 /Fe 2 O 3 photoanode. Simultaneously, NO 3 - /NO 2 - originating from NO x was rapidly reduced to NH 4 + on the CuNW@CF cathode. Ultimately, the generated NH 4 + was selectively oxidized to N 2 by SO 4 • - and SO 4 • - was reduced to SO 4 2- . The results indicated that 99.9 % of TN was removed and 100 % of SO 3 2- was converted to harmless SO 4 2- . This study provides new insights into the treatment of sulfurous and nitrogenous oxides in air and water.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 14
·6958-6966
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IF 3.3
Xingyu Zhan,Hao Zhang,Yunxiong Zeng,Jingcai Xu,Ao Jin,Xinqing Wang,Jing Li,Yanting Yang,Bo Hong
Graphitic carbon nitride (CN) is considered to be a promising metal-free photocatalyst, but the charge carrier separation and rapid complexation of electrons and holes are difficult to modulate for effective and comprehensive photodegradation of TC. In this work, a MoS2 QD decorated sea-urchin carbon nitride nanohybrid was prepared via a water bath method. In comparison to the 85.6% degradation efficiency of sole sea-urchin carbon nitride (SUCN), the optimized 5% MoS2 QDs/SUCN (5%MSUCN) demonstrated a removal efficiency of 96.0% towards aqueous tetracycline (TC) under visible light. Such an outstanding photoactivity was mainly attributed to the interfacial synergistic effect of MoS2 QDs and SUCN, in which the outstanding charge extraction ability and quick surface kinetics of MoS2 QDs were primarily accountable for the subsequent deep photodegradation behavior of 5%MSUCN. A series of factors that may affect photoactivity of 5%MSUCN include pH values, inorganic ions, and organic matter. Finally, the deep photodegradation mechanisms of TC and intermediates were proposed based on ex situ HPLC-MS. This work not only explains the deep decomposition of TC but also presents a facile approach for designing and manufacturing carbon nitride nanohybrids.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2023
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IF 4.4
Yonghui Xuan,Xiang Li,Changling Yan,Gongke Wang
As traditional methods for detection of heavy metal pollution in water involve complex procedures and require expensive equipment, there is a great deal of interest in the development of rapid and simple methods for determining heavy metal ions in water. Here, a nanobiosensor based on molybdenum disulphide (MoS 2 ) nanosheets and fluorophore (FAM) labeled oligonucleotides was proposed, and fluorescence spectroscopy was adopted for detection of Hg 2+ or Ag + ions in aqueous solution. The principle underlying detection by the sensor involves the formation of T-Hg 2+ -T or C-Ag + -C mismatches by single-stranded DNA (ssDNA) rich in thymine (T) or cytosine (C), thereby forming stable double-stranded DNA (dsDNA) structures. By exploiting the different adsorption capacity of MoS 2 nanosheets for ssDNA and dsDNA, when oligonucleotides were in a single chain state, MoS 2 nanosheets possessed a strong adsorption capacity for ssDNA, resulting in fluorescence quenching of FAM. After the addition of Hg 2+ or Ag + , ssDNA formed double chains structure, the fluorescence recovered due to the weak adsorption capacity of MoS 2 nanosheets for dsDNA. Along this line, an “off-on” mode fluorescence nanobiosensor was designed to alternatively detect these two heavy metal ions in water. The sensor showed high sensitivity and excellent selectivity for both Hg 2+ and Ag + ions, with minimum detection limits of 6.8 nM and 8.9 nM, respectively.
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Carbon Letters
·
2023
·Vol. 33
·期 3
·847-862
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IF 4.5
Guo Huilin,Yu Tingting,Zhao Lei,Qian Jun,Yu Jiahe,Zhang Yu,Teng Yongyue,Zhu Chunshui,Yang Tao,Chen Wenbin,Gong Picheng,Jiang Cuishuang,Gao Changfei,Yang Bing,Yang Chenyu
In this study, a bipolar visible light responsive photocatalytic fuel cell (PFC) was constructed by loading a Z-scheme g-C 3 N 4 /carbon black/BiOBr and a Ti 3 C 2 /MoS 2 Schottky heterojunction on the carbon brush to prepare the photoanode and photocathode, respectively. It greatly improved the electron transfer and achieved efficient degradation of organic pollutants such as antibiotics and dyes simultaneously in two chambers of the PFC system. The Z-scheme g-C 3 N 4 /carbon black/BiOBr formed by adding highly conductive carbon black to g-C 3 N 4 /BiOBr not only effectively separates the photogenerated carriers, but also simultaneously retains the high reduction of the conduction band of g-C 3 N 4 and the high oxidation of the valence band of BiOBr, improving the photocatalytic performance. The exceptional performance of Ti 3 C 2 /MoS 2 Schottky heterojunction originated from the superior electrical conductivity of Ti 3 C 2 MXene, which facilitated the separation of photogenerated electron–hole pairs. Meanwhile, the synergistic effect of the two photoelectrodes further improved the photocatalytic performance of the PFC system, with degradation rates of 90.9% and 99.9% for 50 mg L −1 tetracycline hydrochloride (TCH) and 50 mg L −1 rhodamine-B (RhB), respectively, within 180 min. In addition, it was found that the PFC also exhibited excellent pollutant degradation rates under dark conditions (79.7%, TCH and 97.9%, RhB). This novel pollutant degradation system is expected to provide a new idea for efficient degradation of multiple pollutant simultaneously even in the dark.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Fei Long,Qixiang Zhang,Junjie Shi,Li Wen,Yonghui Wu,Ziqi Ren,Zunyu Liu,Yixin Hou,Ke Mao,Ke Niu,Nishuang Liu,Zhi Zhang,Luying Li,Jun Su,Fei Long,Yihua Gao
Aqueous zinc-ion batteries (AZIBs) are a green, low-cost and high-safety energy storage technology. Although MoS 2 is a promising electrode material, low conductivity and poor stability still limit their application in AZIBs. Constructing conductive heterostructures is an effective strategy to overcome these problems. Herein, metallic 1 T-MoS 2 nanosheets are innovatively combined with conductive Ti 3 C 2 MXene, resulting in enlarged 1 T-MoS 2 interlayers (from 9.5 to 9.9 Å) and enhanced hydrophilicity. This novel 1 T-MoS 2 /Ti 3 C 2 MXene heterostructure exhibits exceptional high-rate capability (284.3 mAh/g at 0.10 A/g with 105.2 mAh/g at 10.00 A/g) and long-term cycling stability (93.2 % capacity retention after 3000 cycles). High capacity comes from the expanded ion storage space caused by the extended layer spacing of the metallic 1 T-MoS 2 . Outstanding rate capability thanks to ultrafast electrons and ions transport from Ti 3 C 2 MXene. Prominent long-term cycling stability is attributed to the efficient synergistic effect of 1 T-MoS 2 and Ti 3 C 2 MXene in the 3D interconnected networks. As a proof of concept, the wearable quasi-solid-state Zn-ion battery employing the 1 T-MoS 2 /Ti 3 C 2 MXene cathode exhibits stable electrochemical performance under different bending conditions. This work explores a new route to design high-performance layered cathode materials for AZIBs.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Xiaoqin Wei,Hao Guo,Mingyue Wang,Zongyan Lu,Zeyun Yang,Lei Sun,Zhiguo Yu,Yinsheng Liu,Wu Yang
The detection of acetaminophen (ACOP) and its toxic hydrolyzed product p-aminophenol (4-AP) is very significant for clinical diagnosis and quality control of drug formulation. In this study, a novel electrochemical sensor based on MoS 2 embedding triangular Ag nanoplates (Tri-AgNPs) coated MOF-808 was developed for simultaneous and sensitive detection of ACOP and 4-AP. The morphology and structure MOF-808@MoS 2 /Tri-AgNPs nanocomposite were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), energy dispersive spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS) and so on. The electrochemical and electrocatalytic properties of the composite electrode were evaluated by cyclic voltammetry (CV) and differential pulse voltammetry (DPV). The experimental results demonstrated that the constructed sensor had excellent electrochemical performance for ACOP and 4-AP detection due to the synergistic interaction among MOF-808, MoS 2 and Tri-AgNPs. The proposed sensor exhibited a wide linear range (1–450 μM) and low limits of detection for detection of ACOP (0.054 μM) and 4-AP (0.046 μM). At the same time, the sensor also showed outstanding repeatability, reproducibility, stability and selectivity . In addition, MOF-808@MoS 2 /Tri-AgNPs/GCE was also employed to determine ACOP and 4-AP in acetaminophen tablets and Yellow River water samples with satisfactory recovery rates, which indicated the feasibility of the developed electrochemical sensor in the actual sample analysis.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Xi Chen,Songrong Li,Peizhen Yang,Yunfeng Chen,Cheng Xue,Yuhan Long,Jiayan Han,Jianming Su,Wenli Huang,Dongfang Liu
Peroxymonosulfate (PMS) heterogeneous catalysis dominated by nonradical pathway showed excellent adaptability for pollutant removal in complex water matrixes. Herein, ultra-small Fe-doped MoS 2 nanosheets with N-doped carbon intercalation (CF-MoS 2 ) were synthesized via a one-step hydrothermal method to treat high salinity organic wastewater. CF-MoS 2 exhibited an expanded interlayer spacing by 1.63 times and the specific surface area by 9 times compared with Fe-doped MoS 2 (F-MoS 2 ), substantially increasing the active sites. Homogeneous Fe 2+ catalytic experiments confirmed that the promotion of carbon intercalated MoS 2 (C-MoS 2 ) on Fe 3+ /Fe 2+ redox cycle was much higher than pure MoS 2 . Besides, the considerable removal of tetracycline (TC) under high salinity conditions (0–7.1%) was attributed to the dominant role of PMS nonradical oxidation pathways, including 1 O 2 and surface-bound radicals. The catalytic sites included Fe 3+ /Fe 2+ , Mo 4+ /Mo 5+ /Mo 6+ , C=O, pyridine N, pyrrolic N and hydroxyl groups . Finally, density functional theory (DFT) was employed to get the radical electrophilic attack sites and nucleophile attack sites of TC, and the results were consistent with the TC degradation products determined by HPLC-MS. This work would broaden the application of MoS 2 -based catalysts, especially for PMS catalytic removal of organic pollutants from high salinity wastewater.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2022
·
IF 9.221
Shuang Li,Jiawei Zhang,Cherie S. Tan,Chong Chen,Chang Hu,Yongchang Bai,Dong Ming
As important biomarkers for prostate cancer, total prostate specific antigen (tPSA) and free prostate specific antigen (fPSA) levels in serum play essential roles in early diagnosis. In this study, hybrid molybdenum disulfide (MoS 2 )/Pt@Au-nanoprism/polydopamine (PDA)-modified screen-printed electrodes were utilized to detect both fPSA and tPSA in serum simultaneously. MoS 2 generated by the hydrothermal method assembled on the electrode to provide binding sites for further modification. Au nanoprisms were obtained by reducing chloroauric acid with sodium thiosulfate to achieve uniformity. Pt nanoparticles covered on Au nanoprisms by the displacement method, and the generated Pt@Au-nanoprism structure was then deposited onto the electrode to enhance the electrochemical signals. An electropolymerization-synthesized PDA film further modified the electrode to increase antibody binding sites. The results demonstrated that the proposed electrochemical immunosensor for fPSA and tPSA analysis in serum using differential pulse voltammetry (DPV) had a wide linear range from 0.0001 ng/mL to 100 ng/mL, with limits of detection (3 SD/slope) at 0.1 pg/mL and 1.1 fg/mL, respectively. For clinical patient samples, the proposed biosensor demonstrated good accuracy according to the clinical electrochemiluminescence immunoassay and improved the diagnostic specificity of tPSA concentrations in the “gray zone", suggesting promising prospects for clinical applications of our multiplex biosensors.
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International Journal of Environmental Research and Public Health
·
2022
·Vol. 19
·期 5
·2934
·
IF 4.614
Hong Liu,Houwang Chen,Ning Ding
In this research, the preparation of a Ag3PO4/g-C3N4@MoS2photocatalyst and the performance and mechanism of degradation of 2-amino-4-acetaminoanisole (AMA) were studied. The phase composition and morphology of the synthesized samples were comprehensively characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), ultraviolet–visible diffuse reflectance (UV–Vis), and photoelectron spectroscopy (XPS). The catalytic performance of the photocatalyst was evaluated by the visible-light catalytic degradation of the AMA. The experimental results show that the Ag3PO4/g-C3N4@MoS2composite photocatalyst has stronger photocatalytic oxidation and reduction capabilities than Ag3PO4and Ag3PO4/g-C3N4. The material only decreases by 31.3% after five cycles of use, indicating that the material has good light stability. Free radical capture experiments prove that photo-generated holes (h+) and superoxide radicals (·O2−) are the main active substances in the photocatalytic process. The fundamental studies in the present research provide a new perspective for constructing an innovative type of visible-light photocatalyst and a new way to promote the photocatalytic degradation of organic pollutants.Keywords:catalysis;degradation;nanomaterials;Ag3PO4;heterojunction formation
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