Environmental Science-Nano
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2020
·Vol. 7
·期 10
·3047-3061
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IF 7.683
Yang Bai,Fan Wu,Yanyan Gong
Antimony(III) or Sb(III) contamination in surface waters poses a serious threat to the ecological system and human health, and green and cost-effective technologies are urgently needed to mitigate its toxic effects. We green synthesized a novel oxidative sorbent, referred to as Al2O3-supported Fe–Mn binary oxide nanoparticles (Fe–Mn@Al2O3), and investigated its removal effectiveness and dynamic quantitative removal mechanisms of Sb(III) at environmentally relevant levels from simulated surface water. Fe–Mn binary oxides (Fe–Mn) were successfully attached on the surface of Al2O3via intermolecular hydrogen bonding, resulting in the formation of Fe–Mn@Al2O3 with a larger specific surface area, greater oxidizing reactivity, and more sorption sites compared to Fe–Mn. The resulting composite is mainly composed of FeOOH, Fe2O3, MnO2, and Al2O3. Life cycle assessment (LCA) indicated that the Fe–Mn@Al2O3 synthesis met green chemistry principles. Fe–Mn@Al2O3 at a Fe : Al2O3 molar ratio of 1 : 2 displayed an enhanced Sb(III) sorption capacity of 272.2 mg g−1 at pH 6.4 within 48 h. Sorption kinetic data were adequately simulated with the pseudo second-order kinetic model and the intraparticle diffusion model, suggesting that the sorption kinetics were a combination of chemisorption and intraparticle diffusion. The Freundlich isotherm model outperformed the Langmuir model in simulating the sorption isotherm data, which aligns with the heterogeneous surface sorption sites of Fe–Mn@Al2O3. MnO2 in Fe–Mn@Al2O3 oxidized Sb(III) to Sb(V), whereas FeOOH and Al2O3 acted as adsorption sites towards Sb(III) and Sb(V). Most importantly, Fe–Mn@Al2O3 still maintained high sorption efficiencies towards Sb(III) after five consecutive regeneration cycles. The dynamic quantitative removal mechanisms were proposed thereafter. Upon equilibrium, 92.8% of Sb(III) was sorbed by Fe–Mn@Al2O3, and 94.9% of sorbed Sb(III) was oxidized to produce Sb(V) and Mn(II). 59.1% of the formed Sb(V) was adsorbed onto Fe-Mn@Al2O3 and 40.9% of Sb(V) was released into the solution. The new quantitative and mechanistic insights contribute to an improved understanding of the uptake of Sb(III) by Fe–Mn@Al2O3 in natural and engineered systems, and the results may guide further preparation and application of reactive adsorbents for removal of redox-active contaminants from water.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2020
·
IF 3.232
Rongkun Zhu,Mushen Lai,Mingfang Zhu,Huanru Liang,Qing Zhou,Rui Li,Wenhao Zhang,Hongqing Ye
A functional ratio fluorescence sensor based on the molecularly imprinted polymer (MIP) coated double quantum dots (QDs) being composited of Mn-ZnS QDs and silica-coated graphene quantum dots (GQDs@SiO 2 ) had been established for the sensitive, selective and visual detection of sinapic acid (SA). MIPs@Mn-ZnS/GQDs@SiO 2 was synthesized through a simple one-pot sol-gel reaction, and it exhibited two fluorescence emission peaks with yellow fluorescence of Mn-ZnS QDs at 580 nm and the blue fluorescence of GQDs at 445 nm. SA can selectively enhance the fluorescence of GQDs but quench the Mn-ZnS QDs fluorescence to the MIPs@Mn-ZnS/GQDs@SiO 2 . The ratio of fluorescence enhancement to fluorescence reduction is linear with the concentration of SA from 9 to 81 nM with the detection limits of 0.8388 nM (S/N = 3). And the constructed fluorescent probe can also be used to visually detect SA according to the change of color. More importantly, molecular imprinting technique enables the sensors to selectively recognize the SA while other similar structure molecules hardly interfere with the SA determination in the measurement environment. Meanwhile, the fluorescence sensors have the advantages of fast response time and long duration of fluorescence intensity . These excellent performances made the proposed method to be applied for the determination of SA in Semen Sinapis and Descurainiae Semen .
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Qiang Liu,Bingsi Liu,Qinze Liu,Qiuyue Zhang,Rongnian Xu,Xuanyue Wu,Hong Xia
Refined design of sustainable sorbent demands to tackle the strong dependence for additional mesoporous support and low utilization in hot coal gas desulfurization. Unlike the well-established preparation of loading sorbents supported on zeolites, a vacuum-assisted self-assemble strategy tapping into the ordered channels of walnut wood is proposed to facilely fabricate three-dimensional (3D) (a%Ce–Mn) y Al 2−y O x desulfurizers with anisotropy which provides a desirable macroporosity for rapid diffusion of H 2 S. Benefiting from the inherent straight channle in micron scale, the obtained (8%Ce–Mn) 1.5 Al 0.5 O x presents the highest breakthrough sulfur capacity (289.79 mg g −1 ) and effective utilization (88.42%) at 700 °C. The favorable rapid diffusion of gases in micro/macropores improves greatly the H 2 O-resistance and anti-interference ability of 3D (8%Ce–Mn) 1.5 Al 0.5 O x for high steam and concentration of reducing gas. The fast mass transport in sulfidation reaction at 700 °C is described perfectly by the improved deactivation kinetics model. This study opens a novel design of the ideal 3D desulfurizers with micron porosity inherited from hierarchical architecture of walnut wood for industrialization utilization in the near future.
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RSC Advances
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2021
·Vol. 11
·期 45
·27845-27854
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IF 3.361
Mengxi Fan,Tingting Gan,Gaofang Yin,Fangbeibei Cheng,Nanjing Zhao
As one of the most widely used organophosphorus pesticides, chlorpyrifos (CPF) is toxic to humans. However, the rapid, effective and sensitive detection of CPF is still a challenge. In this paper, a novel molecularly imprinted phosphorescent sensor with a core–shell structure (Mn:ZnS QDs@ZIF-8@MIP) using Mn:ZnS quantum dots (QDs) as phosphorescent emitters was prepared for the highly sensitive and selective detection of CPF, and a simple and rapid room-temperature phosphorescence (RTP) detection method for CPF was proposed. For the prepared Mn:ZnS QDs@ZIF-8@MIP, Mn:ZnS QDs had good phosphorescence emission characteristics, ZIF-8 as support materials was used to improve the dispersibility of Mn:ZnS QDs, and molecularly imprinted polymer (MIP) on the surface of ZIF-8 was used to improve the selectivity of Mn:ZnS QDs for CPF. Under the optimal response conditions, the RTP intensity of Mn:ZnS QDs@ZIF-8@MIP showed a rapid response to CPF (less than 5 min), the RTP intensity ratio of P0/P had a good linear relationship with the concentration of CPF in the range of 0–80 μM, and the detection limit of this method was 0.89 μM with the correlation coefficient of 0.99. Moreover, this simple and rapid method has been successfully used to detect CPF in real water samples with satisfactory results, and the recoveries ranged from 92% to 105% with a relative standard deviation of less than 1%. This method combines the advantages of phosphorescence emission and molecular imprinting, and greatly reduces the potential interferences of competitive substances, background fluorescence and scattered light, which opens up a broad prospect for the highly sensitive and selective detection of pollutants in water based on molecularly imprinted phosphorescent sensors.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Yanhong Wang,Nannan Chen,Xiaoqiang Du,Xinghua Han,Xiaoshuang Zhang
Electrolysis of water is an environmentally friendly and promising hydrogen generation technology, which is one of the best ways to deal with the global energy crisis and environmental pollution. However, the slow anode reaction of water electrolysis is the bottleneck of limiting the efficient hydrogen production. Therefore, it is a key problem to explore an efficient and economical electrocatalyst to assist the anode reaction. Herein, a series of self-supporting M-NiCo 2 S 4 /Ni 3 S 2 (M=Mn, Fe, Cu, Zn) nanostructures grown on a nickel foam (NF) skeleton were prepared through one-step hydrothermal strategy. In this process, doping engineering is employed to adjust the electronic structure of catalyst and improve the performance of the catalyst. Among them, the introduction of Fe not only greatly changed the morphology, but also provided rich active sites. Specifically, the Fe-NiCo 2 S 4 /Ni 3 S 2 electrode can achieve current densities of 50 and 100 mA cm −2 at overpotential of 159 and 210 mV in alkaline media for oxygen evolution reaction (OER). In addition, driving current densities of 50 and 100 mA cm −2 in 1.0 M KOH with 0.5 M urea only requires the ultra-small voltage of 1.37 and 1.39 V (vs. RHE) for urea oxidation reaction (UOR), indicating that UOR can well replace OER to reduce electrical energy consumption. The experimental results and density functional theory calculations (DFT) demonstrate that the superior activity of the catalyst can be attributed to the optimal water adsorption energy, faster electron transfer rate, more active site exposure and good electrical conductivity . This work extends the application of doping engineering in water electrolysis and provides a novel preparation method of efficient catalyst for OER and UOR.
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ACS Sustainable Chemistry & Engineering
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2021
·
IF 8.198
Shen-Gen Gong,Yan-Hong Shi,Yang Su,Yan-Fei Li,Lei Ding,Jian Lin,Guo-Duo Yang,Bing Li,Xing-Long Wu,Jing-Ping Zhang,Hai-Ming Xie,Hai-Zhu Sun
Flexible asymmetric supercapacitor (FASC) systems are expected to exhibit not only excellent energy storage properties and safety but also satisfactory flexibility and robust integration. However, tremendous issues such as low capacitance, narrow voltage window, and poor mechanical properties still exist. In this paper, a novel kind of 3D lamellar Mn(OH)2 nanosheets on Cu-plated carbon cloth with a core-shell integrated framework (CPCC@CuO@Mn(OH)2) is fabricated to obtain the flexible material in the FASC. In this unique CPCC@CuO@Mn(OH)2 electrode material, the high theoretical specific capacity of CuO and Mn(OH)2 brings superior energy storage properties. Meanwhile, as the shell part, the deposited Mn(OH)2 layer and coated CuO layer work as both capacity contributors and substrate protectors, simultaneously maintaining the high capacitance and satisfactory flexibility of the electrodes. Therefore, the capacitance successfully achieves around 8140 mF cm–2 under 0.5 mA cm–2. Significantly, the assembled FASC (named as CPCC@CuO@Mn(OH)2//CC@AC) achieves a working voltage of up to 2.4 V. In the case of a high-power density close to 34.31 mW cm–3, its energy density reaches around 6.29 mW h cm–3. Moreover, the capacity holds 88.9% even after 10,000 cycles, showing its great application potential in the field of wearable electronics.
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TALANTA
·
2019
·
IF 4.916
Xueming Dang,Huimin Zhao
A hybrid of metal-organic frameworks (Fe, Mn) and Au nanoparticles anchored carbon nanotubes (Au/MOFs(Fe, Mn)/CNTs) was fabricated by a facile one-step hydrothermal process. The Au/MOFs(Fe, Mn)/CNTs exhibit highly enhanced peroxidase-like activity, because of the increased active sites, the enhanced partial charge density and electron transfer among the Fermi level of MOFs, Au and CNTs, as well as the synergistic action of Fe and Mn. The hybrid nanomaterials with high catalytic velocity (V max = 17.65 × 10 −7 M s −1 ) and affinity (K m = 0.33 mM) for substrates of H 2 O 2 display a great detection performance in the range of 0.34–53.05 nM with a limit of detection (LOD) of 0.18 nM (S/N = 3). Based on the cascade reaction of the artificial peroxidase and glucose oxidase (GOx), the glucose was further better detected in a linear range of 0.005–0.3 μM with a LOD of 0.002 μM (S/N = 3). Notably, considering the regulated peroxidase-like activity by sulfadimethoxine (SDM) aptamer , the concentration of SDM ranging from 0.54 to 41.58 μg L −1 was also detected with a LOD of 0.35 μg L −1 (S/N = 3). The as-synthesized hybrid nanozymes hold promising applications as the multifunctional sensing platform in environmental and biologic target detection with the combination of corresponding enzyme or specific aptamer.
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Catalysis Science & Technology
·
2019
·Vol. 9
·期 23
·6659-6668
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IF 5.726
Jie Yang,Haochen Yu,Yanbing Wang,Fuyuan Qi,Haodong Liu,Lan-Lan Lou,Kai Yu,Wuzong Zhou,Shuangxi Liu
Four types of Ca–Mn oxides, CaMnO3, CaMn2O4, CaMn3O6 and Ca2Mn3O8, have been prepared and used as supports for Pd nanoparticles. The oxygen activation capacity of these oxides and the catalytic activity of the oxide supported Pd nanocatalysts have been investigated using the aerobic oxidation of 5-hydroxymethyl-2-furfural as a model reaction. It is found that the local coordination environment of lattice oxygen sites plays a crucial role on their redox properties and charge transfer ability from Pd nanoparticles to the support. In particular, the Ca–Mn oxide with lower oxygen coordination number, weaker metal–oxygen bonds and tunnel crystal structure, e.g. CaMn2O4, exhibits promoted oxygen activation capacity, and stronger electron transfer ability. Consequently, Pd/CaMn2O4 exhibits the highest catalytic activity among these catalysts, providing a promising yield of 2,5-furandicarboxylic acid. This work may shed light on future investigations on the design of local structure of active oxygen sites in oxides or oxide supported catalysts for redox reactions.
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Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 38
·20448-20457
·
IF 8.867
Yufeng Wu,Jinxin Wei,Siyi Guo,Kaixin Yu,Zanyong Zhuang,Yan Yu
Utilizing biowaste shells (>95 wt% CaCO3) in chemical synthesis can both remediate environmental pollution and produce novel functional materials. Nonetheless, syntheses of nanomaterials from solid matter such as bio-shells are still rare. Herein, we for the first time reported the synthesis of a 0D/2D nanostructure, i.e., Ca(OH)2 nanosheets decorated with Mn3O4 quantum dots, from bio-shells in a green manner. Specifically, eggshells were calcined to form porous CaO that inherited a hierarchical framework from the source shell. The shell-derived CaO was then stirred together with KMnO4 in anhydrous ethanol at room temperature to generate the 0D/2D Ca(OH)2/Mn3O4 nanostructure (denoted as the Mn–Ca composite), in which Mn3O4 quantum dots were evenly dispersed on thin Ca(OH)2 nanosheets. Mechanism studies revealed that a trace amount of H2O released from the redox reaction between KMnO4 and ethanol regulated the slow hydrolysis and exfoliation of Ca(OH)2 nanosheets from the CaO framework. At the same time, the redox reaction generated Mn3O4 quantum dots that were deposited in situ on the Ca(OH)2 nanosheets, i.e., only where H2O was liberated and the hydrolysis of CaO took place. This mechanism allowed the uniform dispersion of Mn3O4 on the newly formed Ca(OH)2 nanosheets. Thanks to its unique 0D/2D structure, this Mn–Ca composite could highly efficiently extract trace-level Pb(II) from synthetic wastewater and outperformed many other Mn-based nanomaterials prepared purely from chemical reagents. This 0D/2D Mn–Ca composite possessed a high capacity for Pb removal (up to 1580 mg g−1 when the initial Pb(II) concentration was 1 g L−1), and it could also scavenge various other heavy metal ions such as Cu(II), Cd(II), Eu(III), Co(II), and Ag(I). Other biowaste shells such as oyster shells and clam shells also successfully produced a functional nanomaterial via the presented methodology. The current findings open a new way for biowaste recycling and may inspire the design of novel nanomaterials.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Ting Xiang,Xiunan Cai,Zhongqiu Luo,Xintao Zhou,Cuirong Yan,Jinying Yu,Jiayi Ge,Yueying Li
Fe-based composites exhibit favorable photo-Fenton catalytic performance for environmental remediation, but restricted by high electron hole recombination rate, low reactivity, and instability. Herein, a strategy of mechanical activation-strengthened Mn doping was innovatively proposed to construct Fe 2 O 3 porous microspheres derived from copper slag (CS) base polymers (MA-Mn/CS-Fe 2 O 3 ), and used for highly efficient photo-Fenton degradation of chloromycin hydrochloride (CTC). Benefiting from the collision and shearing of mechanical forces, improved mechanical strength and defect-rich structure were realized in the porous microspheres. Experiments and DFT calculation results reveal that mechanical activation (MA) strengthened Mn to replace the cation vacancy sites and iron ion sites in the octahedron of Fe 2 O 3 , resulting in the formation of rich oxygen vacancies (O V ) and new electronic transmission channels of O V Fe Mn, which act as trapping sites to enhance carrier separation, accelerate the Fe 3 + /Fe 2+ redox cycle, and boost the generation and transformation of reactive oxygen species (ROS). The O V Fe Mn facilitates H 2 O 2 adsorption for its barrierless dissociation into •OH by forming a bridging Mn Fe O O Fe Mn bond. Moreover, the hollow porous structure provides confined space for organic degradation, reduces ROS migration distance, and improves light utilization. These specialties contribute to the superior performance of the MA-Mn/CS-Fe 2 O 3 /Vis/Fenton system for CTC removal (97.3 % within 45 min) in a wide pH range (3 −11), remaining above 93.1 % efficiency after five consecutive cycles. This environmentally-friendly method offers new insights into the harmless treatment and valorization of CS and large-scale production of catalyst.
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Nanoscale
·
2017
·Vol. 9
·期 39
·15044-15055
·
IF 7.367
Dong Li,Guanjie Xing,Shilin Tang,Xiaohong Li,Louzhen Fan,Yunchao Li
We report herein a heat-triggered precursor slow releasing route for the one-pot synthesis of ultrathin ZnSe nanowires (NWs), which relies on the gradual dissolving of Se powder into oleylamine containing a soluble Zn precursor under heating. This route allows the reaction system to maintain a high monomer concentration throughout the entire reaction process, thus enabling the generation of ZnSe NWs with diameter down to 2.1 nm and length approaching 400 nm. The size-dependent optical properties and band-edge energy levels of the ZnSe NWs were then explored in depth by UV-visible spectroscopy and cyclic voltammetry, respectively. Considering their unique absorption properties, these NWs were specially utilized for fabricating photoelectrochemical-type photodetectors (PDs). Impressively, the PDs based on the ZnSe NWs with diameters of 2.1 and 4.5 nm exhibited excellent responses to UVA and near-visible light, respectively: both possessed ultrahigh on/off ratios (5150 for UVA and 4213 for near-visible light) and ultrawide linear response ranges (from 2.0 to 9000 μW cm−2 for UVA and 5.0 to 8000 μW cm−2 for near-visible light). Furthermore, these ZnSe NWs were selectively doped with various amounts of Mn2+ to tune their emission properties. As a result, ZnSe NW film-based photochromic cards were creatively developed for visually detecting UVA and near-visible radiation.
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JOURNAL OF SOILS AND SEDIMENTS
·
2025
·
IF 3
Xie Xin,Liu Wei,Wang Mingxin,Pan Xinxing,Xue Jinjuan,Yao Meng
Purpose This study provides a novel resource utilization strategy for the carbonized soil derived from lubricant-contaminated soil. Materials and methods In this study, the lubricant-contaminated soil was treated by pyrolysis and ball milling with manganese carbonate to obtain Mn-loaded carbonized soil (Mn@BCS), which was then reused to activate peroxymonosulfate (PMS) oxidation for degradation of aniline (AN) in wastewater. Results and discussion When the dosage of Mn@BCS and PMS was both 1 g/L, 100 mg/L of AN was almost completely removed within 6 h. Three reactive oxygen species (ROS), including \({\text{SO}}_{4}^{\bullet -}\) , •OH and \({}^{1}{\text{O}}_{2}\) , were detected and verified. The probe-based kinetics models were established with atrazine, nitrobenzene and metronidazole as probes to quantify the generation of ROS. The exposure of the \({\text{SO}}_{4}^{\bullet -}\) , \(\bullet \text{OH}\) and \({}^{1}{\text{O}}_{2}\) at 6 h was 5.32 × 10 –11 , 5.40 × 10 –12 , 2.52 × 10 –10 M s, which contributed 33.62%, 2.02% and 2.98% to AN degradation, respectively. The main active sites include Mn–O, oxygen containing groups and graphitized carbon. The Mn–O and oxygen containing groups can activate PMS to produce \({\text{SO}}_{4}^{\bullet -}\) and \({}^{1}{\text{O}}_{2}\) , respectively. The graphitized carbon promotes AN degradation by generation of \({\text{SO}}_{4}^{\bullet -}\) and accelerating direct electron transfer. Conclusions Ball milling with manganese carbonate significantly improves the activation performance of carbonized soil for PMS oxidation, and thus promote the resource utilization of post-remediation soil.
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