Catalysis Science & Technology
·
2019
·Vol. 9
·期 23
·6659-6668
·
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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高影响因子
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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高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Mengwei Guo,Bo Zhang,Qibo Zhang
In this work, sulfur-doped manganese (S-Mn/CP) pre-catalysts supported by carbon paper (CP) were prepared from choline chloride/ethylene glycol-based deep eutectic solvent containing different manganese salts via electrodeposition method. The effect of anions, including NO 3 – , Cl - , SO 4 2- , CH 3 COO – , and crystal water (H 2 O), on the evolution of the structure and OER activity of as-prepared Mn-based pre-catalysts was analyzed. It turns out that the NO 3 – and H 2 O can be reduced during the electroreduction of Mn(II) species and induce the formation of manganese oxide/hydroxide. Thiourea (TU), used as a sulfur source, decomposes at the cathode and releases S 2- . The TU and H 2 O replace the Cl - in the [Mn(Cl) 6 ] 4- to form [Mn(Cl) 6- x (H 2 O) x ] x -4 and [Mn(Cl) 6- x - y (TU) y (H 2 O) x ] x + y -4 complexes, promoting the electroreduction of Mn(II) species. The OER intrinsic catalytic activity of the amorphous Mn 3 O 4 pre-catalyst is 16.3 times lower than that of the metallic Mn 0 pre-catalyst in a 1.0 M KOH solution. After annealing in an argon atmosphere, the surface of metallic Mn 0 is in-situ converted into Mn 3 O 4 and exhibits superior activity (0.0395 A g −1 cm -2 ECSA ) than the ordinary Mn 3 O 4 electrode (0.0088 A g −1 cm -2 ECSA ). This study brings insights into the effect of anion on the evolution of structure-activity of Mn-based pre-catalysts during the electrodeposition and OER catalytic process.
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Zelai Cheng,Liming Xu,Xi Wang,Xiaohui Wu,Fangyi Huang,Yulan Jing,Hua Su
Gillespite-type SrCu 0.95 B 0.05 (B 2+ :Cu,Co,Mn,Ni,Mg,Zn)Si 4 O 10 (SCBS) ceramics were prepared by high-temperature solid-state method. Their microwave dielectric properties and crystal structure evolution were studied by P–V-L theory, bond valence model, and X-ray photoelectron spectroscopy. Varying B 2+ ion changed ionic polarizability and bond ionicity, causing dielectric constant ε r of SCBS to change. The change in quality factor Q × f was explained by lattice energy, oxidation state of Cu, and internal strain/fluctuation. The temperature coefficient of resonator frequency τ f was regulated by B–O bond length and valence. The optimal microwave dielectric properties were exhibited by SrCu 0.95 Mn 0.05 Si 4 O 10 after sintering at 1050 °C: ε r ∼5.8 ± 0.03, Q × f ∼65,589 ± 2611 GHz (@15.8 GHz), and τ f ∼ -50 ± 4 ppm/°C. These materials show great potential application prospects for 5G/6G wireless communication.
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Materials
·
2023
·Vol. 16
·期 20
·6667
·
IF 3.4
Yukun Li,Svenja Hanson,Cheng Heng Pang,Peng Lyu,Jun Jiang
In order to attain phosphor ceramics with a high Color-Rendering Index (CRI), samples with the composition of Y0.997−xRexCe0.003)3(Al0.9748Mn2+0.024Cr3+0.0012)5O12(Rex= 0, Gd0.333, Gd0.666, Gd0.997, Tb0.333, Tb0.666, Tb0.997and Lu0.997were prepared by solid-state reaction and vacuum sintering, and exhibited potential for high-quality, solid-state lighting. Doping with Cr3+and Mn2+effectively enhanced the red component of Ce3+spectra through the intense energy transfer from Ce3+ions to Mn2+/Cr3+ions. The crystal field splitting of [GdO8] and [TbO8] was more extensive than that of [YO8], causing a massive redshift in the Ce3+emission peaks from 542 to 561 and 595 nm, while [LuO8] had an opposite effect and caused a blueshift with a peak position at 512 nm. White LED devices incorporating Ce/Mn/Cr: (Gd0.333Y0.664)3Al5O12phosphor ceramic exhibited a high CRI of 83.97, highlighting the potential for enhancing the red-light component of white LED lighting.Keywords:garnet phosphor;laser lighting;full spectrum;spectral modulation;Ce/Mn/Cr: (Re,Y)3Al5O12
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高影响因子
ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Zhenyi Hu,Geng Su,Shujun Long,Xiaoting Zhang,Linkun Zhang,Yilin Chen,Chang Zhang,Gonggang Liu
Highly efficient resource recycling and comprehensive utilization play a crucial role in achieving the goal of reducing resource wasting, environmental protection, and achieving goal of sustainable development . In this work, the two kinds waste resources of agricultural rice husk and metal ions (Co, Ni, and Mn) from spent lithium-ion batteries have been skillfully utilized to synthesize novel Fenton-like catalysts. Desiliconized rice husk carbon (DRHC) with rich pore structure and large specific surface area from rice husk has been prepared and used as scalable carrier, and dandelion-like nanoparticles cluster could be grown in situ on the surface of the carrier by using metal ions contained waste water. The designed catalysts (X@DRHC) as well as their preparation process were characterized in detail by SEM, TEM, BET, XRD and XPS, respectively. Meanwhile, their catalytic abilities were also studied by activating potassium peroxomonosulfate (PMS) to remove methylene blue (MB). The results indicate X@DRHC displays excellent degradation efficiency on MB with wide pH range and stable reusability, which is suitable for the degradation of various dyes. This work has realized the recycling and high-value utilization of waste resources from biomass and spent lithium-ion batteries, which not only creates an efficient way to dispose waste resources, but also shows high economic benefits in large-scale water treatment .
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·
IF 5.8
Wang Hongqiang,Huang Sheng,Liao Lei,Mo Shengpeng,Zhou Xiaobin,Fan Yinming
Replacing NH 3 in NH 3 -SCR with VOCs provides a new idea for the simultaneous removal of VOCs and NO x , but the technology still has urgent problems such as high cost of catalyst preparation and unsatisfactory catalytic effect in the low-temperature region. In this study, biochar obtained from sewage sludge calcined at different temperatures was used as a carrier, and different Co and Mn injection ratios were selected. Then, a series of sludge-based biochar (SBC) catalysts were prepared by a one-step hydrothermal synthesis method for the simultaneous removal of acetone and NO in a low-temperature photothermal co-catalytic system with acetone replacing NH 3 . The characterization results show that heat is the main driving force of the reaction system, and the abundance of Co and Mn atoms in high valence states, surface-adsorbed oxygen, and oxygen lattice defects in the catalyst are the most important factors affecting the performance of the catalyst. The performance test results showed that the optimal pyrolysis temperature of sludge was 400 °C, the optimal dosing ratio of Co and Mn was 4:1, and the catalyst achieved 42.98% and 52.41% conversion of acetone and NO, respectively, at 240 °C with UV irradiation. Compared with the pure SBC without catalytic effect, the SBC loaded with Co and Mn gained the ability of simultaneous removal of acetone and NO through the combined effect of multiple factors. The key reaction steps for the catalytic conversion of acetone and NO on the catalyst surface were investigated according to the Mars-van Krevelen (MvK) mechanism, and a possible mechanism was proposed. This study provides a new strategy for the resource utilization of sewage sludge and the preparation of photothermal catalysts for the simultaneous removal of acetone and NO at low cost.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Jinrui Dong,Pin Li,Xiaoyuan Ji,Yong Kang,Xue Yuan,Jingchun Tang,Boxiong Shen,Huajiang Dong,Honghong Lyu
Photocatalytic oxidation technology holds promise for ideal advanced treatment of antibiotic wastewater. Single-atom catalysts (SACs) are a new hotspot in catalytic science, but the photochemical studies on the removal of antibiotics from water and biocompatibility after entering the environment are scarce. In this work, we prepared a single Mn atom immobilized on N-doped biochar (Mn@N-Biochar) by impregnation calcination method for enhancing photocatalytic degradation of sulfanilamide (SNM) in different types of various water systems. Compared with the original biochar, Mn@N-Biochar showed enhanced SNM degradation and TOC removal capacity. DFT calculation concluded that the electrons of d‐orbital (Mn) and p-orbital (N) altered the electronic structure of biochar and enhanced the photoelectric performance. It was shown that Mn@N-Biochar caused negligible systemic inflammation and tissue damage when given orally in mice, and also did not alter cell death and ROS production in human lung, kidney, and liver cells, as compared with biochar. We are convinced that Mn@N-Biochar could enhance the photocatalytic degradation of antibiotics while maintaining biocompatibility, which could be a promising strategy for wastewater treatment .
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高影响因子
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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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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高影响因子
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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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Wenhui Fang,Tingting Tang,Min Li,Shixian Xin,Ying Wu,Yutao Cao,Zhize Yu,Wei Cui,Zengxi Li,Hong Zhao
Designing catalysts at atomic level fine-tune the electronic structure of surface-active site for efficient water splitting, is a highly desirable approach but also poses significant challenges. This study focuses on the synthesis of a series of electronically tunable metal single-atom (M−SAs) catalysts: M 9 @S-Ni(OH) 2 (M=Pt, Mn, Fe or Cu). Experimental results reveal that introduction of trace S-heteroatoms and metal atoms into Ni(OH) 2 lattice can effectively modulate the electronic structure of M 9 @S-Ni(OH) 2 through modulation of p-d and d-d orbital hybridization, resulting in exceptional performance in water electrolysis. Among M 9 @S-Ni(OH) 2 , Pt 9 @S-Ni(OH) 2 and Fe 9 @S-Ni(OH) 2 exhibit excellent hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) performance, respectively, the overpotential requiring only 7 mV and 269 mV, respectively, at current density of 10 mA cm −2 . (−) Pt 9 @S-Ni(OH) 2 ||Fe 9 @S-Ni(OH) 2 (+) presents a high current density of 531.07 mA cm −2 at cell-voltage of 1.80 V in overall-water splitting (OWS), which is 14.07 times higher than that of the commercial (−) Pt/C||IrO 2 (+) (37.86 mA cm −2 ) system. This work achieves the development of cost-effective and stable electrocatalysts, offering a solution for large-scale and sustainable water-hydrogen conversion.
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危险品化学品经营许可证（带存储）