CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Mingjie Huang,Sisi Peng,Wei Xiang,Chen Wang,Xiaohui Wu,Juan Mao,Tao Zhou
This study has revealed how the strong metal-support interaction (SMSI) between carbon nanotubes (CNTs) and Mn 0.65 Fe 2.35 O 4 (MnFeO) in boosting peroxymonosulfate (PMS) activation for rapid sulfamethoxazole (SMX) degradation. As synergized by CNTs, the PMS-activation efficiency of MnFeO could be enhanced by>24 times, but with the similar PMS-activation mechanism. It was explored that the SMSI-induced abundant surface hydroxyl groups, in cooperation with the highly hydrophobic CNTs, favored the rapid in situ interfacial degradation of SMX. This feature also endowed the MnFeO-CNTs catalyst resistance to high salinity waters containing inorganic anions (e.g., Cl - and NO 3 – ) of weak complexing abilities. Moreover, the SMSI allowed the greatly accelerated redox cycle rate of Mn species by electron-rich CNTs, resulting in efficient PMS activation. Furthermore, the application feasibility of the MnFeO-CNTs/PMS system was demonstrated for a SMX-spiked real reverse osmosis (RO) concentrate. It was found that higher concentration of PMS could realize the complete removal of SMX, despite the existence of electron-rich tyrosine-like substances would compete with the SMX degradation in the MnFeO-CNTs/PMS system. This study demonstrated that the SMSI could boost the PMS activation , and could serve as an effective material strategy for in situ interfacial organics degradation in the high salinity wastewater.
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ADVANCED POWDER TECHNOLOGY
·
2019
·
IF 3.25
Lihua Gao,Zhenggen Liu,Yuzhu Pan,Cong Feng,Yang Ge,Mansheng Chu
Carbothermal reduction followed by magnetic separation has been recognized as an effective recovery strategy to achieve separation of Mn and Fe from ferruginous manganese ores (Fe-Mn ores). However, it is difficult to improve the recovery of manganese more than 85% by changing carbothermic roasting reduction and magnetic separation. This work clarified the underlying reason for the poor separation with the magnetic separation process and proposed a promising process for the recovery of Fe and Mn from Fe-Mn ore. The effect of operating variables on recovery and separation of Mn and Fe from Fe-Mn ore is initially investigated during the carbothermic reduction roasting process followed by magnetic separation to reveal the underlying reason for the poor separation from Fe-Mn ores. Then, the stepwise reduction behaviors of the MnO-Fe 2 O 3 and MnO-Fe 2 O 3 -Al 2 O 3 systems were investigated to clarify that the formation of composite oxide Mn 1−x Fe x O (0 < x < 0.497) and hercynite (FeO·Al 2 O 3 ) directly caused the poor separation of Fe and Mn from high-alumina Fe-Mn ores. Then, the stepwise reduction roasting behaviors of Mn 1−x Fe x O and FeO·Al 2 O 3 were investigated by XRD, SEM-EDS and XPS analysis. After adjusting the experimental parameters, iron-rich products with a Fe recovery of 94.31% and a grade of 85.21% and manganese-rich product with a Mn recovery of 90.05% and a grade of 54.35% are obtained. The mass ratio of Mn/Fe increased to 8.5 in the manganese-rich product.
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Analytical Methods
·
2019
·Vol. 11
·期 8
·1111-1124
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IF 2.378
Xiaoheng Qi,Huiming Tian,Xueming Dang,Yaofang Fan,Yaobin Zhang,Huimin Zhao
Metal–organic frameworks (MOFs) with a metal coordination structure mimicking that of enzymes have been widely applied in the sensing field for bioassays, and most of the reports focus on single-metal MOFs. However, bimetallic MOFs have fascinating catalytic capabilities due to their bimetallic coordination. Herein, a two-dimensional sheet-like bimetallic Co/Mn-based MOF (Co/Mn-MOF) with peroxidase-like activity was synthesized through a one-step hydrothermal method to accelerate the decomposition of H2O2 with the generation of ˙OH, which further oxidized the classic chromogenic substrate 3,3′,5,5′-tetramethylbenzidine (TMB) into oxTMB. The Michaelis–Menten constants (Km) and maximum initial velocities (Vmax) of the catalyst were found to be 0.27 mM and 1.64 × 10−7 M s−1 for TMB and 0.24 mM and 5.80 × 10−7 M s−1 for H2O2, respectively. Accordingly, we successfully utilized Co/Mn-MOF-1-1-150 to establish a colorimetric detection platform for the detection of H2O2. A linear absorbance response ranging from 1 to 100 μM with the limit of detection of 0.85 μM (S/N = 3) was obtained under the optimized conditions. The LOD of our catalyst is comparable to that of other MOF-based enzyme mimics for colorimetric detection; this can be ascribed to the synergistic catalytic effect between its two metals, its two-dimensional structure with a small diffusion barrier for the substrate molecules, and large exposed surface area. More importantly, using the proposed sensing method, the determination of H2O2 released by living cells and in spiked water samples was achieved. This revealed that the as-prepared bimetallic Co/Mn-MOF could be a promising candidate as a catalytic material due to its peroxidase activity.
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JOURNAL OF POWER SOURCES
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2019
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IF 7.467
Qin Wang,Yejian Xue,Shanshan Sun,Shanshan Yan,He Miao,Zhaoping Liu
Facile synthesis of high efficient bi-functional oxygen catalysts is important for large-scale application of rechargeable metal-air batteries . Herein, an ethanol-water mediated co-precipitation approach is applied to fabricate Co–Mn–Ni (CMN) ternary spinel oxides with uniform 1D structure. Their catalytic activities toward the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are investigated by the rotating ring-disk electrode (RRDE) techniques. The ternary spinel oxide with the Co/Mn/Ni atomic ratio of 2:3:1 (CMN-231) exhibits the best bi-functional activities among the as-prepared ternary, binary and unitary spinel oxides (△E is as low as 0.88 V), which can be attributed to its reasonable element composition , mesoporous nanorod structure, strong oxygen-adsorption ability and good charger-transfer capability. In addition, the CMN-231 catalyst demonstrates a strong stability during long-term operation. This well-designed catalyst is applied in a homemade zinc-air battery, and exhibits good charge–discharge performances (voltage gap is 0.9 V at 50 mA cm −2 ) and remarkable cycling stability.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2018
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IF 3.779
Dmitrii Rakov,Yuzhi Li,Siqi Niu,Ping Xu
Recently reported transition metal phosphosulfide (MPS 3 or MPS) nanosheets (NSs) demonstrated outstanding activity towards hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), and proper doping of a second transition metal might even enhance the catalytic activity. By considering the oxophilicity of the doping element, here we demonstrate the Mn (with higher oxophilicity) and Ni (with lower oxophilicity) doping of Ni 1- x Mn x PS 3 and Mn 1- x Ni x PS 3 NSs on their HER and OER activity in alkaline solution. It is found that non-substituted NiPS 3 NSs show better catalytic activity than their Mn-doped samples. On the contrary, Ni doping into MnPS 3 NSs significantly improves the electrocatalytic performance. This work may substantially expand the understanding of the role of elemental oxophilicity on the electrochemical water splitting activities of Ni/Mn based catalysts.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2013
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IF 2.145
Wei-guo Pan,Jie-nan Hong,Rui-tang Guo,Wen-long Zhen,Hong-lei Ding,Qiang Jin,Cheng-gang Ding,Shi-yi Guo
MnO x –CuO x /TiO 2 and MnO x –CuO x /Al 2 O 3 catalysts were prepared by sol–gel method and used for low temperature selective catalytic reduction of NO with NH 3 . The results showed that MnO x –CuO x /TiO 2 had better catalytic activity and SO 2 resistance than MnO x –CuO x /Al 2 O 3 in the temperature range of 100–250 °C. The properties of the catalysts were characterized by using XRD, N 2 adsorption, temperature programmed reduction (H 2 -TPR) and temperature programmed desorption (NH 3 -TPD). It was found that the support has a great impact on the acidity of catalyst; TiO 2 and Al 2 O 3 can promote the formation of Lewis acid sites and Brönsted acid sites respectively.
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SENSORS AND ACTUATORS B-CHEMICAL
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2017
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IF 5.401
Zhi-Qiang Zhou,Ren Yan,Jie Zhao,Li-Yun Yang,Ji-Lei Chen,Yan-Jun Hu,Feng-Lei Jiang,Yi Liu
The pollution of Hg 2+ is one of the most serious problems to human health due to their high toxicity, mobility, difficulty in degradation and ability of accumulation in ecological systems. Thus, it is of great importance to develop highly selective and sensitive probe for detecting Hg 2+ in aquatic ecosystems. Here we propose a new turn-on strategy for specific recognition and detection of Hg 2+ . Mn-doped ZnSe quantum dots (QDs) with small size (2.1 nm) were prepared and adopted as probe, the small size of doped QDs makes the replacement of Mn 2+ by Hg 2+ accessible, which eliminates the fluorescence quenching effect of superficial Mn 2+ on Mn-doped ZnSe QDs. Different from traditional semiconductor nanocrystals based turn-off probe for detecting Hg 2+ , we realize a turn-on strategy for the selective detection of Hg 2+ by Hg 2+ -Mn 2+ replacement using semiconductor nanocrystals (Mn-doped ZnSe QDs). This turn-on mechanism was verified by fluorescence spectra, ICP-AES and XPS. In the absence of Hg 2+ , Mn-doped ZnSe QDs possessed low fluorescence intensity. With the addition of Hg 2+ , the fluorescence intensity around 600 nm increased dramatically. Our Mn-doped ZnSe QDs exhibits excellent selectivity and sensitivity for Hg 2+ . The limit of detection is 7.0 nM, which is lower than the mercury toxic level defined by the U.S. Environmental Protection Agency (10 nM). The result of Hg 2+ detection in real samples indicates the feasibility and sensitivity of our probe for application in environmental samples.
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FOOD CHEMISTRY
·
2017
·
IF 4.529
Wengang Zhang,Yong Han,Xiumei Chen,Xueli Luo,Jianlong Wang,Tianli Yue,Zhonghong Li
A Mn-doped ZnS quantum dots (QDs) based nanosensor for selective phosphorescent determination of patulin (PAT) was synthesized with 6-hydroxynicotinic acid (6-HNA) as dummy template via a surface molecular imprinting sol–gel process. FTIR and XRD indicated the successful graft of molecularly imprinted polymer (MIP) onto crystal QDs. Binding tests revealed that the MIP-QDs presented higher selectivity, adsorption capacity and mass transfer rate than non-imprinted polymers, demonstrating a specific recognition for PAT among competitive mycotoxins and its analogues with the imprinting factor of 2.02. The MIP-QDs could recognize PAT in a linear range of 0.43–6.50 μmol L −1 with a detection limit of 0.32 μmol L −1 and a correlation coefficient (R 2 ) of 0.9945. Recoveries of 102.9–127.2% with relative standard deviations <4.95% were achieved in apple juice samples which were in good agreement with high-performance liquid chromatography (HPLC) (P > 0.05). The results indicated a simple phosphorescent nanosensor for PAT detection in complex matrix.
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PubMed
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JOURNAL OF MOLECULAR STRUCTURE
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2024
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IF 4
Yue Yin,Yanming Xu,Ya-Nan Luan,Zhuo Zhao,Yihua Xiao,Changqing Liu
A novel porous Fe-Mn chitosan bead (PFMB) was fabricated through the freeze-drying technique for the enhanced oxidation and adsorption of arsenite (As(Ⅲ)) from aqueous solution. The porous internal structure of PFMB provided a significantly higher As(Ⅲ) oxidation and adsorption rate than solid Fe-Mn chitosan bead (FMB). The experimental results showed that FMB and PFMB exhibited the theoretical maximum As(Ⅲ) adsorption capacities of 27.42 and 49.80 mg/g, respectively. The real-time oxidation and adsorption progress of As(Ⅲ) onto PFMB was deeply evaluated: PFMB effectively oxidized As(Ⅲ) to As(Ⅴ) and the generated As(Ⅴ) was subsequently adsorbed. The operational parameters (initial pH, adsorbent dosage, ionic strength, and HA concentration) were thoroughly investigated and had no significant influence on As(Ⅲ) removal by PFMB. Finally, the regeneration experiment showed that PFMB can be easily regenerated and the recycled PFMB can successfully remove As(Ⅲ) in the following 5 cycles. Column experiments suggested that the column device could effectively remove the As(Ⅲ) in more than 3830 bed volume with the influent velocity at 0.5 mL/min before effluent concentration reached 0.05 mg/L. These results revealed the enhanced oxidation and adsorption performance of As(Ⅲ) onto PFMB and provided a reference for the future application of PFMB in arsenic-contaminated water treatment.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Zhigen Li,Mengfan Zhou,Shuqin Wang,Baowei Hu
Uranium (U(VI)) removal from nuclear-contaminated water is still an obstacle that needs to be solved quickly. Herein, looking for efficient, fast, and highly selective separation of U(VI) versatile material is of great significance. In this study, a novel Ce/Mn bimetallic modified aminated MOF material UiO-66-NH 2 was synthesized through solvothermal reaction by using ZrOCl 2 ·8H 2 O as a sacrificial template, which was employed as an adsorbent in radioactive remediation. The characterization of the adsorbent Ce/Mn-UiO-66-NH 2 was investigated by XRD, FTIR, SEM, and BET and the results indicated that Zr in UiO-66-NH 2 had been partially replaced by Ce/Mn successfully. Through batch adsorption experiments, we found that the maximal capture capacity of the produced adsorbent for U(VI) was 1218.78 mg/g at 313 K, and the elimination process fitted well with pseudo-second-order kinetic model and the Langmuir isotherm model. The thermodynamic parameters indicate that the adsorption process of U(VI) was endothermic and spontaneous which was regulated by chemisorption. After 5 times recycling, the removal rate still exceeded 83.5 %, indicating that Ce/Mn-UiO-66-NH 2 was a promising adsorbent that can effectively remove U(VI) in radioactive wastewater. The increased adsorption capacity was proposed attributed to complexation and electrostatic attraction between the radionuclides and the introducing functional groups as well as Ce or Mn ions. This study provides a reference value for radioactive wastewater remediation.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2024
·Vol. 39
·期 1
·e7959
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IF 3.7
Zhuoqin Li,Minghui Ma,Zhiyin Xiao,Xiujuan Jiang,Xinlei Xu,Hailong Wang,Peter C. Ford,Xiaoming Liu
Five novel manganese (I) tricarbonyl complexes were synthesized by the reaction of Mn (CO) 5 Br with quinoline-2-carboxaldehyde and different anilines. The IR, UV, and myoglobin results indicate that these complexes can be used as photoCORMs (photo photoinduced carbon monoxide releasing molecules) activated by red light. The visible range spectra display strong charge transfer (CT) bands, the maxima of which are sensitive to the ligand substituents. Density functional theory (DFT) and time-dependent density functional theory (TDDFT) computations show that these CT transitions are admixtures of metal-to-ligand and aniline-to-quinoline charge transfers and that increasing the electron-donating ability on the aniline functionality can lead to shifts in the absorption bands of the corresponding compounds to longer wavelengths and to enhanced band intensities, thus enhancing their photoactivity. Photolysis of these complexes in aerobic solution leads to CO photodissociation followed by oxidation of the Mn(I) center to Mn(II).
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
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IF 9.4
Ruipeng Yuan,Jinyu Zhao,Xu Chen,Xiaoming Qiu,Xiaomin Wang
Cobalt-nitrogen-carbon (CoN x C) materials are regarded as promising low-cost electrocatalysts for the oxygen reduction reaction (ORR). However, their susceptibility to deactivation and poor stability in acidic media limits their practical applications. In this study, we develop cobalt (Co) and manganese (Mn) embedded in nitrogen-doped carbon (CoMnN x C) dual-site catalysts by incorporating Mn into CoN x C and leverage a synergistic dual-catalysis strategy to optimize both activity and stability. The dynamic evolution of *OOH intermediate on the catalyst surface is monitored via in situ Raman spectroscopy, confirming that Mn introduction modulates the reaction pathway. Due to electron transfer from Mn to the Co-N x center in CoMnN x C, *OOH activation on the surface is enhanced, and the two-electron ORR process is inhibited. Consequently, the CoMnN x C catalyst exhibits excellent ORR activity (E 1/2 = 0.76 V vs. reversible hydrogen electrode) and a very low hydrogen peroxide (H 2 O 2 ) yield (<2.9 %) in acidic electrolyte. Additionally, the dynamic evolution of *OH on the Mn-N x site confirms that Mn-N x can serve as a potential catalytic site for the hydrogen peroxide reduction reaction (HPRR), facilitating H 2 O 2 decomposition. Differential electrochemical mass spectrometry (DEMS) demonstrates that this parallel catalytic pathway effectively weaks the oxidative corrosion of H 2 O 2 on the carbon carrier. The results indicate that the negative half-wave potential shift of CoMnN x C catalysts in acidic electrolyte after 10,000 accelerated durability tests (ADT) is only 11 mV. The synergistic dual-catalytic strategy proposed in this work offers a novel approach for designing high-efficiency and stable transition metal-nitrogen-carbon catalysts.
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