CATALYSIS TODAY
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2022
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IF 6.562
Shuqi Zhao,Kunli Song,Ruiyu Jiang,Dandan Ma,Hongming Long,Jian-Wen Shi
Nitrogen oxides (NO x ) are typical atmospheric pollutants that harm the environment and human body, and selective catalytic reduction (SCR) with NH 3 is one of the most effective technologies to deal with NO x emissions at present. In this work, a monolithic catalyst, Sm-modified Mn-Ce composite oxides (Sm-MnCe) supported on cordierite (CC), is prepared by impregnation for the first time, and their denitration (de-NO x ) performance in NH 3 -SCR reaction is evaluated in detail. The results show that 0.1Sm-MnCe/CC (Sm/Mn mole ratio is 0.1) has the best de-NO x efficiency with above 80 % NO x conversion from 60° to 270°C, and the high NO x conversion can be maintained within 15 h in the presence of 100 ppm SO 2 . It is found that appropriate introduction of Sm increases the specific surface area and acid sites, improves the redox environment, elevates the content of Mn 4+ on the catalyst surface, which are conducive to the improvement of catalytic activity. In addition, the interaction between active components (Sm, Mn and Ce) also plays a positive role for the excellent de-NO x activity. It is revealed by in-situ diffuse reflectance infrared Fourier transform spectra (DRIFTS) that the NH 3 -SCR reaction over the 0.1Sm-MnCe/CC catalyst follows Eley-Rideal (E-R) and Langmuir-Hinshel (L-H) mechanisms. This work provides ideas for the preparation and modification of monolithic catalysts, which is conducive to promoting the practical industrial application of low-temperature SCR de-NO x technology.
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International Journal of Nanomedicine
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2023
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IF 8
Shaohui Zheng,Min Zhang,Hongyan Bai,Meijuan He,Lina Dong,Lulu Cai,Mingming Zhao,Qi Wang,Kai Xu,Jingjing Li
Background Early diagnosis of renal cell carcinoma is extremely significant for the effective treatment of kidney cancer. The development of AS1411 aptamer modified Mn-MoS2 QDs provides a promising fluorescence/magnetic resonance (MR) dual-modal imaging probe for the precise diagnosis of renal clear cell carcinoma.Methods In this work, Mn-MoS2 QDs were synthesized through a simple “bottom-up” one-step hydrothermal method. AS1411 aptamer was modified on the Mn-MoS2 QDs to improve the specificity to renal cell carcinoma. The characteristics of Mn-MoS2 QDs were confirmed by transmission electronic microscopy (TEM), atomic force microscope (AFM), X-ray photoelectron spectrometer (XPS), photoluminescence (PL) emission spectra, etc. Cellular fluorescence labelling was investigated using the Mn-MoS2 QDs and AS1411-Mn-MoS2 QDs. The T1-weighted MR imaging was assessed by the in vitro MR cell imaging and in vivo MR imaging. Finally, the long-term toxicity of Mn-MoS2 QDs was investigated by the hematology and histological analysis.Results The prepared Mn-MoS2 QDs exhibited excellent aqueous property, intense fluorescence, low toxicity, high quantum yield of 41.45% and high T1 relaxivity of 16.95 mM−1s−1. After conjugated with AS1411 aptamer, the AS1411-Mn-MoS2 QDs could specifically fluorescently label the renal carcinoma cells and present a specific MRI signal enhancement in the tumor region of mice bearing renal carcinoma tumors. Furthermore, Mn-MoS2 QDs revealed low toxicity to the mice via hematology and histological analysis.Conclusion These results demonstrated the potential of AS1411-Mn-MoS2 QD as a novel nanoprobe for targeted MR imaging and fluorescence labelling of renal cell carcinoma.
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Journal of Energy Chemistry
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2022
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IF 13.599
Xiaoling Cui,Jinlong Sun,Dongni Zhao,Jingjing Zhang,Jie Wang,Hong Dong,Peng Wang,Junwei Zhang,Shumin Wu,Linhu Song,Ningshuang Zhang,Chunlei Li,Shiyou Li
By optimizing electrolyte formulation to inhibit the deposition of transition metal ions (TMIs) on the surface of the graphite anode is an effective way to improve the electrochemical performance of lithium-ion batteries. At present, it is generally believed the formation of an effective interfacial film on the surface of the anode electrode is the leading factor in reducing the dissolution of TMIs and prevent TMIs from being embedded in the electrode. It ignores the influence of the solvation structures in the electrolyte system with different composition, and is not conducive to the design of the electrolyte formulation from the perspective of changing the concentration and the preferred solvent to inhibit the degradation of battery performance caused by TMIs deposition. In this work, by analyzing the special solvation structures of the high-concentration electrolyte, we study the main reason why high-concentration electrolyte inhibits the destructive effect of Mn (II) on the electrochemical performance of LIBs. By combining the potential-resolved in-situ electrochemical impedance spectroscopy technology (PRIs-EIS) and density functional theory (DFT) calculation, we find that Mn (II) mainly exists in the form of contact ions pairs (CIPs) and aggregates (AGGs) in high-concentration electrolyte. These solvation structures can reduce the destructive effect of Mn (II) on battery performance from two aspects: on the one hand, it can rise the lowest unoccupied orbital (LUMO) value of the solvation structures of Mn (II), thereby reducing the chance of its reduction; on the other hand, the decrease of Mn 2+ ions reduction can reduce the deposition of metallic manganese in the solid electrolyte interphase (SEI), thereby avoiding the continuous growth of the SEI. This study can be provided inspiration for the design of electrolytes to inhibit the destructive effect of TMIs on LIBs.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
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IF 11.357
Tingting Pan,Hua Deng,Yuqin Lu,Jinzhu Ma,Lian Wang,Changbin Zhang,Hong He
The miscellaneous volatile organic compounds (VOCs) in industrial flue gas streams usually demonstrate significant mutual inhibition effects, and the behavior of a particular VOC in mixtures is not clear, which hinders the application of catalytic technology. This study examines the catalytic oxidation and mixing effects of representative VOCs in industrial exhausts, consisting of acetone (AC), ethyl acetate (EA), and toluene (Tol), on common Mn-based catalysts (e.g., MnO2, Mn2O3, LaMnO3, and Mn3O4) by means of intrinsic activity evaluation, coadsorption, VOC temperature-programmed oxidation, in situ diffuse reflectance infrared Fourier transform spectroscopy, and gas chromatography–mass spectrometry. The results showed no inhibiting effect on the conversion of these VOCs when combusted together; instead, a significant mutual promotion effect was found, especially on Tol destruction, with a sharp decrease in the Tol T50 from 214 to 158 °C on MnO2. It is proposed for the first time that the addition of AC/EA in Tol combustion leads to the generation of o/m-methyl phenol, which changes the rate-determining step of the ring-opening process, thus elevating the conversion of Tol together with AC and EA in the mixture at low temperatures.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Yibin Yang,Di Gao,Yingqing Ou,Yang Yang,Peng Xiao,Yunhuai Zhang
Currently, developing highly active and low-cost electrocatalytic materials for oxygen evolution reaction (OER) is an enormously grand challenge. Herein, we developed a novel and highly active Mn doped Co 2 Fe layer double hydroxide (LDH) electrocatalyst for OER. We discovered that these electrocatalytic materials can be directly grown on carbon papers to construct high-specific-surface-area electrode, which shows the lowest overpotential of 266 mV at 10 mA cm −2 . Furthermore, after introducing Mn element, DFT + U calculation found that the ∗OOH of Fe-site on Co 2 Fe 0.67 Mn 0.33 LDH could draw more electrons than Co 2 Fe LDH due to the electronegativity differences between Fe-site on Co 2 Fe 0.67 Mn 0.33 LDH and Fe-site on Co 2 Fe LDH, which is reason that the energy level of Fe 3d (e g ) was obviously downshifted by d-d repulsion of Mn 3d and Fe 3d in the neighboring sites of Co 2 Fe 0.67 Mn 0.33 LDH after doped Mn element, which leads to reduce charge-transfer energy from O 2p to Fe 3d (e g ) to promote oxygen evolution processes for OER. Meanwhile, the band gap is also decreased after doped Mn element in Co 2 Fe LDH due to the downshifted e g orbital energy of Fe 3d. This study gives a general avenue to design and developing efficiently active LDH electrocatalysts for OER in the future.
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Nano Research
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2023
·Vol. 16
·期 8
·10748-10755
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IF 9.9
Li Junhua,Jiang Yi,Zhang Xu,Huo Yidan,Du Fanglin,Tuo Yongxiao,Guo Zhiyan,Chen Dawei,Chen Shenghua
The electrooxidation of the alcohol and aldehyde molecules instead of water coupled with H 2 production has been proven to be effective for producing high-value fine chemicals under alkaline conditions. It is also noteworthy that under acidic conditions, the stability of non-noble metal water oxidation catalysts remains a great challenge due to the lattice oxygen mechanism. Hence, we coupled the biomass-derived glucose oxidation for high-value D-glucaric acid (GRA) with ultra-durable hydrogen in acid solution over a Yb-MnO 2 catalyst. The Mn 3+ regulated by Yb atoms doped in MnO 2 can effectively optimize the adsorption and desorption processes of the alcohol and aldehyde group and improve the intrinsic activity but cannot for H 2 O. The catalyst exhibited extremely high activity and stability after 50 h for glucose oxidation, inhibiting the lattice oxygen process and MnO 4− formation, while the activity was quickly lost within 0.5 h for water oxidation. Density functional theory (DFT) calculations further demonstrated that glucose oxidation reaction proceeds preferentially due to the oxidation of aldehyde group with lower adsorption-free energy (−0.4 eV) than water (Δ G > 0 eV), avoiding the lattice oxygen mechanism. This work suggests that biomass-derived glucose oxidation not only provides a cost-effective approach for high-value chemicals, but also shows an extremely potential as an alternative to acidic oxygen evolution reaction (OER) for ultradurable H 2 production.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2023
·Vol. 30
·期 44
·99830-99841
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IF 5.8
Chen Yanzhu,Zeng Zheng,Liu Dongyang,Zhang Jing,Guo Yang,Zou Jianwu,Guan Juan,Xu Xiang,Li Liqing
Abstract The controllable preparation of efficient non-crystalline solid solution catalysts is a great challenge in the catalytic oxidation of volatile organic compounds. In this work, series non-crystalline solid solution structured Ce-Mn co-oxide nanofibers were creatively prepared by adjusting Ce/Mn molar ratios using electrospinning. 0.20CeMnO x (the ratio of Ce to Mn was 0.2) displayed an outstanding low-temperature toluene oxidation activity ( T 90 = 233 °C). The formation of the amorphous solid solution and the unique nanofiber structure both contributed to a large specific surface area ( S = 173 m 2 g -1 ) and high adsorbed oxygen content (O ads /O = 41.3%), which enhanced the number of active oxygen vacancies. The synergies between non-crystalline structure and active oxygen species markedly improved oxygen migration rate as well as redox ability of the catalysts. Additionally, in situ diffuse reflectance infrared Fourier transform spectra showed that the absorbed toluene could be completely oxidized to CO 2 and H 2 O with benzyl alcohol, benzaldehyde, benzoic acid, and maleic anhydride as intermediates. In summary, this study provided an alternative route for the synthesis of non-crystalline metal co-oxide nanofibers. Graphical abstract
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Jingyu Ren,Zhouzhou Yao,Qian Wei,Ruotong Wang,Yuan Liu,Long Wang,Kaibin Zheng,Shuai Wang,He Guo,Zhirui Niu,Jian Wang,Jin Han,Lei Lü,Yanzhong Zhen,Jie Li
Organic pollutants of olive mill wastewater (OMW) have caused various negative effect to water environments. It is imperative to develop an effective technology for eliminating organic pollutants in OMW. In this study, representative organic pollutants in OWM, ferulic acid (FA) and caffeic acid (CA), were removed from water by dielectric barrier discharge (DBD) plasma and Mn/CoOOH/activated carbon fiber (ACF) catalyst. The treatment performance and catalytic mechanisms were studied. The results show that the combined system could effectively remove FA and CA. For example, FA and CA degradation efficiency was 81.6% and 94.2% in the 20 L of mixed wastewater with the 100 min treatment using DBD combined with Mn/CoOOH/ACF. Experiments and density functional theory (DFT) calculations indicate that the electron transfer from the catalyst to antibonding orbits of O 3 and H 2 O 2 caused the dissociated adsorption, promoting the transformation of O 3 and H 2 O 2 to ·O, singlet oxygen and ·OH. Additionally, the doping of Mn in CoOOH benefited the electron transfer because Mn had a higher d-band center than Co in Mn/CoOOH, which was conducive to the interaction of O 3 and H 2 O 2 with the catalyst. The possible degradation pathways of FA and CA were proposed.
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Journal of Cleaner Production
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2022
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IF 11.072
Mingjun Xu,Qian Zhang,Ziqi Zhu,Yuwei Xue,Ting Zhang,Junming Hong
Prussian blue analogs (PBAs) have been widely explored as catalyst for peroxymonosulfate (PMS) activation. However, the drawbacks of poor electron transfer ability and degradation performance of PBAs hinder their practical application. In this study, oxygen vacancy (OV)-rich Mn-Fe PBA was regulated through phosphoric acid and ammonia water chemical etching to overcome these drawbacks. Experimental and theoretical investigations indicated that the regulation of OVs was favorable for more Fe 2+ and Mn 3+ active sites exposure and higher specific surface area to facilitate PMS activation. Sulfate radical (SO 4 •− ), hydroxyl radical (HO•), and single oxygen ( 1 O 2 ) were verified as main reactive species for PMS activation during catalytic reaction . Density functional theory calculation results showed that the OV-rich NOE-PC-300 had the highest pollutants degradation capability, with complete degradation of bisphenol A (BPA) and acetaminophen (APAP) within 40 min. Through regulation of OVs by chemical etching, highlighted adsorption ability and elongated O–O bond of PMS were obtained. This research showed that NOE-PC-300 is an efficient and harmless catalyst for activating PMS, and it has immense application potential in practical wastewater treatment .
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Wenqing Du,Yongqian Zheng,Xueyi Liu,Jie Cheng,R. Chenna Krishna Reddy,Akif Zeb,Xiaoming Lin,Yifan Luo
Transition metal oxide anode materials have recently been losing their importance as advanced functional and smart materials due to early capacity decay and sluggish kinetics. In order to address this issue, vacancy engineering approach can be adapted, which can effectively manipulate the electronic structure of transition metal oxide (TMO)-based electrode materials. Herein, a series of MOF-derived oxygen-rich vacancy MFe 2 O 4 /C (M = Ni, Mn, Co) materials are synthesized on a large scale via solvothermal and subsequent calcination treatment for energy storage applications in lithium-ion batteries. All the synthesized O V -NFO (NiFe 2 O 4 ), O V -MFO (MnFe 2 O 4 ) and O V -CFO (CoFe 2 O 4 ) electrodes achieve excellent electrochemical performance, superior multiplier performance and incredible lithium-ion diffusion rate, which was found to be superior than their counterpart electrodes. The oxygen vacancy (O V ) enrichment contribution to higher conductivity was realized by experimental and density functional theory (DFT) calculations results, where it has been established that O V provides additional active sites, accelerates Li + diffusion and improves pseudocapacitive contribution. This vacancy-engineering strategy for modulating electronic structure and reaction kinetics enabled new ideas for the design and execution of other advanced transition metal-based electrode materials.
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Materials Today Physics
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2022
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IF 11.021
Dangli Gao,Qingqing Kuang,Feng Gao,Hong Xin,Sining Yun,Yuhua Wang
Optical characteristics of phosphors, e.g. color output, decay process and external field stimulation mode (including opto-, thermo- and mechano-stimulation), play an important role in the areas of information storage, anti-counterfeiting and bio-imaging applications. Persistent luminescence (PersL) phosphors are particularly suitable for such applications owing to their multimodal luminescence features such as photoluminescence (PL), PersL, photostimulated luminescence and mechanoluminescence. However, conventional PersL phosphors are suffering from a huge challenge to develop a single material for multicolor anti-counterfeiting. Herein, the Zn 1+ x Ga 2−2 x Ge x O 4 :Mn (0 ≤ x ≤ 1) solid solution phosphors are synthesized, which can emit from green to yellow, golden, pink, and red PL. In addition, the phosphors also show the thermo-mechano-opto-stimulated green PersL after irradiation of a UV 254/365 nm lamp. Based on the multimode and multicolor luminescence features, the advanced anti-counterfeiting and optical data storage are designed. Results show that the multimodal luminescence feature with high information capacity can be conveniently identified by using a luggable ultraviolet lamp or NIR laser diode. This extraordinary material will make anti-counterfeiting more sophisticated and show advanced security in the applications of data encryption.
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Nanomaterials
·
2022
·Vol. 12
·期 12
·2029
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IF 5.719
Dangli Gao,Peng Wang,Feng Gao,William Nguyen,Wei Chen
The ability to manipulate the luminescent color, intensity and long lifetime of nanophosphors is important for anti-counterfeiting applications. Unfortunately, persistent luminescence materials with multimode luminescent features have rarely been reported, even though they are expected to be highly desirable in sophisticated anti-counterfeiting. Here, the luminescence properties of Zn3Ga2GeO8:Mn phosphors were tuned by using different preparation approaches, including a hydrothermal method and solid-state reaction approach combining with non-equivalent ion doping strategy. As a result, Mn-activated Zn3Ga2GeO8phosphors synthesized by a hydrothermal method demonstrate an enhanced red photoluminescence at 701 nm and a strong green luminescence with persistent luminescence and photostimulated luminescence at 540 nm. While Mn-activated Zn3Ga2GeO8phosphors synthesized by solid-state reactions combined with a hetero-valent doping approach only exhibit an enhanced single-band red emission. Keeping the synthetic method unchanged, the substitution of hetero-valent dopant ion Li+into different sites is valid for spectral fine-tuning. A spectral tuning mechanism is also proposed. Mn-activated Zn3Ga2GeO8phosphors synthesized by a hydrothermal approach with multimodal luminescence is especially suitable for multiple anti-counterfeiting, multicolor display and other potential applications.Keywords:Zn3Ga2GeO8:Mn phosphors;multicolor emission;hydrothermal approach;afterglow;anti-counterfeiting application
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