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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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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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Guifang Wang,Guangchuan Liang,Huizhen Xiao,Jun Qiu,Haiyan Liu,Shaojian Ma,Sridhar Komarneni
The conventional environmental remediation materials, which are applied for the long-term treatment of mine tailings are easy to fail when affected by acid rain. Therefore, dynamic column simulation experiments were conducted to compare the immobilization persistence of As, Mn, Pb and Zn by the addition of triethylenetetramine modified montmorillonite (TTA-Mt) and calcium-based montmorillonite (Ca-Mt) in sulfide tailings during a simulated 5-year study of acid rain leaching. The structural and morphological characteristics of TTA-Mt were analyzed with FTIR, XRD, SEM, TEM and EDS. Results showed that the additions of TTA-Mt could persistently immobilize the heavy metal ions while Ca-Mt additions had little effect. After long-term simulated leaching for 5 years, TTA-Mt still had superior environmental stability for Zn and As with the immobilization rates of 96% and 86%, and the leaching amounts of Mn and Pb were less than 4.23 and 0.66 mg/kg, respectively. Morphology and chemical fraction analyses confirmed that the immobilization was mainly due to the formation of relatively stable phases by complexation and precipitation. Results presented here demonstrated the significant potential of TTA-Mt for long-term immobilization of heavy metals in tailings against acid rain and thus could provide guidance for remediation of tailings.
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WATER ENVIRONMENT RESEARCH
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2022
·Vol. 94
·期 4
·e10714
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IF 3.306
Yao Shi,Yifei Xing,Zhilian Song,Xueming Dang,Huimin Zhao
Fe–Mn binary oxide (FMBO) is a promising adsorbent for As(III) removal through combined adsorption and oxidation. The calcined oyster shell-supported Fe–Mn binary oxide (FMBO/OS) adsorbent was synthesized by the co-precipitation method. Results indicated that the calcined oyster shell, as a carrier, improved the stability of FMBO and its adsorption capacity for As(III). The maximum adsorption capacity of FMBO/OS on As(III) reached 140.5 mg·g −1 . Under pH 5.0 and 25°C, the removal efficiency of FMBO/OS to As(III) solution (C 0 = 10 mg·L −1 ) reached 87% within 12 h. Moreover, based on the characterization analyses, the removal mechanisms of As(III) were deduced to include the combined adsorption and oxidation process of FMBO and the synergistic effect of oyster shells. This work provides new insights into synthesizing efficient and green adsorbents to remove aqueous As(III). Meanwhile, it provides technical support for reusing waste biomass materials such as the oyster shell. Practitioner Points FMBO/OS was prepared by a simple hydrothermal co-precipitation method. The carrier alleviates the agglomeration of Fe–Mn oxides. The adsorbent shows a strong adsorption capacity of As(III) and good selectivity. The good results benefit from the synergistic effect of calcium arsenate generation. The prepared adsorbent can adsorb arsenic in real samples.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
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IF 11.357
Honglong Zhang,Zhenyu Shi,Jun Ma,Fuyi Cui,Jing Zhang,Timothy J. Strathmann
In this study, a representative redox mediator, 2,2,6,6-tetramethylpiperidine-N-oxyl (TEMPO), and its para-substituted derivatives (TEMPOs: 4-hydroxyl-TEMPO, 4-acetylamino-TEMPO, and 4-amino-TEMPO) significantly accelerated the abatement of trace organic contaminants (TrOCs, i.e., bisphenol-A (BPA), phenol, amines, and phenylbutazone) by Mn(VII) over a wide pH range of 4.0–9.0. The addition of substituents at para to the > N–O• moiety significantly influenced the degradation kinetics of TrOCs by changing the reduction potentials of TEMPOs and the corresponding oxoammonium cations (TEMPOs+); a linear relationship was observed between the substituents’ para Hammett sigma constants and the reduction potentials of TEMPOs and TEMPOs+. Pseudo-first-order reaction rate constants (kobs, min–1) of TrOC degradation by Mn(VII)/TEMPOs were also affected by the pKa of the TrOCs. Generally, the highest kobs values for individual TrOCs were observed at pH near the pKa even for TEMPOs+ with relatively pH-invariant reduction potentials. Overall, TrOC abatement kinetics were related to a combination of reactive species (Mn(VII), in situ formed MnO2, and TEMPOs+). For BPA, the relative contributions (R) of reactive species ranked as R(TEMPOs+) > R(Mn(VII)) > R(in situ formed MnO2) at pH 4.0–8.0, whereas R(Mn(VII)) > R(TEMPOs+) at pH 9.0 mainly owing to a change in BPA speciation as the pH approached the pKa1 value for BPA. The results of this study are useful for the development of heterogeneous TEMPO-based redox mediators and future applications of TEMPO-mediated oxidation systems for accelerated abatement of TrOCs in water.
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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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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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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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Journal of Cleaner Production
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2021
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IF 9.297
Weiye Wang,Qingliang Zhao,Jing Ding,Kun Wang,Junqiu Jiang
Bio-electro-Fenton powered by microbial fuel cell (MFC-powered BEF) can in-situ generate and utilize hydrogen peroxide to degrade refractory pollutants. Most of the previous works loaded transition metal on the cathode to participate in the Fenton reaction showed limited electrical or degradation performance. The coupling of alkaline-earth metal (Mg 0 and MgO) and transition metal on cathode could improve the electrochemical and catalytic properties of MFC-powered BEF system, which had not been reported so far. In this research, a novel cathode of Fe–Mn–Mg/carbon fiber (Fe–Mn–Mg/CF) was developed with good polymerization effect of Mg to Fe and Mn, and outstanding production of reactive oxide species (•OH and •O 2 − ), which further improved the overall electricity generation efficiency and enhanced the degradation of pollutants. Accordingly, the maximum power density generated in MFC-powered BEF system with Fe–Mn–Mg/CF cathode was 2.07 times higher than that of the frequently used Fe–Mn/CF. Owing to the superiority of surface holes and MgO in H + adsorption and electron transfer , the integration of Fe, Mn with Mg promoted the in-situ generation of H 2 O 2 and active radicals, resulting in the highest catalytic performance of degrading refractory pollutants . Initial pH, external resistance, initial concentration of contaminant and cycle use frequency of cathode were also evaluated on the degradation efficiency of the BEF system. Furthermore, reaction and degradation mechanisms were proposed from H 2 O 2 production and free radical characterization. Overall, this study provided a novel cathode preparation approach for the MFC-powered BEF system, which vastly promoted its electrochemical and catalytic properties.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Yaowei Lu,Yongxing Wang,Qinghu Tang,Qiue Cao,Wenhao Fang
The synergistic effect in a bimetallic oxide usually plays a vital role in determining the behavior of supported-metal catalysts. We show the unique synergy in a Sn x Mn 1 O y oxide, which can boost the hydrogenation catalysis of supported Pt nanoparticles for selective conversion of levulinic acid (LA) to γ-valerolactone (GVL). On a series of Pt/Sn x Mn 1 O y catalysts with a similar Pt loading ( ca. 0.44 wt%) and a controlled Pt size ( ca. 2.7 nm), the intrinsic TOF presents a volcano-like dependence on Pt 0 sites and Lewis acidity, which is determined by the variable synergistic effect between MnO y and SnO y . The optimal Pt/Sn 0.8 Mn 1 O y catalyst exhibits a high i TOF of 2709 h −1 and achieves 100% selectivity to GVL at 99% conversion of LA at 120 ℃ and 2 MPa of H 2 . DFT calculations demonstrate that the incorporation of Sn can provide a lower energy barrier for the crucial elementary reactions.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Richao Niu,Rubing Han,Yin Huang,Liming Dai,Hongan Zhao,Yining Wang,Junwu Zhu,Shaochun Tang,Jingwen Sun
Bimetallic compounds can offer higher electrochemical activity and capacity than monometallic ones owing to their rich chemical valences. Herein, the performance enhancement of monometallic compounds by introducing metal ions was demonstrated, and the effects of different metal ions were investigated. Through introduction of metal ions into LDHs under a hydrothermal environment, one kind of 2D/2D hierarchical CoM-LDH(M=Fe or Mn)/MXene composites were successfully synthesized. It was found that the introduced Fe ions extremely improves the specific capacity and the introduced Mn ions extremely enhances the rate capability of monometallic composite. The fabricated CoFe-LDH/MXene (CF-MX10) electrode exhibits a specific capacity of 808 F g −1 at current density of 0.5 A g −1 , much higher than that of CoMn-LDH/MXene (CM-MX10, 562 F g −1 ) and Co(OH) 2 /MXene (C-MX10, 270 F g −1 ). The high areal capacity or rate capacity are attributed to strong synergistic effect between CoM-LDH and MXene, as well as the introduction of metal ions that change the architecture and the electronic or ionic conductivity , which leads to much improved electrical conductivity and electrochemical stability.
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