SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Dongmei Liu,Aiying Guo,Yanling Qi,Zhixin Ji,Hongjuan Li,Xiumei Cao,Zhiwei Zhang,Xinyue Zhang,Kunze Wu,Aijun Cai
Removal of antibiotics and bacteria from wastewater is an effective approach to test the efficacy of catalyst and thus address the issues of water contamination. In this study, a stable magnetic Mg/Mn–layered double oxide–doped biochar composite (MgMnLDO–MBC) was prepared using Lentinula edodes substrate. This composite could further effectively activate the persulfates (PS), such as peroxymonosulfate (PMS) and peroxydisulfate (PDS). MgMnLDO coupling endowed BC and magnetic biochar (MBC) with enhanced surface areas, adsorption sites, and free radicals, which facilitated the improvement of catalytic activity of MgMnLDO–MBC/PS system toward pollutants. MgMnLDO-MBC/PMS system could remove 90.8% of ciprofloxacin (CIP) with 2.8 times the removal efficiency of MBC/PMS system. Density functional theory (DFT) calculation and intermediate analysis showed that the synergistic effect of nucleophilic, electrophilic, and radical active species–mediated reactions improved the removal performance of MgMnLDO–MBC/PMS system. MgMnLDO–MBC/PDS system could efficiently kill 97.6% Escherichia coli and 99.7% Staphylococcus aureus , and destroy the existing biofilms. The effects of composite concentration, PMS loading, pH, temperature, common anions, and humic acid on removal efficiency were also evaluated. After five consecutive cycles, MgMnLDO–MBC/PS system still exhibited high catalytic performance toward CIP removal and bactericidal ability. Results of quenching and electron spin resonance (ESR) showed that ·SO, ·OH, 1 O 2 , and charge transfer were together involved in CIP removal, with ·SO playing a major role. Furthermore, the double–layered metal oxide (LDO) and MBC present in MgMnLDO–MBC composites exhibited a strong synergistic effect in the catalytic process, which resulted in higher reactivity and lower leaching rate of metal ions. In this study, an environment–friendly catalyst was prepared using industrial waste and its efficiency for removal of antibiotics and bacteria from wastewater was verified.
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WATER RESEARCH
·
2023
·
IF 12.8
Yinning He,Jiayi Li,Jingyu Tang,Haijun Cheng,Tao Zeng,Zhiqiao He,Da Wang,Lizhang Wang,Shuang Song,Jun Ma
In this study, N-doped Mn 3 O 4 catalysts (Mn- n N) with electron-dense Mn sites were synthesized and employed in heterogeneous catalytic ozonation (HCO). These catalysts demonstrated excellent performance in pyrazines degradation and odor elimination. The synthesis of Mn- n N was achieved through a facile urea-assisted heat treatment method. Experimental characterization and theoretical analyses revealed that the Mn N structures in Mn- n N, played a crucial role in facilitating the formation of electron-dense Mn sites that served as the primary active sites for ozone activation. In particular, Mn-1N exhibited excellent performance in the HCO system, demonstrating the highest 2,5-dimethylpyrazine (2,5-DMP) degradation efficiency. • OH was confirmed as the primary reactive oxygen species involved in the HCO process. The second-order rate constants for 2,5-DMP degradation with O 3 and • OH, were determined to be (3.75 ± 0.018) × 10 −1 and (6.29 ± 0.844) × 10 9 M −1 s −1 , respectively. Seventeen intermediates were identified through GC-MS analysis during the degradation of 2,5-DMP via HCO process with Mn-1N. The degradation pathways were subsequently proposed by considering these identified intermediates. This study introduces a novel approach to synthesize N-doped Mn 3 O 4 catalysts and demonstrates their efficacy in HCO for the degradation of pyrazines and the elimination of associated odors. The results show that the catalysts are promising for addressing odor-related environmental issues and provide valuable insights about the broader significance of catalytic ozonation processes.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Junyong He,Ya Yang,Peidong Hong,Yulian Li,Chao Xie,Zijian Wu,Minqiang Li,Lingtao Kong
The use of peroxymonosulfate (PMS) activation to eliminate organic contaminants is a promising technology to purify water owing to its strong reactivity. However, because of the existed rate limiting step, the performance of PMS activation was restrained and required external energy consumption. Therefore, a new strategy was proposed to solve this problem by preparing catalysts with abundant electron-rich sites and electron traps to accelerate PMS activation. In this research, a novel MnCeO x -H catalyst with rich surface oxygen vacancies was firstly synthesized to accelerate the transfer of electrons among the catalysts, oxidant and pollutants. The contaminants were rapidly eliminated in the MnCeO x -H/PMS system, while the reaction rate constant of MnCeO x -H/PMS system was 30 times higher than that of CeO 2 /PMS system. The surface oxygen vacancies were able to adsorb and trap PMS, then the free electrons of oxygen vacancies would reduce PMS and produced HO•, 1 O 2 and SO 4 •- , while 1 O 2 played a major role. The contaminants which acted as electron-donors in this system were adsorbed at Mn, Ce sites, achieving effective conversion recycling of Ce(IV)/Ce(III), Mn(III)/Mn(II) and Mn(IV)/Mn(III). This discovery is believed to inaugurate a novel way for designing powerful electron-rich sites and electron traps to accelerate PMS activation for contaminants degradation.
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JOURNAL OF LUMINESCENCE
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2023
·
IF 3.6
Xiaochun Hou,Chengxue Du,Qing Pang,Chaoyang Jia,Xiaojun Wang,Dangli Gao
Up-conversion persistent luminescence (UCPL) nanoparticles have captured tremendous attention due to their unique optical operating performance such as the absence of auto-fluorescence and the charging capacity of near-infrared (NIR) light. However, the weak afterglow intensity as well as low duration limits their practical applications including multimode anti-counterfeiting and biological imaging, etc. Herein, typical green persistent luminescence (PersL) and photo-stimulated luminescence (PSL) of Zn 2 GeO 4 :Mn 2+ phosphors were enhanced via non-equivalent Li + co-doping, in which the preferred site selection of Mn 2+ and Li + have been verified by using the first-principles theory. The possible luminescent enhancement mechanisms were proposed based on improving the oxygen vacancy density and promoting the formation of Mn 4+ defect energy level in bandgap structure by non-equivalent doping of Li + . Interestingly, UCPL of Zn 2 GeO 4 :Mn 2+ ,Li + can be achieved after charging of Vis to NIR light. It is worth noting that this UCPL can be further enhanced by the sensitization of NaYF 4 :Yb,Tm nanoparticles via simply mixing Zn 2 GeO 4 :Mn 2+ ,Li + and NaYF 4 :Yb,Tm under 980 laser stimulation. As a result, Zn 2 GeO 4 :Mn 2+ ,Li + phosphor exhibits the enhanced quintuple-mode luminescence including photoluminescence , PersL, PSL, photo-stimulated persistent luminescence and UCPL. In particular, the achieved NIR rechargeable UCPL hybrid phosphors exhibit enormous potential for higher order anti-counterfeiting and rewriteable data encryption and decryption applications.
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MATERIALS & DESIGN
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2017
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IF 4.364
Xiu Liu,Lei Huang,Dengsong Zhang,Tingting Yan,Jianping Zhang,Liyi Shi
This work reports the synthesis of highly dispersed Mn-Co/RGO via a novel light driven approach having attributes of being green, facile and controllable, for the catalytic degradation of methylene blue (MB) in the presence of H 2 O 2 . The prepared catalysts were characterized by TEM, EDS , IR, XRD and XPS techniques. A synergy between RGO and Mn-Co species existed where the former helped in adsorption of MB and stabilization and dispersion of Mn and Co on the surface while the latter improved H 2 O 2 utilization by generating HO , which enhanced the decomposition of MB. It was found that O 2 •− and O 2 •− /HO • were the main radicals in post Mn/RGO and Mn-Co/RGO treatment, respectively. Both O 2 •− and HO • oxidized MB with a faster rate by the former, but its side reaction can hinder effective utilization of H 2 O 2 while the reverse was true for the latter. A 50 mg/L MB was completely decomposed within 15 min using 10 mg of Mn-Co/RGO. Thus the synergistic effect of RGO by adsorption MB and Co species avoiding the side reaction led to enhanced rate of MB decomposition.
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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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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
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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高影响因子
CRYSTENGCOMM
·
2023
·Vol. 25
·期 20
·3066-3078
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IF 3.1
Jinyu Ma,Qing Sun,Chuan Jing,Faling Ling,Xiao Tang,Yanhong Li,Yongjie Wang,Sha Jiang,Kexin Yao,Xianju Zhou
Since the energy density and voltage window of supercapacitors cannot match that of lithium-ion batteries, supercapacitors are far from replacing batteries but can only be seen as a supplement to battery charge storage or transmission devices. The design of transition metal oxide-based electrodes with high cycling capacitance retention is very important for the development of supercapacitors. In this study, flower-like SAC@NiCoMn-LDH electrode materials with different Mn doping ratios were prepared by a hydrothermal method with mesoporous carbon (SAC) as the substrate. Density functional theory (DFT) calculations confirm that Mn doping can enhance the adsorption of OH− and the desorption of the H proton. In addition, Mn doping increases the density of states of LDH near the Fermi level and increases the number of active electrons, which is conducive to the occurrence of electrochemical reactions. In the three-electrode system, SAC@Ni2Co0.95Mn0.05-LDH with optimal doping ratio increased the specific capacitance by three times compared to that of NiCo-LDH and displayed an excellent cycling stability (83.76% capacitance retention after 50 000 cycles). Moreover, the prepared SAC@Ni2Co0.95Mn0.05-LDH and commercial activated carbon (AC) were made into electrode plates and then assembled into a SAC@Ni2Co0.95Mn0.05-LDH//AC asymmetric supercapacitor (ASC). The ASC exhibited high energy density (23.68 W h kg−1 at 325 W kg−1) and excellent specific capacitance retention (85.32% after 50 000 cycles), making it well suited for efficient wind energy storage and conversion with promising practical applications.
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Nano Research
·
2023
·Vol. 16
·期 8
·10748-10755
·
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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CHEMOSPHERE
·
2023
·
IF 8.8
Linsong Cheng,Yuanxiang Mao,Lei Jiang,Rui Ma,Jiangsen Ma,Yiyuan Zhuo,Qiushi Shen,Caocong Liu,Liuwei Zhao,Xiaoyi Xu,Fangying Ji
The high concentration of salt in organic wastewater has a strong inhibitory effect on the removal of pollutants. A method for the efficient removal of trace pollutants in high-salinity organic wastewater was developed. This study investigated the effect of the combination of permanganate [Mn(VII)] and calcium sulfite [S(IV)] on pollutant removal in hypersaline wastewater . The Mn(VII)-CaSO 3 system removed more pollutants from high-salinity organic wastewater than from normal-salinity wastewater. Chloride (increasing from 1 M to 5 M) and low concentration of sulfate (increasing from 0.05 M to 0.5 M) significantly enhanced the system's resistance to pollutants under neutral conditions. Despite the fact that Cl − can combine with the free radicals in the system and reduce their efficiency in removing pollutants, the presence of chloride ions greatly enhances the electron transfer rate in the system, promoting the conversion of Mn(VII) to Mn(III) and significantly increasing the reaction rate of Mn(III) as the primary active species. Therefore, chloride salts can greatly enhance the removal of organic pollutants by Mn(VII)-CaSO 3 . Although sulfate does not react with free radicals, a high concentration of sulfate (1 M) will affect the formation of Mn(III), which greatly weakens the removal effect of the entire system on pollutants. The system can still have a good pollutant removal effect with mixed salt. Altogether, this study demonstrates that the Mn(VII)-CaSO 3 system offers new possibilities for the treatment of organic pollutants in hypersaline wastewater.
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Green Energy & Environment
·
2023
·
IF 13.3
Changjian Yuan,Xianglei Liu,Xinrui Wang,Chao Song,Hangbin Zheng,Cheng Tian,Ke Gao,Nan Sun,Zhixing Jiang,Yimin Xuan,Yulong Ding
Solar thermochemical energy storage based on calcium looping (CaL) process is a promising technology for next-generation concentrated solar power (CSP) systems. However, conventional calcium carbonate (CaCO 3 ) pellets suffer from slow reaction kinetics, poor stability, and low solar absorptance. Here, we successfully realized high power density and highly stable solar thermochemical energy storage/release by synergistically accelerating energy storage/release via binary sulfate and promoting cycle stability, mechanical strength, and solar absorptance via Al–Mn–Fe oxides. The energy storage density of proposed CaCO 3 pellets is still as high as 1455 kJ kg −1 with only a slight decay rate of 4.91% over 100 cycles, which is higher than that of state-of-the-art pellets in the literature, in stark contrast to 69.9% of pure CaCO 3 pellets over 35 cycles. Compared with pure CaCO 3 , the energy storage power density or decomposition rate is improved by 120% due to lower activation energy and promotion of Ca 2+ diffusion by binary sulfate. The energy release or carbonation rate rises by 10% because of high O 2− transport ability of molten binary sulfate. Benefiting from fast energy storage/release rate and high solar absorptance, thermochemical energy storage efficiency is enhanced by more than 50% under direct solar irradiation. This work paves the way for application of direct solar thermochemical energy storage techniques via achieving fast energy storage/release rate, high energy density, good cyclic stability, and high solar absorptance simultaneously.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Qinghe Liu,Sen Wang,Fei Han,Shupei Lv,Daokui Li,Jing Ouyang
Manganese oxide has been recognized as one of the most promising gaseous heterogeneous catalysts due to its low cost, environmental friendliness , and high catalytic oxidation performance. The modulation of the interfacial coupling effect of manganese oxides by chemical means is considered a critical and effective way to improve the catalytic performance. Herein, a novel one-step synthetic strategy of highly-efficient ultrathin manganese-based catalysts is proposed through optimal regulation of metal/manganese oxide multi-interfacial coupling. Carbon monoxide (CO) and propane (C 3 H 8 ) oxidation are employed as probe reactions to investigate the structure-catalytic mechanism - catalytic performance relationship. The ultrathin manganese (Mn)-based catalyst exhibits superior low-temperature catalytic activity with a 90% conversion of CO/C 3 H 8 realized at 106℃ and 350℃. Subsequently, the effect of “interfacial effect” on the intrinsic properties of manganese oxides is revealed. The ultrathin appearance of two–dimensional (2D) manganese dioxide (MnO 2 ) nanosheets changes the binding force in the vertical direction, thus resulting in an increase in the average manganese-oxygen (Mn-O) bond length and exposing more surface defects . Besides, the introduction of Copper (Cu) species into the catalyst further weakens the Mn-O bond and promotes the generation of oxygen vacancies , which subsequently enhances the oxygen migration rate. This study provides new insights into the optimal design of transition metal oxide interfacial assemblies for efficient catalytic reactions .
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