期刊：
International Journal of Biological Macromolecules,2024年261(Pt 2):129761 ISSN：0141-8130
通讯作者：
Qingtao Liu
作者机构：
[Zhou, Yu] Key Laboratory of Coal Conversion and New Carbon Materials of Hubei Province, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan, Hubei 430081, PR China;Hubei Key Laboratory of Pollutant Analysis & Reuse Technology, College of Chemistry and Chemical Engineering, Hubei Normal University, Huangshi 435002, PR China;[Liu, Xiyu] The Ninth Hospital of Wuhan City, Wuhan, Hubei 430081, PR China;[Liu, Qingtao] National Local Joint Laboratory for Advanced Textile Processing and Clean Production, Wuhan Textile University, Wuhan, Hubei 430200, PR China;School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, PR China
通讯机构：
[Qingtao Liu] N;National Local Joint Laboratory for Advanced Textile Processing and Clean Production, Wuhan Textile University, Wuhan, Hubei 430200, PR China
摘要：
The weak immunity of tumors after chemotherapy could cause tumor metastasis and progression. Therefore, to overcome the dilemma of obvious immune deficiency caused by chemotherapy, a nanosystem (N-IL-12/DOX/α-TOS) consisted of thioketal (TK) bonds linked-hollow mesoporous silica nanoparticles (HMSNs) coated with carboxymethyl chitin (CMCH) by electrostatic interaction, and surface-functionalized glucose-regulated protein 78 binding peptide was prepared for loading doxorubicin (DOX), IL-12 and α-tocopheryl succinate (α-TOS). N-IL-12/DOX/α-TOS displayed a mean size of 275nm after encapsulated DOX, IL-12 and α-TOS with loading contents of 2.04×10(-4), 4.01×10(-2) and 7.12×10(-2), respectively. The drug-free nanoparticles (NPs) showed good biocompatibility to both 4T1 cells and RAW264.7 macrophages. N-IL-12/DOX/α-TOS could achieve localized release of IL-12, DOX and α-TOS by pH and H(2)O(2) trigger in the tumor microenvironment (TME). Moreover, the combined therapy by N-IL-12/DOX/α-TOS remarkably elevated the anti-tumor therapeutic efficacy, enhanced immune responses via promoting tumor-associated macrophage (TAM) polarization into tumoricidal M1 phenotypes, and decreased lung metastasis with reduced side effects. N-IL-12/DOX/α-TOS exhibited as a promising strategy for combining chemotherapy and local macrophage modulation-immunotherapy for anti-tumor therapy.
通讯机构：
[Sun, LB ] N;[Yan, JT ] W;Nanjing Tech Univ, Coll Chem Engn, Jiangsu Natl Synerget Innovat Ctr Adv Mat SICAM, State Key Lab Mat Oriented Chem Engn, Nanjing 211816, Peoples R China.;Wuhan Polytech Univ, Coll Chem & Environm Engn, Wuhan 430023, Peoples R China.
摘要：
Solid base catalysts are widely used in the chemical industry owing to their advantages of environmental friendliness and easy separation. However, their application is limited by basic site aggregation and poor stability. In this study, we report the preparation of magnesium (Mg) single-atom catalysts with high activity and stability by a sublimation-trapping strategy. The Mg net was sublimated as Mg vapor at 620 °C, subsequently transported through argon, and finally trapped on the defects of nitrogen-doped carbon derived from metal-organic framework ZIF-8, producing Mg(1)/NC. Because of the atomically dispersed Mg sites, the obtained Mg(1)/NC exhibits high catalytic activity and stability for Knoevenagel condensation of benzaldehyde with malononitrile, which is a typical base-catalyzed reaction. The Mg(1)/NC catalyst achieves a high efficiency with a turnover frequency of 49.6 h(-1), which is much better than that of the traditional counterpart MgO/NC (7.7 h(-1)). In particular, the activity of Mg(1)/NC shows no decrease after five catalytic cycles, while that of MgO/NC declines due to the instability of basic sites.
摘要：
A green and sustainable approach was employed to synthesize N, O-codoped porous carbon nanorods with two-end-open characteristics. In this method, a crab shell was utilized as a template and activator, while egg white served as a carbon precursor. The resulting carbon nanorods sintered at 700 degrees C (CNRs-700), exhibited cross-linked pore channels, a high surface area, and abundant defects and active sites. These features imparted superior energy storage properties to the material, enabling its application as both an anode for lithium-ion batteries and a supercapacitor. The CNRs-700 demonstrated an exceptional lithium storage capacity of 530.6 mAh g(-1) at 2 A g(-1), corresponding to 90.1% of the capacity achieved at 100 mA g(-1), which is ascribed to the pseudocapacitive contribution. Furthermore, in an evaluation combining a three-electrode configuration in KOH electrolyte at a high current density of 50 A g(-1), the CNRs-700 retained a specific capacitance of 140 F g(-1). For symmetrical supercapacitors based on CNRs-700 in 1 M Na2SO4 electrolyte, the energy density reached 27.1 Wh kg(-1) at a 375 W kg(-1) power density, demonstrating remarkable cyclability over 10,000 consecutive cycles. The superior rate performance and cycling stability would accentuate the suitability of the biomass-derived carbon materials for such systems.
摘要：
This study reports the synthesis of Er-doped, Mn-doped, and Er, Mn co-doped monoclinic BiVO4 photocatalysts via a facile one-pot hydrothermal method. Er6%Mn2%/BiVO4 exhibited a larger specific surface area, bigger pore volume, and smaller average pore size compared to pure BiVO4 and single-doped BiVO4. The co-doping of Er3+ and Mn2+ ions resulted in lattice distortion and crystal particle size reduction of BiVO4, and generated a new impurity level at the bottom of the conduction band, narrowing the band gap and widening the absorption edge of visible light, thus improving the separation efficiency of photogenerated electron-hole pairs. Photocatalytic experiments on rhodamine B showed that Er6%Mn2%/BiVO4 achieved a degradation efficiency of 97.8% under visible light irradiation (lambda >420 nm) within 100 min, which is higher than those of BiVO4, Er-6%/BiVO4, and Mn-6%/BiVO4. The kinetic rate constant (0.0312 min(-1)) of Er6%Mn2%/BiVO4 was 1.3, 2.2, and 4.7 times higher than those of Er-6%/BiVO4, Mn-6%/BiVO4, and BiVO4, respectively. The study also identified <middle dot>O-2(-) and h(+) as the predominant active species involved in the photocatalytic degradation of rhodamine B and demonstrated the excellent stability of Er6%Mn2%/BiVO4 for five cycles of photodegradation experiment. This work highlights that Er6%Mn2%/BiVO4 has great potential as a candidate for treating organic pollutants in water.
摘要：
Due to their large surface area and pore volume, three-dimensional covalent organic frameworks (3D COFs) have emerged as competitive porous materials. However, structural dynamic behavior, often observed in imine-linked 3D COFs, could potentially unlock their potential application in gas storage. Herein, we showed how a pre-locked linker strategy introduces breaking dynamic behavior in 3D COFs. A predesigned planar linker-based 3,8-diamino-6-phenylphenanthridine (DPP) was prepared to produce non-dynamic 3D JUC-595, as the benzylideneamine moiety in DPP locked the linker flexibility and restricted the molecular bond rotation of the imine linkages. Upon solvent inclusion and release, the PXRD profile of JUC-595 remained intake, while JUC-594 with a flexible benzidine linker experienced crystal transformation due to framework contraction-expansion. As a result, the activated JUC-595 achieved higher surface areas (754 m2 g-1) than that of JUC-594 (548 m2 g-1). Furthermore, improved CO2 and CH4 storages were also seen in JUC-595 compared with JUC-594. Impressively, JUC-595 recorded a high normalized H2 storage capacity that surpassed other reported high-surface area 3D COFs. This works shows important insights on manipulating the structural properties of 3D COF to tune gas storage performance.
摘要：
Four typical forest types in Sygera Mountain, namely, Pinus armandii (PA), Picea likiangensis var. linzhiensis (PLL), Abies georgei var. smithii (AGS), and Juniperus saltuaria (JS) were considered using methods such as analysis of variance and stoichiometry. Effects of changes of nutrient content and stoichiometric ratio of various organs of arbor plants were evaluated. Compared with global plant nutrients, this study area had lower N and P contents. The growth of the Juniperus saltuaria forest was jointly restricted by N and P, and as the environmental gradient decreased, the growth of the other three forest types changed from N and P joint restrictions to N restrictions. The distribution order of element content in various organs among different forest types was consistent as follows: leaf>branch>root>trunk. There was a strong domestication reaction between N and P contents. This led to a significantly higher C/N ratio of the square branch Berlin compared to the other three forest types, while the C/P and N/P ratios were opposite. This may be due to the "optimal allocation principle" of nutrients in various organs under different environmental conditions. The nutrient allocation patterns of plant organs in different forest types were not the same, which reflects the differences in life strategies and nutrient utilization among different forest species.
摘要：
We explored the resource acquisition and growth strategies of plants adapting to different environments, focusing on the typical forest types of Sygera Mountain: Pinus armandii, Picea likiangensis var. Linzhiensis, Abies georgei var. Smithii, and Juniperus saltuaria. Then, we analyzed the nutrient content and stoichiometric ratios of C, N, P, and K in different plant organs (leaves, branches, trunks, and roots) to examine the stoichiometric characteristics and nutrient balance mechanisms in these forests. Results show that within the same forest type, different plant organs exhibit high C and low N, P, and K levels. N content in all organs followed the order leaves > branches > roots > trunks. During the growth phase, the concentrations of P and K in PLL and AGS follow the order branches > leaves > roots > trunks. In the dormant phase, the distribution in different organs had the order leaves > branches > roots > trunks. C content remained relatively stable over time. In the same organ across different forest types, increase in nitrogen content in plant leaves is an active adaptation of JS plants, indicating that JS has a conservative growth strategy and can adapt to environmental stress. Owing to the influence of seasons, the evolution process of N and P content fluctuates, allocating nutrients to supporting and transporting organs for resource optimization and allocation. The N and P content were lower in the growth phase than in the dormant phase. Seasonal variations in the C/N, C/P, and C/K ratios in different forests were inversely correlated with changes in N, P, and K content in plant organs, supporting the "growth rate hypothesis." Stoichiometric analysis suggests that different limiting elements exist in organs across various forest types. Principal component analysis indicates that the seasonal patterns of stoichiometric ratios in the organs of different forest types show species-specific characteristics, reflecting the evolutionary nutrient utilization strategies of plant genera. In summary, plant growth in different Sygera Mountain forest types is limited by N and P, with a high tendency toward nitrogen limitation. The nutrient utilization and distribution differences among various organs during different growth stages are primarily influenced by the limited availability of environmental nutrients and inherent physiological characteristics of the plants.
摘要：
Large scale of Cd-contaminated soil has become a serious threat to environmental safety and human health, whereas field applicability of existing remediation technologies has encountered numerous obstacles, such as poor stability, secondary pollution, long operation time, and high chemical cost. Herein, a novel activated calcite with significantly enhanced immobilization stability of Cd in soil has been synthesized based on mechanochemical technology. Our results demonstrate that the passivation rate of bioavailable Cd in Cd-contaminated soil (initial concentration 3 mg/kg) could be maintained at 65 % after 50 days of passivation cultured with activated calcite. Mechanistic studies have revealed that the outstanding performance is attributed to the enhancement of the CO32– and Ca2+ release properties of calcite through mechanical activation, leading to a 550 % increase in Ca2+ release. The CO32– fraction binds in situ to the free Cd in the soil, forming a stable carbonate-bound state. Simultaneously, the OH– released from the continuous hydrolysis of CO32– effectively regulates and stabilizes the soil pH within the neutral range. Further, SEM-EDS and sequential extraction procedures (SEP) analyses implied that the specific adsorption of Cd by in-situ formed iron oxides in soil was visibly related to the release of OH– from activated calcite and immobilized the free state Cd in the more stable iron oxide-bound state. The current work shows the high sustainability and stability of Cd-contaminated soil immobilization by activated calcite materials.
摘要：
In this study, magnetic DTPA-modified chitosan composite microspheres (MDCM) were prepared by reverse emulsion-double crosslinking method (carbodiimide followed by glutaraldehyde) for removal of Pb(II) from aqueous solution. The obtained magnetic adsorbents were characterized by FTIR, SEM, XRD, VSM, BET, and (13)C NMR. The effects of the pH, contact time, initial concentration, and competitive metal cations (Na(I), Ca(II), or Mg(II)) on Pb(II) adsorption were investigated. The results revealed that MDCM exhibited high removal performance over a wide pH range and in the presence of competitive metal cations. The maximum adsorption capacity of MDCM for Pb(II) is 214.63mgg(-1) at pH3, which is higher than most recently reported magnetic adsorbents. Adsorption kinetics and isotherms can be described by the pseudo-second-order model and Langmuir model, respectively. In addition, MDCM is easy to regenerate and can be reused five cycles with high adsorption capacity. Finally, the adsorption mechanism was further revealed by FTIR and XPS analysis. Overall, MDCM has practical application potential in removing Pb(II) from contaminated wastewater due to its high adsorption efficiency, good reusability, and convenient magnetic separation.
通讯机构：
[Liu, YJ; Liu, Y ] T;Tiangong Univ, Sch Chem, State Key Lab Separat Membranes & Membrane Proc, Tianjin 300387, Peoples R China.;Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Peoples R China.
关键词：
CRISPR/Cas9;Controlled-release;Immunotherapy;Metabolic therapy;Theranostic;Triple-negative breast cancer (TNBC)
摘要：
Metabolic heterogeneity and the tumor immunosuppressive microenvironment (TIME) of triple-negative breast cancer (TNBC) hinder therapeutic effectiveness. Although emerging metabolic therapy and immunotherapy show promise, they are limited by off-target effects and immune escape. Here, a redox-activatable, sequentially-releasing nanoparticle (AMANC@M) for tumor-targeted delivery of anticancer agents and CRISPR/Cas9 has been developed. AMANC@M can reverse the TIME through dual metabolic inhibition, thereby enhancing TNBC therapy. AMANC@M demonstrates excellent biosafety and targets tumors precisely through biomimetic hybrid membrane-mediated homologous homing and the enhanced permeability and retention (EPR) effect. Once internalized into tumor cells, the CRISPR/Cas9 system ("energy nanolock") is released through glutathione (GSH) cleavage and effectively knocks down the expression of lactate dehydrogenase A (LDHA) to suppress glycolysis. After peeling off of the gene editing shell, a newly synthesized targeted drug, CPI-Z2 ("nutrihijacker" and "energy nanolock"), is released in a controlled manner to block the mitochondrial tricarboxylic acid (TCA) cycle. Nitric oxide (NO) produced from loaded L-arginine enhances the efficiency of CPI-Z2 and reduces drug resistance. Combined with NO therapy, both blockades of nutrients and energy production transform the hypoxia and acidic TIME into an immunocompetent tumor microenvironment (TME) for tumor elimination. Furthermore, AMANC@M offers capabilities for photothermal (PT) therapy and provides clear imaging through PT, photoacoustic (PA), or computed tomography (CT) signals in tumor tissue. Thus, this study provides a new and promising sequentially stimuli-responsive targeting strategy for nanoparticle development, making it a potential treatment candidate for TNBC and other tumors.
期刊：
Journal of Hazardous Materials,2024年469:133996 ISSN：0304-3894
通讯作者：
Long, Yangke;Li, Sheng
作者机构：
[Long, Yangke] Department of Transportation and Environment, Shenzhen Institute of Information Technology, Shenzhen 518172, China. Electronic address: longyk@sziit.edu.cn;[Zhao, Jiakun] School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China;[Dai, Jian] School of Instrumentation Science and Engineering, Harbin Institute of Technology, Harbin 150080, China;[Lin, Manling; Lu, Guangzhao] Department of Transportation and Environment, Shenzhen Institute of Information Technology, Shenzhen 518172, China;[Li, Sheng] School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China. Electronic address: lfrcs@163.com
通讯机构：
[Li, Sheng] S;[Long, Yangke] D;Department of Transportation and Environment, Shenzhen Institute of Information Technology, Shenzhen 518172, China. Electronic address:;School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China. Electronic address:
摘要：
Atomically dispersed metal activators (ADMAs) have demonstrated unique advantages in environmental remediation, but how to controllably regulate the active site density and electronic structure of ADMAs to further enhance activation efficiency remains challenging. Here, we introduce a sulfur-atom-doping approach that allows the fine-tuning of atomic Co site content and electronic structure, enabling exploration of density-dependent activation performance of ADMAs for peroxymonosulfate (PMS)-based Fenton-like catalysis. Our investigation reveals a direct correlation between activation capacity and single-Co-site density. The optimal SNC@CoSA-0.05 activator with densely populated Co-N(3)S(1) sites (10.1wt%) displays exceptional efficacy in eliminating Rhodamine B, with specific activity of 31.0min(-1) g(-1) L, outperforming most previously published activators. Moreover, SNC@CoSA-0.05 showed a remarkedly reduced metal leaching (47.4μgL(-1)) than its nanocluster counterpart (194μgL(-1)) at pH 3.2. Experimental and theoretical analyses unveiled that coordinated sulfur actively modulates the electronic structure of the central Co atom, enhancing the adsorption and activation of PMS, thereby improving decontamination efficiency. Mechanistic studies further elucidate the predominant electron-transfer regime involved in oxidizing micropollutants by SNC@CoSA-0.05/PMS, with Co(IV)=O, •OH, and SO(4)(•-) being the auxiliary oxidizing species. This study not only offers a method for concurrent adjustment of active site density and electronic structure in ADMAs but also sheds light on the activation mechanisms of atomic metal sites.
摘要：
Although tremendous progress has recently been made in multi-walled carbon nanotubes (MWCNT) and titania, the photocatalytic degradation efficiency is still greatly limited by the ideal cobalt dopant concentration and temperature. Herein, Co-CNT/TiO2 composites were used to improve the photocatalytic degradation efficiency of malachite green (MG) solution. Consequently, compared to the binary CNT/TiO2 and pure TiO2 samples, the ternary Co-CNT/TiO2 samples showed much better photocatalytic activity. The sample calcined at 500 degrees C showed better reactivity, and the ideal cobalt dopant concentration for the highest photocatalytic degradation was 0.5%.
摘要：
In the present study, we demonstrated that the presence of cysteine could remarkably enhance the degradation of atrazine by Fe(3)O(4)/persulfate system. The results of electron paramagnetic resonance (EPR) spectra confirmed the combination of cysteine and Fe(3)O(4) exhibited much higher activity on activation of persulfate to generate more SO(4)(•-) and •OH than Fe(3)O(4) alone. At pH of 3.0, SO(4)(•-) and •OH contributed to about 58.2% and 41.8% of atrazine removal respectively, while •OH gradually dominated the oxidation of atrazine from neutral condition to alkaline condition. The co-existing Cl(-) and HCO(3)(-) could quench SO(4)(•-), resulting in the inhibition of atrazine degradation. The presence of low natural organic matters (NOM) concentration (0-2mgL(-1)) could enhance the atrazine removal, and high concentration (>5mgL(-1)) of NOM restrained the atrazine degradation. During the Cysteine/Fe(3)O(4)/Persulfate process, cysteine served as a complexing reagent and reductant. Through acidolysis and complexation, Fe(3)O(4) could release dissolved and surface bound Fe(2+), both of which contributed to the activation of persulfate together. Meanwhile, cysteine was not rapidly consumed due to a regeneration process, which was beneficial for maintaining Fe(2+)/Fe(3+) cycle and constantly accelerating the activation of persulfate for atrazine degradation. The reused Fe(3)O(4) and cysteine in the Cysteine/Fe(3)O(4)/Persulfate process exhibited high stability for the atrazine degradation after three cycles. The degradation pathway of atrazine included alkylic-oxidation, dealkylation, dechlorination-hydroxylation processes. The present study indicates the novel Cysteine/Fe(3)O(4)/Persulfate process might be a high potential for treatment of organic polluted water.
作者机构：
[Yi Qin; Bo Chai; Ya Sun; Guozhi Fan; Guangsen Song] School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, PR China;[Xiaohu Zhang] College of Chemistry, Huazhong Agricultural University, Wuhan 430070, PR China
通讯机构：
[Bo Chai; Ya Sun] S;School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, PR China
摘要：
A novel cellulose composite (denoted as PEI@MMA-1) with porous interconnected structure was prepared by adsorbing methyl cellulose (MC) onto microcrystalline cellulose (MCC) and cross-linking polyethyleneimine (PEI) with MCC by the action of epichlorohydrin, which had the excellent adsorption property, wettability and elasticity. The performances of PEI@MMA-1 composite for removing tetracycline (TC), Cu2+ and coexistent pollutant (TC and Cu2+ mixture) were systematically explored. For single TC or Cu2+ contaminant, the maximum adsorption capacities were 75.53 and 562.23 mg/g at 30 °C, respectively, while in the dual contaminant system, they would form complexes and Cu2+ could play a “bridge” role to remarkably promote the adsorption of TC with the maximum adsorption capacities of 281.66 and 253.58 mg/g for TC and Cu2+. In addition, the adsorption kinetics, isotherms and adsorption mechanisms of single-pollutant and dual-pollutant systems have been thoroughly investigated. Theoretical calculations indicated that the amide group of TC molecule with the assistance of Cu2+ interacted with the hydroxyl group of PEI@MMA-1 composite to enhance the TC adsorption capacity. Cycle regeneration and fixed bed column experiments revealed that the PEI@MMA-1 possessed the excellent stability and utility. Current PEI@MMA-1 cellulose composite exhibited a promising application for remediation of heavy metals and antibiotics coexistence wastewater.
作者机构：
[Xu Zhang; Xing Peng] Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, Central China Normal University, Wuhan 430079, PR China;[Zixin Yao; Yan Gao; Wenjuan Shen] School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, PR China;[Shuang Yan] School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan 430081, PR China
通讯机构：
[Xing Peng] K;[Wenjuan Shen] S;Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, Central China Normal University, Wuhan 430079, PR China<&wdkj&>School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, PR China
摘要：
The inhibition of electron transfer by the iron oxide passivation layer and the competition of oxygen for electrons limited the efficiency of heavy metal removal by zero-valent iron reduction. Herein we synthesized micron zero-valent iron modified with boric acid by mechanical ball milling, and demonstrated its enhanced copper ions removal performance. Compared to pristine ZVI, B-ZVI is approximately 2.6 times more efficient in the removal of copper. Interestingly, copper removal was significantly inhibited under air atmosphere for pristine ZVI. However, for B-ZVI, copper removal efficiency was almost insignificantly different between air and argon atmosphere conditions. Furthermore, the modification of ZVI with boric acid promoted the Cu(II) reduction proportion. Boronated modification effectively inhibited oxygen competition for electrons in removing heavy metals by zero-valent iron, which was conducive to the improvement of the heavy metal removal efficiency and the electron utilization of zero-valent iron. This study elucidated the importance of surface modification on the reactivity of micron-sized zero-valent iron and provided an efficient heavy metal removal strategy with zero-valent iron for environmental remediation.
摘要：
Monoethanolamine (MEA) electrooxidation occurring on Ni catalyst has proven to be a viable tactics for simultaneous MEA degradation and energy recovery. However, the excessively large overpotential (1505 mV) on Ni catalyst either causes high electricity consumption when acquiring H2 from MEA-containing electrolyzer or leads to low energy output when extracting electricity from direct MEA fuel cell. In this context, the reaction mechanism of MEA electrooxidation on Ni-based catalyst is deciphered at first by employing a specially designed three-step electrochemical procedure and in-situ Raman spectroscopy. Electrochemical data deconvolutions indicate the indirect electrochemical-chemical reaction path, via Ni(OH)2/NiOOH mediator, occupies ∼2.5 % of the total catalytic current density at 0.55 V vs. Ag/AgCl and the direct oxidation of MEA ranks the rest ∼97.5 %. To decrease the onset potential of MEA oxidation, a photoelectric-catalytic system including high-efficient Ni-based photoelectric-catalyst, where Ni is intimately coated on TiO2 by in-situ photodeposition to achieve the shortest carrier transport channel between Ni(OH)2 and TiO2, is developed. Results show the overpotential of MEA electrooxidation under illumination significantly drops to 255 mV. Such a Ni@TiO2/FTO electrode also exerts excellent durability toward MEA oxidation.
摘要：
Accelerated eutrophication in lakes reduces the number of submerged macrophytes and alters the residues of glyphosate and its degradation products. However, the effects of submerged macrophytes on the fate of glyphosate remain unclear. We investigated eight lakes with varying trophic levels along the middle and lower reaches of the Yangtze River in China, of which five lakes contained either glyphosate or aminomethylphosphate (AMPA). Glyphosate and AMPA residues were significantly positively correlated with the trophic levels of lakes (P<0.01). In lakes, glyphosate is degraded through the AMPA and sarcosine pathways. Eight shared glyphosate-degrading enzymes and genes were observed in different lake sediments, corresponding to 44 degrading microorganisms. Glyphosate concentrations in sediments were significantly higher in lakes with lower abundances of soxA (sarcosine oxidase) and soxB (sarcosine oxidase) (P<0.05). In the presence of submerged macrophytes, oxalic and malonic acids secreted by the roots of submerged macrophytes increased the abundance of glyphosate-degrading microorganisms containing soxA or soxB (P<0.05). These results revealed that a decrease in the number of submerged macrophytes in eutrophic lakes may inhibit glyphosate degradation via the sarcosine pathway, leading to a decrease in glyphosate degradation and an increase in glyphosate residues.
通讯机构：
[Peng, X ] C;[Quan, FJ ] W;Wuhan Polytech Univ, Sch Chem & Environm Engn, Wuhan 430023, Peoples R China.;Cent China Normal Univ, Inst Environm & Appl Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
摘要：
Recently, researchers have been paying much attention to zero-valent iron (ZVI) in the field of pollution remediation. However, the depressed electron transport from the iron reservoir to the iron oxide shell limited the wide application of ZVI. This study was aimed at promoting the performance of microscale ZVI (mZVI) for hexavalent chromium (Cr(vi)) removal by accelerating iron cycle with the addition of boron powder. It was found that the addition of boron powder enhanced the Cr(vi) removal rate by 2.1 times, and the proportion of Cr(iii) generation after Cr(vi) removal process also increased, suggesting that boron could promote the reduction pathway of Cr(vi) to Cr(iii). By further comparing the Cr(vi) removal percentage of Fe(iii) with or without the boron powder, we found that boron powder could promote the percentage removal of Cr(vi) with Fe(iii) from 10.1% to 33.6%. Moreover, the presence of boron powder could decrease the potential gap values (ΔE(p)) between Fe(iii) reduction and Fe(ii) oxidation from 0.668 V to 0.556 V, further indicating that the added boron powder could act as an electron sacrificial agent to promote the reduction process of Fe(iii) to Fe(ii), and thus enhancing the reduction of Cr(vi) with Fe(ii). This study shed light on the promoted mechanism of Cr(vi) removal with boron powder and provided an environmentally friendly and efficient approach to enhance the reactivity of the mZVI powder, which would benefit the wide application of mZVI technology in the environmental remediation field.
摘要：
In this work, the Mn, Co, Ce co-doped corn cob biochar (MCCBC) as catalytic particle electrodes in a three-dimensional heterogeneous electro-Fenton-like (3D-HEFL) system for the efficient degradation of coking wastewater was investigated. Various characterization methods such as SEM, EDS, XRD, XPS and electrochemical analysis were employed for the prepared materials. The results showed that the MCCBC particle electrodes had excellent electrochemical degradation performances of COD in coking wastewater, and the COD removal and degradation rates of the 3D/HEFL system were 85.35% and 0.0563 min(-1) respectively. RSM optimized conditions revealed higher COD removal rate at 89.23% after 31.6min of electrolysis. The efficient degradability and wide adaptability of the 3D/HEFL system were due to its beneficial coupling mechanism, including the synergistic effect between the system factors (3D and HEFL) as well as the synergistic interactions between the ROS (dominated by •OH and supplemented by O(2)(•-)) in the system. Moreover, the COD removal rate of MCCBC could still remain at 81.41% after 5 cycles with a lower ion leaching and a specific energy consumption of 11.28 kWh kg(-1) COD. The superior performance of MCCBC, as catalytic particle electrodes showed a great potential for engineering applications for the advanced treatment of coking wastewater.
