期刊：
Journal of Environmental Chemical Engineering,2023年11(3):109704 ISSN：2213-3437
通讯作者：
Meifang Li<&wdkj&>Ping Wang
作者机构：
College of Environmental Science and Engineering, Central South University of Forestry and Technology, Shaoshan South Road, Tianxin, Changsha 410004, PR China;Faculty of Life Science and Technology, Central South University of Forestry and Technology, Shaoshan South Road, Tianxin, Changsha 410004, PR China;[Wu, Shaohua] Guangdong Provincial Key Laboratory of Petrochemical Pollution Processes and Control, Key Laboratory of Petrochemical Pollution Control of Guangdong Higher Education Institutes, School of Environmental Science and Engineering, Guangdong University of Petrochemical Technology, Maoming, Guangdong 525000, PR China;College of Environmental Science and Engineering, Hunan University, Lushan South Road, Yuelu, Changsha 410082, PR China;Key Laboratory of Environmental Biology and Pollution Control, Ministry of Education, Hunan University, Lushan South Road, Yuelu, Changsha 410082, PR China
通讯机构：
[Meifang Li; Ping Wang] C;College of Environmental Science and Engineering, Central South University of Forestry and Technology, Shaoshan South Road, Tianxin, Changsha 410004, PR China<&wdkj&>Faculty of Life Science and Technology, Central South University of Forestry and Technology, Shaoshan South Road, Tianxin, Changsha 410004, PR China
摘要：
Tetracycline (TCN) is a typical antibiotic with ecological toxicity, which is easy to cause bacterial drug resistance. Single-atom catalysts have a broad application prospect in the remediation of antibiotic polluted water by activated persulfate (PDS), but its catalytic properties are limited because of its high surface energy and easy aggregation. Therefore, in our manuscript, a novel nitrogen doped magnetic graphene oxide confined Fe-Co dual single-atom catalyst (Fe/Co(1:1)(S)-NMGO) was prepared by one-step molten salt assisted high temperature pyrolysis. XPS and AC-HAADF-STEM analysis indicated single-atom Fe and Co existed. Fe and Co atoms were bound to the material mainly through coordination with pyridinic N and pyrrolic N. While single-atom Fe and Co were simultaneously introduced into the modified materials, the removal rate of TCN reached 93.1%, implying the significant synergistic effect of single-atom Fe and Co on TCN removal. Molten salt assisted high-temperature pyrolysis significantly improved the TCN degradation rate. In addition, this research showed that the existence of magnetite nanoparticles was beneficial to improve the separation performance of the single-atom catalysts as well as the catalytic performance. At the same time, the effects of some key parameters (Fe/Co molar ratio, catalyst dosage, PDS dosage, initial pH, coexisting anions and humic acids) on TCN degradation in Fe/Co(1:1)(S)-NMGO/PDS system were also investigated. The catalytic potential in actual water and regeneration performance of the material were also evaluated. The possible activation mechanism and degradation pathway of TCN were proposed. These findings will provide important reference for the future design and application of single-atom-involved catalysts.
作者机构：
[Liu, Yuwei; Lin, Baining; Luo, Lukai; Liu, Hongyang; Zhou, Yonghua] Cent South Univ, Coll Chem & Chem Engn, Changsha 410083, Peoples R China.;[Wang, Hanqing; Wang, Ping; Mao, Yu] Cent South Univ Forestry & Technol, Coll Environm Sci & Engn, Hunan Engn Res Ctr Full Life Cycle Energy Efficien, Changsha 410004, Peoples R China.
关键词：
boron defects;direct dehydrogenation of ethylbenzene;metal-free catalysis;phosphorus doped boron nitride;styrene
摘要：
Ethylbenzene dehydrogenation: The m‐PBN with the optimal concentration of B defects improved the styrene production rate to 22.54 mmolST g−1 h−1. Meanwhile, when it was further in‐situ grown on Al2O3, the styrene production rate increased to 23.22 mmolST g−1 h−1 and stably run for more than 300 h. Abstract Phosphorus‐doped boron nitride (PBN) has been confirmed as an effective metal‐free catalyst for the direct dehydrogenation (DDH) of ethylbenzene to styrene. In this paper, we further used barbituric acid as co‐reactant sources to create B defects in both PBN and mesoporous PBN (m‐PBN) materials. The XPS, N2 adsorption‐desorption, UV‐vis DRS, EPR, 11B SS NMR characterizations indicated both the electronic and pore structures of the catalyst with B defects were adjusted. Except for the improvement of mass transfer caused by B defects, DFT calculations showed the increase of electron density in B defects areas could enhance the breaking of C−H in ethylbenzene and the bond‐forming of H−H, which was acted to improve the catalytic activity. The m‐PBN with B defects delivered the styrene production rate of 22.54 mmolST g−1 h−1 and stably run 300 h when in‐situ grown on Al2O3, proving that defect tuning strategy is useful to construct efficient catalysts for styrene production.
关键词：
Constructed wetland;Nitrogen removal;Tidal flow;Macroporous zeolite spheres;Microbial structure and function
摘要：
Tidal flow constructed wetlands (TFCWs) enhance the process of microbial denitrification, while, the influence of substrate pore structure on denitrification are not clear. Herein, we prepare macroporous zeolite ball (MZ) by pore construction technique, and equipped as substrate in TFCWs, to explore the influence of MZ on the structure and function of microbial community. Results show ed that MZ has porous morphology both on the surface and inside. The removal rate of NH4+-N was 12% higher than that of the control. Surface characteristics of MZ provided more attachment sites for microorganisms. BugBase phenotypic and FAPROTAX prediction results showed that MZ had a wider ecological niche, and aerobic bacteria and anaerobic bacteria coexisted on the surface, the main denitrification functional bacteria are Massilia, Pseudarthrobacter, Hydrogenophaga, Acidovorax and Pseudomonas. This study is conducive for improving the purification efficiency of constructed wetland.
作者机构：
[王子钰; 周航; 周坤华; 谭文韬; 蒋毅; 唐棋; 伍港繁; 辜娇峰; Zeng, Peng; 廖柏寒] College of Environment Science and Engineering, Central South University of Forestry and Technology, Changsha;410004, China;Hunan Engineering Laboratory for Control of Rice Quality and Safety, Changsha;State Ecology Environment Key Laboratory of Monitoring for Heavy Metal Pollutants, Changsha;410019, China
作者机构：
[王文禹; 彭佩钦; 欧阳晴雯; 龙坚; 李耀; 侯红波; 郝汉驰; 黄奕航] College of Environmental Science and Engineering, Central South University of Forestry and Technology, Changsha 410004, China;[彭佩钦; 龙坚; 侯红波] Hunan Engineering Laboratory for Control of Rice Quality and Safety, Changsha 410004, China
摘要：
The introduction of iodide (I(-)) has broad perspectives on the decomposition of perfluorocarboxylates (PFCAs, C(n)F(2n+1)COO(-)). However, the iodinated substances produced are highly toxic synthetic chemicals, hence, it is urgent to find a similar alternative with less toxicity. In this work, the defluorination of perfluorooctanoic acid (PFOA) by I(-), bromide (Br(-)) and chlorine (Cl(-)) was systematically compared in the VUV/sulfite process. Results indicated that the PFOA defluorination rates increased with increasing nucleophilicity of halogens (I > Br > Cl). Meanwhile, the introduction of I(-), Br(-), and Cl(-) reduced the interference of the coexisting water matrix on the degrading influence of PFOA. The in situ produced e(aq)(-), SO(3)(•-), H•, and HO• were recognized, among the addition of I(-) maximized the relative contribution of e(aq)(-) but Br(-) and Cl(-) decreased that of H• and other radicals. Additionally, HPLC/MS analysis revealed the presence of I(-), Br(-), and Cl(-) had a vital impact on the difference in product concentrations, while they had a negligible effect on the change in the pathway of degradation. Overall, this study demonstrated the similarities and differences between I(-), Br(-), and Cl(-), which has significant implications for further understanding VUV/sulfite degradation.
通讯机构：
[Hu, XJ ] C;Cent South Univ Forestry & Technol, Coll Environm Sci & Engn, Changsha 410004, Peoples R China.
关键词：
Porous C 3 N 5 nanosheets;Temperature modulation;Photocatalysts;Microcystis-LR;Degradation
摘要：
Microcystin pollution of the environment is a prevalent problem that has gained considerable attention in sustainable development. Photocatalytic degradation is one of the most efficient ways to address this environmental issue. In this study, a porous C3N5 carbon nitride nanosheet (NCN) with high photocatalytic activity was prepared using 3-amino-1,2,4-triazole as the raw material by a simple and environmentally friendly stepwise pyrolysis technique. The morphology, microstructure, chemical composition, and optoelectronic properties of the materials were analyzed by characterization (SEM, TEM, XRD, FI-IR, XPS, UV-vis, PL, Etc.). The specific surface area and charge mobility of NCN were both increased by the porous structure. The specific surface area of NCN was 4.95 times greater than that of CN-650, and it has a narrower band gap and a broader visible absorption range. The degradation rate of microcystin-LR by NCN, driven by visible light, reached 99.99% at 45 min, and the degradation kinetic constant was 9.09 times that of its precursor. Singlet oxygen (1O2) plays the most crucial role in the photocatalytic degradation of MC-LR by NCN. In addition, possible degradation pathways were sought by studying the intermediates of the MC-LR photodegradation process. The NCN photocatalysts developed in this work provide a wide range of possibilities for photocatalyst design and the mechanistic analysis of photocatalytic degradation of microcystins.
摘要：
The frequent occurrence of algal blooms in water bodies leads to a significant accumulation of microcystin-LR (MC-LR). In this study, we developed a porous foam-like self-floating N-deficient g-C(3)N(4) (SFGN) photocatalyst for efficient photocatalytic degradation of MC-LR. Both the characterization results and DFT calculations indicate that the surface defects and floating state of SFGN synergistically enhance light harvesting and photogenerated carrier migration rate. The photocatalytic process achieved a nearly 100% removal rate of MC-LR within 90min, while the self-floating state of SFGN maintained good mechanical strength. ESR and radical capture experiments revealed that the primary active species responsible for the photocatalytic process was OH. This finding confirmed that the fragmentation of MC-LR occurs as a result of OH attacking the MC-LR ring. LC-MS analysis indicated that majority of the MC-LR molecules were mineralized into small molecules, allowing us to infer possible degradation pathways. Furthermore, after four consecutive cycles, SFGN exhibited remarkable reusability and stability, highlighting the potential of floating photocatalysis as a promising technique for MC-LR degradation.
摘要：
Exposure to even trace amounts of Cd(II) and Pb(II) in food can have serious effects on the human body. Therefore, the development of novel electrochemical sensors that can accurately detect the different toxicity levels of heavy metal ions in food is of great significance. Based on the principle of green chemistry, we propose a new type of boron and nitrogen co-doped carbon (BCN) material derived from a metal-organic framework material and study its synthesis, characterization, and heavy-metal ion detection ability. Under the optimum conditions, the BCN-modified glassy carbon electrode was studied using square-wave anodic stripping voltammetry, which showed good electrochemical responses to Cd(II) and Pb(II), with sensitivities as low as 0.459 and 0.509 μA/μM cm(2), respectively. The sensor was successfully used to detect Cd(II) and Pb(II) in Beta vulgaris var. cicla L samples, which is consistent with the results obtained using inductively coupled plasma-mass spectrometry. It also has a strong selectivity for complex samples. This study provides a novel approach for the detection of heavy metal ions in food and greatly expands the application of heteroatom-doped metal-free carbon materials in detection platforms.
摘要：
Biochar derived from bamboo was used to support sulfide nanoscale zero-valent iron (S-nZVI@BC) for simultaneous removal of Cd(II) and As (III) from aqueous media. Scanning electron microscopy (SEM) and X-ray diffraction spectroscopy (XRD) characterization confirmed the successful synthesis of the S-nZVI@BC. Adsorption kinetics and isotherms indicated that co-adsorption of Cd(II) and As(III) onto S-nZVI@BC was well represented by pseudo-second-order model (R(2)(Cd(II))=0.990, R(2)(As(III))=0.995) and Langmuir model (R(2)(Cd(II))=0.954, R(2)(As(III))=0.936). The maximum adsorption was 162.365 and 276.133mg/g for Cd(II) and As(III), respectively, in a co-adsorption system, which was significantly higher than that in a single adsorption system (103.195 and 223.736mg/g, respectively). Batch experiments showed that the Cd(II)-to-As(III) concentration ratio significantly affected the co-adsorption with the optimal ratio of 1:2. Ca(2+) and Mg(2+) significantly inhibited Cd(II) removal. In contrast, phosphate and humic acid significantly inhibited As(III) removal. Electrochemical analysis indicated S-nZVI@BC had a lower corrosion potential and resistance than nZVI@BC, making it more conducive to electron transfer and chemical reaction. Electrostatic adsorption, complexation, co-precipitation, and redox were the primary mechanisms for Cd(II) and As(III) removal. Overall, the present study provides new insights into the synergistic removal of Cd(II) and As(III) by S-nZVI@BC, which is a very promising adsorbent for the effective removal of Cd(II) and As(III) from contaminated wastewater.
通讯机构：
[Chao Huang; Jian Zhu] C;College of Environmental Science and Engineering, Central South University of Forestry and Technology, Changsha, 410004, China
关键词：
Molybdenum carbide (Mo2C);Co-catalyze;Hydrogen peroxide (H2O2);Fenton process
摘要：
Commercial molybdenum carbide (Mo2C) and ferrous iron (Fe2+) were investigated for the first time to co-catalyze the activation of H2O2 for the treatment of organic contaminants. Compared with traditional Fenton process, the presence of Mo2C decomposed hydrogen peroxide (H2O2) more effectively and accelerated the conversion of Fe3+/Fe2+. The Rhodamine B (RhB) degradation rate constant in Mo2C/Fe2+/H2O2 reached appropriately three times that in Fe2+/H2O2, and the co-catalytic reactivity of Mo2C was significantly higher than that of MoS2. In addition, (MoC)-C-2/Fe2+/H2O2 exhibited a board effective pH range of 2.8-8.8, and four-cycle experiments confirmed the stability and reusability of Mo2C. The results of X-ray photoelectron spectroscopy (XPS) indicated that Mo(II) and Mo(IV) played major roles in Fe3+ reduction. Electron Paramagnetic Resonance analysis and quenching experiments demonstrated that hydroxyl radical (.OH), superoxide anion radical (O-2(-)) and singlet oxygen radical (O-1(2)) were all involved in Mo2C/Fe2+/H2O2. Particularly, Mo2C/Fe2+/H2O2 signifi-cantly enhanced the generation of .OH and O-1(2) in comparison to Fe2+/H2O2. Moreover, toxicity assessment analysis by ECOSAR suggested that the toxicity of most degradation products of RhB decreased after treatment. Overall, this study offers a promising Mo2C co-catalyzed Fenton process for rapid and efficient abatement of organic contaminants.
期刊：
Chemical Engineering Journal,2023年471:144517 ISSN：1385-8947
通讯作者：
Li, LQ;Su, RK
作者机构：
[Ma, Xiancheng] Cent South Univ Forestry & Technol, Coll Mech & Elect Engn, Changsha 410083, Hunan, Peoples R China.;[Li, Liqing; Li, LQ; Zeng, Zheng] Cent South Univ, Sch Energy Sci & Engn, Changsha 410083, Hunan, Peoples R China.;[Su, Rongkui; Wang, Hanqing; Su, RK] Cent South Univ Forestry & Technol, Coll Environm Sci & Engn, Changsha 410083, Hunan, Peoples R China.;[Wang, Shaobin] Univ Adelaide, Sch Chem Engn & Adv Mat, Adelaide, SA 5005, Australia.
通讯机构：
[Li, LQ ; Su, RK ] C;Cent South Univ, Sch Energy Sci & Engn, Changsha 410083, Hunan, Peoples R China.;Cent South Univ Forestry & Technol, Coll Environm Sci & Engn, Changsha 410083, Hunan, Peoples R China.
关键词：
Wood-based evaporator;Interfacial water evaporation;Solar energy;Structural design
摘要：
Solar water evaporation plays an important role in the production of low-energy freshwater, which is essential for economic development and human health. The use of solar powered green water evaporation technology has attracted more and more attention as a sustainable solution to water shortage and environmental governance. Among photothermal materials, wood-based photothermal evaporators have attracted researchers' interest because of their abundance, low cost, biodegradability, low thermal conductivity, hydrophilicity and natural capillary mechanism. In this review, we first summarized the advantages of wood-based solar evaporators, including pore structure and chemical structure. Secondly, the latest progress of wood-based solar evaporators is summarized from the aspects of photothermal material decorative wood, carbonized wood, structural design, etc., and the recent progress in the application of wood evaporators in seawater desalination, wastewater purification and energy production were discussed. Finally, the scientific and technical challenges facing the application of wood-based solar evaporators, and future research directions in this field are outlined.
期刊：
Journal of Colloid and Interface Science,2023年646:67-77 ISSN：0021-9797
通讯作者：
Li, LQ;Su, RK
作者机构：
[Ma, Xiancheng; Qi, Tingting] Cent South Univ Forestry & Technol, Coll Mech & Elect Engn, Changsha 410004, Hunan, Peoples R China.;[Li, Liqing; Li, LQ; Zeng, Zheng] Cent South Univ, Sch Energy Sci & Engn, Changsha 410083, Hunan, Peoples R China.;[Su, Rongkui; Su, RK] Cent South Univ Forestry & Technol, Coll Environm Sci & Engn, Changsha 410083, Hunan, Peoples R China.;[Chen, Ruofei] Zhongkai Univ Agr & Engn, Sch Electromech Engn, Guangzhou 510225, Guangdong, Peoples R China.;[Wang, Shaobin] Univ Adelaide, Sch Chem Engn & Adv Mat, 108 King William St, Adelaide, SA 5005, Australia.
通讯机构：
[Li, LQ ; Su, RK ] C;Cent South Univ, Sch Energy Sci & Engn, Changsha 410083, Hunan, Peoples R China.;Cent South Univ Forestry & Technol, Coll Environm Sci & Engn, Changsha 410083, Hunan, Peoples R China.
关键词：
Acetone adsorption;Grand canonical Monte Carlo;Oxygen groups;Pore sizes;Porous carbon
摘要：
The influence of different pore size and oxygen groups for porous carbons on acetone adsorption at different pressure was studied by using experimental data and theoretical calculation, and the results were applied to prepare carbon-based adsorbents with superior adsorption capacity. First, we successfully prepared five types of porous carbons with different gradient pore structure but similar oxygen contents (4.9±0.25 at.%). We found that the acetone uptake at different pressure depends on the different pore sizes. Besides, we demonstrate how to accurately decompose the acetone adsorption isotherm into multiple sub-isotherms based on different pore sizes. Based on the isotherm decomposition method, the acetone adsorption at 18kPa is mainly in the form of pore-filling adsorption in the pore size range of 0.6-2.0nm. When the pore size is greater than 2nm, the acetone uptake mainly depends on the surface area. Second, porous carbons with different oxygen content, similar surface area and pore structure were prepared to study the influence of oxygen groups on acetone adsorption. The results show that the acetone adsorption capacity is determined by the pore structure at relatively high pressure, and the oxygen groups only slightly increase the adsorption capacity. However, the oxygen groups can provide more active sites, thereby enhancing acetone adsorption at low pressure.
摘要：
Although graphitic carbon nitride (g-C3N4) is frequently mentioned as an environmentally friendly and low-cost photocatalyst, its photocatalytic efficiency is severely constrained by its greater band gap and easy recombination of photogenerated carriers. Introducing nitrogen defects into the photocatalyst can effectively improve the photocatalytic efficiency of g-C3N4. As the position and concentration of inserted nitrogen defects are important factors affecting the catalytic performance of g-C3N4, this review summarized the synthesis methods developed in recent years based on the perspective of the regulation of nitrogen defect position and concentration. Additionally, this study provided an overview of the characterization methods for discovering nitrogen defects and accurately identifying their exact positions in g-C3N4. At the same time, the mechanism of nitrogen defects promoting the photocatalytic performance of g-C3N4 was explored from aspects such as enhancing light absorption, promoting the transfer and separation of photogenerated carriers, and increasing the consumption of photogenerated carriers through surface reactions. Finally, the opportunities and challenges of nitrogen defects in identification, synthesis, and mechanism of action were discussed.
摘要：
In this work, the regeneration of spent biochar adsorbent and the degradation of adsorbed PFOA by the system of ultrasonic assisted activation of persulfate were explored. The effects of ultrasound, persulfate and biochar on PFOA removal were investigated through a series of regeneration and degradation experiments. Meanwhile, the degradation mechanism and reaction pathways of PFOA were investigated with electron paramagnetic resonance (EPR) and high-resolution quadrupole orbitrap mass spectrometer. The results showed that PFOA adsorbed by biochar could be degraded efficiently with the synergistic effect of ultrasound and persulfate. The degradation of PFOA in biochar could be finished in 4 h, while the defluorination took longer, with a defluorination efficiency of 50.6% after 4 h and 99.6% after 10 h. In this process, PFOA was degraded and defluorinated gradually by thermal decomposition caused by cavitation bubbles and degradation caused by the attack of SO4 center dot(-) and center dot OH. Two different free radicals controlled different degradation pathways, with SO4 center dot(-) playing a dominant role. In this system, the regeneration of the waste biochar adsorbent was achieved by eliminating PFOA, which could be recycled more than three times. The application potential of the system was evaluated using real water sample, and it was found that the removal of PFOA in real water sample was satisfactory even with the influence of inorganic ions and organic matter, indicating that it has promising application prospects. This work provided new insight into the degradation of adsorbed PFOA and adsorbent regeneration.
期刊：
Separation and Purification Technology,2023年326:124842 ISSN：1383-5866
通讯作者：
Wang, Hui;Hu, XJ
作者机构：
[Hu, Xi; Jiang, Honghui; Hu, Zhenxin; Ouyang, Yuanhao; Hu, Xinjiang; Ouyang, Ke; Wang, Hui; Ji, Xiaodong; Wang, Ping] Cent South Univ Forestry & Technol, Coll Environm Sci & Engn, Changsha 410004, Peoples R China.;[Li, Tingting] Liaocheng Univ, Coll Environm & Planning, Liaocheng 252059, Peoples R China.;[Wang, Hui; Hu, Xinjiang] Cent South Univ Forestry & Technol, Changsha, Peoples R China.
通讯机构：
[Wang, H; Hu, XJ ] C;Cent South Univ Forestry & Technol, Changsha, Peoples R China.
关键词：
Biochar;Peroxymonosulfate;Thiamethoxam;Cadmium sulfide;Density functional theory calculation
摘要：
Mounting evidence highlights the negative impacts of thiamethoxam (THM) on non-target organisms and ecosystem. Herein, multi-phase cadmium sulfide loaded on biochar (CdS@BC) was used to photocatalytic activate peroxymonosulfate (PMS) to remove THM. The obtained CdS@BC significantly improved the photocatalytic performance of PMS on THM degradation with a superior rate constant of 0.165 min-1, 60 times more than that of BC. In addition, the catalyst displayed excellent stability and reusability. The mechanism of free radical formation by adsorption activation of PMS adsorbed on CdS@BC was characterized using active species detection and Density functional theory (DFT) calculations. According to the DFT study, the phase junction and & pi;-conjugated structure contribute to the stable migration of & pi;-electrons, thus effectively activating the PMS to produce active substances for the degradation of THM. The findings provide a theoretical basis for the design and synthesis of effective catalysts for AOPs to remove emerging organic contaminants from wastewater.
摘要：
“Alto2” is a new biomass sorghum variety, which has the characteristics of fast growth, high growth, and strong cadmium (Cd) resistance, so it has the application prospect of soil remediation plants. In order to reveal the Cd resistance mechanism of this plant and pave the way for genetic breeding and cultivation of efficient remediation plants in the future, in this research, through the determination of Cd content in various tissues of sorghum under Cd stress and the physicochemical response combined with RNA-Seq analysis, the mechanism of Cd resistance of “Alto2” was initially revealed. The results show biomass sorghum “Alto2” was mainly connected with aboveground and underground parts through the MAPK signaling pathway and plant hormone signaling pathway, and transmit stress signal in response to Cd stress. Chelase and metal-binding proteins may be the functional genes mainly responsible for Cd enrichment and transport and regulated by stress signals. However, the expression of aboveground transporters was not significant. This may be because Cd in biomass sorghum is mainly concentrated in the underground part and is enriched by the chelation of secondary metabolites from plant roots by the cell wall leading to inhibition of aboveground transporter expression. The results of this study indicate that the biomass sorghum “Alto2” on Cd has high resistance, but the lack of the aboveground enrichment of transportability requires further research to improve the Cd transportability of this plant.
