Simplified creation of polyester fabric supported Fe-based MOFs by an industrialized dyeing process: Conditions optimization, photocatalytics activity and polyvinyl alcohol removal

MIL-53(Fe) was successfully prepared and deposited on the surface carboxylated polyester (PET) fiber by an optimized conventional solvothermal or industrialized high temperature pressure exhaustion (HTPE) process to develop a PET fiber supported MIL-53(Fe) photocatalyst ([email protected]) for the degradation of polyvinyl alcohol (PVA) in water under light emitting diode (LED) visible irradiation. On the basis of several characterizations, [email protected] was tested for the photocalytic ability and degradation mechanism. It was found that temperature elevation significantly enhanced the formation and deposition of MIL-53(Fe) with better photocatalytic activity. However, higher temperature than 130°C was not in favor of its photocatalytic activity. Increasing the number of surface carboxyl groups of the modified PET fiber could cause a liner improvement in MIL-53(Fe) loading content and photocatalytic ability. High visible irradiation intensity also dramatically increased photocatalytic ability and PVA degradation efficiency of [email protected] Na₂S₂O₈ was used to replace H₂O₂ as electron acceptor for further promoting PVA degradation in this system. [email protected] prepared by HTPE process showed higher MIL-53(Fe) loading content and slightly lower PVA degradation efficiency than that prepared by solvothermal process at the same conditions. These findings provided a practical strategy for the large-scale production of the supported MIL-53(Fe) as a photocatalyst in the future.     

Monodisperse amino-modified nanosized zero-valent iron for selective and recyclable removal of TNT: Synthesis, characterization, and removal mechanism

Nitroaromatic explosives are major pollutants produced during wars that cause serious environmental and health problems. The removal of a typical nitroaromatic explosive, 2,4,6-trinitrotoluene (TNT), from aqueous solution, was conducted using a new recyclable magnetic nano-adsorbent ([email protected]₂NH₂). This adsorbent was prepared by grafting amino groups onto [email protected]₂ particles with a well-defined core-shell structure and demonstrated monodispersity in solution. The removal performance of the nano-adsorbent towards TNT was found to be 2.57 and 4.92 times higher than that towards two analogous explosives, 2,4-dinitrotoluene (2,4-DNT) and 2-nitrotoluene (2-NT), respectively, under neutral conditions. The difference in the removal performance among the three compounds was further compared in terms of the effects of different conditions (pH value, ionic strength, humic acid concentration, adsorbent modification degree and dosage, etc.) and the electrostatic potential distributions of the three compounds. The most significant elevation is owing to modification of amino on [email protected]₂ which made a 20.7% increase in adsorption efficiency of TNT. The experimental data were well fit by the pseudo-second-order kinetic model and the Freundlich adsorption isotherm model, indicating multilayer adsorption on a heterogeneous surface. The experimental results and theoretical considerations show that the interactions between [email protected]₂NH₂ NPs and TNT correspond to dipole-dipole and hydrophobic interactions. These interactions should be considered in the design of an adsorbent. Furthermore, the adaptability to aqueous environment and excellent regeneration capacity of [email protected]₂NH₂ NPs makes these remediation materials promising for applications.     

Nickel phosphide on Ni foam as anode and peroxymonosulfate as the chemical oxidizer for effective direct urea fuel cell

The direct urea fuel cell (DUFC) is a low cost and competitive approach for contemporaneous urine or urea-contaminated wastewater treatment and electricity generation. However, the lack of efficient urea oxidation reaction (UOR) electrocatalysts and suitable electron acceptors remains a challenge for practical applications. Here, we developed a DUFC system using Ni₂[email protected] foam as the anode and peroxymonosulfate (PMS) as the chemical oxidizers. The Ni₂[email protected] foam anode showed a high oxidation activity for UOR with an onset potential of 0.30 V vs. Ag/AgCl and Tafel slope of 34.4 mV/dec. PMS with high theoretical potential improved the cell voltage to 1.43 V. A power density of DUFC up to 4.91 mW/cm² was achieved using PMS at room temperature, which was approximately twice as high as using H₂O₂ (2.38 mW/cm²). Ni^II/Ni^III was the redox active species on the Ni₂P anode in the DUFC process, and Ni^II was electrochemically oxidized to Ni^III, which reverted to Ni^II by urea reduction. When real human urine was used as the fuel, a power density of 4.46 mW/cm² can be achieved at room temperature. This DUFC with high cell performance showed potential application in urea wastewater treatment.     

Efficient and recyclable palladium enriched magnetic nanocatalyst for reduction of toxic environmental pollutants

In this paper, highly stable, powerful, and recyclable magnetic nanoparticles tethered N-heterocyclic carbene-palladium(II) ((CH₃)₃[email protected]₃O₄) as magnetic nanocatalyst was successfully synthesized from a simplistic multistep synthesis under aerobic conditions through easily available low-cost chemicals. Newly synthesized (CH₃)₃[email protected]₃O₄ magnetic nanocatalyst was characterized from various analytical tools and catalytic potential of the (CH₃)₃[email protected]₃O₄ magnetic nanocatalyst was studied for the catalytic reduction of toxic 4-nitrophenol (4-NP), hexavalent chromium (Cr(VI)), Methylene Blue (MB) and Methyl Orange (MO) at room temperature in aqueous media. UV-Visible spectroscopy was employed to monitor the reduction reactions. New (CH₃)₃[email protected]₃O₄ magnetic nanocatalyst exhibited excellent catalytic activity for the reduction of toxic environmental pollutants. Moreover, (CH₃)₃[email protected]₃O₄ magnetic nanocatalyst could be easily and rapidly separated from the reaction mixture with the help of an external magnet and recycled minimum five times in reduction of 4-NP, MB, MO and four times in Cr(VI) without significant loss of catalytic potential and remains stable even after reuse.     

MIL-88A@MIP催化活化过硫酸盐靶向降解邻苯二甲酸二丁酯

本实验首次合成了以金属有机骨架MIL-88A作为前驱体,采用分子印迹法改性后的催化剂MIL-88A@MIP,并通过X射线衍射仪(XRD),扫描电镜(SEM)以及EDS能谱和氮气吸附对催化剂进行表征分析.以造纸废水中邻苯二甲酸二丁酯(DBP)作为目标污染物,探究该催化剂活化过硫酸盐(PS)产生SO_4~-·的能力.对比前驱体MIL-88A,靶向改性有效地提高了MIL-88A@MIP的催化活性,在反应480 min后,DBP的去除率高达80.4%.影响因素实验表明该催化剂的最佳活化条件为:PS∶DBP=600∶1、MIL-88A@MIP投加量0.5 g·L~(-1)、体系中pH为3.26.此外,探究了MIL-88A@MIP对于催化PS降解不同污染物的能力,其结果表明该催化剂对于邻苯二甲酸酯类(PAEs)物质均有降解效果,体现了其靶向选择性.     

金属有机骨架MIL-68(Al)对水中典型荧光增白剂VBL的吸附去除

以金属有机骨架材料MIL-68(Al)为吸附剂,探究其对水中典型荧光增白剂VBL分子的吸附行为.采用粉末X射线衍射仪(XRD)、傅里叶变换红外光谱(FTIR)、场发射扫描电镜(SEM)及N_2吸附脱附对MIL-68(Al)的结构性质进行表征.探讨了p H值、离子强度、污染物初始浓度、反应温度及吸附时间对MIL-68(Al)吸附去除水中VBL的影响,并对吸附等温线、动力学、热力学及吸附机制进行了分析.实验结果表明,MIL-68(Al)对VBL的吸附能适应较宽的p H范围,吸附等温线符合Langmuir模型,最大吸附容量达到400.02 mg·g~(-1);吸附速率在前20 min很快,并且能在180 min达到吸附平衡,吸附动力学符合准二级动力学模型;吸附过程是吸热反应,吸附自发进行并且主要由熵驱动;静电作用和氢键作用对吸附均有贡献,静电作用是吸附发生的主要机制.由以上结果可知,MIL-68(Al)是一种潜在的高效吸附剂,在去除水中的VBL分子方面极具潜力.     

Progress of environmental research in China from 2000 to 2019: Case studies of JES and ES&T

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Current status of applying microwave-associated catalysis for the degradation of organics in aqueous phase – A review

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In situ preparation of g-C3N4/Bi4O5I2 complex and its elevated photoactivity in Methyl Orange degradation under visible light

A graphite carbon nitride(g-C_3N_4) modified Bi_4O_5I_2 composite was successfully prepared insitu via the thermal treatment of a g-C_3N_4/Bi OI precursor at 400°C for 3 hr.The as-prepared g-C_3N_4/Bi_4O_5I_2 showed high photocatalytic performance in Methyl Orange(MO) degradation under visible light.The best sample presented a degradation rate of 0.164 min~(-1),which is 3.2 and 82 times as high as that of Bi_4O_5I_2 and g-C_3N_4,respectively.The g-C_3N_4/Bi_4O_5I_2 was characterized by X-ray powder diffractometer(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),Raman,X-ray photoelectron spectroscopy(XPS),ultraviolet-visible diffuse reflectance spectra(DRS),electrochemical impedance spectroscopy(EIS) and transient photocurrent response in order to explain the enhanced photoactivity.Results indicated that the decoration with a small amount of g-C_3N_4 influenced the specific surface area only slightly.Nevertheless,the capability for absorbing visible light was improved measurably,which was beneficial to the MO degradation.On top of that,a strong interaction between g-C_3N_4 and Bi_4O_5I_2 was detected.This interplay promoted the formation of a favorable heterojunction structure and thereby enhanced the charge separation.Thus,the g-C_3N_4/Bi_4O_5I_2 composite presented greater charge separation efficiency and much better photocatalytic performance than Bi_4O_5I_2.Additionally,g-C_3N_4/Bi_4O_5I_2 also presented high stability.·O_2~-and holes were verified to be the main reactive species.     

Robust magnetic laccase-mimicking nanozyme for oxidizing o-phenylenediamine and removing phenolic pollutants

In this study, we report a novel magnetic biomimetic nanozyme(Fe_3O_4@Cu/GMP(guanosine5′-monophosphate)) with high laccase-like activity, which could oxidize toxic ophenylenediamine(OPD) and remove phenolic compounds.The magnetic laccase-like nanozyme was readily obtained via complexed Cu~(2+)and GMP that grew on the surface of magnetic Fe_3O_4 nanoparticles.The prepared Fe_3O_4@Cu/GMP catalyst could be magnetically recycled for at least five cycles while still retaining above 70% activity.As a laccase mimic,Fe_3O_4@Cu/GMP had more activity and robust stability than natural laccase for the oxidization of OPD.Fe_3O_4@Cu/GMP retained about 90% residual activity at 90℃ and showed little change at pH 3–9, and the nanozyme kept its excellent activity after long-term storage.Meanwhile, Fe_3O_4@Cu/GMP had better activity for removing phenolic compounds, and the removal of naphthol was more than 95%.Consequently, the proposed Fe_3O_4@Cu/GMP nanozyme shows potential for use as a robust catalyst for applications in environmental remediation.     

Adsorption performance of CMK-3 and C-FDU-15 in NO removal at low temperature

CMK-3 and C-FDU-15 samples were synthesized using hard-templating and evaporationinduced self-assembly(EISA) methods,respectively.The pore structures of CMK-3 and CFDU-15 as well as commercial activated carbon were characterized by means of X-ray diffraction,field emission scanning electron microscopy,transmission electron microscopy,and N_2 adsorption–desorption.Adsorption of NO was investigated by means of thermogravimetric analysis,temperature-programmed desorption of NO + O_2,and in situ diffuse reflectance Fourier transform infrared spectroscopy.The results show that the CMK-3 and C-FDU-15 materials possessed ordered and uniform structures.The coadsorption capacity of NO and O_2 decreased in the sequence CMK-3(88.6 mg/g) C-FDU-15(71.7 mg/g) AC(25.3 mg/g).There were two main adsorption species on CMK-3 and CFDU-15:nitrite and nitrate.Nitrite is converted to nitrate easily.However,the adsorption species were more complex on AC,with nitrite being the main species.Moreover,CMK-3 and C-FDU-15 exhibit excellent regeneration efficiency compared with AC.The excellent NO adsorption performance of CMK-3 and C-FDU-15 was associated with their ordered mesoporous structures and high surface areas.The research provides more options for NO adsorption in the future.     

Self-feedback LSTM regression model for real-time particle source apportionment

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Assessing negative carbon dioxide emissions from the perspective of a national “fair share” of the remaining global carbon budget

We present an assessment of the plausible Paris-aligned fair share nett cumulative carbon dioxide (CO₂) quota for an example nation state, the Republic of Ireland. By Paris-aligned, we mean consistent with the Paris Agreement adopted at the 21st Conference of the Parties to the United Nations Framework Convention on Climate Change, at Paris, France, in December 2015 (UNFCCC 2015). We compare and contrast this quota with both the aspirations expressed in the current Irish National Policy Position and current national emission projections. The fair share quota is assessed as a maximum of c. 391 million tonnes of carbon dioxide (MtCO₂), equal to 83 tonnes of carbon dioxide (tCO₂) per capita, from 2015, based on a precautionary estimate of the global carbon budget (GCB) and specific interpretation of global equity. Given Ireland’s high current CO₂ per capita emission rate, this would correspond to sustained year-on-year reductions in nett annual CO₂ emissions of over ??11% per year (beginning as of 2016). By contrast, the CO₂ mitigation target indicated in the National Policy Position corresponds to nett annual reduction rates in the range of only ?4.7% per year (low ambition) up to a maximum of ??8.3% per year (high ambition), and projections based on current and immediately planned mitigation measures indicate the possibility, instead, of sustained increases in emissions at a rate of the order of +?0.7% per year. Accordingly, there is a large gap between Paris-aligned ambition and current political and policy reality on the ground, with a significant risk of early emergence of “CO₂ debt” and tacit reliance on rapid deployment of currently speculative (at a relevant scale and feasible cost) negative CO₂ emission technologies to actively remove CO₂ from the atmosphere. While the detailed policy situation will clearly differ from country to country, we suggest that this methodology, and its CO₂debt framing, may be usefully applied in other individual countries or regions. We recommend that such framing be incorporated explicitly into a global mitigation strategy via the statements of nationally determined contributions required to be submitted and updated by all parties under the Paris Agreement processes.

     

CuFeO2改性生物炭对四环素的吸附特性

利用共沉淀和水热法于生物炭（BC250、BC350、BC450、BC550和BC650）负载CuFeO₂,得到的复合材料对水中四环素（TC）具有较好的去除效果.CuFeO₂与BC450质量比为2 ：1的CuFeO₂改性生物炭（CuFeO₂/BC450=2 ：1）对TC的吸附性能最强.TC于CuFeO₂/BC450=2 ：1的吸附符合颗粒内扩散模型,表明吸附是界面和孔隙扩散控制的过程.在中性pH、298 K下,CuFeO₂/BC450=2 ：1对TC的Langmuir最大吸附量为82.8 mg ·g^-1,远大于BC450的13.7 mg ·g^-1和CuFeO₂的14.8 mg ·g^-1.热力学结果表明,CuFeO₂/BC450=2 ：1对TC的吸附是自发和吸热过程.随pH增加,CuFeO₂/BC450=2 ：1对TC的吸附去除呈先增加后降低的趋势,中性条件时效果最佳.CuFeO₂/BC450=2 ：1对TC的强吸附得益于CuFeO₂负载对材料孔隙结构的改善、比表面积的增大和表面官能团、电荷属性的改变.研究结果为净化抗生素污染提供了一种高效的磁性吸附剂.     

Removal of Ni(II) from strongly acidic wastewater by chelating precipitation and recovery of NiO from the precipitates

Strongly acidic wastewater produced in nonferrous metal smelting industries often contains high concentrations of Ni(II), which is a valuable metal. In this study, the precipitation of Ni(II) from strongly acidic wastewater using sodium dimethyldithiocarbamate (DDTC) as the precipitant was evaluated. The effects of various factors on precipitation were investigated, and the precipitation mechanism was also identified. Finally, the nickel in the precipitates was recovered following a pyrometallurgical method. The results show that, under optimised conditions (DDTC:Ni(II) molar ratio = 4:1; temperature = 25 °C), the Ni(II) removal efficiency reached 99.3% after 10 min. In strongly acidic wastewater, the dithiocarbamate group of DDTC can react with Ni(II) to form DDTCNi precipitates. Further recovery experiments revealed that high-purity NiO can be obtained by the calcination of DDTCNi precipitates, with the nickel recovery efficiency reaching 98.2%. The gas released during the calcination process was composed of NO₂, CS₂, H₂O, CO₂, and SO₂. These results provide a basis for an effective Ni(II) recovery method from strongly acidic wastewater.     

Influence of environmental temperature and relative humidity on photocatalytic oxidation of toluene on activated carbon fibers coated TiO2

TiO₂ supported on active carbon fiber (TiO₂/ACF), an absorbable photocatalyst, is a new kind of material applied in air purification. In this paper, the influence of environmental temperature (T) and relative humidity (RH) on the gas-solid adsorption of toluene and the photocatalytic oxidation (PCO) efficiency of adsorbed toluene on TiO₂/ACF were studied, and then, the purification capability of TiO₂/ACF was estimated. PCO results showed that although the PCO efficiency increased under high RH and T levels, the amount of adsorption of toluene decreased. Moreover, quantitative analysis results of intermediates indicated that more environmental risk emerged when PCO of toluene was carried out at higher environmental T and RH levels because more toxic intermediates would be accumulated on the TiO₂/ACF. So, it is significant to control the environmental T and RH conditions in the application of the PCO technique. T = 25°C and RH530% is the optimal condition for purifying toluene in our experimental system. __________ Translated from Urban Environment & Urban Ecology, 2007, 20(5): 10–13 [译自: 城市环境与城市生态]     

Carbon dioxide adsorption behaviors of aluminum-pillared montmorillonite-supported alkaline earth metals

The Al-pillared montmorillonite-supported alkaline earth metal 5M/Al-PILC (PILC = pillared clay, M = Mg, Ca, Sr, and Ba) and xMg/Al-PILC (x = 1, 3, 5, and 7 wt.%) samples were prepared using an impregnation method. Physical properties of the materials were determined by means of X-ray diffraction (XRD) and N₂ adsorption-desorption, and their CO₂ adsorption behaviors were investigated using the thermogravimetric analyzer (TG), CO₂ temperature-programmed desorption (CO₂-TPD), and in situ diffuse reflectance infrared transform spectroscopy (in situ-DRIFTS) techniques. It is shown that 5Mg/Al-PILC possessed the highest CO₂ adsorption capacity (2.559 mmol/g). The characterization results indicate that Al-pillaring increased the specific surface area of montmorillonite, which was beneficial for the adsorption of CO₂. The CO₂ adsorption process on the sample was mainly chemical adsorption, and alkalinity was the main factor influencing its adsorption capacity. The alkalinity of the sample was enhanced by loading an appropriate amount of alkaline earth metal, and the adsorbed CO₂ was present in the form of bicarbonate and carbonate. In addition, the 5Mg/Al-PILC sample exhibited an excellent regeneration efficiency. We believe that the outcome of this research would provide a good option for developing highly effective CO₂ adsorption materials.     

Kinetics of enhanced adsorption by polarization for organic pollutants on activated carbon fiber

The adsorption kinetics for model pollutants on activated carbon fiber (ACF) by polarization was investigated in this work. Kinetics data obtained for the adsorption of these model pollutants at open-circuit, 400 mV, and −400 mV polarization were applied to the Lagergren equation, and adsorption rate constants (K _a) were determined. With the anodic polarization of 400 mV, the capacity of sodium phenoxide was increased from 0.0083 mmol/g at open-circuit to 0.18 mmol/g, and a 17-fold enhancement was achieved; however, the capacity of p-nitrophenol was decreased from 2.93 mmol/g at open-circuit to 2.65 mmol/g. With the cathodal polarization of −400 mV, the capacity of aniline was improved from 3.60 mmol/g at open-circuit to 3.88 mmol/g; however, the capacity of sodium dodecylbenzene sulfonate was reduced from 2.20 mmol/g at open-circuit to 1.59 mmol/g. The enhancement for electrosorption changed with different groups substituting. Anodic polarization enhances the adsorption of benzene with the electron-donating group. But whether anodic or not, cathodal polarization had less effect on the adsorption of electron-accepting aromatic compounds, and decreased the adsorption capacity of benzene-bearing donor-conjugate bridge-acceptor, while increasing its adsorption rate. Electrostatic interaction played a very important role in the electrosorption of ion-pollutants. Translated from Environmental Science, 2006, 27(6): 1111–1116 [译自: 环境科学]     

非活性黑根霉菌对废水中重金属离子的吸附

为探讨发酵工业中废弃的菌丝体黑根霉菌（Ｒｈｉｚｏｐｕｓｎｉｇｒｉｃａｎｓ）对水中重金属离子的吸附特性,考察ｐＨ、浓度、共存离子等因素对吸附能力的影响,进行了实验室吸附试验,绘制出吸附等温线,并由Ｌａｎｇｍｕｉｒ曲线和Ｆｒｅｕｎｄｌｉｃｈ曲线求出相应参数。对化学改性前后的黑根霉进行了吸附对比。初步分析了吸附机理。结果表明,黑根霉在ｐＨ＝３—６．５范围内,对Ｐｂ２＋、Ｃｕ２＋、Ｍｎ２＋、Ｃｒ（ＶＩ）几种主要重金属离子都有吸附作用,其中吸附Ｐｂ２＋能力最高,饱和吸附量可达８８ｍｇ／ｇ。经化学改性的黑根霉可不同程度地提高吸附能力。用０．５ｍｏｌ／ＬＨＣＩ和ＮａｏＨ可以洗脱和再生。