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RSC Advances · 2019 ·Vol. 9 ·期 41 ·23711-23717 · IF 3.049

Recyclable magnetic carbonaceous porous composites derived from MIL-100(Fe) for superior adsorption and removal of malachite green from aqueous solution

Shu-Hui Huo,Chen-Xu Liu,Peng-Xin Zhou,Jing Yu,Lei Bai,Zhen-Gang Han,Xiao-Quan Lu

Development of novel porous materials for efficient adsorption and removal of environmental pollutants from aqueous solution is of great importance and interest in environmental science and chemistry. Herein, we reported a facile synthesis of recyclable magnetic carbonaceous porous composite derived from iron-based metal–organic framework MIL-100(Fe) for superior adsorption and removal of malachite green (MG) from aqueous solution. Because of large surface area and high porosity, the synthesized magnetic carbonaceous porous material presented a superior adsorption capacity of 2090 mg g−1 for MG. The adsorption of MG on magnetic carbonaceous porous composite is endothermic and spontaneous. The prepared magnetic carbonaceous porous composite could be separated easily and rapidly from the solution matrix by an external magnet. The rapid adsorption, large adsorption capacity and good reusability make it attractive for practical use in the adsorption and removal of dyes from aqueous solutions.

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Biochar · 2019 ·Vol. 1 ·期 2 ·203-212 · IF 0

The applicability of biochar and zero-valent iron for the mitigation of arsenic and cadmium contamination in an alkaline paddy soil

Qiao Jiangtao,Yu Huanyun,Wang Xiangqin,Li Fangbai,Wang Qi,Yuan Yuzhen,Liu Chuanping

In paddy fields, the opposing transformation of arsenic (As) and cadmium (Cd) poses many challenges for their simultaneous remediation. In our previous study, we reported that combined biochar and zero-valent iron (ZVI) amendment had great potential for the simultaneous alleviation of As and Cd bioavailability in contaminated acid paddy soil. In this study, an As- and Cd-contaminated alkaline paddy soil was further studied, and the same ZVI–biochar mixtures amendments were applied to evaluate the impact of the mixtures on As and Cd transformation and translocation in the soil–rice system by performing pot experiments with rice. In line with our previous study, the ZVI–biochar composites significantly reduced As and Cd accumulation in different rice tissues, leading to a 42% and 47% decrease in rice grain As and Cd levels, respectively, compared with the control values. The ZVI–biochar mixtures exhibited synergistic effects of biochar and ZVI by enhancing the transformation of bioavailable As and Cd fractions into less bioavailable fractions, and by increasing iron plaque formation to reduce As and Cd bioavailability. Although the bioaccumulation and translocation factors of As and Cd in alkaline paddy soil were generally lower than those in acid paddy soil, particularly in the presence of the ZVI–biochar mixtures, the grain As and Cd levels did not achieve the desired food safety standard levels, probably related to the high soil As content and the small changes in soil pH. Nevertheless, for treating lightly and moderately contaminated paddy soils, ZVI–biochar mixtures can still be a good choice in the future.

CAS / MDL: 7439-89-6
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2019 · IF 6.361

Simultaneous removal of methylene blue and total dissolved copper in zero-valent iron/H2O2 Fenton system: Kinetics, mechanism and degradation pathway

Bo Yang,Peng Zhou,Xin Cheng,Haishen Li,Xiaowei Huo,Yongli Zhang

This study aimed to investigate the simultaneous removal of methylene blue (MB) and total dissolved copper (TCu) by heterogeneous zero-valent iron (ZVI) Fenton-like system (ZVI/H 2 O 2 ) and elucidate the mechanism of synergistic effect for co-contaminants removal. Hydroxyl radical ( OH) formation was hypothesized to be the dominant pathway for the oxidation of MB, confirmed by the quenching experiments and ESR analysis. And the synergistic effect of TCu and ZVI greatly promoted the release of Fe 2+ , further accelerating the generation of hydroxyl radical ( OH) via Fenton reaction. The generation process of OH was unveiled by quenching experiments and electron spin resonance (ESR) analysis, while the processes of ZVI corrosion and TCu reduction were revealed through several characterization approaches including SEM , XRD , FTIR and XPS . The degradation pathway of MB was also investigated by LC-MS analysis. The MB initial concentration, TCu initial concentration, H 2 O 2 dosage, ZVI dosage and initial solution pH could play crucial roles in the removal of MB and TCu. The influence of water matrix including inorganic anions (Cl − , NO 3 − , HCO 3 − ) and actual water was finally conducted to elucidate the role of natural organic matter (NOM) in the environmental systems.

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BIORESOURCE TECHNOLOGY · 2019 · IF 6.669

Synergistic effect of magnetite and zero-valent iron on anaerobic degradation and methanogenesis of phenol

Chunhua He,Weishi Lin,Xiaohao Zheng,Chuanya Wang,Zhenhu Hu,Wei Wang

Anaerobic digestion is widely employed for treating phenol-containing wastewater, but there are still some drawbacks such as slow phenol degradation rate and vulnerable acetoclastic methanogens. Coupling of magnetite (Fe 3 O 4 ) and zero valent iron (ZVI) was firstly used to enhance anaerobic digestion of phenol. The results indicated an obvious synergistic effect was generated with coupling of Fe 3 O 4 and ZVI during the whole anaerobic digestion of phenol. The phenol degradation rate and methane production of Fe 3 O 4 /ZVI-added group were increased by 8.8–23.1% and 11.9–31.6%, respectively compared with Fe 3 O 4 -added group, and enhanced by 5.9–17.1% and 4.4–18.3%, respectively compared with ZVI-added group. ZVI improved the growth of hydrogenotrophic methanogens and Fe 3 O 4 enhanced the growth of syntrophic acetate-oxidizing bacteria. Finally, the syntrophic interaction between acetate-oxidizing bacterium and hydrogenotrophic methanogens played a vital role on the synergistic effect of Fe 3 O 4 and ZVI on the whole anaerobic phenol digestion.

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APPLIED ENERGY · 2019 · IF 8.426

Zeolite catalyst-aided tri-solvent blend amine regeneration: An alternative pathway to reduce the energy consumption in amine-based CO2 capture process

Xiaowen Zhang,Yufei Huang,Hongxia Gao,Xiao Luo,Zhiwu Liang,Paitoon Tontiwachwuthikul

The extensive energy penalty of CO 2 -loaded solution regeneration is one of the most crucial challenges facing industrial application of amine-based CO 2 capture technology. Here, to decrease the energy requirement, the regeneration behaviors of the rich 5 M monoethanolamine (MEA) and 3 M MEA-2.5 M N-methyl-diethanolamine (MDEA)−0.5 M piperazine (PZ) tri-solvent blended amines (tri-blend) with four different solid acid catalysts (H-mordenite, Hβ, HZSM-5 and Al 2 O 3 ) were studied at 98 °C. For the catalyst-free tests, the results revealed that the tri-blend hugely enhanced the CO 2 desorption kinetics and reduced the relative energy consumption compared to 5 M MEA. Based on the results of 13 C NMR, the multiple proton transfer paths and abundant bicarbonate ions in the tri-blend contribute to the improved regeneration performance. Additionally, the use of catalyst further improved the CO 2 desorption activity of the tri-blend. The combination of Hβ and tri-blend presented the best regeneration performance, increasing the desorption performance by 1360.8%, and reducing the relative energy requirement by 66.1% compared with the blank run of MEA. In addition, a plausible catalytic mechanism of solvent regeneration over the solid acid catalyst in the tri-blend was suggested. The superior catalytic performance of Hβ resulted from the large mesoporous surface area, larger number of Brϕnsted acid sites and prominent total acid sites. Furthermore, Hβ displayed excellent stability and had no adverse influence on the CO 2 absorption activity. Results herein manifest that the combination of tri-blend amines with high-efficiency catalyst is exceptional strategy for tremendously decreasing the energy consumption of amine-based CO 2 capture processes, ultimately making this technology more technically and economically feasible.

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Greenhouse Gases-Science and Technology · 2019 ·Vol. 9 ·期 2 ·349-359 · IF 1.693

Promotion of CO2 capture performance using piperazine (PZ) and diethylenetriamine (DETA) bi-solvent blends

Ji Liu,Xiaoshan Li,Zewu Zhang,Liwei Li,Yajun Bi,Liqi Zhang

The carbon dioxide post-combustion capture process using amine solutions is considered the most appropriate method for CO 2 capture from flue gas in power plants. This paper focuses on the CO 2 capture performance of six common organic amines. Two amines, piperazine (PZ) and diethylenetriamine (DETA), which showed better performance, were then filtered out to form amine blends to improve performance further. The absorption heat from the CO 2 absorbing process was measured directly using an advanced C80 micro calorimeter for more accurate calculation of regenerative energy consumption. Experimental results confirmed the optimal amine blend to be 10% PZ plus 20% DETA, with a 42% increase in absorption capacity and a 9% increase in initial absorption rate compared to traditional 30% monoethanolamine (MEA). The regeneration energy consumption of this chosen PZ-DETA blend was calculated to be 3.979 GJ/ton CO 2 , a decrease of 9% compared with MEA. Moreover, it led to an improvement of about 55% in stable cyclic absorption capacity in comparison with 30% MEA. It was confirmed that this PZ-DETA blend can bring practical economic benefits to industrial applications when replacing the current 30% MEA solution. © 2019 Society of Chemical Industry and John Wiley & Sons, Ltd.

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WASTE MANAGEMENT · 2019 · IF 5.431

Treatment of a simulated sludge by ultrasonic zero-valent iron/EDTA/Air process: Interferences of inorganic salts in polyaromatic hydrocarbon removal

Xiaojun Lai,Xun-an Ning,Yao He,Yiqian Yuan,Jian Sun,Yaowei Ke,Xiaoyuan Man

Understanding the occurrence states of persistent organic pollutants such as polycyclic aromatic hydrocarbons (PAHs) in textile dyeing sludge is the key to their further treatment and disposal. Here, the effects of inorganic salts (silicate, sulfate, phosphate, hydroxide, and iron salts) that were typically rich in textile dyeing sludge on PAH adsorption by sludge and PAH degradation by an ultrasound (US) combined zero-valent iron/EDTA/Air (ZEA) system were studied in a simulated sludge system. The results showed that the simulated sludge containing inorganic salts had a larger specific surface area, which was beneficial for the adsorption of PAHs. More low-ring PAHs were adsorbed on the surface of the particles in the simulated sludge because of the inorganic salts, which was conducive to low-ring PAHs degradation by US/ZEA. The PAH removal rates were increased by 15.37% and 11.19%, respectively, in the presence of SiO 3 2− and HPO 4 2− . The yield of hydroxyl radicals ( OH) was increased by 42.39% and 66.25% by SiO 3 2− and HPO 4 2− , respectively. The reason was that the oxidation of the ligand ([Fe Ⅱ (EDTA)]) formed by ethylenediaminetetraacetic acid (EDTA) and divalent iron was promoted by SiO 3 2− and HPO 4 2− . The formation of OH in the US/ZEA system was inhibited by the corrosion inhibition of SO 4 2− on zero-valent iron (ZVI), the reaction of ferric salt with EDTA, and the reaction of Mg(OH) 2 with the ligand ([Fe III (EDTA)]). This work provides an essential theoretical insight into the role of the inorganic components of sludge in the removal of PAHs by advanced oxidation processes.

CAS / MDL: 6381-92-6 7439-89-6
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NEW JOURNAL OF CHEMISTRY · 2019 ·Vol. 43 ·期 24 ·9725-9731 · IF 3.069

Enhancement of CO2 capture and separation of CO2/N2 using post-synthetic modified MIL-100(Fe)

Suresh Mutyala,Sobhy M. Yakout,Shebl S. Ibrahim,Madhavi Jonnalagadda,Harisekhar Mitta

Iron metal–organic framework, MIL-100(Fe) was prepared by a hydrothermal method and used as a support to incorporate diethylenetriamine (DETA) for the study of CO2 adsorption and separation of CO2/N2. All synthesized adsorbents were characterized by PXRD, N2 adsorption–desorption isotherms, FT-IR, TGA, SEM, and elemental analysis. Structural characterization results have revealed that the structure of MIL-100(Fe) was not changed by the incorporation of diethylenetriamine. The CO2 adsorption capacities were 29 cm3 g−1 and 41 cm3 g−1 at 298 K, 1 bar for MIL-100(Fe) and DETA–MIL-100(Fe), respectively. Adsorption of CO2 on DETA–MIL-100(Fe) was higher than that on MIL-100(Fe). The enhancement was due to the presence of amine groups which could form ammonium carbamate by interaction with CO2. Similarly, the N2 adsorption capacities were 3 cm3 g−1 and 0.9 cm3 g−1 at 298 K, 1 bar for MIL-100(Fe) and DETA–MIL-100(Fe), respectively. The decrease in N2 adsorption capacity was due to the decrease in surface area. The selectivity of CO2/N2 on DETA–MIL-100(Fe) was four times higher than that on MIL-100(Fe). The heat of CO2 adsorption was 74.2 kJ mol−1 at low coverage of CO2 on DETA–MIL-100(Fe) and the CO2 adsorption capacity was constant in each adsorption cycle over the same adsorbent.

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SCIENCE OF THE TOTAL ENVIRONMENT · 2019 · IF 5.589

Iron-dependent nitrate reduction by anammox consortia in continuous-flow reactors: A novel prospective scheme for autotrophic nitrogen removal

Zhen Bi,Wenjing Zhang,Ge Song,Yong Huang

Anammox bacteria are chemolithotrophic organisms growing on the conversion of ammonium and nitrite with bicarbonate as the sole carbon source. Meanwhile, anammox bacteria display a metabolic versatility to sustain their metabolism. However, there is less attention on the Fe 0 /Fe 2+ -dependent autotrophic denitrification by anammox consortia. In this study, the autotrophic nitrate reduction using different valence of iron (Fe 0 , Fe 2+ and Fe 0 + Fe 2+ , respectively) as electron donors by anammox consortia were firstly explored in continuous feeding mode. Results revealed anammox consortia showed high adaptability to the niche wherein containing nitrate and iron. They could generate nitrite and ammonium from iron-dependent nitrate reduction, and hence support their central metabolism. During 60-days operation, the maximum nitrate and total nitrogen removal efficiency reached 88.43% and 80.77%, respectively, with coexistence of Fe 0 and Fe 2+ . The expression of key functional genes involved in nitrate reduction (including narG, napA and nrfA ) in 16S rRNA level revealed the coupling of dissimilatory nitrate reduction to nitrite, dissimilatory nitrite reduction to ammonia (DNRA), and anammox processes possibly play pivotal role in nitrogen loss under Fe 0 /Fe 2+ condition. Meanwhile, abiotic reduction by Fe 0 /Fe 2+ also contributed nitrate reduction to provide nitrite and ammonium for anammox consortia. Activities of two vital enzymes hydrazine dehydrogenase (HDH) and nitrate oxidoreduetase (NAR) also inferred higher microbial activities with co-existence of Fe 0 and Fe 2+ . The present study confirms and further extends the versatile metabolisms of Anammox consortia, also it can help to circumvent the accumulation of nitrate produced by anammox process itself and increase the quality of discharge.

CAS / MDL: 7439-89-6
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WATER ENVIRONMENT RESEARCH · 2019 ·Vol. 91 ·期 8 ·770-779 · IF 1.24

Degradation of 4-chlorophenol by BM Fe/Cu-O2 system: The symbiosis of and ·OH radicals

Jinhong Fan,Hehe Qin,Yunfei Zhang,Simin Jiang

In this study, Fe/Cu bimetal composite was prepared by high-energy ball milling (BM) method for the removal of refractory organics. The BM Fe/Cu bimetal was characterized by SEM-EDS, XRD, and XPS. Evenly distributed Fe and Cu was observed in the EDS mapping. In contrasting experiments, the removal rate of 4-chlorophenol (4-CP) by BM Fe/Cu materials was about 10-fold faster than that by chemical substitution deposition (CSD) of Fe/Cu material. Complete 4-CP removal and 66.7% of total organic carbon (TOC) mineralization in the BM Fe/Cu–O 2 system were achieved. Dissolved oxygen plays a crucial role for 4-CP degradation through the in situ generation of reactive oxygen species (ROS) such as H 2 O 2 , ·OH, and via oxygen activation reactions. The predominant reactive radicals were identified to be and ·OH through ESR technique and inhibition experiments. The coexistence of oxidation and reduction of 4-CP in the BM Fe/Cu-O 2 system was proposed. Practitioner points 4-CP removal rate by BM Fe/Cu is 10-fold faster than that by CSD Fe/Cu at the same conditions. Complete 4-CP removal and 66.7% of TOC reduction were achieved. All three ROS including ·OH, , and H 2 O 2 coexisted in the BM Fe/Cu-O 2 system. A harmonious coexistence of oxidation and reduction mechanism was proposed.

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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2019 ·Vol. 26 ·期 10 ·9480-9489 · IF 2.914

Dechlorination and conversion mechanism of trichlorobenzene as a model compound of chlorine-containing wastes by different base-catalyzed combinations

Dai Shijin,Zheng Yilin,Zhao Youcai,Li Qiang,Niu Dongjie

Chlorine-containing organic waste (COWs) is a big threat for the waste incineration because of the dioxin generation and equipment corrosion. Recently, dechlorination and detoxification of COWs is emergent in order to lower the environmental risk and treatment costs. In this study, base-catalyzed decomposition processes with different hydroxides, hydrogen donors, and catalysts were conducted for pre-treatment of COWs to reduce organic chlorine content, with the TCB as a model compound and industrial rectification residues for verification. Results showed that maximum chlorine retention efficiency (CRE) of four alkalis followed the order of KOH > NaOH–KOH > NaOH > Mg(OH) 2 , which were 98.3%, 93.4%, 97.2%, and 1.5%, respectively, and could be expressed as an apparent first-order reaction. The differences were resulted from the varying ionic potentials of the metal cations. Hydrogen donors (glycol, glycerol, paraffin oil, and PEG 200) acted as effective dechlorination regents follow the order of PEG > glycol > paraffin oil > glycerol. In addition, Fe, Ni, Cu, and activated carbon catalysts increased the CRE by 68.9% to 92.4%, 91.9%, 89.2%, and 73.3%, respectively. Residue analysis through X-ray diffraction and Fourier transform infrared spectroscopy revealed that KCl, sodium oxalate, and phenol were the main products and a plausible stepwise dechlorination pathway was proposed. The effectiveness of three optimized combinations including NaOH/PEG, KOH/PEG, and NaOH–KOH/PEG (with the Fe catalyst) was confirmed by using them for dechlorinating rectification residues, and they restrained 98.2%, 91.2%, and 94.6% of the chlorine, respectively. The organochlorine content decreased from 19.2 to 1.8% within 180 min, while inorganic chorine content increased from 1.5 to 18.9%, indicating the potential for COWs dechlorination.

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ACS Applied Materials & Interfaces · 2018 · IF 8.097

Controlled Construction of Cu(I) Sites within Confined Spaces via Host–Guest Redox: Highly Efficient Adsorbents for Selective CO Adsorption

Yu-Xia Li,Yu-Nong Ji,Meng-Meng Jin,Shi-Chao Qi,Shuai-Shuai Li,Ding-Ming Xue,Ming Bo Yue,Xiao-Qin Liu,Lin-Bing Sun

Here, we designed a double-solvent/host–guest redox combined strategy to construct Cu+ sites in metal–organic frameworks (MOFs) for the first time. As a proof of concept, a representative MOF MIL-100(Fe) with tunable valence states of cations was employed as the host. The combined strategy realizes selective introduction of Cu2+ precursors to the interior pores of MIL-100(Fe), remarkably minimizing the aggregation of Cu2+ and subsequently formed Cu+ species. Owing to the proper reducibility of in situ formed Fe2+ in the frameworks, controlled conversation of Cu2+ to Cu+ with ∼100% yield is achieved in the absence of any additional reducing agents. These characteristics make the obtained materials Cu+-modified MIL-100(Fe) highly active in selective CO adsorption. The CO adsorption capacity is up to 3.75 mmol·g–1 at 298 K and 1 bar, which is superior to all other Cu+-containing adsorbents reported so far such as CuCl/activated carbon (2.5 mmol·g–1), CuCl/γ-Al2O3 (1.0 mmol·g–1), and CuCl/SBA-15 (0.50 mmol·g–1). The same adsorbent also exhibits quite high selectivity of CO over N2, and the ideal adsorption solution theory selectivity reaches 424. The outstanding CO adsorption performance make the present adsorbents great potential in separation of CO from various mixtures.

CAS / MDL: 7439-89-6 554-95-0
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