APPLIED ENERGY
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2018
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IF 7.9
Xiaowen Zhang,Rui Zhang,Helei Liu,Hongxia Gao,Zhiwu Liang
To enhance the energy efficiency of the CO 2 desorption process, the regeneration behaviors of the CO 2 -loaded 6 M MEA-AMP-PZ (monoethanolamine, 2-amino-2-methyl-1-propanol and piperazine) tri-solvent blends with different AMP/PZ molar ratios with four different solid acid catalysts (H-ZSM-5, γ-Al 2 O 3 , SAPO-34 and SO 4 2− /TiO 2 ) and a blank at 96 °C were investigated in terms of CO 2 desorption rate, cyclic capacity and relative heat duty. For the no-catalytic runs, the results showed that all the tri-solvent blended amines greatly increased CO 2 desorption rate, cyclic capacity and decreased the relative heat duty in comparison with 5 M MEA. The 13 C NMR analysis indicated that the 3 M MEA-2.5 M AMP-0.5 M PZ blend with the highest AMP/PZ ratio produced the largest amount of bicarbonate and less carbamate, which resulted in the best desorption performance. With regard to catalyst, when the solid acid catalysts were introduced, the regeneration performance of the blend was further improved. The best of the blends along with H-ZSM-5 provided the combination with the best performance in CO 2 desorption, and reduced the relative heat duty by 61.6% as compared to 5 M MEA without catalyst (100%). Five relevant physicochemical properties of the catalyst were obtained and used to better understand the catalytic regeneration process. A possible catalytic CO 2 desorption mechanism was analyzed. The results revealed that the mesopore surface area coupled with total acid sites of the catalyst had the most positive influence on improving the CO 2 desorption performance. Findings from this work imply that the combination of solid acid catalyst with tri-solvent blended amines is a promising alternative method for further reduction of solvent regeneration energy requirement.
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CHEMOSPHERE
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2017
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IF 4.208
Jiang-tao Qiao,Tong-xu Liu,Xiang-qin Wang,Fang-bai Li,Ya-hui Lv,Jiang-hu Cui,Xiao-duo Zeng,Yu-zhen Yuan,Chuan-ping Liu
The fates of cadmium (Cd) and arsenic (As) in paddy fields are generally opposite; thus, the inconsistent transformation of Cd and As poses large challenges for their remediation. In this study, the impacts of zero valent iron (ZVI) and/or biochar amendments on Cd and As bioavailability were examined in pot trials with rice. Comparison with the untreated soil, both Cd and As accumulation in different rice tissues decreased significantly in the ZVI-biochar amendments and the Cd and As accumulation in rice decreased with increasing ZVI contents. In particular, the concentrations of Cd (0.15 ± 0.01 mg kg −1 ) and As (0.17 ± 0.01 mg kg −1 ) in rice grains were decreased by 93% and 61% relative to the untreated soil, respectively. A sequential extraction analysis indicated that with increasing Fe ratios in the ZVI-biochar mixtures, bioavailable Cd and As decreased, and the immobilized Cd and As increased. Furthermore, high levels of Fe, Cd, and As were detected in Fe plaque of the ZVI-biochar amendments in comparison with the single biochar or single ZVI amendments. The ZVI-biochar mixture may have a synergistic effect that simultaneously reduces Cd and As bioavailability by increasing the formation of amorphous Fe and Fe plaque for Cd and As immobilization. The single ZVI amendment significantly decreased As bioavailability, while the single biochar amendment significantly reduced the bioavailability of Cd compared with the combined amendments. Hence, using a ZVI-biochar mixture as a soil amendment could be a promising strategy for safely-utilizing Cd and As co-contaminated sites in the future.
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International Journal of Greenhouse Gas Control
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2017
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IF 3.741
Yan Zhou,Yiheng Rao,Tielin Wang,Klaus-J. Jens
Piperazine (PZ) based amine blends are promising solvents for post-combustion CO 2 capture, but PZ can form potential carcinogenic nitrosamines from nitrite. In this work, the kinetics of the reaction between nitrite and PZ to form N-nitrosopiperazine (MNPZ) was determined in 0.1–0.5 mol L −1 PZ in the presence of 17–170 mmol L −1 formaldehyde at 60–135 °C. The nitrosation of PZ can be catalyzed by formaldehyde, a primary degradation product of PZ. And the reaction involving nitrite and PZ is first order in nitrite, formaldehyde, and hydronium ion. A kinetic model was established, and the activation energy is 33.6 ± 1.8 kJ mol −1 with a rate constant of 2.3 × 10 3 ± 0.4 × 10 3 L 2 mol −2 s −1 at 100 °C. The kinetics will be helpful to develop strategies to reduce nitrosamine formation and accumulation in PZ based CO 2 capture systems.
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CHEMOSPHERE
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2017
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IF 4.208
Jun Wan,Xiaoqing Jiang,Tian C. Zhang,Jiong Hu,Dana Richter-Egger,Xiaonan Feng,Aijiao Zhou,Tao Tao
Finding a good sorbent for phosphorus (P) recovery from the aquatic environment is critical for preventing eutrophication and providing P resources. The activated iron system (mainly consisted of zero-valent iron (ZVI), Fe 3 O 4 and Fe 2+ ) has been reported to exhibit a favorable performance towards various contaminants in wastewater, but its effect on P recovery has not been studied systematically. In this study, we used Fe 2+ -nitrate pretreatment reaction to prepare the activated iron system and then applied it to P recovery. Results show that more than 99% P was removed from water in 60 min; co-existing anions (NO 3 − , Cl − and SO 4 2− ) and natural organic matter (NOM) had little effect on P removal. The P removal capacity of activated iron system is very high compared with currently reported sorbents. Externally-supplied Fe 2+ plays an important role on P removal in the system. Regeneration study shows that the activated iron system exhibited stable P recovery ability by using 0.1 M NaOH solution. Various methods were applied to characterize the ZVI and iron corrosion, and results conclude that sorption precipitation, and co-precipitation contribute to P removal. This method will be promising and have an application potential in the field for efficient and cost-effective recovery of P with cheap microscale zero valent iron.
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FOOD AND AGRICULTURAL IMMUNOLOGY
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2018
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IF 2.568
Zhi-Li Xiao,Wei Tian,Zhen-Lin Xu,Yuan-Ming Sun
In this study, we develop a sensitive indirect competitive chemiluminescent enzyme immunoassay (ic-CLEIA) to detect cadmium (Cd) in cereals. A luminol-hydrogen peroxide chemiluminescence system catalysed by horseradish peroxidase (HRP) was used as the signal detecting system. The method showed a half-maximal inhibition concentration (IC50) of 0.5 ng/mL and a limit of determination (LOD) of 0.06 ng/mL. The assay indicated an effective linear range from 0.16 to 1.56 ng/mL. There were no obvious cross-reactivities with other metal ions, including Hg2+, Pb2+, As2+, Ag+, Fe3+, Cu2+, Cr2+, Au3+, Ca2+, Mg2+, Mn2+ and Zn2+. Recovery rates ranged from 79.2% to 120.0% for rice, maize, wheat, brown rice and glutinous rice samples. Twenty-five practical cereal samples were analysed, and the comparative analysis of the results showed a strong correlation (r = 0.984) between the CLEIA and the GFAAS methods. The results indicated that the ic-CLEIA developed was acceptable to screen for cadmium in cereal samples.
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ENVIRONMENTAL POLLUTION
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2024
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IF 7.6
Yumeng Qi,Wenqian Cao,Ying Zhang,Ruijuan Qu,Rehab Khaled Mahmoud,Mostafa R. Abukhadra,Zongli Huo,Feng Zhu
The present study systematically investigated the elimination of benzalkonium chloride (BAC) in the zero valent iron activated persulfate (Fe 0 /PS) system. The influence of operational parameters, including PS concentration, Fe 0 dosage and pH, were investigated through a series of kinetic experiments. When the Fe 0 dosage was 5.0 mM, the initial ratio of [PS]: [BAC] was 10:1, the degradation efficiency could achieve 91.7% at pH 7.0 within 60 min. Common inorganic anions and humic acid did not significantly affect BAC degradation, implying that Fe 0 /PS system had a potential application prospect in the actual wastewater remediation. Based on the electron paramagnetic resonance test and quenching experiments, the BAC degradation was found to be contributed by •OH, SO 4 • - and Fe(IV). A total of 23 intermediates were identified by the liquid chromatography-mass spectrometry, and the degradation pathways were proposed accordingly, including dealkylation and demethylation, hydroxylation, sulfate substitution and benzyl C-N cleavage reactions. Density functional theory based calculations were conducted to realize the rationality of the proposed reaction mechanisms. The toxicity of transformation products was predicted by ECOSAR program. This work demonstrated the possibility of BAC removal in hospital and municipal wastewater by Fe 0 /PS treatment, and also provides a safe choice for deep treatment of quaternary ammonium salt wastewater.
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Frontiers in Environmental Science
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2024
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IF 3.3
Huang Yuanyuan,Yang Qingwei,Song Ling,Ran Hongjie,Jiang Hui,Sun Da
In this study, we investigated the oxidative mechanisms of nano zero-valent iron (nZVI) enhanced potassium ferrate (K2FeO4), focusing on tributyltin (TBT) and triphenyltin (TPhT) as target pollutants. The addition of nZVI enhanced the degradation of both organic tin compounds by K2FeO4, exhibiting pseudo-first-order kinetics influenced by pH, carbonate, and fulvic acid. nZVI, as a reducing agent, facilitated the generation of stronger oxidizing species Fe (V) and Fe (IV) from K2FeO4 through electron transfer. The presence of hydroxyl radicals (OH) was confirmed by tert-butyl alcohol (TBA) verification. Intermediate products of TBT degradation by nZVI-enhanced K2FeO4 were identified using GC-MS, confirming de-alkylation leading to stepwise oxidation to inorganic tin ions. Due to excessively long Sn-C bonds in diphenyltin, rendering them unstable, Density Functional Theory (DFT) calculations were employed. Results indicated that Fe (IV) and Fe (V) predominantly attacked the Sn-C bonds of TPhT, while OH primarily targeted the benzene ring. HOMO energy levels suggested that Fe (V) was more prone to oxidizing TPhT than Fe (IV). Gibbs free energy calculations demonstrated that, in the presence of Fe (IV) and Fe (V), the energy barrier for breaking bonds and oxidizing into inorganic tin ions decreased, favoring the process over the self-decomposition of TPhT. Additionally, the lower energy barrier for OH indicated an easier degradation of TPhT. This study reveals that nZVI-enhanced K2FeO4 effectively removes TBT and TPhT, contributing to the understanding of the ferrate-mediated degradation mechanism of organic tin compounds. The findings offer insights and theoretical guidance for remediating organic tin pollution in aquatic environments.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Kuang Wang,Zhanqiang Fang
In this work, a cost-effective ball-milling technique was employed to synthesize submicron oxalated zero-valent iron co-doped with graphite and nickel (G@Fe OX bm /Ni), aiming to enhance the removal efficiency of the recalcitrant pollutant 2, 2′, 4, 4′ – tetrabromodiphenyl ether (BDE-47) while minimizing secondary risks. The incorporation of graphite significantly improved the debromination efficiency of BDE-47, with a rate constant of 0.26 day −1 in a tetrahydrofuran/water system, which represents a 59.88 % increase over the oxalated zerovalent Fe/Ni without graphite (0.16 day −1 ). The determination of Ni leaching showed that no nickel ions were detected post-reaction over a broad pH range (3–11). Moreover, the reactivity of G@Fe OX bm /Ni was largely unaffected across the pH range (0.26–0.49 day −1 ), exhibiting excellent resistance to acidic and alkaline conditions. In both ultrapure water and real groundwater matrices, the degradation rate constants for BDE-47 increased to 2.98 day −1 and 0.79 day −1 , respectively, achieving debromination yields of 97.86 % and 50.18 % for the final product, diphenyl ether. Based on the established degradation pathway and electrochemical analysis, the debromination of BDE-47 follows a catalytic debromination and hydrogenation process by adsorbed atomic hydrogen (H* ADS ). The graphite doping enhanced the debromination of BDE-47 by increasing the production of H* ADS . The adsorption effect of graphite on metal ions effectively controlled secondary pollution and improved the material’s tolerance to acidic and alkaline environments. This work offers an efficient method for the degradation of low brominated diphenyl ether pollutants at a low cost and without secondary risks.
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ENVIRONMENTAL POLLUTION
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2024
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IF 7.6
Kuang Wang,Zhanqiang Fang
In the homologous series of polybrominated diphenyl ethers (PBDEs), the debromination of low-brominated diphenyl ethers with higher toxicity remains a challenge. Nano zero-valent iron (nZVI) has been extensively studied for the debromination of PBDEs, but its inherent direct electron transfer mechanism is less efficient for low-brominated diphenyl ethers, and there are issues with high preparation costs. In this work, we synthesize Ni-doped oxalated submicron ZVI (Fe OX bm /Ni) using a low-cost ball-milling method. Fe OX bm /Ni exhibits a debromination rate constant of 0.48 day −1 for 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47) in tetrahydrofuran (THF)/water. The debromination rate of Fe OX bm /Ni for BDE-47 in water is even faster (0.98 day −1 ), with the yield of the complete debromination product, diphenyl ether, reaching 76.71%. In real groundwater, Fe OX bm /Ni also shows high reactivity toward BDE-47, with a rate constant of 0.33 day −1 . Kinetic experiments, quenching experiments, and degradation pathway indicate that the attack of atomic hydrogen on C-Br bonds is the primary degradation mechanism. Electrochemical analysis further show that Ni 0 sites could cleave hydrogen into absorbed atomic hydrogen (H∗ ABS ) and adsorbed atomic hydrogen (H∗ ADS ), with H∗ ADS playing the main role. These findings contribute valuable insights into advancing the large-scale application of ZVI and offer promising strategies for thorough remediation of PBDEs pollution.
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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Xuan Zhang,Siyu Xu,Yawei Gu,Ling Zhang,Longquan Zhang,Fengxu Shang,Xinze Song,Zhen Wang,Xiaoguo Shi,Honglei Zhang,Runze Bi,Jinbo Chen
Zero-valent iron (ZVI) technology has become prevalent for the in situ dechlorination of trichloroethylene (TCE) widely found in soils and groundwater. Nevertheless, ZVI technology still encounters several severe bottlenecks, including inadequate reactivity, poor selectivity, and unelucidated mechanism. Herein, we report that a C&S-mZVI bm material, with the Co-incorporation of C and S into Zero-Valent Iron, could significantly improve the degradation efficiency of ZVI, while simultaneously inhibiting the hydrogen evolution reaction (HER), thereby enhancing the electron selectivity in the TCE dechlorination. Comprehensive characterization techniques have demonstrated that the Co-incorporation of C and S into ZVI leads to better TCE affinity, faster electron transfer and lower charge-transfer resistances. In addition, novel FeS x and Fe 3 C species emerged as new active sites, resulting in two distinct reaction pathways. Specifically, when the C weight percentage is below 2 %, the cumulative quantity of hydrocarbon products surpasses that of DCE, indicating the dominant β-elimination pathway. Conversely, when the weight percentage of C exceeds 2 %, the overall hydrocarbon products fall short of DCE, suggesting that the TCE hydrogenolysis dechlorination reaction becomes the primary pathway. These insights can benefit not only the development of ZVI-based materials but also enhance the broad application of these materials in remediation of groundwater with chlorinated hydrocarbons.
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Journal of Water Process Engineering
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2024
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IF 6.3
Yun-fei Zhang,Xin Quan,Sheng-gui Chen,Jian-hui Xu,Dan Li,Lei Li,Si-hao Lv,Jin-ze Li,Yi-hang Zhang,Zhuo-wei Zhong
In this study, silicon nitride-zero-valent iron (Si 3 N 4 -ZVI) powders were obtained through post-milling and employed as a catalyst to activate peracetic acid (PAA) for the removal of Ranitidine (RAN). The system achieved an impressive 90.4 % of degradation efficiency, with a pseudo-first-order kinetic reaction constant 11.3 times higher than that of the ZVI/PAA system. Quenching experiments and Electron Paramagnetic Resonance (EPR) analysis confirmed that both radical and non-radical processes are involved in RAN degradation within the Si 3 N 4 -ZVI/PAA system. Moreover, the identified ten degradation products are less toxic compared to the byproducts from alternative oxidation methods reported by prior literature. The proposed degradation pathway of RAN includes C S cleavage, oxygenation/hydroxylation demethylation, and denitrification. Furthermore, the Si 3 N 4 -ZVI/PAA system showed effectively in treating RAN-contaminated surface water, artificial wastewater, and dissolved organic matter, demonstrating its great ability in treating diverse organic-contaminated water sources. In conclusion, results of this study suggest that the Si 3 N 4 -ZVI/PAA system possess high pollutant removal efficiency, broad applicability, and less environmental and health risks.
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Journal of Materials Chemistry A
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2025
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IF 9.5
Jiawen Hu,Linwen Jiang,Jiawei Jin,Hang Liu,Anhua Wu,Xiaofeng Zhang
High-entropy alloys (HEAs) are important candidates for efficient electromagnetic-wave absorbing (EMA) materials, but the further design of HEA absorbers with harmonized impedance matching and excellent environmental stability remains a major challenge. In this study, a novel carbonitriding process based on a mechanochemical method is employed to prepare carbonitrided FeCoNiMn HEAs by utilizing a cyano-compound (C3H2N2) as a source of C and N. The introduction of C and N effectively optimizes the permittivity of FeCoNiMn HEAs, achieving the equilibrium of electromagnetic matching and thus improving the EMA performances (especially the bandwidth). The carbonitrided FeCoNiMn HEAs exhibit significant reflection loss (RL) and absorption capability. FeCoNiMnM0.04 achieves a minimum RL of −65.8 dB at 3.44 GHz. FeCoNiMnM0.08 achieves an ultra-broad effective absorption bandwidth (EAB) of up to 7.76 GHz at 1.62 mm, covering the entire Ku-band. In addition, the carbonitrided FeCoNiMn HEAs exhibit excellent corrosion resistance and good mechanical properties, ensuring their suitability for harsh environments. This study highlights the potential of carbonitrided HEAs prepared using a cyano-compound as highly efficient EMA materials, and provides a reference for optimizing the electromagnetic matching of HEAs.
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