ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2021
·Vol. 29
·期 14
·20711-20720
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IF 4.223
Jiang Ying,Du Linna,Cheng Qilu,Jin Zhuo,Hui Cai,Zhao Yuhua,Jiang Hui,Xu Ligen
Nanoparticles and organic pollutants are two major contaminants found in aquatic environments. Algae are regarded as the model organism for the risk assessment of pollutants in water. In our previous study, we investigated the toxic effects of nonylphenol (NP), a typical organic water pollutant, on algae; however, it remains unclear how algae respond to the coexistence of NP and nanoparticles. In this study, a concentration gradient of nanoscale zero-valent iron (nZVI; 10, 50, 100, and 200 mg/L) was added to NP-exposed Dictyosphaerium sp. to investigate both the toxic effects of this combination and the potential for NP removal. nZVI had a dose-dependent effect on NP-exposed algae, with high nZVI concentrations significantly decreasing algal biomass and pigment content, as well as severely damaging algal cellular ultrastructure. In addition, genes involved in antioxidant response, photosynthesis, and ribosome synthesis were significantly altered when NP-exposed algae were incubated with nZVI. In contrast to high nZVI concentrations, adding a small concentration of nZVI led to reduced toxicity in NP-exposed algae, while significantly enhancing the NP removal rate. This study improves our understanding of algal responses to various pollutants and suggests that nZVI may assist in the remediation of NP in aquatic ecosystems.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Tong Liu,Zhican Xie,Peng Zhou,Zhaokun Xiong,Heng Zhang,Zhicheng Pan,Yang Liu,Bo Lai
Transition metal activation of sulfite (S(IV)) is a promising wastewater treatment technology . In this study, the activation of potassium pyrosulfite (PPS) with ferric iron (Fe 3+ ) is proposed firstly to degrade carbamazepine (CBZ). PPS has the advantages of low cost, non-toxicity and acidic solution, which makes it unnecessary to adjust the pH. The results showed that the Fe 3+ cycle was realized during the reaction process, and the degradation trend of CBZ was consistent with the formation rate of Fe 2+ and the decay rate of S(IV). Moreover, oxygen (O 2 ) plays a decisive role in the system and was the initiator of free radical chain reactions. The existence of sulfite radical (SO 3 •− ), sulfate radical (SO 4 •− ) and hydroxyl radicals (HO • ) in Fe 3+ /PPS system was proved by electron paramagnetic resonance (EPR), quenching experiments and terephthalic acid (TA) photoluminescence probing technique. The contribution of SO 4 •− and OH • to the removal of CBZ in Fe 3+ /PPS system is 64% and 35%, respectively. In addition, intermediates of CBZ were identified by Liquid Chromatography–Tandem Mass Spectrometry (LC–MS/MS) and possible removal pathways were also proposed. Finally, the effects of PPS concentration, Fe 3+ concentration, initial pH, anions and humic acid (HA) were also investigated.
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Nature Communications
·
2021
·Vol. 12
·期 1
·1-15
·
IF 14.919
Chen Junjie,Chen Longqi,Wu Yinglong,Fang Yichang,Zeng Fang,Wu Shuizhu,Zhao Yanli
Developing high-quality NIR-II fluorophores (emission in 1000–1700 nm) for in vivo imaging is of great significance. Benzothiadiazole-core fluorophores are an important class of NIR-II dyes, yet ongoing limitations such as aggregation-caused quenching in aqueous milieu and non-activatable response are still major obstacles for their biological applications. Here, we devise an activatable nanoprobe to address these limitations. A molecular probe named BTPE-NO 2 is synthesized by linking a benzothiadiazole core with two tetraphenylene groups serving as hydrophobic molecular rotors, followed by incorporating two nitrophenyloxoacetamide units at both ends of the core as recognition moieties and fluorescence quenchers. An FDA-approved amphiphilic polymer Pluronic F127 is then employed to encapsulate the molecular BTPE-NO 2 to render the nanoprobe BTPE-NO 2 @F127. The pathological levels of H 2 O 2 in the disease sites cleave the nitrophenyloxoacetamide groups and activate the probe, thereby generating strong fluorescent emission (950~1200 nm) and ultrasound signal for multi-mode imaging of inflammatory diseases. The nanoprobe can therefore function as a robust tool for detecting and imaging the disease sites with NIR-II fluorescent and multispectral optoacoustic tomography (MSOT) imaging. Moreover, the three-dimensional MSOT images can be obtained for visualizing and locating the disease foci.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Shuang Zhang,Xinxin Ma,Dong Xie,Weijie Guan,Min Yang,Pan Zhao,Ming Gao,Qunhui Wang,Chuanfu Wu
The addition of activated carbon (AC) may improve the efficiency of anaerobic digestion (AD) system to which zero-valent iron (ZVI) has been added. This study investigated the effects of the addition of AC on the AD system with ZVI added. Results showed that the cumulative methane production of 5 g/L ZVI + 5 g/L AC (5ZVI + 5AC) was 2.77–35.0% higher than that of 5 g/L ZVI, 10 g/L ZVI and control. The combined addition shortened the time to reach maximum daily methane yield by 18.2% compared to ZVI groups. Meanwhile, 5ZVI+5AC had the lowest free ammonia concentration (average 461 mg/L) amongst all groups, thus effectively alleviating the ammonia inhibition. Microbial community analysis showed that the combined addition of ZVI and AC enriched hydrogenotrophic methanogens ( Methanoculleus ) and direct interspecies electron transfer related microorganisms ( Syntrophomonas and Methanosaeta ), possibly enhancing electron exchange to accelerate methane production.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Xiaodong Ma,Tiantong Rao,Mingchen Zhao,Zhiwei Jia,Gengbo Ren,Jingyang Liu,Haiwei Guo,Zhineng Wu,Haijiao Xie
In-situ generation of iron catalysts in electro-Fenton (EF) process deserves more attention like in-situ generation of H 2 O 2 . In this work, a novel induced zero-valent iron (ZVI) electrode, which was composed of a graphite plate with good conductivity, ZVI powders and a small magnet, was for the first time designed through magnetic assembly. Fe 2+ could be slowly generated in-situ from induced ZVI electrode and effectively trigger EF oxidation of chlorobenzenes (CB) under neutral pH. Compared to the in-situ rapid release of Fe 2+ from sacrificial anodes and traditional one-time external dosing of Fe 2+ in EF, in-situ slow release of Fe 2+ from induced ZVI electrode was the most effective way to activate electrogenerated H 2 O 2 under neutral pH. Induced ZVI electrode had obvious advantages in terms of effective active areas, corrosion potentials and current responses. The optimum conditions including pH of 7.0, current of 29.9 mA, ZVI of 0.10 g and electrolysis time of 35.25 min were obtained by the response surface methodology (RSM) model with the maximum removal efficiency of 99.12%. The uniformed weak positive charge on the ZVI powders induced by the electric field was the dominant contribution to the in-situ slow release of Fe 2+ from the induced electrode. And, the impact of magnetic field on the CB removal and the release of iron ions was negligible. The degradation mechanism was revealed through the Fukui function based on the density functional theory (DFT) and by-products analysis. The evolution of acute toxicity to zebrafish in EF was further clarified. Besides, this induced ZVI electrode could be easily reused and has satisfactory stability. In briefly, this work provided a novel idea for the in-situ slow release of Fe 2+ in EF process.
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RENEWABLE ENERGY
·
2021
·
IF 8.001
Wenjing Tian,Jianhao Li,Lirong Zhu,Wen Li,Linyan He,Li Gu,Rui Deng,Dezhi Shi,Hongxiang Chai,Meng Gao
Recent investigations verified CaO 2 accelerated hydrolysis of lignocellulose, but its residue caused a harmful oxidizing environment. This study therefore proposed the combined CaO 2 pretreatment and zero-valent iron (ZVI) addition to enhance high-solid anaerobic digestion of wheat straw, trying to eliminate negative effect of residual oxides . Effects of CaO 2 pretreatment without/with ZVI addition on digestion performance were investigated. Results showed that in non-ZVI added digesters, as CaO 2 dosage increased, total production of SCOD and VFAs increased linearly, while activities of coenzyme F 420 and electron transport system were negatively correlated. Pretreatment using appropriate CaO 2 dosage indirectly increased biogas production by promoting hydrolysis and acidification. Comparably, initial ORP in ZVI-added digesters sharply declined below −350 mV, which was suitable for methanogen growth. ZVI significantly improved activities of cellulase , hemicellulase , acetic kinase and coenzyme F 420 , with the highest improvement percentages of 138%, 48%, 35% and 58%, respectively. Since ZVI could provide electrons for conversion of CO 2 to CH 4 , compared with non-ZVI added digesters (R0-R4), methane content in ZVI-added digesters (RZ0-RZ4) increased by 8.1%, 9.0%, 11.2%, 17.0% and 18.0% successively. Consequently, 0.6 g/g VS CaO 2 pretreatment combined with 0.4 g/g VS ZVI addition achieved the maximum methane production, increasing by 35.6% compared to control digester.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Ningfan Song,Zihan Chen,Jinghua Shi,Dezhi Shi,Li Gu
In the present study, a Pd/Cu bimetallic catalyst supported on a chelating resin (TP207) was prepared in order to selectively reduce nitrate to N 2 with ZVI (zero valent iron) as a reductant. The effects of Pd/Cu mass ratio, temperature, and initial solution pH on the removal of nitrate and TN were then examined. The highest nitrate (63.2%) removal was obtained under neutral conditions at a ratio of Pd/Cu 2:1, in which 57.8% of TN was removed and N 2 accounted for more than 90% of the final products. Additional ammonia (30–40%) were formed when the reaction was conducted at a higher temperature (313 K) compared to when performed at 303 K. The mechanism study for nitrate reduction indicated that this catalyst could broaden the suitable pH range and improve the selectivity of N 2 without the generation of other intermediate compounds or by-products in comparison to ZVI and its combination with a non-supported Pd/Cu catalyst. The slow rate of ZVI corrosion, high Fe(Ⅱ) proportion in corrosion products and high N/H ratio at neutral pH conditions may serve as reasons for the high N 2 selectivity. The chelating resin also played a key role via its load capacity and dispersion ability to Pd/Cu particles in enhancing N 2 selectivity. Accordingly, the proposed method may have great potential application for nitrate reduction to N 2 , which warrants further study.
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ADVANCED FUNCTIONAL MATERIALS
·
2021
·Vol. 31
·期 40
·2102917
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IF 18.808
Ruijin Sun,Shifeng Jin,Jun Deng,Munan Hao,Xin Zhong,Yuxin Ma,Mingxing Li,Xiaolong Chen
High pressure has become a powerful platform for creating and controlling novel states of matter, including high temperature ( T c ) superconductivity. However, the emergent phenomena generally disappear as high pressure is removed and cloud prospects for future applications. Here, from a distinguishing perspective, FeSe 1− x S x is reported as 2D van der Waals materials with extraordinary high- T c at ambient pressure, where the superconductivity is boosted by extreme “chemical pressure” inside the materials. Superior to external high pressure, isovalent S substitution in FeSe leads to a much greater compression rate within the superconducting iron-chalcogenide layer, which guarantees an unabridged superconducting dome that peaked at 37.5 K. Density functional theory calculations reveal that the decreased lattice and structural parameters contribute together for the shift of Fe 3d x 2− y 2 orbital, which creates a new hole-pocket at the Fermi level that intimately correlated with the enhanced superconductivity. This study demonstrates the design of materials with optimized superconductivity by introducing chemical pressure.
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JOURNAL OF ENVIRONMENTAL QUALITY
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2021
·Vol. 50
·期 5
·1123-1134
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IF 2.751
Li Liu,Jinxin Zhao,Weizhao Yin,Sihao Lv,Mei Su,Ping Li,Xiangyu Zheng,Penchi Chiang,Jinhua Wu
In this study, a collaborative system of Fe 0 and mixed anaerobic microorganisms was established for remediating chromium (Cr)-contaminated soil and restraining the translocation of Cr from soil to swamp cabbage ( Ipomoea aquatica Forssk.). Solid phase characterization demonstrated that more reactive secondary minerals such as green rust, magnetite, and lepidocrocite were generated in the composite system as compared with the Fe 0 -only system. Hence, the Fe 0 –microorganisms composite system achieved a remarkably higher aqueous Cr(VI) removal of 85.6%, 2.9 times higher than that in the Fe 0 -only system. After 14 d remediation, easily available Cr(VI) and Cr total species such as water-soluble, exchangeable, and bound-to-carbonates were converted to less available Cr(III) and Cr total species (e.g., Fe–Mn oxides-bound and organic matter-bound species) because of the production of Cr–Fe hydroxides and oxides [Cr x Fe 1−x (OH) 3 or Cr x Fe 1−x OOH] on the Fe 0 surface. A pot experiment showed that Cr uptake by swamp cabbage after the composite system remediation was suppressed by 69.1%, two times higher than that after the Fe 0 -only system remediation. Excessive Fe uptake by swamp cabbage also was efficiently inhibited by the composite system treatment due to enhanced Fe hydroxides and oxides production on the Fe 0 surface because of biological corrosion and mineralization. These results indicated that Fe 0 –microorganisms composite system remediation could efficiently enhance Cr(VI) immobilization and decrease its bioavailability and bioaccumulation by plants, which is a promising technology in Cr-contaminated soil remediation.
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CHEMOSPHERE
·
2021
·
IF 7.086
Jialin Liang,Xiaojian Liao,Maoyou Ye,Zhijie Guan,Zhihua Mo,Xian Yang,Shaosong Huang,Shuiyu Sun
The stabilization and dewaterability of waste activated sludge (WAS) are essential factors for downstream disposal or reuse. Herein, two types of zero-valent metals, zero-valent iron (Fe 0 ) and zero-valent aluminum (Al 0 ), were compared for their ability to activate peroxymonosulfate (PMS) during the WAS conditioning process, with the effects of PMS activation by these two metals on WAS dewaterability and the potential environmental risks evaluated. Results showed that compared to Al 0 /PMS treatment, Fe 0 /PMS treatment achieved superior WAS dewaterability and reduced operational costs. Using PMS combined with Fe 0 and Al 0 treatments under optimal conditions, the water content (Wc) of dewatered sludge decreased to 55.7 ± 2.7 wt% and 59.4 ± 1.3 wt%, respectively. Meanwhile, application of the Fe 0 /PMS treatment system reduced the total annual cost by approximately 33.1%, compared to the Al 0 /PMS treatment. Analysis of the dewatering mechanism demonstrated that in the Fe 0 /PMS treatment, Fe 3+ /Fe 2+ flocculation played an important role in the enhancement of WAS dewatering, while sulfate radical ( S O 4 • − ) oxidation was the dominant factor for WAS dewaterability improvement in Al 0 /PMS treatment. The greater enhancement of WAS dewaterability by Fe 0 /PMS treatment, was mainly attributed to more efficient reduction of hydrophilic extracellular polymeric substances (EPS) and an increase in surface charge neutralization. Environmental risk evaluation results indicated that Fe 0 /PMS and Al 0 /PMS treatments both effectively alleviated the environmental risks of heavy metals and faecal coliforms in dewatered sludge. Overall, this study proposes a novel perspective for the selection of an optimal PMS activator in sludge treatment .
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Gaihong Wang,Lina Qian,Xiaoyu Yong,Yajun Wang,Wei An,Honghua Jia,Jun Zhou
Oil refineries produce a variety of relatively intricate and biodegradable wastewater streams. A ternary micro-electrolysis filler (iron (Fe)-biochar (BC)-copper (Cu)) was synthesized using BC produced from waste Lycium barbarum L. branches by high-temperature anaerobic calcination, and was then used to treat oil refinery water. To evaluate the applicability of Fe-BC-Cu, the effects of various reaction parameters, including the initial pH of wastewater, Fe-BC ratio, and Fe-BC-Cu ratio, were investigated. A comparative study was conducted using three different kinds of fillers (BC, Fe-BC, and Fe-BC-Cu) to determine the reaction behavior, which was characterized by X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET) surface area analysis, scanning electron microscopy (SEM), energy dispersive spectrometry (EDS), and EDS mapping. The results of batch studies revealed that the maximum chemical oxygen demand (COD) and total organic carbon (TOC) removal efficiency was 77.11% and 68.71%, respectively, under the optimal conditions of an initial wastewater pH of 4.0, Fe-BC ratio of 1:1, and Fe-BC-Cu ratio of 1:1:1. The reusability of the Fe-BC-Cu filler was measured to ensure that the COD removal efficiency was maintained at around 80% during 10 cycles. The results of a heavy metal analysis of the effluent indicated that the application of the Fe-BC-Cu filler in wastewater treatment presented no risk of heavy metal release. The microscopic ball-shaped structure revealed by SEM facilitated a suitable micro-electrolysis reaction rate. The removal mechanism of organic pollutants in the wastewater by the Fe-BC-Cu micro-electrolysis filler could be due to the synergistic effects of electrochemical oxidation, adsorption, and coprecipitation of iron hydroxides. The extraordinary performance of the Fe-BC-Cu micro-electrolysis filler for organic pollutant removal indicated its practical potential for industrial applications.
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CHEMOSPHERE
·
2021
·
IF 7.086
Weitong Tan,Yang Ruan,Zenghui Diao,Gang Song,Minhua Su,Li'an Hou,Diyun Chen,Lingjun Kong,Hongmei Deng
Nano zero-valent iron (nZVI) is widely used for decontamination . The main issues associated with nZVI are agglomeration and oxidation in the long term. In this study, the carbothermal reduction of cotton fiber was conducted for the synthesis of nZVI supported on cotton carbon fiber (nZVI/ CF ) to address the agglomeration and oxidation of nZVI. Synergistic adsorption and peroxymonosulfate (PMS) activation using nZVI/CF for removing levofloxacin (LEV) are reported herein. The nZVI concentration and morphology were conveniently adjusted by soaking cotton fiber in ferric nitrate solutions of various Fe 3+ concentrations. The carbothermal reduction of the cotton fiber at 900 °C contributed to the reduction of Fe 3+ into nZVI. A nZVI/CF-900-0.3 system was obtained through the carbothermal reduction of cotton fiber soaked in 0.3 M ferric nitrate. Favorable adsorption of nZVI/CF-900-0.3 to LEV facilitated LEV degradation under PMS activation. Approximately 93.83% of LEV (C 0 = 20 ppm) was removed within 60 min with 0.2 g/L of the catalyst and 1 mM PMS. It was preferable to use nZVI + CF-900 to activate PMS for degrading LEV, thus confirming the favorable effect of LEV adsorption on further degradation. The nZVI/CF-900-0.3 exhibited excellent long-term stability given that it was able to activate PMS after it was stored for 6 months. ·SO 4 − played an important role in LEV degradation in the presence of PMS.
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