ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 30
·期 7
·19439-19449
·
IF 5.19
Wu Junxue,Wang Bin,Qu Han,Wang Fang,Duan Lei,Yu Gang
Phenacetin (PNT) is one of the most frequently detected nonsteroidal anti-inflammatory drugs in the water ecosystems, which poses a potential risk to environmental aquatic organisms. Acid-washed zero-valent aluminum (ZVAl) as a highly efficient activator for persulfate (PS) process was investigated to degrade PNT from the aqueous solution. The results indicated that acid-washed pretreatment for ZVAl could efficiently increase the degradation efficiency of PNT in the PS treatment. The degradation efficiency of PNT (50 μM) was up to 90% in 4 hours with the addition of 0.2 g/L acid-washed ZVAl and 8 mM PS at pH 6.8 and 25 °C. The PNT degradation followed pseudo-first order kinetics in the present system. High activator dosage, PS concentration, and reaction temperature could enhance the PNT degradation. The presence of inorganic anions (i.e., NO 3 - , HCO 3 - ) and humic acid (HA) showed inhibitory effects on the PNT degradation. The reuse results illustrated the acid-washed ZVAl material would have continuous and efficient activation performance for PS to degrade the PNT. Radical scavenger experiments and electron paramagnetic resonance indicated that both SO 4 •- and •OH were major reactive species during the PNT degradation. The possible degradation pathways of PNT mainly included the break of C–N and C–O bonds and further oxidation.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
Desalination and Water Treatment
·
2016
·
IF 1.272
Fenglian Fu,Weijiang Han,Zihang Cheng,Bing Tang
This paper deals with the treatment of hexavalent chromium (Cr(VI)) and its removal mechanism using acid-washed zero-valent aluminum (ZVAl). The acid-washed ZVAl before and after reaction was characterized by scanning electron microscope, X-ray diffraction, and X-ray photoelectron spectroscopy. The influence factors such as ZVAl loading, acid washing time, and pH values on Cr(VI) removal were studied. Cr(VI) removal by acid-washed ZVAl was also evaluated under different humic acid and Fe2+ concentrations. The removal of Cr(VI) was accelerated with increasing acid-washed ZVAl loadings and decreasing initial pH. The addition of humic acid inhibited the Cr(VI) removal, while Fe2+ significantly accelerated the Cr(VI) removal. More than 98% Cr(VI) was removed from synthetic wastewater containing 20.0 mg/L Cr(VI) in 180 min by 0.4 g/L acid-washed ZVAl at initial pH 2.0. Cr(VI) removal by acid-washed ZVAl is proved by reduction, not by adsorption. The remarkable capacity of acid-washed ZVAl in removing Cr(VI) from wastewater displays its potential application in the treatment of wastewater-containing Cr(VI).
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2014
·
IF 4.058
Zihang Cheng,Fenglian Fu,Yansong Pang,Bing Tang,Jianwei Lu
Currently, organic pollution is becoming increasingly severe with continued industrialization. In this study, the characterization of acid-washed zero-valent aluminium (AW-ZVAl) and the mechanism of using AW-ZVAl/Air/H + system in the presence of H 2 O 2 to remove phenol were investigated. The influencing factors including acid washing time, AW-ZVAl concentration, pH, H 2 O 2 concentration, air or N 2 conditions, and humic acid (HA) on phenol removal were studied. AW-ZVAl exhibited a greater capacity to remove phenol than that of ZVAl. In the presence of 4.0 mM H 2 O 2 , the phenol concentration decreased from initial 20.0 mg/L to 0.3 mg/L by 6.0 g/L AW-ZVAl in 3 h at initial pH 2.7. The addition of H 2 O 2 into AW-ZVAl/Air/H + system facilitated the reaction due to the enhancement of hydroxyl radicals generation, while the addition of HA inhibited the reaction due to the competitive reaction of HA and phenol with hydroxyl radicals. The reusing of AW-ZVAl showed that the AW-ZVAl was consistently effective in 5 cycles. The removal mechanism of phenol in the AW-ZVAl/Air/H + and AW-ZVAl/N 2 /H + were discussed. This study demonstrates that AW-ZVAl has a great potential to be applied in treating wastewater containing organic pollutants.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Wenhao Wang,Pei Gao,Chun Yang,Zhiwei Zhao,Shucong Zhen,Youxin Zhou,Tingting Zhang
Destruction of the dense oxide layer on the surface of pristine or re-passivated micro zero-valent aluminum (mZVAl) can rejuvenated its reduction activity, which is beneficial to the removal of aqueous pollutants. To rejuvenated the reduction activity of mZVAl and rapidly recovery passivated mZVAl, in this study, a novel mZVAl/nFe 3 O 4 composite with high activity and magnetic properties was synthesized by ball milling (BM). Compared with pristine mZVAl and nFe 3 O 4 , more than 95% of Cr(VI) could be removed in 30 min at 3.0 g/L mZVAl/nFe 3 O 4 dosage over a wide range of pH (3.00–11.00). The removal of Cr(VI) conformed to the pseudo-first-order adsorption kinetic model, and the equilibrium adsorption data was in accordance with the Langmuir adsorption isotherm model. The maximum absorption (8.14 mg/g) was related to the BM parameters (the weight ratio of mZVAl/nFe 3 O 4 , BM speed and BM time). Accord to the effect of co-existing ions on the removal efficiency of Cr(VI), it was proved that the significance of the adsorption process was a prerequisite step for Cr(VI) reduction. Based on X-ray photoelectron spectroscopy (XPS) and the valence analysis of aqueous Cr, the Cr(VI) removal mechanism by mZVAl/nFe 3 O 4 was also unraveled, in addition to achieving Cr(VI) reduction, also achieves the sequestration of total Cr under neutral environment. Furthermore, the reusability of mZVAl/nFe 3 O 4 was limited by the accumulation of (hydr)oxide on its surface, but can be easily rejuvenated by BM again with a small amount of nFe 3 O 4 . In conclusion, mZVAl/nFe 3 O 4 composite are a promising green material to reductive remove Cr(VI) from near-neutral wastewater.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Hanchen Wang,Yichao Xue,Shiying Yang,Yang Li,Qianfeng Li
The oxidation performance of the zero-valent aluminum (ZVAl)/persulfate (PS) combined system had been studied by researchers in the past, which relied on the activation of PS by ZVAl to generate potent oxidizing radicals (•OH and SO 4 •- ) to degrade pollutants. However, ZVAl is a strong reductant and its reduction effect cannot be ignored. The reductive performance of the ZVAl/PS combined system is still unknown. Therefore, carbon tetrachloride (CT), an antioxidant organic pollutant , was selected as the target pollutant to test the reductive performance of the ZVAl/PS system in this study. We found a significant synergistic effect between ZVAl and PS, and the ZVAl/PS combined system could rapidly degrade CT in a wide pH range of 3–11 after an induction period. By SEM-EDS, TEM, XPS, and XRD analysis, it was found that PS could promote the corrosion of the oxide film on the ZVAl surface. The quenching experiment proved that PS could accept the electrons released from ZVAl to produce superoxide radical anion (O 2 •- ), which led to the degradation of CT rather than the oxidative process by •OH and SO 4 •- . The hydrogen evolution experiment indicated that electronic reduction might play a secondary role in CT degradation. In conclusion, our study further explored the reductive performance of the ZVAl/PS combined system and expanded the pathway of CT degradation without any organic solvent addition, which provides a new strategy for the efficient degradation of refractory halogenated organic pollutants.
研究领域:
环境科学
·
化学
✓ 已验证
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Ran Yang,Jun Cai,Hu Yang
Zero-valent aluminum (ZVAl) is a promising reductant because of its relatively low redox potential , which can efficiently activate molecular oxygen to generate reactive oxygen species . However, its long-term performance is limited by the intrinsic dense oxide layer and the passivation effect of the accumulative Al-(hydr)oxide on its surface during the reaction. In this study, four clay minerals with different compositions were mixed with ZVAl by ball milling to obtain four composites of ZVAl and clay (ZVAl-Clay), which were used to degrade a high concentration of 4-chlorophenol (4-CP) under ambient conditions. The oxidation efficiencies of different ZVAl-Clays were strongly relevant to Fe contained in the clay minerals. The Fe-free ZVAl-Clay presented poor oxidation performance, whereas the reaction efficiencies of those ZVAl composites with Fe-bearing clays exhibited varying degrees of improvement. In comparison with the original ZVAl, the highest oxidation rate increased by 23 times, the maximum increased OH production was approximately 8 times, and the corresponding mineralization efficiency improved by 38.7%. However, the levels of improved oxidation performance of various ZVAl-Clays were not positively correlated with their actual total Fe contents, and their degradation efficiencies might also be affected by other physical and/or chemical properties of different clays. The synergistic mechanism revealed by various characterizations was that electron transfer might occur from ZVAl to the structural Fe(III) of the clay through the basal plane or edge of clays triggered by ball milling. Thus, the partially produced Fe(II) on the clay surface promoted the Fenton-like reaction to decompose H 2 O 2 into OH for efficient oxidation of 4-CP. In short, the ZVAl composites with Fe-bearing clays deserved further exploration as potential materials for efficient degradation of organic matters in wastewater samples.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
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 .
研究领域:
环境科学
·
污水处理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2019
·
IF 5.108
Yuting Jiang,Shiying Yang,Junqin Liu,Tengfei Ren,Yixuan Zhang,Xinrong Sun
Hexabromocyclododecane (HBCD) has been listed in Annex A of the Stockholm Convention on Persistent Organic Pollutants (POPs) in 2013, but till now there is a lack of efficient methods for its degradation. In this study, nanoscale zero-valent aluminum (nZVAl), an excellent reductant with a very low redox potential of E 0 (Al 3+ /Al 0 ) = −1.662 V and strong electron transfer ability, was used to reductively degrade HBCD. Nearly 100% HBCD was degraded within 8 h reaction at 25 °C in ethanol/water (v/v, 50/50) solution without pH adjustment. And about 67% cyclododecatriene (CDT) was obtained, which is the complete debromination product. What’s more, the yield of Br − could achieve nearly 100% after optimizing conditions. The reaction was strongly promoted by increasing the dosages of nZVAl or decreasing the initial concentration of HBCD. The temperature had the most significant influence and the degradation was completed in 40 min with elevating the reaction temperature to 45 °C. The reaction mechanism was further revealed through the characterization of nZVAl particles before and after the reaction by SEM-EDS, TEM , HRTEM , XRD, and XPS. It was found that, after corrosion of the oxide film on the surface of nZVAl, metallic aluminum inside was exposed. The reactive sites were provided and electrons released were transferred from nZVAl to HBCD, causing HBCD degraded to dibromocyclododecadiene (DBCD) and then CDT by reductive debromination. These findings imply that nZVAl can degrade HBCD efficiently with no extra energy input and this offers a new idea for better treatment of HBCD.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Xianzhe Ma,Hanchen Wang,Shiying Yang
Carbon tetrachloride (CT) is a persistent chlorinated organic pollutant frequently detected at high concentrations in industrial wastewater. CT contains four Cl electron-absorbing substituents, which make it difficult to be oxidized but more prone to be reduced. Therefore, we presented a simple and ultrafast approach for the degradation of high-concentration CT by simple physical mixing of ZVAl and KMnO 4 without any addition of organic solvents. This integrated system not only achieved rapid reductive degradation of high-concentration CT under a broad pH range of 3–11 in minutes, but also exhibited strong resistance to interference from dissolved oxygen. During the process, ZVAl and KMnO 4 activated mutually, the mechanism involves following synergistic effects: (1) the oxidation of KMnO 4 promoted the destruction of the passive oxide film on ZVAl, facilitating continuous electron release; (2) these electrons in turn reduce KMnO 4 to generate strongly oxidizing Mn(III) species; (3) the Mn(III) further accelerates ZVAl activation through a self-reinforcing cycle, ultimately facilitating rapid electron-mediated CT reduction. ZVAl/KMnO 4 combined system is expected to realize the quick treatment of CT wastewater, particularly in emergency scenarios involving accidental releases of high-concentration CT.
研究领域:
环境化学
·
污染控制
·
水处理技术
·
环境工程
·
应用化学
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Yuting Jiang,Shiying Yang,Manqian Wang,Yichao Xue,Junqin Liu,Yang Li,Dongye Zhao
Hexabromocyclododecane (HBCD) is one of the priority persistent organic pollutants (POPs), yet a cost-effective technology has been lacking for the removal and degradation of HBCD. Zero-valent aluminum (ZVAl) is an excellent electron donor. However, the inert and hydrophilic surface oxide layer impedes the release of the electrons from the core metallic Al, resulting in poor reactivity towards HBCD. In this research, a new type of modified mZVAl particles (AC@mZVAl bm/NaCl ) were prepared through ball milling mZVAl in the presence of activated carbon (AC) and NaCl, and tested for adsorption and reductive degradation of HBCD in water. AC@mZVAl bm/NaCl was characterized with a metallic Al core with newly created reactive surface coated with a thin layer of crushed carbon nanoparticles . AC@mZVAl bm/NaCl was able to rapidly (within 1 h) adsorb HBCD (C 0 = 2 mg L −1 ) and thus effectively enriched HBCD on the carbon surface of AC@mZVAl bm/NaCl . The pre-enriched HBCD was subsequently degraded by the electrons from the core Al, and ∼63.44% of the pre-sorbed HBCD was completely debrominated after 62 h of the contact. A notable time lag (∼12 h) from the onset of the adsorption to the debromination was observed, signifying the importance of the solid-phase mass transfer from the initially adsorbed AC particles to the reactive Al-AC interface. Overall, AC@mZVAl bm/NaCl synergizes the adsorptive properties of AC and the high reactivity of metallic Al, and enables a novel two-step adsorption and reductive degradation process for treating HBCD or likely other POPs.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yang Liu,Xiaowen Zhang,Fashuai Yang,Cuili Xing,Peng Fan,Yuankui Sun,Xiaohong Guan
Zero-valent aluminum (ZVAl) shows promise for environmental remediation, yet its decontamination performance under circumneutral conditions remains debated. To unravel this paradox, we employed Se(IV) and nitrate (NO 3 − ) as model pollutants to probe how contaminant-specific modulation of Al 2 O 3 transformation dictates ZVAl performance across pH 0 2.0–11.0. Results revealed that Se(IV) sequestration exhibited U-shaped kinetics with minimum efficiency at pH 0 4.0–7.0 (5.8–14.2 %), whereas NO 3 − reduction displayed an inverted U-shaped trend with maximum efficiency (> 95 %) obtained in the same pH range. Mechanistic studies demonstrated that these contrasting trends originate from pollutant-mediated Al 2 O 3 evolution. Specifically, Lewis-basicity-dependent competition for Al 2 O 3 surface sites dictates whether hydration or dissolution dominates activation. Se(IV), acting as a strong Lewis base, inhibited Al 2 O 3 hydration by competing with OH − for Al 2 O 3 surface sites and/or forming passivating Al-O-SeO 3 2− complexes , thereby self-limiting its own removal. Conversely, NO 3 − with weak Lewis basicity negligibly affected Al 2 O 3 hydration to form porous Al(OH) 3 , which can enhance electron transfer by reducing interfacial charge transfer resistance. This work resolves the long-standing pH limitation paradox in ZVAl systems by elucidating the role of Al 2 O 3 evolution, thereby offering a mechanistic framework for the design of adaptive metal-based remediation technologies.
研究领域:
环境修复
·
材料化学
·
表面化学
·
污染物去除
·
机理研究
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Ran Yang,Qianqian Chang,Na Li,Hu Yang
Sulfate radical-based advanced oxidation processes have received increasing attention in contaminated water treatment. As an excellent electron donor, microscale zero-valent aluminum (mZVAl) is a promising persulfate (PS) activator. However, the natural oxide layer of mZVAl impedes electron transfer from the core metal. Herein, a composite comprising mZVAl and Fe-bearing clay (mZVAl-NaNAu-2) was obtained through the simple ball milling (BM), which synergistically activates PS for the efficient degradation of various organic contaminants, such as 4-chlorophenol, benzoic acid, nitrobenzene, phenol, and ofloxacin, in water. The sulfate radicals and hydroxyl radicals were the main reactive species but Fe(IV) was minor in this reaction. The BM can cause fracture of the mZVAl powder and promote exposure of the fresh Al 0 surface. Various Fe species in mZVAl-NaNAu-2 at different reaction times were evaluated by extraction experiments, Mössbauer and XPS spectra. Approximately 47.0% of structural Fe(III) was reduced to Fe(II) after BM. The dissolved Fe(II) and structural trioctahedral Fe(II)-Fe(II)-Fe(II) entities were mainly responsible for the homogeneous and heterogeneous activation of PS, and corroded mZVAl acted as an “electron pool” to regenerate the aforementioned Fe(II) species continuously. The mZVAl-NaNAu-2/PS system also presented certain resistance to a natural organic matter and some anions, such as Cl - and NO 3 - . This study provided a new strategy for the efficient removal of organic contaminants from water and also solved the bottleneck of mZVAl in applications due to its dense oxide film.
研究领域:
环境科学
·
水处理
·
高级氧化过程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）