Environmental Science-Nano
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2020
·Vol. 7
·期 8
·2229-2239
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IF 7.683
Xianjun Tan,Guanhan Chen,Dingyu Xing,Wenhui Ding,Hao Liu,Ting Li,Yuxiong Huang
More and more attention has been redirected to per- and polyfluorinated alkyl substances (PFASs), particularly perfluorooctanoic acid (PFOA), owing to their ecotoxicity and environmental risks. As one of the major emerging and persistent contaminants in the environment, the current treatment processes could not remove PFOA efficiently. The recent advances in heterogeneous photocatalysis have demonstrated high efficiencies in degrading persistent contaminants, which provides an alternative approach for PFOA removal. Notably, Ga2O3-based photocatalysts exhibited great potential for PFOA remediation due to their high oxidizing capability and energy sustainability. Thus, Ga2O3 hierarchical nanosheets modified by a series of transition metals were rationally developed, and applied as heterogeneous photocatalysts for fast and efficient PFOA degradation. Noteworthily, the indium modified Ga2O3 hierarchical nanosheets achieved prominent PFOA decomposition activity, which can completely degrade 20 mg L−1 PFOA within 1 hour. The In–Ga2O3 hierarchical composites have dramatically enhanced the degradation kinetics for PFOA, which was 7.8 times higher than that of pristine Ga2O3. With in-depth mechanism investigation, we have demonstrated that In modification can not only enhance light harvesting and suppress photogenerated carrier recombination, but also favor the improvement of the adsorption ability for PFOA through the coexistence of monodentate and bidentate/bridging coordination modes. The transition metals–modification strategy paves the way for fabricating high-performance nanoscale photocatalysts for the removal of PFASs in water.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Jingzhen Wang,Chunshuai Cao,Ying Zhang,Yinqing Zhang,Lingyan Zhu
Construction of surface defects or/and exposed reactive facets is a promising strategy to improve the performance of photocatalysts . In this study, BiOF photocatalysts with tunable oxygen vacancies on the exposed (101) facets were successfully prepared by adjusting the concentration of ethylene glycol (EG). The prepared product with 50 % EG in the solution displayed remarkable photocatalytic activity for the recalcitrant pollutant perfluorooctanoic acid (PFOA), which could be completely decomposed within 6 h. The appropriate concentration of oxygen vacancy and the exposed (101) facets synergistically promoted the electron transfer from the defective surface to O 2 . Moreover, the oxygen vacancy introduced an intermediate band, which narrowed the bandgap and lowered the energy required for electron transition. DFT calculations and LC-MS-MS results revealed the principal-attack-sites of various active substances and figure out the entire PFOA degradation pathways. These profound findings are instrumental for a comprehensive understanding of the degradation process of PFOA in photocatalytic systems.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Jian Chen,Siyuan Wang,Shuyun Wang,Rong Tang,Huan Chen
As a persistent contaminant with significant risks to environment, health and ecology, perfluorooctanoic acid (PFOA) is urgent to be treated from water. To improve the performance of commercial Ga 2 O 3 in the photocatalytic degradation of PFOA, a Bi 4 O 7 -Ga 2 O 3 composite was facilely obtained through a hydrothermal route, and characterized with diverse techniques. Batch tests were conducted to evaluate the impacts from the experimental conditions on PFOA degradation, where the Bi 4 O 7 -Ga 2 O 3 composite (GaBi10) exhibited optimized photocatalytic performance stems from the enhanced light response, improved separation of photo-generated carriers, and increased adsorption capacity, attributed by Bi 4 O 7 incorporation. Furthermore, a universal parameter, catalytic efficiency ( η ) is proposed for the quantitative comparison of photocatalytic performance across different studies, which demonstrate the outstanding performance of GaBi10 in PFOA degradation, defluorination and mineralization. The quenching tests and intermediates analysis were executed to explore the mechanism underlying the photocatalytic degradation, which indicated the degradation is initiated by h + , and other active species, ·O 2 – and ·OH, propel the mineralization of the intermediates derived from PFOA. The findings provide valuable insights for developing commercial photocatalyst and understanding photocatalytic degradation of PFOA.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jiaoqin Liu,Chengjie Guo,Nannan Wu,Chenguang Li,Ruijuan Qu,Zunyao Wang,Riya Jin,Yina Qiao,Zengdi He,Jing Lu,Xingqiao Feng,Yufan Zhang,Anlong Wang,Jingshuai Gao
In this work, the kinetics and mechanisms of photocatalytic degradation of perfluorooctanoic acid (PFOA) by nitrogen-doped indium trioxide (N-doped In 2 O 3 or NH 4 NO 3 -In 2 O 3 ) under Xe lamp irradiation were systematically investigated. Nitrogen originating from various inorganic and organic nitrogen compounds was doped into In 2 O 3 to examine the catalytic effect. The NH 4 NO 3 -In 2 O 3 catalyst was characterized by SEM , TEM, FT-IR, UV-DRS, BET surface area, XPS, and XRD , and showed the best catalytic performance. After 18 h of irradiation, PFOA was almost completely degraded with addition of 5 mg catalyst, while it was hardly degraded by simulated sunlight alone. The low photocatalytic degradation efficiency of PFOA was observed in different natural waters, which was due to the inhibitory effect of high pH and common anions like SO 4 2− . The calculation results of Materials Studio showed that a shoulder-to-shoulder π system between nitrogen atom and oxygen atom (NO π*) was formed after nitrogen doping into interstitial sites of In 2 O 3 , therefore resulting in a reduction in band gap energy. Occupied NO π* states were responsible for the red shift, while unoccupied NO π* levels restrained the recombination of electrons (e − ) and holes (h + ). Nitrogen doping reduced the excitation energy for electronic transition, and thus accelerated the reaction. According to mass spectrometry analysis, decarboxylation and elimination were still the main photodegradation pathways of PFOA. To the best of our knowledge, this report is the first to explore the reaction mechanisms of PFOA in an N-doped In 2 O 3 /Xe lamp irradiation system.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Changduo Sun,Min Yu,Yuting Li,Bihui Niu,Fenghui Qin,Na Yan,Yinyin Xu,Yian Zheng
Calotropis gigantea fiber (CGF) is a natural cellulose fiber with thin-walled large lumen. Benefitted from its unique structure, CGF was utilized here as a bio-template for the fabrication of hollow carbon microtubes using a facile hydrothermal method , and simultaneously, nano-sized MoS 2 flowers were in-situ generated along the inner and outside surfaces of carbonized fiber microtubes, forming MoS 2 nanoflowers decorated biochar MoS 2 /CGB. Coupled with dual active centers from non-metallic biochar and metallic MoS 2 , MoS 2 /CGB was then used for activating peroxymonosulfate (PMS) to degrade perfluorooctanoic acid (PFOA), one emerging pollutant that had received wide attention in recent years. The experimental results indicated that at room temperature and pH 3.0, MoS 2 /CGB exhibited the degradation efficiency of 79.6% for PFOA, and removal percentage of 50.7% for total organic carbon . During the degradation process, the free radical (SO 4 •− /•OH) and non-radical ( 1 O 2 ) routes coexisted, and the amount of SO 4 •− was about 9 times that of •OH. Combined with mass spectrometry , the possible degradation pathway of PFOA was proposed as transforming into short chained C2- to C5-containing carboxylic acids. With Vibrio fischeri as an indicator, the acute toxicity of PFOA solution and intermediates was evaluated, with the inhibition rate decreased from 27.6% to 4.5%. Finally, MoS 2 /CGB had the ability not only for removing perfluorinated compounds with different carbon chain lengths, but also for catalytically degrading PFOA in tap water and Yellow River water . This work provides plant fiber-based sustainable catalyst for potential application in PMS-based system for boosting PFOA degradation.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
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2017
·
IF 4.208
Dan Wu,Xukai Li,Yiming Tang,Ping Lu,Weirui Chen,Xiaoting Xu,Laisheng Li
Zinc oxide (ZnO) nanorods were prepared by a directly pyrolysis method and employed as catalyst for perfluorooctanoic acid (PFOA) degradation. Comparative experiments were conducted to discuss the catalytic activity and flexibility of ZnO. After ZnO addition, the best PFOA degradation efficiency (70.5%) was achieved by ZnO/UV/O 3 system, only 9.5% by sole ozonation and 18.2% by UV 254 light irradiation. PFOA degradation was sensitive with pH value and temperature. The better PFOA removal efficiency was achieved at acidic condition. A novel relationship was found among PFOA degradation efficiency with hydroxyl radicals and photo-generated holes. Hydroxyl radicals generated on the surfaces of ZnO nanorods played dominant roles in PFOA degradation. PFOA degradation was found to follow the photo-Kolbe reaction mechanism. C 2 –C 7 shorter-chain perfluorocarboxylic acids and fluoride ion were detected as main intermediates during PFOA degradation process. Based on the results, a proposal degradation pathway was raised.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Yuancai Lv,Shiyu He,Shuting Liu,Zhendong Yu,Yanting Jiang,Yihui Hu,Yifan Liu,Chunxiang Lin,Xiaoxia Ye,Guifang Yang,Minghua Liu
Doping polymetals on Fe-based catalysts is proved to be an effective way to improve the performance on activating persulfate. In this paper, a highly efficient persulfate activation catalyst (FeCo@MoS 2 ) was successfully synthesized by introducing MoS 2 onto the surface of FeCo nanoboxes. During the activation of PMS the introduced of MoS 2 effectively promoted the formation of free radicals (∙OH, SO 4 · - ), 1 O 2 and Fe(IV). Due to the synergistic effects between Mo and Fe, FeCo@MoS 2 has better catalytic activity (2.01 times larger of defluorination efficiency and 3.91 times larger of the apparent rate constant ( k obs )) than FeCo. Under the optimal conditions (catalyst dosage of 0.2 g L −1 , PMS dosage of 1.0 g L −1 and initial pH 4.0), the perfluorooctanoic acid (PFOA, 10 mg L −1 ) could be degraded in 60 min, with 90.26 ± 2.64% of the defluorination efficiency. The LC- MS results showed that under the attack of free radicals (∙OH, SO 4 · - ), 1 O 2 and Fe(IV), the PFOA underwent step-by-step defluorination process. In addition, the ECOSAR results showed that during the whole degradation of PFOA in FeCo@MoS 2 /PMS system, no highly toxic intermediates was accumulated, suggesting a green degradation process. This work showed new ideas and strategies for studying the influence of polymetallic doping on the catalytic process of PMS multiphase catalytic system.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2025
·
IF 8.4
Jun Xiao,Juan Huang,Yucheng Chen,Ying Wang,Xiuwen Qian,Dengping Liu,Yuan Cao
Constructed wetland (CW) serve as the final ecological barrier for hazardous materials entering the natural water environment. Due to the ecological toxicity and difficult bioutilization characteristics of perfluorooctanoic acid (PFOA) itself, CW technology faces great challenges in the field of PFOA remediation. In this study, nano zero-valent iron (nZVI) was introduced into CWs to explore the mechanism of the synergistic removal of PFOA and nutrients in nZVI-CW system. The results indicated that the addition of 10 mg/L nZVI improved the removal efficiency of CW for 1 and 10 mg/L PFOA, with an average removal rate increased by 3.53–8.70%. The transformation products in CW effluents were qualitatively detected using HPLC-Q-TOF-MS, suggesting that the degradation of PFOA may involve decarboxylation, hydrolysis, redox, elimination, substitution and intramolecular rearrangement processes. The presence of nZVI enhanced the average removal rates of NH 4 + -N, NO 3 − -N and TP by 2.78–18.4% in CWs. The increase in key substrate enzyme activity confirmed the stimulating effect of nZVI on microbial activity. The addition of nZVI facilitated the growth and enrichment of hydroautotrophic denitrifying bacteria, nitrat-dependent iron-oxidizing bacteria, and dissimilatory iron-reducing bacteria. Two types of dissimilatory iron-reducing bacteria ( Geobacter and Acinetobacter ) may be potential PFOA-degrading bacteria. Additionally, signaling pathways related to carbohydrate metabolism, energy metabolism, and xenobiotic degradation and metabolism exhibited higher abundance in the nZVI treated groups.
研究领域:
环境科学
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生态学
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微生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Jingzhen Wang,Chunshuai Cao,Yuanyuan Wang,Yingnan Wang,Binbin Sun,Lingyan Zhu
The strong persistence, wide presence and potential toxicities of perfluorooctanoic acid (PFOA) in aquatic environment makes it a challenge to develop advanced technologies to eliminate it from water. In this study, novel BiOI@Bi 5 O 7 I p-n heterojunction photocatalysts were facilely prepared by calcinating BiOI at 350 °C < T < 410 °C. Under simulated solar light irradiation, the degradation rate constant ( k = 0.247 h −1 ) of PFOA by the BiOI@Bi 5 O 7 I heterojunction prepared at 390 °C (T-390) was four times of that by pristine BiOI ( k = 0.061 h −1 ) and 1.2 times of that by Bi 5 O 7 I (prepared at 410 °C, k = 0.206 h −1 ). T-390 also exhibited excellent mineralization efficiency by removing about 60% of total organic carbon in 6 h of irradiation. The significantly enhanced photocatalytic activity of BiOI@Bi 5 O 7 I composite was mainly attributed by the unique band gap structure of the p-n heterojunction, which enhanced the visible-light absorbance and accelerated the separation of photogenerated charge carriers. The generated intermediate products were analyzed by ultra-performance liquid chromatography-mass spectrometry, and the results indicated that PFOA was decomposed by stepwise losing CF 2 units. The BiOI@Bi 5 O 7 I heterojunction also possessed very good durability and reusability, displaying a great potential in PFOA containing water treatment.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Jingzhen Wang,Chun-Shuai Cao,Yinqing Zhang,Lingyan Zhu
Perfluorooctanoic acid (PFOA) is refractory owing to the strong C-F bonds and is extremely difficult to be degraded by traditional photocatalysts. In this study, an S-scheme heterojunction was successfully synthesized by incorporating BiOF with wide-bandgap Bi 7 O 5 F 11 . Theoretical calculations, in situ X-ray photoelectron spectroscopy and Kelvin probe force microscopy verified that a build-in electric field was created in the heterojunction, facilitating the separation of electron-hole pairs. Thus, the photoexcited electrons in the conduction-band (CB) of BiOF rapidly recombined with holes in the valence-band (VB) of Bi 7 O 5 F 11 , leading to enrichment of the highly reductive electrons in CB of Bi 7 O 5 F 11 and strongly oxidative holes in VB of BiOF. Additionally, the strong interaction between Bi 7 O 5 F 11 /BiOF and PFOA is conducive to electron transfer from catalyst surface to PFOA. Thus, BOF-2 displayed superbly-high photoactivity to decompose PFOA. PFOA (5 mg/L) was decomposed within 1 h, and 53% of total-organic-carbon was removed in 2 h of irradiation.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2018
·
IF 3.927
Dan Wu,Xukai Li,Jingxian Zhang,Weirui Chen,Ping Lu,Yiming Tang,Laisheng Li
ZnO-reduced graphene oxide (ZnO-rGO) was synthesized successfully at 423 K by a hydrothermal method. The presence of reduced graphene oxide significantly improved the photocatalytic performance of ZnO and its optimal loading ratio was 0.6 wt%. The XRD, SEM, UV–vis and FT-IR were applied to characterize the prepared catalyst. Comparative experiments were conducted to evaluate perfluorooctanoic acid (PFOA) degradation efficiency and the results showed that 99.2% PFOA was degraded in persulfate-assisted photocatalytic ozonation with low dosage of ozone and persulfate at room temperature. The impact factors on PFOA degradation efficiency including loading ratios of GO on ZnO, reaction temperatures and persulfate concentration were inspected and analyzed. The sodium persulfate and ammonium persulfate were compared as common oxidants in photocatalytic ozonation for PFOA degradation and sodium persulfate showed the better PFOA removal. Chloride and humic acid (HA) were common substances in natural water, and they showed inhibition effects on PFOA degradation. Conversion of persulfate to sulfate ion was studied and persulfate concentration during PFOA oxidation was monitored. PFHpA, PFHeA, PFPeA and PFBA were main intermediates during PFOA degradation.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Xudong Zhou,Yashi Zhong,Rui Bai,Wei Chen,Junpeng Li,Lifeng Lin,Xiaochun Tian,Feng Zhao
Per and polyfluoroalkyl substances (PFAS) present profound environmental and health hazards owing to their chemical persistence. Photocatalytic technology harnesses solar energy to generate reactive oxygen species for pollutant degradation. However, prevailing studies have emphasized hydroxyl radical mediated pathways. The short lifetime of hydroxyl radical and the stringent conditions required for its formation constrain the efficiency of this approach against recalcitrant PFAS such as perfluorooctanoic acid (PFOA). In this study, a ZnIn 2 S 4 photocatalyst enriched with sulfur vacancies is synthesized via a facile hydrothermal-calcination approach. The introduction of sulfur vacancies enhances visible light absorption and promotes efficient separation of photogenerated electron-hole pairs. Theoretical calculations further reveal that sulfur vacancies enhance the kinetics of oxygen evolution, oxygen adsorption capacity, and the efficiency of singlet oxygen ( 1 O 2 ) generation, reducing the activation barriers throughout the oxygen activation cascade. Combined electron paramagnetic resonance spectroscopy and radical quenching experiments confirm 1 O 2 as the dominant reactive oxygen species responsible for PFOA degradation, operating via a non-hydroxyl radical mechanism. The catalyst achieves over 93% degradation efficiency for 50 µg L −1 PFOA in surface water and aquaculture wastewater, demonstrating the application potential of sulfur vacancy-engineered photocatalytic systems for the effective remediation of trace emerging contaminants in actual environments.
研究领域:
环境科学
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材料化学
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光催化
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水处理
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污染物降解
✓ 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）