CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Zhuo-Yu Li,Yu-Lei Liu,Pei-Nan He,Xin Zhang,Lu Wang,Hai-Teng Gu,Hao-Chen Zhang,Jun Ma
Hydroxylamine is commonly known to enhance the performance of Fe(II)-based advanced oxidation processes (AOPs) by promoting Fe(II) regeneration from Fe(III). Recently, ferryl ion (Fe(IV)) was found as an important reactive specie in Fe(II)/peroxydisulfate (PDS) system, while the interaction between hydroxylamine and Fe(IV) in Fe(II)/hydroxylamine/PDS system was still ambiguous. Therefore, the role of hydroxylamine, especially in interaction with reactive species, was systematically studied therein. With methyl phenyl sulfoxide (PMSO) as a probe compound, an original function of hydroxylamine to transform the major reactive species from Fe(IV) to radicals (SO 4 - and OH) for potential pollutants oxidation was clarified. Experimental results combined with Density Functional Theory (DFT) calculations showed that SO 4 - , OH and Fe(IV) all contributed to PMSO oxidation. Hydroxylamine showed the greatest promotional effect on the production of SO 4 - , while the production of Fe(IV) was inhibited with concentrations of hydroxylamine increasing from 0.2 to 1.4 mM. Compared with PMSO, hydroxylamine showed stronger scavenging ability towards Fe(IV) than SO 4 - and OH. Thus, more than 50% of radicals was consumed by PMSO and Fe(IV) mainly reacted with hydroxylamine to regenerate Fe(II). In a word, hydroxylamine played a dual role during potential pollutants oxidation in Fe(II)/hydroxylamine/PDS system, namely (1) transforming the major reactive species from Fe(IV) to radials (SO 4 - and OH) and (2) regenerating Fe(II) from both Fe(IV) and Fe(III). This study provides an insight into the role of hydroxylamine and its interactions with Fe(IV), which advances our understanding on similar Fe(II)/reductants/PDS systems.
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Nature Sustainability
·
2021
·Vol. 4
·期 7
·618-626
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IF 19.346
Chen Yao,Xu Mengjiao,Wen Jieya,Wan Yu,Zhao Qingfei,Cao Xia,Ding Yong,Wang Zhong Lin,Li Hexing,Bian Zhenfeng
Precious metals such as gold and platinum are valued materials for a variety of important applications, but their scarcity poses a risk of supply disruption. Recycling precious metals from waste provides a promising solution; however, conventional metallurgical methods bear high environmental costs and energy consumption. Here, we report a photocatalytic process that enables one to selectively retrieve seven precious metals—silver (Ag), gold (Au), palladium (Pd), platinum (Pt), rhodium (Rh), ruthenium (Ru) and iridium (Ir)—from waste circuit boards, ternary automotive catalysts and ores. The whole process does not involve strong acids or bases or toxic cyanide, but needs only light and photocatalysts such as titanium dioxide (TiO 2 ). More than 99% of the targeted elements in the waste sources can be dissolved and the precious metals recovered after a simple reducing reaction that shows a high purity (≥98%). By demonstrating success at the kilogram scale and showing that the catalysts can be reused more than 100 times, we suggest that this approach might be industry compatible. This research opens up a new path in the development of sustainable technologies for recycling the Earth’s resources and contributing to a circular economy.
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Nano Research
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2021
·Vol. 14
·期 7
·2363-2371
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IF 8.897
Lv Yan,Yue Lin,Khan Imran Mahmood,Zhou You,Cao Wenbo,Niazi Sobia,Wang Zhouping
Herein, we report the fabrication of Fe 3 O 4 @TiO 2 nanosheet/Ag/g-C 3 N 4 (Fe 3 O 4 @ns-TiO 2 /Ag/g-C 3 N 4 ) composite photocatalysts with well-designed hierarchical yolk-shell structure. To endow the composites with fascinating features, multiple functional components are perfectly integrated into the definite structure. The photodegradation experiments of organic pollutants revealed a significant enhancement in photocatalytic activity of developed composites as compared to P25, which is mainly due to the synergetic interaction of the tailored three-dimensional (3D) yolk-shell porous nanostructure, extended sunlight response range, and retarded the recombination probability of photogenerated electrons-holes. More importantly, the hybrid samples exhibited superior magnetic properties due to the magnetic component. The excellent magnetic recyclability and reusability of the photocatalysts are verified by the magnetic hysteresis loop and cyclic photocatalytic degradation experiments, which is significant for the green and sustainable applications of photocatalysts. Considering its remarkable photocatalytic performance and expectant magnetic recyclability, the composite photocatalysts are expected to be a promising candidate to dispose of future environmental issues.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Bihui Niu,Min Yu,Changduo Sun,Luhan Wang,Kun Zang,Xiaowen Hu,Lei Zhou,Yian Zheng
Perfluorooctanoic acid (PFOA) is an anthropogenic persistent organic compound that resistant to traditional oxidative decomposition, bringing thus huge pressure to the environment. Here, the open hollow structured Calotropis gigantea fiber (CGF) was developed using a facile pyrolysis and subsequent magnetization method, and the resulting magnetic carbonized fiber (MC-CGF) was applied as an efficient catalyst for PFOA decomposition at room temperature in persulfate-based oxidation process. The experimental results indicated that with the addition of MC-CGF, the removal efficiency of PFOA could reach to 75.76% at 30℃ and pH 2.0. By calculation, the apparent activation energy was reduced from 62.76 kJ/mol to 22.49 kJ/mol, demonstrating that in the presence of MC-CGF, a lower reaction temperature and a shorter time were enough to reach the higher efficiency for PFOA decomposition. Mechanism research showed that during the decomposition process, PFOA underwent a first decarboxylation process and two possible decomposition pathways should also be taken into discussion. Taking pakchoi as the plant model, the process toxicity was finally evaluated, and the changes in chlorophyll content stated that the decomposition process of PFOA by MC-CGF assisted persulfate system was relatively harmless and environmental-friendly.
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Journal of Cleaner Production
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2021
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IF 9.297
Wuming Xie,Zijun Huang,Fengping Zhou,Yuhui Li,Xiaolin Bi,Qiushi Bian,Shuiyu Sun
The presence of the antibiotics in wastewater and drinking water is causing increasing concern around the world, thereby an advanced sustainable technology needs to be developed to remove the antibiotics from water resources. In this study, Metal-organic frameworks (MOFs) derived zero-valent iron embedded in the carbon matrix structure named FMC is prepared by a direct pyrolysis of Fe-based metal organic framework. FMC is used as a heterogeneous Fenton-like catalyst to degrade amoxicillin (AMX) based on the oxidation and degradation reactions. FMC had the strengthened catalytic performance for amoxicillin elimination with high mineralization efficiency (60.41%), which was evaluated over various experimental conditions. The role of reaction in FMC/H 2 O 2 system was identified, suggesting amoxicillin was eliminated by the attack of hydroxyls radicals (·OH). The carbon structures can facilitate the passage of electrons and boost the contact of zero valent iron and Fe 2+ species on FMC surface with H 2 O 2 , resulting in the accelerated production of ·OH and high removal efficiency of amoxicillin. By defining reactive oxidizing species and degradation intermediates, the plausible degradation pathways of amoxicillin have been inferred. This study revealed that FMC/H 2 O 2 system has high AMX degradation efficiency and decent recyclability .
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Weilu Yang,Minghua Zhou,Lei Mai,Huase Ou,Nihal Oturan,Mehmet A. Oturan,Eddy Y. Zeng
Low yields of H 2 O 2 and a narrow range of appropriate pH values have been two major drawbacks for electro-Fenton (EF) process. Herein, metal-free electrochemical advanced oxidation processes (EAOPs) were developed with nitrogen and sulfur co-doped electrochemically exfoliated graphene (N, S-EEGr) electrocatalysts, which was confirmed as an outstanding bifunctional catalyst for synchronous generation and activation of H 2 O 2 via (2 + 1) e − consecutive reduction reactions. Specifically, two elements (N, S) in metal-free N, S-EEGr-CF cathode synergize to promote the formation of H 2 O 2 followed by its activation. With N, S-EEGr-CF cathode, phenol of initial 50 mg L −1 could be effectively removed within pH 3–11 and 6.25 mA cm −2 , and 100% removal efficiency could be achieved within 15-min even at neutral pH. The pseudo-first-order rate constant for phenol removal in metal-free EAOPs with N,S-EEGr-CF at neutral pH was 10 times higher than that with EF process. Detection of active species, coupled with decay kinetics with specific trapping agents, confirmed that OH was the dominant oxidizing species promoting removal efficiencies of organics (phenol, antibiotics and dyes) at pH 3 and pH 7. In the actual wastewater treatment, the synergistic effect of bifunctional catalyst would also be used for improving the degradation efficiency of organics. Thus, the metal-free EAOPs with N,S-EEGr-CF cathode may serve as an alternative in wastewater treatment with a broadened range of solution pH values and avoiding Fe 2+ (catalyst) addition.
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PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2021
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IF 6.707
Hailan Qin,Yushan Zhang,Shuaijun He,Zeyu Guan,Yintao Shi,Xinyi Xie,Dongsheng Xia,Dongya Li,Haiming Xu
Increasing the migration and separation efficiencies of photogenerated carriers can enormously enhance photocatalytic properties. Thus, a novel CQDs/BiOCl nanocomposite with rich oxygen vacancies (OVs) was effectively synthesized via a hydrothermal method by using maltitol as a carbon source to address these issues. The photocatalysts were characterized by XRD, SEM, TEM, FT-IR, BET, XPS, PL, EIS, I-t, DRS and ESR. The experimental results demonstrate that BOC-1 can purify 72% tetracycline hydrochloride (10 mg/L, TC-HCl) within 60 min, which is 4 times higher than pure BiOCl. Moreover, photocatalytic mechanism was thoroughly studied and verified that the cooperation of point discharge effect (PDE) and rational OVs concentration induced by carbon quantum dots (CQDs) can significantly enhance the migration and separation of photo-induced carriers, thereby leading to high photocatalytic activity of the as-prepared nanocomposites. In addition, the contribution of the free radicals was comprehensively calculated based on trapping experiments. the contributions of ·OH, ·O 2 - and 1 O 2 are 6.38%, 48.94% and 8.51%, respectively. This study provides a promising strategy to boosting the photoinduced carrier transfer properties by the coupling of point discharge effect and defect engineering.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Hongwei Luo,Chenyang Liu,Ying Cheng,Yifeng Zeng,Dongqin He,Xiangliang Pan
The biggest problem with Fe/PMS (peroxymonosulfate) system is the slow generation rate of SO 4 − due to inefficient Fe 3+ /Fe 2+ cycle and the low decomposition efficiency of PMS . Here, we report the Fe 3+ -enhanced decomposition of PMS by a two-dimensional transition metal dichalcogenide WS 2 for pollutant degradation and E. coli disinfection. Experimental results showed that the removal rates of six representative pollutants were all above 90% under various pH conditions. Over a wide range of pH values (2–9), the removal rate of carbamazepine (CBZ) in PMS/WS 2 /Fe 3+ system almost reached 100% within 10 min, and E. coli could be inactivated by 97.3% within 1 min. WS 2 in the system accelerated the Fe 3+ /Fe 2+ cycle and participated in the activation of PMS. Electron paramagnetic resonance (EPR) measurements and scavenging experiments demonstrated that the SO 4 − and HO radicals were the main active oxidative species. The degradation pathway of CBZ was revealed based on its intermediates as determined by liquid chromatograph-mass spectrometer (LC-MS). The presence of common anions such as Cl − and HCO 3 − in PMS/WS 2 /Fe 3+ system noticeably affected the CBZ degradation. The characterization results verified the structural stability and the reusability of WS 2 . These research findings suggest that the combination of Fe 3+ and WS 2 is a promising method for PMS activation to remove organic pollutants and inactivate pathogenic bacteria during the process of wastewater treatment .
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Polymers
·
2021
·Vol. 13
·期 10
·1570
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IF 4.329
Naiku Xu,Mengru Ren
Polytetrafluoroethylene emulsion was ultrasonically mixed with an extremely spinnable poly(acrylic acid-co-hydroxyethyl methacrylate) solution to get a dispersion with good spinnability, and the obtained dispersion was then wet-spun into water-swellable fiber. Crosslinking agents and iron species were simultaneously introduced into the water-swellable fiber through simple impregnation and water swelling. A composite fiber with Fenton reaction-catalyzing function was then fabricated by sequentially conducting crosslinking and sintering treatment. Due to crosslinking-induced good resistance to water swelling and PTFE component-induced hydrophobicity, the composite fiber showed a highly stable activity to catalyze H2O2to oxidatively decolorize methylene blue (MB). Within nine cycles, the composite fiber could decolorize more than 90% of MB within one minute in the presence of H2O2and did not show any attenuation in MB decolorization efficiency. The composite fiber still could reduce the total organic carbon of MB aqueous solution from 18.3 to 10.3 mg/L when used for the ninth time. Therefore, it is believable that the prepared fiber has good and broad application prospects in the field of dye wastewater treatment.Keywords:composite fiber;heterogeneous Fenton catalyst;water-swelling resistance;hydrophobicity;methylene blue oxidative decolorization
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Journal of Environmental Sciences
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2021
·
IF 5.565
Yaqian Shen,Ke Zhu,Dongdong He,Jin Huang,Hongmei He,Lele Lei,Wenjin Chen
Recently, metal-based carbon materials have been verified to be an effective persulfate activator, but secondary pollution caused by metal leaching is inevitable. Hence, a green metal-free 3D macroscopic N-doped porous carbon nanosheets (NPCN) was synthesized successfully. The obtained NPCN showed high adsorption capacity of tetracycline (TC) and excellent persulfate (PS) activation ability, especially when calcined at 700 °C (NPCN-700). The maximum adsorption capacity of NPCN-700 was 121.51 mg/g by H-bonds interactions. Moreover, the adsorption process followed pseudo-second-order kinetics model and Langmuir adsorption isotherm. The large specific surface area (365.27 mg/g) and hierarchical porous structure of NPCN-700 reduced the mass transfer resistance and increased the adsorption capacity. About 96.39% of TC was removed after adding PS. The effective adsorption of the catalyst greatly shortened the time for the target organic molecules to migrate to the catalyst. Moreover, the NPCN-700 demonstrated high reusability with the TC removal rate of 80.23% after 4 cycles. Quenching experiment and electron paramagnetic resonance (EPR) test confirmed the non-radical mechanism dominated by 1 O 2 . More importantly, the C = O groups, defects and Graphitic N acted as active sites to generate 1 O 2 . Correspondingly, electrochemical measurement revealed the direct electron transfer pathway of TC degradation. Finally, multiple degradation intermediates were recognized by the LC-MS measurement and three possible degradation pathways were proposed. Overall, the prepared NPCN had excellent application prospects for removal of antibiotics due to its remarkable adsorption and catalytic degradation capabilities.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Libo Zhang,Lianxiang Qiu,Qingyao Zhu,Xiong Liang,Jingxiong Huang,Mengting Yang,Zhenxuan Zhang,Jiang Ma,Jun Shen
Water disinfection would result in unintended formation of halogenated disinfection by-products (DBPs) which pose potential harm to human health. In present work, Fe 78 Si 9 B 13 amorphous ribbons (Fe-Si-B AR ) showed excellent catalytic degradation performance towards an aromatic DBP, 3,5-dichlorosalicylic acid (3,5-DiClSA) by Fenton-like reaction. The catalytic degradation performances of Fe-Si-B AR , Fe 78 Si 9 B 13 crystalline ribbons (Fe-Si-B CR ) and iron powders towards 3,5-DiClSA were compared, and Fe-Si-B AR (0.0166 min −1 ) showed the fastest degradation rate. The faster surface mobility of Fe-Si-B AR , which made it easy for Fe 2+ to be oxidized by H 2 O 2 , facilitated the degradation process. High-valent iron of Fe IV could be generated which accounted for degradation of 3,5-DiClSA. The Fe-Si-B AR also showed better and better catalytic performance in 10 reuse cycles. Besides, the cytotoxicity tests indicated that the overall toxicity level of 3,5-DiClSA was declined by 88.1 % after degradation by Fe-Si-B AR . Our results showed that Fe-Si-B AR is a promising catalyst for the degradation of aromatic DBPs.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Li Li,Qian Zhang,Yuecheng She,Yongbo Yu,Junming Hong
Mn–Fe bimetal catalyst possesses excellent activation properties, and the enhancement of Mn/Fe redox cycle for electron transfer is related to the crystalline structure and surface functional groups. Therefore, material structure optimization is an effective strategy to improve its activation performance in advanced oxidation . In this study, Mn–Fe LDO catalyst with strong Mn/Fe synergistic effect was synthesized, and used for bisphenol A degradation. Under the condition of 0.4 g/L Mn-Fe LDO, 1.5 mM PMS and pH 7.0, Mn-Fe LDO/PMS system exhibited excellent degradation performance that 100% of BPA (20 mg/L) and 72.0% of COD could effective be degraded within 50 min. Five-run recycle and metal ions leaching experiments proved the excellent reusability and stability of Mn-Fe LDO. To deepen the understanding of catalytic mechanism, the synergistic effect and electron transfer between Mn and Fe were confirmed via XPS and CVs results. Moreover, the indispensable role of surface hydroxyl groups were clarified via phosphate masking experiment, ATR-FTIR and LSV analysis. The presence of Mn and Fe active sites and hydroxyl groups on Mn-Fe LDO surface could efficiently promote electron transfer, thus accelerating the redox cycles of Mn 3+ /Mn 2+ and Fe 3+ /Fe 2+ . The generation of SO 4 ·− and HO· as the main radicals was occurred on the surface of Mn-Fe LDO, and SO 4 ·− played a major role during the reaction. On the basis of these experimental conclusions, the mechanisms of Mn–Fe LDO/PMS system for high-efficiency BPA degradation were proposed. GC-MS analysis was performed to detect the BPA degradation intermediates and propose the possible degradation pathways.
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