APPLIED CATALYSIS A-GENERAL
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2022
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IF 5.723
Chao Yin,Yali Liu,Xiaorong Kang,Xin Li
Graphitic carbon nitride (g-C 3 N 4 , CN) has been applied to degrade a variety of pollutants. However, two major defects, the low utilization of light energy and the high recombination of photogenerated electron and hole (e - -h + ) pairs, need to be improved. In this study, a LED-light-driven photocatalyst, carbon dots decorated graphitic carbon nitride (CNC), was successfully prepared by simple thermal polymerization. Due to the remarkable up-conversion photoluminescence properties and superior charge transport capability of CDs, CNC had higher e - -h + separation efficiency and broader visible light response. In this experiment, a combined process of CNC and persulfate (CNC/PS) was used for tetracycline (TC) degradation. High-efficient photocatalytic degradation rate of 81.9% was obtained in the CNC/PS system. Moreover, the mechanism analysis indicated that the reaction between PS and photogenerated e - effectively promoted the separation of electrons-holes pairs, thereby enhancing the formation of dominant active radicals •O 2 - and holes for TC degradation.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
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IF 10.753
Xiaoyu Jiao,Rui Zeng,Guangcai Lan,Siyu Zuo,Jun He,Chengjun Wang
The reactive iodine species may exhibit significant impacts on many global atmospheric issues and the I • /I 2 •− radicals play key roles for inducing the formation of these reactive iodine species. However, the current understanding on the formation of I • /I 2 •− radicals in atmospheric aqueous aerosol is still quite limited. The results reported herein suggest that I • /I 2 •− can be produced simultaneously in aqueous aerosol by several sunlight-driven photochemical pathways including direct photo-dissociation of soluble organic iodine (SOI) at rates of 0.10–1.34 × 10 −9 M ns −1 and 0.99–5.68 × 10 −7 M μs −1 , • OH-mediated oxidation of I − at 0.03–1.41 × 10 −8 M ns −1 and 0.05–4.10 × 10 −6 M μs −1 , and 3 DOM ⁎ -induced oxidation of I − at 1.57–1.65 × 10 −9 M ns −1 and 0.99–5.68 × 10 −7 M μs −1 for generation of I • and I 2 •− , respectively. Meanwhile, the pathway of e aq − -initiated stepwise reduction of IO 3 − to I 2( aq ) and further photolyzed into I • plays negligible role in formation of I • /I 2 •− due to the low reaction rates and severe quenching effect of e aq − by dissolved O 2 . Our work presented the new data on mechanism and kinetics for comprehensive elucidation of I • /I 2 •− formation in coastal atmospheric aqueous aerosol and would help to better understand the transformation mechanism of iodine species, pathways of iodine cycling and the associated environmental impacts involving atmospheric reactive iodine radicals.
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ELECTROCHIMICA ACTA
·
2022
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IF 7.336
Xuedong Du,Pei Su,Wenyang Fu,Qizhan Zhang,Minghua Zhou
To improve the mineralization efficiency of heterogeneous electro-Fenton (Hetero-EF), ultraviolet (UV) process and Hetero-EF process were coupled (Hetero-PEF) for degradation of sulfamethazine (SMT) by FeCu@PC (porous carbon) derived from metal-organic frameworks (MOFs). At 60 min, the total organic carbon (TOC) removal and mineralization current efficiency (MCE) of the Hetero-PEF process was 73.3% and 58.7%, which were both 2.23 times that of the Hetero-EF process due to the photoelectric synergy. Moreover, the Hetero-PEF process had wider pH applicability (3.0–7.0) than the Hetero-EF process. This process could also efficiently remove phenol , carbamazepine and 2, 4-D. Through process comparison, quenching and electron paramagnetic resonance (EPR) tests, the reasons for the improvement of mineralization efficiency by Hetero-EF process were disclosed, in which UV not only activated H 2 O 2 to produce • OH but also excited FeCu@PC to form photo-generated electrons to catalyze H 2 O 2 or O 2 to • OH and O 2 • − , respectively. In addition, UV excitation of Fe(OH) 2+ and Fe(OOCR) 2+ promoted the regeneration of Fe 2+ , which also greatly enhanced the H 2 O 2 conversion efficiency and mineralization current efficiency. In the five cycles of experiments, the removal efficiency of SMT still reached 97.0%. The FeCu@PC/Hetero-PEF process had the application prospect of highly effective removal of organic pollutants in water treatment.
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Journal of Environmental Sciences
·
2022
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IF 6.796
Le Thi Thao,To Van Nguyen,Van Quy Nguyen,Ngoc Man Phan,Ki Jae Kim,Nguyen Nhat Huy,Nguyen Trung Dung
Wastewater containing an azo dye Orange G (OG) causes massive environmental pollution , thus it is critical to develop a highly effective, environmental-friendly, and reusable catalyst in peroxymonosulfate (PMS) activation for OG degradation. In this work, we successfully applied a magnetic MnFe 2 O 4 /α-MnO 2 hybrid fabricated by a simple hydrothermal method for OG removal in water. The characteristics of the hybrid were investigated by X-ray diffraction, scanning electron microscopy, energy‐dispersive X‐ray spectroscopy, Fourier transform infrared spectroscopy , Brunauer–Emmett–Teller method, vibrating sample magnetometry, electron paramagnetic resonance, thermogravimetric analysis , and X-ray photoelectron spectroscopy. The effects of operational parameters (i.e., catalytic system, catalytic dose, solution pH, and temperature) were investigated. The results exhibited that 96.8% of OG degradation was obtained with MnFe 2 O 4 /α-MnO 2 (1:9)/PMS system in 30 min regardless of solution pH changes. Furthermore, the possible reaction mechanism of the coupling system was proposed, and the degradation intermediates of OG were identified by mass spectroscopy . The radical quenching experiments and EPR tests demonstrated that SO 4 • ̶ , O 2 • ̶ , and 1 O 2 were the primary reactive oxygen species responsible for the OG degradation. The hybrid also displayed unusual stability with less than 30% loss in the OG removal after four sequential cycles. Overall, magnetic MnFe 2 O 4 /α-MnO 2 hybrid could be used as a high potential activator of PMS to remove orange G and maybe other dyes from wastewater.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2022
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IF 7.926
Meng Qiao,Lujing Fu,Damia Barcelo
Polycyclic aromatic hydrocarbons (PAHs) ubiquitously exist in aqueous environment , posing considerable chronic and acute ecological risk to aquatic species. Non-metallic photocatalyst g-C 3 N 4 is a promising photocatalyst that can be used in river remediation under visible light irradiation. The removal of a typical PAH phenanthrene (PHE) by g-C 3 N 4 under visible light was detailed studied. The removal efficiency of PHE (initial concentration 5 mg/L) by g-C 3 N 4 -nano sheet (NS) (1 g/L) reached 100% within 10 min under visible light. Reactive oxygenated species, including •O 2 - , 1 O 2 , and •OH, were generated in the g-C 3 N 4 -NS/visible light system. •O 2 - and 1 O 2 were determined as the main active species , whereas photoelectric-hole and •OH were also involved in the reaction. The effects of co-existed substances were investigated, including humic acid (HA), Cl - , and NO 3 - . HA decreased the removal rate of PHE, probably due to its reaction with photo-generated holes. Cl - with lower concentration (0.2 – 10.0 mmol/L) decreased the removal rate of PHE, while with higher concentration (20 mmol/L) increased the removal rate of PHE, probably because of the interaction of Cl - with •OH. NO 3 - with the concentration of 10–100 μmol/L did not significantly affect the removal rate of PHE. This study will provide a possible in-situ route for the removal of typical PAHs in urban river environment.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Yuhan Long,Songrong Li,Peizhen Yang,Xi Chen,Wenhao Liu,Xuesong Zhan,Cheng Xue,Dongfang Liu,Wenli Huang
MOF-derived metal-carbon composite catalyst was an alternative high-efficient catalyst for activating peroxymonosulfate (PMS). In this study, a novel cobalt-carbon-nitrogen doped composite catalyst with honeycomb porous structure (Co-HPNC) was obtained through a simple strategy consisting of three steps: self-growth of ZIF-67 on the SiO 2 core, pyrolysis, and NaOH etching away SiO 2 core. The Co-HPNC exhibited an outstanding catalytic performance (98.1% in 10 min) to activate PMS for acid orange 7 (AO7) degradation. The observed reaction kinetic constant (0.4319 min −1 ) was 2.64 times superior to that of the unmodified Co/NC catalysis system (0.1636 min −1 ). In the meantime, the catalyst demonstrated a high PMS activation capacity over a wide pH range of 3–11 and strong adaptability to the high concentration of inorganic anions (Cl - , SO 4 2- , and CO 3 2– ). After being recycled three times, the removal efficiency could still reach 92.7% in 25 min. The quenching tests and EPR spectrum illustrated the existence of radical and non-radical pathways, in which singlet oxygen was dominant during the degradation process. It was hypothesized that Co(0)/Co(Ⅱ)/Co(Ⅲ), pyridinic-N and pyrrolic-N contributed to the generation of hydroxyl and sulfate radicals, while C=O functional group and graphitic-N were catalytic sites for singlet oxygen. Finally, the radical electrophilic attacking sites of AO7 were calculated by the density functional theory (DFT), and the degradation routes of AO7 were speculated by GC–MS. The toxicity test illustrated that the Co-HPNC/PMS system was an environmental-friendly technology for AO7 degradation. The prepared Co-HPNC with a unique honeycomb porous structure presents a novel synthesis route for MOF-derived catalyst applied in the PMS activation system for wastewater treatment.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
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IF 9.136
Jun Li,Qi Liu,Ge Gou,Shurui Kang,Xiao Tan,Bo Tan,Longguo Li,Naiwen Li,Chao Liu,Bo Lai
Sulfamethoxazole (SMX) degradation was investigated through peroxymonosulfate (PMS) activation by the synthesized flower-like Fe 3 S 4 , which showed the best performance with the highest reaction stoichiometric efficiency (7.9%). 99% of SMX (2 mg/L) was eliminated from reaction solution during 30 min with 20 mg/L Fe 3 S 4 and 0.1 mM PMS. The main reactive oxygen species (ROS) involved in the contaminant decomposition were investigated through quenching experiments, electron paramagnetic resonance, and X-ray photoelectron spectroscopy characterization. In addition to the typical sulfate radical (SO 4 •- ) and hydroxyl radical (HO • ), it should be noted that non-radical singlet oxygen ( 1 O 2 ) was generated and participated in the catalytic oxidation of compounds. The degradation of SMX in the PMS alone system through non-radical pathway and in the Fe 3 S 4 /PMS system by both radical and non-radical pathways were proposed according to the detected intermediates. The ecotoxicity of SMX and its by-products were evaluated through the quantitative structure–activity relationship (QSAR) analysis. The present study provided new insight into the mechanism of organic compound removal by ROS including radical and non-radical in Fe 3 S 4 /PMS system.
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Journal of Environmental Sciences
·
2022
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IF 6.796
Qingqing Su,Peiyue Gao,Ning Li,Feifei Wang,Xin Huang
Recently, layered double hydroxide-peroxodisulfate (LDH-PDS) as an advanced oxidation system can effectively remove organics by the pathway of free radical. However, little has been known if there is a potential risk regarding the formation of high toxic iodine byproducts through another pathway when LDH-PDS is used in high iodide waters at coastal areas. Therefore, this study investigated phenol degradation pathways and transformation products to evaluate both removal mechanism and potential risk by LDH-PDS in high iodide waters. The results showed that in LDH-PDS system, with the degradation of PDS, phenol degraded till below detection limit in 1 hr in the presence of iodide, while PDS and phenol were hardly degraded in the absence of iodide, indicating iodide accelerated the transformation of PDS and the degradation of phenol. What is more, it reached the highest phenol removal efficiency under the condition of 100 mg/L LDH, 0.1 mmol/L PDS and 1.0 mmol/L iodide. In LDH-PDS system, iodide was rapidly oxidized by the highly active interlayer PDS, resulting in the formation of reactive iodine including hypoiodic acid, iodine and triiodide instead of free radicals, which contributed rapid degradation of phenol. However, unfortunately toxic iodophenols were detected. Specifically, 2-iodophenol and 4-iodophenol were formed firstly, afterwards 2,4-diiodophenol and 2,6-diiodophenol were produced, and finally iodophenols and diiodophenols gradually decreased and 2,4,6-Triiodophenol were produced. These results indicated that LDH-PDS should avoid to use in high iodide waters to prevent toxic iodine byproduct formation although iodide can accelerate phenol degradation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Fangshu Xing,Renyou Zeng,Chuchu Cheng,Qiuwen Liu,Caijin Huang
Efficient aromatic alcohol oxidation with simultaneous H 2 evolution under aqueous conditions is achieved in a polyoxometalate (POM)-incorporated ZnIn 2 S 4 dual-functional photocatalytic system. The synergy between HPM and ZIS contributes to the formation of a Z-type heterojunction structure and thus enhances redox capacity. Moreover, the sub-nanometer size of POM clusters endows molecular-level interfacial contact, which acts as an "electron bridge" ensuring faster interfacial charge transfer kinetics. Therefore, an impressive nearly 100% yield of benzaldehyde and 10.6 mmol·g −1 ·h −1 H 2 -evolution rate are observed for POM/ZIS nanocomposites even under an anaerobic atmosphere with water as the solvent. This is the first application of POM-based materials in the anaerobic oxidation of benzyl alcohol with concomitant H 2 production. This study expands the possibilities for designing multifunctional POM-based photocatalysts for economic and ecological photoredox applications.
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Journal of Materials Chemistry B
·
2022
·Vol. 10
·期 5
·748-756
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IF 7.571
Shuangling Wang,Jie Lv,Yu Pang,Shuyang Hu,Yulong Lin,Meng Li
Despite significant achievement in chemotherapy, the off-target actions and low pharmaceutical selectivity of the therapeutic agents still limit their clinical efficacy. Herein, a multifunctional nanoplatform which integrates chemotherapy, chemodynamic therapy (CDT) and photoactivation of TRPV1 channels has been successfully established for specific cancer therapy. Polydopamine (PDA) coated hollow prussian blue nanocages (hPBNCs) are used as the photothermal switches and drug carriers for loading chemotherapeutic drug, doxorubicin (Dox). Conjugating with the TRPV1 antibodies enables the nanoplatform to bind specifically to TRPV1 channels on the plasma membrane of the TRPV1-positive cancer cells and then activate them by local heating upon NIR irradiation, leading to the over-influx of Ca2+. Critically, the laser irradiation can be carefully controlled to not only open the TRPV1 channels but also avoid burning of tumors by hyperthermia. Moreover, the exposed hPBNCs in the acidic tumor cells can decompose endogenous H2O2 into ˙OH by Fenton reaction to realize CDT, which further aggravates cancer cell apoptosis. Together with the chemotherapy caused by Dox, our nanoplatform displays an enhanced anticancer effect both in vitro and in vivo. Our work provides a powerful means for site-specific cancer synergetic therapy with high spatial and temporal resolution.
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CHEMICAL ENGINEERING JOURNAL
·
2022
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IF 16.744
Dan Xu,Jianfeng Li,Boyang Li,Huacheng Zhao,Hanghang Zhu,Jinfang Kou,Fengwei Zhang,Zhengping Dong,Jiantai Ma
The sustainable catalytic transformation of alcohols to high value-added fine chemicals is a significant and challenging research topic. Herein, a set of nitrogen-doped carbon encapsulated Co-based catalysts (Co-Co 3 O 4 @NC-T) were prepared by using low-cost dicyandiamide, glyoxal and cobalt nitrate as precursors. The obtained catalysts were utilized for the selective oxidation of alcohols to high value-added esters and carboxylic acids with air as the oxygen source and displayed wide applicability for the oxidation of both aromatic and aliphatic alcohols. Based on the controlled experiments, the protective effect of N-doped carbon structure and the synergistic effect between Co core and Co 3 O 4 species guaranteed the high reaction conversion and selectivity. Benefitting from heterogeneity and magnetism of the catalyst, it can be easily recycled and reused for long-term stability. Reasonable mechanisms of selective oxidation reaction were proposed through EPR analysis and controlled experiments. The present work provides a facile strategy for potential large-scale preparation of heterogeneous catalyst for sustainable and green catalytic transformations.
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FUEL
·
2022
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IF 8.035
Xing Gao,Yingying Ding,Lilin Peng,Dan Yang,Xiaoyue Wan,Chunmei Zhou,Wen Liu,Yihu Dai,Yanhui Yang
Aqueous phase hydrogenative rearrangement of furfural (FAL) to cyclopentanone (CPO) via furfuryl alcohol (FOL) has been studied over Pd catalysts supported on H–ZSM–5 zeolites. Pd states, zeolite properties and reaction condition parameters were optimized, affording 98% selectivity and 120 h −1 specific reaction rate over 2% Pd/H–ZSM–5(25) catalyst at 160 °C and 3 MPa H 2 . For hydrogenation of FAL–to–FOL, the activity was related to the Si/Al ratio and acid property of zeolite supports. For hydrogenative rearrangement of FOL–to–CPO, pure H–ZSM–5 zeolite could catalyze single–step conversion with relatively low reaction rate, whereas the presence of Pd sites could achieve multi–step transformation with remarkably increased rate, highlighting Pd–zeolite acid sites synergy. Proton and furanylmethoxy–relevant intermediates were captured with spin trapping electron paramagnetic resonance experiments, and 4–hydroxy–2–cyclopentenone and 2–cyclopentenone were also identified as key intermediates in tandem reaction pathway to produce CPO.
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