JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Mengyang Lu,Hanmin Zhang,Yu Tian,Wei Yao,Junsheng Wang,Yuezhu Wang
The integration of catalytic oxidation with forward osmosis (FO) holds promising potential to address two crucial challenges encountered by FO: fouling and unsustainable performance, but suitable approaches are still rare. Herein, we have successfully developed a photocatalysis-assisted forward osmosis (PFO) system. In the PFO, a self-made porous carbon nitride doped functional carbon nanotube photocatalytic hydrogel film (PCN@CNTM) was engaged in the FO process in an inventive way by simply sticking to the commercial FO membrane surface, preventing damage to the membrane from the catalyst's direct insertion and delaying the assault from the oxidation groups. PFO allowed organic pollutants to decompose in the feed solution (90%) and on the membrane surface, regulating the water chemical potential and giving the FO membrane antifouling properties. This resulted in sustainable water flux (11.8 LMH) with no significant membrane fouling in PFO, whereas in FO alone there was a significant fouling and flux drop (from 12.73 to 7.23 LMH in 4 h). Moreover, the expensive FO membrane was protected while the hydrogel film can be replaced on demand. The PFO exemplifies the concept of synergistic technology integration, presenting a new perspective on harnessing the strengths of distinct technologies in a mutually beneficial manner.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jing Wang,Qingfeng Fan,Lidong Kou,Huan Chen,Xing Xing,Wenjie Duan,Kai Jiang
Oxygen vacancies (OVs) and heterostructures of photocatalysts play crucial roles in photocatalysis driven by visible light. In this study, a novel photocatalytic textile was prepared by spraying heterostructures of OVs-rich bismuth oxide (BiO 2-x ) and urea-derived graphitic carbon nitride (UCN) on amine group-modified poly(acrylonitrile) nonwoven textile (APAN), and then studied for sulfamethazine (SMT) removal and bacterial ( S. aureus ) disinfection under irradiation of energy-efficient white light emitting diodes (LEDs). The optimal BiO 2-x , prepared within a much shorter time (i.e. 1 h), was actually a ternary mixture of NaBiO 3 -Bi 2 O 3 -BiO 2-x with rich OVs rather than pure BiO 2-x . Incorporation of UCN could help redistribute electrons and induce formation of more OVs, thereby improve the photocatalytic activity of the BU-0.2 hybrid (i.e. mass ratio of BiO 2-x /UCN = 1:0.2). The BU-0.2 could use full-spectrum white light (i.e. 380–760 nm) to achieve superior SMT removal in a wide pH range (pH 5.0–9.0) and in the co-presence of common water constituents. The enhanced photocatalytic performance of BU-0.2 was attributed to the formation of OVs and heterostructure, which could broaden light absorption, help charges separation, and favor adsorption and activation of molecular O 2 . Detection of reactive species demonstrated that 1 O 2 and holes were the dominant factors responsible for SMT removal. Spraying deposition of BU-0.2 on APAN could endow the resultant textile (i.e. APAN-BU-0.2) with excellent photocatalytic activity for SMT removal and bacterial disinfection under LED white light irradiation. The as-prepared photocatalysts showed promising application prospects in purification of emerging pollutants utilizing LED white light.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Zhongmou Liu,Pan Zhang,Xiangyu Zhao
Reduced graphene oxide supported with ferric ion (Fe(III)-rGO) was successfully prepared, and performed as an excellent catalyst to activate hydrogen peroxide (H 2 O 2 ) and peroxymonosulfate (PMS) for isoprothiolane (IPT) degradation. IPT removal efficiency was proven to be better in the Fe(III)-rGO/H 2 O 2 /PMS system (96.2%) than in the Fenton-like reaction (72.6%) and PMS-AOP (80.0%) individually. X-ray photoelectron spectroscopy showed that Fe(III) was reduced in Fenton-like reaction, and the reduced Fe(II) played a crucial role in the subsequent PMS-AOP. The combination of the Fenton-like reaction and PMS-AOP involved the valence state conversion of Fe, which consequently improved Fe(III)-rGO utilization rate and IPT removal efficiency. Fe(III)-rGO remarkably boosted the Fe(III)/Fe(II) cycle and generated superoxide radical (O 2 − •) and singlet oxygen ( 1 O 2 ) in the Fe(III)-rGO/H 2 O 2 /PMS system. Fe(III)-rGO acts as the electron transfer mediator; thus, promoting electron transfer from IPT to H 2 O 2 and PMS and accelerating the generation of active species. Fe(IV) with high oxidation performance was formed in PMS-AOP and efficiently removed some of the IPT. IPT removal efficiency was more than 90% at a pH range of 3–11; this efficiency could be maintained above 50% even after five consecutive degradation experiments, exhibiting excellent stability and reusability of Fe(III)-rGO. Additionally, iron sludge formation was greatly reduced because of the stable chemical bonding of iron ions to the rGO surface. Therefore, this study provides a new multisystem and synergistic approach for the efficient removal of organic micro-pollutants from water.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xiaohui Fan,Jinjin Zhao,Cheng Cheng,Yin Xu,Hui Zhang
Efficient and low-cost catalysts are important for contaminant remediation in peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs). In this study, a solid waste, generated by the polyferric chloride coagulation of the phenol-saturated powder activated carbon from an industrial wastewater treatment plant, was used to prepare metal/carbon composites under different pyrolysis temperatures (650–950 °C). The catalyst pyrolyzed at 950 °C (FeAC-950) exhibited the highest reactive activity for PMS activation as demonstrated by a series of electrochemical techniques. Nearly complete BPA elimination can be achieved within 60 min by 0.1 g L –1 FeAC-950 and 0.5 mM PMS. The results of electron paramagnetic resonance (EPR), chemical quenching and open circuit potential (OCPT) experiments demonstrate a combined radical and non-radical oxidation mechanism in the FeAC-950/PMS process and BPA was removed dominantly through radical pathway. Various persistent organic pollutants can be efficiently eliminated in the FeAC-950/PMS system. In addition, the present system showed good tolerance to natural organic matter as well as some common anions such as chloride and nitrate. This study dedicated a simple method to prepare an efficient solid waste-based catalyst in environmental catalysis. The outcomes will not only provide a value-added reuse approach for waste management but also facilitate the FeAC-950 applications in wastewater remediation technologies.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Xiaoyue Wang,Jin Wang,Shanjun Liu,Mengmeng Dou,Boru Gao
The sterilization effect of photocatalysis and biotoxicity of nanomaterial catalysts have attracted high attention. In this study, the novel visible-driven defective carbon nitride (VL/DCN) system exhibits non-photoreactivation, non-toxic superior performance compared with traditional ultraviolet radiation (UV) and UV/titanium dioxide (UV/TiO 2 ). The inactivation of antibiotic-resistant bacteria (ARB) by novel VL/DCN still reached 7 log within 4 h, and the reduction rates of aminoglycoside gene strB and tetracycline gene tetA exceeded 0.8 log and 1.2 log, respectively. Further, the sterilization mechanism and nanotoxicity were contrastively and systematically analyzed among above three systems as following. Firstly, in the VL/DCN system, reactive oxygen species (ROSs) generated from photocatalytic process leads to the destruction of cell membranes, resulting in dissolving out of potassium ion (K + ), protein and cell membrane ATP content. Thus, resistant bacteria were completely inactivated and photoreactivation disappears. In contrast, the UV only acted on bacterial DNA and existed the light resurrection. The UV/TiO 2 strictly dependent on ultraviolet light and can be used in limited scenarios. Secondly, in cell viability analysis by human lung cell line BEAS-2B experiments, the 10% inhibition of cell growth when DCN was 600 mg/L much lower than 28% inhibition of cell growth when TiO 2 was only 200 mg/L. The expression of pro-inflammatory cytokines (( Interleukin, IL) -6), IL-8, IL-1β ) under the effect of DCN was 1.5-fold, 5.7-fold and 3.7-fold lower than TiO 2 , respectively. Meanwhile, DCN induced cells to produce less ROSs, malondialdehyde (MDA), and more superoxide dismutase (SOD). Above results demonstrated that DCN has far lower cytotoxicity than TiO 2 . This study provides theoretical support for the application of photocatalytic sterilization technology and the exploration of the toxicity of nanomaterials. Environmental Implication In this study, the novel visible-driven defective carbon nitride (VL/DCN) system exhibits non-photoreactivation, non-toxic superior performance compared with traditional ultraviolet radiation (UV) and UV/titanium dioxide (UV/TiO 2 ). The VL/DCN exhibited excellent sterilization efficiency and a high rate of reduction of the E. coli resistance gene strB. The inactivation of ARB reached 7 log within 4 h without the occurrence of photoreactivation. The reduction rates of the aminoglycoside gene strB and tetracycline gene tetA exceeded 0.8 log and 1.2 log, respectively. This study provides a valuable theoretical basis for the development of a new sustainable and environmentally friendly visible light catalytic sterilization technologies.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
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IF 8.2
Mengmeng Li,Xilan Li,Yujie Gao,Yang Yang,Chenggang Yi,Wei Huang,Bingbing Shen,Dongming Qi,Zhengwei Mao,Jindan Wu
Diabetic ulcer is a severe complication of diabetes that can lead to amputation due to the overproduction of pro-inflammatory factors and reactive oxygen species (ROS). In this study, a composite nanofibrous dressing was developed by combining Prussian blue nanocrystals (PBNCs) and heparin sodium (Hep) through electrospinning, electrospraying, and chemical deposition. The nanofibrous dressing (PPBDH) was designed to take advantage of the excellent pro-inflammatory factor-adsorbing capability of Hep and the ROS-scavenging capabilities of PBNCs, resulting in synergistic treatment. It is worth noting that the nanozymes were firmly anchored to the fiber surfaces through slight polymer swelling caused by the solvent during electrospinning, thereby guaranteeing the preservation of the enzyme-like activity levels of PBNCs. The PPBDH dressing was found to be effective in reducing intracellular ROS levels, protecting cells from ROS-induced apoptosis, and capturing excessive pro-inflammatory factors, including chemoattractant protein-1 (MCP-1) and interleukin-1β (IL-1β). Furthermore, a chronic wound healing evaluation conducted in vivo demonstrated that the PPBDH dressing was able to effectively alleviate the inflammatory response and accelerate wound healing. This research presents an innovative approach to fabricate nanozyme hybrid nanofibrous dressings, which have great potential in accelerating the healing of chronic and refractory wounds with uncontrolled inflammation.
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Fundamental Research
·
2023
·
IF 6.2
Qian Hu,Taoyu Yang,Shanli Wang,Licong Xu,Minghua Wu,Deyou Yu,Kaixing Fu,Jinming Luo
Peracetic acid (PAA) has recently been considered a promising oxidant candidate for heterogeneous Fenton-like reactions; however, the main generation and contribution of organic radicals (R-O•) with unsatisfactory oxidation potential compromises wastewater decontamination efficiency. In this study, we demonstrate the rational design and synthesis of ultrafine FeO x nanocluster-anchored carbonaceous nanosheets (UFe-CN) for altering the PAA activation pathway from R-O• to •OH dominant process via in situ framework collapse carbonization of MIL-53(Fe). The constructed UFe-CN/PAA system effectively accelerated refractory micropollutant ( e.g. , p-nitrophenol (4-NP)) decomposition by the enhanced •OH formation (up to 65.24 μmol L − 1 ) under a wide pH range (3.0–9.0), outperforming the benchmark iron-based catalyst counterparts by 4.2–10.8 times. This outstanding Fenton-like catalytic activity of UFe-CN is primarily attributed to the significant improvement in electron mitigation, ca. 49 times higher than that of its MIL-53(Fe) counterpart, for interface catalysis reactions triggered by iron species cycling. Furthermore, to facilitate adaptive engineering, the organic pollutant removal efficiency could be easily tuned by varying several key treatment factors, including the initial pH, PAA concentration, and UFe-CN dosage. More importantly, the excellent practicality of UFe-CN/PAA was demonstrated by systematically evaluating the impact of the water matrix, catalyst regeneration capability, and wastewater treatment efficiency. Overall, this study provides a significant understanding of •OH-dominated PAA activation and an effective catalyst development paradigm to facilitate the practical application of PAA-based Fenton-like oxidation.
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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.
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CHEMOSPHERE
·
2023
·
IF 8.8
Weiming Xiang,Fahao Xu,Dong Wan,Xing Wang,Fan Luo,Yong Chen
Chloroquine phosphate (CQ) is an antiviral drug for Coronavirus Disease 2019 and an old drug for treatment of malaria, which has been detected in natural waters. Despite its prevalence, the environmental fate of CQ remains unclear. In this study, the direct photodegradation of CQ under simulated sunlight was investigated. The effect of various parameters such as pH, initial concentration and environmental matrix were examined. The photodegradation quantum yield of CQ (4.5 × 10 −5 −0.025) increased with the increasing pH value in the range of 6.0–10.0. The electron spin resonance (ESR) spectrometry and quenching experiments verified that the direct photodegradation of CQ was primarily associated with excited triplet states of CQ ( 3 CQ*). The common ions had negligible effect and humic substances exhibited a negative effect on CQ photodegradation. The photoproducts were identified using high-resolution mass spectrometry and the photodegradation pathway of CQ was proposed. The direct photodegradation of CQ involved the cleavage of the C–Cl bond and substitution of the hydroxyl group, followed by further oxidation to yield carboxylic products. The photodegradation processes were further confirmed by the density functional theory (DFT) computation for the energy barrier of CQ dichlorination. The findings contribute to the assessment of the ecological risk associated with the overuse of Coronavirus drugs during global public health emergencies.
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CHEMOSPHERE
·
2023
·
IF 8.8
Wei Zhang,Wenjie Wu,Jianfei Wu,Xiaobin Liu,Jian Tian,Heng Li,Qingbiao Li,Yanmei Zheng
Although advanced oxidation processes (AOPs) based on persulfate (PS) is an attractive approach for repairing polycyclic aromatic hydrocarbons (PAHs) contaminated soils, limited oxidizability of PAHs and efficient in-situ activation of PS hinder its practical applications. In this study, we comprehensively examined the contributions of five representative surfactants on the oxidative remediation of PAHs-contaminated soil in terms of degradation kinetics of the pollutants, and further proposed an innovative coupling strategy of surfactant-enhanced thermally activated PS remediating PAHs-contaminated soil. The results showed that the degradation process of PAHs in soil was significantly facilitated only via adding sodium dodecyl benzenesulfonate (SDBS) and fitted the pseudo-first-order kinetic pattern. The removal of phenanthrene (PHE) reached 98.56% at 50 mM PS, 50 °C, 5 g L −1 SDBS and 48 h reaction time, accompanying an increase of 25% in reaction rate constant from 0.0572 h −1 (without SDBS) to 0.0715 h −1 . More importantly, SDBS-enhanced thermally activated PS degrading PAHs with higher benzene rings were more effective as the reaction rate constants of pyrene (PYR) and benzo(a)anthracene (BaA) were significantly increased by 49.40% and 56.86%. Additionally, only appropriate dosages (5–10 g L −1 ) of SDBS facilitated the oxidative degradation of PHE, as well as the aging time of contaminant-soil contact slowed down the enhancement of oxidative degradation of PHE by SDBS. Scavenger experiments demonstrated that SO 4 ·- and 1 O 2 were the dominant reactive oxygen species . Finally, a possible oxidative degradation pathway of PHE was proposed, and the toxicity of derived intermediates got alleviation by the assessment using the Toxicity Estimation Software Tool . This investigation was promising for in situ scale-up remediation of PAHs-contaminated soil.
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Environmental Science-Nano
·
2023
·Vol. 10
·期 7
·1897-1906
·
IF 7.3
Yang Yang,Junmin Peng,Huilin Tao,Zhou Yang,Yidong Hou,Wei Lin,Jinshui Zhang
The development of efficient catalysts is of great significance in the photocatalytic ozonation process for organic wastewater treatment. However, the effect of exposed facets and surface defects of the catalyst on the photocatalytic ozonation performance is less covered. Herein, ZnO nanocomposites with different preferentially exposed crystal facets (ZnO-rod and ZnO-disk) were synthesized and used for photocatalytic ozonation of phenol. The characterization and density functional theory calculation results demonstrated that the exposed {0001} facets and oxygen vacancies promoted the separation and transfer of photogenerated charges as well as improved the adsorption and activation of ozone molecules on the catalyst surface. Consequently, the TOC removal rate in the UV-O3/ZnO-disk process (62.4%) was much higher than those in the UV-O3/ZnO-rod process (41.3%) and the UV-O3 process (15%). Moreover, the experimental results of the identification and quenching of active species illustrated that ˙OH was more likely to be produced in the UV-O3/ZnO-disk process, while 1O2 was more likely to be formed over ZnO-rod. A large amount of ˙OH with a stronger oxidation capability than 1O2 contributed to the superiority of ZnO-disk over ZnO-rod in organic pollutant removal. This work demonstrates that the engineering of crystal facets and surface defects provides an effective strategy for constructing efficient catalysts for the photocatalytic ozonation process.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2023
·
IF 7.8
Wei Zhang,Heng Li,Siqiang Xiao,Jianfei Wu,Chuanhu Wang,Xiaobin Liu,Qingbiao Li,Yanmei Zheng
Controllable delivery of persulfate (PS) and the enhancement of oxidative availability of pollutants in in-situ oxidative remediation of low-permeability polycyclic aromatic hydrocarbons (PAHs) contaminated soil are crucial. To tackle the above challenges, the coupling of Tween 80 solubilization enhanced oxidation of phenanthrene (PHE) in low-permeability soil under electrokinetic remediation (EKR) was proposed. Firstly, batch degradation experiments showed that the addition of Tween 80 significantly inhibited the degradation of PHE in soil under thermally activated PS, as the dosage of Tween 80 increased from 0 % to 1 % with the corresponding removal rate declining from 99.19 % to 40.90 %. Accordingly, in-situ electrokinetic delivery of Tween 80 and PS was regulated in further EKR, intending to reduce unproductive consumption. PS was more uniformly delivered to the whole remediation regions from the cathode chamber by electromigration , while Tween 80 was transported into the soil from the anode chamber by electroosmosis , which made Tween 80 solubilization and PS oxidation achieve synergistic effect . And the total removal rate of PHE reached 64.90 % under this strategy, which had increased by 415.90 % and 8.76 %− 130.14 % compared with only EKR or EKR coupling single enhanced technology , respectively. After further thermal activation of transported PS at 50 ℃ by electrical resistance heating, the total removal rate of PHE increased to 71.58 %. EPR spectrum indicated that SO 4 . - and OH . were responsible for the degradation of PHE.
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