SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Chuanyu Chen,Simeng Xia,Fan Chen,Ting Peng,Lin Deng,Huiying Wu,Zhou Shi
The Fe(II)/peracetic acid (PAA) process shows significant potential for the removal of organic pollutants due to the rapid reaction between Fe(II) and PAA. However, the slow reduction from Fe(III) to Fe(II) leads to the continuous or excess dosing of Fe(II) during practical application. In this study, epigallocatechin gallate (EGCG), a typical reagent extracted from green tea, was used to enhance the degradation of coumarin (COU) by Fe(II)/PAA for the first time. A complete elimination of COU (25 μM) was achieved in the presence of 50 μM Fe(II), 300 μM PAA, and 25 μM EGCG, exhibiting a k obs value of 0.108 min −1 , which was 27 times higher than that observed with Fe(II)/PAA (0.004 min −1 ). Further, Fe(II)/EGCG/PAA demonstrated remarkable pH tolerance, with a COU removal efficiency exceeding 80 % across a pH range of 3–9. Mechanisms investigations revealed that •OH played a dominant role in COU degradation by Fe(II)/EGCG/PAA (accounting for 98.2 %). The increase in EGCG concentration from 10 to 100 μM resulted in a decreased formation of •OH yield and an enhanced generation of RO•. These findings highlight the capability of EGCG to improve the oxidation capacity of Fe(II)/PAA and modulate reactive species formation. The outstanding oxidation capacity and environmental friendliness of Fe(II)/EGCG/PAA process render it a potential strategy to eliminate organic pollutants in actual water treatment.
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高影响因子
Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Yuanlu Xu,Qi Peng,Yueling Yu,Zhifei Li,Yanming Liu,Zijian Qin,Xinfei Fan
Heterogeneous electro-Fenton (EF) technology relies on the generation of hydroxyl radicals (•OH) with superior oxidation property that can efficiently remove organic contaminants present in water. Nevertheless, the time-consuming and complex preparation process of heterogeneous EF catalysts is a major obstacle to the broader application. Given this, in the work, a composite cathodic catalyst (Fe/OCNT@CC) was prepared by loading Fe and oxidized carbon nanotubes (OCNTs) onto carbon cloth (CC) via a one-step electrophoretic deposition (EPD) method with the superiorities of easy-operation, rapid synthesis and large-scale application, which successfully reduced the time cost of conventional heterogeneous EF catalyst preparation. Notably, Fe/OCNT@CC exhibited outstanding EF degradation performance, almost 100 % phenol degradation efficiency within 30 min at pH 6.5. Meanwhile, following 5 consecutive runs, the removal rate of phenol could still reach 90.4 %, indicating the excellent stability of Fe/OCNT@CC. Furthermore, the Fe/OCNT@CC catalyst possessed remarkable removal capability for diverse organic pollutants with elimination rates of Rhodamine B, 2,4-DCP and SMX reaching nearly 100 % within 60 min. Therefore, the study offers a novel perspective on how to enhance the preparation efficiency and simplify the synthetic process of heterogeneous EF composite catalysts for efficient organic wastewater treatment.
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高影响因子
FUEL
·
2024
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IF 6.7
Jialong Wu,Xiaoning Zhang,Fucheng Ju,Can Huang,Carrie Donley,Peng Xiao,Lan Xu,Hongju Zhang
The broad use of the electrocatalytic hydrogen evolution reaction (HER) is impeded by challenges associated with the availability and high cost of precious metal-based catalysts. Carbon materials co-doped with transition metals and nitrogen have emerged as highly promising alternatives among non-precious metal-based electrocatalysts due to their advantageous features, such as cost-effectiveness, high activity, and excellent stability. This study focuses on incorporating low-cost sodium molybdate onto silk fabric, which serves as a sustainable precursor for the preparation of nitrogen-doped carbon material. This silk fabric is then carbonized to create a flexible electrode for electrocatalytic hydrogen evolution. The resulting electrode exhibits the in situ growth of Mo 2 C and MoO 3 , and this mechanism facilitates a smoother conduction path for electrons. The resulting electrode not only possesses flexible characteristics but also exhibits a large specific surface area. Transmission electron microscopy analysis reveals the presence of carbon quantum dots, which actively contribute to the heightened catalytic hydrogen evolution activity of the prepared electrode. Experimental findings unequivocally showcase the outstanding electrocatalytic hydrogen evolution capability and operational stability of the fabricated flexible electrode in acidic and alkaline environments. This work substantiates the efficacy of using low-cost sodium molybdate-loaded silk fabric as a catalyst precursor, thereby providing robust support for the design and implementation of non-precious metal-based electrocatalysts for the HER. This approach advances the development and broader application of carbon-free fuels.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2024
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IF 8.2
Yu Hou,Qi Fu,Huajie Zhong,Jiaxing Yu,Yuan Tao,Zeyu Gong,Jianqiang Li,Songbo Wei,Junlang Qiu,Junhui Wang,Fang Zhu,Gangfeng Ouyang
The preparation of waste plastics-derived catalysts is an effective strategy for the waste reclamation . However, plastic-derived material is unsuitable for wastewater purification due to its small specific surface area (SSA) and inadequate active sites (such as N/O sites). Herein, we synthesized graphene-like nanosheets using g-C 3 N 4 as the self-sacrificing soft template and plastic as the carbon precursor. Consequently, this strategy greatly promoted the efficiencies of the emerging organic pollutants degradation with the SSA and N content of the plastic-derived biochar increasing up to 1043.4 m 2 /g and 17.53 at.%, respectively. In detail, 100 % sulfadiazine (SD) removal could be achieved in 180 s via the activation of peroxymonosulfate (PMS) and the catalytic activity is far higher than previous research. Mechanism experiments corroborated that such a striking performance was attributed to the generation of SO 4 •− , O 2 •− and 1 O 2 . Meanwhile, kinds of plastic precursors, even medical waste (i.e., masks, gauze, operating caps and degreasing cotton) were also applicable. And the practical application of the plastic-derived catalyst was further demonstrated by treating pollutants in a continuous flow mode with in situ fabricated membrane. This work provides valuable insights into waste plastics processing and water pollutants removal.
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PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Yuxuan Zhu,Hong Wang,Qinliang Jiang,Alex T. Kuvarega,Jianxin Li
An activated carbon membrane (ACM) doped with hexagonal boron nitride ( h -BN) was fabricated by using activated carbon as the raw material and phenolic resin as the binder. The preparation process involves blending raw materials, ball milling , membrane pressing, and high-temperature carbonization . The conductive ACM was employed as an anode to constitute an electrochemical membrane reactor (EMR) for phenol removal. The effect of h -BN doping rate (0–5 wt%) on the properties of ACM was explored. Results showed that ACM1 (1 wt% h -BN) displayed a small pore size (20 nm), high porosity (41.6 %), large specific surface area (446.8 m 2 /g), and strong mechanical strength (15.4 MPa) compared to the pristine ACM0. The oxygen precipitation potential of ACM1 (2.11 V) was much higher than that of ACM0 (1.53 V), thus reducing oxygen generation at the anode in EMR for phenol degradation. The phenol removal rate of phenol obtained from EMR with ACM1 as the anode at 1.5 V was up to 95.6 %, which was much higher than that for ACM0 (39.3 %). Density functional theory (DFT) calculations and experimental results confirmed that h -BN-doping enhanced the adsorption active sites, and adsorption energy , leading to the high performance of EMR for phenol removal. In addition, the equilibrium adsorption capacity of ACM1 (10.2 mg/g) was much higher than that of ACM0 (3.7 mg/g). The C atoms adjacent to pyridine N in ACM1 were identified as the adsorption and active catalytic sites by X-ray photoelectron spectroscopy (XPS) and DFT calculations. Therefore, this study sheds light on the design and fabrication of conductive carbon membranes for enhanced performance in industrial wastewater treatment .
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Kang Li,Jiaoqun Zhu,Weibing Zhou,Lilong Sun,Shouqin Tian
To improve the photocatalytic performance of single-phase Bi 2 WO 6 , the heterojunction construction is usually employed to effectively separate and transport photo-induced carriers. Herein, MXene/Bi 2 WO 6 heterojunction (NB2 and VB2) with face-to-face contact and hierarchical structure was constructed by growing ultrafine Bi 2 WO 6 nanosheets on the surface of two-dimensional MXene (Nb 2 C and V 2 C) materials. Compared with the original Bi 2 WO 6 , the hybrids exhibited a larger specific surface area (42.17 m 2 ∙g −1 for NB2, 50.15 m 2 ∙g −1 for VB2), and displayed significant enhancements in the photodegradation of anionic MO (13.8-fold, 6.5-fold), cationic RhB (9.1-fold, 4.5-fold), and neutral phenol (8.5-fold, 6.1-fold), respectively. This is mainly attributed to the heterostructures via face-to-face coupling which can facilitate the tuning of the photoresponsive properties and internal energy level structure, as well as the generation of free radicals ( • O 2 - , • OH, and h + ) for the stepwise redox process in photodegradation. Therefore, this work is expected to expand the diverse use of Non-Ti 3 C 2 MXene in photocatalysis, meanwhile provide important guidance for the harmless treatment of organic pollutants.
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高影响因子
ACS Applied Polymer Materials
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2024
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IF 4.4
Qi Jiang,Han Hu,Qingyang Luan,Hanxu Zhu,Jinggang Wang,Jin Zhu
Poly(ethylene 2,5-furandicarboxylate) (PEF) is a type of biobased polyester with a high gas barrier, which has the potential to replace polyethylene terephthalate (PET). In view of the poor toughness of PEF, an innovative attempt was made to install a small amount of 2,5-thiophenedicarboxylic acid (TDCA) into the PEF backbone and synthesize the poly(ethylene furandicarboxylate-co-thiophenedicarboxylate) (PEFS-n) copolyester. The obtained PEFS-n demonstrates thermal stability and glass transition temperature (Tg) comparable to that of PEF. Additionally, the tensile properties of PEFS-n exhibit appreciable enhancements. The impact strength of PEFS-n exhibited a markedly higher value than that of PEF, particularly in the case of PEFS-5, which displays a 138% increase in impact strength. Concurrently, PEFS-n exhibits enhanced barrier characteristics (oxygen, carbon dioxide, and water) than PET, in addition to outstanding solvent resistance and transparency. After 4 h of hydrolysis in alkaline solutions at 80 °C, subsequently simply washing and filtering, more than 90% of FDCA monomer could be recovered. This work provides a direction for high impact and heat-resistant green packaging, as sustainable alternatives to PET.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Meiling Liu,Liping Wang,Qilong Fan,Ningning Xiao,Zhiwen Chen,Yingying Dong,Chuanliang Zhao,Yongxia Sun,Xing Xu,Wendong Wang
Nitrogen (N)-doping has been reported effective to reinforce catalysis in advanced oxidation processes (AOPs) due to the formation of N-related active sites. Although several documents have reported that transition metal-nitrogen (metal-N x ) sites could work as reactive centers, the catalytic mechanism was hardly elucidated. In this study, N-doped cobalt oxide (N-CoO x ) was initiatively prepared via calcination in ammonia atmosphere to construct cobalt-nitrogen (Co-N x ) sites. The emergence of Co-N x sites effectively improved peroxymonosulfate (PMS) activation efficiency (above 5.8 times), leading to higher pollutant decomposition rate (95.8 % at 30 min) and kinetics constant (above 4.1 times). N introduction changed main facets of material and elevated adsorption energy (E ads ) (from −1.81 eV to −3.71 eV) between catalyst and PMS. Co atoms at Co-N x sites could donate larger quantity of electrons (from 1.088 e to 1.583 e) to PMS, therefore, contributed to stretching and breaking O–O bonds of PMS molecules to form reactive species. As a result, both radical and electron transfer pathway (ETP) were enhanced in the oxidation processes. Ultimately, the catalytic membrane coated with N-CoO x maintained 100 % treatment towards continuous antibiotic wastewater at environmentally relevant concentration (μg/L), realizing purification as well as separation of catalyst. This work systematically elaborates the superiority of Co-N x sites and unravels the underlying mechanism to inspire further study to metal-N x tailored catalysis.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Yadong Yang,Yangyang Jian,Lingzhi He
Herein, a highly efficient and recyclable biocatalyst was developed using stabilized enzyme aggregates on amino-functionalized magnetic biochar for removing persistent organic pollutants from water. The biochar derived from biomass featured abundant hydroxyl functional groups, after functionalization with amino functional groups and magnetic nanoparticles, it was employed for laccase immobilization via enzyme electrostatic adsorption, precipitation and cross-linking in a favorable orientation. This immobilized enzyme aggregates exhibited enhanced pH tolerance, thermal and storage stability than free enzyme. Complete removal of 20 mg/L bisphenol A was achieved within 60 min via C-C bond cleavage and hydroxylation. Notably, the removal efficiency remained at approximately 90 % even after six cycles. Furthermore, this biocatalyst was also successfully applied to efficiently remove other various persistent organic pollutants and demonstrated applicability in real environmental water samples. This study highlights the substantial potential of enzyme-based biocatalysts, presenting a sustainable and efficient approach for water purification and biomass resource recovery.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Zhao Song,Yu Zhang,Peiru He,Xuesong Liu,Nanqi Ren,Yidi Chen
Phenolic pollutants are highly toxic and can affect the growth and reproduction of aquatic organisms, as well as contaminate drinking water resources, posing a significant threat to both ecological and human health. However, conventional biological treatment processes are constrained in treating high salinity organic wastewaters due to the potentially lethal effects of high concentrations of dissolved salts on microorganisms. While advanced oxidation processes have shown promise in removing phenolic contaminants from high-saline wastewater, their widespread application is always limited by the high costs associated with energy and chemical usage. In this study, we explored the potential application of directly introducing peroxymonosulfate (PMS) and peracetic acid (PAA) to high-salinity water for the removal of nine phenolic contaminants. By establishing a correlation between the degradation rate constants in the PMS/Cl – ( k PMS ) and PAA/Cl – ( k PAA ) systems and various molecule descriptors, two multiple linear regression models were developed to predict the degradation rate constants under investigation. Additionally, we selected bisphenol A (BPA) as the target contaminant and investigated the impact of common ions found in natural water, such as HCO 3 – , NO 3 – , and humic acid, on the removal of BPA using two systems. Finally, we conducted experiments using tap water and sewage water to demonstrate the practical application and performance of the two systems. These experiments aimed to provide valuable insights into the influence of background chloride on PMS and PAA activation, as well as the potential of direct PMS/PAA introduction for eliminating phenolic micropollutants from high-saline wastewaters.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2024
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IF 5.9
Cheng Yang,Yanmei Shi,Lixin Li,Zhihong Chen,Di Zhao,Weixia Zhu,Kai Hu
Bisphenol A (BPA) is widespread in the environment and has a serious impact on human body. In this study, a novel magnetic metal-organic frameworks@Ti 3 C 2 T x composite, noted as Fe 3 O 4 @Ti 3 C 2 T x /MOF, was prepared and used as adsorbent for the removal of BPA from environmental water. The adsorption parameters that affecting the removal efficiency of BPA, such as solution pH, contact time, adsorbent dosage, co-existing inorganic ions, ionic strength, and humic acid were investigated in detail. Accordingly, the removal efficiency of BPA by Fe 3 O 4 @Ti 3 C 2 T x /MOF was as much as 95 %. Adsorption studies showed that the proposed composite can provide a maximum adsorption capacity of 547.43 mg g −1 for BPA within 5 min, which was superior to most of the reported adsorbents. The adsorption process was consistent with the pseudo-second-order kinetics (K 2 , 1.1063 μg mg −1 min −1 ) and Freundlich isotherm model, indicating that the adsorption was depended by chemisorption and the heterogeneous surface. Furthermore, the thermodynamic results demonstrated the exothermic nature of the adsorption process (ΔH θ = −34.84 kJ mol −1 ). Most importantly, the magnetic properties of the Fe 3 O 4 @Ti 3 C 2 T x /MOF make it easy to collect, so it can be regenerated and reused for at least 4 cycles without significant loss of adsorption efficiency. Overall, the proposed composite can be applied to the efficient removal of BPA from water samples and could be potentially applicable for practical wastewater treatment.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yali Song,Ziyan Li,Cairong Yang,Xiaojing Zhang,Qiong Wang,Xiaoyu Wen,Hongzhong Zhang,Long Huang
A simple method for preparing C self-doped g-C 3 N 4 (CCN) was proposed by calcining urea and barbituric acid to effectively degrade sulfamethoxazole (SMX). X-ray photoelectron spectroscopy and element content analysis implied C atom replaced the original position of the bridging N atom to form CCN. Compared to g-C 3 N 4 , the absorption edge of CCN was red-shifted. As a result, the band gap of CCN was reduced, which improved the light absorption capacity of CCN and the separation efficiency of photogenerated electron-hole. Ultimately, the photocatalytic activity of CCN was finally boosted. CCN can effectively degrade SMX under visible light. Among CCN with various C dosage, when 0.05 g of barbituric acid was added in the preparation process, the obtained sample (CCN-0.05) exhibited uppermost degradation efficiency on SMX, which can reach 99.0 % after irradiation for 60 min. Additionally, the first-order kinetic reaction rate constant (0.086 min −1 ) was 8.9 times higher than that of g-C 3 N 4 (0.0097 min −1 ). Electron paramagnetic resonance and trapping experiments showed that the dominant reactive species on SMX degradation were surface ·O 2 − and photogenerated holes by CCN-0.05 under visible light. Moreover, CCN-0.05 can still achieve effective removal of SMX under actual water backgrounds and showed selective degradation on sulfonamides.
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