ACS Applied Materials & Interfaces
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2023
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IF 9.5
Xueyan Xue,Nan Xue,Dandan Ouyang,Liuqian Yang,Yanan Wang,Hui Zhu,Aikelaimu Aihemaiti,Jiao Yin
Iron single-atom catalysts (Fe SACs) hold great promise for peroxymonosulfate (PMS) activation and degradation of organic pollutants in wastewater. However, insights into crucial catalytic sites and activation mechanisms of biochar-based Fe SACs for PMS remain a challenge. Herein, cotton stalk-derived biochar-based Fe SACs (Fe SACs-BC) with an asymmetric Fe-N/O-C configuration were prepared, and their PMS activation and acid orange 7 (AO7) degradation mechanisms were investigated. The results showed that the removal efficiency of the Fe SACs-BC catalyst with Fe-N3O-C configuration for AO7 and other five investigated organic dyes reached 95–99% within 15 min. The EPR spectrums, quenching experiments, electrochemical analysis, masking experiments, XPS, and theoretical calculations indicated that degradations of organic dyes were dominated by singlet oxygen, which was generated by direct PMS conversion at the electron-deficient carbon and iron sites in the Fe-N3O-C configuration. The Fe SACs-BC/PMS exhibited high removal efficiency and strong tolerance in different water matrices with a wide pH range, various coexisting anions and interfering substances, showing great potential and applicability for efficient treatment of actual textile wastewaters.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Xiaowei Liu,Peng Chen,Xiangdong Li,Jiaen Zhong,Kexin Li,Miaomiao Ye,Lili Wang
The widespread implementation of ultrafiltration (UF) technology, which has gained popularity for drinking water treatment, has been impeded by rising operational costs and shortened membrane lifespans resulting from membrane fouling. Here, an integrated pretreatment technique combining oxidation, adsorption, and coagulation was developed using the S(IV)–Fe(II) binary activated permanganate (PM) system, S(IV)–Fe(II)/PM. The efficacy of S(IV)–Fe(II)/PM pretreatment in mitigating UF membrane fouling was investigated for various raw water sources, including lakes, rivers, and seawater. The operational parameters of S(IV)–Fe(II)/PM pretreatment were optimized, and the underlying mechanisms for fouling alleviation were explored. Relative to conventional pretreatment methods, S(IV)–Fe(II)/PM pretreatment reduced reversible fouling-induced resistance by 13%–92% and irreversible fouling-induced resistance by 11%–86%. The S(IV)–Fe(II)/PM system exhibited optimal mitigation of membrane fouling at a PM:S(IV):Fe(II) dosage ratio of 2:3:3, with G rapid × T rapid = 45948, G slow × T slow = 12480, and a settling time of 30 min (where G is the velocity gradient and T is contact time). The effectiveness of S(IV)–Fe(II)/PM pretreatment in controlling UF membrane fouling can be attributed to the following mechanisms: 1) modification of feed water quality in terms of organic compound characteristics and concentration, colloidal particle quantity and size distribution, and microbial activity and quantity; and 2) adjustment of the membrane surface deposition environment, resulting in reduced polysaccharide and protein content, particle size distribution range, and biomass, as well as alterations in physicochemical properties such as hydrophilicity and interfacial free energy. This study highlights the efficacy of S(IV)–Fe(II)/PM pretreatment in ensuring high-quality UF effluent while effectively reducing membrane fouling, especially its potential for alleviating irreversible membrane fouling.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
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IF 16.6
Ma Dingren,Lian Qiyu,Zhang Yexing,Huang Yajing,Guan Xinyi,Liang Qiwen,He Chun,Xia Dehua,Liu Shengwei,Yu Jiaguo
The structure-activity relationship in catalytic ozonation remains unclear, hindering the understanding of activity origins. Here, we report activity trends in catalytic ozonation using a series of single-atom catalysts with well-defined M 1 -N 3 C 1 (M: manganese, ferrum, cobalt, and nickel) active sites. The M 1 -N 3 C 1 units induce locally polarized M − C bonds to capture ozone molecules onto M atoms and serve as electron shuttles for catalytic ozonation, exhibiting excellent catalytic activities (at least 527 times higher than commercial manganese dioxide). The combined in situ characterization and theoretical calculations reveal single metal atom-dependent catalytic activity, with surface atomic oxygen reactivity identified as a descriptor for the structure-activity relationship in catalytic ozonation. Additionally, the dissociation barrier of surface peroxide species is proposed as a descriptor for the structure-activity relationship in ozone decomposition. These findings provide guidelines for designing high-performance catalytic ozonation catalysts and enhance the atomic-level mechanistic understanding of the integral control of ozone and methyl mercaptan.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Hailun Zhao,Zixuan Zheng,Shangkun Zhu,Ruixin Guo,Yanhua Liu,Jianqiu Chen,Qiulian Yang
Antibiotics are emerging contaminants that have become a global concern because of their refractory and toxic characteristics. The treatment of antibiotic contaminants using advanced electrochemical oxidation processes is currently gaining interest. In this study, we constructed a natural iron-mediated electrochemical system for the removal of antibiotics using natural tourmaline (TM) as the heterogeneous iron catalyst, platinum (Pt) as the anode, and nickel foam (NiF) as the cathode. Sulfamethoxazole (SMX) was selected as the target antibiotic. The surface properties and components of TM were characterized using energy-dispersive X-ray spectroscopy, N 2 adsorption–desorption isotherms, X-ray diffraction, and X-ray photoelectron spectroscopy. Compared with the Pt-NiF electrochemical system, the Pt-NiF-TM electrochemical system showed a 23 times enhanced reaction rate constant of SMX degradation under the optimal conditions of current density 4.17 mA/cm 2 , 200–400 mesh, TM dosage 3 g/L, and initial pH 3, in which SMX was almost completely degraded (removal rate = 99.92 %) after 60 min. The ·OH and ·O 2 – radicals generated in the Pt-NiF-TM electrochemical system were the active species for SMX degradation. Thirteen SMX degradation intermediates were identified and possible SMX degradation pathways were proposed. Density functional theory calculations demonstrated that C3 and N11 are the sites with higher electrophilic reactivity in SMX. Furthermore, toxicity calculations and analysis of SMX and its degradation products showed that after treatment with the Pt-NiF-TM electrochemical system, the toxicity of SMX to the microalgae Oocystis was reduced. Overall, this study provides a novel and environmentally friendly electrochemical system mediated by TM for the highly efficient degradation of antibiotic contaminants.
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INDUSTRIAL CROPS AND PRODUCTS
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2023
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IF 5.9
Wenli Yao,Fenghui Qin,Ziwei Zhao,Zhijun Ma,Chunyang Hu,Lei Zhou,Yian Zheng
Perfluorinated compounds have serious impacts on ecosystems and threats to human health, and exploring technologies to remove them is urgently needed. Using Calotropis gigantea fiber (CGF) as the biological template, the precursor of ZIF-67 was firstly in-situ anchored in the inner/outer walls of the fiber and then pyrolyzed to yield the composite catalyst labelled as Co/C@C. In combination with peroxymonosulfate (PMS), the advanced oxidation system, i.e. Co/C@C/PMS, was constructed for the catalytic removal of perfluorooctanoic acid (PFOA) from water. The experimental results showed that under the optimized conditions of PMS dosage of 1.0 g/L, catalyst dosage of 0.5 g/L and pH 3.0, PFOA achieved the degradation efficiency of 72.2% within 4 h at ambient temperature. Combined with free radical quenching, electron paramagnetic resonance, electrochemistry and nitroblue tetrazolium dichloride-based UV-Vis analysis, the reactive oxygen species and diverse pathways were identified, including SO 4 • − , O 2 • − , O 2 1 and electron transfer process in the Co/C@C/PMS system. The coexisting anions ( HCO 3 − , Cl − , H 2 PO 4 − and NO 3 − ) and real wastewaters showed no significant effects on PFOA degradation, demonstrating that the Co/C@C/PMS system has good resistance to external ions and different media. After four cycles, the degradation efficiency of PFOA was still 62.8%, indicating that Co/C@C has high stability and good reusability. The degradation products of PFOA were mainly short-chain perfluorinated carboxylic acids (C4-C7) and hydrogen-substituted perfluorinated compounds. Based on quantitative structure-activity relationship analysis, their ecotoxicity was finally evaluated via ECOSAR method. In short, natural CGF derived Co/C@C has great potential for the reduction of emerging PFOA to achieve a sustainable water environment for humans.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Yong Chen,Yong Liu,Xiaobo Gong,Jianlong Wang
Photocatalytic hydrogen peroxide (H 2 O 2 ) production and its application in advanced oxidation processes (AOPs) are regarded as low-cost and environmentally friendly wastewater treatment processes. Herein, by modifying a small amount of sulphide on the zeolitic imidazolate framework-8 (ZIF-8), a ZnS@ZIF-8 composite and used for photocatalytic H 2 O 2 production to degrade chlorinated organic pollutants under simulated sunlight (SSL). ZnS@ZIF-8 composite could enhance the separation of photo-induced charge carriers, promote electron transfer from zinc sulphide (ZnS) to ZIF-8, which exhibited good selectivity for the two-electron oxygen reduction reaction (2e - -ORR) and two-electron water oxidation (2e - -WOR) pathways. Based on oxygen (O 2 ) activation, the developed ZnS@ZIF-8/O 2 /SSL system could achieve 6.43 mmol/L H 2 O 2 production within 150 min, which was approximately 8.66 and 10.36 times higher than that of the ZnS/O 2 /SSL and ZIF-8/O 2 /SSL systems, respectively. In the ZnS@ZIF-8/O 2 /SSL system, the ORR, WOR and H 2 O 2 photolysis led to the generation of hydroxyl radical (•OH), while the photochemical behavior of ZnS in ZnS@ZIF-8 composite resulted in the generation of active hydrogen (*H). Benefitting from the high concentration of H 2 O 2 and the coexistence of redox species in the ZnS@ZIF-8/O 2 /SSL system, various chlorinated organic pollutants could be dechlorinated and mineralized. In addition, a possible mechanism for photocatalytic H 2 O 2 production was also proposed. Importantly, the proposed process did not involve an additional sacrificial agent or Fenton-like catalysts. This work provides insights into the potential application of ZnS@ZIF-8 composite for H 2 O 2 production and wastewater treatment.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Rui Li,Yingying Cai,Shuoyang Liang,Aikelaimu Aihemaiti,Zuotai Zhang
Constructing heterojunctions in a rational and effective way plays a vital role in enhancing the catalytic performance of piezo-/ferroelectric nanomaterials. In this paper, a new material called Ag 2 O@KNbO 3 was fabricated using solvothermal and alkaline deposition methods. This material was found to be an effective catalyst for breaking down various organic pollutants, for example, Orange Ⅱ, Methyl orange, etc. Under optimal conditions, Ag 2 O@KNbO 3 (1:1) demonstrated superior piezocatalytic activity with a degradation efficiency of 97.8% for Orange II within 120 min and a high TOC removal efficiency of 58.4%. The cycle stability for Orange II removal was also excellent. After 5 cycles, the degradation efficiency of Orange II still surpassed 95%. The related enhancement mechanism of the piezocatalytic activity was elaborated in detail, with Ag 2 O/KNbO 3 heterojunctions promoting directed charge movement, reducing impedance of charge transport, and hindering electron-hole recombination, thereby improving charge transfer efficiency. Additionally, OH was confirmed to be the primary active species by electron spin resonance analysis and free radical capture experiment. Notably, a possible degradation pathway of Orange Ⅱ was inferred according to the LC-MS measurement. Overall, this study provides a promising approach for designing and synthesizing new piezoelectric catalytic materials.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Meiling Chen,Lei Zhou,Xiuqin Xiong,Shijun Zhu,Xinkai Yuan,Boyin Yan,Bingrui Ma,Jiachuang Shao,Liming Yang,Xubiao Luo,Penghui Shao
Conventional advanced oxidation processes were used to treat heavy metal complexes. However, a considerable amount of oxidants was required to enable effective oxidative degradation, which led to a significant increase of the treatment costs and subsequent difficulties in the sludge disposal. Based on the abundance of anions in heavy metal wastewater, the effects of anions on the in-situ degradation of Ni-EDTA in an oxidant-free electrochemical system with boron-doped diamond (BDD) as the anode were investigated. The presence of Cl - was found to exert a significant effect on improving the degradation process. Moreover, pH had little effect on the removal of nickel (Ni) and Ni-EDTA within a specific pH range (1 < pH < 9). The removal efficiencies of Ni and TOC reached 100 % and 77.45 %, respectively, at pH 2.16 with 0.4 M NaCl electrolyte, 2 mM Ni-EDTA concentration, and a current density of 50 mA/cm 2 . •OH and Cl• played crucial roles in the removal of Ni-EDTA by disrupting the chelation sites of Ni and EDTA molecules. The released Ni 2+ ions could active the H 2 O 2 in-situ generated at the cathode to produce •OH. The formation of the precipitation products such as NiOOH, Ni(OH) 2 , and NiCO 3 in the Cl - /BDD system were conform based on the XRD and XPS analyses, which suggested the possible pathways for the removal of Ni 2+ and Ni 3+ . Finally, the possible degradation pathways of Ni-EDTA were proposed based on the identification of intermediate products using UPLC-MS.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2023
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IF 8.7
Jiaqiao Yuan,Zhan Ding,Jie Li,Anmei Yu,Shuming Wen,Shaojun Bai
This study objective is to degrade xanthate from flotation tailings wastewater by using a coagulation-flocculation co-Fenton oxidation process in an acid mine drainage (AMD)-H 2 O 2 system. More than 98% sodium butyl xanthate (SBX) removal rate was achieved by the method under optimal conditions. The acids and Fe 2+ in AMD were sufficient to initiate a Fenton reaction at the aid of H 2 O 2 . Furthermore, iron ions were reduced to an extremely low level (0.19 mg/L) by participating in an oxidation process. Meanwhile, the Cu 2+ ions in AMD facilitated the coagulation-flocculation process. Comparison experiments confirmed that the method was superior to the AMD alone (54.26%) and H 2 O 2 alone (32.23%) in terms of performance in degrading SBX. The kinetic results showed that SBX degradation followed a pseudo first-order kinetic model . Additionally, the electron paramagnetic resonance (EPR) and quenching results suggested that hydroxyl radicals (•OH) were the main active species in AMD-H 2 O 2 system. Degradation products were analyzed, and two possible pathways of SBX degradation were proposed. One pathway displayed that the SBX was first transformed into butyl xanthate peroxide (BPX), CO 3 2− and S 2 O 3 2− , and then further decomposed into CO 2 , H 2 O and SO 4 2− under the ongoing •OH attack. Another pathway showed that precipitates consisting of butyl copper xanthate and iron oxide species were generated during the SBX degradation. This study provides a novel perspective on the innovative application of AMD in Fenton oxidation and provides a strong basis for the green and sustainable treatment of xanthate wastewater in tailings.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Xin Xiang,Wenxuan Deng,Zhiyi He,Dongyun Chen,Najun Li,Qingfeng Xu,Hua Li,Jianmei Lu
In recent years, oil spills and the discharge of industrial organic wastewater have not only damaged society and the economy, but also have had a negative impact on the human environment. The composition of oily wastewater is complex and hazardous. It mainly comprises insoluble organic substances and unsaturated aliphatic hydrocarbons. It exists in the form of oil–water mixtures, freely suspended emulsions, and stable emulsions containing surfactants. The shortage of fresh water resources and how to effectively separate oil and water present serious challenges to the scientific community. In this study, we designed a graphene aerogel with magnetic oil-absorbing functionality, which not only has emulsion-breaking functionality, but also can repeatedly adsorb organic pollutants . More importantly, it exhibits a strong Fenton catalytic effect and can effectively degrade pollutants. The aerogel designed in this research integrates adsorption, catalysis and degradation, and exhibits excellent purification of wastewater containing pollutants such as dyes, antibiotics and aromatic hydrocarbons , providing a novel insight into the treatment of oily wastewater.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Sheng Guo,Meng Chen,Yu Wei,Liming You,Chao Cai,Qingsong Wei,Kun Zhou
Zero-valent iron (ZVI) has emerged as an efficient catalyst for facilitating the decomposition of organic pollutants. However, practical applications of ZVI remain limited owing to its susceptibility towards oxidation and agglomeration. Herein, we utilize 3D printing to fabricate hierarchically porous ZVI (3D-ZVI), which displays a high level of printing precision and superb compression resistance. The 3D-ZVI catalyst can effectively activate peroxymonosulfate (PMS) to degrade a diverse selection of organic contaminants. Notably, while the catalytic activity of 3D-ZVI is comparable to that of Fe powder under similar conditions, the concentration of leached Fe ions of the former is 6.3 times lower than that of the latter. Moreover, 3D-ZVI is capable of maintaining an efficient catalytic performance throughout 45 continuous reactions, which is significantly superior to most previously reported powder catalysts. The high-valent iron-oxo species generated in the 3D-ZVI/PMS system are primarily responsible for contaminant removal, while hydroxyl and sulfate radicals play a lesser role. Additionally, the degradation intermediates and their toxicity levels are investigated. This work provides insight into the practical applications of the ZVI/PMS system, and it also serves as a guide for the rational design of efficient and stable catalysts that can be conveniently recovered from aqueous environments.
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ACS Nano
·
2023
·
IF 17.1
Naihan Huang,Xiao-Yan Tang,Wei Meng,Ye-Hua Lai,Xuan Zhou,Xue-Zhao Yu,Wen-Hua Zhang,Jin-Xiang Chen
Due to the immunosuppressive tumor microenvironment (TME) and weak radiation absorption, the immune response triggered by radiation therapy (RT) is limited. Herein, a core–shell nanosensitizer UiO@MnS (denoted as UM) was genuinely constructed for the amplification of RT efficacy and induction of immunogenicity via integrating MnS-reprogrammed TME with Hf-based UiO-sensitized RT. The acid-sensitive MnS would produce H2S under acidic TME to improve oxygenation through inhibition mitochondrial respiration and reducing metabolic oxygen consumption, leading to decreased HIF-1α expression and enhanced radiosensitization. In addition, the generated H2S inhibited the catalase activity to increase the H2O2 level, which subsequently enhanced the Mn2+-mediated Fenton-like reaction, resulting in G2/M cell cycle arrest to improve the cellular sensitivity for radiation. This impressive tumor oxygenation, cell cycle arrest, and radiosensitization procedure boosted RT efficacy and resulted in strong antitumor immunogenicity. Taken together, combining the immunosuppressive TME modulation with a sensitizing radiation strategy shows great promise for magnifying immunogenic RT outputs.
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