SCIENCE OF THE TOTAL ENVIRONMENT
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2023
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IF 9.8
Teng Xie,Lixin Zhao,Zonglu Yao,Kang Kang,Jixiu Jia,Tingxia Hu,Xinyi Zhang,Yuxuan Sun,Lili Huo
Investigation on the distribution and mechanism of co-pyrolysis products is vital to the directional control and high-value utilization of agriculture solid wastes. Co-pyrolysis, devolatilization, kinetics characteristics, and evolution paths of corn stalk (CS) and low-density-polyethylene (LDPE) were investigated via thermogravimetric experiments. The co-pyrolysis behaviors could be separated into two stages: firstly, the degradation of CS (150– 400 °C); secondly, the degradation of CS (400– 550 °C). The devolatilization index (DI) increased with the addition of LDPE. Furthermore, a combination of devolatilization chemical analysis with product analysis to analyze the intrinsic mechanism during co-pyrolysis. The results indicated that the yield of alkanes and olefin in gas products increased with the addition of LDPE. Additionally, LDPE pyrolysis maybe abstract hydrogen from CS pyrolysis and evolved into hydrogen, methane, and ethylene. Further, the co-pyrolysis kinetic parameters were computed by using model-free isoconversion methods, which showed promotion of CS pyrolysis and the reduced activation energy. All the activation energy were declined, which indicated a “bidirectional positive effect” during co-pyrolysis. The mean activation energy of P-cellulose (P-CE), P-hemicellulose (P-HM), P-lignin (P-LG), and LDPE decreased by 23.49 %, 12.89 %, 15.36 %, and 27.82 %, respectively. This study further proves the hydrogen donor transfer pathway in the co-pyrolysis process of CS and LDPE, providing theoretical support for the resource utilization of agricultural solid waste.
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高影响因子
WATER RESEARCH
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2023
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IF 12.8
Chaoyun Ying,Chang Liu,Feng Zhang,Lirong Zheng,Xiaoming Wang,Hui Yin,Wenfeng Tan,Xionghan Feng,Bruno Lanson
Manganese (Mn) oxides are extensively used to oxidize As(III) present in ground, drinking, and waste waters to the less toxic and more easily removable As(V). The common presence of multiple other cations in natural waters, and more especially of redox-sensitive ones such as Fe 2+ , may however significantly hamper As(III) oxidation and its subsequent removal. The present work investigates experimentally the influence of Mn(III) chelating agents on As(III) oxidation process in such environmentally relevant complex systems. Specifically, the influence of sodium pyrophosphate (PP), an efficient Mn(III) chelating agent, on As(III) oxidation by birnessite in the presence of Fe(II) was investigated using batch experiments at circum-neutral pH. In the absence of PP, competitive oxidation of Fe(II) and As(III) leads to Mn oxide surface passivation by Fe(III) and Mn(II/III) (oxyhydr)oxides, thus inhibiting As(III) oxidation. Addition of PP to the system highly enhances As(III) oxidation by birnessite even in the presence of Fe(II). PP presence prevents passivation of Mn oxide surfaces keeping As and Fe species in solution while lower valence Mn species are released to solution. In addition, reactive oxygen species (ROS), tentatively identified as hydroxyl radicals (•OH), are generated under aerobic conditions through oxygen activation by Fe(II)–PP complexes, enhancing As(III) oxidation further. The positive influence of Mn(III) chelating agents on As(III) oxidation most likely not only depend on their affinity for Mn(III) but also on their ability to promote formation of these active radical species. Finally, removal of As(V) through sorption to Fe (oxyhydr)oxides is efficient even in the presence of significant concentrations of PP, and addition of such Mn(III) chelating agents thus appears as an efficient way to enhance the oxidizing activity of birnessite in large-scale treatment for arsenic detoxification of groundwaters.
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CHEMOSPHERE
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2023
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IF 8.8
Yanye Tian,Yu Li,Guang-Guo Ying,Yong Feng
The extensive presence of organic micropollutants in complex water matrices requires the development of selective oxidation technologies . In this study, a novel selective oxidation process was developed via the conjunction of FeMn/CNTs with peroxymonosulfate and successfully used to remove micropollutants such as sulfamethoxazole (SMX) and bisphenol A from aqueous solutions. FeMn/CNTs were prepared using a facile co-precipitation method, characterized using a series of surface characterization techniques, and then tested for pollutant removal . The results showed that the FeMn/CNTs had much greater reactivity than CNTs , manganese oxide , and iron oxide . The pseudo-first-order rate constant with FeMn/CNTs was more than 2.9–5.7 times that of the other tested materials. The FeMn/CNTs had great reactivity in a wide range of pH values from 3.0 to 9.0, with the best reactivity found at pH values of 5.0 and 7.0. High-valent metal-oxo species such as Fe(IV) O and Mn(IV) O and superoxide anion radicals were determined to be the reactive species and were responsible for the oxidation of SMX. These reactive species were selective; therefore, the overall removal performance of SMX was not obviously influenced by high levels of water components including chloride ions, bicarbonates , and natural organic matters. The results from this study may promote the design and application of selective oxidation technologies for micropollutant abatement.
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高影响因子
APPLIED SURFACE SCIENCE
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2023
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IF 6.7
Binbin Tan,Jing Wang,Yao Deng,Huidi Zhang,Jiang Wang,Zhihao Zhang,Wenlei Wang
The key to enhancing the activation efficiency of peroxydisulfate (PDS) lies in facilitating the adsorption of PDS and accelerating the rate of electron transfer at the interface. In this work, the oxygen vacancy (Ovs) concentration of ultrathin Bi 4 Ti 3 O 12 (BTO) was controlled in situ by high-energy electron beam bombardment. BTO V -300 exhibited a significant activation effect on PDS. The degradation rate constant ( k obs ) for the removal of ciprofloxacin (CIP) was measured to be 0.2080 min −1 under visible light irradiation, which was 3.71 times greater than that of the original BTO. Density functional theory calculations uncovered the principal role of oxygen vacancies as active sites for PDS activation. Introducing OVs significantly boosted the adsorption energy of PDS on BTO and lengthened the O O bond of PDS. This study represents the potential mechanism behind the activation of PDS by BTO V and provides valuable insights for enhancing the photoactivation efficiency of PDS.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yuxiang Yang,Xiaocui Huang,Mengyang Dong,Ziling Chang,Hongming Yuan,Yan Huang,Xiangnong Liu,Jianbo Zhang,Anbang Dai
As a common pollutant in the environment, trichloroacetic acid (TCA) is difficult to be completely degraded by common advanced oxidation processes (AOPs) due to its high C-Cl bond content. Advanced oxidation–reduction processes (AORPs) may improve the degradation performance of TCA. In this work, we use Fe 0 Ni 0 bimetal as reducing catalyst, hollow mesoporous silicone nanoparticles (HMONs) modified by ZIF-8 as immobilized carrier, horseradish peroxidase (HRP) and Fe 0 Ni 0 were fixed in the carrier to form a AORP system for degradation of TCA. The effects of temperature, pH, H 2 O 2 concentration, doping ratio on the degradation performance of the catalyst and the degradation mechanism of the composite catalyst were investigated. Degradation experiments showed that H· and OH· were present in the dual system, dechlorination and decarboxylation exist at the same time. Under the condition of 55 °C and pH = 4, 30 mg Fe 0 Ni 0 and 20 mg immobilized enzyme shows the best degradation on TCA, and 81.48 % of 20 mg·L −1 TCA could be degraded by 2 h.
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Engineering
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2023
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IF 12.8
Ning Li,Haoxi Dai,Mengting He,Jun Wang,Zhanjun Cheng,Beibei Yan,Wenchao Peng,Guanyi Chen
The distribution pattern of metals as active centers on a substrate can influence the peroxymonosulfate (PMS) activation and contaminants degradation. Herein, atomic layer deposition is applied to prepare Cu single atom (SA-Cu), cluster (C-Cu), and film (F-Cu) decorated MXene catalysts by regulating the number of deposition cycles. In comparison with SA-Cu-MXene (adsorption energy ( E ads ) = −4.236 eV) and F-Cu-MXene ( E ads = −3.548 eV), PMS is shown to adsorb preferably on the C-Cu-MXene surface for activation ( E ads = −5.435 eV), realizing higher utilization efficiency. More SO 4 − · are generated in C-Cu-MXene/PMS system with steady-state concentration and 1–3 orders of magnitude higher than those in the SA-Cu-MXene and F-Cu-MXene activated PMS systems. Particularly, the contribution of SO 4 − · oxidation to sulfamethoxazole (SMX) degradation followed the order, C-Cu-MXene (97.3%) > SA-Cu-MXene (90.4%) > F-Cu-MXene (71.9%), realizing the larger SMX degradation rate in the C-Cu-MXene/PMS system with the degradation rate constants ( k ) at 0.0485 min −1 . Additionally, SMX degradation routes in C-Cu-MXene/PMS system are found with fewer toxic intermediates. Through this work, we highlighted the importance of guided design of heterogeneous catalysts in the PMS system. Appropriate metal distribution patterns need to be selected according to the actual water treatment demand. Metal sites could be then fully utilized to produce specific active species to improve the utilization efficiency of the oxidants.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Shiwen Dong,Wen Xu,Qingqing Guo,Kai Luo,Haijun Cheng,Juntao Tang,Da Wang,Zhiqiao He,Lizhang Wang,Shuang Song,Jun Ma
Designing efficient and environmentally friendly catalysts is essential to activating ozonation for wastewater remediation. This study prepared soybean biochar (SB), adzuki beans biochar (AB), and mung beans biochar (MB) catalysts using moldy legumes as precursors. The biochars were characterized to investigate the surface characters’ effect on ozone activation toward 2, 6-dimethylpyrazine (2,6-DMP) degradation. All prepared samples drastically facilitated the degradation more than with sole ozonation. It was found that at pH 7 with 10 mg L −1 catalysts, the removal rates of 5 μM 2,6-DMP were 88.3 %, 90.7 %, and 87.3 % by SB, MB, and AB at 30 min, respectively. The surface-area-normalized reaction rate constants (k obs /S BET ) showed that AB exhibited the best catalytic activity with the rate of 1.5 × 10 −2 mg·m 2 ·min −1 , which is 2.3- and 23.1-fold higher than that of SB and MB, respectively. Further characterization confirmed that oxygen- (C–O/C = O and –OH) and nitrogen-containing groups (pyridine N and pyrrole N) were crucial to the catalytic degradation, as electron transfer was promoted to form more ROS. In addition, the quenching test and electron paramagnetic resonance (EPR) revealed OH, O 2 − , and 1 O 2 as the main reactive oxygen species (ROS) during the heterogeneous catalytic ozonation (HCO), indicating that 2,6-DMP degradation followed the radical and non-radical oxidation pathways. Overall, this study helped to understand the relationship between surface functional groups and intrinsic activity. It also provided a new direction for utilizing agricultural waste.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Sainan Wang,Chao Yuan,Wei Chen,Yifan Niu,Yexi Yan,Fan Li,Hongmei Jiang
A series of CuO@g-C 3 N 4 composites with different contents of g-C 3 N 4 and different morphologies of CuO have been designed and prepared by hydrothermal method and applied to activate peroxymonosulfate (PMS) for the removal 2,4,6-trichlorophenol (2,4,6-TCP). The results showed that 3D spherical shape CuO-1@g-C 3 N 4 -3, being able to activate PMS to produce a large amount of singlet oxygen ( 1 O 2 ), not only had good catalytic performance, but also reduced the dissolution of Cu 2+ . By comparing the morphological characteristics, catalytic performance, free radical species, decomposition rate of PMS and surface properties of three kinds of CuO, the generation mechanism of 1 O 2 and key reasons of CuO for producing 1 O 2 were deeply explored and finally deduced. Besides, under the conditions of initial pH 7.0, catalyst dosage 50 mg·L −1 , PMS dosage 0.3 mmol·L −1 and initial concentration of 2,4,6-TCP 10 mg·L −1 , the removal rate of 2,4,6,-TCP reached 94 % at 25 min in the first cycle, and 85 % in the fifth cycle. When CuO-1@g-C 3 N 4 was applied in actual water samples, 65 % of 2,4,6-TCP was removed in the Yangtze River, and 60 % of 2,4,6-TCP in Xuanwu and Yueya Lake in 40 min. Quenching experiments and electron paramagnetic resonance (EPR) were used to indentify active species during degradation process and the degradation intermediates of 2,4,6-TCP and possible degradation pathways were determined and proposed by high performance liquid chromatography-time of flight-mass spectrometry (HPLC-TOF-MS 2 ). This study shed light on the 1 O 2 generation mechanism of catalyst and provided theoretical basis and guidance for the design of 1 O 2 catalysts rich in non-radical active species.
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Nano Research
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2023
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IF 9.9
Dong Zhicheng,Xu Yunyun,Wu Can,Chao Jin,Tian Chen,Lin Zhang
Organo-chromium(III) complex is one of the chromium contaminant species, which would transform to high-toxic Cr(VI) during migrating in the environment. Such natural organo-chromium(III) (NOCr) is difficult to remove by traditional degradation or precipitation methods, due to its high stability and solubility. Herein, we demonstrated a novel NOCr removing method by transforming it to certain structures similar to Cr-Fe minerals in nature, through a self-circulating decomplex and immobilization mechanism with nano zero-valent iron (nZVI). Taking chromium glycinate (Cr-Gly) as a probe, nZVI showed a high Cr removal efficiency of 99.4% under ambient conditions. The removal process included three stages of adsorption, decomplexation, and re-immobilization. Cr-Gly was first adsorbed on the surface of nZVI by chemisorption of the oxide shell. Then, the adsorbed Cr-Gly was decomplexed and oxidized to Cr(VI) by ·OH and 1 O 2 , which were generated from molecular oxygen activated by nZVI. Meanwhile, the released Cr(VI) could be in-situ adsorbed and re-reduced to Cr(III), which was further immobilized in form of Cr-O-Fe complex. As the Cr-O-Fe complexing structure was similar to that of Cr-Fe minerals (such as chromohercynite) in nature, this work explored a novel and efficient NOCr removing method that was potential to weaken chromium pollution in the environment.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Lu Xu,Xiaojia Wei,Yuetong Qi,Wei Qiao,Juan Shi,Yabo Shang,Keqian Li,Xin Jin,Xue Bai,Xuan Shi,Pengkang Jin
The activation of persulfate (PS) in dissolved organic matter (DOM) solution using visible light has demonstrated potential for advanced wastewater treatment. This study presents a novel visible light-assisted homogeneous Fenton-like process (DOM-Fe 3+ -PS-Vis) for the efficient DOM degradation, based on the ligand-to-metal charge transfer (LMCT)-induced enhanced Fe 3+ reduction and PS activation. The simultaneous addition of Fe 3+ and PS to DOM-enriched solutions under visible light significantly improved PS activation, leading to the degradation of DOM and coexisting organic contaminants. The PS decomposition rate constant in the DOM-Fe 3+ -PS-Vis process was calculated to be 3.5–20.69 times higher than that of the DOM-PS-Vis, Fe 3+ -PS-Vis, and DOM-Fe 3+ -PS-Dark systems. Notably, over half of the decomposed PS in the DOM-Fe 3+ -PS-Vis process was activated by Fe 2+ generated via the LMCT between DOM and Fe 3+ . SO 4 − and OH were identified as the dominant reactive species present in the DOM-Fe 3+ -PS-Vis process with the steady-state concentration of 1.63–4.11 × 10 −13 M and 0.07 × 10 −13 M, respectively, which were 2.4–81.5 and 0.5–7 times higher than those in the DOM-PS-Vis, Fe 3+ -PS-Vis, and DOM-Fe 3+ -PS-Dark systems. Additionally, hydrophobic components with more aromatic carbon in DOM were found to promote the catalytic performance of the DOM-Fe 3+ -PS-Vis process. This study highlights the efficiency and promise of LMCT-induced enhanced Fe 3+ reduction and PS activation in DOM-enriched solutions under visible light for advanced wastewater treatment.
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Alexandria Engineering Journal
·
2023
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IF 6.8
Changbiao Chi,Buqing Huo,Zedong Liang,Chenxi Hu,Qingyue Sun,Shufeng Zhou
The presence of antibiotics in wastewater has become a significant concern due to their potential environmental impact and contribution to antibiotic resistance. In this study, we investigated the degradation of tetracycline, a commonly used antibiotic, in wastewater using a system based on zero-valent nano iron assisted micro-nano bubbles (MB/nZVI). The synthesized nZVI-BC composite, consisting of nano zero-valent iron particles loaded onto phosphoric acid-activated biochar, served as an efficient adsorbent for tetracycline removal. Our findings revealed that the combination of MBs and nZVI significantly enhanced the degradation efficiency of tetracycline. The MB/nZVI system exhibited the highest removal rate of 82.81% after a 2 h reaction, surpassing the performance of MB alone, nZVI-BC alone, and conventional bubble (CB)/nZVI-BC systems. Furthermore, the MB/nZVI system showed superior degradation performance at a dosage of 25 g/L and an MB flow rate of 30 mL/min. The pH condition had no significant effect on tetracycline degradation in the MB/nZVI system. Our results demonstrate that the use of MB/nZVI has the potential to be a sustainable and efficient approach for the remediation of tetracycline-contaminated wastewater.
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Journal of Materials Chemistry B
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2023
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IF 7
Ting Chen,Jie Yang,He Zhao,Dajian Li,Xiaoyong Luo,Zhiyu Fan,Biye Ren,Yuepeng Cai,Renfeng Dong
Ferroptosis is a non-apoptotic form of cell death that is dependent on the accumulation of intracellular iron that causes elevation of toxic lipid peroxides. Therefore, it is crucial to improve the levels of intracellular iron and reactive oxygen species (ROS) in a short time. Here, we first propose ultrasound (US)-propelled Janus nanomotors (Au–FeOx/PEI/ICG, AFPI NMs) to accelerate cellular internalization and induce cancer cell ferroptosis. This nanomotor consists of a gold–iron oxide rod-like Janus nanomotor (Au–FeOx, AF NMs) and a photoactive indocyanine green (ICG) dye on the surface. It not only exhibits accelerating cellular internalization (∼4-fold) caused by its attractive US-driven propulsion but also shows good intracellular motion behavior. In addition, this Janus nanomotor shows excellent intracellular ROS generation performance due to the synergistic effect of the “Fenton or Fenton-like reaction” and the “photochemical reaction”. As a result, the killing efficiency of actively moving nanomotors on cancer cells is 88% higher than that of stationary nanomotors. Unlike previous passive strategies, this work is a significant step toward accelerating cellular internalization and inducing cancer-cell ferroptosis in an active way. These novel US-propelled Janus nanomotors with strong propulsion, efficient cellular internalization and excellent ROS generation are suitable as a novel cell biology research tool.
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高影响因子
危险品化学品经营许可证（带存储）