WATER RESEARCH
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2022
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IF 13.4
Dehua Xia,Qi Chen,Yimu Jiao,Qiyu Lian,Mingzhe Sun,Chun He,Jin Shang,Tianqi Wang
Solar disinfection (SODIS) is regarded as an affordable and effective point-of-use (POU) water disinfection treatment urgently needed in rural developing world. This work developed an enhanced SODIS scheme that utilized a novel flower pollen-based catalyst (Te-TRP). The bench-scale experiments demonstrated 100% photothermocatalytic inactivation of approximately 7-log E. coli K-12, Spingopyxis sp. BM1-1, or S. aureus bacterium by Te-TRP within 40–60 min. Moving toward practical device design, we constructed a flow-through reactor and demonstrated the outstanding water disinfection performance of Te-TRP. The in-depth mechanistic study revealed the synergetic effect between photocatalysis and photothermal conversion and identified the bacterial inactivation pathway. 1 O 2 and ·O 2 ¯ were verified to be the dominant reactive oxygen species involved in the bacterial inactivation. The damage to bacterial cells caused by photothermocatalytic reactions was systematically investigated, demonstrating the cell membrane destruction, the loss of enzyme activity, the increased cell membrane permeability, and the complete inactivation of bacteria without the viable but nonculturable state cells. This work not only affords a facile approach to preparing biomaterial-based catalysts capable of efficient photothermocatalytic bacterial inactivation, but also proposes a prototype of POU water treatment, opening up an avenue for sustainable environmental remediation.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Siyu Xu,Liangtao Wen,Chen Yu,Song Li,Jingchun Tang
In this study, novel metallic oxide catalyst MnFe 2 O 4 @biochar composite was synthesized by sol–gel pyrolysis loading of MnFe 2 O 4 on biochar, and then used to activate peroxymonosulfate (PMS) to degrade bisphenol A (BPA). Characterization results demonstrated that the Fe and Mn oxide particles were homogeneously distributed on the surface of biochar, which avoided the aggregation of metal oxides. The strong magnetism of the composite was conducive to recycling during practical application. In the PMS system activated by MnFe 2 O 4 @biochar composite, the removal rate and mineralization rate of 20 mg/L BPA reached 100% and 95.9% within 30 min, respectively. The quenching experiments and electron paramagnetic resonance (EPR) study verified the coexistence of free-radical and non-radical pathways in the MnFe 2 O 4 @biochar/PMS system, with O 2 •- as the dominant active species, followed by singlet oxygen ( 1 O 2 ). The catalytic degradation process could adapt a wide pH range from weak acid to the alkaline matrix and showed negligible influence by anions and humic acid. The characterization results confirmed the synergistic effect of the bimetal, proving that the introduction of biochar and second metal source into iron-based catalyst played an important role in the composite. Overall, the MnFe 2 O 4 @biochar showed promising performance in activating PMS for organic pollutant degradation in water with high stability and safe performance.
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Materials Today Chemistry
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2022
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IF 7.613
N. Xu,Y. Zhang,J. Han,C. Xiao
High stretching is an effective route to attain high performance fiber. Therefore, the stretchability of wet-spun poly(acrylic acid) (PAA) fiber is important for the preparation of high performance PAA fiber by stretching. A combination of coordination and hydrogen bonding was synergistically used to prepare highly stretchable wet-spun PAA fibers, and high stretching was subsequently carried out to induce the production of molecular orientation and fibrillar crystals, which can remarkably enhance the strength of resulting fiber. The breaking strength of stretched fiber reached up to 1.631cN/dtex, increasing by 2813% compared to that of unstretched fiber. Moreover, high stretching was used to thin the resulting fiber and promote the transformation of PAA chains from coiled to extensional conformation, so that the carboxyl groups wrapped by coiled PAA chains were exposed to the environment. When the highly stretched fiber was used to decolorize methylene blue (MB) aqueous solution, the exposed carboxyl groups can quickly re-coordinate with the iron ions eluted by MB aqueous solution to minimize the loss of iron ions. The measurement results showed that the average concentration of eluted iron ions was only 3.20 mg/L during 40 operation cycles for the highly stretched fiber, decreasing by 64.0% compared to that of unstretched fiber. Due to low iron ion leaching-out, the highly stretched fiber showed superstable activity in catalyzing H 2 O 2 to oxidatively decolorize MB. The research results revealed that the obtained fiber can decolorize more than 90% MB within 3 min during 40 cycles without showing any obvious attenuation in decolorization efficiency and decolorization rate. In this case, the Fenton catalysts reported by literature are scarcely comparable to the prepared fiber in many aspects. Therefore, the fiber prepared in this work can be expected to show great potential for application in the field of dye wastewater treatment.
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CHEMOSPHERE
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2022
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IF 8.943
Ting Chen,Zhiliang Zhu,Yue Wang,Hua Zhang,Yanling Qiu,Daqiang Yin
Facilitating reactive oxygen species (ROS) generation is an effective way to promote the heterogeneous catalytic efficiency for organics removal. However, the metal leaching in metal-based catalysts and the low activity of non-metallic materials restrict ROS production. In this work, the purpose was achieved by loading a small amount of spinel CuFe 2 O 4 onto porous carbon nitride substrate. The synthesized CuFe 2 O 4 @O–CN composite first to activate peroxymonosulfate (PMS), which produce a plenty of ROS (•OH, SO 4 • − and 1 O 2 ) for organics removal, leading to highly oxidation for diverse organics. Through the comparative analysis of the surface composition before and after reaction, we found that the interface multi-electron transfer routs, including surface Cu(II)/Cu(I), Fe(III)/Fe(II) and their cross interaction, participated in the redox cycle, giving rise to the rapid and massive production of ROS, so that DMPO and TEMP were instantly oxidized in electron paramagnetic resonance (ESR) detection. Importantly, the carrier of porous O–CN, which acted as the electron transfer mediator, not only favors PMS adsorption via surface –OH, but also facilitates the conversion between different metal species. As a result, the CuFe 2 O 4 @O–CN/PMS system can remove 99.1% BPA and achieve 52.6% mineralization under optimized conditions. Thus, this study not only sheds light on the tailored design of heterogeneous catalyst for organics removal and elucidates the interfacial catalytic mechanisms for PMS activation .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Rui Zhang,Changlin Liu,Ruoxi Zhao,Yaqian Du,Dan Yang,He Ding,Guixin Yang,Shili Gai,Fei He,Piaoping Yang
There is an urgent need to develop photosensitive nanoenzymes with better phototherapeutic efficiency through simple processes. By exploiting semiconductor catalysis and defect chemistry principles, herein, a MnMoO x composite semiconductor nanoenzyme was developed to achieve a fully integrated theranostic nanoenzyme for highly efficient photo/chemo-enzyme-dynamic eradication of deep tumors. Relative to iron oxides, manganese oxides offer ideal catalytic performance under near-neutral conditions, which helps to broaden the suitable pH range of the MnMoO x nanoenzyme for antitumor therapy. Furthermore, with the assistance of glutathione depletion, Mn 4+ /Mo 6+ was successfully converted to Mn 2+ /Mo 5+ , inhibiting the scavenging of reactive oxygen species (ROS) and promoting cycling. Therefore, MnMoO x has favorable catalase (CAT)-like activity and oxidase (OXD)-like activity in the tumor microenvironment (TME) for promoting the “H 2 O 2 O 2 O 2 − ” and “H 2 O 2 OH” cascade reactions. The abundant oxygen vacancy defects also promote the surface plasmon resonance (SPR) effect in the second near-infrared (NIR-II) window of MnMoO x , which significantly enhanced its photothermal therapy (PTT) effect and catalytic activity. In detail, ROS production was significantly enhanced due to the adsorption of water and oxygen molecules by the rich oxygen vacancies of MnMoO x . MnMoO x also exhibited excellent multi-modal imaging activity (including computed tomography (CT), magnetic resonance imaging (MRI), and photoacoustic (PA)), which can be exploited to better guide the administration of medication.
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ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Yuan Zhang,Weina Meng,Xiao Li,Dong Wang,Shaomin Shuang,Chuan Dong
Development of multifunctional enzymatic nanomaterials with rapid and sensitive characteristics for glutathione determination is extremely urgent for early cancer diagnosis. Herein, a core–shell ultrasensitive nanozyme (denoted as CPT/DM-FA) for triple-mode glutathione sensing and specific in vitro cancer detection is constructed. The dendritic mesoporous silica nanoparticle (DMSN) core not only acts as a camptothecin carrier, but also offers the nanoplatform to synthesize the MnO2 shell. Due to the DMSN-regulated high dispersion of MnO2, the atomic utilization efficiency of MnO2 is surprisingly enhanced, and leads to notable enzymatic activity with Km 0.136 μM and Vmax 0.59 μM/s. In addition, by integrating the quenching ability based on fluorescence resonance energy transfer and oxidase-mimic-mediated 1O2, O2– generation of MnO2, the fluorescence, UV–vis, and colorimetric method for glutathione sensing is established with a comprehensive linear range from 2 to 250 μM and a limit of detection of 0.654 μM. Besides, after surface folic acid modification, the CPT/DM-FA could also specifically detect cancer cells from 25 to 1 50 000 through the color reaction of 3,3′,5,5′-tetramethylbenzidine. We believe this nanozyme could afford a potential strategy to amplify the nanozyme activity for further biomedical applications.
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ADVANCED POWDER TECHNOLOGY
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2022
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IF 4.969
Yan Wang,Kangkang Miao,Weixing Zhao,Hongbo Jiang,Liangliang Liu,Dengwei Hu,Bin Cui,Yaping Li,Yue Sun
In this study, nanoparticle-assembled Bi 25 FeO 40 materials were synthesized by a novel and simple process, and their microstructure was regulated by different methods of adding Bi 3+ and Fe 3+ . The novel nanoparticle-assembled tetrakaidekahedron Bi 25 FeO 40 materials exhibited more oxygen vacancy and larger specific surface area than irregular or cubic-like Bi 25 FeO 40 microcrystals and revealed better photo-Fenton catalytic oxidation activity toward degrading Rhodamine B (RhB) pollutants. These novel materials activated H 2 O 2 in visible light to produce non-free radicals 1 O 2 and hole (h + ) active oxidative species that dominated the catalytic degradation of RhB. Complete degradation of RhB was achieved after 1 h. The possible reaction mechanisms of the photo-Fenton catalytic system are discussed in detail by radical scavenging tests, X-ray phosphorescence analysis, and electron paramagnetic resonance spectroscopy . The results provided a way to rationally explore and construct photo-Fenton catalysts for wastewater treatment .
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JOURNAL OF CATALYSIS
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2022
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IF 8.047
Yujun Zhang,Hao Tian,Zhaowei Cui,Zhen Yin,Hongsen Hui,Hong Wang,Lei Zhang,Hongchang Pei,Zhenhuan Li,Bhekie B. Mamba,Jianxin Li
To further improve the capability of flow electrochemistry, the multistage plug-flow electrochemical membrane reactor (PF-ECMR) with membrane electrode was developed for enhancing the oxidation of cyclohexane (CHA) to produce KA oil (mixture of cyclohexanol and cyclohexanone). The catalytic results demonstrated that the CHA conversion and the selectivity to KA oil were up to 95.6% and > 99%, which was the highest in comparison with most of the state-of-the-art catalytic processes reported in the previous works. The mechanism was explored by density functional theory (DFT) calculations, indicating the auxo-action effect of cyclohexanone was beneficial for the formation of cyclohexyl hydroperoxide so as to enhance the CHA conversion. The excellent performance of PF-ECMR was also attributed to the staggered electric field and the accumulative effect of the multi-electrodes. This study provided a successful case of a combination of theoretical prediction and experimental verification together for organic synthesis.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Xinyi Zhang,Zhiquan Yang,Xiandi Cui,Wanhui Liu,Baosheng Zou,Wenning Liao
Cobalt-calcium bimetallic oxide (ECCO) was successfully prepared using eggshells and cobalt nitrate, which could be used to activate peroxymonosulfate (PMS) to remove norfloxacin (NOR). The compositional structure and surface properties of the catalysts were explored by various characterization analysis. The degradation efficiency of ECCO was 7.86 and 440 times higher than that of cobalt oxide and calcium oxide , respectively. The prepared ECCO (0.1 g/L) had a high degradation efficiency of over 90% against NOR (10 mg/L, 100 mL) by activating the PMS (0.15 g/L) at a wide pH range of 3.0–9.0 in 35 min. With a NOR removal efficiency of 91.4% after five cycles, the catalyst showed good reusability. The high degradation efficiency of NOR was resulted from enhanced electron transfer capability, the low point of zero charge and diversified reactive oxygen species (ROS). The ROS were identified as SO 4 • − , •OH and 1 O 2 , which were produced by activating PMS on the active sites of Co and oxygen vacancies . It is the first report of the use of eggshells to synthesize cobalt-calcium bimetallic oxides ECCO for the activation of PMS to eliminate NOR, which is important for the development of green and efficient catalysts.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Xi Li,Shiwen Wang,Baokang Xu,Xiao Zhang,Yanhua Xu,Peng Yu,Yongjun Sun
The low surface area, low porosity, weak charge transport, and metal species loss of conventional metal-based carbon materials are the main defects limiting their environmental application. In this study, a metal–organic framework (MOF)-supported Co-doped hollow carbon nitride (ZCCN) catalyst was constructed by etching zeolitic imidazolate framework-67 (ZIF-67). Excellent visible light capture and electron transfer performance of the catalyst were revealed, and 99% tetracycline (TC) degradation and 65.9% peroxymonosulfate (PMS) decomposition were achieved within 40 min. Efficient separation and transport of photogenerated electrons are the key to PMS activation and TC degradation. Meanwhile, the preserved skeleton structure of ZIF-67 and the triazine rings of carbon nitride endowed the catalyst with enhanced stability and lessened Co leaching. Density functional theory (DFT) was applied to investigate the internal effect of PMS activation on Co sites. The reduced toxicity of the intermediates revealed the potential of the ZCCN/PMS system on eliminating environmental risks caused by TC. This study provides new insights into the design of stable MOF-derived metal-based heterogeneous catalysts.
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ACS Omega
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2022
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IF 4.132
Ji Shi,Wenyu Huang,Hongxiang Zhu,Jianhua Xiong,Huiting Bei,Shuangfei Wang
Widespread application of TiO2 for degradation of antibiotics is restricted by mainly the low photodegradation efficiency under solar irradiation. To expand the application of TiO2, the key factors that should be improved are visible-light response, yield of electrons and holes, and durability. Herein, we report a visible-light responsive and durable sugarcane-bagasse-derived biochar supported hydrogenated TiO2 (HSCB/H2-TiO2) photocatalyst with higher electron production fabricated by a facile one-pot hydrogenation. Mild hydrogenation temperature preserved the lotus-stem-like structure of sugarcane bagasse and gave the photocatalyst great separability. The superior durability of HSCB/H2-TiO2 was demonstrated by 12 rounds of repeated degradation of methylene blue (MB). In addition, the electron paramagnetic resonance (EPR) results demonstrated that the biochar skeleton contains abundant persistent free radicals (PFRs), which can provide excess electrons to form more •O2–. Meanwhile, radical quenching experiment and EPR radical trapping results also revealed that •O2– was the most dominant species for enrofloxacin (ENR) degradation. Thus, the as-fabricated photocatalyst shows excellent solar-driven degradation of ENR, and 95.6% of ENR was degraded in 180 min under simulated solar irradiation. Possible ENR degradation pathways and mechanism are also proposed based on the identified intermediates.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Chuangjian Su,Ruhong Li,Chaolin Li,Wenhui Wang
The application of promising persulfate-based advanced oxidation processes (AOPs) for environment remediation is limited by the poor charge separation and the sluggish kinetic for active centers regeneration of the catalysts. Piezocatalytic activation has been proposed to solve the above concern recently, but little is known on its mechanism. Herein, novel piezocatalyst Bi 2 Fe 4 O 9 nanosheets (BFO NSs) are demonstrated to significantly improve peroxydisulfate (PDS) activation efficiency via piezocatalysis, resulting SO 4 •− and •OH as the dominant active species for organic pollutants degradation. Further DFT calculations and experimental investigations confirm that the Fe 2+ in BFO NSs as active sites donate electrons for PDS to generate SO 4 •− , and simultaneously that the piezo-electrons can accelerate the regeneration of Fe 2+ , thus leading to the superior catalytic activity. This work provides atomic-scale insights of catalytic sites and mechanisms of piezocatalytic PDS activation and may inspire the development of more efficient piezocatalysts and AOPs.
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