MOLECULES
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2022
·Vol. 27
·期 17
·5576
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IF 4.927
Songtao Liu,Rui Yan,Muhammad Humayun,Huanli Zhang,Yang Qu,Yingxue Jin
It is highly desired to enhance charge separation and O2adsorption of the pyropheophorbide-a (Ppa) to promote visible-light activity and stability. Herein, Ppa modified 001-facet-exposed TiO2nanosheets (Ppa/001T) nanocomposites with different weight ratios were fabricated via the self-assembly approach by OH induced. Compared with the bare Ppa, the 8% amount optimized 8Ppa/001T sample displayed 41-fold enhanced activity for degradation of Ametryn (AME) under visible-light irradiation. The promoted photoactivities could be attributed to the accelerated charge carrier’s separation by coupling TiO2as thermodynamic platform for accepting the photoelectrons with high energy from Ppa and the promoted O2adsorption because of the residual fluoride on TiO2. As for this, a distinctive two radicals (•O2−and •OH) involved pathway of AME degradation is carried out, which is different from the radical pathway dominated by •O2−for the bare Ppa. This work is of utmost importance since it gives us detailed information regarding the charge carrier’s separation and the impact of the radical pathway that will pave a new approach toward the design of high activity visible-light driven photocatalysts.Keywords:Ppa;001-facet-exposed TiO2;charge separation;visible-light photocatalysis;Ametryn
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高影响因子
Minerals
·
2022
·Vol. 12
·期 9
·1097
·
IF 2.818
Dongyue Wang,Yuhang Meng,Aidong Tang,Huaming Yang
Engineered nanoparticle–support interaction is an effective strategy for tuning the structures and performance of engineered nanoparticles. Here, we show that tuning the dehydroxylation of kaolinite nanoclay as the support could induce zinc oxide–kaolinite interactions. We used free energy theory, electron microscopy, and X-ray photoemission spectroscopy to identify interaction strengths between metal oxides and the underlying nanoclay induced by dehydroxylation. Desirable exposure of nanoparticle sites and the geometrical and crystal structure were obtained by tuning the interface interactions between ZnO nanoparticles and nanoclay. The surface free energy of zinc oxide–nanoclay results in different interfacial interactions, and the properties of the surface free energy electron-donating (γ−) and electron-accepting (γ+) parameters have significant effects on the electron acceptor. This could, in turn, promote stronger interactions between zinc oxide and the kaolinite surface, which produce more active (0001) Zn-polar surfaces with promoting zinc oxide nanoparticles growing along the <0001> direction. Reactive oxygen species, leached zinc ions, and electron transfer can modulate the antibacterial activities of the samples as a function of interface free energy. This further demonstrates the interfacial interactions induced by dehydroxylation. This work has new application potential in biomedicine and materials science.Keywords:kaolinite;dehydroxylation;interfacial interactions;ZnO nanoparticles;antibacterial activities
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ACS Nano
·
2022
·
IF 18.027
Ruoyao Li,Yuanyuan Fan,Lulu Liu,Hongna Ma,Deyan Gong,Zhaohua Miao,Hua Wang,Zhengbao Zha
The exciting success of NBTXR3 in the clinic has triggered a tumult of activities in the design and development of hafnium-based nanoparticles. However, due to the concerns of nondegradation and limited functions, the biomedical applications of Hf-based nanoparticles mainly focus on tumors. Herein, tannic acid capped hafnium disulfide (HfS2@TA) nanosheets, a 2D atomic crystal of hafnium-based materials prepared by liquid-phase exfoliation, were explored as high-performance anti-inflammatory nanoagents for the targeted therapy of inflammatory bowel disease (IBD). Benefiting from the transformation of the S2–/S6+ valence state and huge specific surface area, the obtained HfS2@TA nanosheets were not only capable of effectively eliminating reactive oxygen species/reactive nitrogen species and downregulating pro-inflammatory factors but also could be excreted via kidney and hepatointestinal systems. Unexpectedly, HfS2@TA maintained excellent targeting capability to an inflamed colon even in the harsh digestive tract environment, mainly attributed to the electrostatic interactions between negatively charged tannic acid and positively charged inflamed epithelium. Encouragingly, upon oral or intravenous administration, HfS2@TA quickly inhibited inflammation and repaired the intestinal mucosa barrier in both dextran sodium sulfate and 2,4,6-trinitrobenzenesulfonic acid induced IBD models. This work demonstrated that ultrathin HfS2@TA atomic crystals with enhanced colon accumulation were promising for the targeted therapy of IBD.
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高影响因子
Journal of Water Process Engineering
·
2022
·
IF 7.34
Xingyu Fang,Ying Wu,Lijie Xu,Lu Gan
In this study, a series of coconut shell biochars (CSB) with different pyrolysis temperature were prepared and incorporated with α-MnO 2 for bisphenol A (BPA) degradation in water through activating peroxymonosulfate (PMS). The results showed that with the assistance of CSB, α-MnO 2 /CSB exhibited superior catalytic activity over pristine α-MnO 2 , in which CSB played multiple roles in the composite. Basically, CSB could effectively improve the dispersion and expose more active sites of α-MnO 2 . Besides, CSB could build solid interactions with α-MnO 2 and boost the electron transferring rate between catalyst, PMS and BPA. Moreover, α-MnO 2 and CSB were both enrolled in the generation of radical and non-radical species for BPA degradation. Having multiple active species, the α-MnO 2 /CSB composite could maintain high catalytic performance under a wide pH range with good reusability and adaptability. The existence of both radical and non-radical pathways was further verified through identifying the BPA degradation intermediates. This study provides a new insight for the design of novel composite catalyst for water decontamination using biochar as a multifunctional participant.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Pei Chen,Wei Wang,Ningning Dong,Junjie Zhang,Tao Yang,Fatang Tan,Songwei Tan,Xinyun Wang,Xueliang Qiao,Po Keung Wong
Herein, the novel zinc peroxide/carbon quantum dots (ZnO 2 /CQD) composites were synthesized by an in-situ composite process for visible-light photocatalytic tetracycline (TC) degradation and Escherichia coli ( E. coli ) inactivation. It was found that 0.1 g/L ZnO 2 /CQD composite could degrade over 80 % of 50 mg/L TC and inactivate around 7-log E. coli cells after 2 h and 50 min of irradiation, respectively. The as-obtained ZnO 2 /CQD composites exhibited superior visible-light photocatalytic performance to individual ZnO 2 , and superoxide radical (•O 2 − ) and singlet oxygen ( 1 O 2 ) were identified to be the main reactive oxygen species (ROSs) for TC degradation and E. coli inactivation. The introduction of CQD reduced the particle size and increased specific surface area, benefiting for adsorption. Meanwhile, it promoted visible-light absorption and accelerated the separation of photogenerated electron-hole pairs with a 3-fold increase in photocurrent, thus producing more ROSs under visible-light irradiation. Moreover, the ZnO 2 /CQD composites exhibited a high adaptability towards initial solution pH, common coexisting anions, oxygen-deficient environment, diverse water sources and organic pollutants. This study not only provided highly adaptable visible-light-driven photocatalysts for organic degradation and bacterial inactivation, but also shed light on the multifunctional roles of CQD in boosting visible-light photocatalytic performance.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Jian Ke,Yuhui Ge,Qiulian Yang,Yanhua Liu,Pau-Loke Show,Ruixin Guo,Jianqiu Chen
Excess sludge disposal and management has become a global issue of scientific and public concern owing to its high yield and toxicity. In this study, for the first time, we prepared industrial and livestock sludge-derived photocatalysts using dyeing sludge and swine sludge as raw materials, respectively, using a facile pyrolysis coupled ball-milling process without additives. The photocatalytic performances of the two types of photocatalysts were evaluated using sulfamethazine as the target contaminant. The surface morphology and functional groups of the catalysts were analyzed using field-emission scanning electron microscopy combined with energy-dispersive X-ray spectroscopy and Fourier transform infrared spectroscopy . The sulfamethazine removal rate was 91.5 % under optimal conditions. Degradation intermediates were detected, and a possible degradation pathway was proposed. Major reactive oxygen species in the photocatalytic systems were investigated using electron spin resonance spectroscopy and radical trapping experiments. The results revealed that·O 2 – and h + played main roles in the degradation of SMZ. Furthermore, a pilot-scale experimental setup was designed and manufactured to realize pilot-scale production. Economic analysis of the pilot-scale experiment suggested that the developed photocatalysts are comparatively suitable for practical applications.
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Water
·
2022
·Vol. 14
·期 16
·2569
·
IF 3.53
Weifan Gao,Guichang Zhang,Xiaoping Zhang,Shaoqi Zhou,Zihao Wang
The catalytic capability of original carbon nitride (CN) is limited by a small specific surface area and high electron–hole recombination rate. In this study, WO3-loaded porous carbon nanosheets (MCA-CN/WO3) were synthesized by thermal treatment with melamine, cyanuric acid and WCl6. The MCA-CN/WO3could degrade 98% of the methylene blue (MB) within 30 min in the photo-Fenton-like process, displaying better catalytic activity than the original CN (30%), pure MCA-CN (63%) and original CN/WO3(87%). The results of photoluminescence and electrochemical impedance spectroscopy demonstrated that the Z-scheme heterojunction of MCA-CN/WO3inhibited the recombination of electrons and holes. In addition, the porous nanosheet structure accelerated the electron transfer and provided abundant active sites for MB degradation. A radical quenching experiment indicated that the Z-scheme heterojunction facilitated the decomposition of H2O2to produce1O2for MB degradation. The possible degradation pathways of MB were proposed.Keywords:photo-Fenton-like process;WO3-loaded porous carbon nitride nanosheet;Z-scheme heterojunction;MB degradation
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Journal of Cleaner Production
·
2022
·
IF 11.072
Huiping Zeng,Jianxue Li,Jiaxin Xu,Wei Qi,Ruixia Hao,Da Lin,Dong Li,Jie Zhang
In this study, a novel magnetic biochar (BC-Fe n ), synthesized by one-step pyrolysis at 800 °C using platanus leaves and iron-containing sludge in different mass ratios, was used to activate persulfate (PS) for tetracycline (TC) degradation. Results show that BC-Fe 1:2 exhibited excellent degradation performance (91.4%), much better than the raw biochar (BC) (77.1%). And electron paramagnetic resonance (EPR) techniques demonstrated radical ( S O 4 · − , ·OH, O 2 · − ) and non-radical ( 1 O 2 ) pathways in BC-Fe 1:2 /PS, S O 4 · − was further proved to be the main active species by quenching experiments. Liquid chromatography-mass spectrometry (LC-MS) was utilized to identify the intermediates of TC and three possible degradation pathways were proposed. Additionally, the BC-Fe 1:2 was weakly affected by pH and the coexisting anions in wastewater, and could still remove 80% of TC in the third cycle experiment. This study provides a new idea for converting backwash iron-containing sludge from groundwater treatment plants into valuable catalysts, and provides new insights into the key role of low-cost magnetic biochar in PS activation.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Xinzhi Wang,Zhenguo Chen,Yutian He,Xiaohui Yi,Chao Zhang,Qiao Zhou,Xuezhu Xiang,Yunan Gao,Mingzhi Huang
Imidacloprid (IMI) which has been widely detected in the natural water environment is potentially genotoxic to humans and should be effectively eliminated. Persulfate-based advanced oxidation processes are considered to be reliable means aiming at organic pollutants degradation, while an efficient catalyst is urgently needed for the activation of the reaction. As a two-dimensional material, 1T-MoS 2 is expected to be applied for the activation of persulfates due to its abundant active sites and good electrical conductivity. Therefore, in this study, 1T-MoS 2 was synthesized by a simple and safe two-step solvothermal reaction and proposed as an emerging activator of peroxymonosulfate (PMS) for the degradation of IMI. It was found that 1T-MoS 2 has significantly better catalytic performance on PMS than 2H-MoS 2 and Bulk-MoS 2 , reaching. 76.4 % at pH = 3. The degradation rate of IMI reduced under alkaline conditions due to the inhibition of catalytic processes. Among the different coexisting anions, H C O 3 - had the greatest degree of interference and inhibition to the degradation process, resulting in the lowest IMI degradation rate for only 42.45 %. Quenching experiments and EPR analysis showed that S O 4 - ∙ and OH were the main reactive oxygen species in the 1T-MoS 2 /PMS process. In addition, the IMI degradation pathways analyzed by UPLC-Q-TOF-MS/MS included dehydrogenation, electrophilic addition, heterocyclic ring breakage and intramolecular rearrangement. This study promotes the application of 1T-MoS 2 and is expected to provide a novel persulfate-based advanced oxidation process catalyzed by 1T-MoS 2 for IMI elimination in the aqueous environment.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Ting Chen,Zhiliang Zhu,Xiaolin Shen,Hua Zhang,Yanling Qiu,Daqiang Yin
The construction of single Fe atoms with favorable electron structures is highly desired to boost peroxymonosulfate (PMS) activation for organics degradation. Herein, this study embedded isolated Fe atoms on N, O co-doped porous carbon substrate (Fe SA -N/O C), and first found the constructed FeN 4 O 1 configuration can realize efficient PMS activation via electron transfer by inner-sphere complexation, instead of the usual reactive oxygen species (ROS) as a major role. Structural investigation showed that the FeN 4 O 1 moieties possess high content of high spin (HS) Fe(II), resulting in the delocalization of unpaired electrons around Fe centers, which is benefit to transfer electrons when reacted with PMS. EIS and LSV curves further certified the electron transfer process. Density functional theory (DFT) calculations unveiled that the FeN 4 O 1 configuration can directly adsorb O O bond of PMS, leading to electron accumulation around Fe-O 2 bond, and then ulteriorly trigger the electron shuttling in organics degradation. Consequently, the optimized Fe SA -N/O C/PMS system exhibited superior oxidation ability for various organic pollutants, and was not affected by initial pH variation (3.19 ∼ 10.89), inorganic anions (ClO 4 − , Cl − and H 2 PO 4 − ) and natural organic matter (NOM) interference. Importantly, the developed system presented certain applicability in the treatment of actual water from Taihu Lake basin, China. Hence, this study not only elucidates the inner-sphere complexation-oriented electron transfer mechanism between unique FeN 4 O 1 configuration and PMS, but provides new insights into engineered single atom catalysts for wastewater purification.
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Nanomaterials
·
2022
·Vol. 12
·期 15
·2586
·
IF 5.719
Diyong Tang,Li Lu,Zhipeng Luo,Baokun Yang,Jun Ke,Weidong Lei,Hongran Zhen,Yuan Zhuang,Jie Sun,Ke Chen,Jie Sun
Biochars are considered as promising materials in energy storage and environmental remediation because of their unique physicochemical properties and low cost. However, the fabrication of multifunctional biochar materials with a well-developed hierarchical porous structure as well as self-doped functionalities via a facile strategy remains a challenge. Herein, we demonstrate a heteroatom-doped porous biochar, prepared by a hydrothermal pretreatment followed by a molten salt activation route. With the creation of a high specific surface area (1501.9 m2/g), a hierarchical porous structure, and the incorporation of oxygen-/nitrogen-functional groups, the as-prepared biochar (BC-24) exhibits great potential for supercapacitor application and organic pollutant elimination. The assembled biochar electrode delivers a specific capacitance of 378 F/g at 0.2 A/g with a good rate capability of 198 F/g at 10 A/g, and excellent cycling stability with 94.5% capacitance retention after 10,000 recycles. Moreover, BC-24 also exhibits superior catalytic activity for phenol degradation through peroxydisulfate (PDS) activation. The phenol (0.2 mM) can be effectively absorbed and then completely degraded within only 25 min over a wide pH range with low catalyst and PDS dosages. More importantly, TOC analysis indicates 81.7% of the phenol is mineralized within 60 min, confirming the effectiveness of the BC-24/PDS system. Quenching experiments and EPR measurements reveal that SO4·−and ·OH as well as1O2are involved in the phenol degradation, while the non-radical pathway plays the dominant role. This study provides valuable insights into the preparation of cost-effective carbon materials for supercapacitor application and organic contaminant remediation.Keywords:biochar;supercapacitor;organic pollutant;peroxydisulfate;free radicals;non-radical pathway
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高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Huanxuan Li,Yucheng Lou,Junting Zheng,Liya Su,Shun Lu,Chen Xu,Jingang Huang,Qingwei Zhou,Junhong Tang,Mingzhi Huang
The importance of new water purification technology for maintaining clean water resources and a high quality of life is self-evident. In this study, amino functionalized bimetallic metal-organic frameworks (NH 2 -MIL-101(FeCo)) were prepared to activate peroxymonosulfate (PMS) for removal of organic pollutants from water. The structure, morphology, and physicochemical properties of as-prepared NH 2 -MIL-101(FeCo) were comprehensively evaluated by X-ray diffraction, scanning electron microscopy, N 2 adsorption-desorption isotherms, and X-ray photoelectric spectroscopy. Degradation tests were performed to study effects of PMS concentration, catalyst dosage, initial pH, and common substances on the orange G (OG) removal. The acidic and alkaline conditions promoted the formation of mesoporous structures in NH 2 -MIL-101(FeCo) and enhanced the mass transfer processes to remove OG. 100% of OG was removed through a rate constant of 0.0711 min -1 within 45 min in NH 2 -MIL-101(FeCo)− 2/PMS/OG system, where 1 O 2 , SO 4 •− , and · OH played pivotal contributions in the OG removal. The catalytic activity of NH 2 -MIL-101(FeCo) originated from unsaturated metal sites of Fe(II) and Co(II). This work demonstrates a feasible strategy towards the synthesis of functional MOFs for removal of organic contaminants .
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