SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
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IF 4.831
Qing Li,Yu-Meng Guo,Yue Gao,Guangli Li
Sensitive and selective detection of 2,4,6-trinitrotoluene (TNT) is critical for environmental protection and public health. In this work, a convenient synthesis strategy for preparation of fluorescent PEI-AgNCs was described and further a facile and label-free sensing strategy for detection of TNT was developed. The hyperbranched polyethyleneimine (PEI) were used as template to one-step synthesize functional PEI-AgNCs with bright fluorescence signal and rich amino groups on their surface. PEI can specifically bind to electron-deficient TNT through donor-receptor interaction to form Meissenheimer complex. Interestingly, the absorption spectra of the Meissenheimer complex overlap with the fluorescence emission peak of PEI-AgNCs, thus quenching fluorescence of PEI-Ag NCs through fluorescence resonance energy transfer (FRET). Furthermore, this bonding process also initiate aggregation of PEI-AgNCs and quench the fluorescence of PEI-AgNCs by the aggregation-induced quenching (AIQ) effect. The novel method demonstrates sensitivity with a detection limit for TNT have been obtained as 17 nM. In addition, the proposed sensing method also has good selectivity over other potential interference and displayed a good potential application value in real water samples with satisfactory recoveries, offering a promising platform for sensing TNT in public safety and security environment protection.
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Environmental Science-Water Research & Technology
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2022
·Vol. 8
·期 6
·1252-1260
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IF 5.819
Wei Zhang,Nan Li,Caiwen Wang,Guangchao Li,Julong Sun,Shumin Zhu
Diuron, a persistent organic herbicide, was effectively degraded by the solar/chlorine process in this study. The solar/chlorine process could not only produce HO˙ (hydroxyl radicals) and reactive chlorine species (RCS), but also O3. They are the major contributors to diuron degradation at different solution pH values (6–8). Natural organic matter (NOM), NO2− and a high dosage of Cl−, NO3−, and HCO3− could inhibit the efficiency of diuron degradation. Moreover, a possible degradation pathway of diuron was proposed, which gives detailed reactions in the solar/chlorine process. The co-existence of NO2− in diuron degradation has risks of producing N-nitrosodimethylamine (NDMA). Finally, the ecotoxicity of diuron and its oxidation byproducts was reduced overall according to the calculated results from the Ecological Structure Activity Relationships (ECOSAR) program. But the toxicity of the products is still very high. For that, the solar/chlorine process should be of concern when it is used for diuron degradation.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yuanxi Huang,Lingjun Bu,Yangtao Wu,Shumin Zhu,Shiqing Zhou,Zhou Shi,Dionysios D. Dionysiou
UV/sodium percarbonate (UV/SPC) advanced oxidation process is an efficient and green technology to remove contaminants of emerging concern (CECs), with the simultaneous formation of hydroxyl radical ( • OH) and carbonate radical (CO 3 •− ). This study investigated the degradation of eight CECs in UV/SPC process, including phenol, atrazine, bisphenol A, ibuprofen, sulfadiazine, acetaminophen, carbamazepine, and diuron. A model was established to simulate the experimental results, which shows that both • OH and CO 3 •− played crucial roles in UV/SPC process, and the steady-state concentrations of CO 3 •− were much higher than that of • OH. The higher concentration compensates for the low reactivity of CO 3 •− with CECs and the loss of • OH depleting by CO 3 •− . Also, the Hammett constants decreased linearly with increasing natural logarithms of rate constants, indicating the selectivity of CO 3 •− with electron-donating substituents. In real water, CEC degradation was significantly inhibited due to the competition for light absorption from background compounds and scavenging of free radicals, especially CO 3 •− , by water matrix. Further, demethylation, decarbonylation, hydroxylation, amino oxidation, and quinonization were proposed as the main reactions for CEC degradation in UV/SPC process. The minimum electrical energy per order (EE/O) was calculated as 0.152 kWh m −3 , with SPC dose of 0.138 mM and UV intensity of 2.02 × 10 -7 Einstein L −1 s −1 .
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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Jun Wang,Ying Zhao,Chunting Li,Zijun Yu,Yang Zhang,Yuan Li,Xiaoyao Tan,Shaomin Liu,Shaobin Wang,Xiaoguang Duan
Hierarchically porous iron/nitrogen-doped carbons (Fe-N-PC) were developed for the oxidation of ibuprofen (IBP) with peroxymonosulfate (PMS). The incorporation of trace-level iron and nitrogen dopants promoted the catalytic performance remarkably, leading to 4.8, 16.4 and 22.9-fold enhancement over N-doped carbon (N-PC), porous carbon (PC), and Fe-doped carbon (Fe-PC), respectively. Fe(III) was anchored in nitrogen-coordinated pots (Fe-N x ) in the sp 2 -hybridized carbon network, and graphitic-N could synergistically boost the catalysis. Notably, methyl phenyl sulfoxide (PMSO) transformation, quenching tests, in situ electrochemical analysis and Raman spectroscopy verified high-valent iron-oxo species and direct electron transfer pathway accounted for pollutant oxidation. The relationship between the kinetic constants (ln k obs ) and the oxidation peak potential ( E op ) of pollutants was established with good correlation, manifesting particular selectivity toward oxidizing electron-rich pollutants and great immunity to background inorganic ions and natural organic matters (NOMs) for real wastewater treatment . The deactivation mechanisms of Fe-N-PC were revealed via surface oxidation and dopant refabrication. This work delicates to deepen the understanding of the nonradical mechanisms and structure-oriented PMS activation by engineered carbonaceous materials .
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WATER RESEARCH
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2022
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IF 13.4
Fuwei Sun,Tianhu Chen,Ziyang Chu,Peixun Zhai,Haibo Liu,Qiang Wang,Xuehua Zou,Dong Chen
A system of Cu 2+ /calcite/PDS was constructed to degrade sulfadiazine (SDZ). Different from the traditional Cu-mediated activation, a low concentration of Cu 2+ that met drinking water standards (≤ 1 mg/L) transformed into Cu(Ⅱ) solid in the presence of calcite, and then enhanced the degradation of SDZ via PDS activation over a pH range from 3 to 9. According to scavenger and chemical probe experiments, Cu(Ⅲ), rather than radicals (hydroxyl radicals and sulfate radicals) and singlet oxygen, was the predominant reactive species, which was responsible for the degradation of SDZ. Based on the results of XRD, ATR-FTIR, and CV curves et al., CuCO 3 was the main complex with high reactivity for PDS activation to form Cu(Ⅲ). Moreover, detailed degradation pathways of sulfadiazine were proposed according to the UPLC-ESI-MS/MS and their toxicity was predicted by ECOSAR. Besides, the real water matrix would not seriously affect the degradation of SDZ in the Cu 2+ /calcite/PDS system. In summary, this study reveals a new insight into the synergistic effect of Cu 2+ and calcite on the SDZ degradation, and promotes an understanding of the environmental benefits of natural calcite.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Rongsheng Ning,Zhongsen Yan,Zhenyu Lu,Qiankun Wang,Zengling Wu,Wenxin Dai,Gongduan Fan,Xianzhi Fu
Membrane distillation (MD) is emerging as a promising technology for wastewater reclamation to relieve the shortage of freshwater. However, due to the contamination of semi-volatile organic compounds (s-VOCs), part of s-VOCs would transfer the membrane and impact the permeate quality during the MD process. Herein, an innovative AgCl/MIL-100(Fe)/PTFE photocatalytic membrane (AM/PTFE) was rationally synthesized in view of the increasing s-VOCs rejection. The AM/PTFE membrane was applied in the photocatalytic direct contact membrane distillation (DCMD) system and nitrobenzene (NB) was selected as the model contamination for evaluating removal performance of s-VOCs under visible light. Compared with the MD process, NB removal rate increased from 63.44% to 87.84% in the photocatalytic MD system. Moreover, stable performance was maintained over five NB removal cycles experiment with s-VOCs rejection higher than 84.84% in the end. The enhanced rejection of s-VOCs could be attributed to the combination of adsorption and photocatalytic. The volatile NB molecules were adsorbed on the surface of photocatalytic membranes, and the photo-electrons (e - ) generated by immobilized nanomaterials could effectively remove pollutants under visible light irradiation. This photocatalytic MD system provides an attractive avenue for the water reclamation from s-VOCs contaminated wastewater in the practical applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Zhijun Li,Mingyang Zhang,Xiuli Dong,Siqi Ji,Lili Zhang,Leipeng Leng,Honghong Li,J. Hugh Horton,Qian Xu,Junfa Zhu
The realization of efficient and fully controllable synthesis of single atom catalysts is an exciting frontier, yet still challenging in the modern catalysis field. Here we describe a straightforward high-temperature quenching approach to precisely construct isolated palladium atoms supported over cubic indium oxide, with individual palladium atoms coordinated with four neighboring oxygen atoms. This palladium catalyst achieves exceptional catalytic efficiency in the selective hydrogenation of nitrobenzene to aniline, with more than 99% chemoselectivity under almost 100% conversion. Moreover, it delivers excellent recyclability, anti-CO poisoning ability, storage stability, and substrate tolerance. DFT calculations further reveal that the high catalytic activity stems from the optimized electronic structure and the charge states of palladium atoms in the defect-containing indium oxide. Our findings provide an effective approach to engineering single atom catalysts at the atomic level and open the door to a wide variety of catalytic reactions .
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Yifan Feng,Xu Huang,Huifang Wu,Dawei Li,Yi Sun
Nanomaterials coated ceramic membranes have become one of the most promising methods to degrade organic pollution. In this study, low crystalline metal nanomaterials were coated on ceramic membranes for the first time. This research fabricated a ceramic membrane with low crystalline Fe 2 O 3 @carboxylic multi-walled carbon nanotubes (CMWCNTs) and evaluated its aromatic compounds-degrading ability and self-cleaning ability. The coated membrane demonstrated an excellent removal rate (＞90%) of phenol and atrazine in 120 min’s continuous flow filtration via surface photo-Fenton reaction. Quenching experiments reveal the active substances of the reaction system were singlet oxygen ( 1 O 2 ) and a small amount of hydroxyl radical (·OH). With humic acid (HA) and bovine serum albumin (BSA) as model pollutants, the polluted membranes recovered 84.4% and 77.0% flux through the photo-Fenton reaction respectively, which proved the self-cleaning performance of the coated membrane. After 6 cycles, an average degradation efficiency of 92% for phenol was maintained in continuous flow filtration. These results indicated the efficacy of the photo-Fenton coupling coated membrane for treating organically polluted water and its relevance for the design and application of future photo-Fenton membrane filtration system.
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JOURNAL OF MATERIALS SCIENCE
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2022
·Vol. 57
·期 6
·4265-4282
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IF 4.682
Hu Wenna,Wu Fan,Liu Wei
The objective of this study was to construct the S-scheme Bi 2 WO 6 / α- Bi 2 O 3 heterojunctions with high enhanced visible-light photocatalytic performance. The composites loaded various Bi 2 WO 6 mass ratios were prepared by a ball grinding method. The characterization and reaction mechanism of photocatalysts were explored in detail. Remarkably, the results demonstrated that the Bi 2 WO 6 / α- Bi 2 O 3 presented an outstandingly superior performance for photodegradation of nitrobenzene. Among them, the 10%Bi 2 WO 6 / α- Bi 2 O 3 possessed the best photocatalytic property, and it could reach up to 95.7% in 50 min with the top rate constant of 0.06178 min −1 , which was 4.3 and 3.6 times that of bare Bi 2 O 3 and Bi 2 WO 6 , respectively. Simultaneously, the Bi 2 WO 6 / α- Bi 2 O 3 was well stable after five cycling experiments. The efficiently improved photocatalytic performance was primarily attributed to the formation of S-scheme structure between Bi 2 WO 6 and α- Bi 2 O 3 , which enhanced the conspicuous separating efficiency of photogenerated carriers. The present study not only offers a method to solve the unsatisfactory activity of Bi 2 O 3 , but also provides some insights into the design of other novel S-scheme composites with great potential application in clean energy and environmental remediation. Graphical abstract The efficiently improved photocatalytic performance was primarily attributed to the formation of S-scheme structure between Bi 2 WO 6 and α- Bi 2 O 3 , which enhanced the conspicuous separating efficiency of photogenerated carriers.
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ACS Applied Materials & Interfaces
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2022
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IF 10.383
Ruidong Li,Lu Wu,Ganggang Chang,Shanchao Ke,Yilong Wang,Yao Yao,Yuexing Zhang,Junsheng Li,Xiaoyu Yang,Banglin Chen
Carbon materials with hierarchical morphologies, pores, and compositions have attracted extraordinary attention due to their unique structural advantages and widespread applications. However, their controllable synthesis remains a grand challenge. Herein, a solvent-mediated strategy was demonstrated for the preparation of an urchin-like superstructure via modulating the hydrothermal condition (acetic acid/water ratio) of metal–organic frameworks (MOFs). The direct pyrolysis of a hierarchical NUS-6 precursor produced a well-defined carbon-based composite consisting of sulfur-doped carbon (SC) and HfO2 with an urchin-like morphology and micro-/mesoporosity, while the doped S sites and oxygen vacancies of HfO2 can help to anchor and activate Pd nanoparticles (NPs) through the strong host–guest interaction, which was further confirmed by the calculated results of the binding energy and differential charge density through density functional theory (DFT). The synthesized Pd@SC/HfO2 composite exhibited extremely high catalytic activity and stability toward the water-phase hydrodeoxygenation of vanillin (conversion >99%, selectivity >99%), as well as good universality for the hydrogenation of a series of unsaturated hydrocarbons in an aqueous system. Remarkably, the catalytic activity and structural stability of Pd@SC/HfO2 were largely maintained even after successive 10 cycles.
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CATALYSIS LETTERS
·
2022
·Vol. 152
·期 12
·3725-3732
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IF 2.936
Guo Pan,Zhan Yuzhong,Yang Yanliang,Lu Tianliang
The preparation of high-performance supported Pd catalysts for the hydrogenation of aromatic nitro is of great importance. In this paper, covalent-triazine framework (CTF), an organic porous crystalline material connected by covalent bonds, was employed as the support for the preparation of Pd heterogeneous catalyst. The framework of CTF was maintained due to the utilization of cyclohexene as a moderate reductant for PdCl 2 . The catalysts were characterized by transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. The influence of reaction conditions (temperature, pressure, reaction time, concentration substrate and catalyst dosage) were investigated. At very mild reaction conditions (30 °C, 0.1 MPa H 2 , 2 mg Pd/CTF), the nitrobenzene was nearly stoichiometric hydrogenated to aniline. The Pd/CTF was effective for the conversion of a series of aromatic nitro compounds to the corresponding aromatic amines with good yield. The results showed that Pd/CTF has good catalytic activity and stability in the heterogeneous catalytic hydrogenation. Graphical Abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Lixia Li,Qinkai Guo,Baohe Lv,Minxue Zheng,Wang Zhan,Yanhong Liu,Wanzhen Xu,Ruiwei Wang,Hongbo Zeng,Baodong Mao
The mixed-valent magnetite (Fe 3 O 4 ) played a critical role in H 2 O 2 -based Fenton-like system for the removal of chlorophenols, but high activity and cycle stability of the Fe 3 O 4 -based catalysts are still a huge challenge. Herein, a series of surface hydroxyl- and carboxyl-modified Ag 0 /Fe 3 O 4 nanocomposite catalysts were prepared and used to activate H 2 O 2 for degradation chlorophenols pollutants. Under the optimized condition, nearly 100% degradation ratio were achieved within 2–30 min for 2,4-dichlorophenol, 2,3-dichlorophenol, 3,4-dichlorophenol, 2,4,6-trichlorophenol, p-nitrophenol, and 98% degradation ratio for 2,5-dichlorophenol, 2,6-dichlorophenol and 3,5-dichlorophenol,. Moreover, wide pH applicability was obtained for the Ag 0 /Fe 3 O 4 -H 2 O 2 system, where 95% degradation ratio of 2,4-dichlorophenol was still obtained at pH 6.0. The excellent activity of Ag 0 /Fe 3 O 4 catalyst can be ascribed to the incorporation of Ag 0 nanoparticles that accelerated the Fe(III)/Fe(II) transformation with the assistance of surface hydroxyl and carboxyl groups. Detailed mechanism study indicated a pseudo-second-order kinetic model, where the oxidative degradation and reductive degradation pathways coexisted in the system. The surface-modified Ag 0 /Fe 3 O 4 -H 2 O 2 provide a practical catalyst system for the removal of phenol contaminants with high reaction rate, wide pH adaptability, and validity for a series of chlorophenols.
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