ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 57
·120590-120604
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IF 5.8
Lu Wen,Ren Songyu,Zhang Yanyu,Wen Ximeng,Zhang Zhongguo,Wang Aimin
A comparative study on the mineralization of antibiotic trimethoprim (TMP) in neutral medium was investigated by applying irradiation with five types of ultraviolet lamps. Among these lamps, the whole envelope of one lamp contained ordinary quartz, which could only transmit ultraviolet-C (UVC) light. For the other four lamps, approximately one tenth, a quarter, a half, and full of envelopes were comprised of high-purity synthetic quartz, which can transmit both vacuum ultraviolet (VUV) and UVC light. TMP decay was well fitted to pseudo-first-order reaction kinetics and occurred more quickly as the VUV intensity increased. Poor mineralization was achieved in the absence of VUV light, whereas the mineralization efficiency was also enhanced with increasing VUV intensity. The presence of hydroxyl radicals ( • OH), superoxide radicals (O 2 •− ) and singlet oxygen ( 1 O 2 ) during VUV photolysis of water was confirmed by electron paramagnetic resonance (EPR) analysis. Appropriate radical quenching experiments and fluorescent molecular probe detection provided the evidence that • OH played a significant role in TMP mineralization. Higher VUV intensity favored the generation of H 2 O 2 and • OH. The evolution of NH 4 + and NO 3 − as well as carboxylic acids (formic, acetic, oxalic, and oxamic acids) released in the treated solution were quantified. Ten aromatic intermediates were also identified by UPLC-QTOF-MS. Thereby, a plausible reaction sequence for TMP mineralization in VUV/UVC photolysis was finally proposed. Graphical Abstract
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 57
·120030-120043
·
IF 5.8
Zhou Chuchen,Wan Lei,Lou Zimo,Wu Shuang,Baig Shams Ali,Xu Xinhua
Elevated Sb(V) concentration in textile wastewater is a growing environmental concern worldwide and has received wider attention in recent years. Iron oxides possess appealing characteristics as efficient and cost-effective adsorbents in large-scale applications. In the present study, Sb(V) adsorption capacity of α-Fe 2 O 3 , γ-Fe 2 O 3 , and Fe 3 O 4 was compared under experimental conditions close to the practical textile wastewater treatment. Results demonstrated that α-Fe 2 O 3 performed better under different pH values, reaction times, dye compounds, and co-existing ions as compared to γ-Fe 2 O 3 and Fe 3 O 4 , and the adsorption equilibrium was achieved within 8 h. Sb(V) adsorption is found to be highly pH dependent, and higher removal was achieved in lower pH, indicating the involvement of electrostatic interactions. The pH pzc value of α-Fe 2 O 3 was 7.15, which favored Sb(V) adsorption in practical wastewater having neutral pH value (pH ~ 7). Pseudo-first- and pseudo-second-order described the data and the simulated values of q e fitted well with the experimental values, indicating that pseudo-second-order model described the adsorption kinetics better with R 2 (> 0.95) higher than of pseudo-first-order plots. The Langmuir and Freundlich models both described well the sorption data of all the adsorbents, where the R 2 values were > 0.90 with a better fit in the Freundlich model for α-Fe 2 O 3 , suggesting that the adsorbent has heterogeneous surface characteristics. Similarly, characterizations revealed that the specific surface area, pore volume, and hydroxyl group content in α-Fe 2 O 3 were higher than others, making it easier for contaminants to bind on to the active sites. Furthermore, the effect of dyes and co-existing anions on Sb(V) adsorption was negligible, except for SO 4 2− , CO 3 2− , and PO 4 3− by the formation of inner-sphere complexes with iron oxides through competitive adsorption with [Sb(OH) 6 ] − . Findings from the present study suggested that α-Fe 2 O 3 effectively reduced Sb(V) in textile wastewater and could be a promising alternative for practical textile wastewater treatment. Graphical Abstract
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Li Yuanfeng,Qin Tian,Wei Yuechang,Xiong Jing,Zhang Peng,Lai Kezhen,Chi Hongjie,Liu Xi,Chen Liwei,Yu Xiaolin,Zhao Zhen,Li Lina,Liu Jian
The quest for efficient non-Pt/Pd catalysts has proved to be a formidable challenge for auto-exhaust purification. Herein, we present an approach to construct a robust catalyst by embedding single-atom Ru sites onto the surface of CeO 2 through a gas bubbling-assisted membrane deposition method. The formed single-atom Ru sites, which occupy surface lattice sites of CeO 2 , can improve activation efficiency for NO and O 2 . Remarkably, the Ru 1 /CeO 2 catalyst exhibits exceptional catalytic performance and stability during auto-exhaust carbon particle oxidation (soot), rivaling commercial Pt-based catalysts. The turnover frequency (0.218 h −1 ) is a nine-fold increase relative to the Ru nanoparticle catalyst. We further show that the strong interfacial charge transfer within the atomically dispersed Ru active site greatly enhances the rate-determining step of NO oxidation, resulting in a substantial reduction of the apparent activation energy during soot oxidation. The single-atom Ru catalyst represents a step toward reducing dependence on Pt/Pd-based catalysts.
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Journal of Inorganic and Organometallic Polymers and Materials
·
2023
·
IF 4
Lu Danli,He Zhiping,Liu Weiliang
In this work, a novel NiCo/ZIF-67/rGO catalyst was prepared via a facile impregnation-reduction method, followed by comprehensive characterization using XRD, SEM, TEM, XPS, and ICP-OES techniques. This catalyst featured a hierarchical porous support consisting of Zeolitic Imidazolate Framework-67 (ZIF-67) with a high specific surface area and reduced graphene oxide (rGO) with considerable electronic conductivity, along with strong synergistic interactions between Ni and Co species as well as between the deposited metals and the carbon in rGO. The NiCo/ZIF-67/rGO catalyst exhibited excellent activity in catalyzing the hydrolysis of NaBH 4 , resulting in a low activation energy ( E a ) of 21.08 kJ mol −1 and a high turnover frequency (TOF) value of 5420 \(mL_{{\textit{H}}_\text{2}}g_\textit{M}^{-1}\min^{-1}\) . The hydrogen generation rate was increased by nearly double after five cyclic experiments, demonstrating the exceptional catalytic durability of NiCo/ZIF-67/rGO. The as-prepared NiCo/ZIF-67/rGO catalyst exhibits the advantages of cost-effectiveness, durability, and superior performance for NaBH 4 hydrolysis, rendering it a promising candidate for industrial applications.
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Science China-Materials
·
2023
·Vol. 66
·期 12
·4782-4793
·
IF 8.1
Wu Feng,Lin Xiaoying,Xu Yuqian,Zhang Di,He Yunqing,Liu Mingxian
Soft actuators and micro-robots receive significant attention for their potential applications in transportation, photovoltaic conversion devices, clinical care, and other fields. In this work, a polyvinyl alcohol/Chinese ink mixture was uniformly coated on polyethylene film for preparing structure-stabilized bilayer soft actuators. Due to the significant difference in thermal expansion coefficients between the two layers, the actuator can achieve a large bending deformation with a fast response speed under xenon light. A large amplitude of bending angle of 1260° was achieved in 6 s. A soft-body robot similar to an inchworm was constructed by changing the intensity of xenon or near-infrared light combined with the bionic structure design of an inchworm. The robot can realize various forms of movements (such as crawling and pushing boxes) on different surfaces (such as paper and leaves). Light-driven applications such as hands capable of grasping objects (grasping objects 14 times their weight), cats exhibiting variable expressions, elephant trunks performing curling and retraction, and bionic flowers realizing flowering and closing can be realized. In addition, based on the good photothermal conversion and pressure sensing performance of the bilayer actuator, it is able to monitor daily human activities (such as joint flexion, abdominal breathing, water swallowing, and other movements) and integrate with photoelectric conversion devices. This versatile and diverse drive-mode soft robot exhibits significant potential for applications such as wearable devices, transportation, photovoltaic conversion devices, and clinical therapies.
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Nano Research
·
2023
·
IF 9.9
Cao Chi,Li Jinshuo,Hu Yang,Zhang Lin,Yang Wensheng
Three kinds of metal atoms with different valence electronic configurations, Bi (6s 2 6p 3 ), Y (4d 1 5s 2 ), and Ce (4f 1 5d 1 6s 2 ), were selected to investigate the effect of A-site (La 3 +) doping on electronic band structure, photoelectric properties, and photocatalytic performance of LaFeO 3 perovskite. It was identified that the Bi doped LaFeO 3 presented significantly improved photocatalytic activity towards the reduction of CO 2 , while the Y or Ce doped LaFeO 3 displayed decreased photocatalytic activity compared to the pristine LaFeO 3 . It was revealed that doping of all the three metal atoms resulted in narrowed band gap and thus extended light absorption of LaFeO 3 by lowering its conduction band minimum (CBM). The recombination rate and mobility of the charge carriers were represented by the relative effective mass (D) between holes and electrons for pristine and A-site doped LaFeO 3 . The doping of Bi resulted in increased D value, attributed to the Bi 6s electron states at the valence band maximum (VBM), and thus promoted separation and transfer of the charge carriers and improved photocatalytic activity of LaFeO 3 . In contrast, the doping of Ce resulted in significantly decreased D value, induced by the highly localized Ce 4f hole states at the CBM, and thus higher recombination rate of the charge carriers and decreased photocatalytic activity of LaFeO 3 . Furthermore, the Y doped LaFeO 3 with a slightly decreased D value presented slightly increased recombination rate of the charge carriers and thus decreased photocatalytic activity. Such a work provides new insights into the A-site doping in LaFeO 3 perovskite, which should be helpful for optimizing the electronic band structure and activity of perovskite-type photocatalysts at atomic level.
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Reaction Kinetics Mechanisms and Catalysis
·
2023
·
IF 1.8
Luo Peng,Chen Junteng,Mu Manman
Herein, a series of cobalt nanoparticles embedded in nitrogen-doped porous carbon catalyst (Co@NPC) was prepared through the pyrolysis of tetragonal Co-based metal–organic framework which consisted of Co centers and benzimdazole linkers. Due to large BET specific surface area (389.41 m 2 /g), abundant metallic Co content (39.3%), small Co nanoparticle size and high pyridinic-N content, the as-obtained Co@NPC-700 catalyst exhibited superior catalytic performance for the hydrogenation and one-pot reductive acetylation of nitrobenzene. The high 99.80% conversion of nitrobenzene and 99.56% yield of aniline were acquired in the catalytic hydrogenation of nitrobenzene with hydrazine hydrate at 80 °C for 2 h. Simultaneously, the above catalyst showed high conversion (87.2%) and selectivity (95.3%) for the one-pot reductive acetylation of nitrobenzene in the presence of phenyl silane at room temperature. Additionally, Co@NPC-700 exhibited excellent activities for the catalytic hydrogenation and one-pot reductive acetylation of other nitroarenes as well as good recyclability. This work offered a facile approach to prepare metallic Co loaded on porous carbons, serving as efficient catalysts for catalytic reductive applications.
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Nano-Micro Letters
·
2023
·Vol. 16
·期 1
·1-17
·
IF 26.6
Li Xin,Hu Ruizhe,Xiong Zhiqiang,Wang Dan,Zhang Zhixia,Liu Chongbo,Zeng Xiaojun,Chen Dezhi,Che Renchao,Nie Xuliang
Fe 3+ , Co 2+ , H 3 BTC, and collagen peptide are used to achieve a one-step assembly of stable FeCo-MOG/CP by manipulating the complexation effect and solution polarity.
By optimizing pyrolysis, two kinds of nitrogen-doped carbon aerogels loaded with virus-shaped and nanospherical magnetic particles are obtained.
FeCo/Fe 3 O 4 /NC and FeCo/NC aerogels exhibit excellent electromagnetic wave absorbing and radar stealth performances.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Tana Tana,Han Pengfei,Brock Aidan J.,Mao Xin,Sarina Sarina,Waclawik Eric R.,Du Aijun,Bottle Steven E.,Zhu Huai-Yong
5-hydroxymethylfurfural (HMF) is a valuable and essential platform chemical for establishing a sustainable, eco-friendly fine-chemical and pharmaceutical industry based on biomass. The cost-effective production of HMF from abundant C6 sugars requires mild reaction temperatures and efficient catalysts from naturally abundant materials. Herein, we report how fulvic acid forms complexes with Al 3+ ions that exhibit solar absorption and photocatalytic activity for glucose conversion to HMF in one-pot reaction, in good yield (~60%) and at moderate temperatures (80 °C). When using representative components of fulvic acid, catechol and pyrogallol as ligands, 70 and 67% HMF yields are achieved, respectively, at 70 °C. Al 3+ ions are not recognised as effective photocatalysts; however, complexing them with fulvic acid components as light antennas can create new functionality. This mechanism offers prospects for new green photocatalytic systems to synthesise a range of substances that have not previously been considered.
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BRAZILIAN JOURNAL OF CHEMICAL ENGINEERING
·
2023
·
IF 1.2
Yang Zelong,Yao Pengfei,Qin Haijian,Xia Qing,Yuan Bo,Zheng Chunzhi,Yang Fengli
CO oxidation has attracted much attention in the field of automotive exhaust treatment and fuel cell industrial process. In this study, NiO loaded on the Ta 2 O 5 was prepared and used to catalyze CO oxidation. And the catalyst NiO/Ta 2 O 5 was characterized by Scanning Electron Microscope (SEM), Transmission Electron Microscope (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS). The catalytic performance was evaluated and the mechanism was analyzed. The catalytic performance has been enhanced greatly by combining NiO with Ta 2 O 5 , the catalyst shows excellent activity in a wide CO concentration from 500 to 10,000 ppm, with CO conversion above 90%. In addition, NiO/Ta 2 O 5 has good stability for CO oxidation with no apparent loss of activity for 8 h. The XPS results show that oxygen defects emerged after reaction. The presence of oxygen defects is responsible for the high catalytic activity. Graphical abstract
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JOURNAL OF MATERIALS SCIENCE
·
2023
·Vol. 58
·期 46
·17470-17482
·
IF 4.5
Li Zi-Xia,Xiang Yong-Sheng,Ran Yin
Realizing nano-filler well dispersed in epoxy matrix is essential for the fabrication of high-performance epoxy composites. However, the aggregation of untreated nano-filler in epoxy resin during static curing greatly reduces the material performance. Herein, we report an effective and facile approach to fabricate well-dispersed silica nanoparticle (SiNP)-reinforced epoxy composites through dynamic crosslinking depending on vitrimer chemistry. The epoxy vitrimer synthesized by dynamic crosslinking method was named as EVD, and the epoxy vitrimer synthesized by static curing method was named as EVS. EVD/SiO 2 nanocomposites were prepared by dynamic crosslinking technology with unmodified nano-SiO 2 as a reinforcement filler, sebacic acid as a curing agent, diglycidyl ether of bisphenol A (DGEBA) as an epoxy monomer, zinc acetylacetonate as a transesterification catalyst, and a torque rheometer (internal mixer) as a dynamic crosslinking equipment, and EVS/SiO 2 nanocomposites were prepared by traditional static curing method as counterparts. The structure, properties, and stress relaxation of the EVD/SiO 2 and EVS/SiO 2 were comparatively investigated in detail. When the loading amount of SiO 2 was 5 wt%, EVD/SiO 2 -5 indicated 2.38 times tensile strength and 2.06 times elongation at break of EVS/SiO 2 -5. The Young's modulus of EVD/SiO 2 -5 (6.76 ± 1.07 MPa) was slightly higher than that of EVS/SiO 2 -5 (5.81 ± 1.06 MPa), which was attributed to more well-dispersed SiNP in EVD/SiO 2 -5. Moreover, the amount of SiO 2 can be filled up to 40 wt% in epoxy vitrimer to obtain high-modulus (1001 times of pure vitrimer) composite. We believe that this study provides a new idea for the preparation of other vitrimer composites with desired properties. Graphical abstract
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CELLULOSE
·
2023
·Vol. 30
·期 18
·11737-11751
·
IF 5.7
Song Baiqing,Zhang Tianyi,Li Xinfeng,Yang Kaili,Tian Guangming,Dang Yunzhi,Ma Jianhua
Intelligent, controlled, slow-release antimicrobial materials have shown excellent application prospects in the medical field. Herein, silver particles (Ag) were synthesized using the hydrothermal method and a bacterial cellulose (BC) membrane as a template. The BC/Ag composite membrane was clad with copper alginate (CAlg) via the in-situ dip-coating method. Based on the Cu 2+ ions in copper alginate, a layer of copper sulfide (CuS) was formed through a liquid-phase sulphuration reaction. This CuS layer leads the film to possess a photothermal and electrothermal response. Furthermore, we systematically investigated the microstructure, mechanical strength, and antibacterial properties of the composite film. The tensile strength of the BC/Ag/CAlg/CuS sample can reach 14.7 MPa, which should be attributed to the combination of the Cu 2+ cross-linked CAlg and the inner BC/Ag composite film. Meanwhile, this assembled film exhibited hydrophilic and hygroscopic properties, as the antibacterial Ag particles can be continuously released and migrated from the inner layer to the outer layer. Finally, the BC/Ag/CAlg/CuS film inhibited Staphylococcus aureus and Escherichia coli by 99.9% and 99.6%, respectively, which should be attributed to the synergistic effect of silver ions and CuS’s electrical and photothermal stimulation responses. These characteristics of the thermally responsive BC/Ag composite films indicate that they may successfully serve as wound dressings and other medical biomaterials.
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