RSC Advances
·
2023
·Vol. 13
·期 42
·29695-29705
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IF 3.9
Hui Fui,Shumin Gao,Xinran Ma,Yiping Huang
Layered double hydroxides (LDHs) have been extensively investigated as promising peroxymonosulfate (PMS) activators for the degradation of organic pollutants. However, bulk LDHs synthesized using conventional methods possess a closely stacked layered structure, which seriously blocks active sites and yields low intrinsic activity. In this study, we exfoliated bulk CoAl-LDHs to fabricate CoAl-LDH nanosheets by alkali-etching and Ostwald ripening via a simple hydrothermal process in a KOH solution. The exfoliated LDHs possessed the typical nanosheet structure with more exposed active sites for PMS activation, and hence, boosted the degradation of the pollutants. CoAl-1 exhibited an outstanding catalytic performance as the PMS activator for rhodamine B (RhB) degradation with the apparent rate constant of 0.1687 min−1, which was about 3.63 and 5.02 times higher than that of commercial nano-Co3O4 and bulk CoAl-LDH, respectively. The maximum RhB degradation of 93.1% was achieved at the optimal reaction conditions: catalyst dose 0.1 g L−1, PMS concentration 0.3 mM, pH 7, and temperature 298 K. Further analysis of RhB degradation mechanism illustrated that singlet oxygen (1O2) dominated RhB degradation in the CoAl-1/PMS system, while ˙OH, ˙O2−, and ˙SO4− may mainly serve as the intermediates for the generation of 1O2 and were indirectly involved in the degradation. This study provides a promising strategy for developing two-dimensional LDH nanosheets for wastewater remediation.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Mei-Mei Wang,Yun-Ke Cui,Jia-Tai Wen,Yan-Shan Wang,Meng-Hui Jia,Shu-Zhen He,Wei-Kang Wang,Juan Xu
Radical and nonradical dominated persulfate activation processes have pros and cons in the degradation of pollutants. It is challenging to flexibly tune the contribution ratios of radicals and nonradicals in a persulfate activation process for improved pollutant degradation. Herein, we successfully synthesize copper oxide catalysts derived from metal-organic frameworks. By varying the annealing temperature, valence states of copper can be regulated in the catalyst, thereby enabling the switching between radical and nonradical mechanisms for persulfate activation. Copper oxides annealed at 300 °C (CuBTC-300) demonstrate high performance in peroxydisulfate (PDS) activation for the degradation of bisphenol A (BPA), with the synergy of radical and nonradical mechanisms. The surface activated PDS-catalyst complex and OH are identified as the reactive oxidative species involved in this process. On one hand, PDS undergoes a one-electron transfer reaction with Cu(I) sites in Cu 2 O, generating SO 4 − , which subsequently converts into OH for BPA degradation. On the other hand, the combination of PDS molecules with CuO forms surface-activated complexes, depriving electrons from BPA. The increased content of Cu(II) in the catalyst gradually directs PDS activation towards the nonradical pathway. As the annealing temperature increases from 300 °C to 500 °C, the contribution of nonradical oxidation to BPA degradation increases from 58.65 % to 100 %. This work provides new insights into flexibly regulating persulfate activation mechanisms via rational catalysts design.
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Small
·
2023
·Vol. 20
·期 7
·2306820
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IF 13.3
Zheng Zheng,Bing Wang,Zhuo Li,Hong Hao,ChaoYang Wei,WenYu Luo,LinYu Jiao,Sheng Zhang,Bo Zhou,XiaoXun Ma
Constructing heterojunction of supramolecular arrays self-assembled on metal–organic frameworks (MOFs) with elaborate charge transfer mechanisms is a promising strategy for the photocatalytic oxidation of organic pollutants. Herein, H 12 SubPcB–Br (SubPc–Br) and UiO-66 are used to obtain the step-scheme (S-scheme) heterojunction SubPc–Br/UiO-66 for the first time, which is then applied in the photocatalytic oxidation of minocycline. Atomic-level B–O–Zr charge-transfer channels and van der Waals force connections synergistically accelerated the charge transfer at the interface of the SubPc–Br/UiO-66 heterojunction, while the establishment of the B–O–Zr bonds also led to the directional transfer of charge from SubPc–Br to UiO-66. The synergy is the key to improving the photocatalytic activity and stability of SubPc–Br/UiO-66, which is also verified by various characterization methods and theoretical calculations. The minocycline degradation efficiency of supramolecular SubPc–Br/UiO-66 arrays reach 90.9% within 30 min under visible light irradiation. The molecular dynamics simulations indicate that B–O–Zr bonds and van der Waals force contribute significantly to the stability of the SubPc–Br/UiO-66 heterojunction. This work reveals an approach for the rational design of semiconducting MOF-based heterojunctions with improved properties.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Lufang Fan,Sheng Feng,Kai Wei,Xiaojun Dai,Weijie Zhang,Haihong Wang,Zhaowei Bian,Kaidi Wu,Zhiwen Ge,Jinghao Hua
In this study, we designed and fabricated a Z-scheme Cu 0.5 Cd 0.5 S/MoO 3-x (CMO) heterojunction with localized surface plasmon resonance (LSPR) effect for efficient photocatalytic hydrogen evolution. The oxygen vacancies (OVs) in MoO 3-x induced Schottky-barrier-free LSPR for the generation of hot electrons. The architecture of transition-metal-substituted solid solution (Cu 0.5 Cd 0.5 S, CCS) downshifted the conduction band (CB) of CdS from −0.45 eV to −0.38 eV and upshifted the valence band (VB) from 1.65 eV to 1.54 eV, respectively, weakening the interface barrier of the hot electrons transition from MoO 3-x to CCS and enhancing the Coulomb interaction between the electrons of MoO 3-x and the holes of CCS. Benefiting from the cooperation between Z-scheme heterojunction and LSPR effect, the hydrogen evolution rate (HER) of the optimized CMO was 19.28 mmol·g −1 ·h −1 under visible light with an apparent quantum yield (AQY) of 10.8 % at 420 nm, which was 3.0 and 1.4 times that of the CCS and CCS/MoO 3 . Moreover, the HER of CMO still reached 43.57 μmol·g −1 ·h −1 at 600 nm. This work paved a new path for efficient photocatalysts H 2 evolution by coupling Z-scheme heterojunction and non-noble-metal LSPR effect.
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Materials Today Sustainability
·
2023
·
IF 7.8
B. Chen,L. Liu,Y. Song,H. Liu,Z. Gong,Y. She,J. Liu,R. Niu,J. Gong
The development of hybrid photothermal materials coupling interfacial solar-driven water evaporation with advanced oxidation process has recently aroused extensive attention to simultaneously realize freshwater production and wastewater purification. However, designing advanced hybrid photothermal materials with high specific surface areas and robust active sites remains challenging to meet the distinct requirements of photothermal conversion and photocatalysis . Herein, we report the waste-to-metal-organic framework (MOF) strategy for converting waste poly(ethylene terephthalate) [PET] into Cr-MOF hexahedron with abundant active sites and large specific surface area (896.1 m 2 /g), and subsequently fabricate multifunctional chromium-based metal-organic frameworks (Cr-MOF)/carbon nanotube (CNT) composite solar evaporators in a cost-effective, scalable manner towards simultaneous interfacial solar-driven steam generation and stubborn contaminant removal . First, the composite evaporator presents high light absorption (98%), high photothermal conversion efficiency, super-hydrophilicity, low thermal coefficient (0.087 W/(m/K)) and low vaporization enthalpy. Accordingly, the composite evaporator not only holds a high evaporation rate (2.46 kg/(m 2 /h)), superior to most of advanced solar evaporators, but also owns good flexibility and long-term stability. Subsequently, according to density functional theory (DFT) calculation and COMSOL results, chromium sites of Cr-MOF and local solar heat contribute to the peroxymonosulfate (PMS) activation to produce various reactive species. Thereupon, the composite evaporator exhibits good tetracycline (TC) degradation activity. Finally, in the practical freshwater production and photocatalytic degradation, the freshwater production amount is 7.3 kg/m 2 per day, along with the tetracycline degradation efficiency of 92.4%. This work provides an ingenious strategy to massively synthesize hybrid evaporators and concurrently advances freshwater production and pollutant elimination.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Kunlun Yang,Yanxiao Chi,Yuxuan Yang,Zimo Lou,Tonghui Wang,Dengyang Wang,Hengfeng Miao,Xinhua Xu
To avoid severe aggregation and synergistically utilize the intrinsic and photocatalytic reducibility, pyrite (FeS 2 ) was loaded onto N-doped reduced graphene oxides (N-rGO) to fabricate a novel FeS 2 /N-rGO heterojunction catalyst for enhanced chromium (Cr(VI)) reduction in oxic condition to simultaneously investigate the specific effect and role of dissolved oxygen (DO). Characterization results showed that strong interaction and combination of FeS 2 and N-rGO not only achieved the uniform distribution of FeS 2 , but also increased the defects, and exposed more functional groups. Meanwhile, the Type II heterojunction was formed in FeS 2 /N-rGO, which facilitated the separation efficiency of photo-generated carriers and electrons, endowing FeS 2 /N-rGO a superior photocatalytic activity. Cr(VI) was almost completely reduced via FeS 2 /N-rGO within 60 min under irradiation (Cr(VI) = 10 mg/L, dosage = 0.2 g/L), 3 times that of pristine FeS 2 (18.7 %). Trapping and Electron Spin Resonance (ESR) experiments indicated that photo-generated e − and derived O 2 − species from photoactivation of dioxygen (DO) were the key reactive species for the enhancement of photo-assisted Cr(VI) reduction, rather than reductive Fe 2+ and S 2 2− species. Although the photocatalysis of FeS 2 /N-rGO cannot directly generate hydroxyl radicals ( OH), the oxidative OH ascribed to superoxide radicals ( O 2 − ), photo-induced holes and free DO preferentially consumed by Fe 2+ and S 2 2− with stronger reducibility. Hence, as compared to the anoxic condition , the reduction rate of Cr(VI) was slightly decreased, but still could be totally removed within 60 min in the oxic conditions. Due to the excessive amount of FeS 2 /N-rGO, Cr(III) after reduction would not be influenced by oxidative species and maintain stability under oxic condition. This study provided a facile modification strategy for FeS 2 based composites and uncovered its working mechanism for Cr(VI) decontamination .
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Yudong Xu,Yifei Song,Saisai Chen,Mengting Zhang,Jingqi Chen,Hongyu Li,Min Shi,Fabao Zhang
Lead-based halide perovskite is considered to be a potential visible-light-activated photocatalyst owing to its excellent optoelectronic properties. However, the toxicity of lead and the instability of the material restrict its wide application in the field of photocatalysis . A double perovskite structure is thought to be a solution to this problem. The authors prepared a series of samples, including Cs 2 AgInCl 6 , Cs 2 AgIn 1−x Fe x Cl 6 , and Cs 2 AgFeCl 6 through co-precipitation in acidic solutions. The effects of Fe 3+ doping on the crystal structure and morphology of Cs 2 AgInCl 6 were characterized by XRD and SEM. Based on density functional theory, VB-XPS and UV-Vis absorption characterizations, the band structure of Cs 2 AgInCl 6 and Cs 2 AgFeCl 6 were determined, showing that the bandgap of Cs 2 AgIn 1−x Fe x Cl 6 was reduced linearly by Fe 3+ doping. And Sudan Red III can be photocatalytically degraded by all samples under concentrated xenon lamp irradiation of 175 W, with Cs 2 AgFeCl 6 degrading 96% of Sudan Red III in 45 min. In addition, the Cs 2 AgFeCl 6 sample exhibits good cyclic stability and does not demonstrate any significant changes after two months in storage, showing that Cs 2 AgFeCl 6 may serve as an effective and relatively stable Xenon lamp-activated photocatalyst in degradation of organic dyes.
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Small Methods
·
2023
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IF 12.4
Yunchao Zhao,Shaobo Wang,Shuncheng Yao,Xingyi Wan,Quanhong Hu,Minjia Zheng,Zhuo Wang,Linlin Li
The efficacy of sonodynamic therapy (SDT) mainly relies on the sonosensitizers, which generate reactive oxygen species (ROS) upon ultrasound (US) stimulation. However, the limited availability of high-efficiency sonosensitizers hampers the therapeutic effectiveness of SDT as a standalone modality. In this work, a robust sonodynamic and gas cancer therapeutic platform is constructed based on strontium (Sr) doped barium titanate (BST) piezoelectric nanoparticles functionalized with L-arginine (BST@LA). The doping of Sr into A site of the ABO 3 piezoelectric nanocrystals not only introduces oxygen vacancies into the nanoparticles and enhance the intrinsic piezoelectricity, but also narrows the semiconductor band gap and enhances charge carrier migration, all of which facilitate the sonodynamic production of superoxide anion (•O 2 − ) and hydroxyl radical (•OH). In addition, the generated ROS promotes the decomposition of the surface-tethered LA, enabling the controlled release of nitric oxide (NO) gas at the tumor site, thereby achieving a combination therapeutic effect. In vivo experiments exhibit remarkable tumor suppression rate (89.5%) in 4T1 tumor mice model, demonstrating the effectiveness of this strategy. The ion doping and oxygen vacancy engineering to improve sonosensitizers, along with the synergistic combination of sonodynamic and gas therapy, provides promising avenues for improving cancer therapy.
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Hussein Abdelraouf,Fanyang Zhou,Yulong Li,Jiayi Ren,Guanshu Zhao,Qingliang Zhao,Jian Wei,Xuedong Zhai,Jing Ding
The easily synthesized, cost-effective, and stable photocatalysts for sulfite activation are always required for the enhancement of organic contaminants degradation. Herein, the facile coprecipitation synthesis of Bismuth oxybromide (BiOBr)/Montmorillonite (MMT) was reported, which could activate sulfite (SO 3 2− /HSO 3 − ) under sunlight and accelerate the catalytic performance more effectively than pristine BiOBr. After adding sulfite to the photocatalysis system, the photodegradation efficiency of atrazine (ATZ) achieved 73.7% ± 1.5% after 5 min and 94.4% ± 1.6% after 30 min of sunlight irradiation with BiOBr/MMT. The BiOBr/MMT-sulfite system also presented remarkable photocatalytic performance to eliminate various contaminants, including ciprofloxacin, sulfadiazine, tetracycline , and carbamazepine. The various features of the photocatalyst materials were studied, including their surface morphology, structure, optical properties , and composition. The results illustrated that by adding MMT, the bandgap of the pristine BiOBr was reduced and the surface area was increased, which led to an increased ability to adsorb materials. Results of various influence factors showed this enhanced system had satisfactory and stable removal performance of ATZ in the pH range of 3.0–6.5, but HPO 4 2− had a strong negative effect on the system performance. Oxysulfur radicals (SO 5 ·- and SO 4 ·- ), h + , and 1 O 2 were discovered as the prevailing active species in the BiOBr/MMT-sulfite system. The proposed degradation mechanism of this photocatalyst-enhanced system revealed that sulfite adsorption on the surface of the photocatalyst played a vital role during the initial phase, and the degradation pathway of ATZ was discussed. This study provides a new synthesis strategy of a photocatalyst for sulfite activation and expands the potential uses of Bi-based photocatalysts in degrading difficult-to-remove organic pollutants.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2023
·
IF 6.8
Teng Wang,Lin Liu,Qingsong Zhao,Zhaofu Meng,Wenbin Li
To determine the fates of the persistent pollutants cadmium (Cd) and micro-plastics in agricultural soils, an in-depth understanding of the interactions between Cd and mulching film is required. In the present work, pot experiments are conducted under natural conditions to study the influence of various Cd concentrations on the aging process of polyethylene mulching film in soil collected from Changzhi, Shanxi Province. The results indicate that during 150 days, the aging degree of the mulch film increases gradually as the increased Cd concentration in the soil. Further, the results of attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectrometry and X-ray photoelectron spectroscopy (XPS) demonstrate that the average vinyl index (VI) of the aging mulch film increases from 1.29 to 1.82, while the oxygen-to-carbon (O/C) ratio of the mulch film decreases significantly from 0.344 to 0.045, as the Cd concentration is increased from 0 to 10 mg kg –1 . When the aging time exceeds 90 days, the oxygen-containing functional groups (C–O and C O) generated consumed by the adsorbed Cd. In addition, electron paramagnetic resonance (EPR) measurements indicate that Cd both enhances the formation of hydroxyl radical ( · OH) on the surface of the mulch film and prevents the combination of · OH and electrons, thereby accelerating the aging of the mulch. Hence, the present study indicates that the presence of Cd will hasten the decomposition of mulch, which will inevitably result in the faster release of micro-plastics from the mulch into the soil environment.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Fan Liu,Jing Ding,Qingliang Zhao,Guanshu Zhao,Kun Wang,Lili Li,Shuyan Guan
Advance oxidation process (AOP) is a promising way for micropollutants treatment, but the consumption of chemicals and energies limits its large-scale application. To address this issue, a novel boron-doped biochar (BBC) system was developed for the efficient removal of micropollutants, requiring no external energy or oxidant. Herein we demonstrated that the synthesized BBC could efficiently activate the dissolved oxygen (O 2 ) in the water or oxidize micropollutant directly. The complete sulfamethoxazole (SMX) could be removed within 30 min by the BBC synthesized at 600 °C (BBC-600). The experiments on material characterization and removal performance with quenchers revealed that the introduction of boron into biochar increased the active sites for O 2 activation, including persistent free radicals (PFRs) and boron moieties (BC 3 , BCO 2 , and BC 2 O) on the biochar. The generated reactive oxidation species (ROS), mainly O 2 − , were responsible for the SMX degradation in this BBC system. Different performance of aged experiments in air and N 2 conditions indicated that PFRs could also directly oxidize SMX. Density functional theory (DFT) was used to further illustrate the inner mechanism of enhanced electron transfer via boron moieties for O 2 activation and SMX degradation. Electrons of the adsorbed micropollutant could be transferred to boron moieties, and then trapped by O 2 in water to produce O 2 − and 1 O 2 for SMX degradation. This study provided a new insight into the structure–activity relationship of B-doped biochar for the direct and indirect degradation of micropollutant, and opened a new avenue for micropollutant degradation without external energy and oxidant.
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SENSORS AND ACTUATORS B-CHEMICAL
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2023
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IF 8.4
Wenyuan Zhou,Yajie Li,Guoqiang Zhu,Xuechao Xu,Qin Hu,Zhenquan Yang,Xuewen Gu
Although bacteriophage-based biosensors are promising tools for the rapid, convenient, and sensitive detection of S. aureus in food products, the effect of biosensors using temperate phages as the biorecognition element to detect viable S. aureus isolates remains unclear. In this study, four temperate Staphylococcus aureus phages were isolated, and their biological features were compared. The selected phage, SapYZUs7, was immobilised on an MnCo 2 O 4 nanozyme to prepare SapYZUs7@MnCo 2 O 4 , and the application of SapYZUs7@MnCo 2 O 4 in the S. aureus detection was evaluated. Compared to the other three S. aureus phages, SapYZUs7 exhibited a higher titre, broader host range, greater pH tolerance (3–12, > 91 %), higher absorption rate (71.6 %, 6 min), and more unique gene content. The characterisation of SapYZUs7@MnCo 2 O 4 revealed its successful immobilisation, excellent biological activity, and peroxidase-mimicking ability. Moreover, the SapYZUs7@MnCo 2 O 4 exhibited high sensitivity and specificity for the rapid colorimetric determination of viable S. aureus counts, with a limit of detection of 0.77 × 10 2 CFU/mL. In addition, SapYZUs7@MnCo 2 O 4 was successfully employed for the colorimetric detection of S. aureus in food samples, regardless of different food additives , NaCl concentrations, and pH values. In conclusion, the SapYZUs7@MnCo 2 O 4 is a powerful tool for the detection of viable S. aureus in food matrices.
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