Materials Today Sustainability
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2023
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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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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Xiao Li,Jin Chang,Hexin Zhang,Jing Feng,Jun Ma,Chengying Bai,Yueming Ren
Photocatalytic nitrate (NO 3 - ) reduction is considered a promising green and non-polluting technology to solve the nitrate pollution of groundwater and surface water. Herein, a novel Br-substituted Bi 2 WO 6−x ultrathin nanosheets were prepared by a simple hydrothermal method in a strong acid environment containing sixteen alkyl three methyl bromide (CTAB). The catalytic system solves the problems of low carrier separation efficiency, poor performance under alkaline conditions, and a hard-to-activate N = O bond, achieving efficient NO 3 - removal under alkaline conditions along with high N 2 selectivity . It was confirmed that Br-substituted Bi 2 WO 6−x produced the [W (VI) O 6−x ] units with a strong electron-withdrawing property by changing the polarity of the O-W-O bond. As a result, the effective space charge separation caused by the change of the W valence state and the spontaneous fracture behavior of the N = O bond improved the carriers utilization efficiency and distinctly reduced the reaction energy consumption, synergistically achieving excellent performance.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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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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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
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2023
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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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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Afang Wang,Yang Shi,Yang Liu,Wei Li,Heng Zhang,Xiaoqiang Dai,Li Luo,Gang Yao,Bo Lai
Traditional Fenton and Fenton-like processes are affected by the sluggish kinetics of Fe(II) regeneration and Fe(III) accumulation. This research revealed that the degradation efficiency of pollutants was significantly increased by adding Fe(III) to the Vis/PS system. A mechanism is proposed in which photosensitivity pollutants can boost Fe(III) to produce Fe(II) under visible light irradiation. Intriguingly, Fe(III) rapidly combines with LVF in aqueous environments to form Fe(III)-LVF complexes. This research confirms that Fe(III)-pollutant complexes are generated. The proportion of complexes are calculated using mathematical models. Furthermore, the production of Fe(IV) is verified in the Vis/PS/Fe(III) system, which also plays a vital role in boosting LVF degradation. Overall, this study provides comprehensive insights into the degradation mechanism of micropollutants, involving hydroxyl radical ( OH ∙ ), Fe(IV), and Fe(III)-LVF complexes, providing an efficient and green strategy for contaminant removal during wastewater treatment .
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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
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2023
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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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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Jiangwei Shang,Shuwen Fan,Shihu Cao,Xinrui Gan,Jing Nie,Tianning Zhang,Xiangchen Li,Dan Feng,Xiuwen Cheng
In this study, a CuCo 2 S 4 microporous composite membrane (CCSM) was successfully prepared by loading CuCo 2 S 4 nanoparticles on a membrane substrate, and then used to activate PMS to degrade carbamazepine (CBZ). Meanwhile, the physicochemical properties of the nanomaterial and the effects of various reaction parameters, such as, catalyst film loads, PMS dosage, initial pH value, and co-existing substances on the catalytic degradation performance were investigated. The results showed that CCSM/PMS exhibited admirable catalytic performance, and 90.3% CBZ could be degraded within 3 min under the optimum conditions ([CuCo 2 S 4 ] = 0.05 g L −1 , [PMS]=0.30 g L −1 , [CBZ] 0 =10 g L −1 and Initial pH = 6.95). Furthermore, the CCSM/PMS system could efficiently degrade various antibiotics (sulfamethoxazole, metronidazole, hydrochloride and ciprofloxacin). In addition, the reusable ability of CCSM without significant efficiency loss after 10 cycles. The quenching experiments and electron paramagnetic resonance (EPR) characterization showed that the main active species were SO 4 • - , •OH, O 2 • - and 1 O 2, and SO 4 • - played a dominant role in this system. Finally, based on the data analysis, the study proposed the possible degradation mechanism and four degradation routes of CBZ.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Jiajun Yu,Xiao Wang,Yan Wang,Xiaofeng Xie,Haijiao Xie,Nat Vorayos,Jing Sun
The removal of indoor/outdoor toluene by photocatalysis has drawn much attention due to its low energy consumption and easy availability. However, light inevitably generates heat, and pollutants desorb from catalysts as the temperature rises, which is not beneficial to degradation. Contrast to the frequently occurred phenomena, we firstly found that the adsorption capacity of UiO-66 (Zr) on toluene increased with increasing temperature as adsorption isotherms and in-situ Fourier transform infrared spectra (in-situ FTIR) showed. The optimum temperature was 30 °C. This stage in which adsorption capacity was positively correlated with temperature was called heating-induced adsorption, which achieved a toluene removal efficiency of 69.6 %. By density functional theory (DFT) calculations and changing the metal centers and organic ligands of UiO-66 (Zr) respectively, we disclosed that the heating-induced adsorption was mainly related to the π-π stacking interaction of MOF ligands and toluene. The analysis of samples before and after adsorption showed that the interaction between UiO-66 (Zr) and adsorbed toluene facilitated the charge transfer and prolonged the carrier lifetime, leading to the increase of hydroxyl radicals (•OH) in photocatalysis. Therefore, a synergistic effect between heating-induced adsorption and photocatalysis was proposed by analyzing the adsorption of toluene on UiO-66 (Zr) in detail. This work provided new viewpoint to understand the role of concomitant heat contributed to the adsorption and degradation of toluene during photocatalysis.
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JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Ying Mei,Yushan Huang,Haochen Xu,Wulin Yang,Xiaocheng Lin
Fouling control is the most critical concern in the implementation of nanofiltration (NF) for dye wastewater treatment . In this study, integration of NF and Fenton-like advanced oxidation was realized by tailoring a thin film composite NF membrane (TFNi) with in situ synthesized PDA/MnO 2 interlayer. TFNi was optimized by controlling the amount of MnO 2 nanoparticles incorporated within the interlayer which endowed the membrane with self-cleaning property. Besides it improved the membrane surface hydrophilicity and optimized the water transport path, resulting in alleviated fouling risks and an enhanced water permeance of 24 ± 2 L m −2 h −1 bar −1 compared to the control membrane. Fouling and subsequent chemical cleaning experiments were carried out on TFNi under various water chemistry conditions to elucidate the underlying mechanisms governing the self-cleaning properties. Accordingly, a high flux recovery ratio ( FRR ) (above 95%) was maintained thanks to the generation of free radicals by MnO 2 –H 2 O 2 system which was validated by determining the free radical scavenging activities. Moreover, the interlayer confined radicals can facilitate the decomposition of foulants on TFNi. Conclusively, H 2 O 2 -initiated self-cleaning of TFNi can be of great prospect for the efficient treatment of dye wastewater via in-situ generated free radicals.
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Journal of Environmental Chemical Engineering
·
2023
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IF 7.7
Junyong He,Ya Yang,Peidong Hong,Yulian Li,Chao Xie,Zijian Wu,Minqiang Li,Lingtao Kong
The use of peroxymonosulfate (PMS) activation to eliminate organic contaminants is a promising technology to purify water owing to its strong reactivity. However, because of the existed rate limiting step, the performance of PMS activation was restrained and required external energy consumption. Therefore, a new strategy was proposed to solve this problem by preparing catalysts with abundant electron-rich sites and electron traps to accelerate PMS activation. In this research, a novel MnCeO x -H catalyst with rich surface oxygen vacancies was firstly synthesized to accelerate the transfer of electrons among the catalysts, oxidant and pollutants. The contaminants were rapidly eliminated in the MnCeO x -H/PMS system, while the reaction rate constant of MnCeO x -H/PMS system was 30 times higher than that of CeO 2 /PMS system. The surface oxygen vacancies were able to adsorb and trap PMS, then the free electrons of oxygen vacancies would reduce PMS and produced HO•, 1 O 2 and SO 4 •- , while 1 O 2 played a major role. The contaminants which acted as electron-donors in this system were adsorbed at Mn, Ce sites, achieving effective conversion recycling of Ce(IV)/Ce(III), Mn(III)/Mn(II) and Mn(IV)/Mn(III). This discovery is believed to inaugurate a novel way for designing powerful electron-rich sites and electron traps to accelerate PMS activation for contaminants degradation.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2023
·
IF 6.1
Nian Liu,Yuqi Zhang,Jiaoyan Huang,Sicong Liu,Taiping Qing,Peng Zhang,Bo Feng
In the realm of sensing, carbon dots (CDs) have exhibited remarkable fluorescence characteristics. In the field of catalysis, CDs can function concurrently as electron donors and acceptors and have substantial electron or hole transport capacities. In this study, both merits were integrated into one, and a one-step hydrothermal approach was used to create multifunctional CDs. On the one hand, CDs are employed as a fluorescence probe with good sensitivity and selectivity to detect Cr(VI). On the other hand, CDs exhibit strong photoreduction capabilities for Cr(VI) in the absence of any external cocatalysts or photosensitizers when acting as photoinitiators. The results show that Cr(VI) quenches the CDs fluorescence as a result of the combined effects of static quenching and the inner filter effect. At the same time, under the condition of illumination, the inner filter effect encourages the CDs electrons to move from the valence band to the conduction band, resulting in electron hole pairs. With the help of electrons' reducing power, Cr(VI) can be rapidly and effectively converted to Cr(III). The findings of this study suggest that CDs are a satisfying bi-functional carbon-based material with significant potential for the treatment of industrial wastewater.
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