CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Sen Dang,Wei Hou,Yulin Min,Junfeng Wu,Qunjie Xu,Penghui Shi
This study aimed to further expand the scope of use of spent lithium-ion batteries (LIBs) and improve their value. We proposed a dual-function electro-oxidation strategy that can realize the highly selective recovery of Li + from spent NCM batteries and the in situ modification of delithiation materials. Under the optimum conditions, the selective recovery rate of Li + exceeded 99%. After electro-oxidation, the electrolyte can be directly heated and concentrated to obtain Li 2 CO 3 . Moreover, the large number of oxygen vacancies and metal vacancies produced by electro-oxidation, as well as the changes in structure and morphology, enabled the delithiation material to exhibit excellent catalytic performance. Within 30 min, the degradation rate of sulfamethoxazole reached 100%. This strategy can be used to recycle and reuse spent LIBs and thus achieve the goal of “turning waste into treasure”.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yunlong Zhang,Muhammad Irfan,Zeheng Yang,Kun Liu,Jianhui Su,Weixin Zhang
Anion chemistry of sulfonates plays a crucial role in dictating the electrochemical performance of composite solid polymer electrolytes (CSPEs), hence affecting the cyclability of lithium-ion batteries (LIBs). The CSPEs received great attention for LIBs, however, simultaneously achieving high ionic conductivity and long cycle life in realistic batteries is still a great challenge. Herein, we report new sulfonate anion with hydrophilic aromatic structure and ether alkyl spacer of hydroxyl wing namely lithium hydroxyphenyl propanesulfonate (LHPS), and a series of CSPEs obtained by coupling of the synthesized anions via tetraethyl orthosilicate to be used in LIBs. The CSPEs comprising LHPS achieve higher ionic conductivity and excellent cyclability with impressive stability due to their decent compatibility of hydroxyl wing, and aliphatic ether spacer with the polymeric matrix. The intramolecular and intermolecular interactions of LHPS with other precursors within anion-polymer matrices via hydrogen bonding reduce anionic species migration, thus augmenting Li + ion conduction and impeding lithium dendritic growth during the electrochemical performance. This opens a new avenue for designing conductive and long cycle life CSPEs for LIBs in the future.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xinxin Long,Chuanping Feng,Shengjiong Yang,Dahu Ding,Jinpeng Feng,Meng Liu,Yang Chen,Jihua Tan,Xingjie Peng,Jinan Shi,Rongzhi Chen
Oxygen atoms with lone pair electrons have been used to improve the photocatalytic activity of graphitic carbon nitride (g-C 3 N 4 ). Herein, a one-step annealing strategy without co precursor is used to prepare O-doped graphitic carbon nitride (OCN) for photocatalytic degradation of bisphenol A (BPA). The band structure and photocatalytic performance are tuned by simply controlling the heating time. The degradation rate constant for OCN6 is improved by 29 times compared to the original CN. Experimental and the density functional theory calculated results prove that the doped-O is the key factor in promoting photocatalytic performance. The introduced O not only adjusts local electron density, but also decreases the band gap to boost e - transfer and carrier generation and separation. The elevated conductive band energy is responsible for producing O 2 ∙ - , which is the dominated reactive oxygen species. This work offers a simple and effective way for the self-modification of metal-free catalysts to resolve environmental issues.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Tian-Yu Liu,Cong Wang,Yong-Zhe Han,Chang Bai,Hai-Tao Ren,Yong Liu,Xu Han
Bi 2+x WO 6 are a group of reactive photocatalysts in the photooxidation of various contaminants. However, their catalytic reactivity in the persulfate (PS)-based oxidation processes in the absence of light is still unknown. In this study, Bi 2.15 WO 6 shows a high reactivity in the catalytic oxidation of bisphenol A (BPA) by PS in the absence of light under alkaline conditions, and 20 mg L -1 BPA can be rapidly removed within 30 min at pH 10.0 with the low stoichiometry ratio of 1.79 between consumed PS and removed BPA. Characterizations of the oxidation products indicate that 98.4% of soluble BPA has been oxidatively polymerized to BPA polymers, instead of being oxidized to CO 2 and H 2 O. FTIR, Raman, XPS and electrochemical analyses confirm that surface Bi(III) is the reactive site for the adsorption of BPA and PS, which then initiates reactions between BPA and PS. DFT calculations reveal that the O-O bond in PS is moderately activated via the nonradical pathway after adsorbing on Bi(III), instead of being decomposed to SO 4 •− , followed by H-abstraction from BPA by the activated PS with the formation of phenoxyl radicals and the subsequent polymerization to BPA polymers. The apparently lower energy barrier from adsorbed BPA (Δ G = 0.056 eV) than that from dissolved BPA (Δ G = 0.263 eV) further reveals that H-abstraction from adsorbed BPA to the activated PS on the surface of Bi 2.15 WO 6 is more favorable than that from dissolved BPA. This study gives new insight on the efficient removal of recalcitrant contaminants via the H-abstraction pathway.
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JOURNAL OF CHROMATOGRAPHY A
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2022
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IF 4.601
Yan Wu,Kaixing Luo,Yanjuan Liu,Wei Chen,Zhengwu Bai,Sheng Tang
Developing a versatile stationary phase to achieve the purpose of efficiently separating various target analytes is of great significance. In this work, ureido/dodecyl dual-functionalized silica (Sil-Ur-DD) was synthesized and employed as a new mixed-mode stationary phase for high-resolution chromatographic analysis. It was observed that multiple interactions, including hydrophobic, hydrophilic, hydrogen bonding, electrostatic and π-π interactions, contributed to the retention. Nucleosides and nucleobases could be effectively determined in hydrophilic interaction chromatography mode, and the separation performance of the Sil-Ur-DD was found to be even superior to that of the commercial XAmide column. Environmental endocrine disruptors, including alkylphenols, bisphenols, steroid hormones and phthalates, were more favorably separated in reversed-phase chromatography mode with highly aqueous mobile phases compared with the commercial C18-silica column. The experimental results indicated that the combined effect of ureido and long-chain alkyl groups obviously enhanced separation efficiency and selectivity. More significantly, the proposed method concerning the preparation of an efficient separation material with powerful separation ability is economical and environmentally friendly, which provides a proven and effective way for the recycling and utilization of the discarded chromatographic packing materials, thereby showing a good application prospect.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Wenwei Feng,Yousef Faraj,Yuan Yan,Yaoxiao An,Ruzhen Xie,Bo Lai
The design of a high-efficiency and ecofriendly persulfate (PS) activator with low cost and superior performance in water decontamination still remains a big challenge. Herein, we report a facile strategy for the synthesis of novel pyrolusite-templated mesoporous catalyst (PMC), and used it as a green PS activator for the outstanding removal of bisphenol A (BPA) in water. The N2 adsorption–desorption curves and SEM-EDS images show that pyrolusite templating can successfully modulate the mesoporous structure of the catalyst; the XRD and XPS spectra indicate that pyrolusite templating renders the catalyst with enriched active sites and faster electron transfer. The mechanism studies suggest that both the radical and nonradical pathway [singlet oxygen (1O2)] contributed to BPA degradation, and 86.81% of the total organic carbon (TOC) of 100 mg/L BPA was removed using merely 0.4 g/L PMC, without detectable metal ion leaching. This work provides a new strategy for the structural design and property adjustment of an efficient persulfate catalyst for green environmental remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Zenglong Wu,Wenkai Song,Xiangwei Xu,Jiangnan Yuan,Weiyang Lv,Yuyuan Yao
Applicating co-catalyst into Fenton-like advanced oxidation processes to improve the performance for wastewater remediation has attracted widespread attention. Among them, developing highly active and green heterogeneous catalyst integrating homogeneous ferrous ions and inorganic co-catalyst is a great challenge. Herein, ascorbic acid additive was creatively introduced into the precursor composed of thiourea, sodium molybdate and ferric chloride to synthesize carbon intercalated molybdenum disulfide anchoring iron (C-MoS 2 @Fe) by a simple one-step hydrothermal method. C-MoS 2 @Fe exhibited an amazing apparent first-order constant as high as 0.739 min −1 about 10 times higher than that of the homogeneous Fe 2+ /MoS 2 system for the sulfamethoxazole (SMX) removal and achieved 68.7% removal of TOC in 6 min, which was attribute to the synergistic enhancement of high 1T phase (82.0%) and sulfur vacancies induced by the introduction of ascorbic acid. Notably, the C-MoS 2 @Fe was also capable of efficiently degrading multiple organic contaminants such as pharmaceuticals, phenolic compounds, and organic dyes. Compared with the homogeneous Fe 2+ /PMS system, the C-MoS 2 @Fe/PMS system expanded the effective pH range (2.0 ∼ 9.0) and the ultralow iron ions leaching (0.204 mg L -1 ) avoided the formation of iron containing sludge. The results of electron paramagnetic resonance (EPR), radical quenching and probe experiments indicated that •OH was the main active species with the contribution rate about 60.3%. Furthermore, possible degradation pathways were proposed based on the intermediate products of SMX investigated by LC-MS. This study provides novel insights for the development of highly active and green catalysts for wastewater remediation.
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CHINESE JOURNAL OF POLYMER SCIENCE
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2022
·Vol. 40
·期 3
·310-320
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IF 3.815
Duan Zheng-Yu,Wang Yan-Yan,Pan Qi-Wei,Xie Yun-Feng,Chen Zhi-Yong
Microporous organic polymers with high surface area are widely used in many applications. Among them, hypercrosslinked polymers have been extensively concerned because of their simple processes and low-cost reagents. However, due to most state-of-the-art strategies for HCPs based on condensation reactions, the release of small molecules such as hydrochloric acid and methanol involved in such strategies brings about new hazards to environment. Herein, we propose a method of fabrication of hypercrosslinked polymers via self-addition polymerization of divinyl benzene and its crosslinking with polar aromatic molecules. The hypercrosslinked polyDVB-based products are demonstrated by Friedel-Crafts addition reaction of double bonds on DVB that can connect adjacent phenyl rings of aromatic molecules to form the crosslinked networks. The HCPDVB-CB obtained in 1-chlorobutane as solvent has a high micropore content and displays high surface area up to 931 m 2 /g. Following this finding, DVB is used as a novel external crosslinker for knitting polar aromatic molecules. When L-phenylalanine and bisphenol A are used as the aromatic units, the obtained HCP(Phe-DVB) and HCP(BPA-DVB) could reach surface area of 612 and 471 m 2 /g, and have hydrogen uptake of 0.62 wt% and 0.58 wt% at 77 K and 1.13 bar by comparison with HCPDVB-CB having hydrogen uptake of 0.30 wt%, respectively.
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JOURNAL OF SEPARATION SCIENCE
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2022
·Vol. 45
·期 9
·1493-1501
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IF 3.614
Chengjiang Zhang,Hongmei Yuan,Zeyi Lu,Yuhuang Li,Lirong Zhao,Zhuomin Zhang,Gongke Li
Covalent organic frameworks with tunable porous crystallinity and outstanding stability have exhibited fascinating pretreatment performance as ideal extraction media. Herein, the β-ketoenamine-linked TpPa-1 synthesized by 1,3,5-triformylphloroglucinol and paraphenylenediamine was employed as the absorbent for online micro-solid phase extraction of trace bisphenols combined with high-performance liquid chromatography detection. A series of characterizations indicated that the TpPa-1 possessed large surface areas, high stability, and hydrophobicity. The main experimental parameters affecting the extraction efficiency were optimized in detail. Compared with four commercial sorbents, the TpPa-1 exhibited superior enrichment capacity for extracting bisphenols. Under the optimum conditions, the established method demonstrated a wide linear range and high sensitivity with the limit of detection ranging from 0.05–0.06 μg/L. Furthermore, the developed method was successfully applied to determine bisphenols in plastic samples. Bisphenol A was actually detected in a transparent box with a concentration of 0.31 μg/g, and the recoveries of the four bisphenols in the plastic samples were 80.5–116% with the relative standard deviation less than 9.2%. Such performance was attributed to recognition affinity, including the π-π affinity, hydrophobic effect, and hydrogen bond. These results demonstrated that TpPa-1 possessed great potential to be an excellent pretreatment medium for online separation and analysis of trace analytes in complex samples.
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RSC Advances
·
2022
·Vol. 12
·期 12
·7306-7312
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IF 4.036
Yixiao Li,Qi Min,Yunfei Wang,Xuming Zhuang,Xiaowen Hao,Chunyuan Tian,Xiuli Fu,Feng Luan
In this work, a ratiometric fluorescence sensor along with a portable coffee ring visualized detection method for bisphenol A (BPA) was developed based on carbon dots. The probe was formed by the coordination polymerization of Eu3+ and 5′-adenosine monophosphate on the surface of carbon dots containing a large number of hydroxyl and carbonyl groups. The results showed that the fluorescence intensity ratio and the concentration of BPA had a good linear relationship in a wide range of 0.1–100 μM with a detection limit of 20 nM (S/N = 3). The recoveries of the added standard BPA in water samples ranged from 91.80 to 102.7% with relative standard deviation values no more than 1.84% (n = 3). In addition, the changes of the fluorescence color of the CDs@Eu–AMP suspension with different BPA concentrations can be easily visualized under a UV lamp by the naked eye, which highlights the great potential of the coffee ring detection method for the fast and convenient monitoring of BPA in real water samples.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Dongli Guo,Yuan Yao,Shijie You,Limin Jin,Ping Lu,Yanbiao Liu
Herein, we developed and evaluated an electrochemical periodate (PI) activation system for the ultrafast degradation of aqueous micropollutants (τ < 3 s). Filters constructed from carbon nanotubes (CNT) coated with Fe 2 O 3 nanoparticles on the outer (Fe 2 O 3 -out-CNT) and inner surfaces (Fe 2 O 3 -in-CNT) were prepared to regulate the generation of reactive oxygen species (ROS) during PI activation. The activation function of the electroactive nanohybrid filters lay in their ability to facilitate the redox cycling of Fe(III)/Fe(II) assisted by an electric field. The results showed that a non-radical ( i.e ., 1 O 2 ) pathway dominated the degradation process in the electro/Fe 2 O 3 -in-CNT/PI system, while a contrastive radical pathway ( i.e ., HO • and IO 3 •) was identified in the electro/Fe 2 O 3 -out-CNT/PI system. The electro/Fe 2 O 3 -in-CNT/PI system exhibited enhanced catalytic activity towards the micropollutants degradation relative to its electro/Fe 2 O 3 -out-CNT/PI counterpart. Density functional theory calculations suggested that PI could be directly decomposed under the nanoconfined environment, rather than forming a stable adsorption complex in the unconfined system.
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ENVIRONMENTAL TOXICOLOGY
·
2022
·Vol. 37
·期 7
·1551-1562
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IF 4.109
Dan Song,Yuan Liu,Yaxin Yao,Feng Liu,Wenjing Tao,Xiaolong Zhou,Runsheng Li,Xiaowei Zhang,Xiangchen Li
The aim of this study was to assess the protective effect and potential mechanism of melatonin against bisphenol A (BPA)-induced apoptosis and oxidative damage in FLK-BLV cells. The results showed that BPA reduced cell viability in a dose- and time-dependent manner, caused cell shrinkage and induced oxidative stress and apoptosis in FLK-BLV cells, which were effectively reversed by melatonin. In addition, BPA caused autophagy flux impairment, which was confirmed by the increased of LC3-II and p62 levels, whereas melatonin treatment effectively reduced p62 levels under BPA treatment, and reversed apoptosis-related protein expression patterns caused by BPA. However, inhibition of autophagy by CQ partially abolished the protective effect of melatonin on apoptosis, suggesting that melatonin against BPA-induced oxidative injury and apoptosis by activating autophagy pathway. Moreover, we found that melatonin inhibited BPA-induced the activation of p38 MAPK, which was comparable to SB203580 pretreatment, and companied by the activation of autophagy and decreases of apoptosis when compared to BPA alone, indicating that melatonin protected against BPA-induced apoptosis partially through the p38 MAPK-autophagy pathway. In conclusion, these results suggest that melatonin may prevent BPA-induced FLK-BLV cell damage by inhibiting p38/MAPK signaling pathway and activating autophagy, and it could be a potential therapeutic compound in preventing BPA-induced cell damage.
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