DALTON TRANSACTIONS
·
2026
·
IF 3.3
Jingsha Xu,Xiaofeng Zhang,Shanshan Chen,Weiyi Wang,Wenbo Qiu,Weizhao Cai,Liujiang Zhou
Nonlinear optical (NLO) crystals serve as indispensable components in laser technology. Many modifications of sulfate-based NLO materials rely on introducing a single type of functional cation, which in some cases leads to an imbalanced improvement in either NLO response or birefringence. To enable simultaneous improvement of these key properties, we designed and synthesized a novel sulfate compound, Nb2O2(TeO3)2(SO4), using a double second-order Jahn-Teller (SOJT) strategy that introduces both Nb5⁺ (d0 cation) and Te4+ (lone-pair cation) into the sulfate framework. Remarkably, the introduction of distorted [NbO6] octahedra and [TeO3] pyramids enables the material to achieve a remarkable birefringence of 0.197 at 546 nm and a second-harmonic generation (SHG) response of 0.82 times that of KH2PO4 (KDP). Furthermore, the compound exhibits high thermal stability (> 600 °C), maintains chemical stability in both water and concentrated sulfuric acid, and possesses an ultraviolet (UV) cutoff edge at 305 nm. Theoretical analyses confirm that the synergy between the [NbO6] octahedra and [TeO3] pyramids is the key mechanism for the enhanced SHG response and birefringence. This work demonstrates the potential of Nb2O2(TeO3)2(SO4) as an UV-NLO material and validates the effectiveness of the multi-component synergistic strategy in designing advanced NLO crystals.
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高影响因子
WATER RESEARCH
·
2020
·
IF 9.13
Xiaoyu Yu,Jianliang Sun,Guibiao Li,Yi Huang,Yu Li,Dehua Xia,Feng Jiang
The sulfate radical (•SO 4 − )-based advanced oxidation processes (AOPs) for the degradation of refractory organic pollutants consume a large amount of persulfate activators and often generate toxic organic by-products. In this study, we proposed a novel iron-cycling process integrating •SO 4 − -based AOP mediated by reusable iron particles and a sulfidogenic process to degrade and detoxify Orange II completely. The rusted waste iron particles (Fe 0 @Fe x O y ), which contained Fe II /Fe III oxides (Fe x O y ) on the shell and zero-valent iron (Fe 0 ) in the core, efficiently activated persulfate to produce •SO 4 − and hydroxyl radicals (•OH) to degrade over 95% of Orange II within 120 min. Both •SO 4 − and •OH destructed Orange II through a sequence of electron transfer , electrophilic addition and hydrogen abstraction reactions to generate several organic by-products (e.g., aromatic amines and phenol), which were more toxic than the untreated Orange II. The AOP-generated organic by-products were further mineralized and detoxified in a sulfidogenic bioreactor with sewage treatment together. In a 170-d trial, the organic carbon removal efficiency was up to 90%. The inhibition of the bioreactor effluents on the growth of Chlorella pyrenoidosa became negligible, due to the complete degradation and mineralization of toxic AOP-generated by-products by aromatic-degrading bacteria (e.g., Clostridium and Dechloromonas ) and other bacteria. The sulfidogenic process also well recovered the used Fe 0 @Fe x O y particles through the reduction of surface Fe III back into Fe II by hydrogen sulfide formed and iron-reducing bacteria (e.g., Sulfurospirillum and Paracoccus ). The regenerated Fe 0 @Fe x O y particles had more reactive surface Fe II sites and exhibited much better reactivity in activating persulfate in at least 20 reuse cycles. The findings demonstrate that the integrated process is a promising solution to the remediation of toxic and refractory organic pollutants because it reduces the chemical cost of persulfate activation and also completely detoxifies the toxic by-products.
研究领域:
环境科学
·
污染治理
·
微生物学
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DOI
PubMed
高影响因子
CELLULOSE
·
2022
·Vol. 29
·期 4
·2257-2272
·
IF 6.123
Shi Ning,Zhu Yuju,Qin Bangzhi,Liu Ying,Zhang Hongyan,Huang Hongsheng,Liu Yunhua
A simple and efficient biphasic system comprising H 2 O, tetrahydrofuran (THF), cyclohexane (CHX) and Al 2 (SO 4 ) 3 was employed to convert cellulose into 5-hydroxymethylfurfural (HMF). The volume ratio of the organic phase to the aqueous phase (V org /V aque ), concentration of Al 2 (SO 4 ) 3 in the aqueous phase (C[Al 2 (SO 4 ) 3 ] aque ) and concentration of Al 2 (SO 4 ) 3 in the organic phase (C[Al 2 (SO 4 ) 3 ] org ) of the biphasic system played critical roles in the conversion of cellulose into HMF. In the biphasic systems with H 2 O/THF/Al 2 (SO 4 ) 3 of 4/18/0.4 and H 2 O/THF/CHX/Al 2 (SO 4 ) 3 of 3/16/3/0.4, > 80% of the added H 2 O was dissolved in the organic phase, whereas most of the added Al 2 (SO 4 ) 3 remained in the aqueous phase under the reaction temperature, jointly leading to high V org /V aque , high C[Al 2 (SO 4 ) 3 ] aque and low C[Al 2 (SO 4 ) 3 ] org in the biphasic system. All of these results yield the excellent performance of these biphasic systems in the conversion of cellulose into HMF. The addition of CHX into the biphasic system can decrease the solubility of Al 2 (SO 4 ) 3 in the organic phase, thus improving the stability of HMF in the reaction system. The influences of catalyst usage, reaction temperature and time, and cellulose/solvent ratio were all explored, and a high HMF yield of 71.2% was obtained in the H 2 O–THF–CHX biphasic system with an H 2 O/THF/CHX volume ratio of 3/16/3 under optimized conditions. Graphical abstract
研究领域:
化学工程
·
生物质能
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高影响因子
Heliyon
·
2023
·Vol. 10
·期 1
·e23371
·
IF 4
Mingming Zheng,Yinghao Li,Menghua Cao,Yuxin Guo,Guohong Qiu,Shuxin Tu,Shuanglian Xiong,Dun Fang
In the present study, we demonstrated that the presence of cysteine could remarkably enhance the degradation of atrazine by Fe 3 O 4 /persulfate system. The results of electron paramagnetic resonance (EPR) spectra confirmed the combination of cysteine and Fe 3 O 4 exhibited much higher activity on activation of persulfate to generate more SO 4 •- and •OH than Fe 3 O 4 alone. At pH of 3.0, SO 4 •- and •OH contributed to about 58.2 % and 41.8 % of atrazine removal respectively, while •OH gradually dominated the oxidation of atrazine from neutral condition to alkaline condition. The co-existing Cl - and HCO 3 - could quench SO 4 •- , resulting in the inhibition of atrazine degradation. The presence of low natural organic matters (NOM) concentration (0-2 mg L -1 ) could enhance the atrazine removal, and high concentration (>5 mg L -1 ) of NOM restrained the atrazine degradation. During the Cysteine/Fe 3 O 4 /Persulfate process, cysteine served as a complexing reagent and reductant. Through acidolysis and complexation, Fe 3 O 4 could release dissolved and surface bound Fe 2+ , both of which contributed to the activation of persulfate together. Meanwhile, cysteine was not rapidly consumed due to a regeneration process, which was beneficial for maintaining Fe 2+ /Fe 3+ cycle and constantly accelerating the activation of persulfate for atrazine degradation. The reused Fe 3 O 4 and cysteine in the Cysteine/Fe 3 O 4 /Persulfate process exhibited high stability for the atrazine degradation after three cycles. The degradation pathway of atrazine included alkylic-oxidation, dealkylation, dechlorination-hydroxylation processes. The present study indicates the novel Cysteine/Fe 3 O 4 /Persulfate process might be a high potential for treatment of organic polluted water.
研究领域:
环境科学
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化学工程
·
水处理
·
污染物降解
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2016
·
IF 5.31
Jingchun Yan,Weiguo Gao,Mingang Dong,Lu Han,Linbo Qian,C. Paul Nathanail,Mengfang Chen
A reduced graphene oxide (rGO) supported magnetite nanoparticle (nFe 3 O 4 ) composite (nFe 3 O 4 /rGO) was synthesized and shown for the first time to be an efficient persulfate activator to generate SO 4 − for trichloroethylene (TCE) degradation. The degradation efficiency of TCE (0.15 mmol L −1 ) was 98.6% within 5 min in the presence of 6.94 g L −1 nFe 3 O 4 /rGO with an optimum mass ratio of 1:4 and persulfate concentration of 3.0 mmol L −1 . By dispersing nFe 3 O 4 on the rGO surface, nanoparticle agglomeration was prevented and the aggregation of the rGO sheets was disrupted. Both the redox effect coupled in nFe 3 O 4 and the electron transfer by functional groups containing oxygen on the surface of rGO enhanced the SO 4 − generation. Given the identified free radical species and the characterization of the nFe 3 O 4 /rGO, a persulfate activation mechanism by nFe 3 O 4 /rGO for the degradation of TCE was interpreted.
研究领域:
环境科学
·
化学工程
·
材料科学
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Ruijun Zhang,Wenqian Zhu,Jiayu Tian,Shanshan Gao,Bart Van der Bruggen
Reverse osmosis is an effective seawater desalination way extending the available sources of fresh water, but challenged by the gypsum scaling. Herein, D (+)-glucosamine (DGA) was rationally selected and utilized to prepare a novel polyesteramide (PEA) NF membrane that can reject SO 4 2− but release Ca 2+ . Then it was employed in the pretreatment of seawater reverse osmosis to spatially isolate SO 4 2− and Ca 2+ , thus removing the “foundation” for forming gypsum. Compared to the referenced NF270, the optimized sample denoted as DGA-PEA-NF has a looser structure with stronger negative charge, as well as a higher resistance to both organic fouling and chlorine attack. During the pretreatment of seawater, both the water permeability and SO4 2− /Ca 2+ selectivity of the DGA-PEA-NF membrane were much higher than those of NF270; the seawater permeance and SO 4 2− /Ca 2+ selectivity of DGA-PEA-NF were 10.25 L m −2 ·h −1 ·bar −1 and 7.62, respectively, while those of NF270 were only 5.11 L m −2 ·h −1 ·bar −1 and 2.08. Consequently, the DGA-PEA-NF membrane effectively reduced the gypsum scaling both in NF and RO stages rather than just transferring the fouling problem forwards to NF stage. The implementation of this research is expected to provide guidance for a targeted fabrication of NF membranes, as well as support for the sustainable development of seawater desalination.
研究领域:
材料科学
·
环境工程
·
水处理
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DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Yixin Huang,Jing Zou,Jinbin Lin,Haoyu Yang,Mengyun Wang,Jiawen Li,Wei Cao,Baoling Yuan,Jun Ma
The activation of peroxydisulfate (PDS) by organic compounds has attracted increasing attention. However, some inherent drawbacks including quick activator decomposition and poor anti-interference capacity limited the application of organic compound-activated PDS. It was interestingly found that 2,2′-azino-bis (3-ethylbenzothiazoline-6-sulfonate) (ABTS) could act as both activator and electron shuttle for PDS activation to enhance diclofenac (DCF) degradation over a pH range of 2.0–11.0. Multiple reactive species of ABTS•+, •OH, and SO4•– were generated in the PDS/ABTS system, while only ABTS•+ and •OH directly contributed to DCF degradation. ABTS•+, generated via the reactions of ABTS with PDS, SO4•–, and •OH, was the dominant reactive species of DCF degradation. No significant decomposition of ABTS was observed in the PDS/ABTS system, and ABTS acted as both activator and electron shuttle. Four possible degradation pathways of DCF were proposed, and the toxicity of DCF decreased after treatment with the PDS/ABTS system. The PDS/ABTS system had good anti-interference capacity to common natural water constituents. Additionally, ABTS was encapsulated into cellulose to obtain ABTS@Ce beads, and the PDS/ABTS@Ce system possessed excellent performance on DCF degradation. This study proposes a new perspective to reconsider the mechanism of activating PDS with organic compounds and highlights the considerable contribution of organic radicals on contaminant removal.
研究领域:
环境科学
·
污染控制
·
化学工程
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DOI
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2017
·Vol. 43
·期 7
·3961-3974
·
IF 1.369
Jiao Yinchun,Zhu Man,Deng Renjie,Jian Jian,Yin Yi,You Kuiyi
With the increase in environmental awareness, developing a highly efficient and environmentally benign nitration process has very important academic and applied industrial values in the synthesis of nitro-compounds. Towards this goal, we have developed an efficient and environmentally friendly approach for solvent-free liquid phase nitration of toluene by employing NO 2 as a nitrating agent and sulfated SO 4
2− /WO 3 as a catalyst replacing traditional nitric acid–sulfuric acid under mild conditions. The results indicate that SO 4
2− /WO 3 as an effective and eco-friendly catalyst exhibits excellent catalytic activity and reusability for the nitration of toluene with NO 2 . In addition, the possible pathway for liquid phase nitration of toluene with NO 2 over sulfated SO 4
2− /WO 3 catalyst was suggested. The present method makes this nitration process safe and environmentally friendly, and has the potential to enable a sustainable production of nitro-compounds from the liquid phase nitration of aromatic hydrocarbon with NO 2 in industrial applications.
研究领域:
催化化学
·
绿色化学
·
有机合成
·
环境友好工艺
·
工业化学
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DOI
高影响因子
Science Bulletin
·
2023
·
IF 18.9
Along Zhao,Fangjie Ji,Changyu Liu,Shihao Zhang,Kean Chen,Weihua Chen,Xiangming Feng,Faping Zhong,Xinping Ai,Hanxi Yang,Yongjin Fang,Yuliang Cao
Fe-based polyanionic sulfate materials are one of the most promising candidates for large-scale applications in sodium-ion batteries due to their low cost and excellent electrochemical performance. Although great achievements have been gained on a series of Na 6−2 x Fe x (SO 4 ) 3 (NFSO- x , 1.5 ≤ x ≤ 2.0) materials such as Na 2 Fe 2 (SO 4 ) 3 , Na 2 Fe 1.5 (SO 4 ) 3 , and Na 2.4 Fe 1.8 (SO 4 ) 3 for sodium storage, the phase and structure characteristics on these NFSO- x are still controversial, making it difficult to achieve phase-pure materials with optimal electrochemical properties. Herein, six NFSO- x samples with varied x are investigated via both experimental methods and density functional theory calculations to analyze the phase and structure properties. It reveals that a pure phase exists in the 1.6 ≤ x ≤ 1.7 region of the NFSO- x , and part of Na ions tend to occupy Fe sites to form more stable frameworks. The NFSO-1.7 exhibits the best electrochemical performance among the NFSO- x samples, delivering a high discharge capacity (104.5 mAh g −1 at 0.1 C, close to its theoretical capacity of 105 mAh g −1 ), excellent rate performance (81.5 mAh g −1 at 30 C), and remarkable cycle stability over 10,000 cycles with high-capacity retention of 72.4%. We believe that the results are useful to clarify the phase and structure characteristics of polyanionic materials to promote their application for large-scale energy storage.
研究领域:
材料科学
·
电化学
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yujiao An,Xiaowan Li,Zihao Liu,Zhilan Wang,Xiaoquan Lu
Quinones, widely considered as environmental pollutants in wastewater, have been identified as redox-active substances capable of activating persulfate for decontamination purpose. However, the mechanism of peroxydisulfate (PDS) activation by quinones under alkaline conditions remains elusive. In this study, methyl- p -benzoquinone (MBQ) was chosen as a model quinone to elucidate the intrinsic mechanism of activating PDS. The results showed that MBQ/PDS system can effectively degrade atrazine (ATZ) under alkaline conditions (especially at pH 10.5) and achieve simultaneous removal of MBQ. Derivatization analysis, quenching experiments and electron spin resonance tests revealed that the self-transformation product of MBQ, methyl-semiquinone radical (MSQ − ), played a major role in activating PDS while alkali served as an auxiliary activator. Specifically, MSQ − functioned as a mediator in PDS activation, regulating the generation of sulfate radical (SO 4 − ) and hydroxyl radical ( OH), thereby inducing the degradation of ATZ through free radical pathways. Two degradation pathways of ATZ were proposed based on UPLC-Q-TOF-MS analysis and DFT calculation. ECOSAR evaluation indicated MBQ/PDS system can detoxify ATZ, yet it remains imperative to concern the formation of more toxic by-products. Furthermore, MBQ/PDS system exhibited strong resistance to water matrixes (excluding Cl − ) and favorable degradation capabilities towards diverse contaminants. This work broadened the possibility of applying the persulfate system in actual water bodies with alkaline environments, achieving the dual benefit of degrading target contaminants and simultaneously removing the activator quinones themselves, providing a novel “treating pollution with waste” water treatment strategy.
研究领域:
环境化学
·
水处理
·
污染物降解
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DOI
高影响因子
Energy Technology
·
2024
·
IF 3.6
Dongyin Niu,Tiantian Zhang,Xuedan Zhang,Yufei Tan,Lukai Zhai
Under the background of vigorously promoting clean heating, the introduction of phase-change energy storage technology into heating systems has become a new hot issue. In this study, a novel KAl(SO 4 ) 2 ·12H 2 O/expanded graphite (EG) shape-stabilized composite phase-change material (PCM), with a melting temperature of 91.6 °C, latent heat of 245.7 kJ kg −1 , and high heat conductivity of 2.07 W m −1 K −1 , is prepared to manufacture a PCM-based module for space heating. This phase-change electric heating module is developed, and its heat storage and release characteristics are investigated through experimental and numerical studies. The numerical model is validated by experimental results. In view of the numerical simulation, the structure of the module is optimized and its thermal performance is studied. Based on the optimized module, a peak-valley time-of-use (TOU) electric heating module is finally proposed. It is revealed that the module exhibits good thermal performance and is capable of satisfying the indoor heating demand. The effective heat storage and release duration is 8.12 and 15.34 h, which can perfectly realize the operating mode under the “peak-valley TOU electricity” mechanism. In this study, it is demonstrated that peak–valley electric energy storage heating devices have broad prospects in building space heating and provides reference for future application.
研究领域:
能源工程
·
材料科学
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Tiantian Chen,Zhenyang Yu,Ting Xu,Rong Xiao,Wenhai Chu,Daqiang Yin
Sulfate radical (SO 4 ·- )-based advanced oxidation processes (AOPs) attract increasing attention in the control of micropollutants. However, SO 4 ·- can react with other chemicals present in water and result in undesired oxidation by-products (OBPs) generation. The formation and degradation mechanisms of CX 3 R-type OBPs during cobalt catalyzed peroxymonosulfate (Co 2+ /PMS) oxidation were investigated. In the formation of CX 3 R-type OBPs, both Co 3+ and SO 4 ·- could convert chloride to free chlorine that then reacted with natural organic matter, leading to the formation of CX 3 R-type OBPs. The concentrations of trichloromethane, chloral hydrate, dichloroacetonitrile, dichloroacetamide and trichloroacetamide after 15 min reaction were 9.8, 3.9, 1.2, 5.9 and 22.3 nM, respectively. Compared to SO 4 ·- , Co 3+ played a more significant role in the CX 3 R-type OBP formation and calculated toxicity values of CX 3 R-type OBPs. CX 3 R-type OBPs could not only be formed but also be degraded at the same time during Co 2+ /PMS oxidation. As for the degradation of CX 3 R-type OBPs, both Co 3+ and SO 4 ·- could transform CX 3 R-type OBPs to chloride. Compared to Co 3+ , SO 4 ·- played a more important role in the degradation of CX 3 R-type OBPs and the conversion from chloride to final by-product chlorate. The adverse effects that results from Co 3+ need more attention in SO 4 ·- -based AOPs application.
研究领域:
环境科学
·
化学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）