Nano Energy
·
2021
·
IF 17.881
Pengju Li,Zhipeng Jiang,Xiaobo Huang,Xing Lu,Jia Xie,Shijie Cheng
Electrolyte additives have an important impact on the cycling stability of sodium metal batteries , but their applications are severely impeded by the poor compatibility with different electrolytes. Herein, rational incorporation of nitro groups on fullerene (C 60 ) cage yields nitrofullerene (C 60 (NO 2 ) 6 ) as an effective additive, which displays high compatibility with different electrolytes and can enable highly reversible and dendrite-free plating/stripping of sodium metal anodes (SMAs). In-situ optical observation of Na electrodeposition confirms a great improvement in the cycling stability of metallic Na anodes with the C 60 (NO 2 ) 6 additive, which not only promotes the formation of stable protective layers on SMAs, but also facilitates the uniform Na deposition and effectively suppresses the Na dendrite growth. As a result, the Na||Na symmetrical cells with C 60 (NO 2 ) 6 show low voltage hysteresis , high rate capability and prolonged cycle life in both carbonate and ether electrolytes. Even at 5 mA cm –2 and 5 mAh cm –2 , the Na||Cu half cells can stably cycle over 450 h in the ether electrolyte. Furthermore, a significantly improved cycling stability of the high loading Na||Na 3 V 2 (PO 4 ) 3 @C (8.7 mg cm –2 ) full cell is achieved in the carbonate electrolyte.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2021
·Vol. 27
·期 41
·10666-10676
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IF 5.236
Peng Zhang,Shaonan Xu,Yan Wang,Wei Zhang,Wenqing Li,Cundi Wei,Peiping Zhang,Shiding Miao
Graphical One man‘s trash is another man‘s treasure : A novel template strategy allows fibrous struvite—a composite Pd/Mg 2 P 2 O 7 with a mesoporous structure and an ultrahigh surface area—to be synthesized from wastewater. The prepared Pd/Mg 2 P 2 O 7 nanowires showed excellent performance in the selective hydrogenation of nitrobenzenes. This strategy provided a new pathway for synthesizing highly efficient catalysts as well as a solution for alleviate eutrophic pollution caused by N- and P-containing substances in wastewater. A highly efficient heterogeneous catalyst Pd/Mg 2 P 2 O 7 was fabricated by combining palladium nanoparticles (PdNPs) and mesoporous Mg 2 P 2 O 7 fibers/rods. Mg 2 P 2 O 7 fibers with ultra-high specific surface area were prepared from struvite as templates, which were synthesized from waste water containing N- and P-containing pollutants. This strategy provided a novel pathway for developing advanced catalysts from eutrophication-polluted water. The composite Pd/Mg 2 P 2 O 7 showed brilliant performance in selective hydrogenation of nitro aromatics to give anilines. As an example of nitrobenzene hydrogenation, the conversion to aniline and selectivity were found to reach almost 100 % at a temperature of T =90 °C and under a pressure of P =2.0 MPa. The superior performance was found to originate from PdNPs, which were boosted by electron transfer afforded by the nanofiber Mg 2 P 2 O 7 supports. The favorable adsorption of withdrawing groups (−NO 2 ) was realized by synergistic effects between Pd and oxygen vacancies provided by pyrolysis of struvite. The catalyst remained stable after cycles of reuse with little degradation in catalytic performance.
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CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Yuhang Chen,Yaheng Zhang,Hongwei Zou,Minglei Li,Gang Wang,Min Peng,Jie Zhang,Zhiyong Tang
Difficult handling the solid catalysts remains one of the pain points in the continuous flow photochemistry. In this work, the gas–liquid-solid segmented flow was employed in the photocatalytic production of azo- compounds (azoxybenzene and azobenzene) from nitrobenzene using graphitic carbon nitride (g-C 3 N 4 ) as solid catalyst. Compared with the batch reactor, the photocatalytic reaction rate was greatly improved in the microreactor, and the reaction time was shortened from 180 min of the batch to 7.5 min for near-full conversion of nitrobenzene. The effects of various reaction parameters (temperature, light source power, catalyst content) in the continuous system were examined, and the reaction kinetic was found in first order. The photocatalytic reaction performance was very sensitive to the gas–liquid-solid segmented flow conditions, which needed to be carefully tuned. With the help of high-speed camera and micro particle image velocimetry (µ-PIV) techniques, it was identified that the increasing inert gas fraction resulted in more stable segmented flow with shorter liquid segments, favoring the reaction rate. With a high gas fraction, the intensity of recirculation in the liquid segments was strengthened by the increasing total flow rate, enhancing the local mass transfer, thereby benefiting the photocatalytic reaction. Overall, the continuous microreactor reached 5.6 times higher productivity per volume (26.1 mmol/h*L) of azo- compounds than the batch reactor under the same conditions. The successful photosynthesis of azo- compounds demonstrated the great potential of the presented gas–liquid-solid segmented flow, and the findings of this work provide useful guidance on its future application in other heterogeneously catalyzed reactions.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Hongchao Li,Zihao Zhao,Jieshu Qian,Bingcai Pan
The catalytic activation of peroxymonosulfate (PMS) is under intensive investigation with potentials as an alternative advanced oxidation process (AOP) in wastewater treatment. Among all catalysts examined, Co(II) exhibits the highest reactivity for the activation of PMS, following the conventional Fenton-like mechanism, in which free radicals (i.e., sulfate radicals and hydroxyl radicals) are reckoned as the reactive species. Herein, we report that the primary reactive species (PRS) is proposed to be a Co(II)–PMS complex (Co(II)–OOSO3–), while free radicals and Co(III) species act as the secondary reactive species (SRS) that play a minor role in the Co(II)/PMS process. This Co(II)–OOSO3– exhibits several intriguing properties including ability to conduct both one-electron-transfer and oxygen-atom-transfer reactions with selected molecules, both nucleophilic and electrophilic in nature, and strongly pH-dependent reactivity. This study provides novel insights into the chemical nature of the Co(II)-catalyzed PMS activation process.
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CHEMOSPHERE
·
2021
·
IF 7.086
Qimao Gan,Yangyi Xiao,Chenxing Li,Huan Peng,Tuqiao Zhang,Miaomiao Ye
Currently, seawater desalination based on air-water interface solar heating has triggered significant research interests because it effectively makes use of the solar energy and avoids fossil fuel consumption. However, to prevent the volatile organic compounds (VOCs) from volatilizing with water vapor which later will liquefy and enter the condensed freshwater is still a challenge. In this work, a g-C 3 N 4 /MoS 2 based floating solar still (CM-FSS) combined with thermal/light activation of persulfate (PS) at air-water interface was applied for clean freshwater production for the first time. The CM-FSS was composed of a g-C 3 N 4 /MoS 2 top layer for solar absorption, simultaneous thermal/light activation of PS and then VOCs degradation at air-water interface, a floating layer of expandable polyethylene (EPE) foam for heat isolation, and a transport channel of air-laid paper (ALP) for seawater and PS solution delivery. The water evaporation rate of the CM-FSS was measured at 1.23 kg m −2 h −1 under 1 kW m −2 , which is 4.09 times higher than that of pure water without an evaporator. With the assistance of g-C 3 N 4 /MoS 2 photocatalytic degradation and thermal/light activation of PS at the air-water interface, a high removal efficiency of a selected model VOCs pollutant of nitrobenzene (NB) could reach to 98.2% in condensed freshwater. Finally, when real seawater samples were employed as source water for solar distillation, the typical water-quality indices such as salinity , turbidity , anions, cations and organics of the condensed freshwater were below the limit values of the Standards for Drinking Water Quality in WHO, US EPA and China.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Sisi Zhang,Jiayi Zhu,Xiwang Zhang,Runliang Zhu,Fei Ge,Yin Xu
Zero-valent Cu-Fe bimetallic porous carbon materials were successfully applied to remediate organic wastewater. In this work, we successfully recycled the layered double hydroxides (LDHs) adsorbed with Orange II (OII) to form a zero-valent Cu-Fe bimetallic porous carbon material (CuFe/Carbon). The characterization results showed that CuFe/Carbon was a zero-valent Cu-Fe bimetallic porous graphene-like carbon material. In the course of the experiment, we found that aeration condition had a great influence on the activity of CuFe/Carbon. The removal efficiency of nitrobenzene (NB) was 100 % in nitrogen system and 48 % in air system. The active species of O 2 − and O H was formed under air condition, while there was no active species under nitrogen condition. NB was reduced to aniline directly under nitrogen condition. We proposed there were reduction and oxidation mechanisms under different aeration conditions. This work mainly investigated the conversion process of a novel material under different reaction conditions, which provided theoretical support for the removal of organic matters.
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Frontiers in Chemistry
·
2020
·
IF 3.693
Zhang Qianchun,Liang Junyi,Zhao Li,Wang Yan,Zheng Yuguo,Wu Yun,Jiang Li
A novel carbon quantum dots (CQDs) were successfully synthesized by one-step hydrothermal reaction using Rosa roxburghii as a biomass-based precursor. The CQDs have an average size of 2.5 nm and a narrow size distribution. They display strong blue fluorescence with a quantum yield of 24.8% and good biocompatibility. Notably, these CQDs were capable of detecting trace o-nitrophenol in surface water and sewage with high sensitivity and specificity. The linear range is 0.08–40 μmol/L, and the limit of detection is 15.2 nmol/L. Furthermore, this CQDs was successfully applied for o-nitrophenol analysis in river water and sewage samples. Additionally, Hep3B cells, a human hepatocellular carcinoma cell line, can be easily imaged with high resolution using the as-prepared CQDs as nanoprobes. These results reveal that the as-prepared CQDs have potential applications for detecting o-nitrophenol and cell imaging.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Chun Chen,Ruoyu Fan,Miaomiao Han,Xiaoguang Zhu,Yunxia Zhang,Haimin Zhang,Huijun Zhao,Guozhong Wang
A green process for production of imine and secondary-amine with high selectivity is desirable and challenging. Here, selective production of these nitrogen-containing compounds in one-pot was effectively realized in a hydrogenation-coupling tandem reaction system catalyzed by bi-metallic NiCo catalyst. The investigation of Co/Ni composition vs activity showed a composition-dependence catalysis and the optimal bi-metallic catalyst was NiCo 5 (Ni and Co molar ratio 1:5). Nitrobenzene (NB) could almost completely transform toward imine at 70 °C and secondary-amine at 90 °C, respectively. The adsorption configurations of reactant on catalyst surface were analyzed by DFT calculation to probe the reaction mechanism. And the reaction dynamics were also investigated deeply, suggesting that hydrogenation of NB should be promoted but hydrogenation of benzaldehyde (BA) need inhibiting. Additionally, the catalytic system under moderate reaction conditions could also be applied to a variety of substituted aromatic nitro and aldehyde compounds, showing high yields of corresponding imines.
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ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Tian Tao,Yang Zhou,Chaohui He,Hanping He,Mingyu Ma,Zhiwei Cai,Nan Gao,Kai Wang,Ruizhi Zhu,Gang Chang,Zhihua Liu,Yunbin He
The excessive use of pesticides does great harm to environment and human health, a high performance sensor is urgently needed for the management of pesticides contamination. Herein, a novel graphene electrochemical transistor (GECT) for the detection of methyl parathion (MP) was successfully fabricated for the first time. A single layer of graphene was covered between the source and drain electrodes by the wet transfer method to act as channel for the transistor. Au-ZrO 2 nanocomposites were electrodeposited at graphene channel of the device, considering the special affinity of ZrO 2 nanoparticles toward phosphate group and electrocatalytic ability of Au nanoparticles. The sensing mechanism was attributed to the change of carrier concentration in channel induced by the electrochemical reaction of MP at the graphene channel, which built up the mathematic relationship between the change of channel current and the concentration of MP. Different modified materials and electrodeposition conditions were compared and optimized. Due to the high carrier mobility of graphene and excellent catalytic performance of Au-ZrO 2 nanocomposites in the channel, the developed sensor showed a limit of detection as low as 0.1 ng/mL and ultra-wide linear range from 0.4 ng/mL to 7 μg/mL, which are comparable or superior to those using the large-scale instruments. Meanwhile, the device exhibited good selectivity toward usual interferents and high accuracy for detection of MP in Chinese cabbage samples, demonstrating the promising practicality of the devices. It is expected that GECT can act as a desirable transducer platform for highly sensitive and selective detection of pesticides.
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Water
·
2020
·Vol. 12
·期 11
·3150
·
IF 2.544
Jianye Xu,Siqi Zhou,Erdeng Du,Yongjun Sha,Lu Zheng,Mingguo Peng,Ling Ling
The UV/chlorine process, as a new type of AOP (Advanced Oxidation Process), was utilized to treat amlodipine (AML)-containing water. The influencing factors, including chlorine dose, UV intensity, solution initial pH value, and ammonia concentration, were investigated. The degradation of AML in real water and the relative contributions of OH• and Cl• were also studied. Finally, high-resolution mass spectrometry (HRMS) and GC-MS were used to identify the possible degradation products. The results demonstrated that the AML degradation process was fitted with apparent first-order kinetics. AML degradation had a positive correlation with UV intensity and chlorine dose, and a negative correlation with ammonia concentration. In the presence of ammonia nitrogen and DOM, the removal of AML from real water was reduced. OH• made a dominant percentage contribution of 55.7% to the degradation of AML. Sixteen intermediates were detected and identified. A possible degradation mechanism was also proposed. Acute toxicity tests and risk prediction both illustrated that the complete removal of AML does not guarantee the reduction of acute toxicity, but a prolonged degradation promoted the detoxification of toxic intermediates. The UV/chlorine process can be regarded to be an effective method to remove AML and reduce ecological risk.Keywords:Amlodipine;UV/chlorine;influencing factors;degradation products;ecological risk
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DALTON TRANSACTIONS
·
2020
·Vol. 49
·期 48
·17737-17744
·
IF 4.174
Deyi Zhan,Abdul Saeed,Zixuan Li,Chengming Wang,Zhiwu Yu,Junfeng Wang,Nanjing Zhao,Weihong Xu,Jinhuai Liu
Recently, exploring new luminescent metal–organic frameworks (LMOFs) to selectively detect nitro-aromatic compounds (NACs) has been a hot topic of research. Simultaneously, it is still a challenging issue to understand the sensing mechanism of luminescent MOFs interacting with NACs at the molecular level. In this work, highly fluorescent Sc-tetracarboxylate frameworks (Sc-EBTC) have been successfully synthesized through a solvothermal method. The as-prepared Sc-EBTC crystals have good thermal stability, chemical stability as well as strong fluorescence (λex = 320 nm and λem = 400 nm), and they can detect various NACs rapidly (as short as 30 s), selectively and efficiently by the “turn-off” fluorescence mechanism. The detection limits of Sc-EBTC toward 2,4-DNP and 4-NP are quantified to be 5.71 ppb and 6.26 ppb, respectively. Furthermore, to better understand the sensing mechanism, we attempt to use solid-state NMR and X-ray photoelectron spectroscopy to vividly characterize the charge transfer caused by the interaction between NAC molecules and the MOF at the molecular level. Additionally, test strips were made successfully for the practical detection of the NACs. This study demonstrates that the MOF constructed from the H4EBTC ligands might be a promising candidate for the detection of trace NACs.
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ANALYTICAL LETTERS
·
2020
·
IF 1.467
Yunlong Zhang,Ya Ma,Lishi Wang
A polyfurfural film and copper nanoparticle (Cu NP) modified glassy carbon electrode (GCE) was prepared for the electrochemical determination of 2,4,6-trinitrotoluene (TNT). The polyfurfural film and Cu NPs were prepared by a one-step electrochemical polymerization method and a one-step electrochemical deposition method, respectively. In order to obtain the optimum electrochemical performance, the degree of polymerization of furfural, the deposition time and deposition potential of copper, the enrichment time and enrichment potential of TNT detection, and the pH of the detection solution were optimized. Under the optimal experimental conditions, the modified glassy carbon electrode provided significantly enhanced electro-catalytic activity for TNT with a wide linear detection range from 0.05 to 6 ppm and a low detection limit of 0.0416 ppm due to the excellent synergistic catalytic properties of the polyfurfural film and Cu NPs. The electrode also showed excellent anti-interference ability, stability and reproducibility. Moreover, satisfactory results were obtained when the modified electrode was used for the determination of TNT in tap water samples, showing n excellent prospects for practical applications.
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