CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Zichen Zhang,Hengjun Gai,Qun Li,Bingxiao Feng,Meng Xiao,Tingting Huang,Hongbing Song
In this work, N-rich ionic liquid based on 1,3,5-triimidazole triazine was used to construct poly(ionic liquid) (PIL) through free radical polymerization, and support palladium nanoparticles (Pd NPs), which were used in the catalytic hydrogenation of nitrobenzene. The resulting N-rich PIL had a good dispersion effect and ultrafine Pd NPs as shown by SEM and TEM, thereby significantly enhancing the stability of the loaded metal NPs. The XPS results indicated that the metal-support interaction improved the catalytic performance of the catalyst. In particular, the effects of different anions (Tf 2 N - , PF 6 - , and Cl - ) on the PILs were investigated, and the results showed that the Tf 2 N anion exhibited the best catalytic effect on the hydrogenation of nitrobenzene. Furthermore, density functional theory calculation confirmed that anions played a key role in activating the substrate in the hydrogenation of nitrobenzene. The corresponding results were consistent with the experimental results, which provided reference and research for the application of PILs in the future.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Yunjin Yao,Huanhuan Hu,Hongda Zheng,Hongwei Hu,Yinghao Tang,Xiaoyan Liu,Shaobin Wang
Bimetallic Fe- and Mo-embedded N-enriched porous biochar (Fe-Mo@N-BC) is developed and serves as a cost-effective and highly efficient catalyst for mineralization of non-biodegradation organic contaminants . Fe-Mo@N-BC was prepared by pyrolysis of complex Fe/Mo -containing precursors. Transmission electron microscopy and elemental mapping suggested that Fe and Mo are uniformly dispersed in nitrogen-doped biochar with hierarchical mesopores . In comparison to Fe@N-BC and Mo@N-BC, Fe-Mo@N-BC exhibited a superior activity for activating peroxymonosulfate (PMS). The stable activity was ascribed to N-doping and synergistic effect of Fe and Mo species, where both Fe-N x and Mo-N x can simultaneously serve as the active sites and N-BC can act as a carrier and an activator as well as an electron mediator. Electron paramagnetic resonance and quenching experiments indicated that H O • , O 2 • − and 1 O 2 were responsible for organic degradation . The effects of PMS dosage, initial Orange II concentration, temperature, solution pH, coexisting anions and humic acids on organic degradation were also investigated. With the assistance of an external magnet, Fe-Mo@N-BC can be easily separated after reaction and remains stable in the reusability tests. This work demonstrates a feasible strategy towards the fabrication of Fe, Mo-embedded N-enriched porous biochar catalysts for the detoxification of organic contaminants.
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POLYMER DEGRADATION AND STABILITY
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2021
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IF 5.03
Chao Wan,Huajun Duan,Chenhao Zhang,Jianfan Cao,Jiahao Zou,Junjun Zhang,Huiru Ma
In order to obtain an efficient flame retardant without sacrificing mechanical properties and transparency of epoxy resin (EP), a P/N/S-containing flame retardant (STP) by combining 9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide (DOPO) with Schiff base intermediate synthesized by the reaction of sulfathiazole and 2-thenaldehyde was successfully synthesized. The synthesis of STP was verified and the properties of modified EP were studied. The test results indicated that STP slowed down the degradation rate of EP. The glass transition temperature (T g ) of the flame-retardant epoxy resin (FREP) samples were well maintained and even improved after introducing a certain amount of STP. Furthermore, FREP with low phosphorus content exerted excellent flame retardant ability, EP/5%STP (phosphorus content: 0.27 wt%) obtained the V-0 rating of UL-94 test with the value of limiting oxygen index (LOI) 33.5%. In contrast with EP, the peak heat release rate (PHRR), total heat release (THR) and total smoke production (TSP) of EP/7.5%STP were respectively decreased by 33.31%, 26.04% and 28.75%. Mechanical performance tests show that STP improved the tensile and flexural strength of EP. It is worth mentioning that the EP modified with STP still maintains good transparency.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Shizong Wang,Jianlong Wang
In this study, cobalt embedded into oxygen and nitrogen co-doped CNTs (Co@N-O-CNTs) was prepared by pyrolysis and used to activate peroxymonosulfate (PMS) for degradation of sulfamethoxazole. The experimental results showed that the content of oxygen precursor had important influence on the catalytic activity of Co@N-O-CNTs. When the content of oxygen precursor was 2 g, Co@N-O-CNTs exhibited better catalytic activity than previously reported Co@N-CNTs. Bulk and surface-bound radicals resulted in sulfamethoxazole (SMX) degradation, in which SMX degradation rate reached 0.247 min −1 with the mineralization of 35.6%. The possible pathway of SMX degradation was proposed based on the identified degradation products. Characterization results indicated that nitrogen, oxygen and cobalt in the structure of Co@N-O-CNTs-2 were active sites for PMS activation. Theoretical calculation suggested that nitrogen and oxygen co-doping created more active sites to activate PMS compared with single nitrogen doping. During the six cycling experiments, Co@N-O-CNTs-2 exhibited good catalytic and structural stability. The influencing factors, including temperature, pH, PMS concentration, chloridion, bicarbonate and humic acids were investigated. This study could provide a way to boost active sites of nitrogen doped carbonaceous materials to effectively activate PMS for degradation of emerging organic pollutants.
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Inorganic Chemistry Frontiers
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2021
·Vol. 8
·期 18
·4282-4290
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IF 6.569
Qianliang Zhang,Baojuan Xi,Shenglin Xiong,Yitai Qian
SiO based materials have attracted attention as promising anodes for lithium-ion batteries (LIBs) with high energy density. However, severe volume variation and poor conductivity limit the development of SiO based materials. In this study, carbon coated SiO nanoparticles embedded in N-doped carbon nanosheets (SiO@C/CNSs) have been fabricated through simple ball milling followed by annealing treatment, which is facile and scalable. The g-C3N4 precursor plays a multifunctional role as a sacrificial template, nitrogen source for doping, and minor carbon source. The presence of N-doped porous carbon nanosheets could minimize the volume expansion, enhance the reaction kinetics and retain the integrity of the electrode. The SiO@C/CNS anode exhibits a stable reversible capacity of 690 mA h g−1 up to 400 cycles at 1 A g−1 and excellent rate capability. The SiO@C/CNS//LiFePO4 full cell further confirms its potential as a promising anode for high capacity LIBs.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Kristina Maliutina,Jiajia Huang,Tong Su,Jianglong Yu,Liangdong Fan
This work introduces nanostructured carbon-based composite with enriched CNTs and microstructural defects from pomelo peel biomass precursors through successive chemical pretreatment, heteroatom N, S dual-doping and transition metal oxide loading (Ta 2 O y ) and its application for electrochemical oxygen reduction reaction (ORR) at room temperature. During the microwave pyrolysis process, volatile N, S-containing species from trithiocyanuric acid reactant were trapped and doped into carbonaceous biomass precursor to achieving the rich-defect porous nanotubes and abundant cavity structure. The effect of biomass pretreatment on the textural and structural properties of biochar and formed CNTs were systematically investigated. The impacts of single doping (N) using melamine and dual-doping (N, S) with trithiocyanuric acid on the structural and electrochemical characteristics of biochar were evaluated. An optimized PP-NS-600-Ta-900 electrocatalyst displayed remarkable ORR activity with a half-wave potential of 0.82 V (vs. RHE), a limiting current density of −5.75 mA cm −2 and an electron transfer number of 3.85. The results offer a useful archetypical template to design and construct reliable CNTs enriched biomass-derived biochar for possible electrochemical energy and storage application, illustrating its viability for utilization as ORR electrocatalyst in potential applications, like fuel cells and metal-air batteries.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2021
·Vol. 168
·期 7
·077517
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IF 4.316
Ziyu Zhao,Jialun Luo,Simon Tricard,Jihua Zhao,Qiangming Wang,Jian Fang
The development of effective and accurate catechol (CC) electrochemical sensors is critical for environment and life health perspectives. A facile pyrolysis of 2D bimetallic (Zn/Co) zeolitic imidazolate framework (Zn/Co-ZIF-L) was employed to prepare Zn and Co nanoparticles encapsulated in N-doped porous carbon (Zn/Co@NPC). Prussian blue (PB) was synthesized in situ via the co-precipitation of ferricyanide ([Fe(CN)6]3−) and iron (II) ion originated from the reduction of Fe3+ by Zn/Co@NPC and then served as the main active substance of CC detection. The morphology and composition of the final composite Zn/Co@NPC-PB were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and X-ray powder diffraction (XRD). The Zn/Co@NPC-PB modified glass carbon electrode (GCE) exhibits two concentration linear ranges of 4.13 μM − 1.08 mM (R2 = 0.999) and 1.08 mM−11.82 mM (R2 = 0.999) for CC electrochemical detection with a limit of detection 1.05 μM (S/N = 3). At the same time, the Zn/Co@NPC-PB/GCE shows great selectivity to electrochemical oxidation behavior of CC in presence of 20 folds dihydroxybenzene interferents such as hydroquinone and resorcinol. Furthermore, it showed a long-term stability and near 100% recovery for the detection of a real sample in Yellow River water.
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ENVIRONMENTAL TECHNOLOGY
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2021
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IF 3.247
Yangyang Wang,Wenhao Zhan,Yidan Liu,Shanshan Cheng,Chaosheng Zhang,Jianhua Ma,Runhua Chen
Di-n-octyl phthalate (DOP), a plasticizer used in many different industrial products, is a frequently observed pollutant in the environment. Biodegradation by microorganisms is considered to be a realistic choice for the remediation of DOP contamination. In the present research, the halotolerant bacterial consortium (LF) enriched in our previous research was used to degrade DOP. It was found that the optimal conditions for LF to degrade DOP was temperature 30oC, pH 6.0, inoculum size >5%, and salt content <3%. LF could degrade a high concentration of DOP (2000 mg/L) with the removal efficiency of 96.33%. Substrate inhibition analyses indicated that the inhibition constant, maximum specific degradation rate and half-saturation constant were 2544.6 mg/L, 0.7 d−1 and 59.1 mg/L, respectively. Based on the analysis of the gas chromatography-mass spectrometry (GC-MS), the biodegradation pathway for DOP by LF was proposed. Furthermore, LF could degrade DOP in soil (100 mg/kg) with the highest removal efficiency of 89.3%. This study is the first report on DOP biodegradation by bacterial consortium. These results suggest that LF can be used to remediate DOP-contaminated environment.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Yanling Chen,Xue Bai,Yetong Ji,Ting Shen
A novel reduced graphene oxide-supported hollow Co 3 O 4 @N-doped porous carbon (Co 3 O 4 @NPC/rGO) composite was synthesized via self-assembly and pyrolysis-oxidation using bimetallic zeolite imidazolate frameworks and graphene oxide as precursors. The as-obtained composite exhibited superior performance on peroxymonosulfate (PMS) activation over a wide pH range. Complete removal of sulfamethoxazole (SMX, 25 mg·L −1 ) was achieved within 5 min and the reaction rate constant was higher than those of the most reported heterogeneous catalyst/PMS systems for SMX degradation. It was demonstrated that both radical pathways (SO 4 − , OH, and O 2 − ) and non-radical pathways ( 1 O 2 and direct electron transfer) were involved in the SMX degradation. Significantly, the contribution ratio of each reactive oxidative species (ROS) in the bulk solution or on the catalyst surface was differentiated and calculated for the first time. SO 4 − both in the bulk solution and on the catalyst surface as well as the 1 O 2 in the bulk solution were the dominant ROS. The possible degradation mechanism of SMX by Co 3 O 4 @NPC/rGO/PMS system was proposed. Co active sites with high activity, the electron-rich ketonic group and the nitrogen doping sites within Co 3 O 4 @NPC/rGO contributed to the excellent catalytic activity. The ecotoxicity of SMX and its intermediates was investigated. Besides, the reusability, stability and application potential in actual waterbodies of Co 3 O 4 @NPC/rGO were evaluated. Overall, this work expands the environmental application of metal–organic frameworks (MOFs)-derived hollow nanomaterials and provides a promising heterogeneous catalyst for the elimination of refractory contaminants by sulfate radical-based advanced oxidation processes (SR-AOPs).
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FOOD CHEMISTRY
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2021
·
IF 7.514
Yingying Hu,Rentian Guan,Shuai Zhang,Xiaoyu Fan,Wenjing Liu,Keying Zhang,Xiaodong Shao,Xia Li,Qiaoli Yue
A convenient fluorescence sensor of tetracycline (TC) was constructed based on carbon dots (CDs) and polyvinyl alcohol (PVA) hydrogel film. The immobilization of CDs in PVA carrier can stabilize the fluorescence of CDs by inhibiting the fluorescence quench due to the aggregation of CDs with time. CDs were prepared by a hydrothermal method. CDs showed bright blue fluorescence with the quantum yield of 0.35. The fluorescence of CDs was quenched by TC owing to the inner filter effect. The linear range for TC detection was 0–350 µM and the limit of detection was 0.17 µM. To test conveniently, PVA film was employed to upload CDs. Therefore, a novel sensor for TC was constructed in a visual mode. By comparison with the most of previous works, the present method displayed higher sensitivity and better selectivity. The results suggest that the present sensor has potential applications in the real-time detection of TC in food analysis.
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Energy & Environmental Science
·
2019
·Vol. 13
·期 1
·221-228
·
IF 33.25
Bin Liu,Shijia Feng,Lifei Yang,Chengcheng Li,Zhibin Luo,Tuo Wang,Jinlong Gong
Silicon-based (Si-based) junctions have been widely investigated in recent years as photoelectrochemical (PEC) water splitting photoelectrodes, including buried junctions and metal–insulator–semiconductor (MIS) Schottky junctions. However, Si-based MIS photoelectrodes suffer from low performance for the PEC oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) because of the dilemma that a thin insulator cannot provide enough interfacial passivation while a thick insulator will block the transport of charge carriers. Another trade-off is the fact that the photovoltage extracted from the band offset between the metal and semiconductor will be counteracted by the parasitic light absorption of the metal layer, sacrificing the saturation photocurrent. This paper describes the design and realization of a bifacial passivation strategy for the metal/Si interface of an MIS photoelectrode, featuring a bi-layer stack consisting of amorphous silicon (a-Si) for passivating the silicon surface and a metal oxide (TiO2) for passivating the metal surface. Upon the bifacial passivation of both a-Si and TiO2, the minority carrier lifetime of the Si MIS photoanode was significantly improved from 18 to 2360 μs. Enabled by this extremely long minority carrier lifetime, it becomes possible to place the MIS junction on the back side of a Si substrate to construct an inverted-MIS (I-MIS) structure to eliminate the parasitic light absorption of traditional Si MIS photoelectrodes. The obtained photoelectrode exhibits an excellent onset potential of 0.85 V and 0.62 V vs. reversible hydrogen electrode (RHE) for the OER and HER, respectively. Eventually, unprecedented applied bias photon-to-current efficiencies (ABPE) of 3.91% and 12.66% were obtained by Si MIS and Si I-MIS, which are the highest among MIS-based photoanodes and photocathodes, with 30 h and 108 h stable operation. When pairing the Si I-MIS photocathode with a BiVO4 photoanode to form a PEC membrane-free tandem cell, an unbiased solar-to-hydrogen conversion efficiency of 1.9% is achieved.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2019
·
IF 5.589
Boyin Yan,Zhiquan Liu,Ying Liu,Rui Huang,Yongpeng Xu,Dongmei Liu,Fuyi Cui,Wenxin Shi
β- N -Methylamino- l -alanine (BMAA), a new cyanobacterial toxin , is found in different aquatic ecosystems worldwide and is to threaten the human nervous system. Therefore, it is important for water plants to develop feasible methods to counter the effects of BMAA. In this study, the removal of BMAA by chlorine, as well as its intermediate products, at different pH values and the mechanism of pH on the removal BMAA were investigated. The results showed that the chlorination of BMAA is in accordance with the second-order kinetics model. The reaction rate of chlorinated BMAA increased with the increase in the concentration of chlorine. The pH of the solution significantly affected the reaction rate. The apparent kinetic constant ( k app ) decreased from 6.00 × 10 3 M − 1 ·min − 1 to 35.5 M − 1 ·min − 1 when the pH increased from 4.5 to 9 in the chlorine concentration of 32.23 μM. It is probable that the species distribution and proportion of BMAA and chlorine at different pH values were the main causes of this phenomenon. Additionally, the chlorination reaction consisted of four elementary reactions and hydrogen ions were beneficial to the reaction. The temperature also affected the reaction rate and the activation energy of the reaction was 16.6 ± 1.99 kJ·M − 1 . A variety of degradation products were detected and the path of degradation was speculated. Chlorination, dechlorination , and decarboxylation were the main processes of oxidative degradation. Furthermore, the composition of the degradation products was the same at different pH values.
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危险品化学品经营许可证（带存储）