ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Nan Jia,Ting Yang,Shufeng Shi,Xinbing Chen,Zhongwei An,Yu Chen,Shiwei Yin,Pei Chen
Exploiting efficient electrocatalysts for hydrogen peroxide (H2O2) electroproduction by oxygen reduction reaction (ORR) is highly desired in practical application. Herein, nitrogen- and fluoride-codoped carbon nanocages (NF-Cs) are successfully synthesized through a simple and scalable template method. With the aid of a porous structure, a large surface area, and the introduction of N and F atoms, NF-Cs show excellent electrocatalytic performance for H2O2 electroproduction in alkaline solution (pH 13) with a faradaic efficiency of 89.6% at very positive applied potential (0.74 V). In acid solution (pH 0.35), the faradaic efficiency of H2O2 electroproduction stably maintains at 85%–88% in the range of 0.4–0.72 V potential. The experimental and theoretical results reveal that the strong synergistic effect between the doped N and F atoms facilitate the H2O2 electroproduction through 2e ORR. That is, the doped N atoms promote O2 molecule adsorption on the catalyst surface, and the F atoms facilitate the desorption of the *OOH intermediate, which is the key factor for the NF-Cs efficiently catalyzing H2O2 electroproduction. These results provide beneficial references for reasonably designing effective carbon-based electrocatalysts for H2O2 electroproduction.
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高影响因子
ACS Omega
·
2020
·
IF 2.87
Ning Song,Shao-Peng Chen,Xiao-Wei Fan,Yu-Hui Tan,Wen-Juan Wei,Yun-Zhi Tang
The molecular design and regulation has shown bright future for constructing smart molecular materials such as ferroelectrics, dielectric switches, electro-optic effect, and so forth. Here, by poly-H/F substitution in a simple organic-inorganic hybrid 2[CH2FCH2NH3]·[CdCl4], 1 (CH2FCH2NH3 = fluorine ethylamine cation), we obtained two novel hybrids, namely, 2[CHF2CH2NH3]·[CdCl4], 2 (CHF2CH2NH3 = 2,2′-difluorine ethylamine cation) and 2[CF3CH2NH3]·[CdCl4], 3 (CF3CH2NH3 = 2,2′,2″-trifluorine ethylamine cation). Further investigations show that compounds 1, 2, and 3 experience solid reversible phase transitions with temperatures at 294, 319, and 329 K respectively. These unique phase transitions were confirmed by their remarkable dielectric and heat anomalies around the phase transition temperatures. X-ray single-crystal diffraction analyses before and after the phase transitions show that the order–disorder motions of F atoms and the twist motions from the 2D [CdCl4]2– framework lead to these solid reversible phase transitions. Also, the Hirshfeld surface calculation of compounds 1, 2, and 3 suggests that the increasing ratio of the F···F interaction from the intermolecular interaction makes a major contribution for the substantial increase of their phase transition temperatures.
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PubMed
高影响因子
MICROCHEMICAL JOURNAL
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2019
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IF 3.206
Dan Li,Chongning Li,Aihui Liang,Zhiliang Jiang
Fluoride constitutes an essential component for the formation of hard bones and teeth. However long-term excessive intake of fluoride causes chronic poisoning changes in the body. Therefore, the determination of its content is of great significance. Herein, a sensitive SERS quantitative analysis method was proposed to detect F − . Trace Fe 3+ exhibited strong catalysis of H 2 O 2 oxidizing 3, 3′, 5, 5′-tetramethylbenzidine (TMB) under the ultrasonic irradiation, and the reaction product called TMB diimine (TMB OX ) not only had strong fluorescence, but also had SERS activity in the silver nanosol substrate. Upon addition of fluoride ion (F − ), the stable complex of [FeF 6 ] 3− formed, and could inhibit the catalytic action of Fe 3+ , resulting in the SERS and fluorescence signal decreasing due to the TMB OX concentration decreasing. In the range of 2–1000 nmol/L F − , the SERS intensity Δ I decreased line with the concentration increased, with a detection limit of 0.7 nmol/L. Based on the catalytic amplifying strategy and the TMB OX molecular probes, ultratrace Fe 3+ could be also detected by SERS and fluorescence methods.
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Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 20
·7924-7929
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IF 8.262
Syed Comail Abbas,Kui Ding,Qin Liu,Yiyin Huang,Yakun Bu,Jing Wu,Jiangquan Lv,Muhammad Arsalan Ghausi,Yaobing Wang
The development of efficient oxygen reduction reaction (ORR) electrocatalysts composed of low cost and earth abundant elements is imperative for several energy systems. It has been reported that metal-free co-doped materials play a key role in the oxygen reduction reactions. However, a Si/F co-doped material has never been considered as an electrocatalyst for the ORR. Herein, we report a Si–C–F decorated three-dimensional porous carbon material by a facile pyrolysis of a mixture of D-glucose, ammonium fluoride and SiO2 nanoparticles in an argon atmosphere. It shows an excellent electrocatalytic performance with an onset potential of E = 0.24 V and a limiting current density of I = 4.5 mA cm−2 which is better than that of traditional electrocatalysts under neutral conditions. This outstanding electrocatalytic performance is due to the synergistic effect of silicon and fluorine which causes a change in the charge distribution and energetic characteristics of the Si–C–F decorated porous carbon material. For the practical application, a microbial fuel cell equipped with this electrocatalyst as the cathode reveals a high maximum power output and open circuit voltage (1026 mW m−2 and 780 mV), which are higher than those of commercial 20% Pt/C catalysts (913 mW m−2 and 750 mV).
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JOURNAL OF HAZARDOUS MATERIALS
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2024
·
IF 12.2
Han Zhang,Yinyin Zhang,Luxiang Zhu,Yanan Liu
The frequent detection of 6:2 chlorinated polyfluorinated ether sulfonate (F-53B) in various environments has raised concerns owing to its comparable or even higher environmental persistence and toxicity than perfluorooctane sulfonate (PFOS). This study investigated the plasma degradation of F-53B for the first time using a water film plasma discharge system. The results revealed that F-53B demonstrated a higher rate constant but similar defluorination compared to PFOS, which could be ascribed to the introduction of the chlorine atom . Successful elimination (94.8–100 %) was attained at F-53B initial concentrations between 0.5 and 10 mg/L, with energy yields varying from 15.1 to 84.5 mg/kWh. The mechanistic exploration suggested that the decomposition of F-53B mainly occurred at the gas-liquid interface, where it directly reacted with reactive species generated by gas discharge . F-53B degradation pathways involving dechlorination , desulfonation , carboxylation , C-O bond cleavage , and stepwise CF 2 elimination were proposed based on the identified byproducts and theoretical calculations. Furthermore, the demonstrated effectiveness in removing F-53B in various coexisting ions and water matrices highlighted the robust anti-interference ability of the treatment process. These findings provide mechanistic insights into the plasma degradation of F-53B, showcasing the potential of plasma processes for eliminating PFAS alternatives in water.
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高影响因子
Journal of Water Process Engineering
·
2024
·
IF 6.3
Yanan Liu,Guangyan Wang,Shuaishuai Lu,Siqi Wang,Peijuan Jiang,Huan Chen,Fang Jiang
Pollution caused by per - and polyfluoroalkyl substances (PFASs) has raised global health concerns and there is an urgent need for researchers to find effective treatment methods. The covalent triazine framework (CTF) adsorbent materials with different structures based on various precursors using the ionothermal method were prepared and characterized in this study. Among them, F-doped CTF (F-CTF) is favorable for effective mass transfer in the adsorption process due to its rich microporous structure and large specific surface area. The maximum adsorption capacity (q max ) for PFOA reached 769.2 mg/g under the synergistic effect of electrostatic force and the interaction of F F. After six cycles of adsorption-desorption experiments, the adsorption and desorption rates of the F-CTF 400°C were stable at >90 %. This result indicates that F-CTF 400°C possesses high stability and recyclability. Furthermore, the desorption solution containing a high concentration of PFOA was treated directly by a UV/Na 2 SO 3 system, utilizing the e aq − within the system to decompose PFOA. The reduction and defluorination efficiencies for the desorption solution with high concentrations of PFOA reached 90 % and 40 %, respectively. The study results indicate that by leveraging the high adsorption selectivity and stable recoverability of F-CTF 400°C , the UV/Na 2 SO 3 system can completely remove PFOA. This approach offers a novel solution for the elimination of PFOA pollution in the environment.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yiwei Sun,Xiaoli Wei,Fangcao Liu,Bing Liu,Jiaming Zhao,Yubao Bi,Wenfeng Han
Developing effective techniques to produce and stabilize highly active metastable F-Al-O species in HFCs dehydrofluorination system without being over-fluorinated to Al-F is a major challenge. Herein, we report a new strategy for the formation and stabilization of metastable species. Using NaH 2 PO 4 as a P source, phosphoric acid groups are modified to the surface of Al 2 O 3 leading to the fabrication of AlPO 4 /Al 2 O 3 interface. P and Al 2 O 3 bond to form Al-O-P structure at the interface and stabilize F-Al-O in the dehydrofluorination system. Further studies show that AlPO 4 /Al 2 O 3 interface increase the oxygen vacancy content of catalyst and accelerate the conversion of HFC-152a on the catalyst surface. Meanwhile, AlPO 4 /Al 2 O 3 interface improves the surface acidity of Al 2 O 3 , endue a large number of Lewis weak acid sites, reducing the carbon accumulation of catalyst, and improving the stability of catalyst. The activity test showed that AlPO 4 /Al 2 O 3 interface shows high catalytic performance (74.2 %) and excellent stability (50 h) for 1,1-difluoroethane dehydrogenation compared with Al 2 O 3 (30 % and low stability) without P modification.
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AQUATIC TOXICOLOGY
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2024
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IF 4.1
Peining Cai,Qi Li,Shuhui Wang,Liju Tan,Jiangtao Wang
A large number of nanoparticles are produced and enter the aquatic environment, where they interact with each other, posing a potential threat to aquatic organisms. The toxicity of two types of nanoparticles (nCu and nSiO 2 ) on Nitzschia closterium f. minutissima (N. closterium f. minutissima ) was investigated in this study by examining changes in microalgal cell density, instantaneous fluorescence rate (Ft), and a range of antioxidant parameters in the cells. It was found that both nCu and nSiO 2 showed time- and concentration-dependent toxic effects on N. closterium f. minutissima . nSiO 2 could promote microalgae growth at low concentrations by providing Si, an essential element for the synthesis of siliceous shells. As the exposure time increased, both the growth and photosynthetic efficiency of the microalgae were inhibited. Nanoparticles also produced oxidative stress and caused lipid peroxidation in the microalgae. In the meantime, SOD and CAT activity were altered to protect cells from oxidative damage. Inverted biomicroscopy images showed that the microalgae enhanced their cell size to adapt to the environmental stress as exposed to 1 mg/L nCu. Scanning electron microscope (SEM) images showed that 10 mg/L nSiO 2 could adsorb nCu and reduce the toxic effect of nCu on the microalgae, while 30 mg/L nSiO 2 caused mechanical damage to microalgal cells and accelerated the internalization of nanoparticles and Cu 2+ in the cells.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Shaojin Jia,Sha Yang,Yu Pan,Salah Ud Din,Yuanjie Cai
As an important part of the fields such as renewable energy and electric vehicles, electrochemical energy storage technology faces significant challenges in improving energy density , extending battery life and improving safety. We successfully prepared a composite battery separator of polyvinylidene fluoride-chlorotrifluorinylene (PVDF-CTFE) and fluorinated polyimide (F-PI) -based materials, mixed it with different contents of boehmite nanoparticles , and then modified it by different doses of electron beam irradiation to improve the performance, especially to overcome the problem of maintaining capacity decline in high-speed charging environment. The results showed that the prepared battery separators exhibited outstanding thermal stability, electrochemical properties and ionic conductivity with 12 % boehmite nanoparticles . After 1000 high-speed charge and discharge cycles in current density of 10C, the battery based on the modified separator still maintained a capacity retention rate of 84.4 %, with the initial discharge specific capacity of 111.9 mAhg −1 . This means that irradiated separators not only maintain a high energy density in a high-speed charging environment, but also overcome the problem of maintaining capacity decline. Electron beam irradiation further improved the comprehensive performance of the separator. After 1000 and 1500 cycles at the current density of 10C and 15C, the specific discharge capacity of the battery can still retain more than 90 % and 80 % of the initial specific discharge capacity, which provides a longer life in practical applications.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2024
·Vol. 31
·期 29
·42075-42087
·
IF 0
Zhang Qian,Lan Xin-yue,Huang Zhi,Liu Yan-ying,Hong Jun-ming
Highly active catalysts with salt and acid/alkali resistance are desired in peroxymonosulfate (PMS) activation processes and marine environment applications. F- and Cl-doped graphene (F-GN and Cl-GN) were prepared via electronegative and atom radius adjustment for tetracycline hydrochloride (TCH) pollution removal to satisfy these requirements. The introduction of special F and Cl functionalities into graphene exhibits superior electron transfer properties for PMS activation, considering the experimental and density functional theory (DFT) calculation results. The TCH degradation efficiency reached up to 80% under various pH and salt disturbance conditions with F-GN and Cl-GN. Cl-GN exhibited an activity superior to F-GN due to the higher electron polarization effect of C atoms adjacent to Cl atoms. The presence of more positive charged C sites in Cl-GN (around Cl doping) is more favorable for PMS attachment and sequence radical generation than F-GN. In addition, the main active species functionalized during reaction included ·OH and SO 4 − ·, and the stability of F-GN and Cl-GN was confirmed to be over 60% by recycle test. Final research results provide an effective strategy for designing and preparing PMS activators resistant to salt, acid, and alkali, thereby expanding their application potential.
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Journal of Materials Chemistry C
·
2024
·
IF 5.7
Jinwen Tan,Han Luo,Shiyi Wang,Ling Huang,Liling Cao,Xuehua Dong,Guohong Zou
A short-wave UV antimony(III) oxysalt, RbSb(SO4)(H2PO2)F, by incorporating three different anions (SO42-, H2PO2-, F-) with trivalent antimony cations that possess stereochemically active lone-pair electrons (SCALP), has been successfully synthesized. Significantly, the mixed anions and Sb3+ cations combine to form a low-dimensional 1D infinite anionic chain, denoted as [Sb(SO4)(H2PO2)F]∞-, where synergistic interactions among these units contribute to a substantial birefringence of 0.192 at 546 nm and achieve a short cutoff edge down to 276 nm. This research expands the family of UV birefringent optical materials and provides guidance for the further exploration of novel structural-functional materials.
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高影响因子
VACUUM
·
2024
·
IF 3.8
Zuhong Ji,Yunfei Sun,Xiaodong Guan,Yang Zhou,Junchao Qian,Feng Chen
In this work, the La substitution of iron and replacing the oxygen with fluorine are both adopted to expectantly enhance the rate performance and structure stability of LiFePO 4 during working. The characterizations of X-ray diffraction, scanning electron microscope , transmission electron microscope, charging-discharging tests, electrochemical impedance spectroscopy and safety tests are used to investigate the influences of La 3+ and F − doping on the LiFePO 4 . The results indicate the cathodes after La 3+ doping not only deliver the larger lattice parameters and unit cell volume to broaden the lithium ions migration pathway and accelerate the Li + diffusion speed, but also strengthen the whole bond energy of LiFePO 4 owing to the high bond energy of La–O. In addition, the F replacement of O could increase the length of Li–O bonds and decrease the length of P–O bonds, further be helpful to enhance the Li + diffusion between LiFePO 4 phase and FePO 4 phase due to the weakening of Li–O bonds. Finally, the La 3+ and F − co-doped cathode delivers the superior discharge capacity of 139.3 mAh g −1 at 5C high rate and 127.2 mAh g −1 at −20 °C, with the high discharging capacity of 160.1 mAh g −1 after 100 cycles at 45 °C.
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