ACS Applied Energy Materials
·
2019
·
IF 0
Chenyun Zhang,Baohua Zhang,Zhonghao Li,Jingcheng Hao
The genuine active sites toward oxygen evolution reaction (OER) are usually generated via the in situ transformation of initial electrocatalysts during anodic oxidation. In principle, all the catalysts possessing such a transition might be active toward OER. However, current OER electrocatalysts are still mainly limited in metal oxides, (oxy)hydroxides, phosphides, and chalcogenides, etc. Little attention is paid to the rational design of electrocatalysts based on the transformation-induced strategy. Herein, we demonstrated a Fe-based organic–inorganic hybrid strategy for the construction of OER electrocatalysts based on the in situ transformation. Hierarchically three-dimensional (3D) iron alkoxides of glycerol were synthesized in choline chloride (ChCl)/glycerol deep eutectic solvent (DES). During the OER, the as-prepared Fe-based organic–inorganic hybrid can transform into FeOOH, an active species for electrocatalysis, exhibiting sustainable electrocatalytic performance. It only requires 280 mV to offer a current density of 10 mA cm–2 and has a small Tafel slope of 47 mV decade–1 in 1 M KOH solution, outperforming most reported Fe-based catalysts. This work provides the concept of DES-mediated organic–inorganic hybrid materials as transformation-induced catalysts toward OER, thus casting new light on the rational design of advanced electrocatalysts for water splitting.
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ACS Applied Nano Materials
·
2019
·
IF 0
Yan Zheng,Fei He,Jiaming Wu,Delong Ma,Huailin Fan,Shufei Zhu,Xiang Li,Yizhong Lu,Qing Liu,Xun Hu
Iron (Fe)- and nitrogen (N)-codoped carbon materials hold broad application prospects in the oxygen reduction reaction (ORR) because of their abundant reserves, low cost, and excellent catalytic activity. In this study, a N-doped carbon nanotube (CNT)–graphene framework with encapsulated Fe/Fe3N nanoparticles (Fe–N–CNT@RGO) is designed and synthesized by annealing a mixture of iron acetylacetonate, dicyandiamide, and graphene oxide via a one-step calcination strategy. Fe–N–CNT@RGO has a better ORR catalytic activity than reduced graphene oxide (RGO), N-doped graphene, and N-doped CNTs with encapsulated Fe/Fe3N nanoparticles with respect to the onset potential, limiting current density, and kinetic current density. Fe–N–CNT@RGO also has high stability and a high discharging cell voltage, which approaches those of platinum/carbon in zinc–air batteries. The relationship between the structure and activity of Fe–N–CNT@RGO demonstrates that the high density of Fe–N and pyridinic N sites, moderate wettability, and positive ζ potential promote exposure of the active sites, accelerate the transmission of hydrated oxygen, and enhance the adsorption of HO2– for the 4e– ORR.
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WATER ENVIRONMENT RESEARCH
·
2019
·Vol. 91
·期 8
·770-779
·
IF 1.24
Jinhong Fan,Hehe Qin,Yunfei Zhang,Simin Jiang
In this study, Fe/Cu bimetal composite was prepared by high-energy ball milling (BM) method for the removal of refractory organics. The BM Fe/Cu bimetal was characterized by SEM-EDS, XRD, and XPS. Evenly distributed Fe and Cu was observed in the EDS mapping. In contrasting experiments, the removal rate of 4-chlorophenol (4-CP) by BM Fe/Cu materials was about 10-fold faster than that by chemical substitution deposition (CSD) of Fe/Cu material. Complete 4-CP removal and 66.7% of total organic carbon (TOC) mineralization in the BM Fe/Cu–O 2 system were achieved. Dissolved oxygen plays a crucial role for 4-CP degradation through the in situ generation of reactive oxygen species (ROS) such as H 2 O 2 , ·OH, and via oxygen activation reactions. The predominant reactive radicals were identified to be and ·OH through ESR technique and inhibition experiments. The coexistence of oxidation and reduction of 4-CP in the BM Fe/Cu-O 2 system was proposed. Practitioner points 4-CP removal rate by BM Fe/Cu is 10-fold faster than that by CSD Fe/Cu at the same conditions. Complete 4-CP removal and 66.7% of TOC reduction were achieved. All three ROS including ·OH, , and H 2 O 2 coexisted in the BM Fe/Cu-O 2 system. A harmonious coexistence of oxidation and reduction mechanism was proposed.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Bo Sheng,Fei Yang,Yihao Wang,Zhaohui Wang,Qian Li,Yaoguang Guo,Xiaoyi Lou,Jianshe Liu
Despite the success of Fe(II)/peroxymonsulfate (PMS) process in detoxifying organic pollutants, its intrinsic drawback of sluggish Fe(III) conversion to Fe(II) limits its large-scale practical application. Here we report that commercial MoS 2 , a common metal sulfide, can be used to unlock this kinetic constrain. Addition of MoS 2 greatly accelerates the reduction of Fe(III) to Fe(II), decomposition of PMS, and thus results in enhanced degradation efficiency of 2,4,6-trichlorophenol (TCP) (>95%) and other biorefractory halogenated organic compounds within 30 min. Mass spectroscopy data indicate that TCP can be destructed into low-molecular-weight organic acids, manifesting its powerful oxidation capacity of MoS 2 -assisted Fe(II)/PMS process. Once the Fe(III) in aqueous solution is stabilized by its organic or inorganic ligands, the boosting effects of MoS 2 are largely inhibited and less than 80% of TCP is degraded. Sulfate radicals and hydroxyl radicals are identified as the dominant reactive oxidants in the MoS 2 /Fe(II)/PMS process by radical scavenging tests. The unsaturated S on the fresh MoS 2 surface and the exposed Mo(IV) sites are supposed to react with PMS and Fe(III) in the aqueous solution, respectively. No iron oxides and Mo oxides are detected in X-ray photoelectron spectroscopy (XPS) and X-ray powder diffraction (XRD) measurement, indicating the accelerated Fe(II)/PMS process mainly occurs in the homogeneous solution. MoS 2 exhibits excellent recyclability and sustainable reactivity for the degradation of TCP after 5 consecutive runs. Overall, the present study provides a novel strategy to overcome the rate-limiting step of Fe(III)/Fe(II) that is commonly challenging Fe-based advanced oxidation processes (AOPs) and enable Fe(II)/PMS as efficient as typical Co(II)/PMS.
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高影响因子
Catalysis Science & Technology
·
2019
·Vol. 9
·期 9
·2282-2290
·
IF 5.726
Dawei Zhou,Peixue Wang,Yan Long,Yuqing Fei,Youquan Deng
The thermal cracking behavior of diethyl hexamethylenedicarbamate (EHDC) was investigated in this work. The polymers formed under different conditions were analyzed by IR and TG, indicating that the polymers were mixtures of EHDC, polyureas, imines and others. The polymers could be converted to EHDC by a simple alcoholysis reaction for the first time over Fe–Ni/Al2O3 catalysts. Under the optimized reaction conditions, the yield of EHDC could reach up to 52% with 99% selectivity over 8% Fe–3% Ni/Al2O3 catalysts. The catalysts were extensively characterized by BET, XPS, XRD, SEM, TEM, H2-TPR and NH3-TPD, showing that the interaction effect between Fe species and Ni species may be attributed to high catalytic performance of the catalyst. Meanwhile, the loss of active components resulted in decreased catalytic activity.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2018
·
IF 4.61
Pingping Yan,Qian Sui,Shuguang Lyu,Hongyuan Hao,Horst Friedrich Schröder,Wilhelm Gebhardt
Fe(II) activated sodium percarbonate (SPC) process (SPC/Fe(II)) could efficiently remove sulfamethoxazole (SMX) in the aqueous phase, and has the potential in groundwater remediation . However, the degradation mechanisms, especially the degradation products and pathways till now have remained unclear. In the present study, intermediate products were identified using high resolution liquid chromatography coupled with ion trap and time-of-flight mass spectrometry (LCMS-IT-TOF). Nine intermediate products were identified, six of which have not yet been reported during the oxidation of SMX. The oxidation mechanisms involved hydroxyl substitution, the cleavage of sulfonamide bond, isoxazole ring opening and a rearrangement following the loss of the SO 2 -group. Based on the identified intermediate products, the degradation pathways of SMX by SPC/Fe(II) process were illustrated. Fenton's reaction after the dissolution of SPC was proposed as the main reaction mechanisms, which was checked and confirmed by radical species detection tests and radical species scavenging studies. The results showed that although both O 2 − and HO were present in SPC/Fe(II) system, HO was dominant in the system while O 2 − was seldom involved in the degradation of SMX. These findings provided useful information and supported the application of this advanced oxidation process for antibiotics elimination in the groundwater.
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FOOD CHEMISTRY
·
2018
·
IF 4.946
Nan Wang,Huijuan Chai,Xuelin Dong,Qian Zhou,Lihua Zhu
Iron(III) ethylenediaminetetraacetate (Fe(III)EDTA) is widely used in iron fortification for reducing iron deficiency, and its determination is urgently needed. The present work developed a fluorescent method to straightforwardly determine Fe(III)EDTA by using photoluminescent carbon dots (C-dots) with the aid of F − ions as the masking agent of free Fe 3+ ions. In the presence of F − ions, only Fe(III)EDTA selectively quenched the photoluminescence of C-dots, and both Fe 3+ and Fe 2+ as well as other carboxylic acids have no effect on the emission of C-dots. The sensing mechanism was attributed to the ligand-tailored electron transfer process from C-dots to Fe 3+ . Under optimum conditions, this method showed a linear calibration plot over the Fe(III)EDTA range of 1.0–200 μmol L −1 and a detection limit of 0.4 μmol L −1 . The proposed method was successfully applied to determine Fe(III)EDTA in real samples with acceptable recoveries of spikes (95%−110%) and repeatability (RSD, 4.2%−9.5%).
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PubMed
高影响因子
ENERGY & FUELS
·
2018
·
IF 3.024
Chao Cai,Ning Fu,Ziwei Zhou,Mengchen Wu,Zhenglong Yang,Rui Liu
A tannic acid-Fe coordination compound has been prepared via a simple mechanochemical method. The compound could be used as precursors for the fabrication of porous carbon, which was successfully applied as adsorbent for CO2 capture. The obtained porous adsorbent, NFePC-10-A, exhibited relatively high CO2 uptake capacities of 5.8 and 3.4 mmol g–1 at 0 and 25 °C, respectively. In addition, the initial isosteric heat of adsorption and selectivity for CO2/N2 were as high as 63.16 kJ mol–1 and 22.7 (0 °C). Meanwhile, the adsorbent underwent an efficient reusability, indicating a good potential for practical use. This feasible strategy might provide a novel precursor for the large-scale production of bio-derived carbonaceous adsorbents with tailored texture and porosity for CO2 capture and storage.
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高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2018
·Vol. 317
·期 3
·1223-1233
·
IF 1.181
Liu Zhirong,Yu Jiehao,Yang Lingfang,Dai Ying,Wang Yun,Zhou Liming
Three kinds of method were employed to prepare Fe loaded activated carbon (Fe-AC), liquid reduction method, carbonthermal method, incipient wetness method, respectively. Before and after adsorption, the adsorption property of Fe-AC had been analysed.
Results indicated that the removal mechanisms were mainly redox reaction, adsorption and precipitation. In addition, the adsorption models fitted with the kinetic model and adsorption isotherm model. Based on the analysis of six influencing factors, we obtain some actual information to deal with the humic acid and the “back to acid”.
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高影响因子
CARBON
·
2019
·
IF 7.466
Chao Hu,Ye Mu,Silin Bai,Juan Yang,Lijun Gao,Shao-Dong Cheng,Shao-Bo Mi,Jieshan Qiu
Electrochemically converting CO 2 into fuels or high value-added chemicals hold a great promise for the utilization of emitted CO 2 in the future. Metal-nitrogen active sites (such as Fe–N, Co–N and Ni–N) are supposed to be effective for the electrochemical reduction of CO 2 to CO, whereas their catalytic activities are largely dependent on the dispersibility and bonding structures of the catalytically active metals. In this work, we develop atomically dispersed Fe, N-codoped sandwich-like porous carbon sheets using Fe-containing zeolitic imidazolate framework-8 and graphene oxide as precursors and polyvinyl pyrrolidone (PVP) as a mediator. Compared to catalysts without PVP or with another mediator (i.e. polyetherimide), the PVP-mediated carbon sheets show a porous morphology with a higher specific surface area and a more exposed number of Fe–N active sites. Benefiting from this favourable structure, the resultant Fe, N-codoped porous carbon sheets show higher current densities and improved faradaic efficiencies up to 98.6% at −0.62 V ( vs. the reversible hydrogen electrode, RHE) for the electrochemical reduction of CO 2 to CO. This PVP-mediated strategy could be applied to the fabrication of other metal/nitrogen codoped carbon materials for electrocatalysis.
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高影响因子
CRYSTAL GROWTH & DESIGN
·
2017
·
IF 4.055
Tong-Ying Chang,Bing-Ping Yang,Chun-Li Hu,Dong Yan,Jiang-Gao Mao
The first series of metal phosphate iodates, namely, M(IO3)(HPO4)(H2O) (M = Sc 1, Fe 2, Ga 3, In 4), have been obtained through hydrothermal syntheses. The title compounds are isomorphic and crystallize in the monoclinic space group C2/c (No. 15). Their structures feature a three-dimensional (3D) network composed of 1D [M(HPO4)(H2O)]+ chains that are further bridged by IO3 groups, forming 1D tunnels based on eight-membered rings along the b-axis. Magnetic measurements revealed antiferromagnetic coupling interactions between magnetic centers in compound 2. The UV absorption spectra measurements revealed that compound 2 exhibits a broad absorption peak at about 427 nm. The TGA studies and IR spectra for compounds 1–4 were also performed.
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高影响因子
Journal of Functional Biomaterials
·
2024
·Vol. 15
·期 7
·185
·
IF 5
Yu Wu,Sen Xu,Fengjuan Ding,Weibing Zhang,Haiyan Liu
In this work, a new type of FE-1 COF material is prepared by a reversible imine condensation reaction with diaminoferrocene and diaminodiformaldehyde as materials. The material is connected by imine bonds to form a COF skeleton, and the presence of plenty of nitrogen-containing groups gives the material good hydrophilicity; the presence of metal Fe ions provides the material application potential in the enrichment of phosphopeptides. According to the different binding abilities of N-glycopeptide and phosphopeptide on FE-1 COF, it can simultaneously enrich N-glycopeptide and phosphopeptide through different elution conditions to realize its controllable and selective enrichment. Using the above characteristics, 18 phosphopeptides were detected from α-casein hydrolysate, 8 phosphopeptides were detected from β-casein hydrolysate and 21 glycopeptides were detected from IgG hydrolysate. Finally, the gradual elution strategy was used; 16 phosphopeptides and 19 glycopeptides were detected from the α-casein hydrolysate and IgG hydrolysate. The corresponding glycopeptides and phosphopeptides were identified from the human serum. It proves that the FE-1 COF material has a good enrichment effect on phosphopeptides and glycopeptides.
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