APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Deng Wang,Jin Liu,Jiangbo Xi,Jizhou Jiang,Zhengwu Bai
Efficient catalyst with enhanced activity and high stability is important for chemical industry. Active species, support as well as their interaction play key roles on catalytic performance for supported heterogeneous catalysts . In this work, Pd Fe dual-metal nanoparticles (NPs) were anchored and confined in an interface of double-layered carbon nanotubes/nitrogen-doped carbon (CNT/NC) support to obtain a dual-metal CNT/PdFe/NC catalyst. The microstructure and composition of CNT/PdFe/NC catalyst were systematically characterized by transmission electron microscopy (TEM), X-ray photoelectron spectrometry (XPS), inductively coupled plasma mass spectrometry (ICP-MS), X-ray diffraction (XRD) and surface area analysis. Benefiting from the catalytically active tubular CNT/NC support, uniformly dispersed Pd Fe dual-metal NPs and unique confined structure, the CNT/PdFe/NC catalyst exhibited excellent catalytic activity for nitroarenes reduction reaction. The catalytic activity of the Pd Fe dual-metal NPs was much better than that of monometal counterparts (CNT/Pd/NC and CNT/Fe/NC), showing an enhanced synergetic effect. The catalytic turnover frequency (TOF) of the CNT/PdFe/NC catalyst amounted to 70.36 min −1 toward 4-nitrophenol (4-NP) reduction reaction, being superior to previously reported noblemetal-based catalysts. Furthermore, this catalyst also exhibited an excellent stability and reusability due to the intrinsic confined structure. This work provides valuable insights to rationally design and develop an efficient dual-metal catalyst.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2018
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IF 6.434
Ailin Li,Zihao Wu,Tingting Wang,Shaodong Hou,Bangjie Huang,Xiujuan Kong,Xuchun Li,Yinghong Guan,Rongliang Qiu,Jingyun Fang
The abatement of pharmaceuticals and personal care products (PPCPs), including carbamazepine (CBZ), acetaminophen (ACP) and sulfamethoxazole (SMX), by zero-valent iron (Fe°) activated peroxydisulfate (PDS) system (Fe°/PDS) in pure water and groundwater was investigated. The removal rates of CBZ, ACP and SMX were 85.4%, 100% and 73.1%, respectively, within 10 min by Fe°/PDS in pure water. SO 4 •− , • OH and O 2 •− were identified in the Fe°/PDS system, and O 2 •− was indicated to play an important role in the ACP degradation. The degradation of PPCPs increased with increasing dosages of Fe° and PDS or with decreasing pH and initial PPCP concentrations. Interestingly, the degradation of PPCPs by Fe°/PDS was significantly enhanced in groundwater compared with that in pure water, which was partially attributed to SO 4 2− and Cl − . The first-order constants of CBZ, ACP and SMX increased from 0.021, 0.242 and 0.013 min− 1 to 0.239, 2.536 and 0.259 min −1 , and to 0.172, 1.516 and 0.197 min −1 , respectively, with increasing the concentrations of SO 4 2− and Cl − to 100 mg/L and 10 mg/L, respectively. This study firstly reports the unexpected enhancement of groundwater matrix on the degradation of micropollutants by Fe°/PDS, demonstrating that Fe°/PDS can be an efficient technology for groundwater remediation.
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PubMed
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CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Juntao Tang,Jianlong Wang
Fe-based magnetic nanoparticles (NPs) embedded into mesoporous carbon hybrid (Fe@MesoC) was successfully fabricated from Fe-based metal-organic framework (MIL-100(Fe)) through a pyrolysis method, which was for the first time proposed as a novel Fenton-like catalyst for the degradation of sulfamethoxazole (SMX). The catalytic activity of Fe@MesoC was systematically evaluated on the basis of several reaction parameters including initial pH, initial H 2 O 2 concentration and temperature. Under the optimal conditions, the Fe@MesoC composite demonstrated a superior catalytic activity for decomposing SMX in the presence of H 2 O 2 , and it accomplished 100% SMX and 54.5% total organic carbon (TOC) conversion within 120 min. Such outstanding performance can be explained by the excellent enrichment ability of the outer mesoporous carbon matrix, the abundant active sites of the inner Fe-based NPs, as well as the possible synergistic effect between the two components. Moreover, the facile electrons transfer from Fe 0 to iron oxide in the inner Fe-based NPs could facilitate the reduction of Fe 3+ to Fe 2+ ( represents the iron species anchored to the surface of the catalyst) and further improve the generation of hydroxyl radicals. With the high structural stability and saturation magnetization, the Fe@MesoC composite can be easily recycled for three subsequent runs without significant activity loss. The possible catalytic mechanism and degradation pathways for SMX degradation induced by hydroxyl radicals in Fe@MesoC/H 2 O 2 Fenton-like system were also tentatively proposed.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2018
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IF 3.141
Yong Liu,Shenshen Li,Xiying Li,Liqun Mao,Fujian Liu
Development of efficient catalysts with low cost for the oxygen reduction reaction (ORR) plays an important role in the commercialization of fuel cells. Herein, we reported a facile method to synthesize Fe–N co-doped porous carbon (Fe–N/C) by using green media ionic liquids 1-butyl-3-methylimidazolium tetrachloridoferrate ([Bmim][FeCl4]) as precursor of C, N, and Fe, and spherical silica as a template through one-step pyrolysis. Electrochemical measurements show that Fe–N/C800 possesses excellent ORR catalytic activity. The onset potential and half-wave potential are 0.964 and 0.821 V, respectively, which is close to those on the commercial Pt/C catalyst. Moreover, it exhibits better methanol tolerance and durability in comparison with the Pt/C catalyst. Good performance of Fe–N/C800 in ORR is attributed to its abundant porous structure, large BET surface area, and the synergism of Fe and N dopants.
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TALANTA
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2018
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IF 4.244
Hao Zhang,Chen Nie,Jiahui Wang,Ruifang Guan,Duxia Cao
Organic-inorganic hybrid fluorescent microspheres (OI-FMs) without typical fluorophores were prepared. Fluorescence quantum yield of OI-FMs is up to 70.0% after being heated in an oven at 120 °C (named as OI-FMs-120). Interestingly, OI-FMs-120 shows different detection performances in different solvents. It can be used for qualitative and quantitative detection of Fe 3 + with a detection limit of 37.8 nM in absolute ethanol. While in aqueous solution, it can be applied as an ON-OFF-ON fluorescent probe . Fluorescence of the probe is quenched by Hg 2 + and later recovered by biothiols. The detection limit is as low as 34.9 nM for Hg 2 + , 91.0 nM for Cys, 0.12 μM for Hcy and 0.13 μM for GSH in aqueous medium, respectively.
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Nano Energy
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2018
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IF 13.12
Jiahui Chen,Jianwen Liu,Jin-Qi Xie,Huangqing Ye,Xian-Zhu Fu,Rong Sun,Ching-Ping Wong
The development of high-performance and cost-effective electrocatalysts is of great significance for hydrogen production by water splitting but remains challenge. Herein, a metal organic frameworks (MOFs) templating approach is proposed to synthesize Co incorporating FeP nanotubes (Co-Fe-P nanotubes) for efficient for hydrogen evolution reaction (HER). The MOFs-derived tubular structure with in situ Co substitution lead to abundant catalytic sites, fast mass and charge transport pathways, and desirable electronic configuration. These beneficial effects enable Co-Fe-P nanotubes efficient HER catalytic activity in a wide pH range, achieving small overpotentials of 86, 138, and 66 mV at a current density of 10 mA cm −2 in 1 M KOH, 1 M phosphate buffer solution (PBS), and 0.5 M H 2 SO 4 , respectively. The catalytic activity of Co-Fe-P nanotubes outperforms most of the reported FeP-based electrocatalysts. Density functional theory calculations further reveal that Co substitution results in increased density of states near Fermi level , boosting the intrinsic electrocatalytic activity of Co-Fe-P nanotubes. This work affords a feasible way to the synthesis of cheap and efficient FeP-based electrocatalysts for HER.
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ELECTROCHIMICA ACTA
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2018
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IF 5.116
Xiaona Ren,Fenglei Lyu,Jian Yang,Fangyuan Wang,Linlin Xue,Li Wang,Xiangwen Zhang,Qingfa Wang
To develop highly efficient non-noble-metal electrocatalysts for oxygen evolution reaction is still a great challenge. Herein, cobalt and iron oxide with hollow structure has been fabricated using ZIF-67 as template, via reflux process followed by calcination . The simultaneous structural and electronic modulation are achieved due to the homogenous Fe incorporation. The Co sites in higher oxidation states and Fe sites with higher electron density can enhance the adsorption of H 2 O molecules and OOH species, and thus promote the water oxidation . The unique hollow structure also facilitates the mass transfer at the interface of electrolyte and active atoms. The optimal cobalt and iron oxide hollow nanocages exhibit superior OER performance, delivering an ultralow overpotential of 274 mV at 10 mA cm −2 and a very small Tafel slope of 31 mV dec −1 in alkaline media, which outperform the state-of-the-art RuO 2 . This work provides an efficient approach to design and explore non-precious electrocatalysts for electrochemical energy conversion and storage.
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JOURNAL OF POWER SOURCES
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2018
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IF 6.945
Yuntong Li,Zhongyu Li,Yuzhe Wu,Haiyang Wu,Hong Zhang,Tong Wu,Conghui Yuan,Yiting Xu,Birong Zeng,Lizong Dai
Rational design of high-efficiency and cost-effective nonprecious metal-based catalysts with outstanding oxygen reduction reaction (ORR) performance, is of great importance to replace platinum-based electrocatalysts in fuel cell. Herein, a novel N, B and Fe co-doped carbon materials (Fe-NBC) electrocatalyst is designed through the pyrolysis of a metal-organic coordination polymer precursor, which is formed from the coordination between dendrimer-like terpyridinic monomer and Fe 3+ . The as-prepared Fe-NBC catalyst exhibits superior ORR activity with an onset potential of 0.98 V and a half-wave potential of 0.86 V, which are comparable to that of the Pt/C catalyst. The formation of Fe-N x moieties is considered to be the most important factor for the improved ORR activity of Fe-NBC. Besides, Fe-NBC catalyst displays a better methanol tolerance as well as durability (5 mV negative shift of E 1/2 , after 1000 cycles) in comparison with Pt/C (12 mV negative shift of E 1/2 , after 1000 cycles). This work provides a facile protocol for the design and fabrication of multi-element co-doped carbon materials. Moreover, the excellent ORR performance of these N, B and Fe co-doped carbon materials may be a potential candidate to replace Pt-based catalyst in fuel cells.
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ACS Applied Materials & Interfaces
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2018
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IF 8.097
Yalan Chen,Jingtong Zhang,Peng Guo,Haijun Liu,Zhaojie Wang,Ming Liu,Tian Zhang,Shutao Wang,Yan Zhou,Xiaoqing Lu,Jun Zhang
Hydrogen evolution reaction (HER) driven by high-performance and low-cost electrocatalysts has been well-identified as one of the most promising technologies to explore sustainable power sources. In this work, the authors demonstrated a series of Fe–Mo selenide composite nanomaterials with adjustable HER catalytic activities by a simple one-step hydrothermal reaction. The heterostructured catalyst exhibited significant enhancement in HER activity compared to the pristine MoSe2 and FeSe2 catalysts. It is found that the optimized Mo–Fe selenide can drive the HER at a current density of 10 mA cm–2 by an overpotential of 86.9 mV in acidic solution. Also, it possesses outstanding kinetics (Tafel slope of 57.7 mV dec–1) of the electrochemical reaction. Besides the synergistic effect of different chemicals, the coupled Mo–Fe selenide achieved the electronic modulation of the heterointerface, where electrons were accelerated to transfer from dispersed FeSe2 to the active edges on 1T-MoSe2 and further activated the electrochemical performance.
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ChemElectroChem
·
2019
·Vol. 6
·期 12
·3030-3038
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IF 3.975
Ping Yan,Dewang Kong,Wenjing Yuan,Anjian Xie,Yuhua Shen
Graphical Relaxed conditions : A low-cost method is demonstrated for the synthesis of iron-based one-dimensional nitrogen-doped carbon nanotube nanocomposites (Fe/Fe 2.5 C/Fe 3 N/N-CNT). Unlike most Fe−N−C type CNT materials, Fe/Fe 2.5 C/Fe 3 N/N-CNT does not require a variety of templates or strict experimental conditions during the synthesis process to control the structure and morphology of the products, which makes the preparation process simpler with a lower energy consumption. This greatly increases its potential for practical applications. I n this study, a novel one-dimensional iron-based nitrogen-doped carbon nanotube (N-CNT) nanocomposite (Fe/Fe 2.5 C/Fe 3 N/N-CNT) was successfully synthesized in situ by using a facile and low-cost method. In alkaline media, the typical product (Fe/Fe 2.5 C/Fe 3 N/N-CNT-30) showed an good onset potential ( E onset =0.93 V vs RHE), half-wave potential ( E 1/2 =0.79 V vs RHE), and current density ( J =6.62 mA cm −2 at 0.2 V vs RHE), especially compared to the commercial 20 % Pt/C catalyst (0.95 V, 0.82 V, 5.61 mA cm −2 , respectively). In acidic medium, it also exhibits a good oxygen reduction reaction (ORR) activity. Moreover, Fe/Fe 2.5 C/Fe 3 N/N-CNT-30 exhibited superior long-term durability and methanol tolerance compared to Pt/C in both alkaline and acidic media. The excellent electrocatalytic performance of this material is attributed to the abundant carbon defects in the carbon structure, the high content doping of pyridinic N and graphitic N into the CNTs, the multi-model Fe species as active sites, and the fact that most Fe species within the CNTs avoid corrosion from electrolyte. This study paves a new way for highly active ORR electrocatalysts and promotes the rapid development of CNTs in some frontier fields.
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Journal of Materials Chemistry B
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2015
·Vol. 3
·期 20
·4146-4154
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IF 4.726
Ruizhong Zhang,Shuijian He,Chunmei Zhang,Wei Chen
In this study, a simple and one-pot pyrolysis strategy is developed for the mass production of Fe, N-incorporated carbon nanotubes in situ grown on 3D porous carbon foam (denoted as Fe–Phen–CFs), which provides highly active Fe–N and doped-N species, and a large surface area with exposed active sites. The obtained composite exhibits intrinsic peroxidase-like catalytic activities. With the Fe–Phen–CFs as the catalyst, the peroxidase substrate of terephthalic acid (TA) can be oxidized to the fluorescent product of hydroxyterephthalate (HTA) by H2O2, which provides a unique strategy for fluorescence detection of H2O2. With such a process, as low as 68 nM H2O2 could be detected with a linear range from 0.1 to 100 μM. Meanwhile, by integrating glucose oxidase on the Fe–Phen–CFs composite, sensitive detection of glucose is also achieved with a linear range from 0.5 to 200 μM and a limit of detection of 0.19 μM. Most importantly, such a novel TA/Fe–Phen–CFs system can be successfully applied to glucose determination in real human serum samples. The unique nature and 3D structure of the Fe–Phen–CFs composite makes it promising for the fabrication of low-cost, high-performance biosensors.
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Journal of Materials Chemistry A
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2014
·Vol. 3
·期 5
·2120-2127
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IF 0
Fangyuan Gai,Tianlei Zhou,Yunling Liu,Qisheng Huo
In this study, a water-soluble Fe3+ ratiometric fluorescent sensor was designed and synthesized by encapsulating a donor–acceptor (D–A) dye 4-formacyl-triphenylamine (FTA) into silica cross-linked micellar nanoparticles (SCMNPs). The quenching of FTA-encapsulated SCMNPs (FTA-SCMNPs) on Fe3+ sensing was confirmed using the fluorescence titration method. FTA-encapsulated functionalized SCMNPs (FTA-NH2-SCMNPs and FTA-SO3H-SCMNPs) were synthesized to demonstrate the surface charge effect of nanoparticles on Fe3+ fluorescence sensing. The sensing ability of Fe3+ followed in this order: FTA-SO3H-SCMNPs > FTA-SCMNPs > FTA-NH2-SCMNPs, which indicates that particles with stronger negative charge have better sensing abilities. Moreover, linear correlation between the quenching intensity and lower concentration of Fe3+ was in accordance with the Stern–Volmer equation in FTA-SCMNPs and FTA-SO3H-SCMNPs. FTA-SO3H-SCMNPs showed good selectivity for Fe3+ detection. Because of the charge effect of functionalized SCMNPs on a dye-doped Fe3+ sensing system, these kinds of nanoparticles offered possibilities to construct sensing ability-enhanced fluorescence-quenching sensors by tuning the surface charge.
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