APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Xiao-Cheng Liu,Chuan-Shu He,Zi-Yang Shen,Wen-Qiang Li,Ning Chen,Jun-Sheng Song,Xiao-Guo Zhou,Yang Mu
Fe(III) chelate reduction is of great importance in the homogeneous neutral electro-Fenton (EF) process, but its reduction mechanisms with different reductive species remain unclear. In this study, the reduction mechanisms of several typical Fe(III) chelates through electron and atomic H* were investigated using experiments and density functional theory calculations. The results indicated that the electron reduction efficiencies for [Fe(III)-EDTA] − and [Fe(III)-EDDS] − chelates were 16.23 and 8.31 times higher compared to [Fe(H 2 O) 6 ] 3+ , which was featured by low E LUMO - HOMO and concentrated LUMO distribution around Fe atom. In contrast, the atomic H* reduction efficiency for [Fe(III)-HA] 3+ chelate was 10 times higher than that of electron, attributed to high chelation ability of HA and negative energy barrier of [Fe(III)-HA] 3+ reduction in the atomic H*-dominated system. Additionally, phthalocyanine (Pc) had insignificant effect on pollutant degradation efficiency in the neutral EF systems due to the lower chelate ability of Pc with Fe(III) compared to H 2 O.
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高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2020
·Vol. 22
·期 14
·7218-7223
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IF 3.43
Mengyao Lv,Haichuan Guo,Hangjia Shen,Jun Wang,Jiacheng Wang,Yuichi Shimakawa,Minghui Yang
A key challenge in carrying out an efficient oxygen reduction reaction (ORR) is the design of a highly efficient electrocatalyst that must have fast kinetics, low cost and high stability for use in an energy-conversion device (e.g. metal–air batteries). Herein, we developed a platinum-free ORR electrocatalyst with a high surface area and pore volume via a molten salt method along with subsequent KOH activation. The activation treatment not only increases the surface area to 940.8 m2 g−1 by generating lots of pores, but also promotes the formation of uniform Fe3C nanoclusters within the atomic dispersed Fe–Nx carbon matrix in the final material (A-FeNC). A-FeNC displays excellent activity and long-term stability for the ORR in alkaline media, and shows a greater half-wave potential (0.85 V) and faster kinetics toward four-electron ORR as compared to those of 20 wt% Pt/C (0.83 V). As a cathode catalyst for the Zn–air battery, A-FeNC presents a peak power density of 102.2 mW cm−2, higher than that of the Pt/C constructed Zn–air battery (57.2 mW cm−2). The superior ORR catalytic performance of A-FeNC is ascribed to the increased exposure of active sites, active single-atom Fe–N–C centers, and enhancement by Fe3C nanoclusters.
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高影响因子
JOURNAL OF ORGANIC CHEMISTRY
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2020
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IF 4.335
Zhiwei Chen,Xiang Bai,Jie Sun,Yicheng Xu
A facile Fe(III)-catalyzed oxidative decarboxylative radical coupling reaction of α,α-difluoroarylacetic acids with coumarins has been developed. This transformation, which provides a series of C-3 difluoroarylmethylated coumarins containing various functional groups in moderate-to-good yields, features easily accessible starting materials and operational simplicity.
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高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Fang Liu,Weiyang Jin,Ying Li,Lekai Zheng,Yongchuan Hu,Xuewen Xu,Yanming Xue,Chengchun Tang,Hui Liu,Jun Zhang
The development of efficient non-precious metal catalysts to accelerate the oxygen evolution reaction (OER) kinetics is important for the development of water-derived hydrogen fuel. Iron-cobalt oxide ((Co, Fe) 3 O 4 ) is one of the most promising transition metal-based OER electrocatalysts under alkaline conditions, but its activity is unsatisfactory due to its limited active sites and poor electronic conductivity. Herein, self-supported (Co, Fe) 3 O 4 hierarchical nanosheet arrays with massive oxygen vacancies (denoted as V O -(Co, Fe) 3 O 4 /CC) are synthesized by a simple reduction method at room temperature. Oxygen vacancies can regulate the ratio of Co 2+ /Co 3+ , which leads to the modification of its electronic properties, and it also significantly improves the charge transfer ability and accelerates the reaction. Meanwhile, the unique hierarchical nanosheet arrays structure and abundant oxygen vacancies effectively adjust the number of OER active sites, which has a key role in developing a cost-effective oxygen electrode. Accordingly, V O -(Co, Fe) 3 O 4 /CC exhibits a relatively low overpotential of 286 mV at 10 mA cm −2 and a low Tafel slope of 41 mV dec −1 .
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2020
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IF 7.1
Meizhu Chen,Jia An,Yongqin Hu,Rubing Chen,Ying Lyu,Nan Hu,Mengfei Luo,Mengdi Yuan,Yufei Liu
Perovskite materials have shown great potential in various fields, such as photovoltaic devices, biomedical applications, and fluorescent probes. However, their hypersensitivity has significantly limited their practical application. In this paper, a modified swelling-shrinking strategy was adopted to encapsulate CsPbBr 3 perovskite quantum dots into poly(styrene/acrylamide) nanospheres, in order to create novel hyperstatic and hydrophilic perovskite polymer fluorescent beads. The results show that the fluorescence characteristics did not noticeably change when the polymer materials were dispersed in an aqueous solution over 12 months. Under harsher conditions (acid, alkali, PBS, DMEM, temperature), the novel perovskite polymers showed unprecedented fluorescence stability, which was then applied to the selective sensing of Fe(III) in real samples. The results show that a good linear relationship between 5 and 150 μM was obtained under optimal conditions, and the limit of detection was approximately 2.2 μM. Furthermore, the Fe(III)-sensing applications in Yangtze River water, human serum and tea water has been proven with satisfying results.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2020
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IF 2.627
Dairui Xie,Hongcheng Zhang,Meng Jiang,Hao Huang,Heng Zhang,Yang Liao,Shilin Zhao
Humic acid (HA) was carbonized at 300, 400 and 500 °C and then functionalized with 1 wt%–12 wt% Fe(III) respectively [CHA300/400/500-Fe(III)]. Adsorption of such Fe(III)-functionalized carbonized HA as adsorbents to aqueous tetracycline (TC: 25 mg·L −1 ) was studied. The adsorption equilibrium time for CHA400-Fe(III) to TC was 6 h faster and the adsorption removal efficiency ( R e ) was two times higher than that of HA/CHA. The adsorption R e of CHA400-Fe(III) loaded 10% iron [CHA400-(10%)Fe(III)] to TC could reach 99.8% at 8 h and still kept 80.6% after 8 cycles. The adsorption kinetics were well fitted to the pseudo-second-order equation and the adsorption isotherms could be well delineated via Langmuir equations( R 2 > 0.99), indicating that the homogeneous chemical adsorption of TC occurred on the adsorbents. The main adsorption mechanisms of TC were complexation Fe(III) and hydrophobic distribution. Electropositive and electronegative repulsion between TC and CHA400-(10%)Fe(III) at lowly pH(2) and highly pH(8–10) respectively, leaded to the relatively low adsorption capacity and more notable influence of ion concentration. When the pH was between 4 and 8, TC mainly existed in neutral molecules (TCH 2 ), so the influence of ion concentration was not obvious. The dynamic adsorption results showed that the CHA400-(10%)Fe(III) could continuously treat about 2.4 L TC(27 mg·L −1 ) wastewater with the effluent concentration as low as 0.068 mg·L −1 . Our study suggested a broad application prospect of a new, effective, low-cost and environment-friendly adsorbent CHA400-(10%)Fe(III) for treatment of low-concentration TC polluted wastewater.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
·
IF 4.939
Mingxuan Fu,Qi Zhang,Yuena Sun,Guyang Ning,Xinyu Fan,Haiyang Wang,Haijun Lu,Yufan Zhang,Huan Wang
Electrochemical water-splitting is widely regarded as one of the essential strategies to produce hydrogen energy, while Metal-organic frameworks (MOFs) materials are used to prepare electrochemical catalysts because of its controllable morphology and low cost. Herein, a series of trimetallic porous Pt-inlaid Ni–Fe nanocubes (NCs) are developed with bifunctions of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). In the process of prepare the electrochemical catalysts, Pt nanoparticles are uniformly embedded in the Fe–Ni PBA cube structure, and ascorbic acid is employed as a reducing agent to reduce Pt 2+ to Pt nanoparticles. In this work, the cubic structure of Fe–Ni PBA is maintained and the noble metal Pt nanoparticles are embedded. Remarkably, the formation of PBA cubes, Pt inlay and reduction are completed in one step, and Pt nanoparticles are embedded by a simple method for the first time. By employing acid etching method, a porous structure is formed on the PBA cube, which increases the exposed area of the catalyst and provides more active sites for HER and OER. Due to the porous structure, highly electrochemical active surface area and the embedded of highly dispersed Pt nanoparticles, the porous 0.6 Ni–Fe–Pt nanocubes (NCs) exhibits excellently electrocatalytic performance and durable stability to HER and OER. In this work, for HER and OER, the Tafel slopes are 81 and 65 mV dec −1 , the overpotential η at the current density of 10 mA cm −2 are 463 and 333 mV, and the onset potential are 0.444 and 1.548 V, respectively. And after a 12-h i-t test and 1000 cycles of cyclic voltammetry (CV), it maintained high stability and durability. This work opens up a new preparation method for noble metal embedded MOF materials and provided a new idea for the preparation of carbon nanocomposites based on MOF.
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JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 55
·期 26
·11970-11983
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IF 3.553
Niu Yingchun,Li Xueai,Dong Wenqi,Zhang Can,Zhao Kuihu,Wang Fengyan,Wang Haiyan
Carbon and iron composites have drawn much attention for their unique electromagnetic properties. In addition, nitrogen doping of carbon can effectively modulate the dielectric properties of carbon. Therefore, synthesis of N-doped carbon and iron composites is an alternative method for obtaining high-efficiency microwave absorption materials. In previous studies, the synthesis process was very complicated including multistep routes. In this work, N-doped carbon with embedded Fe/Fe 3 C was synthesized in-situ via pyrolysis of amino phenol formaldehyde resin (APF) scattered with Fe 2 O 3 nanoparticles (APF/Fe 2 O 3 ), which was obtained through a simple hydrothermal process. During the heat-treatment process, the APF resin was converted into N-doped carbon, and simultaneously, the Fe 2 O 3 was reduced to iron nanoparticles. Then, inevitably, the iron nanoparticles reacted with carbon to form Fe 3 C at the interface between the iron particles and carbon. Taking advantage of multiple heterogenous interface, the interfacial polarization relaxation could be enhanced. Therefore, the N-doped carbon with embedded Fe/Fe 3 C particles displays microwave absorption with a maximum reflection loss of − 70 dB. Moreover, the effective absorption bandwidth (reflection loss of less than − 10 dB) reaches 6.02 GHz at a thickness of 2.13 mm. This study not only provides composites of N-doped carbon with embedded Fe/Fe 3 C particles with excellent stable microwave absorption but also offers a simple method for synthesizing N-doped carbon with embedded Fe/Fe 3 C particles.
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高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Xianshu Qiao,Hongjun Kang,Yang Li,Kai Cui,Xin Jia,Henghao Liu,Wei Qin,Max Pupucevski,Gang Wu
We report a highly efficient and stable electrode composed of a porous Fe-doped β-nickel hydroxide nanopyramid array supported on nickel foam (U–Fe-β-Ni(OH)2/NF) for overall water splitting. The unique structure is assembled via a self-templated strategy by utilizing the FeNi oxalate (FeNi–C2O4/NF) nanopyramid as the templates, followed by an anion-exchange reaction at room temperature. Due to the intrinsic activity of Fe-doped β-Ni(OH)2 along with unique porous array structures consisting of two-dimensional (2D) active materials on three-dimensional (3D) conductive substrates, the developed electrode exhibited outstanding electrocatalytic activity for both the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in an alkaline medium. The introduced amount of Fe plays a significant role in promoting OER and HER activity compared to the β-Ni(OH)2 electrode. The optimal electrode (U–Fe-β-Ni(OH)2/NF-2) generated a current density of 10 mA cm–2 at low overpotentials of 218 mV for the OER and 121 mV for the HER. The electrode also demonstrated considerably stable performance during the continuous water splitting process. Furthermore, we elucidated the promotion mechanisms of the active Fe-doped β-Ni(OH)2 compound for the OER and HER based on extensive characterization and electrochemical measurements. Hence, this work provides a facile approach to developing low-cost, efficient, and stable hydroxide-based electrodes for bifunctional OER and HER in water splitting.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
·
IF 4.939
Lei Liu,Huan Liu,Xingwei Sun,Chunping Li,Jie Bai
Transition metal iron-based catalysts are promising electrocatalysts for oxygen reduction reaction (ORR), and they have the potential to replace noble metal catalysts . The one-dimensional of carbon nanofibers with tubular structure can effectively promote the electrocatalytic activity , which facilitates electron transport . Herein, the Pt–Fe/CNFs were synthesized by electrospinning and subsequent calcination . Benefiting from the advantages of one-dimensional structure, Pt–Fe/CNFs-900 with fast electrochemical kinetics and excellent stability for ORR with excellent onset of 0.99 V, a low Tafel slope of 62 mV dec −1 and high limiting current density of 6.00 mA cm −2 . Long-term ORR testing indicated that the durability of this catalyst was superior to that of commercial Pt/C in alkaline electrolyte . According to RRDE test, the ORR reaction process of Pt–Fe/CNFs-900 was close to four-electron transfer routes.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Yuda Zhu,Nini Xin,Zi Qiao,Suping Chen,lingwan Zeng,Yusheng Zhang,Dan Wei,Jing Sun,Hongsong Fan
Traditional tumor treatments suffer from severe side effects on account of their invasive process and inefficient outcomes. Featuring a unique physical microenvironment, the tumor microenvironment (TME) provides a new research direction for designing more efficient and safer treatment paradigms. In this study, we fabricated a polydopamine (PDA)-based TME-responsive nanosystem, which successfully integrates glucose degradation, the Fenton reaction, and photothermal therapy for efficient cancer therapy. Through a convenient hydrothermal method, Fe2+-doped Fe(II)–PDA nanoparticles were successfully fabricated, which show an excellent photothermal effect and interesting reactivity for the Fenton reaction. Instead of introducing toxic anticancer agents, natural glucose oxidase (GOD) was grafted on Fe(II)–PDA, forming a cascade catalytic nanomedicine for a specific response to the glucose in TME. GOD grafted on Fe(II)–PDA–GOD is ought to catalyze abundant glucose in TME into gluconic acid and H2O2. The concomitant generation of H2O2 can enhance the efficiency of the sequential Fenton reaction, producing abundant hydroxyl radicals (•OH) for cancer therapy. Besides, the overconsumption of intratumoral glucose also could inhibit tumor growth by reducing the energy supply. Taken together, the in vitro and in vivo antitumor studies of such TME-based Fe(II)–PDA–GOD nanosystems displayed a favorable synergistic potency of glucose degradation, the Fenton reaction, and photothermal therapy against tumor growth. Our design expands the biological application of multifunctional PDA while providing novel strategies toward effective antitumor treatment with minimal side effects.
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高影响因子
Journal of Analysis and Testing
·
2019
·Vol. 3
·期 3
·238-245
·
IF 0
Sun Shihao,Fan Yaofang,Du Jiaoyang,Song Zhilian,Zhao Huimin
Over the past few decades, the enzyme-mimicking activity of metal–organic frameworks (MOFs) accompanied with structural characteristics has aroused much attention. However, pure MOFs have low affinity with DNA. Here, iron-based MOFs with acidized carbon nanotubes (CNTs) via a simple hydrothermal process have been synthesized, named as MIL-88(NH 2 )-Fe@CNTs. CNTs can enhance the affinity between MOF and DNA, achieving flexible regulation of their catalytic activity benefiting from the strong π − π stacking between CNTs and DNA. Meanwhile, in comparison with conventional iron-based MOFs, the addition of CNTs, which contributes to the acceleration of electron transfer, endowing as-prepared nanocomposites remarkably enhanced peroxidase-like activity to achieve an ultrasensitive detection of H 2 O 2 with the LOD of 17.64 μg/L. Notably, the as-prepared nanocomposites with adsorbed DNA displayed excellent affinity towards both TMB (3, 3′, 5, 5′-tetramethylbenzidine) substrates and H 2 O 2 as well as high catalytic velocity. On the basis of their switchable peroxidase-like activity regulated by different length or sequence of ssDNA, it is believed that our-prepared MOF-based nanomaterials would be promising for fabricating versatile and sensitive label-free colorimetric assays for diverse targets.
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