ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Hui Chen,Wengao Zeng,Yutang Liu,Wanyue Dong,Tao Cai,Lin Tang,Juan Li,Wenlu Li
It is important to find an effective way to enhance the photocatalytic efficiency of metal–organic frameworks. In this work, an organic supermolecule perylene diimide (PDI) semiconductor with a carboxyl terminal was added into the synthesis process of MIL-53(Fe) crystals. The PDI/MIL-53(Fe) (PM) composite photocatalyst was first obtained. The TC-H photodegradation rate of the most efficient 5PM was nearly 94.08% within 30 min, whose apparent reaction rate constant (k) is 4 times that of PDI and 33 times that of MIL-53(Fe), respectively. By investigation and characterization, it has been found that PDI nanofibers were dispersed and fixed in MIL-53(Fe) and bonded to each other by covalent bonds. The radical trap experiments and electron spin resonance analysis illustrated that hydroxyl radical (·OH), superoxide radical (·O2–), and photogenerated holes (h+) were active species. Combined with the band structure of PDI and MIL-53(Fe), it is proposed that the PM photocatalyst was a Z-scheme heterojunction mechanism. Therefore, PM photocatalysts showed excellent charge separation and transfer ability. The performance improvement of 5PM is due to enhanced visible light absorption, efficient charge separation, and excellent redox potential. Five cyclic photocatalytic tests and experiments further demonstrate that the 5PM photocatalyst has a promising future for pollutant removal.
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高影响因子
MOLECULES
·
2020
·Vol. 25
·期 7
·1585
·
IF 3.267
Jianhui Zhu,Amr Abdelkader,Denisa Demko,Libo Deng,Peixin Zhang,Tingshu He,Yanyi Wang,Licong Huang
Room temperature sodium-sulfur batteries have been considered to be potential candidates for future energy storage devices because of their low cost, abundance, and high performance. The sluggish sulfur reaction and the “shuttle effect” are among the main problems that hinder the commercial utilization of room temperature sodium-sulfur batteries. In this study, the performance of a hybrid that was based on nitrogen (N)-doped carbon nanospheres loaded with a meagre amount of Fe ions (0.14 at.%) was investigated in the sodium-sulfur battery. The Fe ions accelerated the conversion of polysulfides and provided a stronger interaction with soluble polysulfides. The Fe-carbon nanospheres hybrid delivered a reversible capacity of 359 mAh·g−1at a current density of 0.1 A·g−1and retained a capacity of 180 mAh·g−1at 1 A·g−1, after 200 cycles. These results, combined with the excellent rate performance, suggest that Fe ions, even at low loading, are able to improve the electrocatalytic effect of carbon nanostructures significantly. In addition to Na-S batteries, the new hybrid is anticipated to be a strong candidate for other energy storage and conversion applications such as other metal-sulfur batteries and metal-air batteries.Keywords:sodium-sulfur battery;catalytic activity;hollow N-doped carbon nanospheres;chemical absorption;polysulfides
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Materials Today Physics
·
2021
·
IF 9.298
A. Wang,Y. Hu,H. Wang,Y. Cheng,T. Thomas,R. Ma,J. Wang
To improve the structure-dominant activity, rational design of oxide-based materials remains challengeable in bifunctional oxygen electrocatalysis , especially from the perspective of electronic modulation. Herein, we demonstrate that the electron configuration of inverse spinel NiCo 2 O 4 can be activated by controllable substitution of Fe into the octahedral centers. Fe-substituted NiCo 2 O 4 nanoparticles embedded in porous N-doped carbon nanofibers (NiCo 2- x Fe x O 4 /NCNF), which were synthesized by scalable electrospinning, exhibit a correlated relationship with Fe atomic content and achieve an optimal bifunctional activity (ΔE = 0.74 V) at 0.25 at.%. Theoretical calculation shows that the substitution of Co 3+ by Fe 3+ modulates the electrons filling in e g orbital of octahedral cation via delocalizing the electrons around O anions. The increased density of states around the Fermi level further regulate the adsorption energy of oxygen intermediates and lead to better bifunctional performance than commercial Pt/C + RuO 2 in rechargeable Zn-air battery. This work provides a new pathway to develop cost-effective bifunctional electrocatalysts for electrochemical energy storage and conversion .
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WATER RESEARCH
·
2019
·
IF 7.913
Yuan Yuan,Wei Zhao,Zicheng Liu,Chen Ling,Changqing Zhu,Fuqiang Liu,Aimin Li
The efficient recovery of heavy metals from complexed wastewater is an essential but challenging task. In this study, a novel low-Fe(III) driven UV/Air process (LFUA) was developed to break the strong complexation between ethylenediamine tetracetic acid (EDTA) and heavy metal ions (HMIs) and enable the enhanced recovery of HMIs via chelating resin adsorption (CRA). The inside mechanism of the LFUA process includes: 1) displacement of HMIs from HMI-EDTA complexes by Fe(III); 2) direct photolysis of Fe(III)-EDTA through a ligand-to-metal charge transition reaction (LMCT) and indirect photolysis of EDTA by HO 2 ·/O 2 · - . The iron dosage was orders of magnitude lower than that previously reported, due to the Fe(II)/Fe(III) redox cycle in the LFUA process. Fe(II) formed during the LMCT reaction of Fe(III)-EDTA was oxidized back to Fe(III) by O 2 and HO 2 ·, and the reformed Fe(III) was then recombined with EDTA to sustains the LMCT reaction. EDTA was completely removed in 20 min at a molar ratio of Fe(III)/EDTA = 0.05. In addition, following the LFUA process, the adsorption amounts of various HMIs onto D463 resin were at least two orders of magnitude higher than those reported using the direct adsorption process. Employing the integrated technique of LFUA + CRA enabled the efficient removal of up to 64.5 mg/L of Cu(II) from inlet wastewater, and residual Cu(II) was below 0.5 mg/L. The results of desorption experiments showed that over 90% of Cu(II) was recovered, and the desorption solution had a Cu concentration of 2.1 g/L and purity of 99%. Furthermore, the economic and practical feasibility of using the combined process of LFUA + CRA was analyzed to substantiate that the technique is highly efficient and clean (produces no harmful sludge). Therefore, it is an appropriate and practical process in removing HMIs-EDTA complexes and recovering HMIs from wastewater.
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Biomaterials Science
·
2018
·Vol. 6
·期 5
·1227-1237
·
IF 5.831
Qianwen Li,Donghui Wang,Jiajun Qiu,Feng Peng,Xuanyong Liu
Hard tissue implant materials which can cause a suitable alkaline microenvironment are thought to be beneficial for stimulating osteoblast differentiation while suppressing osteoclast generation. To make the local pH around the interface between materials and cells controllable, we prepared a series of Mg–Fe layered double hydroxide (LDH) films on acid-etched pure titanium surfaces via hydrothermal treatment. By adjusting the Mg/Fe proportion ratio, the interlayer spacing of Mg–Fe LDHs was regulated, making their OH− exchange abilities adjustable, and this ultimately resulted in a microenvironment with a controllable pH value. In vitro experiments demonstrated that the Mg–Fe LDH film-modified titanium surface possessed good biocompatibility and osteogenic activity, especially the Mg–Fe LDH film with Mg/Fe proportion ratio of 4, which could form a suitable alkaline microenvironment for the growth and osteogenetic differentiation of stem cells. These results demonstrate the potential application of the prepared Mg–Fe LDH films in enhancing the osteogenesis of implant materials while providing a new way into the design of controllable alkaline environment.
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Nanoscale
·
2019
·Vol. 12
·期 3
·2022-2027
·
IF 6.97
Chao Peng,Huanhuan Xing,Yuan Xue,Jin Wang,Jing Li,Erkang Wang
Two-dimensional (2D) Mn–Fe layered double hydroxide (LDH) nanosheets are firstly examined to mediate an O-phenylenediamine (OPD) based fluorescent switch in the presence of ascorbic acid (AA). On one hand, Mn–Fe LDH mimicked the functions of oxidase to catalyze the oxidation of OPD to OPDox, emitting fluorescence at 565 nm. On the other hand, Mn–Fe LDH acts as a superior catalyst for the reaction between AA and OPD to generate 3-(1,2-dihydroxyethyl)furo[3,4-b]quinoxalin-1(3H)-one (N-heterocyclic compound) with an emergence of the maximum emission at 425 nm (ca. 6 fold). The presence of AA not only induces the enhanced emission at 425 nm from the N-heterocyclic compound, but also leads to decreased fluorescence at 565 nm due to the decomposition of Mn–Fe LDH nanosheets. On the basis of the reversed fluorescence response at 425 and 565 nm, ratiometric fluorescence sensing methods (ΔF425 nm/ΔF565 nm) are developed for the determination of AA. With the assistance of alkaline phosphatase (ALP), the activity of ALP can be monitored using the ratiometric platform based on the hydrolyzing ascorbic acid 2-phosphate to yield AA with the detection limit of 0.16 mU mL−1. Different from the traditional ratiometric sensing platform, where two fluorescent probes are often introduced, the present ratiometric system derived from one signal precursor holds great potential in developing a facile platform and broadens the application of 2D nanomaterials in the field of biology.
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高影响因子
ANALYST
·
2020
·Vol. 145
·期 19
·6349-6356
·
IF 3.978
Ye Hu,Chaochao Yue,Jing Wang,Yuhua Zhang,Wenhui Fang,Jiaqi Dang,Ying Wu,Hong Zhao,Zengxi Li
Fe–Ni-MOFs with different amounts of Fe are synthesized through a two-step template etching method. Kinetic analysis indicates that Fe–Ni-MOF exhibits prominent intrinsic peroxidase-like activity, which could catalytically oxidize 3,3′,5,5′-tetramethylbenzidine (TMB) to produce oxidized TMB (oxTMB) with a blue color. As a peroxidase-mimicking MOF, Fe–Ni-MOF with its efficient stable catalysis properties is demonstrated to allow a sensitive colorimetric assay for Sn2+ ions. The mechanism is explored, whereby Sn2+ ions could reduce the peroxidase-like activity of Fe–Ni-MOF based on a redox interaction, making the oxTMB color lighter and decreasing the absorbance intensity at 652 nm. The linear determination of the Sn2+ ion concentration using a UV-vis spectrometer ranges from 0.01 mM to 1.0 mM and from 1.0 mM to 4.0 mM. The presented Fe–Ni-MOF-based assay of Sn2+ ions was successfully applied to real water samples.
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高影响因子
Catalysts
·
2019
·Vol. 9
·期 3
·288
·
IF 3.444
Feihu Liu,Zhong Wang,Da Wang,Dan Chen,Fushan Chen,Xuebing Li
The CeO2ordinary amorphous, nanopolyhedrons, nanorods, and nanocubes were prefabricated by the hydrothermal method, and employed as carriers of Fe/W–CeO2catalysts to selectively catalyze the reduction of NO with ammonia. Characterization results indicated that the morphology of CeO2support originated from selectively exposing different crystal surfaces, which has a significant effect on oxygen vacancies, acid sites and the dispersion of Fe2O3. The CeO2nanopolyhedrons catalyst (Fe/W–CeO2–P) showed most oxygen vacancies, the largest the quantity of acid sites, the largest BET (Brunauer-Emmett-Teller) surface area and the best dispersion of Fe2O3, which was associated with predominately exposing CeO2(111) planes. Consequently, the Fe/W–CeO2–P catalyst has the highest NO conversion rate in the temperature range of 100–325 °C among the ordinary amorphous, nanorods, and nanocubes Fe/W–CeO2catalysts.Keywords:morphology;Fe/W–CeO2;nanopolyhedra;CeO2(111) planes
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Nano Research
·
2020
·Vol. 13
·期 8
·2079-2084
·
IF 8.183
Wang Hong-Hui,Lv Li-Bing,Zhang Shi-Nan,Su Hui,Zhai Guang-Yao,Lei Wei-Wei,Li Xin-Hao,Chen Jie-Sheng
The rational design of highly active and stable atomically dispersed M-X 4 (M = Fe, Co, Ni, etc., X = C, N) -based catalysts holds promises for wide application in almost all realms of catalysis. Despite great effort in the construction of specific M-X 4 centers, the possible effect of non-coordinated heteroatoms on the catalytic activity of metal centers has been rarely explored. Herein, we develop a new type of M-X 4 catalyst composed of Fe-N 4 centers and non-coordinated B heteroatoms (FeNC+B) and find the key role of non-coordinated B adjacent to Fe-N 4 centers in tailoring their electron density and final catalytic selectivity. The experimental and theoretical results demonstrated that non-coordinated boron atoms could decrease the electron density of Fe-N 4 centers to a suitable level and thus boost the selective production of nitriles from amine oxidation by depressing the formation of imines due to the flattened energy barrier of the reversible conversion of imines back to amines. As a reusable heterocatalyst, the state-of-the-art FeNC+B catalyst provides a turn-over frequency (TOF) value of 21.6 mol benzonitrile ·mol Fe −1 ·h −1 (100 °C), outpacing that of bench-marked nonnoble-metal-based homogeneous catalyst by a factor of 3.4.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2023
·
IF 4.3
Ruosong He,Yang Wang,Meng Li,Jianxin Liu,Yongqiang Gu,Wenhang Wang,Qiang Liu,Noritatsu Tsubaki,Mingbo Wu
Graphical Core-shell structured Fe-based catalyst Na−Fe 3 O 4 @C with confinement effect delivered higher productivity of light olefins compared with the naked Na−Fe 2 O 3 counterpart. Multiple characterization and DFT calculation verified that the timely carbon chain-growth termination, as well as unique CO 2 /H 2 ratio and electronic property on the catalytic interface played vital roles in boosting light olefins synthesis. Even though Fe-based catalysts have been widely employed for CO 2 hydrogenation into hydrocarbons, oxygenates, liquid fuels, etc., the precise regulation of their physicochemical properties is needed to enhance the catalytic performance. Herein, under the guidance of the traditional concept in heterogeneous catalysis-confinement effect, a core-shell structured catalyst Na−Fe 3 O 4 @C is constructed to boost the CO 2 hydrogenation performance. Benefiting from the carbon-chain growth limitation, tailorable H 2 /CO 2 ratio on the catalytic interface, and unique electronic property that all endowed by the confinement effect, the selectivity and space-time yield of light olefins (C 2 = −C 4 = ) are as high as 47.4 % and 15.9 g mol Fe −1 h −1 , respectively, which are all notably higher than that from the shell-less counterpart. The function mechanism of the confinement effect in Fe-based catalysts are clarified in detail by multiple characterization and density functional theory (DFT). This work may offer a new prospect for the rational design of CO 2 hydrogenation catalyst.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2019
·
IF 2.931
Jiaqi Xian,Yuhui Weng,Hantao Guo,Yan Li,Bixia Yao,Wen Weng
Iron-doped carbon nitride nanoparticles (Fe-CNNPs) were prepared from citric acid , urea and ferric chloride through a convenient one-pot solvothermal method . Oleic acid was used as the reaction medium. The morphology and chemical composition of the obtained Fe-CNNPs were characterized by multiple methods including transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FT-IR). It is interesting to find that the Fe-CNNPs showed higher catalytic activity than horseradish peroxidase (HRP), and tetramethylbenzidine (TMB) can be catalytically oxidized in the presence of H 2 O 2 to produce a color change in aqueous solution. As H 2 O 2 can be generated in the oxidation process of glucose catalyzed by glucose oxidase (GOD), a novel sensitive method for the detection of glucose with a limit of detection (LOD) of 0.29 μM has been developed combined with the catalytic properties of GOD and Fe-CNNPs. The Fe-CNNPs with peroxidase mimetics activity may have potential applications in biotechnology field.
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Nanoscale
·
2025
·
IF 5.1
Longlong Liu,Lanli Chen,Huaming Zhang,Muhammad Humayun,Yuxiao Liu,Junhong Duan,Yanjun Fu,Mohamed Bououdina,Xinying Xue,Chundong Wang
Rational design of low-cost, highly-efficient electrocatalysts for hydrogen and oxygen evolution reactions (HER/OER) is critical to enable sustainable hydrogen production via water electrolysis. Herein, a novel nanorod arrays catalyst, Fe-NiMoN, has been rationally designed and directly grown on nickel foam (NF) via a facile hydrothermal method followed by a nitridation treatment. The novel 3D porous nanorod architecture is favorable for providing abundant active sites, accelerating mass diffusion/electron transfer, and facilitating gas release. In addition, density functional theory (DFT) simulations reveal that Fe doping shifts the d-band center of NiMoN away from the Fermi level compared to the undoped NiMoN, thereby reducing the hydrogen adsorption free energy (ΔGH*) toward 0, and which in turn enhances the HER activity. Consequently, the Fe-NiMoN catalyst delivers exceptional bifunctional electrocatalytic activity in alkaline media, requiring low overpotentials of 17 mV (HER) and 238 mV (OER) to achieve 10 mA cm–2. Notably, the Fe-NiMoN catalyst assembled into a two-electrode alkaline electrolyzer, requires only a voltage of 1.504 to achieve a current density value of 10 mA cm−2, with no performance declining after 100 h of steady operation. Moreover, for urea-assisted electrolysis, it can deliver 10 mA cm−2 at only 1.367 V. Overall, this work provides a strategy for synthesizing desirable electrocatalysts for green hydrogen production coupled with wastewater treatment.
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