JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY
·
2022
·Vol. 103
·期 2
·505-514
·
IF 2.606
Zou Chang,Guo Xingzhong,Wang Fan,Tian Rui,Hou Yang,Liu Fu,Yang Hui
Three-dimensional macroporous heterostructural Ni-Fe hydroxides with different mole ratio (Ni x Fe (1−x) -PH) were prepared via a sol-gel process combined with phase separation, and the overall water splitting electrocatalytic activity of the resultant macroporous Ni-Fe hydroxides were investigated in detail. The as-prepared Ni-Fe hydroxide has cocontinuous skeletons and interconnected macropores with a narrow pore size distribution (~150 nm), and possesses outstanding electrocatalytic activity with an overpotential of 263 mV for oxygen evolution reaction (OER) and 175 mV for hydrogen evolution reaction (HER) at 10 mA·cm −2 in 1 M KOH, respectively. The Ni 0.6 Fe 0.4 -PH | | Ni 0.6 Fe 0.4 -PH has efficient overall water splitting performance with a cell voltage of 1.61 V at 10 mA·cm −2 and great stability. The fantastic macropore structure and strong synergistic effect between Ni-Fe hydroxides significantly reinforce the contact area between the electrocatalyst and electrolyte, and endow high electrocatalytic performance of bifunctional electrocatalysts.
The epoxide-induced sol-gel process accompanied by phase separation allows the synthesis of macroporous heterostructural Ni-Fe hydroxide bifunctional catalyst with a mass of active sites, displaying excellent electrocatalytic activity and low overpotential at several current densities for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER).
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 18
·8611-8618
·
IF 3.925
Jing Huang,Qi Shan,Yanan Fang,Ning Zhao,Xiaomiao Feng
A new simple strategy to prepare Mn–Fe Prussian blue analogue (PBA) derived oxide micromotors through co-precipitation and heat treatment is demonstrated. The morphology of the precursors could be precisely controlled from cubic-like to spherical-like by introducing citrate. Because of the synergistic catalytic reaction of bimetallic Mn–Fe oxides, micromotors with different shapes could be powered efficiently in H2O2 solution. In particular, the obtained cubic Mn–Fe oxide micromotors showed strong propulsion at a speed of 71.21 μm s−1 in 1% H2O2 solution. With dual mechanisms of adsorption bubble separation (ABS) and Fenton oxidation, the cubic Mn–Fe oxide micromotors showed extraordinary removal ability for Rhodamine B (RhB) as a simulated pollutant and could remove up to 95.2% of RhB within 30 minutes. Magnetic Fe3O4 contained in the component not only could degrade organic pollutants, but also could be recycled by magnetic field and reused with high degradation efficiency. These dual-functional metal oxide catalytic micromotors provide a practical and environmentally friendly strategy for environmental restoration.
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CATALYSIS TODAY
·
2022
·
IF 6.562
Xinyu Guo,Bo Liu,Xinhua Gao,Fugui He,Qingxiang Ma,Subing Fan,Tian-sheng Zhao,Jumei Tian,Prasert Reubroycharoen,Jianli Zhang
The hydrophilic/hydrophobic properties of catalysts greatly influence product distribution by tuning the secondary reactions during Fischer–Tropsch synthesis. Studies have confirmed that hydrophilic modification can inhibit secondary reactions. Herein, hydroxyapatite (HAP)-supported Fe catalysts (Fe/HAP) were prepared using an impregnation method. The effect of the catalyst surface properties on the product distribution in CO hydrogenation was studied. The surface hydroxyl groups on Fe/HAP promoted the growth of carbon chains and improved olefin selectivity. The addition of Na as a promoter to Fe/HAP suppressed the formation of undesirable CH 4 , further improving the selectivity for light olefins and C 5 + hydrocarbons. Compared with Fe 2 O 3 , Fe/HAP showed lower CH 4 selectivity (15%) and higher C 5 + selectivity (45%). Meanwhile, the Fe/HAP -Na catalysts with a higher selectivity of light olefins (with an O/P ratio reaching 4.51).
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JOURNAL OF SOLID STATE CHEMISTRY
·
2022
·
IF 3.656
Zhipeng Zhang,Feifei Li,Guoqiang Li,Rui Li,Yunfang Wang,Yawen Wang,Xiaochao Zhang,Lulu Zhang,Fangfang Li,Jianxin Liu,Caimei Fan
The bottlenecks of photocatalytic nitrogen fixation are adsorption and activation of nitrogen, because N–N bond in dinitrogen is one of the strongest bonds in chemistry . Herein, for the first time, Cu-doped MIL-101(Fe) was applications in photocatalytic nitrogen fixation. The photocatalytic nitrogen fixation activity of Cu-MIL-101(Fe) is three times that of MIL-101(Fe). Characteristic of MIL-101(Fe) and Cu-MIL-101(Fe) are systematically compared by XRD , SEM, TEM, BET, PL and energy band structure . These results indicated that the Cu doping not only enlarge the specific surface area from 1413 m 2 /g to 2097 m 2 /g, but also increase the photoreduction capability from −0.13 V to −0.7 V. These results indicated that nitrogen adsorption and activation capacity can be improved by Cu doping. By combining metal ions doping and components regulation of MOFs , this work provides many future opportunities for enhance photocatalytic nitrogen fixation activity.
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COMBUSTION AND FLAME
·
2023
·
IF 4.4
Erhai An,Yihong Tan,Kehua Han,Xiaoxia Li,Xiong Cao,Yingxin Tan,Peng Deng
Molecular perovskite energetic material DAP-4 is seen as a potential high-energy oxidant due to its high energy, high density, high oxidation capacity, and facile preparation technology. However, optimizing its energy release and reducing its thermal decomposition temperature are huge challenges for its future application. In this work, the role of iron (Fe) nanospheres in the energy release of DAP-4 was studied. Our research has shown that Fe powder can not only serve as a fuel to promote combustion, but also as an important catalyst to significantly improve the thermal decomposition, energy release, and burning rate of DAP-4. By adding 25% Fe nanospheres, the decomposition temperature of DAP-4 was reduced to 299.7 °C, which is the most reduction by 84.7 °C from 384.4 °C (raw DAP-4) to 299.7 °C (DAP-4/Fe-5 with 25wt% Fe nanospheres) was obtained. The decomposition activation energy also decreases by at least 69.5 kJ mol −1 from 229.4 kJ mol −1 (DAP-4) to 159.9 kJ mol −1 (DAP-4/Fe-1 with 5wt% Fe nanospheres). The combustion performance of DAP-4/Fe composites is significantly improved by a 4∼5 times shorter burn rate. The energy-releasing mechanism of DAP-4 with the presence of Fe nanospheres was proposed. Fe x O y at the surface of Fe nanospheres played an important role in the energy releasing of DAP-4. This work showed a new idea for the potential application of molecular perovskite energetic materials.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hailong Liao,Heping Xie,Shuo Zhai,Ling Fu,Yuan Zhang,Senran Hao,Bin Chen,Chuanxin He,Zongping Shao
Aqueous Zn-CO 2 batteries are a new technology for reducing carbon dioxide emissions and converting CO 2 into valuable products. The development of high-performance catalysts is crucial for improving the efficiency of the CO 2 reduction reaction(CO 2 RR) in these batteries. The technical challenges of CO 2 RR catalysts include high cost, complicated synthesis and low Faraday efficiency. In this study, we developed an efficient and cost-effective CO 2 RR perovskite catalyst, by partially substituting Fe to the B site of precious metal-free La 0.5 Sr 0.5 MnO 3 (LSM) perovskite. Comprehensive investigation into the Structure, morphology, coordination information and electrochemical performance of pristine La 0.5 Sr 0.5 MnO 3 (LSM) and substituted La 0.5 Sr 0.5 Fe 0.6 MnO 3 (LSF 0.6 M) catalysts were conducted, LSF 0.6 M catalyst shows enhanced electrochemical performance, Faraday efficiency, battery durability and battery power density than LSM. Specifically, the Fe-doped catalyst shows a significant improvement in CO 2 reduction reaction (CO 2 RR) performance, with an 80% increase in current density, an 82% Faraday efficiency, and a 50% increase in power density of Zn-CO 2 battery. Characterization experimental results and DFT calculation reveal that Fe substitution can increase the perovskite lattice size to favor CO 2 absorption and *COOH formation, thus the improved CO yields. These analyses provided insights into the underlying mechanisms of the catalyst's performance in CO 2 RR within the battery system. These results highlight LSF 0.6 M perovskite as a very promising CO 2 RR electrocatalyst for Zn-CO 2 battery.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Xiumin Yang,Sijia Lv,Liyong Gan,Chun Wang,Zhi Wang,Zhonghai Zhang
A single-atom catalyst (Fe SAs/–N-C) with excellent stability and conductivity was strategically fabricated via high-temperature calcination using the NiFe layered double hydroxide (LDH)/ZIF-8 composite as precursors. With the help of Ni as a catalyst, a great number of carbon nanotubes were produced whereby the isolated carbon bulks were interconnected to form an “island-bridge”-like 3D network structure, which greatly enhanced the exposure of active sites and the electron transfer. Accordingly, caffeic acid (CA) with versatile biological and pharmacological activities was chosen as the model analyte. The Fe SAs/–N-C with Fe–N4 as the catalytic active site was employed to establish the electrochemical sensing of CA with satisfactory sensitivity, selectivity, and long-term stability. This work expands the application range of single-atom catalysts and contributes a significant reference for the synthesis of hybrid double-atom catalysts.
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PubMed
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ziyuan Xiu,Feng Wei,Xin Zhou,Xiaojun Han
Achieving high ammonia yield and Faraday efficiency is a long-sought-after goal in electrochemical N 2 fixation. Yet, the competitive hydrogen evolution in nitrogen reduction process and the low local concentration of nitrogen on the working electrode still limited the electrocatalytic performance. In the present contribution, a Fe-MoSe 2 nanosheet functioned with C18-thiol as a nano-hydrophobic surface was rationally constructed, which efficiently facilitated the three-phase contact of gas (N 2 ), liquid (H 2 O electrolyte), and solid (electrocatalyst). The fabrication of modified hydrophobic surface not only overcame the mass transfer limitation of N 2 and increased the local concentration of N 2 molecules on the catalyst, but also reduced the proton contact with electrocatalyst to inhibit HER. The three-phase electrocatalytic system achieved a high NH 3 yield of 34.75 μg h −1 mg −1 and outstanding Faraday efficiency of 23.31%. The adsorption and activation processes during NRR process were systematically investigated by the combination of experimental results and density function theory (DFT) simulations.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Xingxing Huang,Yingzhang Shi,Cheng Liu,Zhiwen Wang,Jinhong Bi,Jimmy C. Yu,Ling Wu
A series of Cu 2 O clusters/MIL-100(Fe) heterojunctions with different Cu 2 O mass ratios were constructed as the photocatalysts for N 2 fixation. An optimal nitrogen fixation performance of 51.22 μmol·g −1 ·h −1 is achieved when the mass fraction of Cu 2 O is 20 %. Isotope analysis experiments confirmed that the nitrogen source is N 2 . Possible intermediate signals during photocatalytic reactions were detected by in situ DRIFTS. XPS results further confirm the formation of Cu 2 O/MIL-100(Fe) heterojunctions, and that the existence of Cu–O surface interactions is the key to efficient electron transfer. It is revealed that the improvement of the catalytic performance is derived from the formation of heterojunction which regulates the energy band structure as well as promotes the separation of photogenerated electron-hole pairs. This study proposes a possible mechanism of photocatalytic nitrogen fixation and emphasizes the role of surface interaction and electron transfer in type-II heterojunction in improving nitrogen fixation performance.
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ENERGY
·
2021
·
IF 7.147
Genyang Tang,Jing Gu,Zhen Huang,Haoran Yuan,Yong Chen
Biomass-derived chemical looping gasification (BCLG) is a novel technology for lignocellulose energy applications . Ca–Fe oxygen carriers have been proven to be a potential material for efficient lignocellulose conversion and hydrogen-enriched syngas production in process studies. In this study, Thermogravimetry-mass spectrometry (TG-MS), pyrolysis chromatography-mass spectrometry (Py-GC-MS) and fixed-bed experiments were conducted, and the cellulose BCLG product was analyzed to explore the mechanism of reaction between Ca–Fe OCs and biomass char or volatiles. The mechanism of the synergistic effect of Ca–Fe was analyzed to explain the characteristics of the OCs. The results suggest the Ca-based materials act as catalysts to promote the decomposition of cellulose monomers at primary reaction and char at secondary reaction, and also promote the reforming and oxidation of volatiles by chemisorption . Ca participates in the construction of inert substances, such as Ca 2 Fe 2 O 5 , to avoid the deep oxidation of CO and H 2 . Fe-based material supplies oxygen and promotes the reforming of volatile. Compared with Fe 2 O 3 and CaO/Fe 2 O 3 , CaFe 2 O 4 shows a better performance on carbon conversion and H 2 production below 850 °C.
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Scientific Reports
·
2021
·Vol. 11
·期 1
·1-11
·
IF 4.38
Ye Jien,Wang Yi,Xu Qiao,Wu Hanxin,Tong Jianhao,Shi Jiyan
Passivation of nanoscale zerovalent iron hinders its efficiency in water treatment, and loading another catalytic metal has been found to improve the efficiency significantly. In this study, Cu/Fe bimetallic nanoparticles were prepared by liquid-phase chemical reduction for removal of hexavalent chromium (Cr(VI)) from wastewater. Synthesized bimetallic nanoparticles were characterized by transmission electron microscopy, Brunauer–Emmet–Teller isotherm, and X-ray diffraction. The results showed that Cu loading can significantly enhance the removal efficiency of Cr(VI) by 29.3% to 84.0%, and the optimal Cu loading rate was 3% (wt%). The removal efficiency decreased with increasing initial pH and Cr(VI) concentration. The removal of Cr(VI) was better fitted by pseudo-second-order model than pseudo-first-order model. Thermodynamic analysis revealed that the Cr(VI) removal was spontaneous and endothermic, and the increase of reaction temperature facilitated the process. X-ray photoelectron spectroscopy (XPS) analysis indicated that Cr(VI) was completely reduced to Cr(III) and precipitated on the particle surface as hydroxylated Cr(OH) 3 and Cr x Fe 1−x (OH) 3 coprecipitation. Our work could be beneficial for the application of iron-based nanomaterials in remediation of wastewater.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2020
·
IF 3.99
Jiahui Deng,Yalin Cheng,Min Liu,Biyang Tu,Shan Xue,Haisheng Tao
In this study, Fe-Mn co-embed sodium alginate carbon spheres (Fe-Mn/SA-C) were prepared as a cost-effective adsorbent for aqueous Cd(II) removal by a facile pyrolysis method. The morphology and chemical composition of Fe-Mn/SA-C were explored with various characterized techniques. The results indicate that Fe-Mn/SA-C possess porous structures and abundant oxide-based functional groups. Fe-Mn/SA-C exhibits excellent adsorption properties for aqueous Cd(II) and the adsorption process is pH-dependent. The adsorption data could fit pseudo second-order and Langmuir models well, suggesting that chemisorption is a dominant adsorption mechanism and the maximum adsorption capacity is 280.11 mg −1 . Thermodynamic analysis demonstrates that the adsorption is spontaneous and endothermic. The adsorption mechanisms of Cd(II) include the complexation of Cd(II) with oxygen-based functional groups, precipitation, and ion exchange. Finally, the granulated and magnetic Fe-Mn/SA-C is an efficient and practical adsorbent for cadmium-containing wastewater treatment.
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