METALLURGICAL AND MATERIALS TRANSACTIONS B-PROCESS METALLURGY AND MATERIALS PROCESSING SCIENCE
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2022
·Vol. 53
·期 4
·2634-2646
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IF 2.872
Huang Jingdong,Sohn Il,Kang Youngjo,Yang Xiao
Earth’s commercial and affordable zinc reserves are expected to be depleted in less than 50 years. Since electric arc furnace (EAF) dust contains a certain amount of Zn, recovery of Zn from EAF dust has become an important issue to assure a sustainable resource supply in the future. The key technical challenge is that Zn mainly occurs in EAF dust as ZnFe 2 O 4 , a very stable crystal which is difficult to reduce or leach. MgCl 2 is believed to be effective in breaking the structure of ZnFe 2 O 4 . This work investigates the fundamentals of the reaction between MgCl 2 and ZnFe 2 O 4 . Experiments show that Zn in ZnFe 2 O 4 is chlorinated to ZnCl 2 quickly with priority over Fe, implying the efficacy of MgCl 2 in separating Zn and Fe in ZnFe 2 O 4 by selective chlorination. Effects of MgCl 2 /ZnFe 2 O 4 molar ratio and temperature on the reaction are clarified. Overuse of MgCl 2 slows down the reaction and is detrimental to the selective chlorination of Zn. Temperature can effectively increase the reaction rate as well as the priority of chlorinating Zn. Utilization of MgCl 2 could be high, because evaporation of MgCl 2 is not as fast as the reaction with ZnFe 2 O 4 . According to these results, a new technology to recover Zn from EAF dust by using MgCl 2 is proposed.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Yi Liang,Peng Zhao,Jilin Zheng,Yuanyuan Chen,Yiyi Liu,Jia Zheng,Xiaogang Luo,Danqun Huo,Changjun Hou
Reasonable sensor construction for precisely real-time detecting H2O2 produced from living cells has always been of great significance and challenges. Due to the excellent catalytic efficiency and unparalleled peroxidase-like activity, single-atomic catalysts with Fe-Nx active sites show great potential in H2O2 detection. These special atomic active sites make it easier for the Fenton reaction to occur, which provides basic support for H2O2 sensors. Their application in the in situ real-time detection of H2O2 has important market prospects. Herein, single-atomic Fe catalysts with distorted graphitic carbon are obtained through a simpler preparation method. A precursor hemin@zeolitic imidazolate framework-8 (hemin@ZIF-8) is calcined at a high temperature and carbonized to get the nitrogen-carbon codoped Fe single atoms (Fe SAs-N/C) and then successfully prepare a H2O2 electrochemical sensor by modifying it on a glassy carbon electrode (GCE). Its peroxidase activity is calculated by enzymatic kinetics, which shows a better peroxidase activity compared with horseradish peroxidase and other reported single-atom (SA) materials. Moreover, the electrocatalytic kinetics is explained by Laviron calculation, which more directly confirms that it has a faster electron transfer rate. Importantly, Fe SAs-N/C@GCE has a wider linear range than sensors combined with other SA materials and a low detection limit of 0.34 μM. It is an attractive design of H2O2 sensors and single-atomic catalysts with superior substrate affinity that are novel alternatives to natural enzymes.
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高影响因子
JOURNAL OF CATALYSIS
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2022
·
IF 8.047
Minjie Xu,Xianglin Liu,Guiyao Song,Yingying Cai,Bianfang Shi,Yitao Liu,Xiaoxu Ding,Zixu Yang,Pengfei Tian,Chenxi Cao,Jing Xu
Different iron species exhibit distinct activity and selectivity in CO 2 hydrogenation reaction. Herein, by controlling calcination temperature, Fe-Al interaction in Na promoted Fe-Al catalysts has been regulated, which further leads to various compositions of iron oxide (FeO x ) and iron carbides (Fe 7 C 3 and Fe 5 C 2 ) after CO activation and CO 2 hydrogenation reaction. The phase compositions and structures of Fe-Al catalysts are carefully distinguished by multiple characterizations, including XRD, XPS, MES and TEM, and the reactivity of different phases is studied with the combination of experiments (kinetics, TP and in situ DRIFTS) and Density Functional Theory (DFT) calculations. Our FeAl350 with the highest FeC x content shows the highest CO 2 conversion of 48.2% and the lowest CO selectivity of 10.1%, and FeAl900 with the highest Fe 5 C 2 / FeC x ratio presents the highest C 5+ selectivity of 44.6%. Finally, a correlation between different compositions of iron species with the activity and selectivity of Fe-based for CO 2 hydrogenation to olefins was established.
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JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY
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2022
·Vol. 103
·期 2
·505-514
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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
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2022
·Vol. 46
·期 18
·8611-8618
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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
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2022
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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
高影响因子
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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