JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Huijie Ni,Shaojie Xu,Rong Lin,Yi Ding,Jinjie Qian
There is significant anticipation for high-efficiency and cost-effective non-precious metal-based catalysts to advance the industrial application of the anodic oxygen evolution reaction (OER) for hydrogen production. This study introduces an efficient strategy that utilizes ligand-induced metal–organic framework (MOF) building blocks for the synthesis of hollow binary zeolitic imidazolate frameworks 67 (ZIF-67) and Prussian blue analogues (PBAs) (ZIF-67@PBA) heterostructures through a hybrid MOF-on-MOF approach. Manipulating the Co 2+ /Zn 2+ ratio in the precursor ZIF-67 allows for the convenient synthesis of the final product, denoted as Co x Fe-ZP, after pyrolysis , where the inclusion of Zn effectively modulates the distribution of Co in the catalyst. The resulting Co x Fe-ZP catalysts exhibit a positive synergistic effect between hollow graphitic carbon nanomaterials and Fe-doped Co nanoparticles. The optimal Co 0.3 Fe-ZP catalyst demonstrates satisfactory OER performance, achieving an overpotential of 302 mV at 10 mA cm −2 and a small Tafel slope of 60.0 mV dec −1 . Further analysis of the activation energy confirms that the enhanced OER activity of Co 0.3 Fe-ZP can be reasonably attributed to the combined influence of its morphology and composition. This study demonstrates a ligand-induced method for examining the morphology and electrochemical properties of grown binary MOF-on-MOF heterostructures for OER applications.
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Green Chemical Engineering
·
2024
·
IF 9.1
Ruichang Xue,Rongrong Deng,Yan Li,Mengqiu Gao,Jiafu Wang,Qibo Zhang
Developing electrocatalysts with excellent activity, high stability, and low cost is vital for large-scale hydrogen production through electrochemical water splitting. Herein, a bifunctional Ni–Fe–P catalyst in situ grown on Fe foam (Ni–Fe–P/FF) is developed by a simple one-step solvothermal process in the deep eutectic solvent (DES) of ethylene glycol and choline chloride (named Ethaline). The unique solvent environment of Ethaline assisted with the regulating effect of the introduced Fe(III) ions shows an essential role in governing the preparation process. The developed Ni–Fe–P/FF acts as the efficient bifunctional electrocatalyst for water splitting in 1.0 M KOH, requiring overpotentials of 82 mV (229 mV) and 263 mV (370 mV) to deliver 10 mA cm −2 (100 mA cm −2 ) for oxygen and hydrogen evolution reactions, respectively. Furthermore, the self-supported catalyst-assembled electrolyzer also exhibits good catalytic performance with a low voltage of 1.83 V to drive 100 mA cm −2 and good stability over 100 h. This work offers a facile approach to fabricating high-performance bifunctional Ni–Fe–P electrocatalysts to catalyze water splitting.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Junjie Cheng,Xinman Tu,Pengxuan Wu,Rentao zhou,Shaohua Luo,Li Zhang,Jianping Zou,Yanhong Li,Hannah M. Johnson,Qiang Zhang
In the reaction systems involving peroxymonosulfate (PMS) activation, the degradation of organic pollutants is influenced by the distinct roles played by the oxidation of free radicals and non-free radicals. The synergistic effect resulting from both oxidation pathways is often more efficient compared to a single oxidation pathway, as it allows for the optimal utilization of oxidation capacity and adaptation to complex reaction environments. Nitrogen-doped carbon substrates hosting single-atom catalysts (SACs) are anticipated to serve as an optimal platform for managing the dual oxidation pathways in the PMS activation reaction. This is attributed to the availability of numerous reaction sites that meet the activation requirements. However, there's a lack of substantial reports on this subject. Herein, we synthesized a series of single-atoms Fe nitrogen-doped carbon catalysts with different coordination structures by adjusting the coordination numbers between Fe and N atoms. It is used to investigate the reaction pattern of PMS over SACs, so as to enhance the catalytic efficacy of SACs through distinct coordination structures. The experimental and theoretical results indicate that PMS functions as both an electron receiver and provider on FeN x /C catalysts. Moreover, the specific arrangement of the Fe-N-C structure influences the exchange of electrons between the catalysts and PMS. Hence, the co-oxidation pathway of free radicals ( OH, SO 4 − and O 2 − ) and non-free radicals ( 1 O 2 ) can be modulated by altering the coordination number of Fe and N atoms during PMS activation. The elimination efficiency of tetracycline hydrochloride was significantly enhanced due to the abundance of both free radical and non-free radical species generated in the FeN 3 /C/PMS reaction system, exhibiting a degradation kinetic constant of 0.564 min −1 . In addition, it showed promising potential for application in practical wastewater degradation, exhibiting high anti-interference to general environmental disturbances (such as humic acid, chloride ions, bicarbonate ions and nitrate ions).
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Rui Cai,Ping-an Yang,Haibo Ruan,Xin Huang,Zhihao Zhou,Qiao Chen,Yuxin Zhang,Xinglong Gong,Yingang Gui,Rui Li
How to prepare materials according to the target properties has been a hot research topic. In this paper, the target electromagnetic parameters are obtained according to the performance requirements, and the nanoflower rod-like, low-density mulberry-like and high-density mulberry-like one-dimensional (1D) core–shell structured Fe@Ni ( x ) nanowires (NWs) are prepared by liquid-phase reduction method. The effective absorption bandwidth (EAB) of sample Fe@Ni (40) in the low-frequency (2–8 GHz) is up to 1.89 GHz (3.1 mm). Sample Fe@Ni (60) is able to reach a maximum EAB of 3.18 GHz at a thickness of 0.9 mm. Concisely, the sample has the ability to absorb microwaves in low frequency bands and ultra-thin thicknesses. The reason can be attributed to the strong magnetic coupling brought by the bimetallic composition to strengthen the resonance level and the excellent 1D core–shell structure to enhance the efficiency of polarization loss. In conclusion, Fe@Ni ( x ) provides a technological route for the preparation of low-frequency and ultra-thin-thickness absorbers.
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FUEL
·
2024
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IF 6.7
Wenxia Zhang,Hongtao Zhang,Mohamed Abbas,Juan Zhang,Zhijun Huang,Sibudjing Kawi,Jiangang Chen
The advancement of large-scale and environmentally-friendly solid-state synthesis methods is of paramount importance for the production of precipitated catalysts, notably Fe-based catalysts utilized in Fischer-Tropsch synthesis (FTS). In this study, we present an innovative solvent-independent, wastewater-free solid-state approach for the synthesis of highly efficient Fe/ZrO 2 catalysts, elucidating the mechanisms of promotion within this specific methodology. The prepared catalysts underwent rigorous evaluation under industrially-relevant FTS conditions (230–270 °C, 20 bar, and WHSV = 5400 mL/(g cat ⋅h)). A comprehensive suite of characterization techniques was employed to establish the intricate interplay between catalytic activity and structural attributes. We meticulously examined the impact of Na as an alkali promoter and the role of transition metals (Cu and Mn) in enhancing FTS catalytic performance. The catalytic outcomes obtained clearly demonstrate the pivotal role of the synergistic interaction between Mn and Na within the Na-Mn-Fe/ZrO 2 catalyst system in driving the FTS reaction. This synergism significantly enhances FTS performance, yielding an impressive CO conversion rate (89.91 %) while maintaining low selectivity to CH 4 (7.75 %). The incorporation of Mn and Na into the catalyst matrix enhances the dispersion of Fe 2 O 3 , thereby improving the reducibility of Mn/Fe oxides and elevating the electron density on the catalyst surface. These factors facilitate the formation of active Hägg iron carbide (χ-Fe 5 C 2 ), stimulating chain propagation and ultimately leading to the generation of valuable C 5+ hydrocarbon products, which underscores its potential as an optimal candidate for future industrial applications in Fe-based Fischer-Tropsch synthesis.
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Journal of Water Process Engineering
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2024
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IF 6.3
Linke Jiang,Ruiqi Wang,Shuiqin Shi,Junmei Yan,Mingbao Feng,Lianbao Chi
With the aging of the global population and continued economic development, the use of sartan-type antihypertensive drugs (e.g., losartan (LOS), telmisartan (TEL), and valsartan (VAL)) has increased with widespread contamination issues. However, the effect of advanced oxidation processes (AOPs) on the degradation of sartans remains unknown. Therefore, AOPs such as the Fe(II)/peroxymonosulfate (PMS) system and ozonation were used to treat the typical sartans, which led to the formation of various transformation products (TPs). This research involves the formation mechanisms of these TPs following AOPs including aldolization, hydroxylation, ring cleavage, carbonylation and cyclization. The risk evaluation focused on the biodegradability and toxicity of the drugs and their TPs, assessed using computerized toxicity prediction software. The findings indicated that the biodegradability of most TPs was generally poor and most TPs exhibited acute/chronic toxicity. This underscores the need for caution when applying AOPs in water treatment to prevent secondary contamination and suggests the potential necessity of integrating AOPs with complementary purification technologies. This research provides novel insights into the degradation pathways and environmental risks of sartans, emphasizing the importance of a holistic approach to water treatment.
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Heliyon
·
2024
·
IF 3.4
Yige Yan,Mohan Huang,Yongsheng Wang,Dawei He,Jiaqi He
Metal-organic frameworks (MOF) have been wildly synthesised and studied as electrode materials for supercapacitors, and bimetallic MOF of Ni and Co has been broadly studied to enhance both specific capacitance and stability of supercapacitors. Herein, a best performance (about 320 F/g) of Ni–Co bimetallic MOF was found in a uniform preparation condition by adjusting the ratio of Ni to Co. Then tiny third metal ion was introduced, and we found that the morphology of material has a significant change on the original basis. Furthermore, certain ions (Zn, Fe, Mn) introduced make a huge improvement in capacitance based on Ni–Co MOF of 320 F/g. The result shows that Zn–Ni–Co MOF, Fe–Ni–Co MOF and Mn–Ni–Co MOF perform specific capacitance of 1135 F/g, 870 F/g and 760F/g at 1 A/g, respectively. Meanwhile, the asymmetric supercapacitor (ASC) was constructed by Zn–Ni–Co MOF as positive electrode and active carbon (AC) as negative electrode. The Zn–Ni–Co MOF//AC ASC possesses a energy density of 58 Wh/kg at a power density of 775 W/kg. This research provides a new methods to regulate the morphology of MOF and a novel viewpoint for assembling high-performance, low-price, and eco-friendly green energy storage devices.
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CHEMICAL ENGINEERING JOURNAL
·
2022
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IF 16.744
Xin Yang,Lu Yao,Yu Wang,Xinran Zhang,Pengfei Ren
Algae blooms can clog filtration tank, release toxic cyanotoxin and produce undesirable disinfection byproducts (DBPs) in post-chlorination, which brings challenges to conventional water treatment processes. In this study, peroxymonosulfate (PMS) was tested for its ability to improve Fe(III) coagulation of Microcystis aeruginosa in water treatment. Compared with conventional Fe(III) coagulation, the presence of PMS resulted in the formation of larger floc and thus better algae and turbidity removal. The removal of algae by PMS-enhanced Fe(III) coagulation (PMS-Fe(III)) process reached 97.5% at 1 mM PMS, which was 1.5 times higher than that by Fe(III) coagulation alone. The oxidization of surface-adsorbed extracellular organic matter destabilized the algal cells and enhanced their coagulation without greatly damaging the cells’ integrity. Simultaneously, about 80% of Microcystin-LR, a cyanotoxin, was degraded in the enhanced process. Moreover, the formation of DBPs and their associated toxicity during the subsequent chlorination were decreased by 49.2% and 13.6%, respectively. The production of trihalomethanes, haloacetic acids and haloacetronitriles was particularly abated. SO 4 •- and HO • , which were formed from PMS activation through redox cycling of Fe mediated by the existing natural organic matter, were mainly responsible for algae removal. The results indicate that supplementing Fe(III) coagulation with PMS is a promising option for treating water during algal blooms.
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CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Ziyuan Xiu,Wei Mu,Xin Zhou,Xiaojun Han
The electrocatalytic N 2 reduction reaction (NRR) is expected to supersede the traditional Haber-Bosch technology for NH 3 production under ambient conditions. The activity and selectivity of electrochemical NRR are restricted to a strong polarized electric field induced by the catalyst, correct electron transfer direction, and electron tunneling distance between bare electrode and active sites. By coupling the chemical vapor deposition method with the poly(methyl methacylate)-transfer method, an ultrathin sandwich catalyst, i.e., Fe atoms (polarized electric field layer) sandwiched between ultrathin (within electron tunneling distance) BN (catalyst layer) and graphene film (conducting layer), is fabricated for electrocatalytic NRR. The sandwich catalyst not only controls the transfer of electrons to the BN surface in the correct direction under applied voltage but also suppresses hydrogen evolution reaction by constructing a neutral polarization electric field without metal exposure. The sandwich electrocatalyst NRR system achieve NH 3 yield of 8.9 μg h −1 cm −2 and Faradaic Efficiency of 21.7%. The N 2 adsorption, activation, and polarization electric field changes of three sandwich catalysts (BN-Fe-G, BN-Fe-BN, and G-Fe-G) during the electrocatalytic NRR are investigated by experiments and density functional theory simulations. Driven by applied voltage, the neutral polarized electric field induced by BN-Fe-G leads to the high activity of electrocatalytic NRR.
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JOURNAL OF THERMAL SPRAY TECHNOLOGY
·
2025
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IF 3.3
Zhang Jian,Chen Hongxuan,Pang Xiaotong,Liu Shilong,Misra R. D. K.,Sun Junhao
Currently, surface coatings on agricultural machinery are crucial for extending service life. However, achieving coating strength and toughness remains a challenge. In this paper, two types of high-hardness iron-based coatings, referred as S1 and S2, were prepared by modulating the Mo/V ratio in the Fe-C-V-Mo-B system, and their microstructural evolution and property changes were investigated. The results show that the S1 coating primarily consist of martensitic matrix, spherical VC, blocky Mo 2 B, and a small amount of skeleton-like Mo 2 B. In contrast, the S2 coating consist of martensitic matrix, petal-like VC, and skeleton-like Mo 2 B. Compared with S1, the VC volume fraction in S2 increases by 6.5%, and the Mo 2 B volume fraction increases by 16.3%. The average microhardness of S1 and S2 coatings are 737 HV 0.5 and 954 HV 0.5 , respectively, indicating that the S2 coating exhibits a 22.7% higher microhardness compared with S1. The average friction coefficients of S1 and S2 coatings are 0.434 and 0.398, respectively. Furthermore, the wear loss of S2 coating is approximately half that of S1. The fracture toughness of S1 and S2 coatings are 51.9 MPa·m 1/2 and 51.7MPa·m 1/2 , respectively. Fracture analysis reveals that the skeleton-like eutectic structure in S2 can deflect cracks generated by impact, increase the length of propagation path, and improve the toughness of coating. It allows S2 coating to achieve high hardness and wear resistance, while maintaining toughness comparable to S1 coating. This study provides a theoretical basis for the design and development of iron-based coatings with high hardness, high abrasion resistance, and impact resistance for agricultural machinery.
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Journal of Physical Chemistry C
·
2024
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IF 3.3
Mingjun Xu,Zhao Jin,Meiling Xiao,Changpeng Liu,Wei Xing
Pyrolyzed iron and nitrogen codoped carbon materials (Fe–N–C) with atomically dispersed Fe-Nx sites have received extensive attention as a highly promising alternative to Pt for oxygen reduction reaction (ORR), yet there remains a considerable performance gap between them. To further improve the catalytic performance of Fe–N–C catalysts, we herein developed a microwave-assisted method to improve both the active site density (SD) and intrinsic activity, thus achieving outstanding ORR activity. The in situ generated Fe precipitation is beneficial to improve the doping efficiency of Fe and the subsequent formation of synergetic active sites, leading to increased SD. Both the X-ray absorption spectroscopy and operando Raman confirmed the copresence of atomic Fe moieties and nanoclusters, in which the nanoclusters synergically promote the activity of the single atomic sites. The enriched synergetic active sites endow the as-prepared catalyst with excellent performance by showing a current density of 42 mA cm–2 at 0.9 V in a proton exchange membrane fuel cell, approaching the DOE 2025 target. This work not only affords a highly active ORR catalyst but also provides a simple and potentially scale-up approach to Fe–N–C catalysts.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Bai Jingsen,Zhao Tuo,Xu Mingjun,Mei Bingbao,Yang Liting,Shi Zhaoping,Zhu Siyuan,Wang Ying,Jiang Zheng,Zhao Jin,Ge Junjie,Xiao Meiling,Liu Changpeng,Xing Wei
The limited durability of metal-nitrogen-carbon electrocatalysts severely restricts their applicability for the oxygen reduction reaction in proton exchange membrane fuel cells. In this study, we employ the chemical vapor modification method to alter the configuration of active sites from FeN 4 to the stable monosymmetric FeN 2 +N’ 2 , along with enhancing the degree of graphitization in the carbon substrate. This improvement effectively addresses the challenges associated with Fe active center leaching caused by N-group protonation and free radicals attack due to the 2-electron oxygen reduction reaction. The electrocatalyst with neoteric active site exhibited excellent durability. During accelerated aging test, the electrocatalyst exhibited negligible decline in its half-wave potential even after undergoing 200,000 potential cycles. Furthermore, when subjected to operational conditions representative of fuel cell systems, the electrocatalyst displayed remarkable durability, sustaining stable performance for a duration exceeding 248 h. The significant improvement in durability provides highly valuable insights for the practical application of metal-nitrogen-carbon electrocatalysts.
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