ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 34
·期 2
·2308849
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IF 19
Yashuai Pang,Minsen Xie,Xinghao Lu,Zhao Wan,Zhuohang Zhong,Waqas Muhammad,Xiang Long Huan,Yinghua Niu,Zhen Zhang,Weiqiang Lv
Lithium–sulfur (Li–S) batteries have attracted wide attention as high-energy-density energy storage devices, but their practical applications are hindered by the severe shuttle effect and sluggish kinetics of lithium polysulfides (LiPSs). To address these challenges, polar mediators are employed to chemisorb and catalyze LiPSs, but most of them suffer from low electronic conductivity and poor catalytic activity. Here, a novel strategy is reported to enhance both properties by dispersing Fe(III) atoms in VO 2 nanoribbons(Fe-VO 2 ), creating electronic metal-support interactions (EMSI) that modulate the electronic structure and charge transfer of VO 2 . Theoretical calculations reveal that EMSI lowers the energy barrier for the decomposition of Li 2 S from 1.60 to 1.32 eV and increases the electronic conductivity of VO 2 . Fe doping reduces the Li-ions diffusion barrier from 1.42 eV in VO 2 to 0.99 eV in Fe-VO 2 . The Fe-VO 2 catalyst shows strong adsorption and fast converstion of LiPSs, resulting in high energy density and long cycling life of Li-S batteries. The cathode with Fe-VO 2 maintains a higher capacity retention of 67% after 500 cycles at 1 C, compared with 52.4% and 53.6% for the carbon black based cathode and VO 2 based cathode, respectively. This work demonstrates the potential of EMSI for designing efficient catalysts for Li–S batteries and provides new insights into the electronic structure engineering of polar mediators.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jiahang Liu,Xiaoyang Li,Yingying Chu,Ling Yuan,Ruolin Lv,Weiming Zhang
The conventional Fe(III)/H 2 O 2 system is of low efficiency on the removal of most organic pollutants. However, we discovered that the Fe(III)/H 2 O 2 system was robust on remediating tetracycline (TC) in water (0.109 min −1 for the pseudo-first kinetic constant), and the reaction was even slightly faster than that in the conventional Fe(II)/H 2 O 2 system (0.105 min −1 ). The addition of TC could also initiate the degradation of other refractory pollutants in the Fe(III)/H 2 O 2 system. Complexation between Fe(III) and TC with the stoichiometric ratio of 1:1 was observed. Electron transfer from TC to Fe(III) gave rise to the slight production of Fe(II), which served as the initiator of the following Fenton reaction. •OH was ascertained as the main reactive species through quenching experiments, EPR tests and the probe method, while O 2 • − /HO 2 • was also a subsidiary contributor. Hydroquinone intermediates were proved to be generated through the hydroxylation of the benzene ring of the TC molecule by •OH and thus facilitate the reductive transformation of Fe(III) to Fe(II). This study analyzes the relationship between molecular structural features of TC and the catalytic efficiency of ferric Fenton-like reactions. We expect to shed light on new mechanistic insights on autocatalysis in the Fenton-like catalytic processes.
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Xiao Lin,Zhongyu Long,Long Jiang,Zhiyuan Liu,Changyong Liu,Zhangwei Chen
High-performance SiOC(Fe) wave-absorbing ceramics, containing a large number of carbon nanowires, were successfully prepared using a combination of photopolymerization 3D printing technology and the polymer-derived ceramic pyrolysis method. By employing an optimized segmented slow heating scheme with extended holding time, the pyrolysis of SiOC(Fe) ceramics at 1000 °C facilitated the growth of carbon nanowires, Fe 3 C and SiO 2 grains. These carbon nanowires were interlaced and interconnected within the samples, forming abundant conductive networks. This highly conducive network efficiently converted electromagnetic energy into thermal energy, effectively dissipating electromagnetic waves, and consequently enhancing the microwave absorption performance of ceramics. Moreover, this approach not only reduced ceramic cracks but also improved the dielectric loss performance of the materials, achieving a minimum reflectivity value of −35.72 dB. The SiOC(Fe) ceramics added with 5 wt% VcFe effectively enhanced the magnetic loss of the material, reduced the difference between the relative complex permeability (μ r ) and the relative complex dielectric constant (ε r ), and improved the impedance matching between the material surface and air, thereby further improving its microwave absorption performance. This resulted in an increase in the maximum effective absorption bandwidth of the material to 12.7 GHz at 5 mm. This study offers a promising solution for the preparation of ceramic matrix composite materials incorporating carbon nanowires, magnetic particles and ceramic precursors, which would be potentially valuable for radar detection and sensor applications .
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ChemCatChem
·
2021
·Vol. 13
·期 11
·2683-2690
·
IF 5.686
Xinxin Jin,Yan Xie,Junhong Fu,Chaoyue Zhao,Yinghao Xu,Yang Lv,Bingsen Zhang,Keju Sun,Rui Si,Jiahui Huang
Graphical ORR : We fabricated a FeSA/HNPC electrocatalyst with well atomically dispersed FeN 4 species. DFT calculations uncovered that the single-atomic FeN 4 sites within FeSA/HNPC electrocatalyst present in the configurations of pyrrole-N 4 −Fe are more favorable than those of pyridine-N 4 −Fe for boosting ORR performances. Atomically dispersed Fe−N−C electrocatalysts have displayed excellent catalytic performances towards the oxygen reduction reaction (ORR), while the identification of the genuine active sites remains a challenge. Herein, we report a Fe−N−C electrocatalyst of FeSA/HNPC featuring single-atomic FeN 4 sites on hierarchically N-doped porous carbon (HNPC), which shows a very competitive ORR activity in alkaline solution even at a low electrocatalyst loading of 0.2 mg cm −2 on the working electrode. A comparison of energy barriers in ORR reveals that the single-atomic FeN 4 active sites in FeSA/HNPC existing in the form of pyrrole-N 4 −Fe is more favorable than that of pyridine-N 4 −Fe for the enhanced ORR activity. Understanding the nature of FeN 4 active sites will greatly benefit the design of Fe−N−C electrocatalysts with highly effective ORR performances.
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ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Xiang Liang,Wenhui Feng,Dong Liang,Yan Xu,Xiaoqing Qiu
Hydroxyl/amino and Fe(III) co-grafted graphite carbon nitride (CN) is fabricated via alkaline hydrothermal treatment and followed by an impregnation adsorption process. In this unique fabrication, hydroxyl and amino groups enriched on the surface play a vital role in improving the adsorption capacity for volatile organic compounds (VOCs), while the grafted amorphous Fe(III) clusters could dominantly regulate the path of molecular oxygen activation via photo-Fenton reaction, and change the selectivity of intermediate reactive oxygen species (ROS) with the assistant of the rich surficial hydroxyl groups. Meanwhile, both the grafted functional groups and Fe(III) clusters can serve as photogenerated charge acceptors for collaboratively accelerating carriers' separation. Besides, the Fe(III)-mediated interfacial charge transfer effect (IFCT) also could extend visible light absorption and boost carriers’ generation. Benefiting from the virtues of the complementary and synergy of the grafted hydroxyl/amino and Fe(III), the dual-functionalized CN is qualified as an efficient photocatalyst for removal of VOCs, which exhibits 22 and 18 times isopropanol (IPA) adsorption capacity and CO 2 production than of pristine CN during photocatalytic IPA removal, respectively. Moreover, this work provides a new strategy of surficial group-cluster bifunctionalization for systematically improving sustainable solar-to-chemical energy conversion towards VOCs mineralization.
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Tao Zhang,Xiaoying Jin,Gary Owens,Zuliang Chen
Dye-contaminated wastewater resulting from rapid industrialization and urbanization is a global problem. In this study, a ZIF-8@Fe/Ni sample was synthesized for the removal of malachite green (MG), removing more than 99% of an initial MG concentration of 50 mg L −1 within 120 min with a 318 K adsorption capacity of 151.520 mg g −1 . To understand the dye removal mechanism based on adsorption and reduction, ZIF-8@Fe/Ni was characterized by various techniques. XRD showed that the ZIF-8@Fe/Ni composite had a characteristic peak attributable to Fe/Ni around 44.8°, where the presence of Fe/Ni did not affect the structure of ZIF-8. SEM confirmed that ZIF-8@Fe/Ni was successfully prepared, while XRD and FTIR revealed that the structure of ZIF-8@Fe/Ni remained stable following the introduction of Fe/Ni. XPS showed that while Fe/Ni nanoparticles existed in ZIF-8-Fe/Ni, partial oxidation also occurred. GC–MS demonstrated the creation of two major MG degradation products, (4-aminophenyl) (phenyl) methanone and 4-aminophenol. While the overall adsorption process of MG to ZIF-8@Fe/Ni conformed to pseudo-second-order kinetics, degradation followed pseudo-first-order reduction kinetics. When applied to the remediation of wastewater, ZIF-8@Fe/Ni removed 92% of MG. Overall, this study demonstrated that ZIF-8@Fe/Ni could be a promising material for the treatment of wastewater.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Libo Zhang,Lianxiang Qiu,Qingyao Zhu,Xiong Liang,Jingxiong Huang,Mengting Yang,Zhenxuan Zhang,Jiang Ma,Jun Shen
Water disinfection would result in unintended formation of halogenated disinfection by-products (DBPs) which pose potential harm to human health. In present work, Fe 78 Si 9 B 13 amorphous ribbons (Fe-Si-B AR ) showed excellent catalytic degradation performance towards an aromatic DBP, 3,5-dichlorosalicylic acid (3,5-DiClSA) by Fenton-like reaction. The catalytic degradation performances of Fe-Si-B AR , Fe 78 Si 9 B 13 crystalline ribbons (Fe-Si-B CR ) and iron powders towards 3,5-DiClSA were compared, and Fe-Si-B AR (0.0166 min −1 ) showed the fastest degradation rate. The faster surface mobility of Fe-Si-B AR , which made it easy for Fe 2+ to be oxidized by H 2 O 2 , facilitated the degradation process. High-valent iron of Fe IV could be generated which accounted for degradation of 3,5-DiClSA. The Fe-Si-B AR also showed better and better catalytic performance in 10 reuse cycles. Besides, the cytotoxicity tests indicated that the overall toxicity level of 3,5-DiClSA was declined by 88.1 % after degradation by Fe-Si-B AR . Our results showed that Fe-Si-B AR is a promising catalyst for the degradation of aromatic DBPs.
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Journal of Water Process Engineering
·
2021
·
IF 5.485
Qiuya Zhang,Jun Xu,Xiaoyan Ma,Jinmei Xu,Zeping Yun,Qiaosheng Zuo,Liping Wang
Metal-organic frameworks (MOFs) are new porous materials that attract wide attention due to their environmentally-friendly photocatalytic characteristics. However, poor charge separation in most MOFs largely limits their photocatalytic activity. In this study, a novel Fe-based bi-MOFs heterojunctions material, namely NH 2 -MIL-88B(Fe)@MIL-100(Fe) was prepared by internal extended growth of MIL-100(Fe) on spindle-like NH 2 -MIL-88B(Fe). Compared with pure NH 2 -MIL-88B(Fe) and MIL-100(Fe), the synthesized Fe-based bi-MOFs structure catalyst displayed excellent photocatalytic degradation of tetracycline (TC), with optimal removal of 99.9% achieved in 90 min under neutral conditions. This result is attributed to the sufficient visible light absorption , and the enhanced separation and transfer of h + and e − by the bi-MOFs structure. In particular, ∙O 2 − , h + and ∙OH showed synergistic effects in the photodegradation process, and Fe-based bi-MOFs displayed high stability after five cycles. The inhibition ratio of luminescent bacteria of the degraded solution was lower than 24%, indicating the high efficiency and safety of this Fe-based bi-MOFs for the treatment of antibiotic-contaminated water.
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JOURNAL OF MAGNETISM AND MAGNETIC MATERIALS
·
2021
·
IF 2.993
Desheng Pan,Qifeng Kuang,Peng Tong,Wei Tong,Liubing Fan,Jing Zhao,Da Li,Chuljin Choi,Zhidong Zhang
Challenges still remain in producing room-temperature ferromagnetism/ferrimagnetism in inorganic–organic hybrid compounds. Here, we report the Fe vacancy-doped inorganic–organic (Fe x Se 2 ) 2 Fe(dien) 2 (dien = diethylenetriamine, x = 0.86) hybrid cuboids by self-assemble of finite one-dimensional (1D) FeSe 2 chains and Fe(dien) 2 complexes. A growth model is proposed by kinetically controllable syntheses of novel Fe 2x+1 Se 4 (dien) 2 hybrids. The Rietveld refinement reveals that Fe vacancies in the Fe 2.71 Se 4 (dien) 2 hybrid cuboids induce large distortions of the FeSe 2 chains and the room-temperature lattice parameters are a = 9.225(4) Å, b = 18.021(8) Å and c = 11.609(6) Å. Magnetic measurements and electron spin resonance spectra of the Fe 2.71 Se 4 (dien) 2 hybrid cuboids show the ferrimagnetism with the Curie temperature (T C ) of 600 K and the spin glass state with the freezing temperature (T f ) of 108 K. Impressive room-temperature ferrimagnetic properties of the Fe 2.71 Se 4 (dien) 2 hybrid cuboids were ascribed to the high concentration of Fe 3+ vacancies (0.29 per cell) in the hybrid cuboids, which is supported by the 57 Fe Mössbauer spectrum fitting based on the ferrimagnetic model.
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CRYSTENGCOMM
·
2021
·Vol. 23
·期 13
·2538-2546
·
IF 3.545
Min Yang,Guangshe Li,Huixia Li,Junfang Ding,Yan Wang,Liping Li
Manipulating the growth behavior of nano-sized supports is proved to have extremely favorable effects for optimizing the performance of hybrid catalysts. Herein, we investigated the growth kinetics of MgFe2O4 and revealed its size-dependent behavior of Fe occupancies at octahedral and tetrahedral sites and CO oxidation catalytic activity for the first time. MgFe2O4, with particle size ranging from 8.1 nm to 190.0 nm, was prepared via a sol–gel method after post-annealing treatment at a temperature from 400 °C to 1000 °C. The growth of MgFe2O4 nanoparticles obeys the Ostwald ripening mechanism with the quantitative formula D5 = 2.08 × 1014t exp(−122.13/RT). The systematic characteristics show that the redox behavior and O2 activation of hybrid catalysts of Pt/MgFe2O4-T rely on the grain size of MgFe2O4 nanoparticles. The Pt/MgFe2O4-500 catalyst with a support size of 20.6 nm exhibits a remarkable CO oxidation performance due to its abundant chemisorbed oxygen species on the surface and enhanced metal–support interactions among all examined catalysts. Our findings offer significant insight into the size-dependent structure, redox ability and oxygen activation properties of spinel materials and can greatly impact future exploration of novel materials in heterogeneous catalysis.
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APPLIED ENERGY
·
2021
·
IF 9.746
Yunlei Zhao,Bo Jin,Xiao Luo,Zhiwu Liang
Many works have focused on the reactivity and valence transition of Fe-based oxygen carriers in chemical looping partial oxidation reforming process. However, the reforming performance and impacts of operating factors are unclear with the co-feeding of CaO being CO 2 carrier to realize simultaneous CO 2 capture and utilization. In this work, thermodynamic equilibrium calculation, reactivity test and material characterization are carried out to optimize the process characteristics. The impacts of feeding conditions (Fe/Al weight ratio, methane amount, Ca/Fe mole ratio and packing manner) on the reforming reactivity are obtained to reveal the interaction between CaO and Fe 2 O 3 . The gas product distribution indicates that the carbon deposition and oxidation degree is closely related to CH 4 amount. The spatial configuration between CaCO 3 and Fe 2 O 3 reforming is essential to obtain the desirable reforming products. The difference of FeO existence on the theoretical and experimental phase components illustrates that reaction degree is affected by the reduction agent amount. By comparing the methane temperature-programmed reaction of CaCO 3 , Fe 2 O 3 and their mixture, it is suggested that the existence of CaCO 3 is beneficial for accelerating iron-based methane reforming. This study provides a way to improve reaction degree and optimize process characteristic for chemical looping reforming process.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xuqian Wang,Yi Xie,Kun Chen,Likexin Yi,Yabo Wang,Yongkui Zhang
Ferruginous rhodochrosite with high impurity is difficult to be utilized by traditional beneficiation process due to the complex characteristics. Herein, a bioleaching process driven by Acidithiobacillus ferrooxidans was proposed to recover Mn and Fe in ferruginous rhodochrosite with economic and environmental benefits. The biogenic Fe 3+ , H + and extracellular polymeric substances produced in bioleaching process significantly promoted the metal recovery and reduced the H 2 S emission. Optimal metal leaching efficiencies (95.94% of Mn and 97.54% of Fe) were achieved in bioleaching group. Furthermore, the Mn and Fe mixed leaching solutions could be directly adopted to fabricate Mn-Fe oxide based materials (MFO). When applied as catalysts for peroxymonosulfate (PMS) activation, the as-synthesized MFO performed well for sulfathiazole (STZ) degradation with a 98.66% removal efficiency in 40 min. Both radical process and non-radical process occurred in the advanced oxidation process, which induced the generation of abundant active species of ̇OH, SO 4 ̇ − and 1 O 2 . Meanwhile, charge transfer also contributed to STZ degradation. Favorably, MFO-3 exhibited good reusability in recycle study and showed adaptability towards various natural water matrixes. This research not only provided novel insights into the utilization of recalcitrant ferruginous rhodochrosite resources, but also enriched the strategy of PMS activator design for environmental remediation.
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