Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 37
·19757-19768
·
IF 14.511
Min Lu,Li An,Jie Yin,Jing Jin,Rui Yang,Bolong Huang,Yang Hu,Yong-Qing Zhao,Pinxian Xi
The electrochemical oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) are key electrochemical processes in metal–air batteries and water splitting devices. Aluminium–air batteries, as an important type of metal–air battery, have been considered to be promising power candidates for flexible electronics. Here, we describe electronically engineered amorphous Fe–Co–S sites embedded in Prussian blue analogue (FeCoSx-PBA) hetero-nanoframes. The experimental results and DFT calculations reveal the critical role of the introduced FeCoSx layer to PBA, which enhances the electron transfer and alleviates the overbinding effect of OH* during the OER. The FeCoSx-PBA hybrid system supplies an optimized electronic structure for the alkaline OER, which is also confirmed by the much-lowered overpotential (266 mV at 10 mA cm−2) for the alkaline OER. Furthermore, a flexible Al–air battery based on an FeCoSx-PBA cathode catalyst exhibits a high peak power density (58.3 mW cm−2) and energy density (1483 W h kgAl−1), and outstanding stability for more than 50 h of operation under bending or stretching conditions, demonstrating its potential in the practical application of flexible electronic devices. Our results may provide a new strategy of modulating the electronic structure of air electrode catalysts to efficiently promote the reactivity of alkaline OER and Al–air battery processes.
研究领域:
材料科学
·
电化学
·
能源技术
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Hongguan Li,Jing Wang,Ruijuan Qi,Yongfeng Hu,Jing Zhang,Hongbin Zhao,Jiujun Zhang,Yufeng Zhao
Charge and spin manipulations of electrons are considered to be of great significance in boosting the catalytic activity of M N C electrocatalysts. However, to the best of our knowledge, most current studies focus only on the charge engineering, the interplay between spin and charge is not well understood, and the simultaneous manipulation of both charge and spin remains challenging. Herein, we show that the cooperative interplay between charge itineration and spin-polarization of electrons has a profound impact on the catalytic behavior through density functional theory (DFT) calculations for the first time. Following this concept, we report a Fe-Ni atomic pair as a superior bifunctional catalyst for high performance ORR and OER, with a very small potential difference (ΔE) of 0.691 V. We confirm that the coexistence of Fe 3d itinerant charge and moderate spin polarization (magnetic moment: 1.48 μ B ) is responsible for the superior functional catalytic activity for the Fe Ni atomic pairs.
研究领域:
电催化
·
材料化学
·
物理化学
·
纳米催化
·
能源材料
·
计算化学
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2020
·
IF 6.155
Manigandan Ramadoss,Yuanfu Chen,Yang Hu,Bin Wang,Ramkumar Jeyagopal,Karpuraranjith Marimuthu,Xinqiang Wang,Dongxu Yang
The sluggish kinetics and high cost of the noble-metal based electrocatalyst for oxygen evolution reaction (OER) still seriously limits the efficiencies of water splitting. Herein, for the first time, we rationally design a porous hierarchical nanoarchitecture, constructed by ultrathin CoSe 2 embedded Fe-CoO nanosheets (CoSe 2 @Fe-CoO), which is synthesized via self-assembly hydrolysis driven in-situ synergetic selenization of Fe/Co/O/Se precursor followed by Ostwald ripening. As an OER catalyst, the porous CoSe 2 @Fe-CoO hybrid with abundant CoOOH electroactive sites delivers a small Tafel of 56.2 mV/dec with very low onset overpotential of 280 mV@10 mA/cm 2 and excellent long-term physicochemical stability till 62 h without obvious decay, which outperforms well-established benchmark electrocatalysts (RuO 2 ). The boosted OER performance of CoSe 2 @Fe-CoO nanosheets is mainly attributed to its iron-doping effect, porous nanoarchitecture, and multicomponent synergetic/interfacial effect between ultrathin cobalt (II) oxide and conductive cobalt selenide (CoSe 2 ) nanoframework. This work presents a facile construction strategy to find a nonprecious hybrid OER electrocatalyst with excellent performance and long-term stability.
研究领域:
材料科学
·
电化学
·
纳米技术
·
催化
✓ 已验证
DOI
高影响因子
Arabian Journal of Chemistry
·
2022
·
IF 6.212
Run Yuan,Yihe Qin,Can He,Zichen Wang,Lu Bai,Hong Zhao,Zijian Jiang,Lingyao Meng,Xuwen He
It is important to develop a catalyst that has high catalytic activity and can improve the degradation efficiency of refractory organic pollutants in the catalytic ozonation process. In this study, Fe-Mn-Cu-Ce/Al 2 O 3 was synthesised via impregnation calcination for catalytic ozonation of bio-treated coking wastewater. The physical and chemical characteristics of the catalysts were analysed using X-ray diffraction (XRD), X-ray fluorescence spectrometry (XRF), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), and Brunauer–Emmett–Teller nitrogen adsorption–desorption methods. The effects of catalyst dosage, pH, and reflux ratio on the degradation efficiency of wastewater were examined in laboratory-scale experiments. The chemical oxygen demand (COD) removal rate of bio-treated coking wastewater was estimated to be 52.76 % under optimal conditions. The experiments on the catalytic mechanism demonstrated that the surface hydroxyl formed by the Lewis acid sites on the surface of the catalyst can react with ozone as the active site forming the active oxygen (·OH, ·O 2 – , and 1 O 2 ), thereby efficiently degrading the organic pollutants in coking wastewater. Furthermore, a pilot-scale experiment on the catalytic ozonation of bio-treated coking wastewater was carried out using an Fe-Mn-Cu-Ce/Al 2 O 3 catalyst, while the effects of the initial pollutant concentration, ozone concentration, and gas flow on the COD removal rate were studied on a pilot scale. It was found that the COD removal rate of the wastewater was ∼ 60 % under optimal parameters. After the treatment, the wastewater steadily reached the coking wastewater discharge standard (COD < 80 mg/L), while the operating cost of catalytic ozonation reached ∼ 0.032$/m 3 , thereby paving the way toward economic engineering applications. The COD degradation kinetics in the bio-treated coking wastewater followed pseudo-second-order kinetics. Three-dimensional fluorescence and gas chromatography–mass spectrometry revealed that macromolecular organic pollutants in the bio-treated coking wastewater were greatly degraded. In summary, Fe-Mn-Cu-Ce/Al 2 O 3 exhibited good reusability, high catalytic activity, and low cost and has a wide application prospect in the treatment of coking wastewater.
研究领域:
环境科学
·
催化材料
✓ 已验证
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Chenxuanzi Wang,Mingxuan Zhong,Yongcheng Cai,Zewei Zhang,Bo Xiao,Tingting Xu,Xun Wang
The chemical looping reforming coupled with CO 2 splitting (CLR-CS) offers a promising solution for syngas production and simultaneous decomposition of CO 2 . In this study, the Sr-Fe based oxygen carriers (OCs) were evaluated in CLR-CS using ethanol as fuel. The presence of Sr significantly improved the oxidation performance of iron oxides. The Sr element in fresh Sr-Fe based OCs mainly formed two crystal phases, including SrFe 12 O 19 and Sr 4 Fe 6 O 13 . Increasing the amount of Sr element made it easier to form Sr 4 Fe 6 O 13 crystal phase. The Sr 4 Fe 6 O 13 was favorable for syngas production, due to the higher surface oxygen vacancy formation energy with a range of 3.13–3.37 eV. However, the lower oxygen transfer capacity (OTC) of Sr 4 Fe 6 O 13 resulted in a lower CO yield in the of stage of CO 2 decomposition. Compared with Sr 4 Fe 6 O 13 , SrFe 12 O 19 exhibited the higher OTC and the higher reactivity of lattice oxygen, which was preferable to produce more CO 2 in the stage of ethanol reforming in fuel reactor. During the cycle tests, the crystalline phase of SrFe 12 O 19 didn’t regenerate under the CO 2 atmosphere but transformed into Sr 4 Fe 6 O 13 . It was attributed to the lower energy barrier of CO 2 oxidation on the oxygen defect surface of Sr 4 Fe 6 O 13 . The phase transformation of SrFe 12 O 19 accompanied the formation of Fe 3 O 4 . The excessive Fe 3 O 4 had poor stability and inactivated easily due to sintering and agglomeration in Sr1Fe4 and Sr1Fe6 samples. The Sr1Fe2, namely the molar ratio of SrO to Fe 2 O 3 of 1:2, exhibited the better performance for syngas (0.291 Nm 3 /kg OC) and CO (0.141 Nm 3 /kg OC) coproduction at 800 °C. Additionally, the Sr1Fe2 presented an excellent cyclic stability in 30 cycles due to the suitable proportion of Sr 4 Fe 6 O 13 and iron oxides formed, which maintained a high syngas yield and avoided sintering of iron oxides. Overall, the Sr1Fe2 is a promising OC candidate in CLR-CS process.
研究领域:
能源科学
·
材料科学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2020
·
IF 7.864
Tian Tian,Ke Zhou,Yu-Sheng Li,Dong-Feng Liu,Han-Qing Yu
Phosphorus (P) recovery from wastewater can be completed by iron-involved autotrophic denitrification via forming Fe(III)–P precipitates and/or adsorbing P onto Fe(III) oxyhydroxides. However, so far, most studies focused on the final P-containing products, while the P-capturing pathways in such a process remain unclear. In this work, autotrophic iron-dependent denitrification (AIDD) was used as a typical anoxic iron-involved P-capturing biosystem to investigate the main P recovery pathways. The AIDD biosystem showed a relatively stable capability of capturing P coupled with nitrate reduction. Direct formation of amorphous Fe(II)–P precipitates after the phosphate was fed, followed by microbially driven oxidation into Fe(III)–P minerals, was found to be the primary pathway for the P capture. In addition, adsorption of phosphate onto the formed iron oxyhydroxides also contributed to the P recovery. This work provides better understanding about recovering P in AIDD and iron-involved denitrification and highlights the important roles of iron oxidizers in the iron-related biological wastewater treatment processes.
研究领域:
环境工程
·
水处理技术
·
生物地球化学
·
环境微生物学
·
资源回收
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Su Ding,Jinquan Wan,Yan Wang,Zhicheng Yan,Yongwen Ma
In this work, persulfate (PS) activation by a novel functioned metal-organic framework catalyst was investigated for the targeted degradation of DMP, a toxic phthalate pollutant. The catalyst, a molecularly imprinted water-stable Fe-MOF-74 (Fe-MOF-74@SiO 2 @MIP), showed excellent capability of PS activation, high selectivity and efficient targeted degradation performance of DMP. The results of total organic carbon indicated that DMP was mineralized during the catalysis. EPR measurement and quenching experiments suggested the coexistence of SO 4 •− and • OH, and SO 4 •− was predominant in this system. It was found that increasing catalyst loading (0.01 - 0.05 g L -1 ) inhibited the DMP elimination, due to the aggravated radical consumption. A higher pseudo-first order rate of DMP degradation was observed with an increasement of PS (5.2 - 52 mM) and temperature (15 - 45 °C). Besides, coexisting chloride ions (Cl − ) promoted the DMP degradation at the concentration 1 mM, but decreased the degradation performance at other concentrations. According to EPR and XPS analysis, the effect of Cl − was ascribed to the formation chlorine radicals, which changed the radical distribution and the catalytic site property. Chlorinated intermediates were detected by LC-MS, confirming the involvement of Cl-related radicals. Finally, possible degradation pathways were proposed.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
POLYMERS FOR ADVANCED TECHNOLOGIES
·
2019
·Vol. 30
·期 9
·2458-2467
·
IF 2.162
Zhongwei Chen,Tingting Chen,Yuan Yu,Qingwu Zhang,Zhiquan Chen,Juncheng Jiang
Metal-organic framework MIL-53 (Fe)@C/graphite carbon nitride hybrid (MFeCN), a novel flame retardant, was synthesized by hydrothermal reaction and subsequently added into unsaturated polyester resin (UPR). The structure, morphology, and thermal stability of MFeCN were characterized by Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy-dispersive X-ray spectroscopy (EDS), and thermogravimetric analysis (TG). The thermal stability and flammability of the UPR composites were characterized by TG and cone calorimeter tests (CCT). The results of CCT demonstrated that the peak heat release rate (pHRR), total heat release (THR), peak smoke production rate (pSPR), and total smoke production (TSP) of UPR/MFeCN-4 were reduced by 39.8%, 10.2%, 33.3%, and 14.5%, respectively, comparing with UPR. The results of TG and CCT indicated that MFeCN could improve the thermal stability, flame retardancy, and smoke suppression properties of the UPR composites. The residues after CCT were then characterized by laser Raman spectroscopy (LRS), XPS, and SEM. Finally, based on the above experimental results and analysis, the flame retardancy mechanism of MFeCN was proposed.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
Environmental Science-Nano
·
2024
·Vol. 11
·期 7
·3092-3103
·
IF 5.8
Manoj Kumar Panjwani,Feiyu Gao,Ting He,Pan Gao,Feng Xiao,Shaoxia Yang
M–Nx single-atom catalysts (SACs) with a high coordination number (x > 4) are effective catalysts for eliminating organic pollutants, while the origin of SACs with high activity still remains elusive. In this work, we successfully synthesized an Fe–N5 SAC with axial N coordination, which exhibited exceptional catalytic performance by peroxymonosulfate (PMS) activation for degrading 4-chlorophenol (4-CP) in a wide pH range (4.0–10.0). The rate constant of Fe–N5 (2.99 min−1) was 6.36 times higher than that of Fe–N4, and the turnover frequency (TOF) of Fe–N5 was found to be 4–149 times higher than those of state-of-the-art SACs and nanocatalysts reported in the literature for 4-CP degradation by PMS activation. Moreover, Fe–N5 was not significantly affected by coexisting substances (HA, HCO3−, SO42−, H2PO4−, NO3−, and Cl−) and had satisfactory degradation efficiency for various chlorophenols. Electron paramagnetic resonance (EPR), quenching experiments, and radical probe experiments demonstrated that 1O2 played a key role in the Fe–N5/PMS system for 4-CP degradation. Density functional theory calculations confirmed that a narrower gap between the Fe-3d band center and Fermi level enhanced the electron transfer in Fe–N5, which resulted in promoted PMS activation. In addition, the Fe–N5/PMS system showed good potential for application in real wastewater. The above findings offer important implications for the future of coordination chemistry in designing M–Nx–C SACs (x > 4), highlighting their practical applications in environmental remediation.
研究领域:
环境化学
·
催化
·
材料科学
·
环境工程
✓ 已验证
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
En-Hui Yuan,Meng Li,Ming-Hui Yang,Xiaosheng Huang,Kun Zhang,Weiliang Han,Zhicheng Tang,Zhong-Wen Liu
A direct hydrothermal synthesis strategy is developed to prepare the Cu–Fe-ZSM-5 zeolites by using the ethylenediaminetetraacetic acid disodium dihydrate (EDTA-2Na·2H 2 O) chelated Cu 2+ and Fe 3+ precursors as metal sources. During the crystallization, the metal chelates were spontaneously embedded into the ZSM-5 crystals and subsequently transformed to the zeolites encapsulated copper and iron species after removing the chelating agent via the high-temperature calcination . Rigorous characterizations indicate that the resulted Cu 2+ /Cu + and Fe 3+ /Fe 2+ species are formed ultra-small nano-composites with an average diameter of ∼2.2 nm and highly dispersed in the ZSM-5 zeolite crystals. The acidity of the ZSM-5 zeolites is subtly modulated by the encapsulated Cu–Fe nano-composite. As expected, the as-prepared Cu–Fe-ZSM-5 exhibits outstanding catalytic performance for the selective catalytic reduction of NO x with ammonia (NH 3 -SCR) in the broad reaction temperature ranges of 220–480 °C, which is much better than the Cu–Fe/ZSM-5 prepared with the conventional wetness impregnation method. Furthermore, the resultant zeolites show high stability and good tolerance to H 2 O and SO 2 , and it is very competitive for practical application to eliminate NO x . The developed one-pot hydrothermal synthesis route by using EDTA-2Na·2H 2 O as chelating agent is very convenient and easily reproducible, providing a general guideline to design and fabricate the superior transition metal modified zeolite catalysts for NH 3 -SCR and the related reactions.
研究领域:
催化
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
Science Advances
·
2024
·Vol. 10
·期 15
·
IF 11.7
Kerong Chen,Anwei Zhou,Xinyuan Zhou,Jielei He,Yurui Xu,Xinghai Ning
Disruptions in metal balance can trigger a synergistic interplay of cuproptosis and ferroptosis, offering promising solutions to enduring challenges in oncology. Here, we have engineered a Cellular Trojan Horse, named MetaCell, which uses live neutrophils to stably internalize thermosensitive liposomal bimetallic Fe-Cu MOFs (Lip@Fe-Cu-MOFs). MetaCell can instigate cuproptosis and ferroptosis, thereby enhancing treatment efficacy. Mirroring the characteristics of neutrophils, MetaCell can evade the immune system and not only infiltrate tumors but also respond to inflammation by releasing therapeutic components, thereby surmounting traditional treatment barriers. Notably, Lip@Fe-Cu-MOFs demonstrate notable photothermal effects, inciting a targeted release of Fe-Cu-MOFs within cancer cells and amplifying the synergistic action of cuproptosis and ferroptosis. MetaCell has demonstrated promising treatment outcomes in tumor-bearing mice, effectively eliminating solid tumors and forestalling recurrence, leading to extended survival. This research provides great insights into the complex interplay between copper and iron homeostasis in malignancies, potentially paving the way for innovative approaches in cancer treatment.
研究领域:
肿瘤学
·
纳米技术
·
治疗学
·
生物医学工程
✓ 已验证
DOI
PubMed
高影响因子
SOLID STATE COMMUNICATIONS
·
2021
·
IF 1.804
Shaohui Su,Jiahao Yu,Xianguo Liu,Jieyi Yu
Magnetic-dielectric composites attract numerous attentions for good microwave absorption performances based on magnetic-dielectric loss mechanism and tunable electromagnetic parameters. Fe/carbon fibers are prepared through carbonization of Fe doped polyaniline nanotubes , in which Fe nanoparticles are embedded in carbon fibers. The introduction of Fe nanoparticles results in good electromagnetic impedance and proper quarter-wavelength cancellation induced, which ensure that microwave penetrate composites to the great extend and is consumed as much as possible, leading to enhanced microwave absorption performance. The minimal reflection loss of Fe/carbon fibers composites starts being less than −10 dB from 1.7 mm and is up to −44.09 dB at 6.62 GHz and 4.1 mm and the effective bandwidth reaches 6.0 GHz with 2.4 mm.
研究领域:
材料科学
·
电磁学
·
纳米复合材料
·
功能材料
·
微波工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）