JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Sijun Yang,Jie Yu,Chengli Yao,Shikuo Li,Anjian Xie
The development of efficient non-precious-metal catalysts for oxygen reduction reaction (ORR) is greatly important for accelerating the commercial application of fuel cells. Herein, polystyrene (PS) nanospheres are used as templates for the growth of zeolitic imidazolate framework (ZIF) complex precursors with variable molar ratios of Fe 3+ to Zn 2+ in situ. Through carbonization at a high temperature, the hierarchical porous carbon (HPC) materials with different proportions (xFeyZn-HPC, x + y = 100) have been prepared. The typical product 5Fe95Zn-HPC is composed of nitrogen (N)-doped hierarchical porous carbon loaded with Fe/Fe 5 C 2 nanoparticles obtained at optimal molar ratio. As an electrocatalyst, the 5Fe95Zn-HPC shows a positive onset potential of 0.92 V (vs. RHE), half-wave potential of 0.77 V (vs. RHE) and limiting current density of 5.60 mA cm −2 at 0.055 V (vs. RHE). The hydrogen peroxide yield is less than 4.2%, and the electron transfer numbers are between 3.91 and 3.99 at 0.055 V~1.055 V in the catalytic ORR, which indicate that the reaction is dominated by four-electron reduction. The 5Fe95Zn-HPC has higher stability and methyl alcohol resistance in alkaline and acidic solutions. The above results indicate the excellent catalytic ORR performance of the 5Fe95Zn-HPC, almost as the commercial Pt/C. Additionally, 5Fe95Zn-HPC has the capacity to catalyze oxygen evolution reaction (OER) and adsorb methylene blue pollutants. Therefore, this work provides a practical method to design the hierarchical porous carbon-based material with outstanding multi-functions.
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CATALYSIS LETTERS
·
2019
·Vol. 149
·期 7
·1874-1887
·
IF 2.372
Mei Jing,Yuan Guojun,Ma Yusha,Chen Xu,Ren Lili
Nowadays, increasing attention has been focused on tailor-made aerogels through the addition of different components, which have been employed in specific catalytic reactions. In this study, Fe-doped alumina aerogel as a novel heterogeneous catalyst for degradation of Rhodamine B (RhB) was constructed by sol–gel one-step method, which is not only simple, but also can avoid the leaching of active components during degradation of RhB. Besides, the catalyst maintains high activity for the degradation of RhB within a wide range of pH values (2–10). Heat treatment could lead to enhancement of Fe–O–Al bond and significantly inhibit iron leaching. Effects of some parameters, including reaction temperature, dosages of H 2 O 2 , pH values and RhB concentrations on RhB degradation were also investigated. FTIR and ICP analysis shows that the catalyst exhibits low iron leaching, good structural stability and high catalytic efficiency after reuse. The catalytic mechanism and RhB degradation pathway were proposed based on the results of electron paramagnetic resonance (EPR) and the liquid chromatography-mass spectrometry (LCMS). We believe that Fe-doped alumina aerogel can be an efficient and green heterogeneous catalyst for the degradation of organic pollutants. Graphical
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CRYSTENGCOMM
·
2019
·Vol. 21
·期 40
·6010-6017
·
IF 3.382
Shuai Fang,Hongan Ma,Zhanke Wang,Zhiqiang Yang,Zheng-hao Cai,Luyao Ding,Xinyuan Miao,Liangchao Chen,XiaoPeng Jia
FeS is the main sulfur-containing compound in natural diamond inclusions. The research on FeS-doped diamond crystals plays an extremely important role in exploring the growth environment of natural diamond and the chemical composition of the earth. In our work, the characteristics of FeS doped diamond crystals were studied by using a China-type large volume cubic high-pressure apparatus with an iron–nickel alloy as a catalyst at 6.0 GPa and 1300–1350 °C. The crystals were characterized by OM, SEM, XPS, FTIR and Raman. Scanning electron microscopy of the crystal shows that the {100} plane of the crystal is rougher than {111}, which is related to the number of dangling bonds on different crystal faces of the crystal. The residue on the surface of the crystal was detected by mapping, and the test result showed that it was a sulfur iron and a sulfur nickel compound. FeS will decompose in the synthesis system, and the decomposition products are Fe and S2.The XPS spectrum of the crystal shows that S was successfully incorporated into the diamond lattice by forming C–S–O and C–S–SO2–C bonds, and the peak intensity was strong. The infrared spectrum shows that the N content in the crystal gradually increases as the doping ratio increases. Raman spectroscopy analysis shows that the S-doped Ib-type diamond single crystal has a high-quality sp3 structure, and the full width at half maximum (FWHM) of the crystal gradually broadens as the doping ratio increases.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Mang Ma,Anuj Kumar,Danni Wang,Yiyan Wang,Yin Jia,Ying Zhang,Guoxin Zhang,Zifeng Yan,Xiaoming Sun
Atomically dispersed metal-nitrogen-carbon complexes on carbon supports have drawn tremendous attention in the electrocatalysis fields. Herein, we managed the synthesis of atomically dispersed binary Ni x Fe 100-x -NC (x = 0–100) materials with tunable Ni/Fe ratios and investigated their underneath synergy effects for the enhancement of oxygen reduction (ORR) and oxygen evolution reactions (OER). EXAFS revealed the abundant presence of Ni(N 3 )-Fe(N 3 )-C n moieties in Ni 66 Fe 34 -NC sample. XPS fine scans indicated deep synergy of dual-site Ni/Fe that favored more charge localized over Ni/Fe sites. Electrochemical measurments showed that the Ni 66 Fe 34 -NC delivered a very high ORR half-wave potential ( E 1/2 ) of 0.85 V and a low OER overpotential of 467 mV at ∼10 mA cm −2 ( E j=10). The Fe site with Ni neighboring, as suggested by DFT simulations and in-situ Raman, was the responsible site for both ORR and OER. Furthermore, the Ni 66 Fe 34 -NC-assembled Zn-air battery afforded large specific power density and extraordinary cycling stability.
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MODERN PHYSICS LETTERS B
·
2024
·
IF 1.8
Li Liu,Qifu Bao,Tiangui Zhao,Kun Liu,Detai Shi,Siyu Li,Wei Zhu,Xiaolong Li,Jianer Zhou
A series of Zn 1 − x Fe x O ( x = 0 , 0.015, 0.045, 0.075) nanoparticles were synthesized using the solution co-precipitation method, and their structural and property characteristics were investigated. X-ray diffraction (XRD) analysis revealed that all Zn 1 − x Fe x O samples exhibited a hexagonal wurtzite crystal structure with the P63mc space group. The introduction of Fe doping led to a slight lattice distortion in the samples. The morphology of the nanoparticles, including polydispersion and agglomeration, as well as the presence of the second phase ZnFe 2 O 4 , was examined by scanning electron microscope (SEM) and transmission electron microscope (TEM). UV–Vis diffuse reflectance spectroscopy demonstrated that the band gap of Zn 1 − x Fe x O lies between 3.152 and 3.163 eV. With the increase in Fe ion doping, the band gap shows a slight decreasing trend. Mössbauer spectroscopy revealed that iron ions in the nanoparticles existed in a trivalent state and exhibited two different configurations: One involved iron replacing zinc without creating a vacancy, while the other involved iron substituting zinc with a vacancy. The ferromagnetic nature of the Fe-doped samples can be attributed to the exchange interaction between two Fe 3 + ions mediated by the F-center mechanism.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Qixia Dong,Haoran Dong,Yangju Li,Junyang Xiao,Shuxue Xiang,Xiuzhen Hou,Dongdong Chu
In this work, zero-valent Fe-Cu bimetallic nanoparticles were synthesized using a facile method, and applied to activate sulfite for the degradation of sulfamethazine (SMT) from the aqueous solution. The key factors influencing SMT degradation were investigated, namely the theoretical loading of Cu, Fe-Cu catalyst dosage, sulfite concentration and initial solution pH. The experimental results showed that the Fe-Cu/sulfite system exhibited a much better performance in SMT degradation than the bare Fe 0 /sulfite system. The mechanism and possible degradation pathway of SMT in Fe-Cu/sulfite system were revealed. The reactive radicals that played a dominant role in the SMT degradation process were •OH and SO 4 •- , while the loading of Cu induced the synergistic effect between Fe and Cu. The redox cycle between Cu(I)/Cu(II) remarkably contributed to the conversion of Fe(III) to Fe(II), greatly enhancing the catalytic performance of Fe-Cu bimetal. In real groundwater applications, the Fe-Cu/sulfite system also exhibited satisfactory SMT degradation. The 30-day aging tests of Fe-Cu particles demonstrated that the aging of catalyst was not obviously affecting the removal of SMT. Furthermore, the reusability of catalyst was evidenced by the recycling experiments. This study provides a promising application of bimetal activated sulfite for enhanced contaminant degradation in groundwater.
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 15
·7145-7157
·
IF 11.301
Jinling Xue,Yinshi Li,Jue Hu
It remains a major challenge to develop a facile method to prepare non-noble metal electrocatalysts with high activity and durability to drive the sluggish oxygen reduction reaction (ORR) for proton exchange membrane fuel cells (PEMFCs). Herein, a highly efficient bimetallic Zn/Fe@N-doped hierarchical porous carbon (Zn/Fe–N–C) catalyst derived from ZIF-8 and hemin (host–guest) was firstly reported by one-step thermal treatment. Fe2+ spatially separated by using the hemin guest in the ZIF-8 framework and hydrocarbon-branched chains form rich Fe–Nx active sites, and the evaporation of Zn2+ generates a highly porous structure in the Zn/Fe–N–C catalysts. Benefitting from this unique structure and composition, the resulting Zn/Fe2–N–C catalyst exhibits excellent ORR activities in both 0.1 M KOH (onset potential, Eonset = 1.08 V, and half-wave potential, E1/2 = 0.86 V vs. RHE) and 0.5 M H2SO4 media (Eonset = 1.04 V and E1/2 = 0.81 V), which are even comparable to those of the commercial Pt/C catalyst, and ranks among the top reported electrocatalysts. In addition, it also has outstanding long-term durability and good methanol resistance, much better than those of Pt/C in both acidic and alkaline media, which makes it one of the best non-noble alternatives of Pt-based catalysts for ORR electrocatalysis. This work highlights the potential to rationally design and fabricate high-performance ORR catalysts for fuel cell applications.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Chen Wen,Ligang Chen,Yating Xie,Jingying Bai,Xin Liang
In order to explore the effect of Fe doped CoP nanosheets on both hydrogen evolution reaction (HER) and hydrodesulfurization (HDS), FeCoP/C nanosheets have been successfully synthesized by the solvothermal process with Fe doped ZIF-67/C for the growth of FeCo-hydroxides nanosheets , as well as a following low-temperature phosphorization process. The performance evaluation results show that the FeCoP/C nanosheet exhibits an excellent acidic HER performance and an ordinary HDS performance compared to CoP/C and FeP/C catalysts. Experimental characterization and density functional theory results show that the high HER activity of the FeCoP/C nanosheet can be attributed to the fact that the nanosheet structure facilitates the exposure of active sites and the doped Fe atoms make CoP have a suitable hydrogen adsorption energy , while the ordinary HDS activity of the FeCoP/C nanosheet can be attributed to the fact that the doped Fe atoms can inhibit the cleavage of C–S bonds by CoP.
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Frontiers in Chemistry
·
2022
·
IF 5.545
Zhou Liang,Yang Zhiyong,Wei Deju,Zhang Heng,Lu Wei
A series of composite catalysts with different Fe-based load amounts were prepared and applied to the experiment of biomass gasification assisted by steam. The structure of the catalyst was analyzed by XRD, SEM, TEM, N2 adsorption-desorption, and H2-TPR. The effect of the change of Fe load amounts on the catalytic activity was studied, and the optimal conditions of the gasification reaction were selected. The relationship between catalyst structure and catalytic capacity was clarified. The results showed that under the optimal reaction conditions, the catalyst showed better catalytic activity when Fe load amounts were 10%. The proportion of hydrogen in the gasification gas is as high as 42.2% and the hydrogen production is 27.65 g/kg. The tar content reaches the lowest value of 34.07g/Nm3.
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Water
·
2021
·Vol. 13
·期 11
·1543
·
IF 3.103
Cancan Xu,Rui Liu,Wei Zheng,Lichu Lin,Lvjun Chen
Pd/Fe bimetallic particles were synthesized by chemical deposition and used to remove absorbable organic halogens (AOX) in the activated sludge of a chemical dyestuff wastewater treatment plant. Bath experiments demonstrated that the Pd/Fe bimetallic particles could effectively remove AOX. It indicated several factors, such as Pd loading, the amount of Pd/Fe used, initial activated sludge pH, and reaction time, which could affect the removal effect. The results showed that increasing the Pd content in Pd/Fe particles, from 0.01 to 0.05 wt %, significantly increased the removal efficiency of AOX in activated sludge. The Pd/Fe particles had a much higher removal efficiency of AOX in the activated sludge than bare Fe particles. A slightly acidic condition with a Pd content of 0.05% and 10 g/L of Pd/Fe was beneficial to the process of removing AOX in activated sludge. In detail, the removal efficiency of AOX in the activated sludge could reach 50.7% after 15 days of reaction with 10 g/L of Pd/Fe (Pd loading 0.05 wt %) and at an initial pH of 6.0 during the experiments. It also showed that the control samples without Fe0and Fe/Pd additions only removed 7.9% of AOX under the same conditions. Meanwhile, the concentrations of AOX in the supernatant of activated sludge were lower than the initial AOX concentration in the supernatant during the activated sludge remediation with Pd/Fe bimetallic particles. The results indicated that the AOX removal from the activated sludge matrix might be mainly due to the Pd/Fe bimetallic particles, and not just by phase transfer.
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Frontiers of Chemical Science and Engineering
·
2024
·Vol. 18
·期 11
·1-10
·
IF 4.3
Liang Haoting,Zhao Qiao,Liu Shengkun,Wei Chongyang,Wang Yidan,Wang Yue,Huang Shouying,Ma Xinbin
The Fe-Mn bimetallic catalyst is a potential candidate for the conversion of CO 2 into value-added chemicals. The interaction between the two metals plays a significant role in determining the catalytic performance, however which remains controversial. In this study, we aim to investigate the impact of tuning the proximity of Fe-Mn bimetallic catalysts with similar nanoparticle size. And its effect on the physicochemical properties of the catalysts and corresponding performance were investigated. It was found that closer Fe-Mn proximity resulted in enhanced CO 2 hydrogenation activity and inhibited CH 4 formation. The physiochemical properties of prepared catalysts were characterized using X-ray diffraction, H 2 temperature programmed reduction, and X-ray photoelectron spectroscopy, revealing that a closer Fe-Mn distance promoted electron transfer from Mn to Fe, thereby facilitating Fe carburization. The adsorption behavior of CO 2 and the identification of reaction intermediates were analyzed using CO 2 -temperature programed desorption and in situ Fourier transform infrared spectroscopy, confirming the intimate Fe-Mn sites contributed to CO 2 adsorption and the formation of HCOO* species, ultimately leading to increased CO 2 conversion and hydrocarbon production. The discovery of a synergistic effect at the intimate Fe-Mn sites in this study provides valuable insights into the relationship between active sites and promoters.
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Small
·
2023
·Vol. 19
·期 23
·2300106
·
IF 13.3
Ziqin Liu,Xin Dong,Jing Wen,Pu Hu,Chaoqun Shang
The high reactivity of Li metal and the inhomogeneous Li deposition leads to the formation of Li dendrites and “dead” Li, which impedes the performance of Li metal batteries (LMBs) with high energy density. The regulating and guiding the Li dendrite nucleation is a desirable tactic to realize concentrated distribution of Li dendrites instead of completely inhibiting dendrite formation. Here, a Fe-Co-based Prussian blue analog with hollow and open framework (H-PBA) is employed to modify the commercial polypropylene separator (PP@H-PBA). This functional PP@H-PBA can guide the lithium dendrite growth to form uniform lithium deposition and activate the inactive Li. In details, the H-PBA with macroporous structure and open framework can induce the growth of lithium dendrites via space confinement, while the positive Fe/Co-sites lowered by polar cyanide (−CN) of PBA can reactivate the inactive Li. Thus, the Li|PP@H-PBA|Li symmetric cells exhibit long-term stability at 1 mA cm −2 for 1 mAh cm −2 over 500 h. And the Li-S batteries with PP@H-PBA deliver favorable cycling performance at 500 mA g −1 for 200 cycles.
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