ADVANCED MATERIALS
·
2022
·Vol. 35
·期 5
·2208034
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IF 32.086
Kai Jia,Jun Ma,Junxiong Wang,Zheng Liang,Guanjun Ji,Zhihong Piao,Runhua Gao,Yanfei Zhu,Zhaofeng Zhuang,Guangmin Zhou,Hui-Ming Cheng
A large amount of spent LiFePO 4 (LFP) has been produced in recent years because it is one of the most widely used cathode materials for electric vehicles. The traditional hydrometallurgical and pyrometallurgical recycling methods are doubted because of the economic and environmental benefits; the direct regeneration method is considered a promising way to recycle spent LFP. However, the performance of regenerated LFP by direct recycling is not ideal due to the migration of Fe ions during cycling and irreversible phase transition caused by sluggish Li + diffusion. The key to addressing the challenge is to immobilize Fe atoms in the lattice and improve the Li + migration capability during cycling. In this work, spent LFP is regenerated by using environmentally friendly ethanol, and its cycling stability is promoted by elevating the d-band center of Fe atoms via construction of a heterogeneous interface between LFP and nitrogen-doped carbon. The Fe O bonding is strengthened and the migration of Fe ions during cycling is suppressed due to the elevated d-band center. The Li + diffusion kinetics in the regenerated LFP are improved, leading to an excellent reversibility of the phase transition. Therefore, the regenerated LFP exhibits an ultrastable cycling performance at a high rate of 10 C with ≈80% capacity retention after 1000 cycles.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2022
·
IF 7.926
Chunying Dong,Yuang Pang,Yan Chen,Zhan Gao,Meiqiang Cai,Micong Jin,Zongsu Wei
Sludge based catalysts (SBCs) has been considered as a promising and viable approach to sludge reclamation. Herein, we fabricated bimetallic Fe-Ti doped SBCs via a facile synthesis with sludge containing polyacrylamide (PAM) as N-precursor. The adsorption capacity and degradation efficiency of as-synthesized SBCs were assessed using tetracycline (TC) as a target pollutant, in which PAM in sludge played a dual role by promoting porosity, active sites, and structural defects beneficial for persulfate (PS) activation. Fe-Ti doping induced the activation of PS by a fast redox cycle of Fe 3+ /Fe 2+ associated with the coexistence of Ti 4+ /Ti 3+ , which enabled an efficient electron transfer between the catalyst and PS. The synergistic effect of PAM-derived N doping and Fe-Ti bimetals resulted in prevention of iron leaching and enhanced catalyst stability over a wide pH range. The surface SO 4 •− was the primary oxidant in the TC degradation process based on free-radical quenching experiments, and degradation pathways of TC were proposed given the intermediate evidence from UPLC-HRMS analysis. This study promotes the reclamation of PAM-containing sludge providing an eco-friendly and efficient process to activate PS for wastewater treatments .
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WATER RESEARCH
·
2022
·
IF 13.4
Tianwei Hao,Yao Huang,Fangbai Li,Yundang Wu,Liping Fang
Fe(II) redox chemistry is a pivotal process of biogeochemical Fe cycle and the transformation of organic pollutants in subsurface aquifers, while its interfacial reactivity on iron oxides with varying surface chemistries remains largely unexplored. In this study, the redox processes of Fe(II) on two hematite with highly exposed {001} and {110} facets and their impacts on the transformation of nitrobenzene were investigated. Results suggest that Fe(II) adsorption is the rate-limiting step of the redox chain reactions, controlling the reduction potential ( E H ). Nitrobenzene activates the facet electron transfer on hematite, leading to nitrobenzene reduction and Fe(II) oxidation. Moreover, {001} facet exhibits a higher reactivity and electron transport efficiency than {110} facet, which is attributed to a lower site density (0.809 #Fe/nm 2 ) and a lower E H of hematite {001} facet than that of {110} facet. It is worth noting that the facet-dependent reduction activity is more intense at low pH or high Fe(II) activity. A slight dissolution of {110} facet was observed, indicating hematite {001} facet exhibits higher thermodynamic stability than {110} facet. This study confirms the facet-dependent reducing activity of surface bound Fe(II) on hematite, providing a new perspective for in-depth understanding of the interfacial reactions on hematite. The findings of this work broaden the biogeochemical process of Fe cycle in subsurface environments and its impact on the fate of organic pollutants in groundwater.
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Nanomaterials
·
2022
·Vol. 12
·期 5
·811
·
IF 5.719
Kang-Ping Cui,Yu-Ying He,Kai-Jie Xu,Yu Zhang,Chang-Bin Chen,Zheng-Jiang Xu,Xing Chen
In this work, the combination of high surface area diatomite with Fe and Cu bimetallic MOF material catalysts (Fe0.25Cu0.75(BDC)@DE) were synthesized by traditional solvothermal method, and exhibited efficient degradation performance to tetracycline hydrochloride (TC). The degradation results showed: Within 120 min, about 93% of TC was degraded under the optimal conditions. From the physical–chemical characterization, it can be seen that Fe and Cu play crucial roles in the reduction of Fe3+because of their synergistic effect. The synergistic effect can not only increase the generation of hydroxyl radicals (•OH), but also improve the degradation efficiency of TC. The Lewis acid property of Cu achieved the pH range of reaction system has been expanded, and it made the material degrade well under both neutral and acidic conditions. Loading into diatomite can reduce agglomeration and metal ion leaching, thus the novel catalysts exhibited low metal ion leaching. This catalyst has good structural stability, and less loss of performance after five reaction cycles, and the degradation efficiency of the material still reached 81.8%. High performance liquid chromatography–mass spectrometry was used to analyze the degradation intermediates of TC, it provided a deep insight of the mechanism and degradation pathway of TC by bimetallic MOFs. This allows us to gain a deeper understanding of the catalytic mechanism and degradation pathway of TC degradation by bimetallic MOFS catalysts. This work has not only achieved important progress in developing high-performance catalysts for TC degradation, but has also provided useful information for the development of MOF-based catalysts for rapid environmental remediation.Keywords:Fenton-like catalyst;bimetallic MOF;diatomite;synergistic effect;antibiotics
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APPLIED CLAY SCIENCE
·
2022
·
IF 5.907
Qiushi Jiang,Zhaolian Han,Nan Qu,Lianzhi Sun,Yafeng Yuan,Yating Ren,Zhiqiang Cheng
A low-cost palygorskite (Pal)/MIL-101(Fe) was prepared by solvothermal method and calcined under nitrogen protection to form the magnetic derivant Pal/MIL-101(Fe)-400, the successful combination of which was confirmed. The band gap (1.47 eV) of Pal/MIL-101(Fe)-400 was lower than 2.25 eV of Pal/MIL-101(Fe), indicating a significant improvement in light absorption performance. In addition, Pal/MIL-101(Fe)-400 exhibits stronger photocurrent response and lower impedance due to the formation of Fe 3 O 4 clusters with high electrical conductivity and new active centers by calcination. The prepared Pal/MIL-101(Fe)-400 can achieve 90 mg/g RhB removal completely, which is better than 77.0% adsorption of MIL-101(Fe) and 67.2% adsorption-photocatalytic of Pal/MIL-101(Fe), which also shows superparamagnetism properties and excellent cyclic stability. In addition, Pal/MIL-101(Fe)-400 mainly relies on the action of peroxy radical to oxidize organic pollutants, which is different from Pal/MIL-101(Fe). This work provides a new perspective for the construction of magnetic MOF multifunctional materials for the efficient treatment of pollutants in water.
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Small Structures
·
2022
·Vol. 3
·期 4
·2100211
·
IF 11.343
Fan Tang,Sijie Guo,Yonggang Sun,Xijie Lin,Jianhua Qiu,Anmin Cao
Developing high-performance, low-cost, and robust electrocatalysts is of great importance to boost the efficiency of oxygen evolution reaction (OER). Herein, based on the integrated design of chemical composition and geometric structure, Fe-doped CoO nanotubes (NTs) with high OER activity are prepared by a facile template-free approach. The construction of this tubular structure is realized via a simple wet-chemical reaction to prepare solid nanorods as precursor and a subsequent calcination treatment of the precursor to form hollow cavity. The favorable composition and unique hollow structure endow these Fe-doped CoO NTs with remarkable activity toward OER. When used as the electrocatalyst for OER, the Fe-doped CoO NTs show a small overpotential of 282 mV at the current density of 10 mA cm −2 , a low Tafel slope of 78.26 mV dec −1 , and a high turnover frequency of 0.0965 s −1 at the overpotential of 282 mV, which is superior to those of CoO NTs and solid CoO nanoparticles. Moreover, the Fe-doped CoO NTs also exhibit excellent long-term stability of 24 h at the current density of 10 mA cm −2 .
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MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 4
·1-5
·
IF 6.408
Tian Dazhi,Xiang Wen,Wang Hao,Jiang Wentao,Li Ting,Yang Minghui
B-doped core–shell Fe@BC nanozyme was synthesized. The peroxidase (POD) like activity of Fe@BC nanozyme was studied and utilized for detecting the activity of alanine aminotransferase (ALT). In the presence of ALT as well as ALT co-substrates l -alanine and α-ketoglutarate, l -glutamate is generated. The following catalytic oxidation of l -glutamate by glutamate oxidase leads to the generation of H 2 O 2 . The POD-like activity of Fe@BC can oxidize 3,3′,5,5′-tetramethylbenzidine (TMB) to oxTMB in the presence of H 2 O 2 , generating a blue-colored compound. Through the detection of the amount of H 2 O 2 generated, ALT activity can be determined through measuring the absorbance intensity variation at 450 nm. The limit of detection of the assay is 4 U/L, with a linear range from 10 to 1000 U/L. For human serum samples, the ALT levels determined by our assay are comparable to those determined by the hospital with a correlation coefficient of 0.991, demonstrating the reliability of our assay results. Graphical abstract
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Advanced Materials Interfaces
·
2022
·Vol. 9
·期 15
·2200276
·
IF 6.389
Dong Liu,Chenxi Huyan,Yuanyuan Zhao,Terence Xiaoteng Liu,Ding Wang,Jining Sun,Sheng Dai,Fei Chen,Ben Bin Xu
Carbon-based single-atom iron electrocatalysts with nitrogen coordination (CSAIN) have recently shown enormous promise to replace the costly Pt for boosting the cathodic oxygen reduction reaction (ORR) in fuel cells. However, there remains a great challenge to achieve highly efficient CSAIN catalysts for the ORR in acidic electrolytes. Herein, a novel CSAIN catalyst is synthesized by pyrolyzing a precursor mixture consisting of metal–organic framework and conductive polymer hybrid. After pyrolysis at a high temperature, the CSAIN with a structure of carbon nanosheet supported polyhedral carbon is achieved, where the unique structure endows CSAIN with expediting electron transfer and mass transport, as well as largely exposed surface to host atomically dispersed iron active sites. As a result, the optimal CSAIN catalyst shows a high ORR activity with its half-wave potential of 0.77 V (vs RHE) and a Tafel slope of 74.1 mV dec –1 , which are comparable to that of commercial Pt/C catalyst (0.80 V and 81.9 mV dec –1 ).
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CHEMOSPHERE
·
2022
·
IF 8.943
Jiayi Luo,Yunqiang Yi,Long Zhou,Zhanqiang Fang
The potassium-doped magnetic biochar (KMBC) preparation was inevitably introduced the different anions in the process of modifying magnetic biochar (MBC) with different potassium salts, but the effect and mechanism of different anion on KMBC activation properties has not been reported. Therefore, in this paper, five different KMBCs were prepared using several common potassium salts under the same dosage of K + and Fe 2+ , and then was added in the presence of persulfate (PS) for the removal of metronidazole (MNZ). The removal rate of metronidazole was ordered as KMBC K2SO4 (98.40%) > KMBC KNO3 (76.84%) > KMBC KCl (20.79%) > KMBC K2CO3 (19.02%) > KMBC K2C2O4 (14.23%). However, the semi-quantitative of Fe(II) experiments results confirmed that the effectively increase of Fe(II) content by potassium salts modification played the dominant role in improvement of KMBC activation performance. The Fe(II) content of KMBC were ordered as KMBC K2CO3 > KMBC K2SO4 > KMBC KNO3 > KMBC KCl > KMBC K2C2O4 , with the Fe(II) content of KMBC of 36.74, 17.70, 8.79, 5.24 and 4.85 mg/g, respectively. The indicated that the introduction of different anions would lead to different optimal Fe(Ⅱ) content in KMBC modified with different potassium salts, which was most directly reflected in 1 O 2 content in different KMBC/PS systems, and account for the difference in MNZ degradation efficiency. Meanwhile, when the Fe(II) content in KMBC reached the range of 13.7–28.8 mg/g, KMBC had the better performance of activating PS.
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WATER RESEARCH
·
2022
·
IF 13.4
Zheng-Yu Dong,Yi-Li Lin,Tian-Yang Zhang,Chen-Yan Hu,Yang Pan,Renjie Pan,Yu-Lin Tang,Bin Xu,Nai-Yun Gao
To improve the performance of the conventional coagulation process, a permanganate (Mn(VII)) pre-oxidation combined with Fe(III)/peroxymonosulfate (PMS) coagulation process (Mn(VII)-Fe(III)/PMS) that can significantly improve the removal of dissolved organic carbon (DOC), turbidity, and micropollutants is proposed in this study. Compared with conventional Fe(III) coagulation, the Mn(VII)-Fe(III)/PMS process can also significantly enhance the removal of iohexol and sulfamethoxazole in raw water. During this process, the primary reduction product, Mn(IV), after Mn(VII) pre-oxidation was adsorbed on the floc surfaces and involved in the Fe(III)/PMS process. The natural organic matter (NOM) in raw water mediated the redox cycle of iron. The synergistic effect of NOM, Fe, and Mn facilitated the redox cycle of Mn(III)/Mn(IV) and Fe(III)/Fe(II) to promote the activation of PMS. The sulfate radical (SO 4 •− ) played an important role in the degradation of micropollutants. The formation potential of the detected volatile disinfection by-product (DBP) during the subsequent chlorination was reduced by 21.9% after the Mn(VII)-Fe(III)/PMS process. This study demonstrated the promising application of the Mn(VII)-Fe(III)/PMS process for coagulation and micropollutant control and illustrated the reaction mechanism. This study provides guidance for improving conventional drinking water treatment processes.
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COMPOSITES PART B-ENGINEERING
·
2022
·
IF 11.322
Fucheng Wang,Jinfeng Zhang,Kaixin Sun,Liwei Quan,Jing Wang,Naiqin Zhao,Chunsheng Shi,Shijian Zheng
Interfacial bonding is an important factor affecting the mechanical properties of composites. The interface between the in-situ synthesized ceramic phase and the metal matrix is considered ideal, so little attention is paid to the interfacial modification. In this work, we found that interfacial segregation affects the growth of the MgAlB 4 whisker and the interface of reinforcement and matrix in the composites. Systematic experiments and theoretical calculations indicate Fe solute prefer to segregate at the MgAlB 4 - { 10 1 ‾ 0 } /Al interfaces in in-situ synthesized MgAlB 4 /Al composites, which is helpful to reduce system free energy. On the one hand, Fe segregation induces the whisker coarsening and the formation of planar defects with a sandwich structure formed by a layer of Fe atoms and two layers of Al atoms in coarse-whiskers, on the other hand, it improves the interfacial strength . Although extra Fe aggravates the whisker coarsening, the synergistic reinforcing effect of the whiskers and the extra Fe is greater than the sum of their individual reinforcing effects. This work demonstrates that interfacial segregation can be used to modulate the size of reinforcements and improve interfacial strength.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-11
·
IF 17.694
Wan Xin,Liu Qingtao,Liu Jieyuan,Liu Shiyuan,Liu Xiaofang,Zheng Lirong,Shang Jiaxiang,Yu Ronghai,Shui Jianglan
Simultaneously increasing the activity and stability of the single-atom active sites of M–N–C catalysts is critical but remains a great challenge. Here, we report an Fe–N–C catalyst with nitrogen-coordinated iron clusters and closely surrounding Fe–N 4 active sites for oxygen reduction reaction in acidic fuel cells. A strong electronic interaction is built between iron clusters and satellite Fe–N 4 due to unblocked electron transfer pathways and very short interacting distances. The iron clusters optimize the adsorption strength of oxygen reduction intermediates on Fe–N 4 and also shorten the bond amplitude of Fe–N 4 with incoherent vibrations. As a result, both the activity and stability of Fe–N 4 sites are increased by about 60% in terms of turnover frequency and demetalation resistance. This work shows the great potential of strong electronic interactions between multiphase metal species for improvements of single-atom catalysts.
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