Journal of Physical Chemistry Letters
·
2024
·
IF 4.8
Yanchang Wang,Yao Xiao,Jiangnan Huang,Chunxiao Zhang,Kentaro Yamamoto,Yoshiharu Uchimoto,Weifeng Wei,Hongshuai Hou,Datong Zhang,Xiaobo Ji
For cathode materials of sodium-ion batteries, O3-type Ni/Fe/Mn-based (Na-NFM) layered oxides have garnered extensive attention because of high economic viability, environmental friendliness, and the potential for high energy density. Among them, Fe-rich compositions exhibit higher initial charge capacity and lower bill-of-material costs, while they fade rapidly and exhibit low initial coulombic efficiency, hindering their commercialization prospects. In this work, we investigate the failure of Fe-rich Na-NFM materials through X-ray absorption spectroscopy methods. The results reveal a combined failure mechanism that encompasses not only the conventional theory of Fe migration but also an abnormal Ni-redox deterioration, which has not yet been reported. More factors related to the failure of Fe-rich Na-NFM layered oxides are discussed in detail. These findings are expected to inspire targeted research efforts toward Fe-rich Na-NFM materials, thereby accelerating the practical application of sodium-ion batteries.
研究领域:
材料科学
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电化学
·
固态化学
·
储能
✓ 已验证
DOI
高影响因子
Advanced Science
·
2020
·Vol. 7
·期 21
·2002199
·
IF 15.84
Qiuyu Shen,Xudong Zhao,Yongchang Liu,Youpeng Li,Jian Zhang,Ning Zhang,Chenghao Yang,Jun Chen
Iron/manganese-based layered transition metal oxides have risen to prominence as prospective cathodes for sodium-ion batteries (SIBs) owing to their abundant resources and high theoretical specific capacities, yet they still suffer from rapid capacity fading. Herein, a dual-strategy is developed to boost the Na-storage performance of the Fe/Mn-based layered oxide cathode by copper (Cu) doping and nanoengineering. The P2-Na 0.76 Cu 0.22 Fe 0.30 Mn 0.48 O 2 cathode material synthesized by electrospinning exhibits the pearl necklace-like hierarchical nanostructures assembled by nanograins with sizes of 50–150 nm. The synergistic effects of Cu doping and nanotechnology enable high Na + coefficients and low ionic migration energy barrier, as well as highly reversible structure evolution and Cu/Fe/Mn valence variation upon repeated sodium insertion/extraction; thus, the P2-Na 0.76 Cu 0.22 Fe 0.30 Mn 0.48 O 2 nano-necklaces yield fabulous rate capability (125.4 mA h g −1 at 0.1 C with 56.5 mA h g −1 at 20 C) and excellent cyclic stability (≈79% capacity retention after 300 cycles). Additionally, a promising energy density of 177.4 Wh kg −1 is demonstrated in a prototype soft-package Na-ion full battery constructed by the tailored nano-necklaces cathode and hard carbon anode. This work symbolizes a step forward in the development of Fe/Mn-based layered oxides as high-performance cathodes for SIBs.
研究领域:
材料科学
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电化学
·
能源存储
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2015
·
IF 1.964
Xin Zhao,Lei Huang,Hongrui Li,Hang Hu,Jin Han,Liyi Shi,Dengsong Zhang
Different transition metals were used to modify V 2 O 5 -based catalysts (M-V, M = Cu, Fe, Mn, Co) on TiO 2 via impregnation, for the selective reduction of NO with NH 3 . The introduced metals induced high dispersion in the vanadium species and the formation of vanadates on the TiO 2 support, and increased the amount of surface acid sites and the strength of these acids. The strong acid sites might be responsible for the high N 2 selectivity at higher temperatures. Among these catalysts, Cu-V/TiO 2 showed the highest activity and N 2 selectivity at 225–375 °C. The results of X-ray photoelectron spectroscopy, NH 3 -temperature-programmed desorption, and in-situ diffuse reflectance infrared Fourier transform spectroscopy suggested that the improved performance was probably due to more active surface oxygen species and increased strong surface acid sites. The outstanding activity, stability, and SO 2 /H 2 O durability of Cu-V/TiO 2 make it a candidate to be a NO x removal catalyst for stationary flue gas.
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Materials Advances
·
2021
·Vol. 3
·期 1
·272-281
·
IF 0
J. Cheng,P. Ganesan,Z. Wang,M. Zhang,G. Zhang,N. Maeda,J. Matsuda,M. Yamauchi,B. Chi,N. Nakashima
Perovskite oxides with a low cost and high catalytic activity are considered as suitable candidates for the oxygen evolution reaction (OER)/oxygen reduction reaction (ORR), but most of them favour only either the ORR or the OER. Besides, their underlying catalytic mechanisms are subject of an ongoing debate. Herein, La0.8Sr0.2CoO3−δ (LSC) was selected as a base perovskite oxide for doping different elements into its B-site to fabricate four different La0.8Sr0.2Co0.8M0.2O3−δ (LSCM; M = Ni, Fe, Mn, and Cu) perovskite oxides. Among the catalysts tested with and without multi-walled carbon nanotubes (MWNTs), La0.8Sr0.2Co0.8Fe0.2O3−δ (LSCF) outperformed any other catalysts in terms of both OER and ORR activity. The OER/ORR activity enhancement with LSCF is also discussed based on spectroscopic and microscopic analyses and lattice oxygen transportation.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
CHEMOSPHERE
·
2022
·
IF 8.943
Yanchao Li,Can Wang,Shuang Pan,Xin Zhao,Ning Liu
Fe/Mn@carbon cloth (CC) was successfully fabricated through high-temperature shock (HTS) technique and used as cathode modification in heterogeneous electro-Fenton (hetero-EF) process for methylisothiazolinone (MIT) degradation. The nanocrystalline on Fe/Mn@CC electrode is doped with Fe and Mn oxides and coated with carbon layer, which could markedly enhance the electrocatalysis with high electro-chemical active area and low resistance. Fe/Mn@CC modified cathode can efficiently in-situ produce and activate H 2 O 2 , showing high electrocatalytic activity to MIT degradation. The 95.2% MIT degradation with in 100 min were achieved under the condition of 30 mA current, 0.75 L min −1 aeration intensity and initial pH = 3. Based on the CV curves and stability test, the high degradation activity revealed the kinetically beneficial regeneration of Fe II /Mn II in Fe/Mn@CC and activation of H 2 O 2 . The electron transfer between Fe II/III and Mn II/III , together with the direct Fe II /Mn II regeneration on the cathode, could markedly promote the H 2 O 2 utilization, and eventually lead to MIT degradation.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Tongdong Shen,Wentao Su,Qiangqiang Yang,Jun Ni,Shaoping Tong
MgM x O y (M = Fe, Mn) powders prepared by the sol-gel method were used as the catalysts for ozonation of p -hydroxybenzoic acid ( p -HBA) and acetic acid (AcOH) (20 mg/L) at a neutral pH for 9 min. The study aims to bring an insight into the synergetic mechanism for basic and acid sites of MgM x O y in heterogeneous catalytic ozonation. 84.8 %, 88.2 %, 86.7 % p -HBA were removed by ozonation catalyzed by MgFe x O y , MgMn x O y and MgO, respectively. 49.3 %, 65.8 %, 64.3 % AcOH were removed by ozonation catalyzed by the three catalysts, respectively. MgMn x O y exhibited the highest catalytic activity in ozonation of p -HBA and AcOH owing to the action of acid sites of MgMn x O y for additional ozone decomposition. The increase of solution pH, the protonation of surface hydroxyl groups and the electron transfer on acid sites induce ozone decomposition into reactive oxygen species in MgM x O y catalytic ozonation.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Dongdong Chu,Haoran Dong,Yangju Li,Junyang Xiao,Xiuzhen Hou,Shuxue Xiang,Qixia Dong
In this work, sulfur/nitrogen modified reduced graphene oxide (S/N-rGO) was employed as both electron shuttle and support to fabricate Fe-Mn bimetallic organic framework@S/N-rGO hybrids (BOF@S/N-rGO) via a facile two-step solvothermal route. Compared with the transition metal ions (Fe 2+ /Mn 2+ ), the classical metal oxide catalyst (Fe 2 O 3 and Fe 3 O 4 ) and nano zero-valent iron (nZVI), BOF@S/N-rGO catalyst can more effectively activate peroxydisulfate (PDS) with ultra-low concentration (0.05 mM) to degrade sulfamethazine (SMT). Quenching experiments, electron paramagnetic resonance (EPR) measurement and linear sweep voltammetry (LSV) showed that the activation pathways of PDS between the two catalysts were different. In BOF@N-rGO+PDS system, the degradation of SMT was mainly attributed to the oxidation of radicals including SO 4 •− and •OH, especially SO 4 •− . However, in BOF@S-rGO+PDS system, in addition to the radical pathway, there are also non-radical pathways, namely 1 O 2 and direct electron transfer . Furthermore, the applicability of BOF@S/N-rGO used in the PDS-mediated advanced oxidation processes (AOPs) was systematically investigated in terms of the effects of operating parameters and coexisting substance (anions and humic acid (HA)), the degradation of other pollutants, as well as the stability and reusability of the catalyst. This study proved that BOF@S/N-rGO was a promising activator of PDS with ultra-low concentration for the degradation of SMT.
研究领域:
环境科学
·
材料科学
·
催化化学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Rui Huang,Shaohua Luo,Qi Sun,Xin Yan,Haoran Zhang,Lixiong Qian,Xin Liu,Xingzhong Cao,Peng Zhang,Shengxue Yan
Fe/Mn-based cathode is considered a viable choice for sodium-ion batteries (SIBs) because of its affordability and high theoretical capacity. Nonetheless, bad actually comprehensive performance still impede its commercial application. In this work, based on the systematic study of P2-Na 2/3 Fe 1/2 Mn 1/2 O 2 cathode materials with fewer Mn vacancies (NFM-Q), we realized a superior rate, cycling performance, air stability and more importantly unraveled the operation mechanism. Specifically, dual function of fewer Mn vacancies were explicitly clarified, which included the effect of shrinking sodium layers and the sodium-ion diffusion promoting effect, as confirmed by combining XRD, XANES, XAFS, EIS and GITT. So Mn vacancy engineering had the potential to break the contradiction between “sodium limiting” based on air-stabilization mechanism and “sodium promoting” based on kinetics. This has rarely been found before. And a series of characterizations strongly declared rapidly cooling rate could effectively regulated the creation of Mn vacancies. As a result, NFM-Q cathode not only delivered outstanding discharge capacity (192.7 mAh/g), cycling stability (123.8 mAh/g, 65 %, after 50 cycles) and energy density (574.0 Wh Kg −1 ), but also possessed splendid air stability (185.8 mA h/g, 61.8 % after 50 cycles and immersion). Moreover, ex-situ XRD and XAS further expounded structural evolution and charge compensation mechanism of NFM-Q cathode, confirming its superior performance. This work might offer fresh understanding about the roles of Mn vacancy engineering, which could open up new possibilities on the material design and the property improvement of Fe/Mn-based cathodes.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Hua Zhong,Qin Qin,Zhuozhuo Wang,Hua Zhang,Yanling Qiu,Daqiang Yin,Xiaochang Liu,Zhiliang Zhu
Water pollution caused by emerging contaminants poses significant environmental and health risks, while the management of invasive algal biomass remains an underutilized resource. This study presents a novel Fe/Mn-modified in situ N-doped Enteromorpha prolifera-derived biochar catalyst (Fe/Mn/EP), addressing the dual challenges of efficient peroxymonosulfate (PMS) activation and utilization of invasive algal biomass. Through a straightforward one-step pyrolysis approach, the obtained catalyst integrated nitrogen functionalities and bimetallic active sites, enabling it to achieve an outstanding catalytic performance. It completely degraded carbamazepine (CBZ) in water samples within 30 min. The degradation process relied on the synergy between radical and nonradical pathways, primarily dominated by singlet oxygen (1O2) and superoxide radicals (·O2–). Specifically, in situ nitrogen doping, particularly involving pyrrole and graphite nitrogen, enhanced PMS activation by regulating the electronic properties and increasing the density of active sites. The degradation of CBZ significantly reduces the toxicity of the system by analysis prediction based on quantitative structure–activity relationship. The Fe/Mn/EP catalyst demonstrated broad adaptability across various emerging pollutants and real water matrices. This work highlights a sustainable strategy to transform problematic algae into high-performance biochar-based catalysts, offering a scalable solution for water pollution remediation.
研究领域:
环境科学
·
催化材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL GEOCHEMISTRY AND HEALTH
·
2019
·Vol. 42
·期 6
·1601-1615
·
IF 3.252
Tao Huan-yu,Ge Hui,Shi Jianghong,Liu Xiaowei,Guo Wei,Zhang Mengtao,Meng Yaobin,Li Xiao-yan
Abstract In this study, the effect of biochar (BC) derived from Litchi chinensis Sonn. and its modification, including Ca-biochar (Ca-BC) and Fe–Mn-biochar (Fe–Mn-BC), on the transportation of oestrone (E1) in water and soil was investigated. Fe–Mn-BC showed better adsorption ability than other types of biochar (BC, Ca-BC) under different conditions (humic acid, pH, ionic strength) in an aqueous environment. The maximum mass of sorbent at 298 K increased from 1.12 mg g −1 (BC) to 4.18 mg g −1 (Fe–Mn-BC). Humic acid had a greater impact on aqueous E1 adsorption on these biochars than did the pH and ionic strength. Fe–Mn-BC as a soil amendment had a great control of E1 transport in soil, and no leachate of E1 was observed in the column experiment. E1 mobility showed strong retardation in amended soil with Ca-BC ( R f = 11.2) compared with raw soil ( R f = 7.1). These results suggested that Fe–Mn-BC was more effective in controlling E1 transportation, and Fe–Mn-BC could be used as an alternative and inexpensive adsorbent to reduce E1 contaminants from water and soil. Graphic abstract
研究领域:
环境科学
·
土壤学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Xiao Zhou,Yabo Wang,Xuqian Wang,Yongkui Zhang
Peroxymonosulfate (PMS) activation technology represents an efficient approach to generate reactive oxygen species for treating pharmaceutical pollutants, and the fabrication of effective catalysts is of great significance for PMS activation technology. In this study, iron-manganese (Fe-Mn) layered double oxides (LDO) with flaky structure formed by metal oxide nanoparticles were synthesized by coprecipitation-calcination method and used to activate oxidant PMS to generate reactive oxygen species so as to realize the degradation of sulfathiazole (STZ). Benefiting from the well-dispersed structure and synergistic effect between bimetallic oxides, about 90% of STZ (20 mg L −1 ) could be removed with the dosage of catalyst (LDO-400, 0.4 g L −1 ) and PMS (0.4 g L −1 ) in 40 min catalysis process. Quenching experiments and in-situ electron paramagnetic resonance (EPR) analysis revealed that radical pathways dominated by surface-bound SO 4 − • and •OH were involved in the removal of STZ in LDO-400/PMS system. Besides, EPR and linear sweep voltammetry (LSV) analysis indicated the non-radical pathways containing 1 O 2 and electron transfer also contributed to STZ degradation. Five consecutive cycles were conducted to prove the stability and reusability of LDO-400. The intermediates in the STZ degradation process were identified to propose the STZ degradation pathways. Particularly, ecological structure-activity relationship (ECOSAR) predicted the relatively low ecological risk of LDO-400/PMS system for STZ degradation. This study not only proves the advantages of synergistic effect between bimetallic oxides, but also enriches the design strategy of environmental remediation.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
BIOMATERIALS
·
2023
·
IF 14
Zhenzhen Feng,Gui Chen,Min Zhong,Ling Lin,Ziyi Mai,Yan Tang,Guimei Chen,Wen Ma,Guang Li,Yuanyuan Yang,Zhiqiang Yu,Meng Yu
Pyroptosis is an inflammatory form of programmed cell death (PCD) that is regulated by the Gasdermin protein family in response to various stimuli, playing a critical role in the development of tumor therapy strategies. However, cancers are generally known to escape from PCD via immunosuppressive pathways or other resistant mechanisms. In this study, an acid-responsive Fe/Mn bimetal-organic framework nanosystem carrying metal ions and immune adjuvant R848 (FeMn@R@H) was designed for combining pyroptosis and augmented immunotherapy. The FeMn@R@H would be triggered to disintegrate and release Fe 3+ and Mn 2+ ions in response to the acidic tumor microenvironment (TME), thereby initiating Fenton-like reactions for ROS-mediated pyroptosis. On the one hand, the pyroptosis-caused cell rupture would induce the release of proinflammatory cytokines and immunogenic constituents from tumor cells, further resulting in immunogenic cell death (ICD) to promote antitumor immune responses. On the other hand, the co-delivered R848 could reverse suppressive tumor immune microenvironment (TIME) and induce inflammatory responses by activating the TLR7/8 pathway. In conclusion, this tumor-specific therapy system can co-deliver metal ions and R848 to tumor tissues to perform pyroptosis-mediated PCD and augmented anti-tumor immunotherapy.
研究领域:
癌症生物学
·
纳米技术
·
免疫治疗
·
药学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）