CARBON
·
2022
·
IF 11.307
Wenjie Wei,Fenghong Lu,Lixiu Cui,Yu Zhang,Yanze Wei,Lingbo Zong
Tuning of the coordination environment of atomically dispersed single atoms (SAs) by heteroatom doping is a promising strategy to boost the electrocatalytic activity for oxygen reduction reaction (ORR). The synergistic effect of dual heteroatom doping provides additional degrees of freedom to achieve higher ORR efficiency through decreased energy barriers of the intermediates in catalytic processes. Herein, Fe–SAs anchored within the N, S co-doped porous nanosized carbonaceous spheres (Fe–SAs@N/S-PCSs) was fabricated through the pyrolysis of anchored heteroatom sources and ferric precursors. Under the low catalyst loading capacity of 0.255 mg cm −2 , the obtained Fe–SAs@N/S-PCSs exhibits exceptionally high performance with ORR onset potential (E onset ) of 1.02 V, and half wave potential (E 1/2 ) of 0.90 V (vs. RHE) in 0.1 M KOH solution, outperforming benchmark Pt/C (E onset = 1.01 V, E 1/2 = 0.86 V). Superior oxygen evolution reaction (OER) activity (450 mV at 10 mA cm −2 ) is also demonstrated, thus displaying outstanding performance for Zn-air battery. The porous structure , rich accessible Fe SAs, and the optimal binding of ORR-related species induced by S doping in carbon matrix generate the excellent ORR activity and durability. This work provides insights into the rational design of cost-effective single atom catalysts (SACs) with impressive electrocatalytic activities for efficient energy conversion applications.
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WATER RESEARCH
·
2022
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IF 13.4
Qinyue Wu,Yan Zhang,He Liu,Hongbo Liu,Jia Tao,Min-Hua Cui,Zhiyong Zheng,Donghui Wen,Xinmin Zhan
For preparing high performance biochar to be applicated in persulfate-based oxidation treatment of wastewater, the feasibility of deriving Fe-N biochar from pharmaceutical sludge by endogenous Fe and exogenous N doping was investigated. With exogenous urea doping, Fe x N contained biochar (PZBC800U) was successfully derived from endogenous Fe(OH) 3 contained pharmaceutical sludge . PZBC800U effectively activated peroxymonosulfate (PMS) to remove 80 mg·L −1 levofloxacin (LEV) within 90 min. The main mechanism of PMS activation by PZBC800U for LEV degradation was revealed as non-radical pathways dominated by 1 O 2 generation and direct electron transfer . The formation of Fe x N combined with the increase of pyridinic-N in the biochar changed the electronic structure, improved the electron transfer ability, and thus achieved the excellent PMS activation capacity of the biochar. The vital function of endogenous Fe(OH) 3 was verified by comparing PZBC800U to Fe leached and extra Fe added controls. A total of 18 intermediates in the degradation of LEV were identified, and degradation pathways were proposed. Combined with the average local ionization energy calculation, the priority of piperazine breakage during LEV degradation was experimentally proved and mechanistically elucidated. This study provides a new insight into Fe x N biochar preparation from pharmaceutical sludge and the mechanisms of its excellent PMS activation performance for LEV degradation.
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高影响因子
Biomass Conversion and Biorefinery
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2022
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IF 4.05
Qu Qiang,Guo Xiaohui,Shao Zhijiang,Wang Xiuzhang,Zhu Mingqiang,Qiu Ling
Zanthoxylum branch became agricultural waste without proper utilization, and the pristine biochar (PB) had the limited removal capacity of Cr(VI) (21.75 mg g −1 ). In this study, zanthoxylum branch was fabricated to modified biochar (MZB) through impregnating with 0.4, 0.6, 0.8, and 1.0 mol L −1 Fe (NO 3 ) 3 solution and then pyrolyzing at 500 and 900 ℃. After sieving by batch adsorption experiment of Cr(VI), the optimal MZB was prepared with impregnating solution concentration of 0.4 mg L −1 and pyrolysis temperature of 900 ℃ (900MZB4), and displayed the outstanding Cr(VI) removal capacity (110.43 mg g −1 ). Besides, the effect of initial solution pH was evaluated, and removal process of Cr(VI) was a reaction of consuming protons. The fitting results of Langmuir model and pseudo-second-order kinetic model confirmed that the Cr(VI) removal reaction was a homogeneous chemisorption. Thermodynamic parameters demonstrated that the adsorption of Cr(VI) was an endothermic spontaneous process. The results of SEM and XRD suggested that zero-valent iron (Fe 0 ) particles were located on 900MZB4 surface and participated in the removal reaction of Cr(VI). The XPS analysis indicated 78.37% of Cr(VI) was reduced to Cr(III) by the cooperation of oxygen-containing functional groups (OFG) and Fe 0 . More OFG and higher surface area (130.36 m 2 g −1 ) revealed by FTIR and BET also contributed to the better characteristic of 900MZB4. In addition, 900MZB4 maintained removal efficiency at 81.22% after sixth regeneration cycles. Therefore, it is feasible to prepare high-efficient adsorbent from zanthoxylum branch for wastewater treatment. Graphical abstract
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CHEMOSPHERE
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2022
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IF 8.943
Lu Zheng,Yifan Gu,Baolv Hua,Jiarui Fu,Fengting Li
Metal-organic frameworks have been investigated in Fenton-like catalysis for tetracycline hydrochloride degradation, a widely used antibiotic which threatens the growth and health of creatures. However, powder phase and absence of large pores limit the materials’ degradation performance and application. In this work, a hierarchical macro-meso-microporous composite melamine sponge@MIL-101-Fe-NH 2 was firstly designed and constructed. While the micropores provided plenty of active sites to generate reactive oxygen species , the macropores and mesopores accelerated mass transfer. Besides, MIL-101-Fe-NH 2 particles dispersed on melamine sponge individually, exposing more catalytic sites and avoiding inactivation caused by aggregation compared to powder catalysts. Its catalysis performance for tetracycline hydrochloride degradation was evaluated through changing various influence factors like H 2 O 2 concentration, catalyst amount, pH and coexisting ions. Different from the preference of homogenous Fenton catalysts for pH 2–4, the composite displayed the most effective degradation at a subacid environment closer to nature with 77.24% in 30 min. Owing to the synergistic effect of hierarchical porous structure and monodispersed nanoparticles , the composite exhibited faster reaction rate and longer persistence compared to powder MIL-101-Fe-NH 2 . Easy recycling and less ion leaching made it advantages for practical application. •OH, •O 2 − and 1 O 2 active species contributed together to the degradation and two main possible degradation pathways were put forward based on 35 detected intermediates.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
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2022
·Vol. 57
·期 28
·13527-13540
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IF 4.682
Chen Dongli,Zhu Ming,Zhan Wenwei,Long Lei,Yu Lu,Zhu Tao,Kang Peibin,Yang Xiaoping,Sui Gang
Abstract Lithium–sulfur (Li–S) batteries have been considered as a promising substitute for lithium-ion batteries because of their high theoretical specific capacity, low cost, and environmental friendliness. However, the further practical application of Li–S batteries is greatly limited by the intrinsic insulation of sulfur, the shuttle effects of polysulfides and sluggish kinetics of the redox reaction. Herein, a well-designed Fe, N co-doped mesoporous carbon sphere (Fe-N-MCS) was fabricated to modify separator for absorbing and reutilizing polysulfides in high-performance Li–S batteries using cost-effective S cathode. The obtained Fe-N-MCS was not only acted as a physical barrier layer to block polysulfides, but also as trapper to capture and anchor polysulfides due to its highly porous structure and N dopants in the carbon frameworks. Furthermore, the high-conductive Fe-N-MCS barrier layer can facilitate electron and ion transfer to improve the electrochemical reutilization of polysulfide trapped therein, because the Fe-N-MCSs exhibited high catalytic activity for enormously boosting the redox kinetics of polysulfides. In consequence, the Li–S batteries with Fe-N-MCS modified separator exhibited high reversible capacity, superior rate capability and impressively cycling stability. The construction of non-precious metal barrier layer with catalyst activity is a promising pathway for the development of high-energy–density Li–S batteries. Graphical abstract The polysulfides were anchored and reutilized by the Fe-N-MCS layer for high-performance lithium sulfur battery.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Mingjie Huang,Sisi Peng,Wei Xiang,Chen Wang,Xiaohui Wu,Juan Mao,Tao Zhou
This study has revealed how the strong metal-support interaction (SMSI) between carbon nanotubes (CNTs) and Mn 0.65 Fe 2.35 O 4 (MnFeO) in boosting peroxymonosulfate (PMS) activation for rapid sulfamethoxazole (SMX) degradation. As synergized by CNTs, the PMS-activation efficiency of MnFeO could be enhanced by>24 times, but with the similar PMS-activation mechanism. It was explored that the SMSI-induced abundant surface hydroxyl groups, in cooperation with the highly hydrophobic CNTs, favored the rapid in situ interfacial degradation of SMX. This feature also endowed the MnFeO-CNTs catalyst resistance to high salinity waters containing inorganic anions (e.g., Cl - and NO 3 – ) of weak complexing abilities. Moreover, the SMSI allowed the greatly accelerated redox cycle rate of Mn species by electron-rich CNTs, resulting in efficient PMS activation. Furthermore, the application feasibility of the MnFeO-CNTs/PMS system was demonstrated for a SMX-spiked real reverse osmosis (RO) concentrate. It was found that higher concentration of PMS could realize the complete removal of SMX, despite the existence of electron-rich tyrosine-like substances would compete with the SMX degradation in the MnFeO-CNTs/PMS system. This study demonstrated that the SMSI could boost the PMS activation , and could serve as an effective material strategy for in situ interfacial organics degradation in the high salinity wastewater.
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TALANTA
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2021
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IF 6.057
Xuemin Huang,Qingfeng Liu,Cuimin Wu,Zhenyu Lin,Aiwen Huang,Bin Qiu
As a popular controllable-released carrier, intelligent hydrogels are often used in drug delivery and disease therapeutics. Meanwhile, benefit from the mimic-enzyme activity performance, Fe–N–C nanozymes have been widely used in sensing and analysis. However, the combination of intelligent hydrogels with specific degradability and Fe–N–C nanozymes with enhanced activity in one system to achieve controllable and sensitive detection is rare. Herein, we combine intelligent hydrogel with mimic peroxidase activity enhanced Fe–N–C nanozymes to construct a ratiometric fluorescence probe for sensitive detection of hyaluronidase (HAase). The modification of copper ions has been proved to enhance the mimic enzyme activity of Fe–N–C nanozymes greatly. Cu 2+ modified Fe–N–C nanozymes were embedded in hyaluronic acid hydrogel. In the presence of HAase, the HA hydrogel structure was hydrolyzed and released Cu 2+ -Fe-N-C nanozymes gradually. The released Cu 2+ -Fe-N-C nanozymes are used to catalyze the hydrogen peroxide system so that o-phenylenediamine is oxidized to orange fluorescent 2, 3-diaminophenolazine (DAP). Due to the electrostatic interaction , the fluorescence resonance energy transfer can occur between the negatively charged copper nanoclusters emitted by 430 nm and the positively charged DAP emitted by 560 nm. The activity of HAase was monitored according to the ratio of fluorescence intensity at 560 nm and 430 nm (F560/F430). The linear range of this method is 0–10.0 U/ml and the detection limit is 0.43 U/mL (S/N = 3). This strategy has been further applied to biological samples successfully.
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Journal of the Taiwan Institute of Chemical Engineers
·
2021
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IF 5.876
Xin Li,Shengxiao Zhang,Mingwu Yu,Hu Xu,Jungang Lv,Shuangshuang Yang,Xiaotong Zhu,Li Li
Background It was an effective method and research focus to remove recalcitrant organic pollutants by advanced oxidation processes based on persulfate activation with composite material as heterogeneous catalysts. Methods Fe/N co-doped biochar (Fe/N-BC) was synthesized via one-pot calcination method with anhydrous FeCl 3 , melamine, and grape skin powder as precursors. Characterization results showed that biomass and melamine could anchor iron species on BC matrixes by coordination. Significant findings The Fe/N 0.1 -BC exhibited significant activities toward peroxymonosulfate (PMS) activation, and 20 mg/L RhB can be degraded completely in 10 min with 0.05 g/L of the material and 0.5 g/L PMS. Electron paramagnetic resonance (EPR) study and free radical quenching experiments indicated that singlet oxygen ( 1 O 2 ), sulfate radicals (SO 4 •− ), and hydroxyl radicals (•OH) were the main reactive oxidizing species, and non-radical mechanism and free radical process were considered to be involved in the degradation of the pollutants. Control experiments revealed that the enhanced active sites were mainly ascribed to rich defects as well as the synergistic effect among Fe and N doping into carbon substrate. The Fe/N-BC owned the merits of environmentally friendly raw materials, easy synthesis, and high activation efficiency, exhibiting splendid prospect for environmental application.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2021
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IF 5.455
Zhongqing Wang,Lan Zhou,Rui Li,Konggang Qu,Lei Wang,Wenjun Kang,Haibo Li,Shenglin Xiong
The development of non-previous-metal electrocatalyst with low cost, high activity and stability towards oxygen reduction reaction (ORR) remains a challenge. Covalent organic frameworks (COFs) have emerged as promising candidates for the preparation of porous metal/nitrogen co-doped carbon catalysts. In the present work, porous Fe-N x nanoclusters/carbon catalysts are prepared by pyrolyzing iron-containing covalent-triazine organic frameworks. It is found that the synthesis conditions including pyrolysis temperature and pressure have great impacts on the surface area of micropores, mesopores and macropores, which in turn influences the ORR activity of catalysts by varying the mass diffusion and the contact of active centers with electrolytes. The optimized catalyst (denoted as Fe 1.2 NC-0.02-800), having the highest both BET and external surface areas, shows much higher kinetic current density and catalytic stability than commercial Pt/C catalyst in ORR process. When being assembled into Zn-air battery, it also exhibits excellent performances in terms of open circuit voltage (1.45 V), power density (210 mW cm −2 at 330 mA cm −2 ) and specific capacity (713.1 mA h g Z n − 1 ), which outperform the corresponding values of Pt/C-based Zn-air battery. Moreover, 15 light-emitting diodes can be powered by two series-connected Zn-air batteries with Fe 1.2 NC-0.02-800 as the air-cathode catalyst, implying its promising application in clean energy conversion field.
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BIOMASS & BIOENERGY
·
2021
·
IF 5.061
Jingyue Wang,Yuelong Xu,Meifang Yan,Bin Ren,Xiaoxi Dong,Junfeng Miao,Lihui Zhang,Xinqiang Zhao,Zhenfa Liu
Porous biomass-carbon materials for supercapacitor applications have recently attracted attention. Chitin , which has abundant amides and hydroxyl groups, was used as an ideal precursor for carbon in this work. The chitin was treated with a one-step method to produce a heteroatom-loaded porous carbon material, and its electrochemical properties were significantly improved through the introduction of loaded elements. A mixture of chitin, zinc chloride , and heteroatoms was carbonized to obtain heteroatoms (N and S) and the bimetallic sulfide loaded hierarchical porous carbon. Then, the porous carbon with S, N, Zn, and Fe heteroatoms loading was used to prepare a supercapacitor with a specific capacitance of 277.4 F g −1 at 1 A g −1 . In addition, the supercapacitor had a specific capacitance retention rate of 90% at 5 A g −1 after 10,000 cycles. Therefore, hierarchical porous carbon materials loaded with heteroatoms and bimetallic sulfide were prepared by carbonization activation with chitin as the precursor. The resulting supercapacitor showed that the as-prepared porous biomass materials possessed ideal charging-discharging performance. Moreover, this work provides strategies for obtaining metal sulfides and heteroatom co-loading of carbon materials with excellent properties using a simple and efficient one-step method for renewable energy storage device applications.
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RSC Advances
·
2021
·Vol. 11
·期 18
·10540-10547
·
IF 3.361
Anxia Li,Xiaoxin Yang,Juan Chen
Metal–organic frameworks (MOFs), such as MIL-53(Fe), have considerable potential as drug carriers in cancer treatment due to their notable characteristics, including controllable particle sizes, high catalytic activity, biocompatibility and large porosity, and are widely used in a broad range of drugs. In this study, a new approach for the synthesis of MIL-53(Fe) nanocrystals with controlled sizes has been developed using a non-ionic surfactant PVP as the conditioning and stabilizing agent, respectively. During the nucleation of MIL-53(Fe), the PVP droplet, as a nano-reactor, controlled the growth of the crystal nucleus. The size and aspect ratio (length/width) of nanocrystals increased with an increase in PVP in the synthetic mixture. The MIL-53(Fe) nanocrystals showed a homogeneous morphology, with approximately 190 nm in length and 100 nm in width. MIL-53(Fe) not only was used to load the anticancer drug doxorubicin (DOX) but also generated hydroxyl radicals (˙OH) via a Fenton-like reaction for ROS-mediated/chemo-therapy of cancer cells. The approach was expected to synthesize numerous types of nano-size iron(III)-based MOFs, such as MIL-53, 89, 88A, 88B and 101. The MIL-53(Fe) nanocrystals hold great promise as a candidate to improve the controlled release of drugs and treatment effect for cancer therapy.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
·
IF 4.539
Bin Ren,Junfeng Miao,Shasha Wang,Yuelong Xu,Zuozhao Zhai,Xiaoxi Dong,Zhenfa Liu
In this study, a 3D Fe-based and N-doped coral-like carbon composite (Fe-NGLC) was successfully prepared via the simple impregnation of a self-made 3D nitrogen-enriched and porous layered graphene-like support with Fe 2 (SO 4 ) 3 as the precursor. It was characterized through X-ray diffractometry, scanning electron microscopy, X-ray photoelectron spectroscopy, etc.; Fe-NGLC exhibited regular three-dimensional coral-like structures with dense porosity and high of Fe–N species content. As a heterogeneous Fenton catalyst of the methylene blue (MB) degradation, the prepared composite showed impressive activity over a wide pH range (4–10). Almost 100% of the MB could be degraded in 60 min, and the results agreed well with the pseudo-first-order kinetic model . To identify the crucial active sites of MB degradation, the correlation between the rate constant derived from the pseudo-first-order kinetic model and the different Fe species in the catalyst prepared under various conditions was investigated. This revealed the key role of the Fe–N complexes for the heterogeneous Fenton reaction. Moreover, Fe-NGLC exhibited recyclability and only a slight decrease in removal efficiency after five cycles. The excellent performance of Fe-NGLC demonstrates its great potential as a Fenton catalyst for wastewater treatment .
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