Environmental Science-Advances
·
2023
·Vol. 2
·期 5
·731-739
·
IF 0
Wen Wen,Yina Liu,Zhongping Li,Guangming Wen,Hung-Wing Li,Li Li
In this study, we report a simple pyrolytic strategy for N–C co-doped Fe-based nanoparticles (Fe–N–C) and exhibit their oxidase-mimicking and peroxidase-mimicking activity in a chromogenic reaction with 3,3′,5,5′-tetramethylbenzidine dihydrochloride (TMB) as a substrate. Structural analysis revealed that Fe–NX and Fe3C structures were formed with Fe-Imace coordination compounds as precursors and melamine as the nitrogen source, which provided abundant active sites for the Fe–N–C nanozyme. Interestingly, owing to the blocking effect triggered by π–π stacking between the tetracycline antibiotics (TCs) tetraphenyl skeleton and Fe–N–C, the substrate affinity of the Fe–N–C was significantly blocked, resulting in the solution fading. Under the optimum conditions, the UV absorption intensity versus the concentration of TCs was found to be linear over the range of 0.08–90 μM for tetracycline (TC), 0.1–80 μM for chlortetracycline (CTC) and 0.09–100 μM for oxytetracycline (OTC). The detection limits were 62 nM for TC, 85 nM for CTC and 88 nM for OTC. The Fe–N–C displayed good storage and long-term stability when stored at 4 °C for 30 days. In addition, based on its superparamagnetism, Fe–N–C can be effectively recycled and reused through an external magnetic field, avoiding secondary pollution.
研究领域:
分析化学
·
生物医学工程
·
环境科学
✓ 已验证
DOI
Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
·
IF 16.6
Zhang Shuo,Wu Jianghua,Zheng Mengting,Jin Xin,Shen Zihan,Li Zhonghua,Wang Yanjun,Wang Quan,Wang Xuebin,Wei Hui,Zhang Jiangwei,Wang Peng,Zhang Shanqing,Yu Liyan,Dong Lifeng,Zhu Qingshan,Zhang Huigang,Lu Jun
Electrochemical conversion of nitrate to ammonia offers an efficient approach to reducing nitrate pollutants and a potential technology for low-temperature and low-pressure ammonia synthesis. However, the process is limited by multiple competing reactions and NO 3 − adsorption on cathode surfaces. Here, we report a Fe/Cu diatomic catalyst on holey nitrogen-doped graphene which exhibits high catalytic activities and selectivity for ammonia production. The catalyst enables a maximum ammonia Faradaic efficiency of 92.51% (−0.3 V(RHE)) and a high NH 3 yield rate of 1.08 mmol h −1 mg −1 (at − 0.5 V(RHE)). Computational and theoretical analysis reveals that a relatively strong interaction between NO 3 − and Fe/Cu promotes the adsorption and discharge of NO 3 − anions. Nitrogen-oxygen bonds are also shown to be weakened due to the existence of hetero-atomic dual sites which lowers the overall reaction barriers. The dual-site and hetero-atom strategy in this work provides a flexible design for further catalyst development and expands the electrocatalytic techniques for nitrate reduction and ammonia synthesis.
研究领域:
催化
·
电化学
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 46
·17265-17274
·
IF 4.39
Yun-Wu Li,Shi-Kun Su,Cai-Zhen Yue,Jun Shu,Peng-Fang Zhang,Fang-Hui Du,Su-Na Wang,Hui-Yan Ma,Jie Yin,Xin Shao
Electrochemical water splitting is convinced as one of the most promising solutions to combat the energy crisis. The exploitation of efficient hydrogen and oxygen evolution reaction (HER/OER) bifunctional electrocatalysts is undoubtedly a vital spark yet challenging for imperative green sustainable energy. Herein, through introducing a simple pH regulated redox reaction into a tractable hydrothermal procedure, a hierarchical Fe3O4@MnOx binary metal oxide core–shell nano-polyhedron was designed by evolving MnOx wrapped Fe3O4. The MnOx effectively prevents the agglomeration and surface oxidation of Fe3O4 nano-particles and increases the electrochemically active sites. Benefiting from the generous active sites and synergistic effects of Fe3O4 and MnOx, the Fe3O4@MnOx-NF nanocomposite implements efficient HER/OER bifunctional electrocatalytic performance and overall water splitting. As a result, hierarchical Fe3O4@MnOx only requires a low HER/OER overpotential of 242/188 mV to deliver 10 mA cm−2, a small Tafel slope of 116.4/77.6 mV dec−1, combining a long-term cyclability of 5 h. Impressively, by applying Fe3O4@MnOx as an independent cathode and anode, the overall water splitting cell supplies a competitive voltage of 1.64 V to achieve 10 mA cm−2 and super long cyclability of 80 h. These results reveal that this material is a promising candidate for practical water electrolysis application.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
PubMed
高影响因子
BIOMATERIALS
·
2013
·
IF 7.604
Shuai Xu,Jing Liu,Dian Li,Liming Wang,Jia Guo,Changchun Wang,Chunying Chen
We propose a modular synthetic strategy to constitute metallosalphen prodrugs in the form of coordination polymer nanoparticles , comprising magnetite nanocrystal colloidal cluster as core and salphen-In III coordination polymer as shell. These composite nanoparticles are not only equipped with intense photoluminescence , sensitive magnetic responsiveness and pH-dependent degradability, but also serve as prodrugs to accomplish intercellular conversion from non-toxic nanoparticles (Fe 3 O 4 @Salphen-In III ) to pharmacologically active complexes (Fe–salphen), allowing to specifically inhibit the proliferation of A549 cancer cells via caspase activation.
研究领域:
材料科学
·
生物医学工程
·
肿瘤学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Yaping Zhang,Yanan Zhao,Yixin Qi,Yanyan Lin,Yuhang Cheng,Mengmeng Sun,Lei Wang
Photogenerated holes have emerged as critical mediators for activating peroxymonosulfate (PMS) in the coupled photocatalytic PMS activation system, enabling novel dual-channel activation pathway. A tandem system based on Fe-MOF@BiVO 4 (Vis/PMS/Fe-MOF@BVO) with spatially separated active sites was constructed to form a dual-channel activation mechanism. The BiVO 4 (010) face provides the active sites for photogenerated electrons to drive the Fe 3+ /Fe 2+ cycle and activate PMS, while the BiVO 4 (110) face serves as the active sites for photogenerated holes to activate PMS. Consequently, the Vis/PMS/Fe-MOF@BVO system achieved complete degradation of 10 mg/L BPA within 6 min, with a degradation rate constant (K obs ) of 0.74 min −1 . It also demonstrated high removal efficiency for various organic pollutants with excellent immunity to interference and reusability. This work provides a new insight into the coordinative mechanism for coupled photocatalysis and PMS activation system.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Ning Liu,Fuhao Fei,Wangxi Dai,Jianqiu Lei,Fukun Bi,Botao Wang,Guixiang Quan,Xiaodong Zhang,Liang Tang
Herein, a highly efficient Z-scheme SnS 2 /MIL-88B (Fe) (SnSFe) heterojunction was successfully synthesized to use both as photocatalysts and persulfate (PS) activator for ibuprofen (IBP) degradation. Flower-liked SnS 2 was uniformly loaded on MIL-88B (Fe), and SnSFe retained the original polyhedral morphology of MIL-88B (Fe). The highest removal of IBP was achieved in the presence of SnSFe with 0.5% SnS 2 (SnSFe0.5). Characteristic results and density functional theory calculations demonstrated that the enhanced degradation of IBP was due to the difference in Fermi energy levels of SnS 2 and MIL-88B (Fe) leading to electrons transferred from SnS 2 to MIL-88B (Fe), and Sn O bond was formed in SnSFe. , OH and O 2 − were the main active species in SnSFe0.5/PS/visible light system. Z-scheme heterojunction of SnSFe was constructed to propose the degradation mechanism. This research revealed that the synergism of photocatalysis and PS activation using SnS 2 /Fe-based MOFs composites possessed great potentials in wastewater remediation.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
Energy Storage Materials
·
2020
·
IF 16.28
Chong Bai,Huijie Jin,Zongshuai Gong,Xizheng Liu,Zhihao Yuan
Aqueous Fe-I 2 rechargeable batteries are highly desirable for large-scale energy storage because of their intrinsic safety, cost effective, and wide abundance of iron and iodine. However, their development suffers from Fe dendrite growth and severe shuttle effect during cycling. Herein, we demonstrate a high-performance Fe-I 2 rechargeable battery using metal iron as anode, iodine/hierarchically porous carbon composite as cathode and an eco-friendly aqueous electrolyte. The anode modified with ascorbic acid effectively suppresses the formation of iron dendrite, while the cathode doped with nitrogen greatly reduces the shuttle of iodine species. The battery operates a reversible redox reaction of FeI 2 /I 2 pair with fast kinetics. A capacity ~190 mAh g -1 at current densities up to 5000 mA g -1 and excellent cycle stability of 100% after 550 cycles at 2000 mA g -1 are obtained. The battery achieves superior power density of ~1300 W kg -1 at 120 Wh kg -1 and high energy density of 130 Wh kg -1 at 356 W kg -1 . Our study shows great promise for high-performance rechargeable batteries with low-cost, eco-friendliness and high safety.
研究领域:
能源存储
·
电池技术
·
材料科学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2018
·
IF 4.229
Jiqiong Lian,Yihui Wu,Houan Zhang,Siyong Gu,Zhiwei Zeng,Xiaoyun Ye
Design of inexpensive and highly efficient bifunctional electrocatalyst is paramount for overall water splitting . In this study, amorphous Ni–Fe–P alloy was successfully synthesized by one-step direct-current electrodeposition method. The performance of Ni–Fe–P alloy as a bifunctional electrocatalyst toward both hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) was evaluated in 30 wt% KOH solution. It was found that Ni–Fe–P alloy exhibits excellent HER and OER performances, which delivers a current density of 10 mA cm −2 at overpotential of ∼335 mV for HER and ∼309 mV for OER with Tafel slopes of 63.7 and 79.4 mV dec −1 , respectively. Moreover, the electrolyzer only needs a cell voltage of ∼1.62 V to achieve 10 mA cm −2 for overall water splitting. The excellent electrocatalytic performance of Ni–Fe–P alloy is attributed to its electrochemically active constituents, amorphous structure, and the conductive Cu Foil.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Ruixue Shi,Tianbao Liu,Jing Lu,Xiangjing Liang,Andrei Ivanets,Junqin Yao,Xintai Su
Biochar derived from municipal sludge can be applied to adsorption. But it usually requires activation and pickling due to the generation of impurities such as metal oxide particles, which is uneconomical. Here, a facile strategy, acidification-one-step calcination, was developed and sludge-based Fe–C materials with good Cr(VI) removal effect were obtained by regulating the amount of hydrochloric acid . The results show that the adsorption capacity of Fe/C-5 (the best sample) for Cr(VI) was 150.84 mg g −1 . According to the Langmuir isotherm and pseudo-second-order kinetic model, the removal of Cr(VI) by Fe/C-5 is spontaneous and endothermic chemisorption process. In addition, Fe/C-5 has good ability to remove Cr(VI) under the interference of coexisting ions, and has good cycle stability. The removal of Cr(VI) by Fe/C-5 is considered to be synergistic process of adsorption and reduction. The Fe atoms were highly dispersed in Fe/C-5 and tightly bonded with C atoms, which not only strengthened the Cr(VI) adsorption by electrostatic attraction, but also activated the C atoms in the biochar material, so that the C atoms can reduce Cr(VI) to Cr(III) under acidic conditions. This may be due to the fact that acid pretreatment converted the iron in municipal sludge in the form of Fe–O/OH to free Fe 3+ and entered the C lattice during the calcination process. In this work, Fe–C materials with excellent Cr(VI) adsorption capacity were prepared by one-step calcination method, which has important reference significance for the resource utilization of municipal sludge.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
Journal of Water Process Engineering
·
2023
·
IF 7
Guobin Li,Zhenbang Han,Tao Wang,Minghui Zhang,Qiaoqiao Liu,Tong Zhang,Xiaoming Zhao
Fe-doped graphitic carbon nitride (g-C 3 N 4 ) represents an attractive photo-Fenton catalyst for organic contaminants removal, but the practical performances still need to be improved for large-scale application. Herein, we developed a high-efficiency photo-Fenton catalyst by anchoring Fe-g-C 3 N 4 onto an amidoxime-functionalized polyacrylonitrile fiber (AP) substrate through a simple hydrothermal approach. Comprehensive characterizations demonstrate the strong catalyst-support interaction via the axial coordination bonding between -OH groups and Fe 3+ , which could induce electric polarization of Fe-g-C 3 N 4 to promote the H 2 O 2 adsorption and activation. The fibrous support could also accelerate the photoelectrons transfer from g-C 3 N 4 to Fe 3+ by strengthening the d-π conjugated large π bond, as well as alleviate the backflow recombination from Fe 3+ to g-C 3 N 4 through the electron sink effect. These synergistic qualities resulted in superior photo-Fenton performance for organic contaminants removal, which delivered 4.0-fold higher degradation kinetics than that of the Fe doped g-C 3 N 4 powder catalyst and exhibited unexpected high activity at strong basic environment (pH = 12). Our work demonstrates an ingenious and simple way to design exceptional photo-Fenton catalysts for environmental remediation.
研究领域:
环境科学
·
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
Journal of Cleaner Production
·
2019
·
IF 6.395
Shuanghong Tian,Shuang Xu,Jinting Liu,Chun He,Ya Xiong,Pingyun Feng
A water-stable cationic Fe based metal organic framework, CPM-97-Fe, was successfully synthesized in a large scale by a modified method (CPM: Crystalline Porous Materials). The adsorption behaviors , including removal efficiency, adsorption kinetics and isotherms of nine hazardous dyes in wastewater were investigated with different pH and organic solvents. The pseudo-second-order adsorption rate constant follows the order of Reactive Brilliant Red X-3B (X-3B, 0.0205 g mg −1 min −1 ) > Acid orange 7 (AO7, 0.0112 g mg −1 min −1 ) > Congo Red (CR, 0.0080 g mg −1 min −1 ) > Methylene Blue (MB, 0.0061 g mg −1 min −1 ) > Rhodamine B (RhB, 0.0049 g mg −1 min −1 ) > Croscein Scarlet 3B (CS3B, 0.0041 g mg −1 min −1 ) > Methyl Blue (MB, 0.0017 g mg −1 min −1 ) = New Coccine (NC, 0.0017 g mg −1 min −1 ) > Acid Black 1 (AB1, 0.0014 g mg −1 min −1 ). It is found that the adsorption quasi-equilibrium can reach quickly within 30 min, but the dyes with proper structure (i.e. proper distance between two sulfonic groups, less azo benzene hindrance effect, more reactive Cl groups, and more benzene rings), smaller molecular size, more negative charges, lower molecular mass favor the faster adsorption. The adsorption capacity obeys another sequence of CR (831 mg g −1 ) > X-3B (648 mg g −1 ) > AO7 (502 mg g −1 ) > MLB (380 mg g −1 ) > CS3B (356 mg g −1 ) > AB1 (325 mg g −1 ) > RhB (306 mg g −1 ) > MB (304 mg g −1 ) > NC (157 mg g −1 ). It is disclosed that CPM-97-Fe can adsorb more dyes with larger molecular mass , less negative charges, and a proper structure. Especially for Congo red, the adsorption capacity on CPM-97-Fe is 831 mgg −1 , 8.1 times that on activated carbon (103 mgg −1 ). Even the adsorption capacities of very bulky Rhodamine B and Methyl Blue reach as high as 306 and 304 mgg −1 , respectively, ranking the highest level among MOF materials. The special structure of CPM-97-Fe with big open windows and high specific surface area of 1397.0 m 2 g -1 contributes to the fast adsorption and high capacity towards all investigated dyes via the host-guest encapsulation mechanism including electrostatic interaction, ion exchange, π-π stacking interaction, as well as pore filling.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2023
·Vol. 170
·期 9
·092505
·
IF 3.9
Shuna Liu,Ben Yang,Anran Zuo,Yongming Tang
Ti/SnO2-Sb/PbO2 anodes were electrodeposited from methanesulfonate-based baths, and the effect of dopants such as PVP and Fe on the surface morphology, phase composition, electrocatalytic activity and stability was investigated. It is revealed that the inclusion of Fe effectively enhances the stability of PbO2 anode, while PVP can significantly improve its electrocatalytic activity. The Fe,PVP-codoped anode, Ti/SnO2-Sb/Fe-PVP-PbO2, exhibits the higher stability and electrocatalytic activity compared to the respective inclusion of Fe and PVP. The gradation efficiency of methyl orange (MO) on the Ti/SnO2-Sb/Fe-PVP-PbO2 anode is affected by the applied current density and the initial MO concentration. During degradation, the azo structure of MO is firstly cleaved, resulting in the rapid decolorization of solution. Demethylated MO and the anion of sulfanilic acid are detected as intermediates, and thus a plausible pathway of MO degradation is proposed.
研究领域:
环境科学
·
材料科学
·
电化学
✓ 已验证
DOI
高影响因子