Journal of Materials Chemistry A
·
2025
·
IF 9.5
Hui Wang,Xuefeng Zhang,Xiangfeng Wu,Yewei Kang,Yirui Huang,Zhaoye Zhao,Ziyan Li,Tingting Zhou,Junchuan Wang,Wei Zhu,Chengsi Pan
Bimetallic iron-based metal organic frameworks (MFe-MOFs) exhibit promising photocatalytic properties but face challenges typical of pristine MOFs, including low photoresponsive activity, inadequate band gap regulation, and weak photoconductivity. Here, we designed porphyrin-based COFs (TpPAM-COFs) to serve as a shell grown on NH2-Fe-MIL-101 nanoparticles (NPs) using an in situ solvothermal approach. Subsequently, a ligand-anchoring full-range metallization process was applied to introduce hetero metal ions throughout the core–shell composites, establishing a type-II scheme heterojunction (Fe/Cu-M@PC-Cu) via covalent bonding between NH2-Fe/Cu-MIL-101 and Cu-TpPAM-COFs. The Cu-TpPAM-COF shell, with broad light absorption range, enhanced the generation of photogenerated electrons, facilitating the reduction of Cu2+ and Fe3+ within the Fe/Cu-M@PC-Cu heterojunction and promoting the regeneration of Cu+ and Fe2+ Fenton active sites. Moreover, rapid electron transfer between Fe3+ and Cu+ centers amplified the Fe3+/Fe2+ redox cycle, accelerating the catalytic decomposition of H2O2 and increasing ·OH radical production. Additionally, the optimized bandgap structure of Cu-TpPAM-COFs enhanced the oxidation capacity, as evidenced by the Fe/Cu-M@PC-Cu composite achieving exceptional photo-Fenton catalytic efficiency with 92.7% tetracycline hydrochloride (TCH) degradation in 35 minutes, surpassing that of most reported similar catalysts. Furthermore, the composite showed excellent stability, with only an 11.9% loss in photo-Fenton degradation efficiency after 8 cycles, highlighting its great potential for addressing challenging environmental pollutants.
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
Nature Catalysis
·
2022
·Vol. 5
·期 6
·503-512
·
IF 40.706
Xiao Fei,Wang Qi,Xu Gui-Liang,Qin Xueping,Hwang Inhui,Sun Cheng-Jun,Liu Min,Hua Wei,Wu Hsi-wen,Zhu Shangqian,Li Jin-Cheng,Wang Jian-Gan,Zhu Yuanmin,Wu Duojie,Wei Zidong,Gu Meng,Amine Khalil,Shao Minhua
Proton exchange membrane fuel cells convert hydrogen and oxygen into electricity without emissions. The high cost and low durability of Pt-based electrocatalysts for the oxygen reduction reaction hinder their wide application, and the development of non-precious metal electrocatalysts is limited by their low performance. Here we design a hybrid electrocatalyst that consists of atomically dispersed Pt and Fe single atoms and Pt–Fe alloy nanoparticles. Its Pt mass activity is 3.7 times higher than that of commercial Pt/C in a fuel cell. More importantly, the fuel cell with a low Pt loading in the cathode (0.015 mg Pt cm −2 ) shows an excellent durability, with a 97% activity retention after 100,000 cycles and no noticeable current drop at 0.6 V for over 200 hours. These results highlight the importance of the synergistic effects among active sites in hybrid electrocatalysts and provide an alternative way to design more active and durable low-Pt electrocatalysts for electrochemical devices.
研究领域:
材料科学
·
电化学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Fei Miao,Zehao Liu,Xin Kang,Cheng Cheng,Xiaoyu Mao,Ruimeng Li,Heng Lin,Hui Zhang
Heterogeneous catalytic oxidation based on iron species for peroxymonosulfate (PMS) activation is considered as one of the most attractive strategies for wastewater treatment. However, the rate-limiting regeneration of Fe(II) from Fe(III) heavily hampers the efficient activation of PMS. In this study, the introduction of electric field to the Fe-supported bentonite (Fe-B) activated PMS process was proposed to enhance the Fe(III)/Fe(II) redox cycle. The Fe-B catalyst performed well in the removal of Acid Orange 7 (AO7) through the synergistic effect of electrolysis and the continuous redox cycle of Fe(III)/Fe(II) for PMS activation. The use of 0.5 g L −1 Fe-B catalyst and 10 mM PMS yielded nearly complete removal of the AO7 (50 mg L −1 ) in 60 min at 2 mA cm −2 of current density. Based on the results of electron paramagnetic resonance (EPR) spectroscopy, chemical quenching tests, X-ray photoelectron spectroscopy (XPS) analysis, and electrochemical measurements, the decolorization of AO7 was dominantly attributed to surface-bound radicals (SO 4 •− ads and • OH ads ) and also the direct electron transfer at DSA anode. Moreover, the electro/Fe-B/PMS system showed an effective pH range from 2.6 to 9.0 and the abatement of AO7 was slightly affected in the presence of natural background anions. This work provides a feasible strategy of PMS activation by cost-effective Fe-B catalyst coupling with electric field and gives an insight into the accelerated oxidation of recalcitrant pollutants.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Ruobai Li,Zhiming Chen,Meixuan Cai,Jiaxing Huang,Ping Chen,Guoguang Liu,Wenying Lv
Metal-organic frameworks (MOFs) have attracted tremendous interest as photocatalysis for the destruction of organic contaminants. Herein, we synthesize a Fe-based MOF namely MIL-53(Fe), combined with Fe(III) and percarbonate, exhibits photocatalytic activity for the destruction of Sulfamethazine (SMT) under visible LED light irradiation. The morphology and physicochemical properties of the MIL-53(Fe) were determined using X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive X-ray spectra (EDS), Fourier transform infrared spectroscopy (FTIR) and photoluminescence spectroscopy (PL). The results indicated that the photocatalytic performance of MIL-53(Fe) with unsatisfactory efficiency resulted from the rapid recombination of photogenerated electrons and holes. This may be suppressed through the introduction of an external electron acceptor (e.g., Fe(III) and percarbonate) to the catalytic process. It could be seen that the SMT degradation efficiency in the system of Vis/MIL-53(Fe)/Fe(III)/SPC attained nearly 90% within 60 min, while only 12% achieved in the system of Vis/MIL-53(Fe). The quenching experiments and EPR analysis were employed to illuminate the predominant reactive species in the system of Vis/MIL-53(Fe)/Fe(III)/SPC. It must be mentioned that the higher separation efficiency of photoinduced electron- hole pairs was achieved via the addition of Fe(III). The accelerated photocatalytic degradation of SMT could be attributed to the subsequent formation of reactive species, which were generated from the activation of SPS by Fe(II) reduced from Fe(III) in the Vis/MIL-53(Fe)/Fe(III)/SPC system. Furthermore, the mineralization of SMT was systematically investigated, as well as the effects of operating parameters (e.g., the dose of catalyst, the concentration of Fe(III), and pH). The work has expanded the possibility of MOFs as visible light responsive photocatalysts together with percarbonate for the remediation of contaminated water.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Ning Gu,Yueyang Xu,Yan Yin,Xuzhao Gao,Yongping Zeng
SO x released from the combustion of sulfur-containing compounds in fuels pollute the environment and have a serious impact on human health. Adsorption desulfurization is an effective and environmentally friendly technique for removing sulfur-containing compounds from fuels. Metal-organic frameworks (MOFs) have high specific surface areas and can be easily modified and functionalized, making them excellent candidates for adsorption desulfurization in fuels. In this work, the precursor MIL-100(Fe)-SA was prepared using the hydrothermal method , and the adsorbent Ni@MIL-100(Fe)-SA was obtained by doping Ni 2+ into the resulting MIL-100(Fe)-SA using the impregnation method. FT-IR, X-ray diffraction, scanning electron microscopy, transmission electron microscopy and nitrogen adsorption-desorption isotherms were used to analyze the samples. The results indicated that Ni 2+ was successfully loaded onto MIL-100(Fe)-SA, and the MOF's structure remained stable. The adsorption performance of benzothiophene and thiophene was evaluated through batch adsorption experiments. The adsorption capacities of Ni@MIL-100(Fe)-SA for thiophene and benzothiophene were 23.68 mg S/g and 49.58 mg S/g, respectively. These observations could be ascribed to the π-complexation interactions between Ni 2+ of the framework and thiophenic compounds. The regeneration experiments demonstrated that the spent 11Ni@MIL-100(Fe)-SA-1.5 reach 86% of the adsorption capacity of fresh adsorbent after four cycles. Additionally, the regenerated adsorbent maintained good crystallinity after recycling.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS ES&T Water
·
2020
·
IF 0
Mingyue Zhao,Zhicheng Cui,Liang Fu,Fabrice Ndayisenga,Dandan Zhou
The slow reduction of Fe(III) to Fe(II) in electro-Fenton technology limits pollutant removal and causes Fe sludge production. This study hypothesizes that Shewanella, a dissimilatory iron-reducing bacteria, can accelerate the iron reduction of the Fenton reaction. A Shewanella biofilm coupled with Fe2O3 coated electrode (F/S) was used to drive the electro-Fenton reaction, and compared the results with the singlet Fe2O3 (F) anode and Shewanella biofilm anode (S). Meanwhile, dissolved oxygen (DO) is studied as an important influencing factor. The suitable DO was verified at ∼2 mg/L, phenol removal of F/S was 67% higher than that of the sum of three other singlet systems. The chemical oxygen demand (COD) removal was 72% and 50% higher than that of F and S, respectively. F/S corrosion current (Icorr) was 6.3 times higher than F, and induced hematite to transform into Fe2PO5 and FeOOH on the anode. Long-term operation showed that phenol was almost 100% removed for F/S; COD removal was generally 20% higher than F; thus, the toxicity of the effluent could be significantly decreased. The total Fe loss did not exceed 10% at the end of operation. This paper provides a feasibly novel method for electro-Fenton reaction, by employing Fe-reducing bacteria.
研究领域:
环境科学
·
微生物学
✓ 已验证
产品关联
DOI
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Xin Zhang,Qingling Fu,Hongqing Hu,Jun Zhu,Yonghong Liu
The co-oxidation of Fe(II) and As(III) occurs under aerobic conditions , and Fe(II) may largely determine the fate of As(III), but the effect of Fe(II) on the As(III) oxidation is barely explored. In this research, the limiting and driving roles of Fe(II) in As(III) oxidation were systematically studied through batch kinetic studies in combination with X-ray photoelectron spectroscopy (XPS) depth profiling, scanning electron microscopy and energy dispersive X-ray spectrometry (SEM-EDS), and quenching experiments. The results showed that As(III) oxidation efficiency increased with the increase of Fe/As molar ratio (from 63.1% to 98.3%), but decreased with the increase of pH (from 96.0% to 44.2%) and the increase of air flow rate (from 88.1% to 75.1%). The Fe(II) oxidation rate increased with the increase of pH and air flow rate. When Fe(II) was oxidized rapidly, As(III) was more likely to be immobilized in the “inner sphere” of formed Fe (hydr)oxides, limiting As(III) oxidation. On the other hand, Fe(II) was oxidized to produce Fe (hydr)oxides to adsorb or fix As(III); meanwhile, the ROS generated by Fenton-like reaction of Fe(II) promoted As(III) oxidation, especially, •O 2 − and H 2 O 2 were important ROS that drove the As(III) oxidation. These findings might provide a new insight for Fe(II) and As(III) geochemistry cycling in naturally occurring environment.
研究领域:
环境科学
·
地球化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Nan Zhao,Kunyuan Liu,Bofang Yan,Ling Zhu,Chuanfang Zhao,Jia Gao,Jujun Ruan,Weihua Zhang,Rongliang Qiu
In the last years, the synthesis and applications of biochar/Fe composites have been extensively studied, but only few papers have systematically evaluated their removal performances. Herein, we successfully synthesized and structurally characterized Fe 0 , Fe 3 C, and Fe 3 O 4 -coated biochars (BCs) for the removal of chlortetracycline hydrochloride (CH). Evaluation of their removal rate and affinity revealed that Fe 0 @BC could achieve better and faster CH removal and degradation than Fe 3 C@BC and Fe 3 O 4 @BC. The removal rate was controlled by the O–Fe content and solution pH after the reaction. The CH adsorption occurred on the O C groups of Fe 0 @BC and the O C and O Fe groups of Fe 3 C@BC and Fe 3 O 4 @BC. Electron paramagnetic resonance analysis and radical quenching experiments indicated that HO and 1 O 2 / O 2 − were mainly responsible for CH degradation by biochar/Fe composites. Additional parameters, such as effects of initial concentrations and coexisting anions, regeneration capacity, cost and actual wastewater treatment were also explored. Principal component analysis was applied for a comprehensive and quantitative assessment of the three materials, indicating Fe 0 @BC is the most beneficial functional material for CH removal.
研究领域:
环境科学
·
材料科学
·
化学工程
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS ES&T Engineering
·
2022
·
IF 0
Kunjie Hou,Zhoujie Pi,Fei Chen,Li He,Fubing Yao,Shengjie Chen,Xiaoming Li,Haoran Dong,Qi Yang
The practical application of the traditional Fenton system (Fe(II)/H2O2) is seriously hampered by the sluggish Fe(III)/Fe(II) cycle and the stringent acidic reaction condition. In this work, we found that trace-dissolved S(-II) (DS(-II), 5 μM) could significantly accelerate the Fe(III)/Fe(II) cycle and trigger a rapid H2O2 activation process in the Fe(III)/H2O2 system. Thus, more hydroxyl radicals (·OH) were generated for the rapid removal of various organic pollutants such as bisphenol A (BPA) and sulfamethoxazole (SMX) from water. Besides, the additive DS(-II) effectively broadened the application pH range of the Fenton or Fenton-like system. The constructed Fe(III)/DS(-II)/H2O2 system showed extensive applicability to different water matrices and maintained high BPA removal in the actual water sources. Furthermore, the toxicity assessment revealed that the toxicity of the target contaminant was diminished. The harmless SO42– was the final product of DS(-II) in the Fe(III)/DS(-II)/H2O2 system, and the residual DS(-II) was less than the threshold limit value for fresh or saltwater (0.5 mg/L). This discovery is expected to promote the large-scale practical application of iron-based Fenton or Fenton-like systems in practical organic wastewater purification.
研究领域:
环境科学
·
水处理
·
污染控制
✓ 已验证
DOI
TALANTA
·
2022
·
IF 6.556
Xuemei Ma,Jiayi Yu,Lin Wei,Qian Zhao,Liyong Ren,Zhiyong Hu
Simultaneous selective determination of Fe (Ⅱ) and Fe (Ⅲ) is of great significance to the study of iron ion tracking and release of iron supplement in gastric fluid. In this paper, a composite material (N-CQDs/AgNPs/β-CD) was prepared by a one-pot method. The various characterizations confirmed the silver nanoparticles (AgNPs) grew in situ on the surface of nitrogen-doped carbon quantum dots (N-CQDs), and the β-cyclodextrin (β-CD) and AgNPs linked together by Ag–O bonds finally presented gourd-like nanoparticles on the surface of N-CQDs. Then, N-CQDs/AgNPs/β-CD modified glassy carbon electrode (GCE) was applied to detect Fe(II) and Fe(III) simultaneously. The cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) results confirmed that N-CQDs/AgNPs/β-CD enhanced electrode performances because of the synergistic effect between N-CQDs, AgNPs and β-CD. The sensor was successfully applied for the determination by differential pulse voltammetry (DPV) of Fe(II) and Fe(III) released from four iron supplementations in simulated gastric fluid (SGF).
研究领域:
分析化学
·
生物医学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Sciences
·
2023
·
IF 6.9
Ting He,Jie Sun,Liangwei Deng,Jialin Ming,Changwei Hu
Due to its high efficiency, Fe(II)-based catalytic oxidation has been one of the most popular types of technology for treating growing organic pollutants. A lot of chemical Fe sludge along with various refractory pollutants was concomitantly produced, which may cause secondary environmental problems without proper disposal. We here innovatively proposed an effective method of achieving zero Fe sludge, reusing Fe resources (Fe recovery = 100%) and advancing organics removal (final TOC removal > 70%) simultaneously, based on the in situ formation of magnetic Ca-Fe layered double hydroxide (Fe 3 O 4 @CaFe-LDH) nano-material. Cations (Ca 2+ and Fe 3+ ) concentration (≥ 30 mmol/L) and their molar ratio (Ca:Fe ≥ 1.75) were crucial to the success of the method. Extrinsic nano Fe 3 O 4 was designed to be involved in the Fe(II)-catalytic wastewater treatment process, and was modified by oxidation intermediates/products (especially those with COO − structure), which promoted the co-precipitation of Ca 2+ (originated from Ca(OH) 2 added after oxidation process) and by-produced Fe 3+ cations on its surface to in situ generate core-shell Fe 3 O 4 @CaFe-LDH. The oxidation products were further removed during Fe 3 O 4 @CaFe-LDH material formation via intercalation and adsorption. This method was applicable to many kinds of organic wastewater, such as bisphenol A, methyl orange, humics, and biogas slurry. The prepared magnetic and hierarchical CaFe-LDH nanocomposite material showed comparable application performance to the recently reported CaFe-LDHs. This work provides a new strategy for efficiently enhancing the efficiency and economy of Fe(II)-catalyzed oxidative wastewater treatment by producing high value-added LDHs materials.
研究领域:
环境工程
·
废水处理
·
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
CATALYSIS COMMUNICATIONS
·
2017
·
IF 3.33
Zhiming Chen,Bo Xu,Xiaomei Wang,Li Zhang,Xiaoqing Yang,Cuncheng Li
Separation and recycling of noble metal nanoparticles after catalytic reaction is critical to promote its application efficiency and cut down the cost. This work presents a facile synthesis strategy for the fabrication of sandwich-like MIL-100(Fe)@Pt@MIL-100(Fe) (denoted as S-Pt) nanoparticles with high stability and improved catalytic activity for hydrogenation of nitrophenol. MIL-100(Fe) acts as both carrier to make the catalyst easily separated and shield to protect the tiny Pt nanoparticles from leaching or aggregation during reaction. Moreover, mass transfer effect of the porous MIL-100(Fe) with its pore structure serving as nano-reactor is also benefit for promoting the catalytic efficiency.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）