Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 19
·11792-11801
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IF 10.733
Xiang Ao,Wei Zhang,Zhishan Li,Lin Lv,Yunjun Ruan,Hong-Hui Wu,Wei-Hung Chiang,Chundong Wang,Meilin Liu,Xiao Cheng Zeng
The scarcity and weak durability of precious metal catalysts are among the biggest obstacles to achieving cost-effective electrocatalysts in fuel cells and metal–air batteries. Hence, it is imperative to develop low-cost non-precious metal catalysts with comparable oxygen reduction reaction (ORR) activity to precious metal catalysts. Herein, we report a highly effective strategy for the facile synthesis of Fe/N-functionalized 3D porous carbon networks. A major advantage of the newly designed catalyst is that ultrafine Fe4N nanoparticles are grown and uniformly mounted on the carbon framework upon pyrolysis treatment at 800 °C, and co-exist with numerous in situ formed Fe–N4 moieties in the carbon matrix, being evidenced by using X-ray absorption and photoelectron spectroscopy. The new electrocatalysts exhibit high ORR activity, comparable/superior to that of the state-of-the-art Fe/N–carbon based catalysts reported to date. Specifically, the catalysts show a half-wave potential of 0.890 V (vs. RHE) and a limited current density of 6.18 mA cm−2. By resorting to experimental measurements and density-functional theory (DFT) calculations, the synergistic effects between Fe–N4 moieties and the Fe4N support are identified for the first time, which play a key role in boosting the catalytic performance of the Fe/N-functionalized porous carbon networks.
研究领域:
材料科学
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电化学
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催化
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能源材料
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Xingxing Huang,Yingzhang Shi,Cheng Liu,Zhiwen Wang,Jinhong Bi,Jimmy C. Yu,Ling Wu
A series of Cu 2 O clusters/MIL-100(Fe) heterojunctions with different Cu 2 O mass ratios were constructed as the photocatalysts for N 2 fixation. An optimal nitrogen fixation performance of 51.22 μmol·g −1 ·h −1 is achieved when the mass fraction of Cu 2 O is 20 %. Isotope analysis experiments confirmed that the nitrogen source is N 2 . Possible intermediate signals during photocatalytic reactions were detected by in situ DRIFTS. XPS results further confirm the formation of Cu 2 O/MIL-100(Fe) heterojunctions, and that the existence of Cu–O surface interactions is the key to efficient electron transfer. It is revealed that the improvement of the catalytic performance is derived from the formation of heterojunction which regulates the energy band structure as well as promotes the separation of photogenerated electron-hole pairs. This study proposes a possible mechanism of photocatalytic nitrogen fixation and emphasizes the role of surface interaction and electron transfer in type-II heterojunction in improving nitrogen fixation performance.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Chenrui Liu,Yun Liu,Zhi Dang,Shuai Zeng,Chengcheng Li
In this paper, a kind of novel core-shell structured heterogeneous photo-Fenton catalyst, boron-doped reduced graphene oxide wrapped Fe 3 O 4 (Fe 3 O 4 @B-rGO) composite, was successfully synthesized by heating the mixture of Borane-Tetrahydrofuran adduct and graphene oxide wrapped Fe 3 O 4 (Fe 3 O 4 @GO) under reflux conditions. The core-shell structure of the catalyst had been confirmed by X-ray diffraction (XRD), Raman spectroscopy, scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photo electron spectra (XPS), and electron energy loss spectrum (EELS). The experimental results for Bisphenol A (BPA) degradation demonstrated that the as-prepared catalyst exhibited much higher photo-Fenton catalytic activity than Fe 3 O 4 and reduced graphene oxide wrapped Fe 3 O 4 (Fe 3 O 4 @rGO). Additionally, Fe 3 O 4 @B-rGO with mass concentration of doped boron at 9.3% exhibited the optimum catalytic property, in which system the BPA degradation kinetic rate constant was almost 1.96 times and 1.82 times of that in the systems with Fe 3 O 4 and Fe 3 O 4 @rGO, respectively. Finally, the mechanism analyses verified that OH, O 2 − and h + were the main reaction species in this system, and photo-electron generated by boron doped reduce graphene oxide (B-rGO) can accelerate the redox between Fe(II) and Fe(III). The excellent photo-Fenton performance, stability and magnetic separation properties make it promising for the degradation of organic compounds in waste water under visible light.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Yujing Chen,Jipeng Meng,Di Bai,Chuang Li,Xiao Chen,Changhai Liang
Pt/xFe/ZSM-23 catalysts with various Fe contents were prepared to explore the influence of extra-framework Fe (EF-Fe) on the n-hexadecane (n-C16) hydroisomerization performance. UV–vis and 57Fe Mössbauer spectroscopic results suggest that the Fe species composition was significantly different under various Fe contents, with (HO–Fe(III)–O–Fe(III)–OH) and [Fe(OH)2]+ as the main Fe species at low Fe content (<1.98 wt %), whereas the Fe2O3 clusters/particles as the dominant ones at high Fe content (>1.98 wt %). Moreover, the concentration of Brønsted acid sites and Pt dispersion could be controlled by tailoring the Fe content. Correspondingly, the hydroisomerization performance of n-C16 over Pt/xFe/ZSM-23 catalysts was dramatically changed with various Fe contents. The Pt/1.98Fe/ZSM-23 catalyst with 1.98 wt % EF-Fe content exhibited considerably excellent hydroisomerization performance, and both n-C16 conversion and selectivity to iso-hexadecane (i-C16) could reach over 80 wt % when the reaction temperature was 310 °C.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2019
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IF 4.175
Xiang Li,Erbiao Cui,Zhen Xiang,Lunzhou Yu,Juan Xiong,Fei Pan,Wei Lu
Electromagnetic (EM) wave absorbing materials have been extensively applied in the electronic devices and wireless communication to solve the increasingly serious problems of electromagnetic pollution and radiation. In this work, Fe-MOFs/biomass cotton derived Fe@nanoporous carbon@carbon fiber (Fe@NPC@CF) composites were successfully obtained by means of in-situ synthesis and thermal decomposition processes. It was found that the Fe@NPC composites were uniformly distributed on the carbon fibers matrix. As a result, EM wave absorbing performances were greatly promoted via the synergic effects among Fe nanoparticles , nanoporous carbon and carbon fibers. A strong reflection loss ( RL ) of −46.2 dB and a wide absorbing bandwidth of 5.2 GHz ( RL < -10 dB) with a matching thickness of 2.5 mm were achieved for the Fe@NPC@CF composites with a low filling ratio of 25%. Therefore, this work not only paved the way for development of biomass as a green, low-cost and renewable high-performance carbon-based absorber, but also provided a good design and fabricating concept for the composite materials of EM wave absorber.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2024
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IF 4.1
Bo Wang,Peng Li,Zongbo Xie,Zhanggao Le
The photocatalytic hydroxylation of benzene to phenol using low-cost Fe-based materials is of great significance but remains a great challenge for the conversion of benzene in an efficient manner. Here we report a novel method to construct polymeric Fe-BTC-350 with highly dispersed coordinatively unsaturated (CUS) Fe centers by a simple pyrolysis of iron benzene tricarboxylic acid (Fe-BTC) coordination polymer. The CUS Fe centers in Fe-BTC-350 function as Lewis acid sites to accept both electrons and hydroxyl radicals, thus enhancing photocatalytic phenol generation. An optimal phenol yield of 22.7 % has been achieved over optimized Fe-BTC-350 which is 2.8 times that of the Fe-BTC. No evident decay in the activity was found after 4 cycles of consecutive reactions, indicating the robust stability of the photocatalyst. It is expected that the construction of CUS transition metal centers can also be utilized for other photocatalytic radical reactions.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2016
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IF 5.31
Yunfei Xue,Xiaogang Gu,Shuguang Lu,Zhouwei Miao,Mark L. Brusseau,Minhui Xu,Xiaori Fu,Xiang Zhang,Zhaofu Qiu,Qian Sui
The ability of Fe(II)-activated calcium peroxide (CaO 2 ) to remove benzene is examined with a series of batch experiments. The results showed that benzene concentrations were reduced by 20–100% within 30 min. The magnitude of removal was dependent on the CaO 2 /Fe(II)/Benzene molar ratio, with much greater destruction observed for ratios of 4/4/1 or greater. An empirical equation was developed to quantify the destruction rate dependence on reagent composition. The presence of oxidative hydroxyl radicals (HO ) and reductive radicals (primarily O 2 − ) was identified by probe compound testing and electron paramagnetic resonance (EPR) tests. The results of the EPR tests indicated that the application of CaO 2 /Fe(II) enabled the radical intensity to remain steady for a relatively long time. The effect of initial solution pH was also investigated, and CaO 2 /Fe(II) enabled benzene removal over a wide pH range of 3.0–9.0. The results of radical scavenging tests showed that benzene removal occurred primarily by HO oxidation in the CaO 2 /Fe(II) system, although reductive radicals also contributed. The intermediates in benzene destruction were identified to be phenol and biphenyl. The results indicate that Fe(II)-activated CaO 2 is a feasible approach for treatment of benzene in contaminated groundwater remediation.
研究领域:
环境科学
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化学工程
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DOI
PubMed
高影响因子
MOLECULES
·
2022
·Vol. 27
·期 7
·2288
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IF 4.927
Mengyuan Xu,Xi Li,Huiying Zheng,Jiehan Chen,Xiaohua Ye,Tiantian Liu
Nanomaterial technology has attracted much attention because of its antibacterial and drug delivery properties, among other applications. Metal-organic frameworks (MOFs) have advantages, such as their pore structure, large specific surface area, open metal sites, and chemical stability, over other nanomaterials, enabling better drug encapsulation and adsorption. In two examples, we used the common pathogenic bacteriumStaphylococcus aureusand highly infectious influenza A virus. A novel complex MIL-101(Fe)-T705 was formed by synthesizing MOF material MIL-101(Fe) with the drug favipiravir (T-705), and a hot solvent synthesis method was applied to investigate the in vitro antibacterial and antiviral activities. The results showed that MIL-101(Fe)-T705 combined the advantages of nanomaterials and drugs and could inhibit the growth ofStaphylococcus aureusat a concentration of 0.0032 g/mL. Regarding the inhibition of influenza A virus, MIL-101(Fe)-T705 showed good biosafety at 12, 24, 48, and 72 h in addition to a good antiviral effect at concentrations of 0.1, 0.2, 0.4, 0.8, 1.6, and 3 μg/mL, which were higher than MIL-101(Fe) and T-705.Keywords:MIL-101(Fe);favipiravir;antibacteria;antiviral
研究领域:
纳米技术
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药学
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病毒学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Feng Cheng,Peng Zhou,Xiaowei Huo,Yang Liu,Yunxin Liu,Yongli Zhang
The photocatalytic behavior of the graphene oxide (GO) modified Fe(III)/peroxymonosulfate (Fe/PMS) system for bisphenol A (BPA) degradation was investigated. With the addition of GO, a dramatic enhancement of BPA degradation was obtained at pH 3.0 under visible light irradiation. According to ESR analysis and quenching tests, both SO 4 - and OH are responsible for BPA degradation. The characterization analysis demonstrates that Fe(III) can chelate with the oxygenic functional groups on the surface of GO forming a stable GO-Fe(III) complex. The detections of different kinds of Fe species reveal that Fe(III) can be reduced to Fe(II) by GO via intramolecular electron transfer in the GO-Fe(III) complex, and visible light could enhance this process. The Fe(III)/Fe(II) cycle not only occurs on the surface of GO, but also in aqueous solution via homogeneous reactions. In addition, the degradation pathway of BPA was proposed based on the identification of the intermediates using GC–MS and LC-MS techniques.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2024
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IF 8.1
Yunzhan Ying,Shikun Liang,Fayang Zhang,Xiangwei Xu,Chenbo Qian,Long Jiang,Jing Zhou,Yulong Wan,Lie Wang,Yuyuan Yao
The harmful impact of organic pollutants on aquatic ecosystems underscores the pressing need for effective remediation. While activating peroxymonosulfate (PMS) with Fe catalyst offers a promising approach for eliminating these pollutants, its widespread use is hindered by the sluggish regeneration of Fe 2+ from Fe 3+ . Here, this study demonstrates for the first time that combining an Fe catalyst with Mo 2 C (Fe-Mo 2 C) enhances the Fe³⁺/Fe 2 ⁺ cycle, thereby improving PMS activation. The Fe-Mo 2 C/PMS system achieved near-complete degradation of carbamazepine (CBZ) within only 8 minutes, with an impressive observed rate constant ( k obs ) of up to 0.624 min -1 , about 15 times greater than that of Fe-C catalyst. It also exhibits the capability to degrade a broad range of common antibiotics, phenols, and dye-like organic compounds. Through electron paramagnetic resonance (EPR) analysis and quenching experiments, it was verified that hydroxyl radicals (·OH), sulfate radicals (SO 4 ·- ), singlet oxygen ( 1 O 2 ), and superoxide radicals (·O 2 - ) species during the reaction, with the former three serving as the primary active species. These findings offer a hopeful avenue for the systematic development and enhancement of catalysts specifically designed to efficiently remediate organic pollutants in wastewater.
研究领域:
环境科学
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化学工程
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催化
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水处理
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Yingying Guo,Chenhui Wang,Yuhang Xiao,Xiaohong Tan,Weidong He,Jianpo Chen,Yan Li,Hao Cui,Chengxin Wang
Fe single-atom catalysts (SACs) have emerged as a promising alternative to platinum for catalyzing oxygen reduction reactions (ORR). Nevertheless, their practical applicability is hindered by insufficient stability caused by structural corrosion during ORR. Here, we developed an effective strategy to optimize and stabilize the Fe SAs (single-atoms) sites by implanting chromium (Cr) atomic clusters (ACs) to address the formidable deactivation issue of the best-performing yet unstable Fe-N-C catalysts. Cr AC -Fe 1 /N-S-C demonstrates an amazing stability with a negligible decline in activity after 100,000 CV cycles, and can maintain 81% of initial current after a continuous 50-hour operation period. Theoretical calculations and experimental evidence substantiate that the integration of Cr ACs not only weakens the binding of OH* to the Fe site, thereby facilitating the ORR process, but also eliminates in situ-generated reactive oxygen species (ROS) and retards Fe ion leaching from active sites, thus stabilizing of the Fe SA sites.
研究领域:
催化
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材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
QUIMICA NOVA
·
2024
·
IF 0.5
Wei Fuhua,Ren Qinhui,Wang Nannan,Chen Hongliang,Zhang Yutao,Liang Zhao
The synthesis of Fe-MOFs (metal-organic frameworks) was conducted using a solution heat method, followed by characterization through XRD (X-ray diffraction), SEM (scanning electron microscopy), and TG (thermogravimetry) analysis techniques. Subsequently, the Fe-MOFs were employed for norfloxacin removal. The experimental findings demonstrate that theoretical simulations of norfloxacin adsorption by Fe-MOFs involved the application of pseudo-first kinetic model, pseudo-second kinetic model, and adsorption isotherm. Chemisorption was identified as the primary mechanism observed. Notably, a maximum adsorption capacity of 197.7 mg g-1 was achieved at pH 10. These results underscore the practical feasibility of utilizing Fe-MOFs in applications related to norfloxacin adsorption.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子