Materials Today Communications
·
2023
·
IF 3.8
Huilin Gao,Qizhang Huang,Qiaoguang Li,Lianying Wu,Haiyan Liao,Murtaza Hasan,Sheng Gong,Xinhua Zhou
Accurate detection of Fe 3+ is an urgent need due rapid increase of hemochromatosis, methemoglobinemia, mental decline and physical weakness throughout the world. Here, nitrogen-doped carbon quantum dots (NCQDs) having blue fluorescence were prepared by facile one-spot hydrothermal method by using binary carbon source. This innovative primed hybrid NCQDs were well characterized by using FT-IR, XPS , and EDS and SEM for purpose of chemical composition and surface functionality. The morphology of NCQDs were confirmed their spherical shape and an average diameter was 4.3 nm by TEM measurement. Surface coating for functional group and nitrogen doped was monitored by the FTIR, XPS and EDX analysis. The photoluminescence measurements showed that NCQDs were non-wavelength dependent with a quantum yield of 73.89%. The NCQDs showed strong evidence to be a excellent fluorescent sensor for the rapid and quick estimation of Fe 3+ with high selectivity and sensitivity. The fluorescence power of NCQDs were slowly declined with higher amount of Fe 3+ concentration ranging from 0.01 to 0.5 and 1–33.3 μM. The accurate range of detection limit was very narrow and found to be 5 nM for Fe 3+ by this method. Furthermore, the function of novel NCQDs for estimation of trace element such as Fe 3+ in different sources of water was yielded at very acceptable recoveries (97.30% ∼ 98.04%). The current designed functional probe provided a promising fluorescent range at narrow level for the Fe 3+ detection is highly appreciable in the future studies.
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高影响因子
FUEL
·
2023
·
IF 7.4
Fei Wang,Songyin Yu,Hui Xu,Junfeng Feng,Feihong Guo,Xiaoxiang Jiang,Jianchun Jiang
To solve the problem of harsh reaction conditions in lipid hydrogenation into fatty alcohol over Cu based bimetallic catalysts, the cheap Ni-base catalyst with high activity was synthesized. By using the hydrothermal method, the flower-like SiO 2 -ZrO 2 support was prepared. The Ni-Fe/SiO 2 -ZrO 2 catalyst was further prepared by the impregnation method and utilized in the fatty acid hydrogenation to produce fatty alcohol. Under the reaction conditions (240 °C, initial H 2 pressure: 2 MPa and reaction time: 3 h), the Ni-Fe/0.13SiO 2 -ZrO 2 catalyst attained 96.0% conversion and 86.4% fatty alcohol yield, much higher than that of Ni-Fe/ZrO 2 without SiO 2 (conversion 86.1% and fatty alcohol yield 61.9%). The high catalytic activity of Ni-Fe/0.13SiO 2 -ZrO 2 was ascribed to the increase of surface area, reduction of NiO grain size, and formation of flower-like morphology. The high selectivity to fatty alcohol over Ni-Fe/0.13SiO 2 -ZrO 2 was related to the increase of Lewis acidity (extra active sites) and the decrease of oxygen vacancy which weakened the adsorption of aldehyde (enol) on the catalyst and thus facilitated the formation of fatty alcohol.
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 27
·71088-71102
·
IF 5.8
Fan Xinfei,Liu Na,Yang Jia,Yu Yueling,Xu Yuanlu,Song Chengwen,Liu Yanming
Persulfate activation is emerged as an alternative applied in environment remediation, but it is still a great challenge to develop highly active catalysts for efficient degradation of organic pollutants. Herein, a heterogeneous iron-based catalyst with dual-active sites was synthesized by embedding Fe nanoparticles (FeNPs) onto the nitrogen-doped carbon, which was used to activate peroxymonosulfate (PMS) for antibiotics decomposition. The systematic investigation indicated the optimal catalyst exhibited a significant and stable degradation efficiency of sulfamethoxazole (SMX), in which the SMX can be completely removed in 30 min even after 5 cycle tests. Such satisfactory performance was mainly attributed to the successful construction of electron-deficient C centers and electron-rich Fe centers via the short C-Fe bonds. These short C-Fe bonds accelerated electrons to shuttle from SMX molecules to electron-rich Fe centers with a low transmission resistance and short transmission distance, enabling Fe (III) to receive electrons to promote the regeneration of Fe (II) for durable and efficient PMS activation during SMX degradation. Meanwhile, the N-doped defects in the carbon also provided reactive bridges that accelerated the electron transfer between FeNPs and PMS, ensuring the synergistic effects toward Fe (II)/Fe (III) cycle to some extent. The quenching tests and electron paramagnetic resonance (EPR) indicated O 2 ·− and 1 O 2 were the dominant active species during the SMX decomposition. As a result, this work provides an innovative method to construct a high-performance catalyst to active sulfate for organic contaminant degradation.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Aotian Gu,Kaiwei Chen,Xinyu Zhou,Chunhui Gong,Peng Wang,Yan Jiao,Ping Mao,Kai Chen,Jigen Lu,Yi Yang
Advanced oxidation processes based on high-valent metal species have attracted much attention due to their high reactivity and selectivity in degrading refractory organic pollutants, but the preparation of such catalysts remains a great challenge. Herein, FeCoCu-nitrogen-doped carbon (FeCoCu-NC), a trimetallic catalyst capable of producing high-valent metal species, was synthesized by direct carbonization of core–shell Metal-organic frameworks (MOFs). The rationally designed catalyst exhibited high catalytic activity in wide pH range and high resistance to common radical scavengers, anions and natural organics. The incorporation of Cu in FeCoCu-NC (TNC X ) not only enhanced the catalytic activity but also changed the activation mechanism of peroxymonosulfate (PMS) from a radical pathway to a non-radical pathway dominated by high-valent metal species. In addition, the TNC 5 /PMS system showed higher trichlorophenol (TCP) removal efficiency and PMS utilization compared to the radical-dominated FeCo-NC/PMS system and the 1 O 2 -dominated CoCu-NC/PMS system. This study provides a facile strategy to the preparation of advanced catalysts from multi-metal MOFs and is expected to provide guidance for the design of heterogeneous high-valent metal catalysts.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Can Feng,Heng Zhang,Yi Ren,Mengfan Luo,Siying Yu,Zhaokun Xiong,Yang Liu,Peng Zhou,Bo Lai
Zerovalent iron (ZVI)-based Fenton-like processes have been widely applied in degrading organic contaminants . However, the surface oxyhydroxide passivation layer produced during the preparation and oxidation of ZVI hinders its dissolution and Fe(III)/Fe(II) cycling, and restricts the generation of reactive oxygen species (ROS). In this study, copper sulfide (CuS) was found to effectively enhance the degradation of diverse organic pollutants in the ZVI/H 2 O 2 system. Moreover, the degradation performance for the actual industrial wastewater (i.e., dinitrodiazophenol wastewater) in the ZVI/H 2 O 2 system was impressively improved by 41% with CuS addition, and the COD removal efficiency could reach 97% after 2 h of treatment. Mechanism investigation revealed that the introduction of CuS accelerated the sustainable supply of Fe(II) in the ZVI/H 2 O 2 system. Specifically, Cu(I) and reductive sulfur species (i.e., S 2– , S 2 2– , S n 2– and H 2 S (aq)) from CuS directly induced efficient Fe(III)/Fe(II) cycling. The iron-copper synergistic effect between Cu(II) from CuS and ZVI expedited Fe(II) generation from ZVI dissolution and Fe(III) reduction by formed Cu(I). This study not only elucidates the promotion effects of CuS on ZVI dissolution and Fe(III)/Fe(II) cycling in ZVI-based Fenton-like processes, but also provides a sustainable and high-efficiency iron-based oxidation system for removal of organic contaminants.
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高影响因子
ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Wenjun Zhu,Xiaohua Zuo,Xiaofei Zhang,Xiangyi Deng,Deng Ding,Chunlei Wang,JunTao Yan,Xiaobo Wang,Guanghui Wang
A novel CuO–Fe 3 O 4 encapsulated in the carbon framework with abundant oxygen vacancies (CuO–Fe 3 O 4 @C) was successfully prepared by thermal conversion of Cu(OAc) 2 /Fe-metal organic framework. The as-prepared catalyst exhibited excellent peroxymonosulfate (PMS) activation performance, good recyclability and fast magnetic separation. Under optimal conditions, the added BPA (60 mg/L) could be completely removed by CuO–Fe 3 O 4 @C/PMS system within 15 min with the degradation rate constant ( k ) of 0.32 min −1 , being 10.3 and 246.2 times that in CuO/PMS (0.031min −1 ) and Fe 3 O 4 /PMS (0.0013 min −1 ) system. A deep mineralization rate of BPA (＞80%) was achieved within 60 min. The results demonstrated the synergistic effect of bimetallic clusters, oxygen vacancies and carbon framework was a key benefit for the exposure of more active sites, the electron donor capacity and the mass transfer of substrates, thereby promoting the decomposition of BPA. Capture experiments and EPR indicated that 1 O 2 was the predominant reactive oxygen species (ROSs). The degradation routes of BPA and the activation mechanism of PMS were proposed. This study offers an opportunity to develop promising MOFs-derived hybrid catalysts with tailored structures and properties for the practical application of SR-AOPs.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Bin Hu,Yongqing Yang,Wei Cao,Xixi Wang,Chuan Zhou,Yiyang Mao,Lei Ge,Ran Ran,Wei Zhou
The high cost and unfavorable catalytic performance for oxygen reduction reaction (ORR) is one of the crucial obstacles that impede widely commercialization of proton-exchange membrane fuel cells (PEMFCs). Herein, we provide a novel, mass-producible ORR catalyst made of low-loading (10 wt%) Pt nanoparticles bound to patchy nitrogen-doped carbon (PNC) with uniformly dispersed FeN 4 sites (Pt/FeN 4 -PNC). The derived catalyst exhibits significantly improved catalytic activity and stability, obtaining a promising mass activity (MA) of 0.94 A mg pt −1 at 0.9 V (vs. RHE) with a negligible decay after 30,000 cycles accelerated durability test (ADT). In the fuel-cell assessment (under H 2 -Air conditions at 80 ℃), the Pt/FeN 4 -PNC and Pt/FeN 4 -PNC-10 g (scaled-up production) achieved peak power densities of 1.13 W cm −2 and 1.14 W cm −2 , respectively, and retained 88.5 % and 88.1 % of the initial values after 30,000 voltage cycles (0.60–0.95 V). The patchy structure of PNC substrate guarantees fast electron routes and resistance to corrosion. With the FeN 4 active sites in the PNC substrate, the oxygen molecules are concurrently reduced on the surfaces of the carbon substrate and Pt nanoparticles, thereby causing the ORR reaction zone on the catalyst layer to expand.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 17
·8334-8346
·
IF 3.3
Peifu Sun,Xiao Zhang,Zhiren Guo,Xinyue Liu,Yuanming Lan,Dongxiang Zhang,Hansheng Li,Jinying Li,Helei Liu,Xiyan Xu
The excessive discharge of isothiazolinone bacteriostatic agent-containing wastewater has posed serious threats to human health and environmental safety. As 1,2-benzisothiazolin-3-one (BIT) is one of the most commonly used isothiazolinones, its effective degradation is necessary and urgent. In the current study, a NH2-MIL-53(Fe)-based adsorptive photo-Fenton-like system was constructed for efficiently adsorbing and photodegrading BIT under solar light. The equilibrium BIT adsorption capacity Qe of NH2-MIL-53(Fe) reached 1140.89 mg g−1. The adsorptive photo-Fenton-like system has achieved more than 90% removal of BIT using NH2-MIL-53(Fe) in the presence of H2O2 under solar light irradiation, and the band gap of NH2-MIL-53(Fe) was calculated by UV-Vis analysis to be 2.10 eV. The influences of pH, dosage of photocatalysts and H2O2 were also assessed. It was found that H2O2 reduced the recombination of electron–hole pairs, and the radical quenching experiments and EPR testing result confirmed that h+, ˙OH and O2˙− played a crucial role in the photocatalytic process. This study supports the application of Fe-based MOF materials for simultaneous adsorption and the solar light photocatalytic degradation of BIT.
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高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Jie Li,Hua Yin,Haoyu Luo,Yingchao Li,Xufa Rong,Zhi Dang
Polychlorinated biphenyls (PCBs) degradation by peroxymonosulfate (PMS) activation through •OH and SO 4 •– radical oxidation process was the effective technology in the last decades; however, there were few research focusing on removing PCBs by O 2 •– and 1 O 2 induced by PMS activation. In this work, 90.86% of 2,4,4-trichlorodiphenyl (PCB 28) was degraded by 0.3 g/L Fe 3 C@Fe-800 activated 0.5 mM PMS system under the synergistic action of O 2 •– and 1 O 2 . The structures of Fe 3 C@Fe-800 were identified by Scanning electron microscope (SEM), High resolution-transmission electron microscopy (HR-TEM), X-ray photoelectron spectroscopy (XPS), Brunauer-Emmett-Teller (BET), Raman spectra and Fourier transform infrared (FT-IR) spectra. Electron paramagnetic resonance (EPR) measurements and quenching tests verified that O 2 •– and 1 O 2 were the primary reactive species in Fe 3 C@Fe-800/PMS/PCB 28 ternary reaction system. Density functional theory (DFT), Linear sweep voltammetry (LSV), and chronoamperometry test revealed that electron-deficient Fe atoms on Fe 3 C were the main active sites in Fe 3 C@Fe-800 for PMS activation to generate 1 O 2 . Unlike the reported •OH and SO 4 •– mediated degradation induced by the iron-based catalyst, both O 2 •– and 1 O 2 contributed to PCB 28 degradation： nucleophilic dichlorination reaction by O 2 •- and then ring-open oxidation process by 1 O 2 . Fe 3 C@Fe-800/PMS system had excellent catalytic performance under different reaction conditions and possessed desirable inorganic salt and natural organic matter resistance. This work elucidated the important role of Fe 3 C in PMS activation to generate O 2 •- and 1 O 2 for PCB 28 decontamination by nonradical way and provided a clue to design rationally catalysts in polychlorinated biphenyl pollution remediation.
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高影响因子
Journal of Cleaner Production
·
2022
·
IF 11.072
Xinyu Zhang,Hai Nguyen Tran,Yena Liu,Chao Yang,Tingwei Zhang,Jiaqi Guo,Wenyuan Zhu,Mehraj Ahmad,Huining Xiao,Junlong Song
Magnetic biochar displays promising applications in dye wastewater treatment since it can be effectively separated by magnetism. However, the preparation of magnetic biochar with a large specific surface area is complicated and the effects of ferrous and/or ferric ions on dye adsorption are not clear enough. Herein, a facile one-pot approach of magnetic self-nitrogen-doped biochar fabrication was developed, using K 3 [Fe(C 2 O 4 ) 3 ] as an activator and iron supplier. Magnetic self-nitrogen-doped biochar could be easily separated with a magnet. Magnetic self-nitrogen-doped biochar had a large specific surface area (1034 m 2 /g) and excellent adsorption capacities for Congo red (1360 mg/g) and Rhodamine B (320 mg/g). From thermodynamics studies, Congo red adsorption on magnetic self-nitrogen-doped biochar is better than Rhodamine B. Based on the larger adsorption energies , magnetic self-nitrogen-doped biochar has a relatively stronger binding ability for Congo red than Rhodamine B, and the ferrous ions loaded on biochar surface are more beneficial for dye adsorption than ferric ones.
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Dashi Lei,Chunli Gou,Chunli Wang,Juanqin Xue,Zhongshen Zhang,Weizhen Liu,Zhang Lin,Jing Zhang
The reduced chromite ore processing residue (rCOPR) deposited in environments is susceptible to surrounding factors and causes reoccurrence of Cr(VI). However, the impact of natural sunlight on the stability of rCOPR is still unexplored. Herein, we investigated the dissolution and transformation behaviors of Cr(III)–Fe(III) hydroxide, a typical Cr(III)-containing component in rCOPR, under visible light. At acidic conditions, the release rate of Cr(III) under illumination markedly increased, up to 7 times higher than that in the dark, yet no Cr(VI) was produced. While at basic conditions, only Cr(VI) was obtained by photo-oxidation, with an oxidation rate of ∼7 times higher than that by δ-MnO2 under dark conditions at pH 10, but no reactive oxygen species was generated. X-ray absorption near-edge structure and density functional theory analyses reveal that coexisting Fe in the solid plays a critical role in the pH-dependent release and transformation of Cr(III), where photogenerated Fe(II) accelerates Cr(III) produced at acidic conditions. Meanwhile, at basic conditions, the production of intermediate Cr(III)–Fe(III) clusters by light leads to the oxidation of Cr(III) into Cr(VI) through the nonradical “metal-to-metal charge transfer” mechanism. Our study provides a new insight into Cr(VI) reoccurrence in rCOPR and helps in predicting its environmental risk in nature.
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PubMed
高影响因子
Metals
·
2022
·Vol. 12
·期 12
·2050
·
IF 2.695
Yongfeng Li,Yanzhen Liu,Shuai Chen,Xiaoming Li,Shengguo Ma
A FeNx-C-based catalyst is considered one of the most promising candidates for the highest oxygen reduction reaction (ORR) activities among nonprecious metal-based electrocatalysts. In this work, a unique catalyst of nitrogen-doped twisted macroscopic graphene tubes decorated with Fe-Nx and bamboo-like carbon nanotubes (CNT) was prepared by using twisted iron wire as a template and cyanamide as a carbon source. The microstructure and physicochemical natures of the samples were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopic (XPS), X-ray diffraction (XRD), and nitrogen adsorption/desorption measurements. Torsion can promote the dislocation of the iron wire lattice, and activate the surface Fe atoms, thus leading to the growth of bamboo-like carbon nanotubes and forming iron nitride. The product has a graphene-like macroscopic tube structure and exhibits excellent ORR activity. Such excellent ORR performance may be ascribed to the synergistic effect, including high ORR catalytic sites caused by the dislocation of the iron wire lattice, nitrogen heteroatoms doping, favorable reactant transport channels provided by macroscopic tube structure, and fast electron transfer rate induced by 3D continuous networks.Keywords:twisted iron wires;catalyst;graphene tube;electrocatalytic activity
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高影响因子
危险品化学品经营许可证（带存储）