CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Jing Wu,Mei Lin,Xiulan Weng,Gary Owens,Zuliang Chen
Emerging contaminants such as Mitoxantrone (MTX) are a major environmental concern because they have potential genotoxicity and mutagenesis to both aquatic organisms and humans. In this study, a pre-adsorption/Fenton-like oxidation system was developed which used a reduced graphene oxide/iron nanoparticles hybrid (rGO/Fe NPs) as both the adsorbent and the Fenton catalyst to remove MTX from solution. While the addition of H 2 O 2 alone removed only 11.3% of MTX, the rGO/Fe NPs/H 2 O 2 system was significantly more efficient removing 99.8% of MTX in the same period. This indicated that rGO/Fe NPs had excellent catalytic activity even at pH 7. This efficient removal was attributed to significant production of ·OH mainly by heterogeneous catalysis but supplemented by a homogeneous Fenton reaction, where ·OH had a higher affinity for MTX than SO 4 − ·. The sequential Fenton-like oxidation process best fits a pseudo-second-order kinetic model (R 2 ≥ 0.974). Characterizations of rGO/Fe NPs before and after the reaction, together with the identification of specific MTX degradation products , allowed possible degradation pathways to be proposed together with insights into the underlying mechanisms of MTX degradation when using rGO/Fe NPs in a pre-adsorption/Fenton-like oxidation system. Finally, the rGO/Fe NPs developed was successfully applied for the removal of MTX from spiked wastewater with 93.6% removal efficiency, which indicated that the proposed system had significant potential for wastewater treatment applications.
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NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 6
·3120-3127
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IF 3.591
Yixuan Huang,Liyan Xie,Kangji Zhuo,Hao Zhou,Yanhui Zhang
MIL-101(Fe)-based composite materials and their application for the generation of H2 by the catalytic reduction of nitro organics are reported in this study. NaBH4 and water contribute hydrogen for the catalytic reduction of nitro organics, but the possibility of nitro organics as a potential hydrogen source is often overlooked due to the simplicity of the reaction. However, experiments have revealed that the reaction process is accompanied by the production of H2, which is affected by the concentration of nitro organics. Moreover, the reaction is more conducive to the generation of H2 compared to NaBH4 hydrolysis under the same conditions. Unlike specially catalyzing the expensive NaBH4 hydrolysis, hydrogen is a by-product of the reduction of pollutants by inexpensive catalysts (NaBH4 acted as an electron donor for the catalyst). Accordingly, the reaction mechanism of p-nitrophenol hydride reduction was optimized. This work provides a new perspective on the application of this reaction.
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Scientific Reports
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2020
·Vol. 10
·期 1
·1-11
·
IF 3.998
Dong Zijun,Chen Guanhan,Li Mu,Sun Feiyun,Jiang Chengchun,Bharti Bandna
Iodinated contrast media (ICM), which was widely used in medical imaging and was difficult to remove by conventional wastewater treatment methods, attained much attention due to its potential environmental impacts. Herein, iopamidol (IPM), one typical compound of ICM, was found to be rapidly degraded by ferrous activated persulfate oxidation (Fe(II)/PS) as compared with PS or Fe(II) alone. With a persulfate concentration of 1 mmol L −1 , n(Fe(II))/n(PS) of 1:10, and a pH of 3.0, 78% IPM was degraded within 60 min, with a degradation rate of 0.1266 min −1 . It was demonstrated that IPM degradation and deiodination were favored by a high temperature, while affected positively by acidic and neutral conditions. Radical quenching experiments and Electron Paramagnetic Resonace (EPR) spectra showed that the combined effects of SO 4 − · and · OH contributed dominantly to degrade IPM, while the · OH played an essential role during the degradation reaction. Through the Discrete Fourier Transform quantum chemical calculation, the possible reaction pathways for the oxidation of IPM by · OH are as follows: IPM-TP651-TP667-TP541-TP557, IPM-TP651-TP525-TP557, IPM-TP705-TP631-TP661, and IPM-TP705-TP735. The obtained results showed that IPM could be degraded effectively by Fe(II)/PS system, giving a promising technique for IPM removal from water.
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 32
·16265-16270
·
IF 11.301
Wenjuan Han,Ming Lu,Junnan Chen,Haojie Li,Haibo Li,Bingsen Zhang,Wei Zhang,Weitao Zheng
EMIm+, as a substitute for Li+, can solve the initial problems that accompany lithiation/delithiation processes on an anode. However, the larger size of EMIm+ limits the options when it comes to electrode materials. Herein, a multilayered Ti3C2Tx MXene was electrochemically pre-intercalated with Fe ions to achieve EMIm+ hosting abilities. As a result, a pre-intercalated MXene electrode exhibited enhanced EMIm+ transport and storage capabilities. When integrated with an EMIm+[PF6]− ionic liquid electrolyte, the assembled DIB provides an energy density of 76 W h kg−1 at a power density of 360 W kg−1, and 94.3% of the energy density is retained after 50 cycles. Compared with a pristine example, the Fe pre-intercalated Ti3C2Tx MXene showed a significant increase in electrochemical performance. Employing this approach to optimize layered materials may open up a new route for accurately tuning intercalated materials.
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Science Advances
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2020
·Vol. 6
·期 18
·
IF 13.117
Chen-Cheng Xue,Meng-Huan Li,Yang Zhao,Jun Zhou,Yan Hu,Kai-Yong Cai,Yanli Zhao,Shu-Hong Yu,Zhong Luo
The rapid development of treatment resistance in tumors poses a technological bottleneck in clinical oncology. Ferroptosis is a form of regulated cell death with clinical translational potential, but the efficacy of ferroptosis-inducing agents is susceptible to many endogenous factors when administered alone, for which some cooperating mechanisms are urgently required. Here, we report an amorphous calcium carbonate (ACC)–based nanoassembly for tumor-targeted ferroptosis therapy, in which the totally degradable ACC substrate could synergize with the therapeutic interaction between doxorubicin (DOX) and Fe2+. The nanoplatform was simultaneously modified by dendrimers with metalloproteinase-2 (MMP-2)–sheddable PEG or targeting ligands, which offers the functional balance between circulation longevity and tumor-specific uptake. The therapeutic cargo could be released intracellularly in a self-regulated manner through acidity-triggered degradation of ACC, where DOX could amplify the ferroptosis effects of Fe2+ by producing H2O2. This nanoformulation has demonstrated potent ferroptosis efficacy and may offer clinical promise.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2020
·
IF 3.807
Xiaoying Zhai,Weiguo Lin,Jinkai Liu,Xu Chen,Junfeng Yong,Wensheng Yang
The development of earth-abundant electrocatalysts to replace noble metal for oxygen reduction reaction (ORR) has attracts tremendous interest. In this work, Fe, N-codoped porous carbon-embedded Fe 3 C nanoparticles (Fe 3 C/Fe, N-PCR) is fabricated from petroleum vacuum residue via a simple template-assisted and subsequent doping-assisted calcination method. The unique hybrid material shows great features: abundant active sites including pyridinic N, Fe N, and Fe 3 C nanoparticles, a relatively large surface area (509.3 m 2 g − 1 ) and 3D interconnected hierarchical porous structure. The Fe 3 C/Fe, N-PCR as an electrocatalyst exhibits remarkable ORR catalytic activity in alkaline medium, with a high onset potential of 1.02 V and half-wave potential of 0.86 V, which surpass commercial Pt/C (20 wt%) by ca. 30 and 20 mV, respectively. Moreover, Fe 3 C/Fe, N-PCR has outstanding long-term stability and tolerance to methanol poisoning, outperforming Pt/C. Combining with the exciting performance, abundant and cheap raw material, and facile synthetic method, Fe 3 C/Fe, N-PCR catalyst has promising future in ORR. This study also provides a new approach for high value utilization of petroleum vacuum residue.
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Scientific Reports
·
2020
·Vol. 10
·期 1
·1-9
·
IF 3.998
Zhang Lei,Weng Yi-jin,Liu Xiao,Gu Wen,Zhang Xia,Han Lei
Surface Enhanced Raman Scattering (SERS) has been widely applied in many research fields such as biological detection and chemical analysis. However, for the common Au nanoparticles, it’s too hard to guarante the three aspects: the great enhanced effect, the controllable aggregation and the uniformity of nanoparticles, the environmental friendliness and biocompatibility of nanoparticles. In this paper, phytate acid (IP6)-coated Au nanoparticles (IP6@Au NPs) are more stable and have a higher enhancement factor than Au nanoparticles. In order to achieve the uniformity of the spherical IP6-coated@Au nanoparticles (IP6@Au NPs), IP6 was used as a soft template. In the presence of IP6, IP6@Ag nanoparticles were first synthesized by reducing AgNO 3 with trisodium citrate, then IP6@Au NPs were obtained by reducing HAuCl 4 with Ag nanoparticles. The IP6@Au NPs exhibit excellent Raman signal enhancement by using p-aminothiophenol (4-ATP) as the probe molecules. The effects of Fe 3+ on the performance of IP6@Au NPs SERS substrates were also studied. The results show that SERS has the best enhancement effect when adding proper amount of Fe 3+ (0.56 PPM), and the limit of detection was 10 −7 M 4-ATP.
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Arabian Journal of Chemistry
·
2020
·
IF 4.762
Zijun Dong,Feng Wang,Xiulan Song,Miao Zhang,Chengchun Jiang,Feiyun Sun,Mu Li
Iodoform (CHI 3 ) is one of the disinfection by-products (DBPs) that is formed in the pre-oxidation and disinfection processes of drinking water treatment. In this study, Fe(II)-activated persulfate oxidation (Fe 2+ /PS) was employed to degrade iodoform, the effects of initial reactants concentration, reaction parameters, kinetics model were investigated, and the underlying mechanisms of CHI 3 degradation in Fe 2+ /PS oxidation process was unveiled. The results showed that the mole ratio Fe 2+ /PS of 1:5, initial PS concentration of 15 μmmol/L, and pH of 3.0 were identified as the optimum operating parameters. In addition, a relatively higher temperature could enhance CHI 3 removal and deiodination. The kinetic model has two different reaction steps: a fast one during the first ten minutes of reaction; then followed by a much slower one. Suppression of the reaction by TBA and MeOH showed that the combined effects of SO 4 − · and ·OH contributed to the degradation of CHI 3 , but ·OH played a dominant role. The degradation pathways and the products of total liberated iodine species demonstrate that the applicability of the Fe 2+ /PS oxidation process for CHI 3 degradation. These results indicated that the Fe 2+ /PS oxidation process is an effective advanced oxidation process for CHI 3 removal in water treatment.
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 8
·4369-4375
·
IF 11.301
Lulu Chen,Yelong Zhang,Lile Dong,Wenxiu Yang,Xiangjian Liu,Ling Long,Changyu Liu,Shaojun Dong,Jianbo Jia
Rational design of isolated metal atom doped carbon catalysts is essential for revealing the essence of high activity for the oxygen reduction reaction (ORR), which can promote the development of robust catalysts for clean energy conversion devices. Herein, we report a simple one-step strategy to prepare Fe and Co atomically supported on N-doped nanocarbon (FeCo-IA/NC) from metal–organic frameworks with excellent ORR activity. The isolated Fe–N4 and Co–N4 sites are characterized by atomic-resolution aberration-corrected scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy. The electrochemical results and density functional theory calculations indicate that the synergetic effect between Fe–N4 and Co–N4 accounts for the enhanced ORR activity. Benefiting from the large BET surface area, microporous feature, and high content (85%) of pyridinic and graphitic N, the well-designed catalyst exhibits better ORR activity (half-wave potential of 0.88 V) and Zn–air battery performances (higher open circuit potential and power density) than commercial Pt/C. This work may lay a foundation for further exploring efficient non-precious metal-based catalysts for the ORR and developing clean energy conversion devices.
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ANALYTICA CHIMICA ACTA
·
2020
·
IF 5.977
Xiaobin Zhou,Mengke Wang,Junyang Chen,Xiaolei Xie,Xingguang Su
Single atom nanozymes are the artificial enzymes with enzyme-like activity, which have attracted a great deal attention in recent years due to their unique merits such as remarkable stability, excellent atom utilization and low cost. Herein, a convenient and sensitive colorimetric strategy was developed for the sensing of galactose based on Fe–N–C single-atom nanozyme (Fe-SAzyme). The Fe-SAzyme was prepared through “isolation-pyrolysis” method that exhibited intrinsic peroxidase mimicking activity, which can quickly catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to produce blue-colored oxTMB in the presence of hydrogen peroxide (H 2 O 2 ). Galactose can be oxidized by galactose oxidase (Gal Ox) to generate H 2 O 2 , and Fe-SAzyme can be utilized for quantitative colorimetric detection of galactose. A good linearity between absorbance and the galactose concentration in the range of 50–500 μM was obtained with a detection limit of (LOD) 10 μM. The Fe-SAzyme based colorimetric strategy offered a rapid, convenient and economic way for galactose quantification detection, which could be used as an alternative method for galactosemia diagnosis.
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ACS Omega
·
2020
·
IF 2.87
Tianzhao Hu,Jiafu Chen,Xiaoqing Lu,Jing Chen,Zhimin Chen,Jianwei Fu,Yong Chen
Graphene sheets have a vast number of potential applications due to their excellent properties. However, poor quality and harsh preparation conditions restrict their application. Here, few-layer graphene (FLG) sheet powder with high quality has been synthesized from waste expanded polystyrene (EPS) at low temperature by dense Fe cluster catalysis. The micron-sized FLG sheets comprising about three layers show high crystallinity and good electrical conductivity that are comparable to those of the shear-exfoliated graphene nanoplatelets. More than 70% carbon yield of FLG sheets from cheap EPS and their safe, controllable synthesis conditions make it easy to expand production. The catalytic formation mechanism of FLG sheets is studied.
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ACS Biomaterials Science & Engineering
·
2020
·
IF 4.152
Guangchao Xie,Liang Zhang,Jinbin Pan,Xuejun Zhang,Shao-Kai Sun
Photothermal agents with good biocompatibility, high tumor accumulation efficiency, large-scale production ability, and low cost are crucial for potential photothermal treatment in clinic. Herein, we proposed a green and highly efficient strategy to fabricate a kilogram-scale alginate-Ca2+-Fe powder hydrogel (ALG-Ca2+-Fe) by turning commercial Fe powder into hydrogel for enhanced photothermal therapy. The ALG-Ca2+-Fe was formed by simply dispersing commercial Fe powder into the preformed alginate-Ca2+ hydrogel in a green and energy-/time-saving way. The hydrogel exhibited the advantages of ultrahigh loading capacity of Fe powder (>100 mg mL–1), excellent large-scale production capacity (>1 kg in lab synthesis), low cost (<1.7 $/kg), and good injectability. More importantly, large size and hydrophobicity endowed Fe powder with excellent tumor retention effect and minimal diffusion to surrounding tissues, greatly benefiting improving treatment efficiency and reducing side effects. In vivo and in vitro studies both proved that the large-scale produced ALG-Ca2+-Fe can be used for highly efficient and biosafe tumor treatment in vivo by simple noninvasive injection. The developed ALG-Ca2+-Fe with multiple superiors opens up a novel green way to develop efficient and safe photothermal therapeutic agents with great clinic transformation potential.
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