CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Yangke Long,Yixuan Huang,Huiyi Wu,Xiaowen Shi,Ling Xiao
In this study, Fe-N-codoped carbonaceous catalysts (Fe-N-C-x) with different structures including one-dimensional carbon nanotubes (1D CNTs) and two-dimensional porous carbon sheets (2D NC) to three-dimensional carbon nanotubes/porous carbon sheets composites (3D CNTs/NC) were systematically synthesized and applied as peroxymonosulfate (PMS) activators. It was found that the Fe-N-C-x catalysts exhibited structure-dependent catalytic performance, following the order of 2D NC > 3D CNTs/NC > 1D CNTs, and also substrate-dependent degradation performance that the reaction kinetics varied greatly for different organic pollutants. Benefiting from the unique structure characteristic and high density of active sites, 2D Fe-N-C-1 showed far superior catalytic performance than the generally used carbocatalysts with negligible Fe leaching. Besides, various influential factors affecting the catalytic performance were systematically investigated. Fe-N-C-1 showed high catalytic efficiencies toward a broad spectrum of organic pollutants, and it was confirmed that both radical and non-radical degradation pathways existed during pollutants degradation. The competitive radical quenching tests and electron paramagnetic resonance measurements verified that the superoxide anion radical ( Â O 2 Â · - ) was the primary reactive oxidized species for degradation of p -chlorophenol (4-CP). The chronoamperometry analysis demonstrated that Fe-N-C-1 facilitated the electron transfer from 4-CP to PMS, resulting in the degradation of 4-CP through a non-radical mechanism. Our result not only reveals the structure-dependent PMS activation performance of transition-metal and nitrogen codoped carbocatalysts but also provides solid evidence that the defect-rich carbon materials with amorphous carbon and partial graphitic structure also favor the electron transfer mechanism.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Zhen Zhang,Jiang Wu,Bin Li,Huibin Xu,Dongjing Liu
Zeolite (ZSM-5), as a kind of carbon-free sorbent or catalyst, has been widely applied in many fields due to its big surface area, good chemical and thermal stability, and excellent adsorption performance. In this study, Mn-Fe modified ZSM-5 are synthesized via sol-gel approach and employed for elemental mercury (Hg 0 ) removal from simulated flue gas at low temperature. The results show that pure ZSM-5 shows poor mercury capture ability with Hg 0 removal efficiency of ~8.5–18.8% at 100–300 °C. Mn or Fe modification can both efficiently enhance the Hg 0 removal efficiency of the ZSM-5. The sorbent with Mn/Fe molar ratio of 1:2 exhibits the optimal mercury capture ability with the highest Hg 0 removal efficiency near 100% at temperatures of 200 and 250 °C due to the significant synergy effect between Mn 2 O 3 and Fe 2 O 3 . The presence of NO has a negligible effect on the Hg 0 removal performance of Mn/ZSM-5 and Mn1Fe2/ZSM-5, while the existence of SO 2 considerably degrades the Hg 0 capture performance of Mn/ZSM-5 owing to competing adsorption and side reactions. Fe addition can protect Mn active sites from SO 2 poisoning and thereby enhancing the SO 2 resistance of Mn/ZSM-5 to some extent.
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高影响因子
Journal of Cleaner Production
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2019
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IF 6.395
Yutao Peng,Yuqing Sun,Runze Sun,Yaoyu Zhou,Daniel C.W. Tsang,Qing Chen
Highly efficient and cost-effective adsorbents for phosphate (P) recovery are the key to control eutrophication and recover phosphorous from waste streams to enhance food production . This study assembled waste biomass (corn stalk, almond shell, and dairy manure)-derived biochars with Fe/Al (hydr)oxides through co-precipitation method. The fabricated biochar composites presented excellent performance for the adsorption of P due to good amounts of surface area, pore volume, and reactive surface hydroxyl sites. Response surface methodology (RSM) was applied to optimize the production conditions of the Fe–Al (hydr)oxides-biochars for maximizing the P removal. The effects of three key independent variables, i.e. , Fe 3+ concentration (0.2–1.0 mol L −1 ), Al 3+ concentration (0.2–1.0 mol L −1 ), and mass-to-volume ratio (0.05–0.20 g mL −1 ) on the P removal were investigated. The synthesized composites outperformed other sorbents for the P removal, suggesting the synergistic effects of Fe/Al (hydr)oxides and biochar support. These results offer valuable insights to develop high-performance biochar-based composites for green and sustainable environmental remediation.
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2019
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IF 6.393
Qian Wu,Peijin Wang,Xue Yang,Min Wei,Mao Zhou,Yuxin Pu,Mingxiao Zhang
An ultrasensitive electrochemiluminescence (ECL) biosensor was constructed by using Fe y Co 3-y [Co(CN) 6 ] 2 prussian blue analogues (Fe-Co-Co PBAs) as a novel electrochemically regenerable co-reaction accelerator for methotrexate (MTX) detection. In this work, we synthesized the core-shell Fe-Co-Co [email protected] 3 N 4 tags with luminophores and co-reaction accelerators via a facile and green method. To the best of our knowledge, it is the first time that Fe-Co-Co PBAs was used as an efficient co-reaction accelerator of the carboxylated graphene-like carbon nitride /peroxydisulfate (C-g-C 3 N 4 /S 2 O 8 2− ) ECL system for signal amplification. In view of the prominent quenching effect of MTX on the ECL response of the C-g-C 3 N 4 , the proposed ECL biosensor exhibited high sensitivity to quantify the concentration of MTX from 5 pM to 10 μM with a detection limit of 1.1 pM. Simultaneously, the biosensor has also been successfully applied to MTX detection in human serum and urine samples with reasonable recoveries. Hence, the proposed method holds a new perspective of PBAs nanomaterials in biosensing and provides a potential analysis method for the rapid detection of MTX in biological systems.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2019
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IF 3.375
Yanshu Luo,Bingqiong Tan,Xianghui Liang,Shuangfeng Wang,Xuenong Gao,Zhengguo Zhang,Yutang Fang
With an S-shaped water sorption isotherm and high vapor uptake, as one of the famous metal organic frameworks (MOFs), MIL-100(Fe) (MIL stands for Materials of Institute Lavoisier) has been considered as a very promising candidate for adsorption heat pumps. Usually, MIL-100(Fe) is synthesized by a hydrothermal method under harsh synthesis conditions, such as high temperature and vapor pressure. In this study, in the absence of any solvent, a novel facile MIL-100(Fe) synthetic strategy, which used the dry gel conversion method, was developed. X-ray diffraction (XRD) patterns showed that the new dry gel conversion technology could expediently synthesize MIL-100(Fe) with a low reaction temperature (140 °C) and high yield (85%), which is superior to the hydrothermal method with reaction temperature of 160 °C and yield of 76%. Scanning electron microscopy (SEM) images illuminated that, compared with the conventional synthesized MIL-100(Fe) in the liquid aqueous solution, the new process synthesized one in the dry gel state exhibited a smaller crystal size (about 50 nm) due to the confined growth of the crystals. The pore analysis indicated that the MIL-100(Fe) synthesized by both processes had a similar hierarchical porous structure with the mesopore and micropore; however, compared with the traditional synthesized adsorbent, the new technology synthesized one possessed a larger pore volume due to the formation of the extra mesopores from the interconnection of the nanocrystals. The static adsorption curve exhibited that the water vapor adsorption capacity of MIL-100(Fe) synthesized by the new process was a little higher than the one synthesized by the traditional hydrothermal method. Moreover, it had a smaller desorption activation energy and better cycle stability.
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WATER AIR AND SOIL POLLUTION
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2019
·Vol. 230
·期 11
·1-11
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IF 1.774
Zuo Wenda,Wang Xu,Zhang Dongyan,Sun Ying,Xu Jingbo,Guo Ping
A composite catalyst of MCM-41-supported graphene oxide (GO) and iron (GO-MCM-Fe) was synthesized with solvothermal method and shown for the first time to be an efficient peroxydisulfate (PDS) activator to remove levofloxacin hydrochloride (LVF) in water. A total of 97.10% of LVF were removed within 10 min in the GO-MCM-Fe/PDS system. And the apparent rate constant of the GO-MCM-/Fe/PDS system was 11.78 and 1.35 times that of the GO-MCM-Fe system and MCM-Fe/PDS system, respectively. GO-MCM-Fe catalyst achieved lower iron ions (0.27%) than MCM-Fe (0.89%) at 60 min. Although GO could strengthen stability of the catalyst; this effect was negatively related with GO dosages in this work. And 5%wt Fe and 30 mL GO solution were chosen as the optimal condition for catalyst synthesis. The GO-MCM-Fe catalyst could be reused and the LVF removal ratio reached about 86% even after the fifth run. Both SO 4 − · and ·OH played the important roles and the latter was a dominant role. Additionally, in the process of GO-MCM-Fe activating PDS, there existed a redox interaction between the C=C of GO and Fe 3+ , in which the C=C of GO was oxidized into C=O; meanwhile, Fe 3+ was reduced to Fe 2+ which further activated PDS to generate radicals. This study provides a promising catalyst in effectively activating PDS to remove organic pollutants in water.
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CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Tao Pan,Yu Wang,Xin Yang,Xiong-fei Huang,Rong-liang Qiu
Fe(II)-catalyzed peroxymonosulfate (PMS) activation process was able to degrade persistent organic pollutants, such as polybrominated diphenyl ethers (PBDEs), but the slow transformation rate from the generated Fe(III) to Fe(II) restricted the efficiency of this process. In this study, we found that the addition of small quantities of gallic acid (GA), a model compound of natural polyphenols, in the Fe(III)/PMS process (namely GA/Fe(III)/PMS process) could exert a long-term influence on Fe(II) recycle and accelerated the degradation of 2,2′,4,4′-tetrabromodiphenyl ether (BDE47) over 72 h. Under conditions of 20.3 µM GA, 13.6 µM Fe(III) and 400 µM PMS, the degradation efficiency of BDE47 reached 85%, which was 9.4 times higher than that in the Fe(III)/PMS process. The degradation kinetics can be divided into an initial “fast stage” (k obs1 = 0.298 h −1 ) and a second “slow stage” (k obs2 = 0.021 h −1 ). Aromatic radicals such as hydroxycyclohexadienyl radical (poly-HCD ) produced by the attack of SO 4 − /HO on GA was proposed to be responsible for Fe(II) recycle in the first stage, while ring-opened products following SO 4 − /HO attack of GA-quinone mainly initiated Fe(III) reduction in the second stage. Owing to the multiple Fe(III) reduction pathways, PMS would be continuously activated by Fe(II) to form SO 4 − and HO , which were the dominant reactive species for BDE47 degradation. Finally, natural polyphenols extracted from green tea were proven effective in enhancing BDE47 degradation in Fe(III)/PMS process. This study not only provides a new way to propagate Fe(II)-activated persulfate chain reactions for the degradation of refractory organic contaminants, like PBDEs, but also sheds new insight into the reactivity of organic byproducts toward Fe in PMS-based oxidation system.
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CLAYS AND CLAY MINERALS
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2019
·Vol. 67
·期 4
·325-333
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IF 1.835
Guo Yu-Hua,Pan Guo-Xiang,Xu Min-Hong,Wu Tao,Wang Yong-Ya
Adsorption desulfurization is a potential new method for deep desulfurization of fuel oil. The development of adsorbents with high adsorption capacity and selectivity is the core of deep adsorption desulfurization. The adsorption behavior of thiophene in MCM-41 mesoporous materials modified by various metal ions was studied in order to understand the adsorption desulfurization process of molecular sieves. The Fe-, Co-, and Zn-modified MCM-41 materials were prepared using a one-step in situ hydrothermal synthesis method. The modified MCM-41 molecular sieves maintained the mesoporous structure, and the metal ions had specific dispersion on the surface of the molecular sieves. Adsorption of thiophene on the surfaces of molecular sieves had both physical and chemical characteristics. The adsorption desulfurization performance of the modified molecular sieve was superior to that of the pure silica molecular sieve. In the simulated gasoline with sulfur content of 220 μg/g, when the amount of adsorbent used was 100 mg, the adsorptive desulfurization performance tended to be in equilibrium, and the optimum adsorption temperature was 30°C. Fe-MCM-41 and MCM-41 molecular sieves reached adsorption equilibrium after ~60 min, but the desulfurization rate of Co-MCM-41 and Zn-MCM-41 still increased slightly. The kinetic simulation results indicated that the pseudo-second-order kinetics adsorption model described well the adsorption process of thiophene on molecular sieves. The molecular sieve Fe-MCM-41 had the best desulfurization performance with an equilibrium adsorption capacity of 14.02 mg/g and the desulfurization rate was ~90%.
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ChemSusChem
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2019
·Vol. 13
·期 4
·811-818
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IF 7.804
Chunlei Peng,Nian Ran,Gang Wan,Wanpeng Zhao,Zhaoyu Kuang,Zheng Lu,Chengjun Sun,Jianjun Liu,Lianzhou Wang,Hangrong Chen
Graphical All good in theory and practice ! Theoretical calculations are performed to prove the higher activity of edge Fe sites. The active Fe sites are induced on nickel–iron layered double hydroxide through a facile acid treatment owing to the difference in their solubility product constant. The activity tests show that the samples containing more edge Fe sites exhibit higher oxygen evolution activity. Nickel–iron layered double hydroxide (NiFe LDH) is a promising oxygen evolution reaction (OER) electrocatalyst under alkaline conditions. Much research has been performed to understand the structure–activity relationship of NiFe LDH under OER conditions. However, the specific role of the Fe species remains unclear and under debate. Herein, based on DFT calculations, it was discovered that the edge Fe sites show higher activity towards OER than either the edge Ni sites or lattice sites. Therefore, a facile acid-etching method was proposed to controllably induce the formation of edge Fe sites in NiFe LDH, and the obtained sample exhibited higher OER activity. X-ray absorption near edge structure and extended X-ray absorption fine structure analyses further revealed that the interaction of the edge Fe species with Ni is believed to contribute to the enhancement of the OER performance. This work provides a new understanding of the structure–activity relationship in NiFe LDH and offers a facile method for the design of efficient electrocatalysts in an alkaline environment.
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PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2019
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IF 5.589
Jaehyeong Park,Ganesh Dattatraya Saratale,Si-Kyung Cho,Sungjun Bae
A novel Cu catalyst was developed using water-washed coal fly ash (WFA) as a support material for catalytic reduction of p -nitrophenol ( p -NP) in the presence of NaBH 4 . Cu/WFA showed ~ × 10 5 times higher estimated rate constant k obs-p-NP /C Cu (L min −1 g Cu −1 ) compared with Cu/SiO 2 , Cu/Al 2 O 3 , and other Cu catalysts previously reported. Surprisingly, we obtained a significant lower price value (Price’/K) (0.027–0.068 USD/L min −1 ) for Cu/WFA in comparison with other Cu catalysts and precious metallic catalysts (Pd, Au, Ag, and Pt). Various surface analyses and additional experiments using Fe/SiO 2 , Cu/Fe 2 O 3 /SiO 2 , and Cu/HCl-treated WFA demonstrated that Cu(0) nanoparticles were well loaded on the surface of WFA, where Fe elements were abundant, resulting in a dramatic enhancement of the Cu/WFA catalytic activity . Particularly, X-ray photoelectron spectroscopy revealed the abundance of Cu(0)/Fe(III) and Cu(0)/Fe(II) in the WFA surface. This indicates that Cu(0) was the main driving force for the activation of H ad molecule, and that the reduction of Fe(III) to Fe(II) by NaBH 4 can accelerate the reduction of Cu(II) to Cu(0). Recycling and phytotoxicity tests showed that Cu/WFA can be applied as a reusable catalyst with low environmental impact, revealing the remarkable potential of non-precious metal/WFA catalyst in the field of environmental remediation.
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PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2019
·Vol. 29
·期 36
·1904056
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IF 15.621
Jing Zhu,Chengchao Chu,Dongsheng Li,Xin Pang,Huili Zheng,Junqing Wang,Yesi Shi,Yang Zhang,Yi Cheng,En Ren,Jingliang Cheng,Xiaoyuan Chen,Gang Liu
To address the urgent need for effective sonodynamic therapy (SDT), a facile and efficient strategy is developed for fabricating a new class of sonotheranostics. Herein, a Fe(III)-porphyrin nano-sonosensitizer is prepared by a one-step coordination synthesis, and then anchored with Bis(DPA-Zn)-RGD and manganese superoxide dismutase (SOD2) siRNA. Benefiting from the delicate interactions of the Fe(III)-coordinated nanoformulations, a highly potent sono/gene combinational therapy guided by fluorescence/magnetic resonance imaging is achieved. Importantly, this sonotheranostics significantly enhances the SDT effect of porphyrin through the cancer-targeted delivery capability and enhanced reactive oxygen species production via triple-regulated approaches, including down-regulation of SOD2, depletion of glutathione, and generation of Fenton reaction. This work opens up new perspectives for developing versatile sonotheranostics to overcome the clinical challenges of SDT.
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CARBON
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2019
·
IF 7.466
Yu-Jiao Zhang,Jin Qu,Qiu-Yu Ji,Ting-Ting Zhang,Wei Chang,Shu-Meng Hao,Zhong-Zhen Yu
The loss and sluggish kinetics of intermediate polysulfides in electrochemical processes seriously reduce electrochemical activity of sulfur in lithium-sulfur batteries (LSBs). Herein, we design and synthesize freestanding graphitized carbon interlayers decorated with Fe/Fe 3 C nanocatalysts by thermal treatment of cellulose paper with adsorbed ferric nitrate at 1000 °C, during which the freestanding carbon network derives from the cellulose paper while the Fe results from the reduction of Fe 3+ with a carbothermal reduction process; simultaneously, the in situ formed Fe boosts graphitization of carbon to enhance electrical conductivity of the interlayer, and the carbon network effectively helps confine and accommodate Fe/Fe 3 C nanoparticles . Therefore, the well dispersed Fe/Fe 3 C nanoparticles catalytically accelerate electrochemical conversion of polysulfides, while the enhanced conductive network of carbon benefits the electron transfer during the electrocatalytic process. The cell with an optimal carbon/Fe/Fe 3 C interlayer delivers excellent cyclability and rate performances. At current densities of 0.2C and 2C, the specific capacities are close to 1000 and 735 mA h g −1 , respectively. Even after 200 cycles at 1C, the reversible specific capacity is still 772 mA h g −1 . Such a synergistic catalytic interlayer with an enhanced conversion kinetic towards polysulfides provides a new approach for improving electrochemical performances of LSBs.
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