APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Zhenyu Yan,Wenyu Gao,Chenkai Zhong,Qiangqiang Jiao,Shujie Tian,Jia Liu
Ammonia (NH 3 ) plays an important role in agricultural production and is also an ideal zero-carbon energy source in sustainable hydrogen economy. Electrocatalytic nitrate (NO 3 - ) reduction reaction can simultaneously consume nitrogen pollutants in water during the synthesis of NH 3 , which is the most promising and gentle alternative process to the Haber-Bosch. However, due to the interference of hydrogen evolution reaction and high overpotential, the development of efficient directional ammonia conversion catalysts has become the key. In this study, Mo-Fe 2 O 3 material were fabricated by crystal face engineering and orbital manipulation strategies. The (001) face of α-Fe 2 O 3 with the best electrochemical performance was exposed by thermodynamic control, and the in-situ substitution of Mo single atoms for near-surface Fe atoms was further used to achieve excellent ammonia synthesis activity. NH 3 yield of 493.67 μg/h/mg cat and Faraday efficiency of 95.0% were achieved at -0.5 V vs. RHE (pH=7, 0.1 M PBS+500 ppm NO 3 - ). The mechanistic analysis showed that the highly electronegative Mo atoms induced strong interaction by Fe-O-Mo bond, which prompted Fe(III) to preferentially fill the lower t2g orbital and form a low-spin state. The weaker anti-bonding state enhances the interaction between Fe(III) and the coordinating O atoms in NO 3 - , thereby strengthening electron transfer. In summary, the targeted regulation of the crystal facet and electronic orbitals of catalysts presents a promising strategy for enhancing the conversion of NO 3 - to NH 3 .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Rong Li,Yiziqi Lu,Meiqian Lu,Yue Liu,Guodong Zhang,Qiuling Ma,Jian Zhou,Tiecheng Wang
Iodinated X-ray contrast media, as a frequently used medical diagnosis in the imaging of internal organs, soft tissues, and blood vessels, are widely encountered in water environments because of their non-metabolic ability. Herein, a series of co-precipitates (DBC-FeO x ) of dissolved black carbon (DBC) and FeO x were successfully synthesized. The chelation of Fe species with COO – groups in DBC enhanced the excellent electron transfer capability and persulfate (PS) activation performance of the resulting DBC-FeO x , thus boosting iopamidol (IPM) degradation. The IPM removal rate constant in the DBC-FeO x /PS was 35 times and 4.6 times higher than those observed in the DBC/PS and FeO x /PS systems, respectively. There existed an appropriate C/Fe molar ratio in the DBC-FeO x co-precipitates for PS activation, and the IPM degradation was driven by both radical and non-radical pathways. Fe sites were the primary active sites in DBC-FeO x for PS activation, and C=O groups played an important role in accelerating the Fe(III)/Fe(II) cycle by promoting rapid electron transfer, thereby enhancing radical oxidation pathways. Concurrently, DBC-FeO x acted as an electron shuttle to promote the electron transfer from IPM to PS, creating non-radical pathways for IPM removal. IPM degradation processes involved amide hydrolysis oxidation, hydrogen extraction, and deiodination. The typical iodine species HOI was also converted to non-toxic IO 3 - after IPM decomposition, thus reducing potential risks.
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Nanoscale Advances
·
2020
·Vol. 2
·期 4
·1483-1492
·
IF 0
Honggang Yin,Die Gao,Yan Qiu,Gaoyi Yi,Jun Li,Yingying Dong,Kailian Zhang,Zhining Xia,Qifeng Fu
In recent years, photoluminescent (PL) carbon dots (CDs) have attracted enormous attention because of their many fascinating properties. However, the traditional synthesis routes of PL CDs usually suffer from relatively low quantum yields (QYs) and require complicated operation processes as well as lots of externally supplied energy. Herein, we report a room temperature, green, ultrafast and energy-efficient route for large scale synthesis of highly PL N, S-codoped CDs without any external energy supply. The N, S-codoped CDs are prepared through a novel carbon source self-heating strategy, using the sole precursor tetraethylenepentamine (TEPA) simultaneously as the carbon, nitrogen and heat source, triggered by the heat initiator sodium persulfate (Na2S2O8). The large amount of heat released from Na2S2O8-triggered oxidation of TEPA could effectively promote the spontaneous polymerization and carbonization of TEPA precursors themselves as well as the in situ co-doping of sulfur, which had marked synergistic effects on the fluorescence enhancement of CDs, eventually leading to the high-yield (58.0%) preparation of highly fluorescent N, S-codoped CDs (QY 26.4%) at room temperature within 2 min. Moreover, the fluorescence of N, S-codoped CDs could be selectively quenched by Fe3+ ions in the presence of EDTA, in an ultra-wide range of 0.2–600 μM, with a detection limit of 0.10 μM. Ultimately, the fluorescent nanoprobe was successfully used for the quantitative detection of Fe3+ in human serum samples, indicating its great potential for sensing and biomedical applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Haidong Li,Han Song,Yuankun Yang,Haitao Wang,Beibei Fan,Juncheng Zheng,Weiguo Tu,Xuemei Luo,Shu Chen
Efficient and economical reduction and elimination of co-pollution of vanadium (V) and chromium (Cr) from water sources is a major challenge. In this study, sulphate green rust (GR SO4 ) was successfully prepared by co-precipitation method and used for the removal of V(V) and Cr(VI). The findings from batch adsorption experiments indicated that the adsorption capacity of GR SO4 for V(V) and Cr(VI) individually was 30.66 mg⋅g −1 and 39.48 mg⋅g −1 , respectively, with equilibrium reached in 25 min and 10 min. Intriguingly, in a binary system with both V(V) and Cr(VI) present, the time to reach adsorption equilibrium for V(V) removal by GR SO4 was 30 % shorter comparison to the single system under identical conditions. By analyzing the surface characteristics, crystal structure and elemental valence changes of GR SO4 minerals before and after the reaction, it can be obtained that: i) Direct adsorption mainly drives the removal of V(V) by GR SO4 , whereas the removal of Cr(VI) is preceded by reduction and followed by adsorption. ii) In a binary coexistence system, the formation of Fe(III)-Cr(III) oxide (GR-Cr(III)) during the removal of Cr(VI) by GR SO4 formed during the removal of Cr(VI) by GR SO4 creates additional adsorption sites for V(V), which shortens the equilibrium time of the V(V) removal reaction by GR SO4 and reduces the amount of V(V) leached. These findings are of great practical significance for understanding the mechanism and practical application of GR SO4 in the synergistic removal of V(V) and Cr(VI) heavy metals and provide valuable insights into their geophysical-chemical cycling.
研究领域:
环境科学
·
化学
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BIORESOURCE TECHNOLOGY
·
2012
·
IF 4.98
Xiaoyan Wang,Zuoming Zhou,Guohua Jing
Magnetic poly(styrene–glycidyl methacrylate) porous microspheres (MPPM) with high magnetic contents were prepared by surfactant reverse micelles and emulsion polymerization of monomers, in which the well-dispersed Fe 3 O 4 nanoparticles were modified by polyethylene glycol (PEG) and oleic acid (OA) respectively. The characterizations showed that both of the OA–MPPM and the PEG–MPPM were ferromagnetic, however, the OA–MPPM was used to immobilize the bacteria for more advantages. Therefore, the effects of monomer ratio, surfactant, crosslinker and amount of Fe 3 O 4 on the structure, morphology and magnetic contents of the OA–MPPM were investigated. Then, the OA–MPPM was utilized to immobilize Klebsiella sp. FD-3, an iron-reducing bacterium for Fe(III)EDTA reduction applied in NO x removal. Compared with free bacteria, the immobilized FD-3 showed a better tolerance to the unbeneficial pH and temperature conditions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Qiangshun Wu,Hanpei Yang,Li Kang,Zhao Gao,Feifan Ren
In this work, a series of Fe-based metal-organic frameworks (Fe-MOFs) were synthesized and served as Fenton-like catalysts for tetracycline hydrochloride (TC–HCl) degradation. Herein, for the first time, we have demonstrated that visible light can accelerate Fe(II)/Fe(III) cycle in the photo-Fenton system based on iron-oxo (Fe-O) clusters in frameworks. Among these Fe-MOFs, MIL-101 possessed the highest activity mainly ascribed to its largest specific surface area and pore volume, and the most coordinatively unsaturated iron sites. The synergistic effect in the MIL-101/H 2 O 2 /visible light system was derived from the efficient separation and migration of photogenerated carriers. Due to the function of solid acid catalysts, MIL-101 extended effective pH range up to 10.2 and exhibited good reusability and stability. Hydroxyl radicals generated from H 2 O 2 coordinated at iron active sites were determined as the main reactive oxidative species and acceleration of Fe(II)/Fe(III) cycle was responsible for highly effective degradation of TC–HCl.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Jiajie Xu,Zhiyu Liu,Tenghui Jin,Xusheng Yang,Huihuang Chen,J. Paul Chen
Fenton reaction has been widely used for efficient treatment of organic wastewater. However, its applications are limited by such key factors as pH < 3. In this study, we developed, tested, and optimized an alginate/C 3 N 4 porphyrin bead (C 3 N 4 por-SA) as a recyclable photocatalyst in a photocatalysis-self-Fenton process to overcome these limitations. Porphyrin-modified C 3 N 4 (C 3 N 4 por) was used as the H 2 O 2 donator, while Fe(III) nodes served as the Fenton reagent . The as-prepared floating alginate/C 3 N 4 por bead utilized the light source as a driving force for the catalysis. Under visible light irradiation for 6 h, the model pollutant atrazine was degraded by 70.96 % by the optimized photocatalyst (named as C 3 N 4 por-SA-Fe1Ca5), demonstrating better photocatalytic performance than alginate/C 3 N 4 beads. This improvement was attributed to the higher H 2 O 2 yield from C 3 N 4 por. The alginate/C 3 N 4 por bead showed better photocatalytic activity even after several consecutive cycles and could easily be recovered for reuse. Furthermore, Fe(III)/Ca(II) bimetallic alginate bead exhibited better photocatalytic activity and a higher content of •OH radicals than the Ca(II) monometallic alginate beads, due to the ability of Fe(III) nodes to serve as a Fenton reagent. The influences of light sources, and commonly existing matters (namely SO 4 2− , Cl − , CO 3 2− , NO 3 − , and humic acid) were investigated. Moreover, the alginate/C 3 N 4 por bead demonstrated good photocatalytic performance in a simulated natural environment without the addition of extra H 2 O 2 , with an atrazine removal percentage of up to 96.3 % after 3-h irradiation. These findings indicated the great potential of alginate/C 3 N 4 por bead in practical applications.
研究领域:
环境科学
·
化学工程
·
材料科学
·
水处理
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CHEMOSPHERE
·
2025
·
IF 8.1
Qianying Zong,Xiaofei Niu,Xin Cheng,Yifan Liu,Cong Liu,Tingyue Shi,Jiapeng Liu,Xiaohong Yang,Wentao Wang,Zikuan Guo,Fengjuan Xiao
Nanoscale FeWO 4 /BiVO 4 heterojunctions were directly grown on the graphite fiber felt (GF) with good conductivity to construct a FeWO 4 /BiVO 4 @GF solar photo-Fenton like wastewater treatment system. The removal effect of COD from phenolic wastewater and the mechanism of synergistic improvement of wastewater treatment efficiency by this system were investigated. The FeWO 4 /BiVO 4 heterojunction prepared by hydrothermal method exhibited higher photoelectric conversion efficiency and solar light utilization rate, thus endowing FeWO 4 /BiVO 4 with excellent solar-Fenton like reaction activity.The photo-Fenton activity can be maintained well even within the pH range of 2–8. Loading FeWO 4 /BiVO 4 nano-heterojunction on GF helped to increase the contact area between Fenton reagents and wastewater, facilitate the electron transfer on the FeWO 4 /BiVO 4 heterojunction and enable the recovery and reuse of the Fenton reagents.Under solar light radiation, the COD removal efficiency of FeWO 4 /BiVO 4 @GF/H 2 O 2 system in phenolic wastewater was more than 92%. Even after five cycles, the system still exhibited excellent operation stability. FeWO 4 /BiVO 4 @GF promoted the conversion and cycling of Fe(III)/Fe(II) by accelerating the separation and transport of photogenerated electrons/holes and increasing the concentration of active species, thereby stimulating excellent solar photo-Fenton like activity.The results are significance to the development of green and efficient photo-Fenton process for advanced treatment of industrial wastewater.
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