Frontiers of Materials Science
·
2023
·Vol. 17
·期 2
·1-11
·
IF 2.7
Xiao He,Xue Shoufeng,Fu Zimei,Zhao Man,Zhang Li,Zhang Junming,Wu Haishun,Jia Jianfeng,Yang Nianjun
Developing high-activity and low-cost catalysts is the key to eliminate the limitation of sluggish anodic oxygen evolution reaction (OER) during electrocatalytic overall water splitting. Herein, Ni–Fe/black phosphorous (BP) composites are synthesized using a simple three-electrode system, where exfoliation of bulky BP and synthesis of NiFe composites are simultaneously achieved. Under light illumination, the optimized Ni–Fe/BP composite exhibits excellent photoelectrocatalytic OER performance (e.g., the overpotential is 58 mV lower than a commercial RuO 2 electrocatalyst at a current density of 10 mA·cm −2 ). The electron transfer on this composite is proved to follow a Ni–BP–Fe pathway. The electronic structure of this Ni–Fe/BP composite is effectively regulated, leading to optimized adsorption strength of the intermediate OH* and improved intrinsic activity for the OER. Together with active sites on the support, this Ni–Fe/BP composite possesses abundant electrochemical active sites and a bug surface area for the OER. The introduction of light further accelerates the electrocatalytic OER. This work provides a novel and facile method to synthesize high-performance metal/BP composites as well as the approaches to reveal their OER mechanisms.
研究领域:
电化学
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催化
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材料科学
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纳米技术
·
能量转换
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DOI
高影响因子
JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Shuhao Li,Feng Wang,Zongli Xie,Derrick Ng,Boxiong Shen
Zeolitic imidazolate framework-8 (ZIF-8) based catalysts are considered as promising candidates for the selective catalytic reduction of NO by CO (CO-SCR) reaction due to their large specific surface area. However, the structure of ZIF-8 will be damaged during the synthesis procedure of the catalyst, leading to a decrease in their physical properties, which in turn affects the catalytic performance of the catalyst. Herein, a CeO 2 -ZIF-8 core-shell structure was synthesized and doped with Fe, resulting in the formation of Fe@CeO 2 -ZIF-8, for CO-SCR reaction. Characterization results show that the Fe@CeO 2 -ZIF-8 core-shell catalyst has better morphology, thermal stability, and higher specific surface area than the FeCe co-impregnated ZIF-8 catalyst (FeCe@ZIF-8 (IM)). Moreover, the reducibility of the reactive Fe species in the Fe@CeO 2 -ZIF-8 core-shell catalyst is also enhanced. As a result, the Fe@CeO 2 -ZIF-8 core-shell catalyst exhibited higher low-temperature CO-SCR catalytic activity with its NO conversion reaching 99% at 250 °C versus the FeCe@ZIF-8 (IM) catalyst (89% at 250 °C). The experimental results were further verified by density functional theory (DFT) calculations including Electron Localization Function (ELF), Valence Charge Density Difference (VCDD), Projected Density of States (PDOS) and Bader charge analyses. The calculation results revealed that the core-shell configured Fe@CeO 2 -ZIF-8 catalyst has a stronger active metal-support charge transfer and better capacity for the adsorption of the reactants. The reaction mechanism over Fe@CeO 2 -ZIF-8 core-shell catalyst was investigated via in situ DRIFTS experiments, and results showed that the nitro compounds and formate species are critical intermediates in this reaction at a higher temperature range (300–350 °C). This work provides a new strategy for the synthesis of ZIF-8 based catalysts with better properties for CO-SCR reaction.
研究领域:
催化化学
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环境化学
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材料科学
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物理化学
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能源化学
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表面科学
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纳米材料
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DOI
高影响因子
Journal of Inorganic and Organometallic Polymers and Materials
·
2023
·Vol. 34
·期 4
·1751-1764
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IF 4
Zhou Zhuyou,Zou Congyang,Wang Yong,Liu Menghe,Ji Yufeng
A one-step solvothermal synthesis technique was employed to fabricate C 60 /MIL-101(Fe) composites. The C 60 /MIL-101(Fe) composites showed a better performance in the degradation of methylene blue (MB) and tetracycline hydrochloride (TCH) when compared to MIL-101(Fe) in the photo-Fenton system, which can be credited to the charge transfer and separation facilitated by the addition of C 60 . Results showed that C 60 /MIL-101(Fe) had the capacity to nearly completely eliminate TCH and MB over a broad pH range. The catalysts demonstrated remarkable catalytic degradation on various organic pollutants and water samples. Through active substance quenching experiments and EPR, it was determined that hydroxyl radical (·OH) is the main factor in the photocatalytic reaction process.
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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纳米技术
✓ 已验证
DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 59
·54623-54635
·
IF 3.289
Jing Wang,Chao Liu,Ijaz Hussain,Cheng Li,Jiansheng Li,Xiuyun Sun,Jinyou Shen,Weiqing Han,Lianjun Wang
A series of iron–copper bimetallic nanoparticles supported on hollow mesoporous silica spheres with different Fe/Cu ratios were prepared using a simple post-impregnation and sodium borohydride reduction strategy. Different Fe/Cu ratios were obtained by addition of various amounts of ferric and copper salts. The catalysts were characterized by XRD, XPS, nitrogen physisorption, SEM and TEM. To explore the difference of catalytic reactivity among the various FeCu/HMS composites, Fenton-like catalytic oxidation of orange II was chosen as the model catalysis reaction. The catalytic results showed that the catalytic activity depended highly upon the Fe/Cu ratio. Particularly, 1/3 (2Fe6Cu/HMS) is the optimum Fe/Cu mass ratio to achieve the best catalytic activity. Based on the results of detection of ˙OH radicals and cyclic voltammograms, the important origin of the synergetic effect in 2Fe6Cu/HMS is considered as the combination of iron and copper species, which can accelerate the interfacial electron transfer in redox cycles of Fe3+/Fe2+ and Cu2+/Cu+ pairs, followed by the increase in the ˙OH radical generation. The 2Fe6Cu/HMS also possesses less pH dependence and maintains its high activity even under alkaline conditions. The optimal parameters in the degradation of 100 mg L−1 orange II are 27.4 mM of H2O2 with 1.0 g L−1 of catalyst, performed at a pH of 7.0 and 30 degree celsius. It is worth noting that 2Fe6Cu/HMS also possesses potential to treat a high concentration of dye pollutants. 77.7% of orange II was removed when conducted at 1000 mg L−1 initial dye concentration. The stability and recoverability of the composite catalyst were assessed it exhibited a good performance after 5 consecutive runs. The as-synthesized composite catalyst proved to be an attractive alternative for dye wastewater treatment applications.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yibo Zhang,Peng Hu,Yaseen Muhammad,Ying Tang,Shan Shao,Zhu Gao,Jiaxing Wang,Ruimeng Wang,Yang Hu,Lihan Kuang,Zhongxing Zhao,Zhenxia Zhao
Hollow nano-sphere NH 2 -MIL88(Fe) (HS NMIL88(Fe)) with interfacial defects was fabricated to load laccase as a host. Through metal multi-coordination, dopamine engineered large amount of defective pores with large size on NH 2 -MIL88(Fe) interface. This defect-interfacial structure provided a high-density host for laccases, which efficiently protected enzyme from structure deformation and then inhibited inactivation. Besides, the unique hollow structure will help to fasten reactant diffusivity, and thus improved the catalytic reaction process. Experimental results showed that the maximum immobilized capacity and maximum activity recovery for laccase reached up to 213.2 mg/g and 75.8% beyond many state-of-the-art enzyme hosts, respectively. Meanwhile, the immobilized laccase exhibited better pH, thermal and storage stabilities on HS NMIL88(Fe) than free and loaded on NMIL88(Fe) ones. Thermal deactivation kinetics analysis showed that HS NMIL88(Fe)-Lac had much higher apparent activation energies of (105.2 kJ/mol) than that of free laccase (89.2 kJ/mol). Catalyzing decolorization performance of dye Remazol Brilliant Blue R (RBBR) was finally carried out and exhibited the decolorization rate of 1.8 times and 2.6 times faster than solid NMIL88(Fe)-Lac and free laccase, respectively. Moreover, the interaction mechanism of laccase for RBBR was investigated and revealed by molecular docking.
研究领域:
生物化学
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环境科学
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材料科学
✓ 已验证
DOI
高影响因子
WATER RESEARCH
·
2022
·
IF 13.4
Wenkai Liu,Changrong Zhao,Shiqing Zhou,Bin Liu,Xiaoxiang Cheng,Zhihao Xue,Tingting Zhu
This study was aimed to evaluate the effects of a pre-treatment involving sulfite (S(IV)) synergistically activated by ultraviolet (UV)/Fe(II) on natural organic matter (NOM)-enhanced Ca 2+ scaling during nanofiltration treatment. Based on the variations in the physicochemical properties and correlation analyses of irreversible resistance, the intrinsic fouling mechanisms were revealed from two aspects: bulk crystallization (interaction between NOM and inorganic ions) and surface crystallization (morphology of surface crystallization and a change in the Ca 2+ concentration in the scaling layer). Furthermore, the degradation contribution rates of different free radicals during the UV/Fe(II)/S(IV) (UFS) treatment process were evaluated. During the reactions in the UFS, three free radicals (SO·–4, OH ·– and e- aq) were generated, and in-situ Fe(III) was formed in-situ . The carboxyl groups of the NOM were attacked by the free radicals, resulting in decreased of carboxyl concentration and density. In addition, the bond between Ca 2+ and NOM weakened, and hydrophobic (HPO) substances were mineralized. However, the Fe(III) formed in-situ was active and electropositive, competing with Ca 2+ for the complexation active sites on the NOM. The synergy effect of bulk crystallization and surface crystallization led to a significant decrease in the particle size of feed solution. The crystal size and roughness of membrane surface also decreased, which was conducive to reducing the membrane irreversible resistance. Correlation analysis revealed that the HPO ratio, carboxyl density and particle size (> 100 nm) ratio were effective characterization parameters for predicting irreversible resistance. This study not only provides guidance for alleviating membrane fouling caused by NOM-enhanced Ca 2+ scaling during the nanofiltration process, but also presents the rationality of irreversible resistance during nanofiltration process and various indicators with strong linear correlation.
研究领域:
环境科学
·
水处理工程
✓ 已验证
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 12
·期 3
·737-749
·
IF 6.119
Zhicheng Xu,Yuran Li,Yuting Lin,Bin Wang,Panting Gao,Tingyu Zhu
The reduction of NO by CO was proposed to be applied for regeneration gas to remove NOx from industrial flue gas with activated carbon purification technology. To improve the activity and sulfur resistance for the reduction of NO by CO in regeneration gas, Cu and Fe modifications on activated carbon were investigated. And various samples were characterized by XRD, XPS, TPD, H2-TPR, in situ DRIFTS and DFT calculations to explain the reaction mechanism and poisoning mechanism. The synergistic effects of oxygen-containing functional groups and metal sites show that –COOH acts as an anchor site for metals and that C–O–C acts as a protective site for Fe3+ under a SO2 atmosphere. Cu2+ sites have a high activity at low temperatures due to the large amount of adsorbed NO and the intermediate NOx− participating in the reaction with the NOx− pathway. Fe3+ sites have a high activity at high temperatures due to the high N–O dissociation activity with the *N pathway and –NCO pathway. DFT calculations proved that the binding Cu2+ and Fe3+ sites have higher activity than free Cu2+ and Fe3+ sites. A high content of SO2 exhibits various poisoning effects, mainly including the sulfation of metal sites, deposition of S, and consumption of CO. AC-Fe-H exhibits excellent resistance and stability against SO2 and H2O due to less S deposition caused by consumption through the S–CO reaction, slight sulfation caused by the protective effect of Fe2+ and C–O–C on Fe3+ sites and better hydrophobicity.
研究领域:
环境科学
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化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
WATER RESEARCH
·
2022
·
IF 13.4
Zhen Wang,Yangyi Yu,Qin Guo,Chaoting Guan,Jin Jiang
Multiple reactive intermediates have been proposed to be involved in peroxydisulfate (PDS) activation by zerovalent iron (ZVI), including sulfate radical (SO 4 ·− ) produced via iron-oxide shell mediated electron transfer, ferryl ion species (Fe(IV)) formed from Fe(II)-PDS interaction, and hydroxyl radical ( · OH) generated by ZVI aerobic oxygenation. In this study, evolution of the relative role of these intermediates in microscale and nanoscale ZVI (mZVI vs. nZVI) activated PDS processes is comparatively investigated by using a methyl phenyl sulfoxide (PMSO) probe that selectively reacts with Fe(IV) to produce methyl phenyl sulfone (PMSO 2 ). Interestingly, during PMSO transformation by mZVI/PDS process, yields of PMSO 2 (η(PMSO 2 )) exhibit three-stage behavior that they first increase to a maximum (∼80% but lower than 100%) (Stage I) and then plateau for a period (Stage II) followed by a decrease phase (Stage III). Accordingly, the relative role of Fe(IV) in PMSO transformation is unceasingly improved in Stage I and subsequently reaches equilibrium with that of free radicals in Stage II, while it finally decreases in Stage III. Similar η(PMSO 2 ) evolution trends are obtained in nZVI/PDS process, except that the η(PMSO 2 ) increase in Stage I is negligible, possibly due to the exceptional fast nZVI dissolution. It was further clarified by tert -butyl alcohol scavenging assay that, in addition to Fe(IV), the free radical involved in Stages I and II is SO 4 ·− , while · OH was dominant in Stage III. Moreover, studies on O 2 effect reveal that ZVI aerobic oxygenation participates in mZVI corrosion during the entire process, while it is only involved in nZVI corrosion when PDS content is reduced to a low concentration, indicating that the reactivities of PDS and O 2 are similar in mZVI corrosion, but differ greatly in nZVI corrosion. Additionally, effects of reactant dose and pH on η(PMSO 2 ) evolution are also explored. Dynamics of the relative role of different reactive oxidants should be taken into account in further applications of ZVI/PDS in situ chemical remediation technology considering their different chemistries.
研究领域:
环境科学
·
化学工程
·
水处理
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DOI
高影响因子
WATER RESEARCH
·
2024
·
IF 11.4
Zhaobin Liu,Shiliang Heng,Qicai Dai,Yijing Gao,Yule Han,Lingtian Hu,Yisheng Liu,Xueqin Lu,Guangyin Zhen
Waste activated sludge properties vary widely with different regions due to the difference in living standards and geographical distribution, making a big challenge to developing a universally effective sludge dewatering technique. The Fe(II)-activated persulfate (S 2 O 8 2− ) oxidation process shows excellent ability to disrupt sludge cells and extracellular polymeric substances (EPS), and release bound water from sludge flocs. In this study, the discrepancies in the physicochemical characteristics of sludge samples from seven representative cities in China (e.g., dewaterability, EPS composition, surface charge, microbial community, relative abundance of antibiotic resistance genes (ARGs), etc.) were investigated, and the role of Fe(II)-S 2 O 8 2− oxidation in enhancing removal of antibiotic resistance genes and dewatering ability were explored. The results showed significant differences between the EPS distribution and chemical composition of sludge samples due to different treatment processes, effluent sources, and regions. The Fe(II)-S 2 O 8 2− oxidation pretreatment had a good enhancement of sludge dewatering capacity (up to 76 %). Microbial analysis showed that the microbial community in each sludge varied significantly depending on the types of wastewater, the wastewater treatment processes, and the regions, but Fe(II)-S 2 O 8 2− oxidation was able to attack and rupture the sludge zoogloea indiscriminately. Genetic analysis further showed that a considerable number of ARGs were detected in all of these sludge samples and that Fe(II)-S 2 O 8 2− oxidation was effective in removing ARGs by higher than 90 %. The highly active radicals (e.g., SO 4 − ·, ·OH) produced in this process caused drastic damage to sludge microbial cells and DNA stability while liberating the EPS/cell-bound water. Co-occurrence network analysis highlighted a positive correlation between population distribution and ARGs abundance, while variations in microbial communities were linked to regional differences in living standards and level of economic development. Despite these variations, the Fe(II)-S 2 O 8 2− oxidation consistently achieved excellent performance in both ARGs removal and sludge dewatering. The significant modularity of associations between different microbial communities also confirms its ability to reduce horizontal gene transfer (HGT) by scavenging microbes.
研究领域:
环境工程
·
微生物学
·
污水处理
✓ 已验证
DOI
PubMed
高影响因子
Environmental Sciences Europe
·
2019
·Vol. 31
·期 1
·1-10
·
IF 5.878
Zhou Qingxiang,Wu Yalin,Yuan Yongyong,Zhou Xianqi,Wang Hongyuan,Tong Yayan,Zhan Yali,Sun Yi,Sheng Xueying
Background Sudan red dyes are widely used as color additions in various fields. Due to their potential carcinogenicity and large consumption, they have absorbed much more attention and become a research hot topic. There have been a few of existing methods for their analysis from samples; however, it is of great importance to develop simple, sensitive, and low-cost analytical method for public health and safety. This article described a new method based on magnetic Fe@NiAl-layered double hydroxides for enrichment of Sudan red dyes in combination with high-performance liquid chromatography. Results The as-prepared magnetic Fe@NiAl-layered double hydroxides (Fe@NiAl-LDHs) exhibited good adsorption capacity for Sudan red dyes, and could be used as an effective adsorbent for preconcentration of three Sudan Red dyes from environmental water samples. The proposed method provided low limits of detection in the range of 0.002–0.005 μg L −1 with magnetic solid-phase extraction in combination with high-performance liquid chromatography. Conclusion The developed method utilized the easy to prepare magnetic materials as adsorbents and conventional analytical instrument and provided high sensitivity, which provided a robust and low consumption of toxic organic solvent alternative method. The results of present study are of great value for interested laboratories to monitor the level of Sudan red dyes in water samples or develop sensitive determination methods to monitor other pollutants at trace level in environmental waters.
研究领域:
分析化学
·
环境科学
·
食品安全
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Mingran Li,Xia Qin,Jiaxin Cui,Rui Guo,Chengrui Guo,Ziyuan Wang,Tinghui Li
In this study Cu-Fe bimetallic aerogel-like carbon based on sodium alginate (SA) was prepared as catalytic particle electrode by freeze-drying and carbonization process. The characterization indicates that Cu and Fe were loaded on the surface and inside SA-based biomass carbon (SAC) in the form of a zero-valent copper-iron alloy to form a Cu-Fe/Sodium alginate Carbon (Cu-Fe/SAC) particle electrode. After using a three-dimensional Electro-Fenton (3D-EF) system with the prepared particle electrode, the optimal experimental operating parameters for removal of fulvic acid (FA) were obtained as follows: voltage 2.5 V, pH 5.4, and catalyst dosage 4 g/L. A removal efficiency from 82.9% to 74.4% for FA was achieved in a wide pH range of 3–7. Comparison experimental results indicate that the 3D-EF system with bimetallic Cu-Fe/SAC as the catalytic particle electrode (CPE) has higher FA degradation rate and mineralization efficiency than two-dimensional Electro-Fenton (2D-EF) system, even higher than the 3D-EF system with Cu/SAC or Fe/SAC. Hydroxyl radicals (·OH) trapping experiments showed that the main contribution to FA degradation and mineralization in the 3D-EF system would be the ·OH radical produced by a heterogeneous Fenton-like reaction. The comparison and trapping experiment results indicate that the possible mechanism of the 3D-EF with Cu-Fe/SAC as CPE for FA degradation may involve adsorption, anode oxidation, heterogeneous and homogeneous Fenton-like reactions.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2021
·
IF 6.558
Jiabi Xu,Yanyan Xing,Yutong Liu,Mingzhe Liu,Xiaohong Hou
In recent decades, artificial nanozymes with excellent stability, low cost and availability have been gradually explored to avoid the limits of natural enzymes such as poor stability, high cost and difficult preparation. Herein, for the first time, we investigated the capability of nanoscale Fe 3 O 4 @MIL-100(Fe) as a nanozyme, which was quickly synthesized in situ by a microwave-assisted method within 20 min using Fe 3 O 4 as the metal precursor. The obtained Fe 3 O 4 @MIL-100(Fe) showed satisfactory intrinsic dual enzyme mimetic activities, including peroxidase (POD)- and catalase (CAT)-like activities. Moreover, a simple and effective colorimetric biosensor was fabricated to detect glutathione (GSH) based on its POD-like activity. The proposed measurement had a linear range of 1–45 μM and a limit of detection (LOD) of 0.26 μM (3.3 δ/S). It was proved that the established colorimetric sensing system could be successfully applied to detect GSH in actual biological samples. Importantly, the outstanding reusability and stability made it extremely valuable as a catalyst. The present work implied that Fe 3 O 4 @MIL-100(Fe) synthesized in situ by the microwave-assisted method was a very promising candidate for biocatalyst and biosensing.
研究领域:
纳米生物技术
·
分析化学
·
生物传感
·
酶模拟
·
分子诊断
·
转化医学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）