DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 34
·13085-13093
·
IF 4.569
Lijun Guo,Feifei Li,Jianxin Liu,Zehui Jia,Rui Li,Zhuobin Yu,Yawen Wang,Caimei Fan
The scaling relations between nitrogen adsorption and NHx destabilization are key challenges to the widespread adoption of the photocatalytic synthesis of ammonia. In this work, a FeII-rich MIL-101(Fe) (MIL-101(FeII/FeIII)) was synthesized using a one-step solvent thermal method with ethylene glycol (EG) as a reducing agent, which can break the scaling relationship by photoinduced FeII (high nitrogen adsorption ability) and FeIII (high NHz destabilization ability) cycling. XPS was used to detect the change in iron valence state in the MIL-101(FeII/FeIII) material. The photocatalytic nitrogen fixation efficiency of MIL-101(FeII/FeIII) under visible light without any sacrificial agent was 466.8 μmol h−1 g−1, five times that of MIL-101(Fe). After photocatalytic experiments, MIL-101(FeII/FeIII) retained an unchanged FeII/FeIII rate, indicating that this FeII/FeIII cycling can be maintained. DFT modeling of the FeII-rich MOF material showed that a FeII1 FeIII2 system has a higher N2 activation capacity than a FeIII3 system. The catalytic mechanism was further proved by in situ infrared spectra and N15 isotopic tracers. Therefore, the improvement of photocatalytic activity was mainly attributed to the change in the nitrogen adsorption capacity during the photoinduced FeII/FeIII cycling.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
·
IF 5.107
Yuqi Cui,Li-chao Nengzi,Jianfeng Gou,Yan Huang,Bo Li,Xiuwen Cheng
Z-scheme heterojunction photocatalyst can simultaneously reduce the recombination of photo-generated electron-hole pairs and preserve its outstanding redox ability during the process of photocatalytic reaction. In this study, Z-scheme MIL-53(Fe)/α-Bi 2 O 3 /g-C 3 N 4 photocatalyst was successfully fabricated via an accessible method and comprehensive characterized by XRD, FT-IR, SEM, TEM, XPS, N 2 adsorption-desorption isotherms, UV–vis diffuse reflection spectroscopy and photoelectrochemical analysis. The as-obtained MIL-53(Fe)/α-Bi 2 O 3 /g-C 3 N 4 composite exhibited superior photocatalytic activity for amino black 10B degradation than that of pure g-C 3 N 4 , α-Bi 2 O 3 , MIL-53(Fe) and α-Bi 2 O 3 /g-C 3 N 4 binary composite under visible light irradiation and the photodegradation rate would achieve the maximum when the mass fraction of MIL-53(Fe) was 32% in ternary composite. The enhanced photocatalytic performance of MIL-53(Fe)/α-Bi 2 O 3 /g-C 3 N 4 ternary composite could be mainly ascribed to improved visible light absorption range and the construction of an effective interfacial heterojunction driven by direct solid-state dual Z-scheme mechanism, which significantly facilitates the separation and transfer of photo-generated charge carriers. Eventually, the as-prepared ternary composite was confirmed to have prominent stability and reusability after consecutive 4 recycling run.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
JOURNAL OF SOILS AND SEDIMENTS
·
2022
·Vol. 22
·期 7
·2009-2021
·
IF 3.536
Liu Quanfeng,Yu Jiang,Jiang Yinying,Zhong Chengwei,Ding Senxu,Zhou Peng,Jin Yuanxiao
Purpose Soil organic matter pollution is a serious threat to the human living environment. The purpose of this paper is to investigate the effect of MIL-101(Fe)/g-C 3 N 4 catalyzed peroxynitrite degradation of 2-chlorophenol in soil and to analyze the reaction mechanism and further to explore the optimal parameters of this reaction system with utilizing the mathematical model. Methods MIL-101(Fe)/g-C 3 N 4 was successfully obtained by hydrothermal synthesis method by growing MIL-101(Fe) on the surface of g-C 3 N 4 to catalyze the degradation of 2-CP (2-chlorophenol) in soil by sodium persulfate. The influence factors on the removal rate of 2-CP were analyzed by the response surface methodology (RSM) and combined with theoretical calculations. RSM can be used to model continuous variable surfaces with less data and determine the optimal level range. Results MIL-101(Fe)/g-C 3 N 4 had a good catalytic performance due to its good catalytic properties and the adsorption of g-C 3 N 4 on 2-CP in the system and made the best removal rate of 2-CP increase to 91.2%. The correlation of model fitting results was significant, and the verification of its optimal parameters yielded results with an error of only 4.1%. Conclusion Further studies revealed that SO 4 •− and • OH were the reactive radicals, and SO 4 •− was the dominant, which impelled Fe 2+ and Fe 3+ to interconvert in the complex system. Possible degradation pathways were derived by analyzing the intermediates. Generally, this experiment provides some ideas for future research of MOFs in soil organic pollutant removal systems. Graphical abstract
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xiangyang Li,Min Yang,Yushi Xie,Longjiao Zhu,Wentao Xu
Every year, a significant amount of fruit and vegetable spoilage caused by microbial contamination leads to substantial food waste and economic losses in the agricultural and food sectors. There is an urgent need to develop highly efficient and safe multifunctional preservation materials. Curcumin (Cur) is known for its excellent antioxidant and antibacterial properties; however, its poor water solubility and low bioavailability severely limit its practical applications. In this study, we synthesized highly stable and water-dispersible metal-biomolecule network nanoparticles by self-assembly of ferrous ions (Fe 2+ ) with DNA in an aqueous solution at room temperature. Furthermore, by leveraging the strong coordination interaction between Iron(Fe) and Cur, we prepared Cur-modified nanoparticles (Fe-DNA-Cur) with dual antioxidant and antibacterial functions. Fe-DNA-Cur not only preserves the biological activity of curcumin, but also effectively addresses its inherent poor water solubility. After further compounding with chitosan (CS), the as-prepared Fe-DNA-Cur@CS composite demonstrates breakthrough antimicrobial performance, thereby providing an innovative solution for developing novel, highly effective and safe fruit/vegetable preservatives. When used as a sustainable food packaging coating for perishable fruits at room temperature, the Fe-DNA-Cur@CS coating can reduce dehydration, prevent nutrient loss, inhibit microbial growth, increase nutraceutical value, maintain strawberry quality, and extend shelf life during storage. This study demonstrates the potential of Fe-DNA-Cur@CS as a multifunctional coating material to reduce food waste and agricultural economic losses caused by microbial contamination.
研究领域:
食品科学
·
纳米技术
·
农业工程
·
材料科学
·
微生物学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Cleaner Production
·
2022
·
IF 11.072
Xiangyu Wang,Wei Zhang,Xu Zhang,Lang Ran,Quanlin Zhao,Binze Zou,Lincheng Zhou,Zhengfang Ye
Chloromethyl styrene-divinylbenzene (PS–Cl) resin was usually chemically modified for the adsorption of heavy metal ions in wastewater. However, this work will introduce a new application of resin for catalytic degradation of antibiotics. The core-shell PS-NH 2 @MIL-53(Fe) catalyst was fabricated by simple two-step route including chemical synthesis and step-by-step self-assembly strategy. The catalysts exhibited excellent catalytic activity toward the degradation of tetracycline (TC) in the presence of H 2 O 2 , with a degradation efficiency and degradation rate constant ( k ) of 94.15% and 0.05643 min −1 within initial 20 min, respectively. Moreover, the mineralization and stability of PS-NH 2 @MIL-53(Fe) both showed excellent performance. The advantage of PS-NH 2 @MIL-53(Fe) is that the degradation efficiency of TC could be modulated by the number of self-assembly. Additionally, we utilized the Yellow River water to explore the effect of the catalyst for TC removal in the actual wastewater treatment . Meanwhile, several possible catalytic degradation pathways were analyzed on the basis of using HPLC-MS to detect the intermediates generated in the process of catalytic degradation, and a potential catalytic degradation mechanism was proposed. In brief, the new application of amination resin modified by MIL-53(Fe) in catalytic degradation of TC shows promising prospect, especially in the field of environmental remediation.
研究领域:
环境科学
·
催化化学
·
废水处理
✓ 已验证
DOI
高影响因子
PHOTOCHEMISTRY AND PHOTOBIOLOGY
·
2024
·
IF 2.6
Rong Zhang,Zhuannian Liu,Taoli Chen
Developing cost-effective and efficient photo-Fenton catalysts is crucial for advancing photo-Fenton technology. MoS 2 is a representative transition metal disulfide with attractive photoresponsiveness, making it ideal for preparing composite photo-Fenton catalysts. In this study, natural molybdenite was innovatively utilized as a source of MoS 2 (OM) to synthesize a low-cost and efficient Fe@MoS 2 (OMF) composite photo-Fenton catalyst by comminution and adsorption, which was then applied to the remediation of antibiotic-contaminated water. The OMF composites exhibited significant catalytic activity, with a kinetic rate constant of 0.022 min −1 , which was 3.1 times higher than that of the original OM (0.007 min −1 ), indicating a 3% increase. This was attributed to the synergistic effect of many photogenerated electrons and reversible Mo 4+ /Mo 6+ redox pairs, which accelerated the regeneration of Fe 2+ . After three cyclic tests, the concentrations of dissolved Fe 2+ and Mo 2+ ions remained below 0.38 mg/L and 0.17 mg/L, respectively. This indicates the high reusability of the catalyst in cyclic experiments. Ultimately, the main active species, •OH and •O 2 − , were generated during the photo-Fenton process, contributing significantly to TC degradation. This study may serve as a reference for the development and application of natural mineral composite photo-Fenton catalysts in the treatment of organic wastewater.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2023
·Vol. 154
·期 5
·2182-2196
·
IF 2.8
Liu Jialu,Song Zhi,Liu Boxia,Zhang Xiayan,Huang Yeqiong,Han Dongxu
Because of its high toxicity and severe degradation, phenol has caused serious environmental pollution, and it is urgent to explore a stable and efficient degradation method of phenol. In this study, Ni/Fe bimetallic atomic cluster composite catalyst activated peroxymonosulfate (PMS) to degrade phenol efficiently. The experimental results show that the phenol degradation rate can reach 100% in a wide range of pH (3–11), and the system offers good stability in repeated experiments. The free radical quenching investigation and electrochemical characterization showed that the non-free radical pathway dominated the degradation system, and a large amount of singlet oxygen and rapid electron transfer promoted the efficient degradation of phenol in wastewater. This study opens up a new way for bimetallic atom cluster catalysts to activate PMS to degrade organic pollutants. Graphical
研究领域:
环境科学
·
催化
·
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Qiao Han,Mooeez Ur Rehman,Junhu Wang,Alexandre Rykov,Oliver Y. Gutiérrez,Yujun Zhao,Shengping Wang,Xinbin Ma,Johannes A. Lercher
The catalytic hydrodeoxygenation (HDO) of lignin-derived phenolic compounds is a critical step in the upgrading of bio-oil. Here, bimetallic Ni-Fe nanoparticles supported on mesoporous carbon spheres (MCSs) were fabricated and applied in HDO of phenol. In comparison with monometallic Ni and Fe catalysts, the bimetallic Ni-Fe catalyst exhibited better performance for phenol HDO due to the formation of Ni-Fe alloy phase identified by X-ray powder diffraction (XRD) and Mössbauer spectroscopy techniques. Among several explored ratios, the catalysts with Ni/Fe ratio of 3/1 presented the highest cyclohexane yield. The reaction occurred in two consecutive steps: the hydrogenation of phenol to cyclohexanol and the further hydrogenolysis of cyclohexanol to cyclohexane. Kinetic studies showed that the hydrogenolysis of cyclohexanol controlled the overall reaction rate of phenol HDO due to the lower reaction rate of this step. Indeed, the turnover frequency (TOF) values of cyclohexanol normalized by surface metallic Ni sites exhibited a linear correlation with Ni-Fe alloy sites. The alloying of iron in the bimetallic Ni-Fe catalysts significantly enhanced the adsorption strength of cyclohexanol, which is the reason of the high activity of the Ni-Fe alloy particles. Thus, Fe-containing sites adsorb the hydroxyl species while Ni sites perform the H 2 activation, their synergistic effect plays a key role in phenol HDO process.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2025
·
IF 4.7
Jiaze Chen,Huijie Xie,Yusen Chen,Dong Guo,Binjie Li,Xuanxuan Sun,Volodymyr Turkevych,Caixia Li,Dehong Chen,Lei Wang,Bin Li
Fenton-like degradation based on iron catalyst have been developed to remove organic pollutants from wastewater. However, iron-based catalysts still face challenges of poor accessibility and stability of active sites. Here, we report a facile and green method for the preparation of Fe x Cu (1-x) @HZSM-5 catalyst using ethylenediamine as an organic ligand to stabilize metal species via a combination of solid-state grinding and steam-assisted crystallization methods without organic templates. Due to the confinement of zeolite ZSM-5 framework and synergistic effect of Fe and Cu bimetals, the optimized Fe 0.8 Cu 0.2 @HZSM-5 catalyst exhibits excellent activity and reusability in the Fenton-like degradation of methylene blue at the neutral condition. Our strategy for fabricating bimetal@zeolite can bring about new thoughts for the preparation of iron-based catalyst with high efficiency for Fenton-like degradation.
研究领域:
环境科学
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
·
2025
·
IF 6.3
Jun-Feng Lu,Huan Wang,Yi Zhou,Xue-Ying Mao,Xiao-Qian Feng,Shuang Wang,Yong-Hua Zhao
Background Rhodamine B (RhB) poses a significant threat to aquatic ecosystems. While Fenton oxidation process is promising approach for RhB degradation, the conventional Fenton reaction has the narrow pH range and poor reusability. To overcome these, this study developed Fenton-like system with Fe-Cu/HZSM-5 catalyst for effective RhB degradation. Methods A series of Fe x Cu 5-x /HZSM-5 catalysts (x represents the molar ratio of Fe to Cu) were prepared by impregnation. These catalysts were integrated with H 2 O 2 to construct Fenton-like system for the degradation of RhB. The catalysts were characterized by XRD, NH 3 -TPD, XPS, FT-IR, and N 2 adsorption-desorption at low temperature techniques. Significant findings Among the tested catalysts, Fe 3 Cu 2 /HZSM-5 exhibited optimal performance, achieving near-complete RhB degradation (∼100%) under the condition of 45 °C, 5.3 mM/L H 2 O 2 , 3.0 g/L catalyst dosage, and broad pH range (2–5). Mechanistic studies confirmed that hydroxyl radicals (·OH) were the primary oxidants responsible for RhB degradation in Fenton-like system. Under ·OH attacking, RhB underwent a series of reactions such as N-deethylation and disruption of the conjugated structure and was eventually mineralized into CO 2 and H 2 O. Overall, a novel Fe-Cu/HZSM-5 catalyst was developed to address the limitations of the traditional Fenton reaction, providing valuable insights for future research in this field.
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Xu Yang,Rui Qiu,Ming-Jian Lan,Gang Chen,Wei Xu,Yu Shen
Designing the efficient, low-cost and stable electrocatalyst is of great significance for storage and conversion of the renewable energy to hydrogen. Herein, the binder-free Ni–Fe–S electrocatalysts were directly electrodeposited on Ni foam, which exhibited the excellent hydrogen evolution reaction performance with the overpotential of 51.4 mV at the current density of 10 mA cm −2 . Based on the analysis and results of as-synthesized Ni, Ni–Fe and Ni–S, the boosted electrocatalytic activity can be attributed to the composite effect between Ni and the introduced Fe and S. Additionally, the Ni–Fe–S electrocatalysts also displayed the low cell voltage (1.59 V at 10 mA cm −2 ), remarkable durability and high Faraday efficiency in overall water electrocatalysis . Moreover, the water electrolysis device with Ni–Fe–S bi-electrodes can be driven by a small wind power generation and producing 4 mL H 2 in 39 min, indicating the prepared Ni–Fe–S electrocatalyst has the great potentials in producing hydrogen via renewable energy.
研究领域:
材料科学
·
能源转换与存储
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 33
·80817-80827
·
IF 5.8
Huang Guofu,Wang Mianmian,Sun Xinying,Liu Haijian,Liu Fangfang
In this work, pomegranate peel extracts were used as the green reducing agent to synthesize Cu/Fe nanoparticles (P-Cu/Fe nanoparticles) and removed tetrabromobisphenol A (TBBPA) in aqueous solution. P-Cu/Fe nanoparticles were amorphous and irregularly spherical. The surfaces of nanoparticles contained Fe 0 , Fe 3+ oxides (hydroxides), and Cu 0 . The bioactive molecules from pomegranate peel were extremely important for the synthesis of nanoparticles. P-Cu/Fe nanoparticles had excellent removal performance for TBBPA, and 98.6% of TBBPA (5 mg L −1 ) was removed within 60 min. The removal reaction of TBBPA by P-Cu/Fe nanoparticles was well-fitted with the pseudo-first-order kinetic model. The Cu loading was critical for TBBPA removal with an optimum value of 1.0 wt%. A weakly acidic condition (pH 5) was more favorable for the removal of TBBPA. The removal efficiency of TBBPA increased with the rise of temperature and decreased with increasing initial TBBPA concentration. The activation energy ( E a ) was 54.09 kJ mol −1 , indicating that the removal of TBBPA by P-Cu/Fe nanoparticles was mainly surface-controlled. Reductive degradation was the main mechanism of TBBPA removal by P-Cu/Fe nanoparticles. In conclusion, green synthesized P-Cu/Fe nanoparticles using pomegranate peel waste show great potential for the remediation of TBBPA in aqueous solution.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）