APPLIED CLAY SCIENCE
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2021
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IF 5.467
Zhou Cao,Yuefa Jia,Qizhao Wang,Hongfei Cheng
Traditional homogeneous Fenton reactions can only be carried out under acidic conditions; however, visible light can greatly enhance the activity and stability of iron-doped semiconductor catalysts in the Fenton system. Therefore, in this study, a commercially applicable Fe/graphitic carbon nitride (g-C 3 N 4 )/kaolinite composite photocatalyst was prepared for the first time using an in-situ calcination process. The results showed that Fe ions and g-C 3 N 4 were successfully loaded onto kaolinite with a two-dimensional uniform sheet structure. The as-synthesized Fe/g-C 3 N 4 /kaolinite composite containing 0.9 mmol of Fe (Fe/CN/K-0.9) showed a degradation efficiency of 89% for tetracycline hydrochloride (TCH) within 80 min in the photo-Fenton system. Compared with photocatalytic degradation (29.6%) and Fenton degradation (76.6%), a photo-Fenton degradation efficiency of 85% was maintained after three cycles. Free radical scavenging experiments also showed that hydroxyl radicals were the main active substances. The enhanced photocatalytic activity of the composite was attributed to the large specific surface area of kaolinite, which could effectively adsorb TCH. Furthermore, Fe III acted as a photo-generated electron acceptor , which not only avoided photo-generated electron-hole recombination but also effectively reduced the consumption of H 2 O 2 to realize a stable Fe II /Fe III cycle reaction, thus improving photo-Fenton catalytic activity .
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF SOILS AND SEDIMENTS
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2022
·Vol. 22
·期 7
·2009-2021
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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
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催化化学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2016
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IF 8.328
Jianqing Ma,Qunfeng Yang,Yuezhong Wen,Weiping Liu
Heterogeneous Fe-N complexes are a kind of promising catalysts for the Fenton-like reaction. The present study selected a stable and inexpensive g-C 3 N 4 as the chelating agent and combined with the graphitized mesoporous carbon (GMC). The fabricated Fe-g-C 3 N 4 /GMC composite was characterized by several techniques including FTIR, XRD, XPS, TEM and STXM. Results showed clear sheets of g-C 3 N 4 and graphite with Fe evenly distributed mostly in the Fe-N coordination form. The catalyst expressed high activity in the Fenton-like reaction in a wide pH range of 4–10. 99.2% removal of Acid Red 73 was obtained in 40 min, and the degradation data well fitted with the pseudo-first-order kinetics model. By correlating the constant of reaction rates calculated from the model and the Fe speciation contents of the samples prepared at different conditions, we deduced that Fe-N species are the most important active sites for the Fenton-like reaction. More importantly, hydroxyl radicals played a great role in the whole reaction yet their generation was independent of visible light. Cyclic voltammetry results confirmed that the GMC can accelerate the Fe(III)/Fe(II) redox cycle by enhancing electron transfer, and thus enable this Fenton-like catalyst to perform well in a wide pH range.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Qun Ding,Xuejun Zou,Jun Ke,Yuying Dong,Yubo Cui,Hongchao Ma
Herein, a ternary TiO 2 /MIL-88A(Fe)/g-C 3 N 4 heterojunction is successfully constructed through a facile hydrothermal strategy for enhancing solar energy harvesting and efficiency of catalytic nitrogen reduction induced by enlarged light absorption range, increasing interfacial charge transfer ability and desirable stability. Under the simulated sunlight irradiation, the N 2 fixation experiment shows that the yield of NH 3 reaches 1084.31 μmol/(g·h) over the TiO 2 /MIL-88A(Fe)/g-C 3 N 4 photocatalyst, and the yield is significantly enhanced, which is 33.68 and 13.94 times that is higher than the pure TiO 2 and g-C 3 N 4 , respectively. In a mean time, the excellent performance of the photocatalytic N 2 fixation over the ternary TiO 2 /MIL-88A(Fe)/g-C 3 N 4 is verified based on density function theory calculation and the decisive step over the composite is investigated by calculating Gibbs free energies of nitrogen reduction paths. The performance enhancement mechanism of TiO 2 /MIL-88A(Fe)/g-C 3 N 4 is speculated, which indicates that the hybridized three-component system presents a desirable Z-scheme band alignment, resulting in the improvement of separation and transfer efficiency of photoinduced charge carriers. The article shows a new and high-efficiency TiO 2 /MIL-88A(Fe)/g-C 3 N 4 photocatalysis for excellent nitrogen reduction ability.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Huihu Wang,Hao Tu,Feng Chen,Huang Xu,Ziguan Zhang,Guode Chen,Chenhuinan Wei,Xing Xiang,Zhixiong Xie
Through a facile oil bath method, a novel highly dispersed NH 2 -MIL-101(Fe)/carboxylated g-C 3 N 4 (NM-101(Fe)/CCN) heterostructure was prepared using the chemical bonding between carboxyl groups and -NH 2 groups. Compared with the octahedral morphology of pure NM-101(Fe), the chemical bonding interaction promoted the heterogeneous nucleation and growth of NM-101(Fe) to form nanometer-sized granular morphology, which was homogeneously dispersed on CCN surface. Cr(Ⅵ) and ciprofloxacin (CIP) were selected as the typical pollutant models in micro-polluted water sources. The results showed that 10 %NM-101(Fe)/CCN heterostructure could remove 97 % of Cr(Ⅵ) in 60 min and 88 % of ciprofloxacin (CIP) in 120 min. In the dual pollutant system of Cr(Ⅵ) and CIP, Cr(Ⅵ) reduction and CIP degradation can promote each other, and the degradation efficiency of CIP reached 96 % within 120 min. The apparent rate constant of 10 %NM-101(Fe) /CCN heterostructure for Cr(Ⅵ) reduction was 4.30 and 9.67 times of that of NM-101(Fe) and CCN, respectively, which may be ascribed to the interface electric field and good interface bonding of heterojunction . The charges separation efficiency was significantly improved, which effectively enhanced the photocatalytic activity.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Xue Bai,Juan Shi,Lu Xu,Xin Jin,Xuan Shi,Pengkang Jin
To overcome the shortcomings of homogeneous Fe ion activating peroxymonosulfate (PMS), such as high pH-dependence, limited cycling of Fe(III)/Fe(II) and sludge production, graphite carbon nitride (g-C 3 N 4 ) is chosen as a support for Fe ions, and reduced graphene oxide (rGO) is employed to facilitate the electron transfer process, thereby enhancing catalysis. Herein, a ternary catalyst, Fe-g-C 3 N 4 /rGO, is first applied under lightless condition for PMS activation , which exhibits ideal performance for contaminant mineralization. 82.5 % of the total organic carbon (TOC) in 100 mL of 5 mg/L bis -phenol A (BPA) was removed within 20 min by the optimal catalyst named 30%rFe 0.2 CN, which shows a strong pH adaptability over the range of 3–11 compared with a common Fenton-like system. Moreover, the highly stable Fe-g-C 3 N 4 /rGO/PMS catalytic system resists complex water matrices, especially those with high turbidity . To unveil the mechanism of PMS activation and pollutant degradation , the physicochemical properties of the as-prepared catalysts are comprehensively characterized by multiple techniques. The Fe(III) contained in both the Fe-N group and α-Fe 2 O 3 component of 30%rFe 0.2 CN not only directly reacts with PMS to produce sulfate radicals ( SO 4 − ) and hydroxyl radicals ( OH), but also combines with PMS to form the essential [Fe(III)OOSO 3 ] + active complex, thereby generating superoxide radicals ( O 2 − ) and singlet oxygen ( 1 O 2 ). Among the various reactive oxidizing species, 1 O 2 plays an important role in pollutant removal , which is additionally generated by the C O moiety of the catalyst activating PMS as well as PMS self-oxidation, indicating the dominance of the non-radical pathway in the pollutant degradation process. Due to the advantages of high efficiency, wide pH adaptability and stability, the proposed lightless Fe-g-C 3 N 4 /rGO/PMS catalytic system represents a promising avenue for practical wastewater purification.
研究领域:
环境科学
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催化材料
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废水处理
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Guanshu Zhao,Jing Ding,Jiayi Ren,Qingliang Zhao,Qingwei Gao,Kun Wang,Liangliang Wei,Xueqi Chen,Fanyang Zhou,Dionysios D. Dionysiou
A novel Fe-modified g-C 3 N 4 with rich N vacancies (NVs) under N 2 calcination was developed to active sulfite for the efficient removal of contaminants and bacterial inactivation under visible light (VIS). The degradation rates of VIS/sulfite/Fe/g-C 3 N 4 (N 2 ) for acetaminophen (ACT) were 10.94, 4.88, and 2.85 times higher than those of VIS/Fe/g-C 3 N 4 (N 2 ), VIS/sulfite/g-C 3 N 4 (N 2 ), and VIS/sulfite/Fe/g-C 3 N 4 (CO 2 ), respectively. Escherichia coli (E. coli) with an initial concentration of 2.5 × 10 8 CFU/mL decreased by 6.1 and 8.4 log CFU/mL within 60 min and 80 min of inactivation, respectively. The activation of sulfite led to the generation of oxysulfur radicals, and the consumption of hole (h + ) by sulfite inhibited its recombination with electron (e − ), promoting the formation of superoxide radical ( • O 2 – ). The synergistic effect of Fe, NVs, and g-C 3 N 4 in VIS/sulfite/Fe/g-C 3 N 4 (N 2 ) system promoted the generation of oxysulfur radicals. Density functional theory (DFT) calculations indicated that NVs facilitated charge transfer from Fe to g-C 3 N 4 substrate, accelerating the Fe 3+ /Fe 2+ and oxysulfur radical cycles. Fe/g-C 3 N 4 with rich NVs exhibited lower adsorption binding energy, faster charge transfer, and longer S-O bond length than pristine Fe/g-C 3 N 4 during sulfite adsorption. This work unraveled the synergistic mechanism of Fe, NVs, and g-C 3 N 4 , which provides new insights into heterogeneous photocatalysts on sulfite activation for water treatment.
研究领域:
环境科学
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材料科学
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生物学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Huayu Wang,Yanhua Cao,Changsheng Guo,Ming Ge
Heterogeneous catalyst/persulfate advanced oxidation process has been widely used in antibiotic wastewater treatment . As-designed MIL-88A(Fe)/g-C 3 N 4 composite catalyst firstly activated peroxydisulfate (PDS) to degrade tetracycline (TC) in this work. Activating PDS by MIL-88A(Fe)/g-C 3 N 4 has a higher efficiency and rate toward TC degradation compared with MIL-88A(Fe) and g-C 3 N 4 . After 60 min, the optimal MIL-88A(Fe)/g-C 3 N 4 -5 activated PDS to degrade about 80% of TC in water. The existence of g-C 3 N 4 increases the specific surface area and active Fe 2+ content of MIL-88(Fe), promotes PDS adsorption and utilization, thus showing an excellent catalytic performance for PDS activation. MIL-88A(Fe)/g-C 3 N 4 activated PDS oxidation process synergistically removed TC by free radicals (O 2 •− , •OH and SO 4 •− ) with non-free radicals ( 1 O 2 ), and the effect of some important operating factors on TC removal, the TC degradation pathways and toxicity of TC intermediates were analyzed. Moreover, the MIL-88A(Fe)/g-C 3 N 4 -5 powdered catalyst was designed into a catalytic membrane, which could remove 96% of TC in a short time (<10 min). The cycle tests confirm that powdered MIL-88A(Fe)/g-C 3 N 4 composite catalyst and its catalytic membrane have a good recyclability and stability, demonstrating that this catalyst possesses a practical application potential in the treatment of TC polluted wastewater.
研究领域:
环境科学
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催化材料
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废水处理
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Shi-Wen Lv,Qiuyu Zheng,Lingjie Ye,Chun-Yang Li,Jing-Min Liu,Yanqing Cong,Shuo Wang
Nowadays, simultaneous removal of organic pollutants and heavy metals from wastewater is still a complicated task with great challenge. Herein, a newly-designed Fe-g-C 3 N 4 /α-Fe 2 O 3 composite with an active N-Fe-O bridge was prepared by coupling Fe-doped g-C 3 N 4 (namely Fe-g-C 3 N 4 ) and α-Fe 2 O 3 . Interestingly, the combination of Fe-g-C 3 N 4 with α-Fe 2 O 3 broadened the light absorption region and restrained the photoinduced electron-hole pair recombination. Meanwhile, elaborate construction of N-Fe-O bridges based on coordination interaction can reduce electrochemical impedance and facilitate electron transfer, thereby prolonging the charge lifetime. As expected, the Fe-g-C 3 N 4 /α-Fe 2 O 3 composite displayed excellent photocatalytic performance in simultaneous removal of tetracycline (TC) and Cr(VI). More importantly, Fe-g-C 3 N 4 /α-Fe 2 O 3 -mediated electron transfer from TC to Cr(VI) also played an essential role on TC oxidation and Cr(VI) reduction under visible light. Both experimental analyses and theoretical calculations revealed that the migration route of photogenerated carriers followed a direct Z-scheme heterojunction mechanism under built-in electric field. The Fe-g-C 3 N 4 /α-Fe 2 O 3 composite with great stability also displayed promising practical application potential. In short, the current work not only provided a highly-efficient photocatalyst with N-Fe-O bridges but also shared new insights into the simultaneous removal of organic pollutants and heavy metals.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Chenjie Ding,Shifei Kang,Wenxin Li,Weikang Gao,Zhihao Zhang,Lulu Zheng,Lifeng Cui
Heterogeneous photo-Fenton catalysts prepared by doping metal ions in g-C 3 N 4 are promising alternatives to traditional homogeneous Fenton catalysts, but are restricted by poor mesoporous structure and agglomerate of metal species. Recently, the highly uniformly dispersed metal-N active sites in various photocatalysts have been proved to be the critical reason for their enhanced catalytic activity. In this study based on reasonable control of mesoporous structure and metal-N active sites, mesoporous Fe-g-C 3 N 4 was synthesized using a simple one-step thermal shrinkage polymerization method using ferrous oxalate as iron source and pore-forming agent. The Fe and N elements in the triazine ring skeleton of Fe-g-C 3 N 4 form a σ-π bond, thus the photogenerated electrons can be quickly transferred to Fe 3+ to form Fe 2+ under the interaction of chemical bonds, accelerating the Fenton reaction rate. Density functional theory calculations results demonstrate that the energy band structure and electron cloud density distribution of Fe-Nx active structure are better than that of routine FeOx crystal structure with metal species agglomeration. In addition, the excellent mesoporous structure of Fe-g-C 3 N 4 creates conditions for the high exposure of Fe-Nx active sites in the photo-Fenton reaction under visible light. The as-developed Fe-g-C 3 N 4 system shows high recyclability and excellent photo-Fenton performance for removal of typical intractable pollutants (The degradation rate of dye and tetracycline reaches 98.2% and 98.7% at 60 and 120 min, respectively). This work provides a facile and sustainable route to develop mesoporous highly-active heterogeneous Fenton-like catalysts and even further general the design of general catalyst with ideal metal-N active sites, thereby promoting a feasible and efficient wastewater remediation solution.
研究领域:
环境科学
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材料科学
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催化
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光化学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL PHYSICS LETTERS
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2025
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IF 3.1
Kangyue Qiao,Songyao Du,Yue Wang,Tongxin Xiao,Guodong Hao,Chao Sui,Yihan Yan
To address the severe Cr(VI) contamination in industrial wastewater, an NH 2 -MIL-101(Fe)/g-C 3 N 4 type-II heterojunction photocatalyst was synthesized via a solvothermal one-pot method. Structural characterization using XRD, SEM, XPS, and BET confirmed successful composite formation with high specific surface area and favorable interfacial contact. Photocatalytic experiments revealed that under conditions of pH = 2, a catalyst dosage of 20 mg, and an initial concentration of 10 mg/L, NM-101(Fe)/0.2CN achieved a 99.5 % reduction efficiency within 80 min. Its reaction rate constant was 3.6 times higher than that of NM-101(Fe) used alone. This study provides new insights for developing highly efficient MOF/polymer composite photocatalysts.
研究领域:
环境科学
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材料化学
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光催化
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废水处理
✓ 已验证
产品关联
DOI
高影响因子
Surfaces and Interfaces
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2024
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IF 5.7
Qian Cheng,Xiaohan Liu,Chuhan Huang,Hongman Sun,Fazle Subhan,Xinyi Zhou,Yuankai Liu,JiaHui Yang,Qi Li,Youhe Wang,Zifeng Yan
Recently, there has been a growing interest in the fundamental understanding of the mechanism of how MIL-101(Fe)/g-C 3 N 4 heterojunctions facilitate the occurrence of photocatalytic nitrogen fixation reactions, especially the electron transfer mechanism has attained increasing attention in photocatalysis. Herein, we implemented a "triple win scenario" strategy to fabricate the S-scheme MIL-101(Fe)/g-C 3 N 4 heterojunction through a straightforward solvothermal process. The MC-6 heterojunction minimizes the recombination of photogenerated carriers, enhances light utilization efficiency, and activates the N≡N bond, thus boosting photocatalytic nitrogen fixation efficiency. The transition metal iron activates the N≡N bond, while S-scheme heterojunctions reduce the photogenerated carrier recombination. In addition, the decrease in band gap (E g ) leads to an increase in visible light utilization efficiency. ISIXPS proved the mechanism of interelectron transfer of MIL-101(Fe)/g-C 3 N 4 heterojunction under illumination. Upon the creation of the heterojunction, electrons migrate from g-C 3 N 4 to MIL-101(Fe), establishing an inherent electric field due to the disparate Fermi levels between the two materials. The electrons (e - ) on the g-C 3 N 4 CB with a more negative reduction potential and the holes ( h + ) on the MIL-101(Fe) VB are retained, which increased the redox capacity to a great extent required for the reduction of N 2 to NH 3 . The ammonia production efficiency of MC-6 photocatalyst was 160 µmol g cat -1 h -1 , representing an 8-fold and 2.8-fold improvement over pristine g-C 3 N 4 (20 µmol g cat -1 h -1 ) and MIL-101(Fe) (57 µmol g cat -1 h -1 ), respectively.
研究领域:
材料科学
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环境科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）