LANGMUIR
·
2024
·
IF 3.7
Zhuangzhi Sun,Jiawei Lin,Suwei Lu,Yuhang Li,Tingting Qi,Xiaobo Peng,Shijing Liang,Lilong Jiang
The electrochemical nitrogen reduction reaction (eNRR) has emerged as a promising strategy for green ammonia synthesis. However, it suffers unsatisfactory reaction performance owing to the low aqueous solubility of N2 in aqueous solution, the high dissociation energy of N≡N, and the unavoidable competing hydrogen evolution reaction (HER). Herein, a MIL-53(Fe)@TiO2 catalyst is designed and synthesized for highly efficient eNRR. Relative to simple MIL-53(Fe), MIL-53(Fe)@TiO2 achieves a 2-fold enhancement in the Faradaic efficiency (FE) with an improved ammonia yield rate by 76.5% at −0.1 V versus reversible hydrogen electrode (RHE). After four cycles of electrocatalysis, MIL-53(Fe)@TiO2 can maintain a good catalytic activity, while MIL-53(Fe) exhibits a significant decrease in the NH3 yield rate and FE by 79.8 and 82.3%, respectively. Benefiting from the synergetic effect between TiO2 and MIL-53(Fe) in the composites, Fe3+ ions can be greatly stabilized in MIL-53(Fe) during the eNRR process, which greatly hinders the catalyst deactivation caused by the electrochemical reduction of Fe3+ ions. Further, the charge transfer ability in the interface of composites can be improved, and thus, the eNRR activity is significantly boosted. These findings provide a promising insight into the preparation of efficient composite electrocatalysts.
研究领域:
材料科学
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电化学
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催化化学
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Chen Li,Chuncai Zhou,David French,Ian T. Graham,Zixuan Wang,Yunfei Li,Feng Wang,Guijian Liu
As strategic emerging industries represented by clean energy technologies develop rapidly, gallium (Ga), one of the critical elements due to its use in these technologies and limited supply, has attracted worldwide attention. The discovery of appropriate materials to adsorb Ga is crucial for improving the utilization of Ga resources. With the goal to recover Ga ions more efficiently and selectively, carbon nanotubes (CNTs) and amino-functionalized MIL-53 series metal–organic skeletons were hydrothermally synthesized into CNT/NH2-MIL-53(Fe) composite adsorbents. The composite's morphology, structure, chemistry and other physicochemical features were characterized, and the adsorption conditions including pH, initial Ga concentration, along with adsorbent dosage were optimized. The outcomes suggest that 2-CNT/NH2-MIL-53(Fe) performs better than the unmodified material in adsorption, and the theoretical maximum adsorption amount of Ga is 1483.8 mg g−1. The adsorption exhibited a single layer chemisorption with an endothermic spontaneous reaction. The adsorption mechanism for Ga onto 2-CNT/NH2-MIL-53(Fe) was mainly via ion exchange and chelation, accompanied by hydrogen bond interaction. The outstanding adsorption capacity and reproducibility using CNT/NH2-MIL-53(Fe) composites provide a novel method for adsorbing Ga from aqueous solutions.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2024
·
IF 5.9
Fuhao Gan,Chunmei Gao,Shifeng Ji,Yunqing Xing,Tianming Gong,Lihui Tian,Yiming Bai,Zhuolong Wu
In this study, the iron-based metal–organic framework MIL-53(Fe) was successfully prepared by a solvent method and used as a photocatalyst for the efficient degradation of DDBAC under visible light. The morphology, structure and photocatalytic properties of MIL-53(Fe) were investigated by SEM, XRD, XPS and UV–vis DRS characterization methods. The optimum conditions for the degradation of DD pathways of DDBAC were analyzed in combination with DFT calculations. Based on molecular orbital theory and free radical quenching experiments, it was demonstrated that hydroxyl radicals were the main contributors in the oxidative degradation of DDBAC. The toxicity of DDBAC and its intermediates was evaluated by culturing Chlorella vulgaris, and the results showed that the Vis/MIL-53(Fe)/H 2 O 2 system was capable of solution detoxification.
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
ENERGY & FUELS
·
2021
·
IF 3.605
Jianwen Guo,Jiang Wu,Yu Guan,Jianmin Wang,Qizhen Liu,Xu Mao,Xuemei Qi,Ping He,Huaning Wang
A Z-scheme heterojunction polyhedral-shaped BiOIO3/MIL-53(Fe) photocatalyst is prepared by a solvothermal method. The samples are characterized by XRD, XPS, SEM, TEM, FT-IR, UV–vis, PL, and other material characterization analysis methods. The photocatalytic performance of photocatalysts is studied for removal of vapor-phase mercury (Hg0) under visible-light irradiation. The results suggest that the Hg0 removal efficiency of the BiOIO3/MIL-53(Fe) composite is significantly improved compared with that of MIL-53(Fe). When the molar ratio of BiOIO3 and MIL-53(Fe) is 2:1, the BiOIO3/MIL-53(Fe) composite photocatalyst exhibits the best Hg0 removal efficiency, reaching 74.19%. BiOIO3 and MIL-53(Fe) form a Z-scheme heterojunction with a suitable energy band structure, which results in the effective separation of photoinduced electron–hole pairs and delays their recombination. Finally, the photocatalytic oxidation mechanism of Hg0 by the BiOIO3/MIL-53(Fe) composite is proposed, which paves the way for the study of the built-in electric field and electron transport channels between binary photocatalyst materials.
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
ACS Applied Nano Materials
·
2024
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IF 5.3
Baixin Liu,Xuelian Chen,Guojuan Hai,Wenwen Zhao,Kai Li,Zhicong Yuan,Xiaoyong Zhang
The design and synthesis of metal–organic frameworks (MOFs) for direct use as electrode materials are crucial for enhancing the electrocatalytic oxygen evolution reaction (OER). Herein, the ultrathin MIL-53(Fe) nanosheet arrays with enriched coordinatively unsaturated metal sites (denoted as MIL-53(Fe)/NF-B0.2-2) are obtained under the inhibition and modulation of benzoic acid (BA) ligands via a substitution-suppression process. The results confirm that this unique ultrathin structure effectively increases the electrochemical active surface areas (ECSA) and exposes the coordinatively unsaturated metal sites. More importantly, the enriched coordinatively unsaturated metal sites acting as active sites facilitate the adsorption of OH– during the OER process. Additionally, MIL-53(Fe)/NF-B0.2-2, with its optimized energy band structure, exhibits superior charge transfer ability and diffusion processes, significantly improving the reaction kinetics in alkaline electrolytes. As a result, the MIL-53(Fe)/NF-B0.2-2 electrode only requires extremely low overpotentials of 190 and 229 mV to reach current densities of 10 and 100 mA cm–2 for OER, respectively. This research not only proposes a novel strategy for designing efficient electrocatalysts but also provides insights into the structure–activity relationship, advancing the rational design of MOFs as effective electrode materials.
研究领域:
材料科学
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电化学
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能源催化
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产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2020
·Vol. 31
·期 6
·4822-4835
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IF 2.22
Zhou Nan,Tan Junjie,Li Xi,Wang Lu,Jin Chenglong,Chen Ming,Yu Zhengsong,Liang Yani,Qiu Zhidong,Li Wenlong,Dong Yulin,Xie Zhizhong,Lin Yawei,Qu Deyu,Zhang Chaocan
A series of Bi 5 O 7 I/MIL-53(Fe) (BOI/MIL- w ) composites were successfully prepared by a facile in-situ solvothermal approach. The matched energy bands enabled Bi 5 O 7 I and MIL-53(Fe) to form a Z-scheme heterojunction which resulted in an efficient separation of the photo-induced electron–hole pairs. The photocatalytic activity of BOI/MIL- w was evaluated by the degradation of Rhodamine B (RhB) in water under the visible light irradiation. Compared with Bi 5 O 7 I, photocatalytic performances of BOI/MIL- w notably boosted. When the content of added MIL-53(Fe) was 3 wt%, BOI/MIL-3 presented the highest activity with a degradation efficiency of 99.7% only after 60 min of irradiation. The reaction rate constant k could reach 0.0992 min −1 which was nearly 12.6 times as high as that of Bi 5 O 7 I. Moreover, BOI/MIL- w had a good stability and reusability, which could ensure its practical application. Trapping experiments confirmed that h + and ·O 2 − were the dominant active species during the photocatalytic process, and further demonstrated the formation of the Z-scheme heterojunction facilitated the photocatalytic performance of BOI/MIL- w .
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2019
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IF 3.261
Shengchao Miao,Zhenxing Zha,Ying Li,Xinxiang Geng,Jiahui Yang,Shihai Cui,Jing Yang
The novel semiconductor heterojunction of MIL-53(Fe)/BiOCl composite was first prepared through the solvothermal reaction. The prepared materials were characterized by Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), Brunner-Emmet-Teller (BET) and ultraviolet-visible diffuse reflectance spectroscopy (DRS). MIL-53(Fe)/BiOCl heterojunction is a kind of photoexcited materials and it accelerates the photoreactivity of BiOCl under the visible light irradiation. It was used to remove Rhodamine B (RhB) with the existence of persulfate (PS). The UV–vis spectrophotometer and the TOC detector show that the degradation rate and TOC removal efficiency of RhB (20 mg/L) are 99.5% and 69.4%within 30 min visible-light irradiation, respectively. Due to the proper band gap of material and the presence of electron acceptor, PS, the survival time of active radicals are increased. The active species h + , ·SO 4 − and ·OH are found to play the important roles during the reaction system. The possible mechanism for the RhB degradation of MIL-53(Fe)/BiOCl/PS is also proposed. Furthermore, the results of the material reusability for the degradation of RhB indicate that the MIL-53(Fe)/BiOCl has a good stability and can be used in the environmental water sample treatment.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 17
·8334-8346
·
IF 3.3
Peifu Sun,Xiao Zhang,Zhiren Guo,Xinyue Liu,Yuanming Lan,Dongxiang Zhang,Hansheng Li,Jinying Li,Helei Liu,Xiyan Xu
The excessive discharge of isothiazolinone bacteriostatic agent-containing wastewater has posed serious threats to human health and environmental safety. As 1,2-benzisothiazolin-3-one (BIT) is one of the most commonly used isothiazolinones, its effective degradation is necessary and urgent. In the current study, a NH2-MIL-53(Fe)-based adsorptive photo-Fenton-like system was constructed for efficiently adsorbing and photodegrading BIT under solar light. The equilibrium BIT adsorption capacity Qe of NH2-MIL-53(Fe) reached 1140.89 mg g−1. The adsorptive photo-Fenton-like system has achieved more than 90% removal of BIT using NH2-MIL-53(Fe) in the presence of H2O2 under solar light irradiation, and the band gap of NH2-MIL-53(Fe) was calculated by UV-Vis analysis to be 2.10 eV. The influences of pH, dosage of photocatalysts and H2O2 were also assessed. It was found that H2O2 reduced the recombination of electron–hole pairs, and the radical quenching experiments and EPR testing result confirmed that h+, ˙OH and O2˙− played a crucial role in the photocatalytic process. This study supports the application of Fe-based MOF materials for simultaneous adsorption and the solar light photocatalytic degradation of BIT.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Hailin Tian,Tirusew Araya,Ruiping Li,Yanfen Fang,Yingping Huang
Microcystin-LR (MC-LR), which is produced from cyanobacteria, is the common microcystin with a serious threat to aquatic life and human beings. And the efficient removal method of MC-LR is urgent needed. In this work, the MIL-100/MIL-53 (Fe) photocatalysts, which were successfully prepared by the electrostatic interaction with each other, were applied for the photocatalytic degradation of MC-LR. The structure and optical properties of the MIL-100/MIL-53 (Fe) photocatalysts were characterized by using SEM, XRD, XPS, FT-IR and UV–vis DRS. The very low dosage of the MIL-100/MIL-53 (Fe) photocatalysts achieved the degradation of MC-LR, and the optimized loading was the 50% MIL-100/MIL-53 (Fe) photocatalyst. Compared to MIL-100 (Fe) and MIL-53 (Fe), the MC-LR degradation was up to 96.5% after 3 h under visible light illumination with the 50% MIL-100/MIL-53 (Fe) photocatalyst due to the pore-effect adsorption and the effective separation of photogenerated carriers. The effect of coordinate immobilized layers between MIL-100 (Fe) and MIL-53 (Fe) contributed to the stable and efficient removal of MC-LR for the 50% MIL-100/MIL-53 (Fe) photocatalyst. The MC-LR photocatalytic mechanism and degradation pathway, which the photogenerated holes (h + ) were the main active species, were proposed by radical capture experiments and LC-MS analysis.
研究领域:
环境科学
·
生物学
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2021
·Vol. 56
·期 28
·15782-15797
·
IF 4.22
Jiang Danni,Zhou Yu,Wang Ping,Huang Chao,Zhu Jian,Liu Zhiming
In the MOFs-based composites, the co-catalyst nanoparticles loads tend to agglomerate. In the self-assembly process of MOFs-based composites, the use of acid modulators solved the accumulation of AgI nanoparticles cocatalyst. The active sites of carboxyl groups and mesoporous structure brought by acid modulator provide more loading sites for AgI nanoparticles. The novel AgI/D-MIL-53(Fe) showed good adsorption and photocatalytic performance in the process of removing tetracycline pollutants. Compared to the degradation efficiency of the MIL-53(Fe) with 50.8%, it of AgI/MIL-53(Fe) increased to 85.1% and which further increased to 96.2% by AgI/D-MIL-53(Fe) based on the HCl modulator. On the one hand, it is beneficial for the mesoporous D-MIL-53(Fe) modulated by HCl modulator to disperse the AgI nanoparticles co-catalyst. On the other hand, AgI nanoparticles, as a photosensitive agent, adsorb visible light to generate photogenerated electrons and holes, and electrons rapidly transferred to the heterojunction bridge Ag 0 and then captured by the holes from the D-MIL-53(Fe). The construction of AgI/D-MIL-53(Fe) Z-scheme heterojunction provided favorable conditions for the rapid separation and photogenerated electrons and holes. Finally, ·O 2 − , ·OH and h + as the main active free radicals were driving forces. This study provided more possibilities and opportunities for the construction of mesoporous MOFs-based composites.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
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 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
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废水处理
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）