ACS Applied Materials & Interfaces
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2022
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IF 10.383
Qiufan Sun,Yuxiang Zhu,Xiang Zhong,Meng Jiang,Yanchen Fan,Jianfeng Yao
In this work, MIL-68(In) functionalized with various ligand substitutions including amine, hydroxyl, bromine, nitro, and methyl groups was prepared, via a one-pot solvothermal reaction for visible-light photocatalytic ammonia synthesis. The diversity of ligands tunes the morphology, geometry, pore environment, and electronic structure of MIL-68(In)-based photocatalysts due to the polarity and intraframework interactions. Amine-inserted MIL-68(In) outperforms its counterparts, presenting a boosted nitrogen photofixation rate of 140.34 μmol gcat–1 h–1 with an apparent quantum efficiency of 5.69% at 420 nm. Further, the size of the batch solvothermal reactor and the amine group content also influence the photocatalytic activity. The combined experimental and theoretical results reveal that amine substituents improve the chemisorption of nitrogen molecules and the conversion of nitrogen into ammonia follows a dual pathway, i.e., a Mars–van Krevelen process and a ligand-to-metal charge transfer mechanism. This work provides a molecular engineering strategy via dual catalysis toward efficient ammonia production.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
PubMed
高影响因子
RARE METALS
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2025
·
IF 11
Wang Dan-Dan,Xu Meng-Yang,Lin Zhao-Xin,Wu Jia-Hui,Yang Wei-Ting,Li Hong-Ji,Su Zhong-Min
The goal of photocatalytic CO 2 reduction is to obtain a single energy-bearing product with high efficiency and stability. Consequently, constructing highly selective photocatalysts with enhanced surface and optoelectronic properties is crucial for achieving this objective. Here, we have developed a simple one-pot vulcanization method to synthesize a MIL-68(In)-derived CdIn 2 S 4 /In 2 S 3 heterojunction that exhibited stable and high selectivity. Multiple characterizations of the CdIn 2 S 4 /In 2 S 3 heterojunction revealed a hierarchical tubular structure with numerous surface reactive sites, a high visible-light utilization rate ( λ < 600 nm), efficient charge separation, and a prolonged charge-carrier lifetime. Moreover, an S-scheme charge transfer mechanism, based on the interleaved band between the two components, improved the reduction capability of the electrons. Benefiting from the compositional and structural synergy, the yield CO by CdIn 2 S 4 /In 2 S 3 -250 (CI-250) reached 135.62 μmol·g −1 ·h −1 , which was 49.32 times and 32.88 times higher than that of In 2 S 3 and CdIn 2 S 4 , respectively. The CdIn 2 S 4 /In 2 S 3 heterojunction exhibited a quantum efficiency of 4.23% with a CO selectivity of 71%. Four cycle tests confirmed the good stability and recyclability of the CI-250. This work provides a new approach for designing and preparing high-performance hollow MOFs-based photocatalysts for scalable and sustainable CO 2 reduction.
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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DOI
高影响因子
JOURNAL OF POROUS MATERIALS
·
2021
·Vol. 29
·期 1
·181-192
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IF 2.496
Wang Li,Zhou Yu,Xu Qi,Wu Xian-Kun,Xu Guo-Dong,Guo Ji-Xiang,Fang Dong
The development of high efficient and cost-effective photocatalysts for organic matters degradation and hydrogen evolution is of great importance. In this study, heterojunction photocatalysts based In 2 S 3 and MIL-68(In) were synthesized by hydrothermal method. These composites exhibit excellent bi-functionality of photocatalytic Rhodamine B degradation and hydrogen evolution. And it was found that the photocatalytic performance of the composites was dependent on the ratio of In to S. The optimum catalyst In 2 S 3 /MIL-68(In)-1.5 exhibits much enhanced photocatalytic performance, offering a removal efficiency of 94.7% within 30 min for 20 ppm of Rhodamine B and a hydrogen evolution rate of 1618.8 µmol h −1 g −1 as a result of the synergist effect of heterojunction between the two components, promoting the charge separation. Besides, the mechanisms for photocatalytic degradation of Rhodamine B and photocatalytic hydrogen evolution were also proposed. This protocol could provide guiding information on the development of other functional photocatalysts.
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
高影响因子
ACS Applied Materials & Interfaces
·
2024
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IF 8.3
Yiling Wu,Kaiji Xu,Jian Tian,Longmei Shang,Kok Bing Tan,Hao Sun,Kang Sun,Xiaoping Rao,Guowu Zhan
The efficient and economic conversion of CO2 and renewable H2 into methanol has received intensive attention due to growing concern for anthropogenic CO2 emissions, particularly from fossil fuel combustion. Herein, we have developed a novel method for preparing Ni/In2O3 nanocatalysts by using porous MIL-68(In) and nickel(II) acetylacetonate (Ni(acac)2) as the dual precursors of In2O3 and Ni components, respectively. Combined with in-depth characterization analysis, it was revealed that the utilization of MIL-68(In) as precursors favored the good distribution of Ni nanoparticles (∼6.2 nm) on the porous In2O3 support and inhibited the metal sintering at high temperatures. The varied catalyst fabrication parameters were explored, indicating that the designed Ni/In2O3 catalyst (Ni content of 5 wt %) exhibited better catalytic performance than the compared catalyst prepared using In(OH)3 as a precursor of In2O3. The obtained Ni/In2O3 catalyst also showed excellent durability in long-term tests (120 h). However, a high Ni loading (31 wt %) would result in the formation of the Ni-In alloy phase during the CO2 hydrogenation which favored CO formation with selectivity as high as 69%. This phenomenon is more obvious if Ni and In2O3 had a strong interaction, depending on the catalyst fabrication methods. In addition, with the aid of in situ diffuse reflectance infrared Fourier transform spectroscopy and density functional theory (DFT) calculations, the Ni/In2O3 catalyst predominantly follows the formate pathway in the CO2 hydrogenation to methanol, with HCOO* and *H3CO as the major intermediates, while the small size of Ni particles is beneficial to the formation of formate species based on DFT calculation. This study suggests that the Ni/In2O3 nanocatalyst fabricated using metal–organic frameworks as precursors can effectively promote CO2 thermal hydrogenation to methanol.
研究领域:
催化化学
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材料科学
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环境科学
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DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Jun He,Xiaoyu Qi,Jingjing Liu,Hao Zhang,Zhongliao Wang,Deliang Li,Shuwang Duo
Triethylamine is a typical volatile toxic gas that can cause respiratory system diseases, blood diseases, and eye lesions upon prolonged inhalation. To mitigate this problem, a highly sensitive triethylamine sensor was achieved by loading the precious metal Au onto hexagonal hollow prisms of In 2 O 3 . Prominently, the microstructure of the hollow hexagonal prisms was derived from Material Institute Lavoisier(MIL)-68(In), which provided a larger specific surface area and more active sites. The sensing test results manifested that the sensor based on 0.6% Au/In 2 O 3 owned the best sensing performance among all samples, especially with the response value of 476.3 ( R a / R g ) towards 100 ppm triethylamine at 200°C, which was 37 times higher than that of pristine In 2 O 3 sensor. Additionally, the stability deviation value was less than 5.6% and the selectivity ( Response triethylamine / Response ethanol ) reached up to 28.8. Such distinguished characteristics can be attributed to the delicate hollow hexagonal prisms structure and the decoration of Au, which accelerated gas molecules transport and enhanced oxygen molecule adsorption and dissociation. This work may open up new visas for morphology manipulation of triethylamine sensing materials and intrinsic mechanism of performance enhancement.
研究领域:
材料科学
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传感器技术
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环境监测
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DOI
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
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IF 4.831
Ning Wu,Hao Guo,Mingyue Wang,Liping Peng,Yuan Chen,Bingqing Liu,Zhilan Pan,Yinsheng Liu,Wu Yang
Ratio fluorescence has attracted much attention because of its self-calibration properties. However, it is difficult to obtain suitable fluorescent materials with well-resolved signals simultaneously under one excitation. In this work, we report a different strategy, using MIL-68(In)-NH 2 as both the fluorescence element and the scattered light unit, and coupling the fluorescence and the scattered light to construct the fluorescence and scattered light ratio system. Based on the optical properties and the second-order scattering (SOS) of the material nanoparticles , the synthesized MIL-68(In)-NH 2 can be used to realize the ratio detection of Hg 2+ . Because the scattering intensity of small particle MIL-68(In)-NH 2 is weak, SOS is not obvious. When Hg 2+ is introduced the coordination reaction between the amino nitrogen atoms of MIL-68(In)-NH 2 and Hg 2+ make the particles larger, resulting in the decrease of fluorescence and the enhancement of SOS. As a result, a novel Hg 2+ ratiometric detection method is developed by using the dual signal responses of the fluorescence and scattering. Under the optimal conditions (pH = 6, reaction time 5 min, room temperature , and the maximum excitation wavelength 365 nm), the linear range of the method is 0–100 μM, and the detection limit is 5.8 nM (Ksv = 9.89 × 10 9 M −1 ). In addition, the probe is successfully used to evaluate Hg 2+ in actual water samples. Compared with the traditional method of recording only the fluorescence signal, the proposed fluorescence-scattering method provides a new strategy for the design of ratiometric sensors.
研究领域:
材料科学
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分析化学
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环境科学
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产品关联
DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Ning Sui,Yifeng Xu,Peng Zhang,Shuang Cao,Tingting Zhou,Tong Zhang
The crucial challenge to exploit effective ozone (O 3 ) gas sensors lies in developing novel functional sensing materials to meet the requirement of trace-level detection threshold (50 ppb). Metal oxide semiconductors (MOSs) with controllable heterogenous composites as high-performance sensing layers are expected to break through this bottleneck. This work proposes the hybridization of MIL-68 (In) and ZIF-8, which are employed as dual metal organic frameworks (MOFs) sacrificial templates to design n-n heterostructures . The derived In 2 O 3 backbone showed a hexagonal prismatic structure with a large aspect ratio. The robust architecture enabled the uniform decoration of mass of ZnO nanoparticles (NPs) on the surfaces without the damage of high porosity for the gas diffusion. Consequently, the optimal sensor with appropriate ZnO NPs loading amount exhibited trace O 3 detection ability as low as 15 ppb, which was attributed to the smart design of n-n heterostructure, rich active sites and improved oxygen-adsorbing capacity. Thus, this work inspires a new way to utilize the versatile dual MOFs template for constructing heterogenous composites as O 3 sensing materials.
研究领域:
材料科学
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传感器技术
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环境监测
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Yan Jiang,Ping Wang,Ji Li,Xianfa Zhang,Yingming Xu,Hui Zhao,Xiaoli Cheng,Shan Gao,Lihua Huo
The porous and tubular structure is conducive to improving performance of sensing materials. At present, how to obtain sensitive materials with unique porosity and high surface activity by green, low-cost and simple synthesis methods is still a challenge. In this work, novel In 2 O 3 porous microtubes were obtained by water etching of MIL-68-In and calcination methods for the first time. The as-prepared microtubes exhibit excellent NO 2 sensitivity at 50 ℃ (S=156–3 ppm NO 2 ), and the limit of detection is 50 ppb. The sensor also has good NO 2 detection ability in the actual environment. The excellent NO 2 sensing performance at low temperature is closely related to high surface activity of In 2 O 3 porous microtubes. Combined with TPD, in-stiu DRIFT and XPS technologies, the NO 2 sensing mechanism was detailed analyzed. This work provides useful guidance for constructing high performance NO 2 sensor. The excellent NO 2 sensing performance at low temperature makes a positive contribution to promoting the application of metal oxide sensors in environmental detection.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Boyi Yan,Zhongqiao Sun,Yide Han,Hao Meng,Xia Zhang
The construction of a tightly contacted heterojunction consisting of multi-components is proven to be one of the effective strategies to promote the photogenerated charges separation and to develop high-efficient photocatalysts in hydrogen evolution . Herein, a ternary hollow heterostructure of ZnS/ZIS/In 2 S 3 has been fabricated by using a binary MOF@MOF (ZIF-8@MIL-68(In)) as the precursor, and an in-situ sulfurization of ZIF-8@MIL-68(In) is controlled to optimize the photocatalytic performances. The resulting samples are signed as Z@M- t , where the t is pointed to the sulfurization time being varied from 4 h to 48 h. It’s shown that the hierarchical and hollow architecture is formed for Z@M- t , and with the reinforced light harvest ability in both UV and visible light regions. In the subsequent visible-light-induced photocatalytic hydrogen generation, the optimized Z@M-24 manifests significantly improved hydrogen evolution rate of 607.34 μmol g -1 h −1 , which values are evidently higher than that by the single MOF and binary ZIF-8@MIL-68(In) heterostructure. The electrochemical analyses and the electron paramagnetic resonance (EPR) spectrum were analyzed to clarify the charge transfer routes and the enhanced photocatalytic mechanism, in which the contribution of each metal sulfide is also discussed. Finally, the good photocatalytic stability and reusability of Z@M-24 heterostructure are also represented, which define the structure superior brought by the effective heterojunction based on the in-situ sulfurization strategy of binary ZIF-8@MIL-68(In), and determine their prospect applications in the efficient H 2 production under visible light irradiation.
研究领域:
材料科学
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化学
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光催化
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
CELLULOSE
·
2022
·Vol. 29
·期 2
·1017-1034
·
IF 6.123
Sun Lijian,Qian Xueren,An Xianhui
Cellulose-based bioplastics with degradability and remarkable mechanical performance have recently attracted increasing attention. As a high-performance material, cellulose-based bioplastics have a strong potential to replace synthetic plastic substrates in many applications. However, its poor shielding performance to UV light limit its application. In this work, transparent and UV-blocking MIL-68(In)-NH 2 @cellulose bioplastic (M(In)CBP) sheets are fabricated via a featured processing method, i.e., cellulose liquefaction, rapid solidification, in-situ synthesis and hot-press drying. The as-obtained functional bioplastic sheet (M(In)CBP1) exhibits high visible-light transparence (74.7% a 600 nm) and the existence of MIL-68(In)-NH 2 allows superior UV-blocking ability (below 400 nm, transmittance was under 4%). The M(In)CBP sheets show high photostability even after continuous UV irradiation (365 nm) for over 12 h. The superior UV-shielding performance is attributed to the uniform distribution and the high UV absorbance of MIL-68(In)-NH 2 in M(In)CBP sheets. High resistance to penetration by aqueous/nonaqueous liquids was proved. Moreover, the M(In)CBP sheets also show excellent mechanical properties and thermal stability. The present work designed a UV-blocking bioplastic constructed from cellulose and MIL-68(In)-NH 2 , which is potential candidates to replace synthetic plastics in many advanced applications such as a UV protection layer for electronic products, or useful as packaging materials to prevent food spoilage. Graphical abstract
研究领域:
材料科学
·
环境科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Wei Zhao,Mengru Yan,Xinran Yang,Xiaojun Zeng,Yantong Chen,Benlin Dai,Xiaozhong Chu,Xuekun Hong,Feihu Mu,Shijie Li,Dennis Y.C. Leung
Environmental pollution caused by the overusage and uncontrolled discharge of antibiotics such as amoxicillin will endanger public health and ecosystems. Herein, a novel Ag/MIL-68(In)-NH 2 /Bi 4 O 7 plasmonic heterojunction has been successfully prepared through a two-step route followed by photoreduction for environmentally friendly photocatalytic amoxicillin degradation. Ag/MIL-68(In)-NH 2 /Bi 4 O 7 displayed the most efficient photocatalytic performance, which was 3.7 and 3.2 times that of Bi 4 O 7 and MIL-68(In)-NH 2 , respectively. The superior photocatalytic activity was directly linked to its large surface area and localized surface plasmon resonance (LSPR) effect, which provides more active sites and effectively promotes visible light absorption. Moreover, the degradation path of amoxicillin was explored in detail by combining Gaussian software calculation with liquid chromatography-mass spectrometry (LC-MS) analysis. Finally, a series of characterizations and simulations were carried out to demonstrate the S-scheme photocatalytic mechanism.
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
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Jiamin Wei,Qing Wang,Mian He,Shuai Li,Yunan Zhang,Yang Yang,Shipeng Luo,Lianshe Fu,Xin Wang,Tinghai Yang
The development of highly efficient strategy to facilitate comprehensive charge transmission and effective spatial charge separation is expected as a promising approach to improve photocatalytic performance. Herein, the Fe(III) doping modified AgI/NH 2 -MIL-68(In/Fe) Z-scheme heterojunction (ANM-x composite) with unique internal and interfacial charge transmission performance was fabricated by a facile ion exchange precipitation method. The optimized ANM-50 composite exhibits the maximum photocatalytic activity for the degradation of tetracycline, which is about 9.54, 2.61 and 1.86 times higher than that of pure NH 2 -MIL-68In, NH 2 -MIL-68(In/Fe) and AgI, respectively. The characterization results displayed that Ag nanoparticles (NPs) were generated during the photocatalytic procedure, which not only served as a charge transfer-highway, but also reduced the charge flow energy barrier, thereby accelerating charge transfer efficiency and consolidating the stability of the Z-scheme heterojunction. Mechanism exploration reflected that the superior photocatalytic performance was associated with synergetic effect among the introduced Fe(III), constructed ANM Z-scheme heterojunction and the generated Ag NPs, which significantly expands visible light response range and promotes more effective internal and interfacial charge separation. This research not only designs an efficient photocatalyst for decomposing tetracycline, but also opens a new perspective for rational developing Z-scheme heterojunction with unique internal and interfacial charge flow steering.
研究领域:
材料科学
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环境科学
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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）