Surfaces and Interfaces
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2024
·
IF 5.7
Yanping Zhang,Yinian Zhu,Yinming Fan,Shengpeng Mo,Xiaobin Zhou,Zongqiang Zhu
A set of MOFs-derived Co 3 O 4 @MnO x hollow-sphere were synthesized to develop a catalyst for the photothermal catalytic removal of NO using acetone as a reducing agent. The study systematically investigated the impact of organic ligands and photoactive substances on energy transfer and photothermocatalytic reactions involving acetone and NO under 5 vol % H 2 O with the catalysts. At 240°C, sample C-5/1 (with an organic ligand added and Co/Mn molar ratio of 5/1) demonstrated 75 % NO conversion and 65 % acetone conversion. The highest catalytic performance was observed in the L-Py sample (with photoactive substance was added), achieving 80 % NO and 69 % acetone conversion at 240°C. The catalyst demonstrated low crystallinity, and the introduction structural defects through ligands adjusted the ratio of active components. Meanwhile, enhanced catalytic performance was attributed to light energy scattering in the inner space of microspheres, resulting in the efficient transfer of 2.17 eV energy with the addition of two photoactive substances. The elevated concentration of surface-active oxygen facilitated oxidation, while M n /M n+1 (Mn 3+ /Mn 4+ and Co 2+ /Co 3+ ) redox cycling supplied surface oxygen in the photothermal low-temperature response. The proposed mechanism for the simultaneous degradation of acetone and NO was elucidated using Density Functional Theory calculations.
研究领域:
环境科学
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材料科学
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催化化学
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Ruolan Li,Xingyan Liu,Yacen Tang,Jianning Yu,Ya Chen,Min Fu,Siqi Li,Youzhou He
In this study, a highly efficient bifunctional porphyrin-based MOFs with uniformly in-situ generated g-C 3 N 4 quantum dots (g-CNQDs) was fabricated for photocatalytic hydrogen evolution and NO removal, in which PtTCPP as the organic ligand and mixed Zr/Ti-oxo clusters as the metal nodes. Compared with most reported Zr-based porphyrin MOFs, the g-CNQDs@Zr-MOFs(Pt)(Zr/Ti) exhibited outstanding hydrogen evolution activity (14511.57 μmol g −1 ) and NO removal rate (31.9 %) under visible light irradiation. The obviously improved photocatalytic performance could be attributed to the significantly enhanced charge separation and transfer rates by the mixed Zr/Ti-oxo clusters via the rapid Ti 3+ /Ti 4+ process. Moreover, the uniformly in-situ generated g-CNQDs via confinement effect in the cavity of MOFs could also improve the utilization of visible light especially through the up-conversion effect, and promote charge carriers separation. This work provides an idea for us to expand the scope of light utilization and promote charge transfer and separation rates of MOFs via functionalizing host MOFs matrix and coupling guest active species to improve photocatalytic performance further.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Longlong Liu,Zunpeng Hu,Minghui Wang,Jinliang Ma,Zihao Chen,Xin Ning,Ding Yuan
The construction of a hybrid hierarchical architecture is a promising strategy for optimizing the electrocatalytic activity and the performance of flexible Zn-air battery. However, it still remains a challenging task. This study reports on the use of a simple approach in the preparation of a flexible 3D self-supporting bifunctional catalyst. Ultrathin NiFe-based layered double hydroxide nanosheets (NiFe-LDH) have in this approach been strongly coupled to a metal-organic framework (MOF)-derived carbon nanoflake array, to be used in flexible Zn-air batteries. Importantly, the introduction of Co nanoparticles that were anchored onto the nitrogen-doped porous carbon (Co-NC) nanoflakes provided an abundance of active sites for the oxygen reduction reaction (ORR). Moreover, the catalytic oxygen evolution reaction (OER) process was improved by altering the local electronic structure of the Ni and Fe species in NiFe-LDH. The 3D interconnected conductive network structure, in addition to the strong coupling between NiFe-LDH and Co-NC, was found to give a catalyst with superior electrocatalytic OER performances. The overpotential was only 284 mV at 50 mA cm −2 in an alkaline medium, which is a result that outperforms the commercial RuO 2 catalyst. This bifunctional catalyst did also exhibit a good catalytic performance that is comparable to that of commercial Pt/C towards ORR. Interestingly, when this catalyst was used as binder-free air cathode, the assembled flexible solid-state Zn-air battery demonstrated a favorable power density, cycling stability, and mechanical flexibility. The present work offers a facile and efficient strategy for the development and construction of self-supporting bifunctional OER/ORR electrocatalysts , to be used in wearable and flexible electronic devices.
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Nanoscale
·
2021
·Vol. 13
·期 16
·7801-7809
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IF 7.79
Wanguo Gao,Xiaoman Li,Xu Zhang,Senda Su,Shijian Luo,Rong Huang,Yuan Jing,Min Luo
The vacancies of semiconductors have proven to be effective active sites for photocatalytic nitrogen fixation, but what about the role of defects in MOF materials? Herein, we report the first UiO-66 with photo-excited cluster defects and linker defects for photocatalytic nitrogen fixation. It was determined through the post-synthetic ligand exchange (PSE) process that the linker defects, rather than cluster defects, can greatly improve the performance, which is due to linker defects forming unsaturated metal nodes such as the vacancy in a semiconductor. Specifically, for photo-activated UiO-66, the NH4+ production rate was 196 and 68 μmol g−1 h−1 in air atmosphere under ultraviolet-visible (UV-Vis) and visible light, respectively. This report provides a new effective strategy to design efficient nitrogen fixation photocatalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Jing Xia,Yanxin Gao,Gang Yu
The adsorptive removal of tetracycline (TC) was studied with three types of zirconium-based metal–organic frameworks (Zr-MOFs), UiO-66, NU-1000 and MOF-525. The adsorption kinetics best fitted with the pseudo-second-order kinetic model and the adsorption equilibrium was rapidly reached within 40 min on UiO-66 and NU-1000, and 120 min on MOF-525. The adsorption isotherms best fitted with Sips model, and the maximum Sips adsorption capacities of TC on UiO-66, NU-1000 and MOF-525 were 145 mg·g −1 , 356 mg·g −1 and 807 mg·g −1 respectively, which were much higher than common adsorbents. The X-ray photoelectron spectra measurements and the influence of pH suggested that the π-π interaction played a crucial role during the adsorption. Pore characteristics and topology of MOFs showed great effect on adsorption performance. The cages whose size match well with TC helped MOF-525 to get highest adsorption amount per surface area among MOFs we studied. The proper topology of NU-1000 contributed to its high adsorption rate. River water was also used to confirm the excellent adsorptive performance of these three Zr-MOFs in practical application. These results might aid us to comprehend the adsorption of TC on Zr-MOFs and expand the application of Zr-MOFs in water treatment for removal of emerging contaminants.
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Journal of Advanced Research
·
2020
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IF 6.992
Tengfei Li,Meng Lu,Yuhang Gao,Xiaodong Huang,Guangyang Liu,Donghui Xu
In this study, a novel metal-organic framework (M-ZIF-8@ZIF-67) was successfully prepared using the single layer Fe 3 O 4 -ZIF-8 as magnetic core and wrapped a layer of ZIF-67 outer. This M-ZIF-8@ZIF-67 was employed as an adsorbent for the adsorption and removal of fipronil and its metabolites from environmental water and cucumber samples. The characterization results suggested that M-ZIF-8@ZIF-67 has the double layer structure a polyhedral structure with uniform pores, while ZIF-67 was successfully coated on the surface of Fe 3 O 4 -ZIF-8. The unique structure endowed M-ZIF-8@ZIF-67 a high surface area (219 m 2 /g) and high adsorption capacity for fipronil, fipronil desulfinyl, fipronil sulfide and fipronil sulfone. To our knowledge, this is the first report detailing the adsorption properties of M-ZIF-8@ZIF-67 with double layer structure relating to the adsorption and removal of pesticides. Furthermore, the adsorption model analysis demonstrated that the static adsorption data fitted the Freundlich bimolecular layer adsorption model better than the Langmuir monolayer adsorption model. This study indicates that M-ZIF-8@ZIF-67 has significant potential in the adsorption and removal of fipronil and its metabolites in water and vegetable samples.
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Molecular Catalysis
·
2019
·
IF 2.938
Xuewei Li,Tianqinji Qi,Jing Wang,Wei She,Guijie Mao,Pengfei Yan,Weizuo Li,Guangming Li
Rational design and development of stable nitrogen-doped carbon supported non-noble metal based nanocatalysts with unique natures of active species and support for highly chemoselective hydrogenation of nitroarenes to arylamines remains a grand challenge. Here, firstly, an N, Fe-containing metal-organic frameworks (MOFs) has been designed and synthesized. Furthermore, an efficient N-doped carbon fiber supported FeO x -based nanocatalyst (FeO x @CN- hpes ) was prepared via pyrolysis of MOF@polymer composite towards electrospun nanofiber crosslinked N, Fe-containing MOFs. Remarkably, the developed FeO x @CN- hpes enables the hydrogenation of nitrobenzene to aniline with unprecedented performance (215.8 h −1 ) compared to those of FeO x @CN- hp (176.2 h −1 ) and FeO x @CN- pes (45.2 h −1 ) catalysts prepared by conventional approaches. The comparative characterizations have revealed that the high dispersion of FeO x species, enhanced basicity, and more structural defects and Fe-N x species towards FeO x @CN- hpes are responsible for the high performance. Moreover, the effect of the pyrolysis temperature towards FeO x @CN- hpes on the performance of hydrogenation reaction was also systematically investigated. The results indicated that the FeO x @CN- hpes -400 catalyst prepared at 400 °C was identified as the best hydrogenation catalyst. More importantly, the FeO x @CN- hpes -400 catalyst exhibited excellent activity and exclusive selectivity for the hydrogenation of functionalized nitroarenes to corresponding arylamines, as well as successive recyclability without any loss in both activity and selectivity. Therefore, this work provides a feasible strategy for the synthesis of other heterogeneous MOFs-based derived catalysts with superior catalytic performance for diverse industrial processes.
研究领域:
催化化学
·
材料科学
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Yukun Yang,Xiaoxing Zeng,Yu Tian,Xiaomin Wang,Xu Jing,Ligang Yu,Baoqing Bai,Jinhua Zhang,Shu Qin
A universal design of turn-on fluorescent aptasensor based on aptamer functionalized gold nanoparticles (AuNPs) and luminescent metal–organic frameworks (LMOFs) complex (AuNPs-Apt/NH 2 -MIL-125(Ti)) was realized for bisphenol A (BPA) detection. LMOF NH 2 -MIL-125(Ti) was prepared using facial hydrothermal method. BPA aptamer functionalized AuNPs were prepared and adsorbed on the surface of NH 2 -MIL-125(Ti) to obtain platform of the fluorescent aptasensor. The fabrication process, sensing performance and applicability of the proposed aptasensor were characterized and investigated carefully. Linear detection range of the constructed aptasensor was from 1 × 10 –9 mol L –1 to 1 × 10 –4 mol L –1 with good selectivity, repeatability, stability and reproducibility under optimal experimental conditions. Meanwhile, the fluorescent aptasensor was successfully utilized for BPA detection in real samples with the recoveries of 95.80%-103.12%. The proposed aptasensor based on AuNPs-Apt/NH 2 -MIL-125(Ti) holds significant potential for BPA detection in environmental and food samples, promoting the construction and application of LMOFs-based aptasensor.
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Environmental Science-Nano
·
2024
·
IF 5.8
Jingwei Hong,Wanli Li,Jin Shang,Hiromi Yamashita,Yun Hu
Utilizing electrocatalysis to convert CO2 into high-value industrial raw materials can not only effectively reduce CO2 emissions but also achieve a closed carbon cycle. This method holds great potential for addressing global warming and alleviating the fossil fuel crisis. Here, we report a novel electrocatalyst for CO2 reduction composed of a composite material derived from Cu-MOF74 and Cu2O, synthesized under the regulation of an appropriate amount of KOH. The research results indicate that the unique Cu0/Cu+ interface in Cu-MOF74/Cu2O-350 enhances the adsorption of reaction intermediates, providing more active sites for CO2 reduction. Additionally, the moderate carbonization during the thermal treatment process increases conductivity and enriches the electrochemical active surface area, accelerating the charge transfer rate. Consequently, this composite exhibits excellent CO2 reduction performance. At -1.3 V vs. RHE, the Faraday efficiency (FE) for C2H4 production reached up to 32.48%, which was significantly higher than that of pure Cu2O-350 (9.25%) and Cu-MOF74-350 (15.52%). Even after 6 hours of reaction, the FE for C2H4 remained above 24.52%, reflecting its good stability. Furthermore, we utilized in-situ infrared spectroscopy to study the key intermediates of the relevant reduction products, inferring the possible reaction pathways for the formation of HCOOH and C2H4. This study provides a simple synthesis method for the preparation of high-selectivity MOF-derived composite catalysts for the electrocatalytic reduction of CO2 to value-added chemicals.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Weiguang Hu,Qinghua Xia,Lian Ying Zhang,Jianguo Lu,Qinggang He,Weiyong Yuan
Amorphous MOFs (a-MOFs) could be highly promising cocatalysts of 3-D α-Fe2O3 to greatly improve its photoelectrochemical oxygen evolution performance, but their effective synthesis and assembly on 3-D α-Fe2O3 presents formidable challenges. A conformal and ultrathin layer of amorphous Co–TDPAT (a-Co–TDPAT) MOF cocatalyst has been in situ self-assembled on an α-Fe2O3 nanosheet array (NSA) by employing 5,5′,5″-(1,3,5-triazine-2,4,6-triyl)tris(azanediyl)triisophthalic acid (H6TDPAT) as the organic ligand. The obtained α-Fe2O3 NSA@a-Co–TDPAT core–shell NSA exhibits a photocurrent density of 1.54 mA cm−2 (1.23 V), onset potential of ∼0.48 V, and photoconversion efficiency of 0.25%, 6.2 times higher, 290 mV lower, and 12.5 times higher, respectively, than those of the α-Fe2O3 NSA. The photocurrent density and the photoconversion efficiency are among the highest reported for photoanodes based on the FTO-supported α-Fe2O3 NSA without addition of noble metals, and the onset potential is the lowest among those of FTO-supported α-Fe2O3-based photoanodes reported. It is discovered that a-Co–TDPAT significantly enhances charge separation and accelerates charge transport and transfer for a fast oxygen evolution reaction, thus greatly boosting PEC oxygen evolution. This work not only provides a novel strategy to produce highly efficient, highly stable, low-cost, and earth-abundant core–shell water splitting photoanodes via in situ self-assembly of conformal, ultrathin a-MOFs on an α-Fe2O3 NSA, but sheds light on the mechanisms for controlled self-assembly of MOFs and PEC performance enhancement of α-Fe2O3-based photoelectrodes.
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MOLECULES
·
2025
·Vol. 30
·期 4
·820
·
IF 4.6
Huijuan Han,Yalei Zhang,Chunrui Zhou,Haixin Yun,Yiwen Kang,Kexin Du,Jianying Wang,Shujun Chao,Jichao Wang
To achieve the “double carbon” goal, it is urgent to reform the energy system. The oxygen evolution reaction (OER) is a vital semi-reaction for many new energy-storage and conversion devices. Metal nanoparticles embedded in heteroatom-doped carbon materials prepared by the pyrolyzing of metal–organic frameworks (MOFs) have been a key route to obtain high-performance electrochemical catalysts. Herein, a nanocatalyst embedding Ni nanoparticles into S- and N-co-doped carbon nanoplate (Ni NPs@SN-CNP) has been synthesized by pyrolysis of a Ni-MOF precursor. The prepared Ni NPs@SN-CNP exhibits superior oxygen evolution performance with an overpotential of 256 mV to attain 10 mA cm −2 and a low Tafel slope value of 95 mV dec −1 . Moreover, a self-assembled overall-water-splitting cell with Ni NPs@SN-CNP/NF||Pt-C/NF achieves a low potential of 1.56 V at 10 mA cm −2 and a high cycling stability for at least 10 h. The improvement in this performance is benefit from its large surface area, unique morphology, and the nanostructure of the electrocatalyst. This study presents a novel and simple approach to designing high-performance OER catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Niu Liu,Dongfang Guo,Shiwang Gao,Hanming Liu,Hongwei Niu,Lianbo Liu,Shiqing Wang,Qi Wang,Huanjun Wang,Wei Xu,Hongjun Zhang
To elucidate the direct air capture (DAC) performance and CO 2 selective sieving mechanisms of distinct porous materials under trace CO 2 conditions, three types of materials, anion-pillared materials, open site MOFs, and amine-modified materials, were synthesized, with their DAC performance systematically characterized. DFT-D3 calculations revealed that in NbOFFiVE-1-Ni, the C···F distances (3.04 Å) between CO 2 and the pillared NbOF₅ 2− anions, as well as the O···H distances (2.89 Å) between CO 2 and pyrazine linker hydrogens, are shorter than those in SIFSIX-3-Ni and GEFSIX-3-Ni. These synergistic C···F van der Waals (vdW) and O···H hydrogen-bonding interactions afford NbOFFiVE-1-Ni the highest CO 2 binding energy (62.74 kJ/mol), exceeding that of SIFSIX-3-Ni (57.79 kJ/mol), GEFSIX-3-Ni (60.47 kJ/mol), and MIL-101(Cr) (22.86 kJ/mol). Consistently, NbOFFiVE-1-Ni exhibits the highest atmospheric CO 2 uptake (1.15 mmol/g) among these materials. Given the low atmospheric CO 2 uptake of pristine MIL-101(Cr), two amines (PEI and TEPA) were used to modify it, leveraging its abundant unsaturated metal sites to enhance CO 2 adsorption capacity. DAC performance of amine-modified MIL-101(Cr) first increased then decreased with amine loading, with optimal values of 2.07 mmol/g (50 wt% TEPA) and 1.52 mmol/g (70 wt% PEI). DFT-D3 calculations demonstrated that TEPA molecules and PEI chains bind directly to the unsaturated metal sites of MIL-101(Cr), forming tadpole-like amine-modified MOF structures with binding energies of 210.01 kJ/mol and 178.30 kJ/mol, respectively. Positron annihilation lifetime spectroscopy (PALS) confirmed that TEPA incorporation generates new cavities, microporous structures, and abundant active amine sites in MIL-101(Cr) crystals, synergistically enhancing its DAC performance.
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