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MICROPOROUS AND MESOPOROUS MATERIALS · 2022 · IF 5.876

Preparation and gas separation performance of seeding-free aqueous synthesis ZIF-8 membrane by homologous-like ligands method

Tao Yan,Jianhua Yang,Jinming Lu,Liang Zhou,Yan Zhang,Gaohong He

Due to the poor heterogeneous nucleation properties of MOFs crystal on ceramic substrates resulting from the absence of interaction of MOFs with support substrate surface, it is usually difficult to prepare well-intergrown MOF membranes on substrate by simple in situ growth. In this work, a novel synthesis strategy was used to prepare defect-free ZIF-8 membranes on α-Al 2 O 3 supports by depositing gold particles modified with 2-mercaptoimidazole which creates pseudo-surfaces to bridge the metal centers with support. The end groups of the 2-mercaptoimidazole guides the heterogeneous nuclei to the support surface as homologous-like ligands. Furthermore, investigation of the metal sources revealed that the ZIF-8 membranes prepared with Zn(OAc) 2 as the zinc source possessed more continuous and well-intergrown ZIF-8 membranes with a thickness of about 1 μm compared to other zinc sources. The results of gas separation performance show that the optimized ZIF-8 membranes possess high hydrogen permeance and thermal stability. The gas separation selectivity for binary H 2 /CH 4 mixture reached 20.8 at 150 °C and 1 bar, with a high H 2 permeance of about 6.15 × 10 −7  mol m −2  s −1 Pa −1 , which is promising for hydrogen separation and purification. Moreover, free-organic solvents and room temperature growth by our strategy dramatically reduces the difficulty of preparation and environmental destruction, thus offering a new avenue to prepare MOFs membrane with good separation performance.

CAS / MDL: 693-98-1 7646-85-7
研究领域: 材料科学 · 化学工程
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Nature Chemistry · 2024 ·Vol. 16 ·期 6 ·893-900 · IF 19.2

Deprotonated 2-thiolimidazole serves as a metal-free electrocatalyst for selective acetylene hydrogenation

Zhang Lei,Bai Rui,Lin Jin,Bu Jun,Liu Zhenpeng,An Siying,Wei Zhihong,Zhang Jian

Metal-free catalysts offer a desirable alternative to traditional metal-based electrocatalysts. However, metal-free catalysts, featuring defined active sites, rarely show activities as promising as metal-based materials. Here we report 2-thiolimidazole as an efficient metal-free catalyst for selective electrocatalytic hydrogenation of acetylene into ethylene. Under alkaline conditions, the sulfhydryl and imino groups of 2-thiolimidazole are spontaneously deprotonated into dianions. Deprotonation thus enriches the negative charges of pyridinic N sites in 2-thiolimidazole to enhance the adsorption of electrophilic acetylene through the σ -configuration. Ethylene partial current densities show a volcano relationship with the negative charges of the pyridinic N sites in various imidazole derivatives. Consequently, the deprotonated 2-thiolimidazole exhibits an ethylene partial current density and faradaic efficiency competitive with metal-based catalysts like Cu and Pd. This work highlights the tunability and promising potential of metal-free molecules in electrocatalysis.

研究领域: 电化学 · 催化 · 材料科学
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Journal of Materials Chemistry B · 2024 · IF 6.1

Mercaptoimidazole-capped gold nanoparticles as a potent agent against plant pathogenic fungi

Tang Xu,Wenshuai Hao,Ran Du,Dai Dai,Cuixia Wang,Suhua Li,Carol Sze Ki Lin,Ruitao Cha,Jianbin Yan,Chong Li

Plant pathogenic fungi pose a substantial challenge to agricultural production, but the conventional fungicide-based approaches are losing importance. As agents with broad-spectrum antibacterial effects, gold nanoparticles (Au NPs) are found to have antifungal effects; however, no study has examined their application in agriculture as fungicides. Accordingly, this study investigates the activity of 2-mercaptoimidazole-capped Au NPs (MI-Au NPs) against the ‘top’ plant pathogenic fungi, finding that they could inhibit Magnaporthe oryzae, Botrytis cinerea, Fusarium pseudograminearum and Colletotrichum destructivum by inducing cytoplasmic leakage. Moreover, MI-Au NPs are found to protect plants from infection by B. cinerea. Specifically, pot experiments demonstrate that MI-Au NPs decrease the incidence rate of B. cinerea infection in Arabidopsis thaliana from 74.6% to 6.2% and in Solanum lycopersicum from 100% to 10.9%, outperforming those achieved by imazalil. Furthermore, the biosafety assays reveal that MI-Au NPs cannot penetrate the cuticle of plant cells or negatively influence plant growth, and it is safe to mammalian cells. In summary, the findings of this study will support the development of NP-based antifungal agents for use in agriculture.

CAS / MDL: 208255-80-5 872-35-5
研究领域: 农业科学 · 纳米技术 · 植物病理学
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Journal of Materials Chemistry A · 2026 · IF 9.5

Manipulating d-Band Center of Cu(I)-MOFs for Catalytic Ignition of [BMIM]N(CN) 2 IL-H 2 O 2 Propellants

Qing Cheng,Yuqi Zhang,Yingying Cao,Long Liu,Yanqiang Zhang

The novel ionic liquid-H2O2 propellants are urgently to solve the intrinsic ignition problem for achieving the aerospace applications. We addressed this issue by tuning the d-band center to adjust the catalyst's adsorption strength for IL/H2O2 toward the optimal value, thus enhancing catalytic activities for the efficient decomposition of H2O2 to generate reactive oxygen species. Herein, the regulation of the d-band center of Cu(I) in Cu(I)-MOF catalyst by precise ligand engineering design was studied. Remarkably, The Cu-S3 coordination of Cu-SH' shifts its d-band center closer to the Fermi level, promoting the adsorption of [BMIM]N(CN)2 and H2O2. Cu-SH' enables efficient H2O2 activation and robust •OH and 1 O2 generation to trigger the rapid self-ignition of [BMIM]N(CN)2-H2O2 propellant. The resulted tid as low as 18.4 ms is nearly 34% lower than that of homogeneous catalyst [FcCH2N(CH3)3]2[Cu2I4]. This work provides fundamental insights into the design of efficient ligand-based combustion catalysts for the higher performance of rockets and spacecrafts.

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MICROCHIMICA ACTA · 2025 ·Vol. 192 ·期 12 ·847 · IF 5.3

Core–shell ZIF-8@Au labels for high-sensitivity lateral flow assays via thiol-functionalization and seed-mediated growth

Ma Haibo,Ru Changhai,Zhang Fanghao,Hoettges Kai,Zhu Junhui,Song Pengfei

ZIF-8-core/Au-shell (ZIF-8@Au) nanoparticles were fabricated through a two-step strategy involving thiol-modification of ZIF-8 substrates and subsequent Au shell growth via seed-mediated approach, and the ZIF-8@Au nanoparticles were applied to the screening of clostridium difficile infection (CDI). Through regulating dosage of thiol-modifier, we established a surface functionalization protocol that introduced tunable thiol groups onto ZIF-8 particles while preserving their pristine morphology and crystallinity. Subsequent refinement of Au coating parameters enabled the construction of ZIF-8@Au core–shell nanostructures via seed-mediated growth. The resulting ZIF-8@Au nanoparticles were successfully applied to detect biomarkers of CDI, including toxin A, toxin B, and glutamate dehydrogenase (GDH), with sensitivities of 7 pg/mL, 115 pg/mL, and 27 pg/mL, respectively. These results demonstrate the promising potential of this nanoparticle-based platform for lateral flow assays. Graphical

研究领域: 纳米技术 · 生物传感器 · 分析化学 · 医学诊断 · 材料科学
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Processes · 2024 ·Vol. 12 ·期 3 ·626 · IF 2.8

A Molecularly Imprinted Fluorescence Sensor Based on Upconversion-Nanoparticle-Grafted Covalent Organic Frameworks for Specific Detection of Methimazole

Yan Liu,Tian Zhao,Shuzhen Li,Yichuan Cao,Guozhen Fang

Rapid detection and sensitive analysis of MMZ is of great importance for food safety. Herein, a fluorescent molecularly imprinted sensor based on upconversion nanoparticles (UCNPs) grafted onto covalent organic frameworks (COFs) was designed for the detection of MMZ. COFs with a high specific surface area and excellent affinity serve as substrates for grafting of UCNPs, which can inhibit the aggregation burst of UCNPs and improve the mass transfer rate of the sensor. Through a series of characterizations, it was found that the proposed UCNP-grafted COFs@MIP-based sensor had good optical stability, high adsorption efficiency, strong anti-interference ability, and high sensitivity owing to the integration of the advantages of UCNPs, COFs and MIPs. Under the optimal conditions, a good linear relationship was presented between the fluorescence intensity of UCNP-grafted COFs@MIPs and the methimazole concentration in the range of 0.05–3 mg L−1, and the detection limit was 3 μg L−1. The as-prepared UCNP-grafted COFs@MIPs were successfully applied for the detection of MMZ in actual samples, and the results were relevant with those determined by high-performance liquid chromatography. The sensor has good sensitivity, reusability, and high selectivity, which are highly valuable in the rapid analysis and detection of food safety.

研究领域: 食品安全 · 分析化学 · 材料科学
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FOOD CHEMISTRY · 2019 · IF 5.399

Hollow molecularly imprinted polymer based quartz crystal microbalance sensor for rapid detection of methimazole in food samples

Xiaolei Zhao,Yu He,Yanan Wang,Shuo Wang,Junping Wang

In this study, a novel detection method of methimazole was proposed based on the hollow molecularly imprinted quartz crystal microbalance (QCM) sensor, in which the hollow imprinted polymers (H-MIPs) were firstly prepared through the surface imprinted techniques, using hollow silica spheres as matrix supporting material and methimazole as template molecule. The characterizations of H-MIPs were carefully studied. Compared with traditional MIPs, H-MIPs exhibited faster mass transfer rate and higher adsorption capacity. After coating onto the surface of Au chip, the H-MIPs QCM sensor was fabricated. Based on the frequency shift, good linear behavior in the range of 5–70 μg L –1 , limit of detection of 3 μg L –1 , and good recoveries of 88.32%–107.96% in the spiked pork, beef and milk were obtained. The analysis process could complete within 8 min. The developed sensor provided an effective, fast and accurate method for the methimazole detection in food samples.

研究领域: 分析化学 · 食品安全
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Journal of Energy Chemistry · 2021 · IF 9.676

Small molecule interfacial cross-linker for highly efficient two-dimensional perovskite solar cells

Hongming Hou,Taotao Hu,Fu Zhang,Rui Liu,Jialong He,Chang Liu,Yue Yu,Dong Chen,Qiaofeng Wu,Meng Zhang,Hua Yu

The nonradiative recombination of charge carriers at the hole transport layer (HTL)/perovskite interface generally induces remarkable performance loss of the inverted two-dimensional perovskite solar cells (2D PSCs). Herein, a cross-linkable small molecule of 2-mercaptoimidazole (2-MI) was introduced into the nickel oxide (NiO x )/2D perovskite interface. Experiments have confirmed the formation of Ni-N covalent bond by N atom in the 2-MI and Ni in the NiO x and the coordinating between S atom of 2-MI and under-coordinated Pb 2+ near to the NiO x /perovskite interface, which contributes to creating a cross-linking between NiO x /perovskite interface to restrain charge carrier recombination and enhance   the extraction of hole carriers at the interface. Besides, the 2-MI modification layer is also beneficial for promoting the crystallinity of 2D perovskite. Consequently, the inverted 2D PSCs with 2-MI modification achieved the best power conversion efficiency of 15%. This paves a route to acquire highly efficient 2D PSCs by constructing a cross-linking at the NiO x HTL/2D perovskite interface.

研究领域: 材料科学 · 光伏技术 · 化学工程
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INORGANIC CHEMISTRY · 2022 · IF 5.436

Stable Core–Shell Structure Nanocrystals of Cs4PbBr6-Zn(moi)2 Achieved by an In Situ Surface Reconstruction Strategy for Optical Anticounterfeiting

Xiaoxia Feng,Pengxiao Xu,Jinli Liu,Xiyue Zhao,Jing Cao,Jiacheng Liu

Zero-dimensional Cs4PbBr6 nanocrystals (NCs) possess attractive photoluminescence (PL) properties and feature facile chemical synthesis, making them promising for application in luminescent materials. However, Cs4PbBr6 remains sensitive to polar solvents and thermal stimuli because of soft ionic nature of Cs4PbBr6 and dynamic behavior of surface ligands. Herein, a strategy controlled by an in situ surface coordination reaction is developed to fabricate stable NCs with a Cs4PbBr6-Zn(moi)2 core–shell structure. It was found that the Cs4PbBr6 surface regulated by the use of 2-mercaptoimidazole (called moi) and the coordination between the −NH group of moi and Zn2+ is critical for the formation of Cs4PbBr6-Zn(moi)2 core–shell NCs. Meanwhile, the thickness of the Zn(moi)2 shell can be facilely controlled by the growth time because of the solubility of moi and Zn(OAc)2·2H2O in ethyl acetate. Compared to bare Cs4PbBr6, Cs4PbBr6-Zn(moi)2 NCs exhibited highly improved polar solvent resistance and thermal stability. By combining the sensitivity of Cs4PbBr6 and the stability of Cs4PbBr6-Zn(moi)2, we used two NCs as PL security inks to fabricate optical anticounterfeiting labels. Thus, the disposable or reusable optical anticounterfeiting label is achieved by changing the external dual-stimuli. This work provides a novel strategy to enhance the stability of Cs4PbBr6 and develop its potential interest for application in anticounterfeiting technologies.

CAS / MDL: 872-35-5
研究领域: 材料科学 · 光学工程
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ACS Nano · 2023 · IF 17.1

Ligand-Modified Gold Nanoparticles as Mitochondrial Modulators: Regulation of Intestinal Barrier and Therapy for Constipation

Wenshuai Hao,Ruitao Cha,Mingzheng Wang,Juanjuan Li,Hongbo Guo,Ran Du,Fengshan Zhou,Xingyu Jiang

Intestinal metabolism-related diseases, such as constipation, inflammatory bowel disease, irritable bowel syndrome, and colorectal cancer, could be associated with the dysfunction of intestinal mitochondria. The mitochondria of intestinal epithelial cells are of great significance for promoting intestinal motility and maintaining intestinal metabolism. It is necessary for the prophylaxis and therapy of intestinal metabolism-related diseases to improve mitochondrial function. We investigated the effect of 4,6-diamino-2-pyrimidinethiol-modified gold nanoparticles (D-Au NPs) on intestinal mitochondria and studied the regulatory role of D-Au NPs on mitochondria metabolism-related disease. D-Au NPs improved the antioxidation capability of mitochondria, regulated the mitochondrial metabolism, and maintained intestinal cellular homeostasis via the activation of AMPK and regulation of PGC-1α with its downstream signaling (UCP2 and DRP1), enhancing the intestinal mechanical barrier. D-Au NPs improved the intestinal mitochondrial function to intervene in the emergence of constipation, which could help develop drugs to treat and prevent mitochondrial metabolism-related diseases. Our findings provided an in-depth understanding of the mitochondrial effects of Au NPs for improving human intestinal barriers.

CAS / MDL: 208255-80-5 872-35-5
研究领域: 纳米技术 · 药理学 · 胃肠病学 · 分子生物学 · 治疗学
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