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CHEMISTRY OF MATERIALS · 2015 · IF 8.354

Generalized Water-Processed Metal Chalcogenide Complexes: Synthesis and Applications

Zhe Xia,Jie Zhong,Meiying Leng,Long Hu,Ding-Jiang Xue,Bo Yang,Ying Zhou,Xinsheng Liu,Sikai Qin,Yi-Bing Cheng,Jiang Tang

Metal chalcogenide complexes (MCCs) have attracted considerable attention recently due to their high solubility in polar solvents, low-temperature decomposition to metal chalcogenide films, and service as ligands for colloidal nanocrystals (NCs). However, most of the MCCs were typically synthesized in the highly toxic and explosive hydrazine (denoted as hydrazine-MCCs), severely restricting the wide applications of MCCs. Here we present a versatile and environmentally benign water-based solution method for the preparation of various MCCs (denoted as water-MCCs) through directly dissolving a series of bulk V2VI3 chalcogenides (V = Sb, As and VI = S, Se, Te) in water with the presence of (NH4)2S at room temperature and ambient atmosphere. We further show that such water-MCCs can be readily processed into corresponding semiconducting thin films upon mild thermal treatment and then be extended to fabricate compositionally controlled semiconductor alloys with tunable band gaps (i.e., Sb2(S1–x,Sex)3, 0 ≤ x ≤ 1) through simple control of substrate temperature. Furthermore, we present that our water-MCCs, especially for Sb4S72–, can be utilized to serve as ligands for in-situ-synthesized water-based PbS quantum dots (QDs), achieving a homogeneous and stable aqueous QDs solution without needing further conventional secondary ligand exchange. Our study provides a general strategy for the synthesis of various MCCs using water as safer and more environmentally friendly solvent alternative to hydrazine, thus greatly enhancing the wide applications of MCCs in solution-processed inorganic semiconductors.

CAS / MDL: 13494-80-9 12135-76-1
研究领域: 材料科学 · 化学
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Nanoscale · 2020 ·Vol. 12 ·期 11 ·6522-6528 · IF 6.895

Low-temperature direct synthesis of perovskite nanocrystals in water and their application in light-emitting diodes

Xuefeng Zhang,Long Gao,Min Zhao,Yanqin Miao,Zhiyuan Wang,Chengqiang Wang,Peizhi Liu,Bingshe Xu,Junjie Guo

Cesium lead halide perovskite nanocrystals (PNCs) have aroused tremendous research attention because of their excellent optoelectronic properties. Herein, we developed a facile and green low-temperature strategy free of organic solvents, in which only pure water was adopted as the solvent, to synthesize CsPbBr3 NCs. Intriguingly, although formed with the assistance of water, the obtained CsPbBr3 NCs present a cubic crystal structure, photoluminescence quantum yield (PLQY) of 75%, and narrow emission line width for bright green emission. Furthermore, both electroluminescence (EL) and photoluminescence (PL)-based light-emitting diodes (LEDs) present intrinsic green emission originating from the as-prepared CsPbBr3 NCs. Hence, this work offered a novel eco-friendly avenue for the preparation of perovskite NCs for their practical applications in LEDs.

研究领域: 材料科学 · 纳米技术 · 光电
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GREEN CHEMISTRY · 2024 · IF 9.3

Green, efficient and controllable synthesis of high-quality MOF-74 with high gravity technology

Xin-Ran Shi,Meng Qiao,Yan Wei,Ling-Xia Yun,Jie-Xin Wang,Jian-Feng Chen

MOF-74 or M2(dhtp) (M = metal ions, dhtp = 2,5-dihydroxyterephthalic acid), as a typical class of metal–organic frameworks (MOF), have garnered considerable interest due to their abundant unsaturated metal sites. However, environmental and economic limitations caused by the extensive use of organic solvents in traditional syntheses hinder their industrial applications. Although water as a green solvent is considered to be the best candidate solvent, water-based MOFs often have poor crystallinity and long synthesis time, and controlling the particle size is difficult. Herein, a water-based strategy is proposed to synthesize high-quality MOF-74–Co with controllable particle sizes in a rotating packed bed (RPB) reactor using high-gravity technology. MOF-74–Co could be rapidly prepared in the RPB, and shows a smaller and more uniform particle size, higher crystallinity, and larger specific surface area, as compared to the counterpart prepared in a traditional stirred tank reactor. Further adopting acetic acid as a modulator, the as-prepared MOF-74–Co has the highest BET surface area (1599 m2 g−1) in the reported literature so far and simultaneously possesses a high space–time yield (293 kg m−3 day−1). High-quality MOF-74–Zn and MOF-74–Ni can also be prepared, proving the generality of this strategy. Furthermore, the small-sized MOF-74–Co-78 nm exhibits a faster adsorption rate and a larger saturation adsorption capacity (298 mg g−1) for CO2 compared with large-sized samples. This study not only advances the field of green synthesis of MOFs but also paves the way for efficient manufacturing processes in MOF-74 synthesis for CO2 adsorption.

研究领域: 材料科学 · 化学工程 · 环境科学
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Nano Materials Science · 2022 · IF 0

Water-based synthesis of nanoscale hierarchical metal-organic frameworks: Boosting adsorption and catalytic performance

Yi Yu,Zewei Liu,Xiaofei Chen,Shujun Liu,Chongxiong Duan,Hongxia Xi

The combination of nano sizes, large pore sizes and green synthesis is recognized as one of the most crucial and challenging problems in constructing metal-organic frameworks (MOFs). Herein, a water-based strategy is proposed for the synthesis of nanoscale hierarchical MOFs (NH-MOFs) with high crystallinity and excellent stability. This approach allows the morphology and porosity of MOFs to be fine tuned, thereby enabling the nanoscale crystal generation and a well-defined hierarchical system. The aqueous solution facilitates rapid nucleation kinetics, and the introduced modulator acts as a deprotonation agent to accelerate the deprotonation of the organic ligand as well as a structure-directing agent (SDA) to guide the formation of hierarchical networks. The as-synthesized NH-MOFs (NH-ZIF-67) were assessed as efficient adsorbents and heterogeneous catalysts to facilitate the diffusion of guest molecules, outperforming the parent microZIF-67. This study focuses on understanding the NH-MOF growth rules, which could allow tailor-designing NH-MOFs for various functions.

研究领域: 材料科学 · 化学工程 · 纳米技术 · 催化 · 环境科学
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