JOURNAL OF POROUS MATERIALS
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2026
·
IF 3
Sun Zepan,Hu Tao,Pan Yajing,Liu Zhiqing,Wu Chonggang
Surface modification of porous particles with functional groups is a common way to anchor noble metal catalysts. Herein, surface modification of mesoporous silica (SBA-15) was performed using polyphenols (PNs) through oxidative copolymerization of tea polyphenols and theophylline. The PNs modification ratios on subsequent both Pt loading and chemical states of supported Pt are thoroughly investigated. Catalytic activity of the resulting catalysts was evaluated through various hydrosilylation reactions, while its recyclability was also examined. Results show that modification with PNs can not only facilitates the loading of Pt, but also favors the formation of more active Pt 0 species, thereby increase the catalytic activity of the catalyst. Among them, the SBA-15-PNs-Pt-2 catalyst with the highest PNs ratios exhibits both high activity, good selectivity of anti-Markovnikov addition products and excellent recycling performance. Meanwhile, whether it is under low catalyst loadings or toward the hydrosilylation reactions between a series of substrates, the SBA-15-PNs-Pt-2 catalyst all exhibit undeclined activity, which again signifies the substantial role of PNs in both loading and anchoring Pt species.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2026
·
IF 4.8
Shiyu Yang,Wenqi Qin,Yanji Zhang,Jun Chai,Ronghuan Wan,Hong Lei,Yi Wei
The Pt/γ-AlOOH-IP was prepared using γ-AlOOH support by impregnation method. • The strong MSI and electron-rich Pt sites are fabricated in Pt/γ-AlOOH-IP. • Pt/γ-AlOOH-IP exhibits excellent catalytic performance in the hydrosilylation. • Electron-rich Pt sites promote the TES adsorption and Si–H bond cleavage. Hydrosilylation is a highly important method for the preparation of organosilicon compounds, in which homogeneous Pt catalysts exist poor recyclability and high production costs. Here, we prepared supported Pt-based catalyst (Pt/γ-AlOOH-IP) using γ-AlOOH support by impregnation (IP) method, in which strong metal-support interactions (MSI) and electron-rich Pt sites were fabricated. Catalytic measurements show that Pt/γ-AlOOH-IP has the best catalytic activity in the conversion of 1-octene and triethoxysilane (TES)via hydrosilylation to n-octyltriethoxysilane (OTES), the yield of OTES is 93.6% with 94.3% selectivity at 80 ℃, 2.5 h, m (Pt) /m (1-octene) = 7.5 × 10 −5 and n (TES) /n (1-octene) = 1.33, which are commensurate with homogeneous Karstedt’s catalyst. The significant catalytic performance of Pt/γ-AlOOH-IP originates from more electron transfer between Pt and γ-AlOOH. Electron-rich Pt sites promote TES chemisorption and Si–H bond dissociation, and improve catalytic activity, which are corroborated by the DFT calculations. This finding enhances the insight of MSI and offers an easy method to prepare efficient heterogeneous catalysts for industrial hydrosilylation reactions. Download: Download high-res image (166KB) Download: Download full-size image
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2020
·Vol. 35
·期 1
·e6027
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IF 3.14
Zinan Dai,Zehao Yu,Ying Bai,Jiayun Li,Jiajian Peng
A simple method for the hydrosilylation of olefins by using air-stable cobalt catalysts is developed. The catalyst system is composed of simple, cheap, and readily available cobalt(II) salts and well-defined terpyridine derivatives as cocatalysts or ligands, and the hydrosilylation processes can be processed smoothly under mild conditions without either Grignard reagents or NaHBEt 3 as activator.
研究领域:
有机化学
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催化化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Changkun Song,Zilong Zheng,Wenchao Zhang,Ye Yang,Guowei Zeng,Chunpei Yu,Jiaxin Wang,Yajie Chen,Kefeng Ma,Zhipeng Cheng
The huge energy release and highly adjustable combustion characteristics of nanoporous silicon (nPS) make it one of the most attractive inorganic energetic materials. However, nPS will be oxidized slowly from its surface when it is left in ambient air to be aged. Explanations vary as to the aging mechanism, and the corresponding anti-ageing strategy remains to be fully investigated. The present study provides an efficient strategy of a thermal-induced hydrosilylation to improve the long-term chemical stability of H-terminated nPS. The nPS of 75 μm in depth was etched with a pore diameter of 52.5 nm and a gravimetry-determined porosity of 79.6%. The DSC and FTIR data confirm that oxygen is able to infiltrate the H-terminated layer and preferentially attack the weak Si-Si over Si-H bonds. The prime oxidizer is not sodium perchlorate but oxygen from the air to cause a backbond oxidation. After a modification, the heat of reaction is determined to be 1436 J·g −1 . Interestingly, this value is of almost no detectable change to be 1402 J·g −1 and 1387 J·g −1 when aged for 24 or 48 h, respectively. All the evidences suggest that the alkyl-terminated nPS exhibits an excellent anti-oxidation ability to ambient air, which is well consistent with a high-speed video analysis from the combustion behavior of nPS impregnated with NaClO 4 ·H 2 O. This work suggests that only one step may be away from a practical application of nPS energetic materials.
研究领域:
材料科学
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化学工程
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高影响因子
Coatings
·
2019
·Vol. 9
·期 10
·605
·
IF 2.33
Jianye Ji,Xin Ge,Weijie Liang,Xiaoyan Pang,Ruoling Liu,Shuyi Wen,Jiaqi Sun,Xunjun Chen,Jianfang Ge
To overcome the inherent limitation that the preparation of high molecular weight MQ copolymers (Mw ≥ 30,000 g/mol) via the hydrolysis and condensation of solicate salts generally results in an intractable gel, vinylphenyl-containing MQ silicone resin with a high molecular weight was designed and synthesized through the hydrosilylation reaction of vinyl-containing MQ silicone resin and linear poly(diphenylsiloxane) with two terminal Si–H bonds. The weight average molecular weight of these modified copolymers reported here is at least 30,000 dal·mol−1. These polymers have favorable thermal stability and a higher refractive index than that of the base resin due to the formation of novel regular macromolecular structures and the introduction of phenyl groups. These inorganic/organic hybrid materials could be used as a potential component for temperature-resistance electronics adhesive, heat-resistant coatings and high-performance liquid silicone rubber. Moreover, the proposed process also provides a possibility to choose higher molecular weight MQ silicones according to application requirements.Keywords:MQ silicone resin;modified;hydrosilylation;high molecular weight
研究领域:
材料科学
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有机化学
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MICROPOROUS AND MESOPOROUS MATERIALS
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2021
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IF 5.455
Xiaomei Miao,Keyu Mao,Yue Yan,Yongbing Pei,Michael J. Sailor,Lianbin Wu
Porous silicon was widely used in displays, optical sensors , and biological imaging due to its high surface areas, adjustable microstructure, large adsorption capacity and excellent optical performance. Unfortunately, there are numerous reactive silane groups on the freshly etched porous silicon surface, which are susceptible to oxidization in the air, thereby affecting the optical performance and stability of porous silicon. This study provides an efficient strategy of using photocatalytic reaction to graft dodecafluoroheptyl methacrylate to freshly prepared n-type porous silicon surface, thereby generating a fluorine-modified porous silicon with high stability and superhydrophobic surface. The structure and composition of porous silicon before and after modification were analyzed by scanning electron microscope (SEM), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy-energy dispersive spectrometer (SEM-EDS) and X-ray photoelectron spectroscopy (XPS). The effects of UV light, reactant mass fraction and reaction time on the surface properties of porous silicon were studied by water contact angle (WCA) and photoluminescence (PL). The results indicated that the dodecafluoroheptyl methacrylate was successfully grafted onto n-type porous silicon surface by photocatalytic reaction. The superhydrophobic and luminescent porous silicon was prepared by reacting 40 min in a dichloride solution containing 10 wt% dodecafluoroheptyl methacrylate under UV light. The WCA of the fluorine-modified porous silicon surface could reach 153° and had good photoluminescence intensity. This modified porous silicon surface had great stability in alkaline and air environment. After treated with alkaline droplets for 30 min, the WCA of modified porous silicon could maintain above 150° and had good photoluminescence. And under room temperature within a week, the porous silicon surface still showed great hydrophobic properties and photoluminescence intensity. In addition, the modified porous silicon has different responsiveness to ethanol solutions of different concentrations, which could be applied to alcohol sensors and has great development prospects.
研究领域:
材料科学
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表面化学
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高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
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2022
·Vol. 36
·期 6
·e6648
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IF 4.072
Zehao Yu,Zijie Song,Chunshan Lu,Ying Bai,Jiayun Li,Jun Liu,Peng Liu,Jiajian Peng
Hydrosilylation employing metal–organic frameworks (MOFs) as the catalyst are promising because of their high catalytic reactivity and sustainability of heterogeneous catalyst. A highly simple and efficient method for the hydrosilylation of olefins catalyzed by an air-stable MOF-cobalt catalysts is developed. This approach is featured by 0.1% of Co-MOFs catalyst with excellent reactivity, recyclability, and good functional group tolerance. The Co-MOFs can catalyze hydrosilylation of styrene or its derivatives with Ph 2 SiH 2 in the presence of NaBHEt 3 . Moreover, the catalysts we developed show excellent stability, and the activity is not significantly reduced after repeating the cycle for five times.
研究领域:
化学
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材料科学
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催化反应
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高影响因子
International Journal of Applied Ceramic Technology
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2023
·Vol. 20
·期 4
·2593-2602
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IF 2.1
Guiqin You,Daoyang Han,Huijie Tian,Junfang Liang,Chang-An Wang,Keke Yuan,Jilin He,Mingliang Li,Hailong Wang,Rui Zhang,Gang Shao
Polymer-derived ceramic materials exhibit adjustable composition, microstructure, and dielectric properties and are widely used as high temperature microwave absorption materials in the aerospace field. In this study, polymer-derived SiCN ceramic aerogels with excellent electromagnetic wave absorption (EMA) properties were successfully fabricated through a combination of the sol-gel, freeze- drying, and polymer precursor conversion methods. The hydrosilylation reaction between the Si-H bond in polysilazane (a polymer ceramic precursor) and the C = C bond in divinylbenzene (a cross-linking agent) occurs to form a wet gel. The effects of the molar ratios of the two bonds (C = C/Si-H) on the microstructure and EMA properties of the SiCN ceramic aerogels were systematically studied. At a C = C/Si–H molar ratio of 1.25:1, the minimum reflection loss of the SiCN ceramic aerogels is −37.57 dB at 10.88 GHz. Moreover, the corresponding effective absorption bandwidth covers almost the entire X-band, showing excellent EMA properties.
研究领域:
材料科学
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航空航天工程
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RSC Advances
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2016
·Vol. 6
·期 100
·98520-98527
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IF 3.289
Huachao Zai,Yizhou Zhao,Shanyu Chen,Rui Wang,Lei Ge,Changfeng Chen,Yujing Li
Recycling of noble-metal-based catalysts remains difficult and limits their applications towards catalysis in organic synthesis reactions with high viscosity. This work demonstrates a magnetically responsive hydrosilylation catalyst with novel core–shell nanostructure, which can be recycled from highly viscous reaction solutions. The supporting material, with core–shell structure, incorporates a Fe3O4 nanoparticle as the core coated with silica shell through reverse microemulsion approach to form SiO2/Fe3O4 nanoparticles which show superparamagnetic behavior. Ultrafine Pt NPs are facilely prepared and loaded on SiO2 shell via a simple hydrothermal protocol, forming Pt/SiO2/Fe3O4 catalyst. As-synthesized catalysts exhibit high catalytic activity towards the hydrosilylation of allyl polyether with low-hydro silicone oil. Despite the high viscosity of the reaction system, the catalyst dispersed in reaction solution shows superparamagnetic response upon the application of magnetic field and can be recycled up to 7 times without appreciable loss in the catalytic activity. This work demonstrates a highly efficient and recyclable catalyst to catalyze hydrosilylation reaction with high viscosity and proposes a new philosophy to design reusable catalyst for organic reaction.
研究领域:
催化化学
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纳米材料
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有机合成
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磁性材料
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绿色化学
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DOI
高影响因子
ACS Catalysis
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2025
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IF 13.1
Yi Lu,Fengjian Zhu,Chenglong Li,Zhiying Du,Liwei Niu,Hong Chi,Qiang Chang,Dan Xu,Xingwu Liu,Zunqi Liu,Jianbin Chen
Constructing thermally durable single-atom catalysts resembling mononuclear homogeneous catalysts for the hydrosilylation industry is usually challenging. Herein, a stable single-atom catalyst with Pt single atoms anchored on a nonreducible and industrially fundamental γ-Al2O3 support (Pt1/γ-Al2O3) was fabricated using atomic layer deposition technology. The catalyst enabled anti-Markovnikov hydrosilylation under room-temperature and solvent-free conditions and exhibited activity exceeding that of the homogeneous Karstedt’s catalyst. The Pt1/γ-Al2O3 catalyst not only afforded a broad substrate scope in high yields, encompassing various alkenes and alkynes, but also exhibited robust stability and recyclability. Extended X-ray absorption fine structure and X-ray absorption near-edge structure analyses confirmed that the Pt atoms were stabilized by bonding with oxo ligands, forming a PtO4 moiety embedded in γ-Al2O3 lattices with coordination geometries resembling those of mononuclear homogeneous catalysts. Density functional theory calculations revealed that the unexpected catalytic performance could be attributed to the partially positively charged and atomically dispersed Pt atoms in the Pt1/γ-Al2O3 catalyst, which arose from metal–support interaction through oxo ligands, resulting in an elevated d-orbital energy and an upshift in the d-band center away from the Fermi level. This electronic effect facilitated the easier dissociation of phenylethyl and promoted its coupling with the dimethylphenylsilyl group on the catalyst surface, ultimately leading to the desired product.
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JOURNAL OF ORGANIC CHEMISTRY
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2024
·
IF 3.3
Yue Zhang,Ting Wang,Yuan-Yuan Liu,Zheng-Bing Zhang,Pan Han,Linhai Jing
Geminal and vicinal borosilanes have unique applications in functional materials and synthetic transformations. Herein, a convenient method for the synthesis of geminal and vicinal borosilanes is developed via photoredox metal-free hydrosilylation of vinylboronic esters. This strategy features the advantages of high atom economy, environmental friendliness, and excellent functional group compatibility. The mechanism studies reveal that the catalytic reaction goes through photoredox HAT catalysis and a radical addition pathway.
研究领域:
有机化学
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材料科学
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DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2024
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IF 4
Changhui Liang,Kairui Liu,Huixiang Li,Xiaoqiang Zhang,Jun Shen,Z. Conrad Zhang
Single atom catalysts (SACs) offer high atom efficiency with highly selective reaction pathway. Various strategies have been developed to synthesize SACs, among which thermally stable metal centers are usually in high oxidation while they are susceptible to facile sintering in reduced state or under reducing conditions. One of the strategies developed very recently to achieve stable zero valent metal atoms is based on the selection of ligands with moderate coordination strength with the metal center. In this work, the crucial importance of ligand to the stability of single Pt 0 atoms is investigated. While HCl and diether have been found to be able to stabilize single Pt 0 atoms by forming Pt 1 @HCl adducts, HBr coordinated Pt single atom (Pt 1 @HBr) obtained by simply exchanging HCl with HBr shows increased thermal stability over the Pt 1 @HCl under H 2 atmosphere at elevated temperature, as evidenced by DRFITs of CO chemisorption and HRTEM. This work offers a facile approach to tune the stability of Pt single atoms while keeping the structure of active sites of single atom center to achieve excellent catalytic performance, using hydrosilylation in the demonstrative studies.
研究领域:
催化化学
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材料科学
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高影响因子
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