SURFACE AND INTERFACE ANALYSIS
·
2022
·Vol. 55
·期 4
·279-287
·
IF 1.702
Mengnan Qu,Bin Zhang,Yandong Wang,Yanqing Lv,Jianwei Ge,Yaxin Wu,Min Yan,Lei Shen,Jinmei He
Wettability is an important property of solid surfaces, superwetting materials can be prepared by controlling the surface morphology and surface energy. In recent years, superwetting materials have been researched and used widely in the fields of self-cleaning, anti-fogging, microfluidics, and oil–water separation, but few studies about superwetting materials in chemical reactions have been conducted. In the multiphase reaction, the low solubility and diffusion rate of gas lead to inferior mass transfer, which restricts the reaction kinetics and reduces the reaction rate. Therefore, it may be a breakthrough to make the solid surface obtain underwater superaerophilicity. In this paper, 1H,1H,2H,2H -perfluorooctyltriethoxysilane (POTS) with low surface energy was constructed on the palladium-carbon nanotubes (Pd-CNTs), as-prepared Pd-CNTs/POTS composite has excellent hydrophobicity and underwater superaerophilicity. When Pd-CNTs/POTS composite was utilized in the catalytic hydrogenation, Pd-CNTs/POTS composite shows higher catalytic activity than Pd-CNTs; the higher catalytic performance is attributed to the underwater superaerophilicity, which enables gaseous hydrogen to rapidly accumulate on the surface of material, increasing the gas–liquid–solid reaction interface formed. The strategy looks forward to providing a new way for developing novel and efficient heterogeneous catalysts and reaction systems.
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Polymer Chemistry
·
2020
·Vol. 12
·期 4
·526-533
·
IF 5.342
Huanhuan Ma,Linan Wang,Yachao Liang,Zhe Cui,Peng Fu,Minying Liu,Xiaoguang Qiao,Xinchang Pang
Tetraphenylethylene (TPE)-containing 4-amino-2,2,6,6-tetramethylpiperidine-1-oxyl (NH2-TEMPO) and 3-(((2-cyanopropan-2-yl)oxy)(cyclohexyl)amino)-2,2-dimethyl-3-phenylpropanenitrile (Dispolreg 007) were synthesized and utilized to mediate/initiate NMP in both homogeneous and heterogeneous polymerization systems. The introduction of TPE groups decreased the C–O bond dissociation energy (BDE) of NH2-TEMPO-St and led to more efficient NMP with a higher reaction rate, even at lower temperatures. Moreover, for both solution polymerization and miniemulsion polymerization, quantitative information of the polymerization process could be easily acquired with the naked eye without destroying the reaction system, by building the relationship between the increased photoluminescence (PL) intensity of the system and monomer conversion as well as the molecular weight (Mn).
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2020
·
IF 2.627
Xianfeng Liu,Fu Yang,Shuying Gao,Bo Shao,Shijian Zhou,Yan Kong
Design and synthesis of low cost and efficacious industrial catalyst for the oxidation of styrene has been an important research project. Herein, ZSM-5 zeolite containing tetrahedral vanadium (V) and Brønsted acid sites (V-H-ZSM-5) was prepared, and identified by characterizations such as XRD, SEM, UV–vis, NH 3 -TPD, H 2 -TPR N 2 -adsorption/desorption and FTIR. V-H-ZSM-5 performed extremely enhanced catalytic activity for the oxidation of styrene with 30% H 2 O 2 at 40 °C. Moreover, in-situ FTIR spectrum was used to investigate the catalytic mechanism. The results demonstrate that Brønsted acid site could not only increase the adsorption concentration of styrene in the micropores of V-H-ZSM-5 via the π complex interaction between double bond of styrene and Brønsted acid sites, but also increase the oxidation potential of H 2 O 2 . The synergetic action of tetrahedral vanadium (V) and Brønsted acid enhanced the catalytic activity for the oxidation of styrene with 30% H 2 O 2 . Impressively, V-H-ZSM-5 performed high reusability within five runs at a low reaction temperature (40 °C) for the first time.
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APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Fu Yang,Bo Shao,Xianfeng Liu,Shuying Gao,Xu Hu,Man Xu,Yun Wang,Shijian Zhou,Yan Kong
Multiple catalytic active centers tactically generated on the 2-dimentional catalytic carrier could afford certain promoting function thanks to their existed special synergy. Herein, Ni-based nanosheet-like metasilicate catalytic materials were developed as heterogeneous catalysts towards styrene oxidation for the first time. Concurrently, the special heteroatom cobalt or magnesium-incorporated Ni-based nanosheet-like metasilicate were developed together via the proposed synthesis tactics. The resulted sheet-like nanomaterials were meticulously characterized and identified through valid techniques. The introduction of heteroatom metal elements of cobalt or magnesium incorporated in the Ni-based nanosheet-like metasilicate was proven to trigger the regulated catalytic effect including positive and negative aspects towards styrene oxidation, and their function was identified and understood based on the reaction exploration results, in which the present cobalt significantly give rise to the promotive catalytic conversion activity and selectivity towards styreneoxide(conversion 96.8%, selectivity 78.4%), while the magnesium oppositely induced the restraining catalytic capacity(conversion 72%, selectivity 51.3%) on the Ni-based metasilicate compared with pure one. The obtained heterogeneous Ni-based metasilicate retain durable catalytic activity during five recycling for styrene oxidation and inherit the regulated catalytic performance in the substrate expansion.
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 32
·21398-21405
·
IF 10.7
Yi Yu,Meng Wang,Ying Wu,Hongxia Xi
Covalent organic frameworks (COFs) with permanent porosity, high structural stability and framework modifiability offer unique superiority for heterogeneous catalysis. Herein, we propose an in situ metallization strategy to construct a series of metal-functionalized 2D COFs (M/COFs, M = Co, Ni and Zn). The 2D matrix provides inherent accessible Lewis base sites, along with the introduced metal species acting as Lewis acid sites. These active sites with synergistic effects boost the catalytic CO2 conversion performance of these materials. Our results show that these M/COFs efficiently convert CO2 and olefins into cyclic carbonates through one-pot tandem catalysis. Specifically, Co/COFs achieve nearly complete styrene conversion and 85% yield of styrene carbonate without a co-catalyst at 80 °C and 1 bar. Simulation results further reveal the higher interaction energy of Co/COFs and guests and elucidate the underlying catalytic mechanisms of COF catalysts before and after modification. This work provides both scientific and applicational insights into designing high-performance metal-functionalized materials for optimal tandem catalytic performance.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-17
·
IF 14.7
Zheng Botuo,Zhong Liling,Wang Xiaoxiao,Lin Peiyao,Yang Zezhou,Bai Tianwen,Shen Hang,Zhang Huagui
Inverse vulcanization exploits S 8 to synthesize polysulfides. However, evolution of products and its mechanism during inverse vulcanization remains elusive. Herein, inverse vulcanization curves are obtained to describe the inverse vulcanization process in terms of three stages: induction, curing and over-cure. The typical curves exhibit a moduli increment before declining or plateauing, reflecting the process of polysulfide network formation and loosing depending on monomers. For aromatic alkenes, in the over-cure, the crosslinked polysulfide evolves significantly into a sparse network with accelerated relaxation, due to the degradation of alkenyl moieties into thiocarbonyls. The inverse vulcanization product of olefins degrades slowly with fluctuated relaxation time and modulus because of the generation of thiophene moieties, while the inverse vulcanization curve of dicyclopentadiene has a plateau following curing stage. Confirmed by calculations, the mechanisms reveal the alkenyl groups react spontaneously into thiocarbonyls or thiophenes via similar sulfur-substituted alkenyl intermediates but with different energy barriers.
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