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ADVANCED FUNCTIONAL MATERIALS · 2020 ·Vol. 30 ·期 36 ·2002488 · IF 16.836

An Efficient Emulsion-Induced Interface Assembly Approach for Rational Synthesis of Mesoporous Carbon Spheres with Versatile Architectures

Xuanyu Yang,Penghao Lu,Lei Yu,Panpan Pan,Ahmed A. Elzatahry,Abdulaziz Alghamdi,Wei Luo,Xiaowei Cheng,Yonghui Deng

Mesoporous carbon matrix with open pore structure, short diffusion length, and large pore size can favor the in-pore immobilization of active species and facilitate mass diffusion during catalytic reactions. However, a great difficulty still remains on controllable synthesis of uniform mesoporous carbon spheres with these structural characteristics. Herein, using amphiphilic Pluronic F127 as the surfactant, 1,3,5-trimethyl benzene (TMB) as the pore swelling and interface-adjusting agent, and dopamine as the carbon source, a robust emulsion-induced interface assembly approach for rational synthesis of mesoporous carbon spheres is demonstrated. The interface assembly process, including dopamine polymerization and fusion of TMB/F127/dopamine emulsions, can be regulated by tuning the dosage of dopamine and ammonia water, resulting in mesoporous carbon spheres with tunable pore sizes and versatile architectures, such as vesicles, walnut shapes, spheres with dendritic-like 3D radially aligned mesochannels (RA-MC), and isolated spherical mesopores. Moreover, the derived RA-MC is used as a promising matrix to immobilize ultra-small Au nanoparticles (≈3 nm). The Au/RA-MC exhibits no mass diffusion limitations in reduction of 4-nitrophenol, showing high conversion efficiency and good recyclability. This work paves a new avenue for controllable synthesis of mesoporous carbon spheres with well-developed mesoporosity and architectures and their application as novel heterogeneous catalysts.

CAS / MDL: 16903-35-8 16940-66-2
研究领域: 材料科学 · 催化化学
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Catalysis Science & Technology · 2016 ·Vol. 6 ·期 12 ·4503-4510 · IF 5.287

Reactivity and mechanism investigation of selective hydrogenation of 2,3,5-trimethylbenzoquinone on in situ generated metallic cobalt

Diefeng Su,Zhongzhe Wei,Shanjun Mao,Jing Wang,Yi Li,Haoran Li,Zhirong Chen,Yong Wang

Efficient and inexpensive catalysts are urgently desired for the hydrogenation of 2,3,5-trimethylbenzoquinone (TMBQ) to 2,3,5-trimethylhydroquinone (TMHQ), a key vitamin-E intermediate. In this study, a one-step method was developed to synthesize uniform cobalt-based NPs supported on porous nitrogen-doped carbon for the hydrogenation of TMBQ to TMHQ. The as-prepared catalyst shows a high yield (>90%) and selectivity (>99%) for TMBQ hydrogenation as well as α,β-unsaturated carbonyls. The satisfactory performance is attributed to the small particle size and homogeneous distribution. Meanwhile, metallic Co is proved to be responsible for the catalytic activity. Furthermore, density functional theory calculation discloses that the excellent chemoselectivity towards TMBQ is due to the preference for a desorption process over sequential hydrogenation of TMHQ. This novel material has great potential as a non-precious-metal catalyst for heterogeneous hydrogenation processes, due to its outstanding catalytic performance, simple preparation method and low production cost.

研究领域: 催化化学 · 材料科学 · 理论计算
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ATMOSPHERIC ENVIRONMENT · 2025 · IF 3.7

Heterogeneous Oxidation of Sulfur Dioxide by Organic Peroxides in 1,3,5-Trimethylbenzene-derived Secondary Organic Aerosol: Kinetics and Formation of Inorganic and Organic Sulfates

Min Yao,Yong Zhang,Chongxuan Chang,Wenbo Huang,Haiping Luo,Yufeng Jiang,Chenxi Li,Yue Zhao

The heterogeneous oxidation of sulfur dioxide (SO 2 ) by organic peroxides (POs) in aerosol represents an important pathway for atmospheric sulfate formation. However, the reactivity of SO 2 with POs arising from anthropogenic sources and the resulting sulfate formation characteristics remain poorly understood. Here, we investigate the heterogeneous reaction of SO 2 with secondary organic aerosol (SOA) derived from the photooxidation of 1,3,5-trimethylbenzene (1,3,5-TMB), one of major precursors of anthropogenic SOA. The reactive uptake coefficient (γ SO2 ) of SO 2 on 1,3,5-TMB-derived SOA was determined to be on the order of 10 −4 , depending markedly on aerosol liquid water content and particulate PO concentration. The second-order reaction rate constant ( k obs ) between 1,3,5-TMB-derived POs and dissolved SO 2 is estimated to range between 352 and 3.3×10 4 M −1 s −1 at pH of 3 to 5, which are comparable to the k obs values previously determined for monoterpene-derived POs under similar conditions. Furthermore, 1,3,5-TMB-derived peroxides efficiently convert S(IV) into inorganic sulfate (30-88%) and organosulfates (12-70%). This study reveals the heterogeneous reactivity of anthropogenic SOA and POs towards SO 2 and allows for a more accurate assessment of the role of PO-SO 2 interactions in the formation and aging of secondary aerosol.

CAS / MDL: 7681-11-0
研究领域: 大气化学 · 环境科学 · 物理化学 · 气溶胶科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Mussel-inspired interface deposition strategy for mesoporous metal-phenolic nanospheres with superior antioxidative, photothermal and antibacterial performance

Youyou Feng,Gen Wang,Bingxi Feng,Ping Li,Jing Wei

Metal-phenolic networks (MPNs) have emerged as a versatile and multifunctional platform applied in bioimaging, disease treatment, electrocatalysis, and water purification. The synthesis of MPNs with mesoporous frameworks and ultra-small diameters (<200 nm), crucial for post-modification, cargo loading, and mass transport, remains a formidable challenge. Inspired by mussel chemistry, mesoporous metal-phenolic nanospheres (MMPNs) are facilely prepared by direct deposition of the metal-polyphenol complex on the interface of oil nano-droplets composed of block copolymers/1,3,5-trimethylbenzene followed by a spontaneous template-removal process. Due to the penetrable and stable networks, the oil nano-droplets gradually leak from the networks driven by shear stress during the stirring process. As a result, MMPNs are obtained without additional template removal procedures such as solvent extraction or high-temperature calcination. The materials have a large pore size (∼12.1 nm), uniform spherical morphology with a small particle size (∼99 nm), and a large specific surface area (49.8 m 2 g −1 ). Due to the abundant phenolic hydroxyl groups, the MMPNs show excellent antioxidative property. The MMPNs also have excellent photothermal property, whose photothermal conversion efficiency was 40.9 %. Moreover, the phenolic hydroxyl groups can reduce Ag + in situ to prepare Ag nanoparticles loaded MMPNs composites, which have excellent inhibition performance of drug-resistant bacteria biofilm.

CAS / MDL: 7647-14-5 56-81-5
研究领域: 材料科学 · 纳米技术 · 生物医学工程 · 化学 · 药学
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