CHEMISTRY OF MATERIALS
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2020
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IF 9.567
Yangfan Lin,Jingwei Jiang,Yaguang Zhang,Xueqin He,Jianguo Ren,Peng He,Chunlei Pang,Chengmao Xiao,Deren Yang,Ning Du
The promoting effect of hydroxyls on a silicon surface on the decomposition of an electrolyte is studied by comparing the performance of silicon–hydroxyl (Si–OH) and silicon–alkyl (Si–C3H7) electrodes. X-ray photoelectron spectroscopy (XPS) characterization of solid electrolyte interphase (SEI) layers on both electrodes demonstrates the influencing mechanism that hydroxyls can react with LiPF6 to form POF3, which further induces the decomposition of the electrolyte solution. This study provides a new consideration that limiting the amount of hydroxyls on the silicon surface in an appropriate range is significant to the electrochemical performance of silicon-based anode materials.
研究领域:
材料科学
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电化学
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电池技术
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产品关联
DOI
高影响因子
FUEL
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2024
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IF 6.7
Jinhui Song,Tianfu Zhang,Mengjiao Xing,Junfeng Zhou,Lu Tang,Jiaxin Xie,Zimin Peng,Wenyao Gu,Jianyu Tang,Suyao Liu,Tong Chang,Yi Liu,Yiwen Fang
With the potential application of biomass-derived feedstock upgradation to sustainable aviation fuels, it is essential to enhance the hydroisomerization performance of ZSM-22 zeolite while improving its resistance to residual oxygen-containing compounds. As the defect sites in the ZSM-22 zeolite, the abundant Si-OH groups are closely related to the catalytic performance and stability, serving as the main attack sites for the generated water. In this work, liquid-mediated defect-healing treatment is performed to heal Si-OH to Si-O-Si, leading to the enhancement of the crystallinity and pore connectivity without affecting the Si/Al, micropore volume, and morphology and preventing the micropores blockage and dealumination caused by conventional silylation and silication procedures. The outcome of the declined Si-OH groups is the reduction of the Lewis acid site without altering the Brønsted acidity. In the n-dodecane hydroisomerization, the catalyst obtained by the liquid-mediated defect-healing treatment route shows an increased conversion and isomer yield compared to the parent and healed catalysts prepared by other healing methods. This is mainly due to enhanced confinement of the micropore void, resulting in decreased apparent activation energy and reduced yield to multi-branched isomers prone to cracking. Furthermore, the healed catalyst exhibits improved resistance and structure stability in the hydroisomerization of feedstocks containing butanol. The work provides a prospective application of ZSM-22 zeolite in the hydroisomerization for complex and severe reactants through the essential Si-OH healing method.
研究领域:
催化化学
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材料科学
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能源化学
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产品关联
DOI
高影响因子
MOLECULES
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2025
·Vol. 30
·期 16
·3319
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IF 4.6
Tong Chang,Renhui Deng,Jiaxin Xie,Jianyu Tang,Wenyao Gu,Zimin Peng,Suyao Liu
The abundant Si-OH groups serving as the defect sites in the ZSM-22 zeolite framework are not only closely associated with physicochemical properties and catalytic performance but are also the primary sites for attack by water molecules, thereby restricting applications involving or producing water. In the present study, a liquid-mediated healing process was used to convert the Si-OH groups in ZSM-22 zeolite into Si-O-Si bonds. The systematic investigation of the treatment solution’s composition and the hydrothermal conditions revealed that the crystallinity of ZSM-22 zeolite can be effectively enhanced following optimal healing treatment. Furthermore, the healed ZSM-22 zeolite exhibited enhanced ordering degree and pore connectivity without significant changes to the Si/Al and morphology. Moreover, the decline in Si-OH groups reduced the Lewis acid sites without altering the Brønsted acidity, which led to a slight decrease in the dispersion of Pt particles. In n-decane hydroisomerization, compared to the parent ZSM-22 zeolite catalyst, the healed catalyst demonstrates higher reactant conversion and increased isomer yield, attributing to its enhanced confinement within the micropore voids, which leads to a reduced yield of multi-branched isomers susceptible to cracking. This study presents a potential application of ZSM-22 zeolite in hydroisomerization for complex and challenging feedstocks.
研究领域:
催化化学
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材料科学
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化学工程
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石油化工
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沸石化学
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
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2026
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IF 6.6
Qian Li,Tong Yu,Tangze Deng,Jie Zhang,Jinwei Chen,Gang Wang,Zongbo Shi,Runsheng Zhuo,Ruilin Wang
Surface hydroxyl modulation on S-1 enables the rational design of PtCu catalyst. • Surface OH modulates particle surface density and promotes PtCu interaction. • The optimal 0.5Pt2Cu/S-1–950 demonstrated an approving PDH activity. Propane dehydrogenation (PDH) is a promising approach for propylene production. However, Pt-based catalysts suffer from severe coke deposition and metal sintering at high temperature, thus leading to a rapid deactivation and low propylene yield. Herein, a surface hydroxyl (OH) strategy is developed to modulate the dispersion and configuration of PtCu active sites on silicalite-1 (S-1). The precise regulation of OH density effectively optimizes the particle density of PtCu species. The properly introduced surface OH provides suitable sites to anchor the PtCu active sites with an enhanced catalytic activity and stability. The optimal 0.5Pt2Cu/S-1–950 catalyst achieves an initial propane conversion of 63.4%, propylene space–time yield of 0.60 g g cat. -1 h −1 , and exceptional long-term stability. Moreover, the catalyst also exhibits low coke formation rate with a total coke content of only 1.5 wt% after 6 h of reaction, thereby avoiding the coverage of active sites. The surface Si-OH-modulation offers an effective strategy for constructing high-efficiency Pt-based catalysts with an improved durability for propane dehydrogenation. Download: Download high-res image (111KB) Download: Download full-size image
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DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2026
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IF 5.4
Chenxiang Feng,Wei Jian,Agula Bao,Yang Dong
The massive accumulation of fly ash poses serious threats to the environment and land resources, making its effective utilization urgently needed. Although fly ash can be used to prepare silicon-carbon composites, the formation pathways of Si-OH/Si-O-C groups, the construction of Si-C bonds, and the regulation of microstructure remain unclear. In this study, a series of novel silicon-carbon composites (FAKXNY-Z) with unique microstructures were synthesized via high-temperature activation combined with hydrothermal crystallization, using fly ash and chitosan as raw materials. Among them, FAK2N2–150 exhibits a high specific surface area (1511.7 m 2 /g) and abundant active functional groups (Si-OH). This material achieves an adsorption capacity of 550.55 mg g −1 for tetracycline at room temperature. Density functional theory (DFT) calculations based on the experimental structure confirm its distinctive amorphous silica layer derived from sodalite collapse and reveal the adsorption mechanism toward tetracycline (TC), clarifying the strong affinity between Si-OH groups and TC molecules. This work not only provides a feasible strategy for the resource utilization of fly ash, but also offers theoretical support for the design of solid-waste-based functional adsorbents.
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产品关联
DOI
高影响因子
Surfaces and Interfaces
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2024
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IF 5.7
Zihan Zhou,Yunwen Wu,Silin Han,Tao Hang,Huiqin Ling,Jie Guo,Su Wang,Ming Li
3D NAND is one of the most promising storage devices due to its high storage density and low energy consumption. Selective wet etching of Si 3 N 4 by hot-concentrated phosphoric acid (PA) solution is a key process for 3D NAND fabrication. However, the channel material, polycrystalline silicon (poly-Si), is unexpectedly dissolved due to its inevitable exposure to the PA etching solution, which causes device failure and thus limits the stacking density of 3D NAND. Herein, to avoid the detrimental dissolution of poly-Si, we unveil the mechanism of poly-Si dissolution in PA solution from kinetic and thermodynamic perspectives. We find that the etch process shows a two-stage reaction, in which H 2 O plays a key role in lowering the activation barrier for poly-Si etching. Further thermodynamic analysis demonstrates that poly-Si prefers to be oxidized by H 2 O to suboxide rather than to SiO 2 . Combined with surface chemistry characterization, we propose the dissolution mechanism as a two-stage process involving the dissolution of suboxide interface and bulk poly-Si, where the nucleophilic substitution of Si–H with Si–OH on bulk poly-Si surface determines the overall etch rate. This study advances the 3D NAND development by establishing a theoretical foundation for identifying and implementing efficacious strategies to impede detrimental dissolution.
研究领域:
半导体器件
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材料科学
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纳米技术
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化学工程
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DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2020
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IF 4.551
Yue Wei,Gang Li,Jiaxu Liu,Yanhui Yi,Hongchen Guo
The sluggish interfacial mass transfer usually hinders the achievement of high-efficiency catalytic transformation of biomass, especially for solvent-free immiscible reagent systems. Herein, amphiphilic hybrid Ti-containing catalysts in situ incorporated with organic groups (Cn-Ti-HMS) were developed for boosting biphasic solvent-free epoxidation of methyl oleate (MO) with H 2 O 2 . Benefiting from the mutual effect between organic/inorganic precursors, the resulting low-defect catalysts exhibit well-mediated surface hydrophilic/hydrophobic balance and porosity by incorporating alkyl groups. Such mediation effect exhibits two superiorities: i) accelerated adsorption of reactants by amphiphilicity; ii) boosted substrate or product diffusion by porosity property. As such, remarkably promoted catalytic properties were achieved when compared with conventional Ti-HMS. Typically, methyl-functionalized C1–Ti-HMS-50 displays the optimal catalytic performance with a 95% conversion of MO. Further mechanism study recognizes the dominant role of surface wettability and Si–OH defects content in influencing MO conversion and epoxidized MO selectivity.
研究领域:
催化
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材料科学
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化学工程
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环境化学
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DOI
高影响因子
危险品化学品经营许可证（带存储）