Surface oxidation via water plasma for increased H2 permselectivity of Allylhydridopolycarbosilane (AHPCS)-derived SiC membranes

IF 8.4 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science Pub Date : 2024-11-17 DOI:10.1016/j.memsci.2024.123521

Gusni Sushanti , Shun Aoyama , Norihiro Moriyama , Hiroki Nagasawa , Masakoto Kanezashi , Toshinori Tsuru

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Abstract

The objective of this research was to enhance the H₂ permselectivity of Allylhydridopolycarbosilane (AHPCS)-derived membranes through water plasma (WP) modification and subsequent pyrolysis. The WP modification, applied for 10 s, significantly improved the surface properties of the membranes to form ≡ Si–H, leading to enhanced H₂ permselectivity. Pyrolysis at 500−700 °C further transformed the membranes into a dense ceramic structure while maintaining high permeability for He and H₂ (0.3–1 × 10⁻⁶ mol/(m² s Pa)), achieved a significant increase in the permeance ratios of conventional SiC membrane from approximately 20 to 300 for H₂/N₂ and from 80 to 500 for He/N₂. Structural evolution analyses via Water contact angle (WCA) and X-Ray photoelectron spectroscopy (XPS) confirmed significant surface oxidation of ≡ Si–H groups to silanol ones via WP and condensation via pyrolysis. These modifications resulted in a structure ≡ of Si–O–Si ≡ on the surface, but SiC in bulk had markedly higher selectivity and permeance than AHPCS membranes pristine and modified with other methods. This design offers excellent thermal and chemical resistance, particularly for small to mid-sized molecules like He and H₂.

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通过水等离子体进行表面氧化，提高烯丙基hydridopolycarbosilane (AHPCS) 衍生碳化硅膜的 H2 许可选择性

本研究的目的是通过水等离子体（WP）改性和随后的热解来提高烯丙基hydridopolycarbosilane（AHPCS）衍生膜的H2过选择性。经过 10 秒钟的水等离子体改性，膜的表面性质得到了显著改善，形成了≡Si-H，从而提高了对 H2 的选择性。500-700 °C 高温分解进一步将膜转化为致密的陶瓷结构，同时保持了对 He 和 H2 的高渗透率（0.3-1 × 10-6 mol/(m2 s Pa)），实现了传统 SiC 膜渗透率的显著提高，对 H2/N2 的渗透率从约 20 提高到 300，对 He/N2 的渗透率从 80 提高到 500。通过水接触角（WCA）和 X 射线光电子能谱（XPS）进行的结构演化分析证实，≡Si-H 基团通过可湿性粉末氧化成硅醇基团，并通过热分解缩聚成硅烷醇基团。这些改性导致表面形成了≡Si-O-Si ≡结构，但与原始的 AHPCS 膜和用其他方法改性的 AHPCS 膜相比，块状 SiC 的选择性和渗透性明显更高。这种设计具有出色的耐热性和耐化学性，特别是对 He 和 H2 等中小分子而言。

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来源期刊

Journal of Membrane Science 工程技术-高分子科学

CiteScore

17.10

自引率

17.90%

发文量

1031

审稿时长

2.5 months

期刊介绍： The Journal of Membrane Science is a publication that focuses on membrane systems and is aimed at academic and industrial chemists, chemical engineers, materials scientists, and membranologists. It publishes original research and reviews on various aspects of membrane transport, membrane formation/structure, fouling, module/process design, and processes/applications. The journal primarily focuses on the structure, function, and performance of non-biological membranes but also includes papers that relate to biological membranes. The Journal of Membrane Science publishes Full Text Papers, State-of-the-Art Reviews, Letters to the Editor, and Perspectives.