以溶劑裂解合成中孔洞氧化石墨烯及其摻雜之應用

Abstract

本研究以溶劑熱裂解法生長氧化石墨烯於中孔洞沸石表面，並利用酸性官能基調控並催化氧化石墨烯之生成。使用高比表面積（800-900 m2/g）、同時具中孔（5-6 nm）及微孔（<1 nm）的沸石奈米粒子（MZNs）作為生長模板及催化劑，比較化學氣相沉積法在高溫（825°С）氬氣環境下乙烯及四氫呋喃裂解的效應。沸石表面之布洛酸性位點及微孔結構的空間限制效應可生成穩定的碳自由基，所合成出中孔洞氧化石墨烯奈米粒子（MGNs）不僅可作為光致類芬頓反應催化劑有效降解有機染料，並可塗布於網印碳電極（SPCE）上，利用碘摻雜及預還原的方式調控在電化學中的感測。溶劑熱裂解法具有經濟碳源優勢、可大量合成及多樣選擇性且避免錳汙染、板模移除等優勢，並符合綠色化學原則中衍生物減少、降解設計及低毒性的溶劑選擇，為孔洞碳材提供便利合成、有效降解及電化學檢測之應用。In this study, few-layer graphene oxides were grown on mesoporous zeolite surface by thermal solvent-cracking method, regulated and catalyzed by acid functional groups. Pyrolysis of ethylene and tetrahydrofuran via chemical vapor deposition (825°С) in argon atmosphere was conducted over mesoporous zeolite nanoparticles (MZNs) as hard templates and catalysts that have intrinsic high surface area (800-900 m2/g), mesoporous (5-6 nm) and microporous (<1 nm) .Space confinement effect of micropores and Brønsted-Lowry acid of Al sites in zeolites can generate stable carbon radicals in mesoporous graphene-oxide nanoparticles (MGNs) which can be applied to photo-Fenton catalysts for organic-dye degradation, electrochemistry sensing materials after iodine doping, as well as pre-reduced electrodes as active screen-printed carbon electrodes (SPCE). The thermal solvent-cracking method has several advantages of economical carbon sources, large-scale synthesis and solvent selectivity, not only avoiding manganese contamination and pore blocking without hard-template removal but also matching principles of green chemistry, including reduced derivatives, designed degradation, and low-toxic solvent usage. Radical-based MGNs in merit of graphene-oxide growths provide alternative synthesis of photocatalysis and electrical materials.