硼碳氮氧複合物奈米結構之製備及其作為新型光觸媒之應用

近年來，無金屬奈米材料，如石墨氮化碳、氧化石墨烯及硼碳氮化物，由於其可調的能隙結構、優異的化學穩定性及眾多活性點，已成為克服金屬材料缺陷的新一代光觸媒材料。硼碳氮氧複合物(BCNO)最初被開發為無稀土金屬摻雜的奈米熒光材料，由於其可調的光致發光特性、高量子產率和長載子壽命，BCNO展現出作為高性能無金屬光觸媒的潛力。本碩士論文對兩個系列BCNO的製備、表徵與光催化活性進行了初步研究。通過改變前驅物成分、比例及加熱溫度，合成了兩種具有不同形貌和結構的BCNO，即：（1）BGH（胍系列）以及（2）BMH（三聚氰胺系列）。X光繞射圖譜(XRD)、傅立葉轉換紅外線光譜(FTIR)以及核磁共振圖譜(NMR)的分析都指出BGH如文獻所述，是由碳、氧摻雜的氮化硼組成，較高的退火溫度會導致BN骨架中有較多三配位點BNx(OH)3-x形成，此三配位點也在後續被證實為BGH主要的光催化活性點。相較之下，BMH則確定為硼、氮摻雜的氧化石墨結構，其在本論文所研究的BCNO中表現出最佳的光催化活性。BMH的光催化活性是由帶路易斯酸性的BNx(OH)3-x三配位點結合sp2混成C=C石墨結構所產生的協同作用造成的，較高退火溫度下，BN鍵的形成以及導電sp2混成C=C結構的消失會使BMH失去活性。此外，也發現了BN2(OH)2以及BN3鍵結的形成與本論文中無光催化活性的BCNO有極大的關聯。結構與特性之間更詳盡的研究發現將在本論文中深入討論。

關鍵字

光催化；無金屬光觸媒；硼碳氮氧複合物；染料降解；結構-特性關聯

並列摘要

Recently, metal-free nanomaterials, such as graphitic carbon nitride, graphene oxide, and boron carbon nitride, have emerged as promising candidates for photocatalysis to overcome limitations imposed by their metal-based counterparts due to their tunable bandgap, excellent chemical stability, and numerous active sites. Boron carbon oxynitride (BCNO) was initially developed as a non-rare-earth metal-doped nano phosphor. BCNO exhibits potential as a promising metal-free photocatalyst due to its tunable photoluminescent behavior, high quantum yield, and long charge carrier lifetime. In this Master Thesis, preliminary investigation on the preparation, characterization, and photocatalytic activity of two series of BCNO were investigated. By varying precursor sources, ratios, and annealing temperature, two series of BCNO with different morphologies and structures were synthesized, namely: (1) BGH (guanidine series) and (2) BMH (melamine series). X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), and nuclear magnetic resonance spectroscopy (NMR) analyses suggested that BGH consisted of carbon, oxygen-doped boron nitride, as reported in the literature. In this Thesis work, BCNO prepared at higher annealing temperature possessed higher composition of tricoordinate boron sites, BNx(OH)3-x, in the BN framework, which was later found to serve as one of the major catalytic sites in BGH. In contrast, the structure of BMH was determined to be boron, nitrogen-doped graphite oxide, which exhibited the highest photocatalytic activity among all the BCNO investigated in this Thesis. The high photocatalytic activity of BMH was induced by the synergistic effect of the Lewis acidic tricoordinate BNx(OH)3-x sites incorporated within the sp2 C=C graphitic domain. Higher temperature annealing of BMH leads to the formation of BN bonding and the disappearance of the conductive sp2 C=C network, which renders their inactivity. Furthermore, it was found that the formation of BN2(OH)2 and the formation of the tricoordinate BN3 bonding are shared among all inactive BCNO investigated in this Thesis. More detailed investigations of the structure-property relationship will be discussed throughout this Master Thesis.

並列關鍵字

Photocatalysis ； Metal-free photocatalyst ； Boron carbon oxynitride ； Dye degradation ； Structure-property relationship

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硼碳氮氧複合物奈米結構之製備及其作為新型光觸媒之應用

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