Unique Structure and Surface-Interface Reactivity of Nanostructured Minerals
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摘要: 纳米矿物是纳米地球科学（Nanogeoscience）的核心研究对象之一.鉴于"纳米矿物"的概念在实际运用时较宽泛，有时与经典定义不符，建议用"纳米结构矿物"代替"纳米矿物"，并简析了纳米结构矿物（Nanostructured Minerals）的概念.以管状纳米结构矿物（埃洛石和伊毛缟石）、球状纳米结构矿物（水铝英石）、层间纳米结构矿物（蒙脱石和伊/蒙混层矿物）和多孔纳米结构矿物（硅藻质蛋白石）为例，分析了纳米结构矿物的结构、表面基团的特殊性及其所衍生的特殊界面反应性，讨论了它们对矿物资源利用和油气生成等地球物质循环过程的重要意义.Abstract: Research on naturally occurring nanosized minerals is a central domain of Nanogeoscience. However, the use of the concept "Nanominerals" is acutally not as strict as it is supposed, i.e., sometimes the use of the concept is inconsistent with the classical definition of "Nanominerals". In this paper, the concept "Nanostructured Minerals" is proposed to replace the concept "Nanominerals", and a brief description on the suggested concept, as well as a related discussion, is given. A definition of the term nanostructured minerals is proposed and discussed. Exemplified by the tubular nanostructured minerals (halloysite and imogolite), the globular nanostructured mineral (allophane) and the porous nanostructured mineral (diatomaceous opal-A), the unique structure and surface-interface reactivity of nanostructured minerals are comprehensively discussed. The role of the above-mentioned uniqueness in the applications of the nanostructured minerals is summarized. In addition, the functions of the interlayer nanostructure exhibited by some nanostructured minerals such as montmorillonite on the earth matter circle (hydrocarbon generation and shale gas storage) are discussed.
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图 1 (a) 埃洛石层间结构和(b)埃洛石纳米管结构示意
Fig. 1. Schematic diagram of crystalline structure of halloysite (a) and structure of halloysite particle (b)
图 2 不同产地埃洛石TEM图
a.新西兰Matauri Bay；b.澳大利亚Te Puke；c.澳大利亚Kalgoorlie；d.新西兰Opotiki；e.澳大利亚Camel Lake；f.新西兰Northland；g.美国Atlas Mine；h.中国贵州大方.据Joussein(2016)及本研究组前期工作(Yuan et al., 2008)
Fig. 2. TEM images of halloysite sourced from different mines
图 3 Hal-1100的TEM图(a~d)和Hal-700，Hal-800，Hal-900，Hal-700/D，Hal-800/D，Hal-700/M的漫反射红外光谱图(e~j)
Fig. 3. TEM images of Hal-1100 (a-d) and DRIFT spectra of Hal-700, Hal-800, Hal-900, Hal-700/D, Hal-800/D, Hal-700/M (e-j)
图 4 有机硅烷与埃洛石内腔表面羟基反应机制示意
据Yuan et al.(2008)；a.低度聚合的硅烷通过多种作用力与内腔表面羟基形成交联结构；b.硅烷水解产物硅醇直接嫁接于表面羟基
Fig. 4. Schematic representation of the proposed reaction mechanism between organic silane and inner surface hydroxyl of halloysite
图 5 埃洛石表面断裂的TEM图(a)和埃洛石边缘和表面缺陷的AFM图(b~c)
Fig. 5. TEM image of the surface breakage of halloysite (a) and AFM images of the edges and surface defects of halloysite (b-c)
图 6 埃洛石管状端部附着的纳米级稀土矿物颗粒的形貌图及其EDX谱图
Fig. 6. Morphology of nano-sized REE grains attached on polar ends of halloysite tubes and EDX spectrum
图 7 伊毛缟石和水铝英石的结构与形貌
a, b, d, f, g.据本组未发表数据；c, e.据Levard et al.(2012)和Bishop et al.(2013).a.伊毛缟石结构示意图；b.合成伊毛缟石的AFM图；c.伊毛缟石和水铝英石结构单元示意图；d.天然水铝英石矿样；e.水铝英石结构示意图；f, g.合成水铝英石的STEM和AFM图
Fig. 7. Structure and morphology of imogolite and allophane
图 9 伊毛缟石六方堆积形成的管束示意
据Bonelli(2016).A、B和C是其中一管束对应的孔
Fig. 9. Ideal representation of three bundles formed by imogolite organized into a nearly hexagonal packing
图 10 硅藻质蛋白石表面羟基和吸附水类型、脱羟过程及硅烷接枝反应机理示意
Fig. 10. A schematic representation of the types of proton species on diatom-silica surface, the process of dehydroxylation and the roles of hydroxyl species in silylation reaction
图 11 不同温度热处理后的硅藻质蛋白石与三甲基氯硅烷发生接枝反应产物的1H MAS NMR谱(a)以及热处理硅藻质蛋白石与γ-氨丙基三乙氧基硅烷接枝反应产物的热重曲线(b)
PD.硅藻质蛋白石；PD-T.接枝反应产物；样品名中的数字为热处理温度(℃)；TG曲线表示质量与温度的关系；DTG曲线表示失重速率与温度的关系.a.据Yuan et al.(2006)；b.据Yuan et al.(2013a)
Fig. 11. 1H MAS NMR spectra of silylated diatom-silica samples (a) and TG and DTG curves of the γ-aminopropyl triethoxysilane-modified diatom-silica sample (b)
图 12 纳米磁铁矿(a)均匀负载于硅藻蛋白石(b)表面后所形成的硅藻蛋白石-磁铁矿复合体(c~h)的透射电镜(TEM)图
据Yuan et al.(2010).a.磁铁矿纳米颗粒；b.硅藻质蛋白石；c~h.硅藻质蛋白石-磁铁矿复合物的TEM图
Fig. 12. TEM images of magnetite nanoparticles (a); diatom-silica (b) and diatom-silica/magnetite nanocomposites (c-h)
图 13 舟形藻起源硅藻质蛋白石经聚焦离子束-能量色散X射线谱(FIB)局部刻蚀后的硅(a)和铝(b)的元素分布
据本研究组未发表数据
Fig. 13. Si (a) and Al (b) elemental distribution of diatomaceous silica originated from Navicula sp. after FIB etching
图 14 硅藻蛋白石及硅藻蛋白石基多孔炭的扫描电镜图、透射电镜图及模板炭对亚甲基蓝的吸附等温线
据Liu et al.(2010, 2012).a~f.圆筛藻起源硅藻质蛋白石及利用其固体酸性制备的多孔炭：a.单颗粒硅藻质蛋白石的扫描电镜图；b.多孔炭的柱状形貌扫描电镜图；c.多孔炭的有序大孔排列扫描电镜图；d.有序的大孔炭形貌透射电镜图；e.炭柱形貌透射电镜图(插入部分为选区电子衍射图)；f.炭柱中的介孔结构透射电镜图(插入部分为放大后的微孔结构)；g.舟船藻起源硅藻质蛋白石所制备的多孔炭扫描电镜图(插入部分为炭管放大图)；h.不同硅藻起源硅藻质蛋白石所制备多孔炭的亚甲基蓝吸附等温线
Fig. 14. The SEM, TEM of diatomceous silica of coscinodiscus sp. and porous carbon prepared by its solid acidity and methylene blue adsorption isotherms of different porous carbons
图 15 蒙脱石表面可能的固体酸性来源示意
B site.B酸位；L site.L酸位.据Bu et al.(2017)
Fig. 15. Schematic representation of the possible sources of solid acid sites of montmorillonite
图 16 ALA及蒙脱石-ALA层外复合体(Mt-ALA)和层间复合体(Mtinter-ALA)的3D红外光谱图和高压封闭体系下的总气态烃产率(∑C1-5)，CO2产率和及异构烃/正构烃比值
a~c.据Liu et al.(2013b)；d~f.据Yuan et al.(2013b).a.ALA的3D红外光谱图；b~c.层外复合体(Mt-ALA)和层间复合体(Mtinter-ALA)的3D红外光谱图；d.高压封闭体系下ALA及其蒙脱石层外(Mt-ALA)和层间复合体(Mtinter-ALA)的总气态烃产率(∑C1-5)；e.CO2产率；f.异构烃/正构烃比值
Fig. 16. 3D FTIR spectrum and the total gaseous hydrocarbon (∑C1-5) and CO2 of ALA and the external clay-OM complex (Mt-ALA) and the interlayer clay-OM complex (Mtinter-ALA) in the high pressure closed system and the ratios of iso-alkanes/n-alkanes
图 17 纯相有机质热解(a)和蒙脱石层间有机质热解(b)
据Bu et al.(2017).a.纯相有机质热解以亲核反应为主；b.蒙脱石层间有机质热解以霍夫曼消除反应为主
Fig. 17. Schematic representation of the processes of Nucleophilic substitution reaction in the pyrolysis of pure OM (OTAB) (a) and Hoffmann elimination reaction in the pyrolysis of the interlayer clay-OM complex (Mtinter-OTAB) (b)
图 18 蒙脱石(Mt)、高岭石(Kaol)、累托石(Rt)和伊利石(Il)的甲烷吸附曲线(a)和蒙脱石热处理产物的甲烷吸附曲线(b)
a.据Liu et al.(2013c)及部分未发表数据；b.据Liu et al.(2013c)
Fig. 18. The adsorption isotherms of CH4 on montmorillonite (Mt), kaolinite (Kaol), rectorite (Rt) and illite (Il) (a) and Mt and its heated products (b)
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