GC×GC-TOFMS analysis of ethanodiamondoids in Ordovician oil from well SN1, Tarim Basin
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摘要: 运用全二维气相色谱—飞行时间质谱方法（GC×GC-TOFMS）从塔里木盆地顺托果勒地区顺南1井奥陶系原油中定量检测到81个1~3笼的乙基桥键金刚烷化合物，包括47个乙基桥键单金刚烷化合物，总含量为27 594.0 μg/g；32个乙基桥键双金刚烷化合物，总含量为4 415.1 μg/g；2个乙基桥键三金刚烷系列化合物，总含量为16.8 μg/g；建立了金刚烷—乙基桥键金刚烷的二维色谱保留指数图版。结果显示，金刚烷类和乙基桥键金刚烷类化合物保留时间位置具有如下关系：单金刚烷系列 < 乙基桥键单金刚烷系列 < 双金刚烷系列 < 乙基桥键双金刚烷系列 < 三金刚烷系列 < 乙基桥键三金刚烷系列 < 四金刚烷系列。作为石油中热稳定性最高的饱和烃类，乙基桥键金刚烷化合物的定量分析结果，有望为原油裂解和硫酸盐热化学还原反应（TSR）等油藏次生改造作用提供新的指标。
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关键词:
- 乙基桥键金刚烷 /
- 全二维气相色谱—飞行时间质谱 /
- 奥陶系 /
- 顺南1井 /
- 塔里木盆地
Abstract: By 2D gas chromatography and time-of-flight mass spectrometry (GC×GC-TOFMS), 81 ethanodiamondoids with 1-3 cages were detected quantitatively in Ordovician crude oil from well SN1, Shuntuoguole area, Tarim Basin, including 47 ethanoadamantanes with total content of 27 594.0 μg/g, 32 ethanodiamantanes with total content of 4 415.1 μg/g, and 2 ethanotriamantanes with total content of 16.8 μg/g. The template of 2D chromatogram retention index of diamondoids-ethanodiamondoids was constructed. The results demonstrated that the position of retention time of diamondoids and ethanodiamondoids has the following relationship, namely, adamantanes < ethanoadamantanes < diamantanes < ethanodiamantanes < triadamantanes < ethanotriamantanes < tetradamantanes. Quantitative analytical result of ethanoadamantanes as saturated hydrocarbons with the highest thermal stability in crude oil, is expected to provide new indexes for secondary reservoir reconstruction, i.e. crude oil cracking and thermochemical sulfate reduction (TSR).-
Key words:
- ethanodiamondoids /
- GC×GC-TOFMS /
- Ordovician /
- well SN1 /
- Tarim Basin
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图 1 金刚烷、乙基桥键金刚烷化学结构
Figure 1. Chemical structures of diamondoids and ethanodiamondoids
图 2 塔里木盆地顺托果勒地区顺南1井(SN1)构造位置
Figure 2. Structural location of well SN1 in Shuntuoguole area, Tarim Basin
图 3 塔里木盆地顺托果勒地区顺南1井原油GC×GC-TOFMS总离子流图
Figure 3. TIC (total ion chromatogram) by GC×GC-TOFMS of crude oil from well SN1, Shuntuoguole area, Tarim Basin
图 4 塔里木盆地顺托果勒地区顺南1井原油中乙基桥键金刚烷GC×GC—TOFMS点阵图
a.乙基桥键单金刚烷系列；b.乙基桥键双金刚烷系列；c.乙基桥键三金刚烷系列
Figure 4. GC×GC-TOFMS lattice diagram of ethanodiamondoids in crude oil from well SN1, Shuntuoguole area, Tarim Basin
图 5 塔里木盆地顺托果勒地区顺南1井原油中乙基桥键单金刚烷系列化合物质谱图
Figure 5. Mass spectrum of ethanoadamantanes in crude oil from well SN1, Shuntuoguole area, Tarim Basin
图 6 塔里木盆地顺托果勒地区顺南1井原油中乙基桥键双金刚烷化合物质谱图
Figure 6. Mass spectrum of ethanodiamantanes in crude oil from well SN1, Shuntuoguole area, Tarim Basin
图 7 塔里木盆地顺托果勒地区顺南1井原油乙基桥键三金刚烷化合物质谱图
Figure 7. Mass spectrum of ethanotriamantanes in crude oil from well SN1, Shuntuoguole area, Tarim Basin
图 8 塔里木盆地顺托果勒地区顺南1井原油金刚烷和乙基桥键金刚烷保留时间
Figure 8. Retention time of diamondoids and ethanodiamondoids in crude oil from well SN1, Shuntuoguole area, Tarim Basin
表 1 塔里木盆地顺托果勒地区顺南1井原油中乙基桥键金刚烷定性和定量结果
Table 1. Qualitative and quantitative analysis results of ethanodiamondoids in crude oil from well SN1, Shuntuoguole area, Tarim Basin
序号 峰号 化合物名称 分子式 一维保留时间/s 二维保留时间/s 定量质量数 含量/(μg·g-1) 0 I.S.-1 D16-金刚烷 C10D16 1 796 1.41 152 332.9 1 EA-1 乙基桥键单金刚烷 C12H18 2 484 1.83 162 424.8 2 EA-2 1-甲基-乙基桥键单金刚烷 C13H20 2 524 1.65 161 737.4 3 EA-3 6-甲基-乙基桥键单金刚烷 C13H20 2 564 1.69 161 2 269.6 4 EA-4 2-甲基-乙基桥键单金刚烷 C13H20 2 596 1.77 161 833.8 5 EA-5 C1-乙基桥键单金刚烷 C13H20 2 620 1.74 161 77.5 6 EA-6 C1-乙基桥键单金刚烷 C13H20 2 676 1.83 161 314.7 7 EA-7 C1-乙基桥键单金刚烷 C13H20 2 700 1.88 161 87.4 8 EA-8 C2-乙基桥键单金刚烷 C14H22 2 884 1.77 161 402.8 9 EA-9 C2-乙基桥键单金刚烷 C14H22 2 892 1.81 161 477.2 10 EA-10 C2-乙基桥键单金刚烷 C14H22 2 596 1.51 175 2 196.1 11 EA-11 C2-乙基桥键单金刚烷 C14H22 2 636 1.55 175 1 713.5 12 EA-12 C2-乙基桥键单金刚烷 C14H22 2 660 1.56 175 358.9 13 EA-13 C2-乙基桥键单金刚烷 C14H22 2 668 1.64 175 930.3 14 EA-14 C2-乙基桥键单金刚烷 C14H22 2 692 1.57 175 668.5 15 EA-15 C2-乙基桥键单金刚烷 C14H22 2 700 1.59 175 1 139.1 16 EA-16 C2-乙基桥键单金刚烷 C14H22 2 700 1.7 175 153.7 17 EA-17 C2-乙基桥键单金刚烷 C14H22 2 716 1.64 175 733.0 18 EA-18 C2-乙基桥键单金刚烷 C14H22 2 740 1.66 175 1 794.8 19 EA-19 C2-乙基桥键单金刚烷 C14H22 2 756 1.66 175 715.7 20 EA-20 C2-乙基桥键单金刚烷 C14H22 2 772 1.72 175 452.5 21 EA-21 C2-乙基桥键单金刚烷 C14H22 2 780 1.79 175 375.5 22 EA-22 C2-乙基桥键单金刚烷 C14H22 2 796 1.73 175 706.9 23 EA-23 C2-乙基桥键单金刚烷 C14H22 2 812 1.76 175 505.8 24 EA-24 C2-乙基桥键单金刚烷 C14H22 2 836 1.79 175 150.9 25 EA-25 C2-乙基桥键单金刚烷 C14H22 2 852 1.82 175 357.1 26 EA-26 C2-乙基桥键单金刚烷 C14H22 2 908 1.91 175 156.3 27 EA-27 C3-乙基桥键单金刚烷 C15H24 2 684 1.45 189 493.2 28 EA-28 C3-乙基桥键单金刚烷 C15H24 2 716 1.46 189 345.8 29 EA-29 C3-乙基桥键单金刚烷 C15H24 2 724 1.41 189 1 261.2 30 EA-30 C3-乙基桥键单金刚烷 C15H24 2 732 1.5 189 141.2 31 EA-31 C3-乙基桥键单金刚烷 C15H24 2 764 1.47 189 931.0 32 EA-32 C3-乙基桥键单金刚烷 C15H24 2 804 1.51 189 388.9 33 EA-33 C3-乙基桥键单金刚烷 C15H24 2 828 1.61 189 188.8 34 EA-34 C3-乙基桥键单金刚烷 C15H24 2 844 1.56 189 763.4 35 EA-35 C3-乙基桥键单金刚烷 C15H24 2 852 1.59 189 1 069.3 36 EA-36 C3-乙基桥键单金刚烷 C15H24 2 860 1.59 189 277.5 37 EA-37 C3-乙基桥键单金刚烷 C15H24 2 868 1.56 189 457.6 38 EA-38 C3-乙基桥键单金刚烷 C15H24 2 884 1.65 189 271.9 39 EA-39 C4-乙基桥键单金刚烷 C16H26 2 740 1.26 203 211.5 40 EA-40 C4-乙基桥键单金刚烷 C16H26 2 764 1.29 203 634.2 41 EA-41 C4-乙基桥键单金刚烷 C16H26 2 828 1.43 203 51.2 42 EA-42 C4-乙基桥键单金刚烷 C16H26 2 852 1.46 203 439.4 43 EA-43 C4-乙基桥键单金刚烷 C16H26 2 860 1.47 203 194.8 44 EA-44 C4-乙基桥键单金刚烷 C16H26 2 892 1.44 203 222.7 45 EA-45 C4-乙基桥键单金刚烷 C16H26 2 964 1.52 203 427.8 46 EA-46 C5-乙基桥键单金刚烷 C17H28 2 860 1.17 217 75.9 47 EA-47 C5-乙基桥键单金刚烷 C17H28 2 916 1.2 217 13.2 48 ED-1 乙基桥键双金刚烷 C16H22 3 452 2.53 214 260.5 49 ED-2 乙基桥键双金刚烷 C16H22 3 540 2.62 214 52.6 50 ED-3 C1-乙基桥键双金刚烷 C17H24 3 468 2.27 213 103.9 51 ED-4 C1-乙基桥键双金刚烷 C17H24 3 476 2.25 213 197.4 52 ED-5 C1-乙基桥键双金刚烷 C17H24 3 500 2.32 213 322.6 53 ED-6 C1-乙基桥键双金刚烷 C17H24 3 532 2.41 213 129.3 54 ED-7 C1-乙基桥键双金刚烷 C17H24 3 556 2.45 213 115.1 55 ED-8 C1-乙基桥键双金刚烷 C17H24 3 564 2.32 213 85.9 56 ED-9 C1-乙基桥键双金刚烷 C17H24 3 604 2.49 213 41.8 57 ED-10 C1-乙基桥键双金刚烷 C17H24 3 620 2.6 213 72.5 58 ED-11 C1-乙基桥键双金刚烷 C17H24 3 636 2.57 213 33.2 59 ED-12 C1-乙基桥键双金刚烷 C17H24 3 652 2.57 213 101.8 60 ED-13 C1-乙基桥键双金刚烷 C17H24 3 676 2.54 213 29.5 61 ED-14 C1-乙基桥键双金刚烷 C17H24 3 684 2.65 213 53.1 62 ED-15 C1-乙基桥键双金刚烷 C17H24 3 692 2.6 213 27.1 63 ED-16 C2-乙基桥键双金刚烷 C18H26 3 772 2.38 213 49.4 64 ED-17 C2-乙基桥键双金刚烷 C18H26 3 780 2.43 213 57.5 65 ED-18 C2-乙基桥键双金刚烷 C18H26 3 476 1.95 227 312.9 66 ED-19 C2-乙基桥键双金刚烷 C18H26 3 524 2.06 227 125.6 67 ED-20 C2-乙基桥键双金刚烷 C18H26 3 548 2.14 227 148.7 68 ED-21 C2-乙基桥键双金刚烷 C18H26 3 564 2.19 227 165.8 69 ED-22 C2-乙基桥键双金刚烷 C18H26 3 596 2.21 227 111.2 70 ED-23 C2-乙基桥键双金刚烷 C18H26 3 628 2.21 227 97.2 71 ED-24 C2-乙基桥键双金刚烷 C18H26 3 652 2.26 227 303.7 72 ED-25 C2-乙基桥键双金刚烷 C18H26 3 700 2.38 227 149.4 73 ED-26 C2-乙基桥键双金刚烷 C18H26 3 724 2.45 227 119.5 74 ED-27 C2-乙基桥键双金刚烷 C18H26 3 756 2.41 227 128.5 75 ED-28 C2-乙基桥键双金刚烷 C18H26 3 788 2.51 227 311.7 76 ED-29 C3-乙基桥键双金刚烷 C19H28 3 492 1.75 241 272.4 77 ED-30 C3-乙基桥键双金刚烷 C19H28 3 572 1.88 241 59.8 78 ED-31 C3-乙基桥键双金刚烷 C19H28 3 748 2.21 241 249.4 79 ED-32 C3-乙基桥键双金刚烷 C19H28 3 796 2.21 241 126.3 80 ET-1 乙基桥键三金刚烷 C20H26 4 276 3.3 266 11.4 81 ET-2 C1-乙基桥键三金刚烷 C21H28 4 348 3.15 265 5.5 
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