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化学进展 2019, Vol. 31 Issue (5): 654-666 DOI: 10.7536/PC181032 前一篇   后一篇

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指纹遗留时间的研究方法

王红娟, 时蜜, 田璐, 赵亮**(), 张美芹**()   

  1. 北京科技大学生物工程与传感技术研究中心 北京市生物工程与传感技术重点实验室 北京 100083
  • 收稿日期:2018-10-26 出版日期:2019-05-15 发布日期:2019-03-21
  • 通讯作者: 赵亮, 张美芹
  • 基金资助:
    国家自然科学基金项目(21775011); 国家自然科学基金项目(21727815); 国家自然科学基金项目(21675011)
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Methods for Studying the Age Determination of Fingermarks

Hongjuan Wang, Mi Shi, Lu Tian, Liang Zhao**(), Meiqin Zhang**()   

  1. Research Center for Bioengineering & Sensing Technology, Beijing Key Laborotary of Bioengineering & Sensing Technology, University of Science & Technology Beijing, Beijing 100083, China
  • Received:2018-10-26 Online:2019-05-15 Published:2019-03-21
  • Contact: Liang Zhao, Meiqin Zhang
  • About author:
    ** E-mail: (Meiqin Zhang);
    (Liang Zhao)
  • Supported by:
    work was suported by the National Natural Science Foundation of China(21775011); work was suported by the National Natural Science Foundation of China(21727815); work was suported by the National Natural Science Foundation of China(21675011)

自19世纪末期,指纹鉴定一直是世界上犯罪侦查中最有效的个体识别物证手段之一。但是,指纹遗留时间的确定至今仍是一个相对未开发的研究领域。指纹脊线的物理形貌特征和残留物的化学成分因遗留者、遗留客体和环境的不同而产生显著差异。而且,随着指纹存留条件和老化时间的不同,其物理特征和化学组成的分子种类及含量等也随之变化。研究指纹残留物的物理特征和起始化学组成以及随遗留时间的变化关系是法医科学研究的重点课题,不仅有利于发展新的指纹检测方法和技术,而且可以提升鉴别犯罪现场发现的指纹的相关性。本文主要讨论已发展的各种方法和技术,如液相色谱、荧光光谱、红外光谱、紫外-可见光谱、拉曼光谱、质谱和高分辨率成像等方法,以及这些方法在指纹残留物的物理特征和化学组成及其随遗留时间的变化关系的研究中取得的进展以及局限性。最后,对发展潜在更可靠的指纹遗留时间确定方法中面临的挑战和未来的发展趋势进行展望。

关键词： 刑侦化学, 指纹组成, 遗留时间确定, 老化, 影响因素

Since the end of the 19th century, fingermark identification has always been one of the most useful evidences of individual identification for criminal investigation worldwide. However, up to now the age determination of a fingermark remains a relatively unexplored area. The physical features of the fingermark ridges and chemical compositions of the fingermark residues vary remarkably with different donor characteristics, substrate properties and environmental variables. Moreover, the physical ridge features, molecular species and content of the chemical components in fingermark change dramatically with different storage factors and aging kinetics. Studying the ridge physical features, the initial chemical compositions of fingermark residues and their relationship with the fingermark age is a crucial topic in the forensic science field, because it contributes not only to the development of new fingermark detection approaches and techniques, but also to the correlating identification of fingermarks found at crime scenes. This review discusses the previous achievements of fingermark dating methods and techniques such as liquid chromatography, fluorescence spectroscopy, infrared spectroscopy, ultraviolet-visible spectroscopy, Raman spectroscopy, mass spectrometry and high-resolution imaging, and the limits for the application of such approaches in practice. Besides, the challenges and perspectives of developing a potentially more reliable methodology for fingermark age determination are described.

Key words: forensic chemistry, fingermark composition, age determination, aging, influence factors
()
表1 来源于指纹残留物中皮脂腺的目标化合物及其老化动力学[15,16]
Table 1 Target compounds from sebaceous identified in fingermark residue and aging kinetics[15,16]
Target compounds Content Aging kinetics
Free fatty acids 37.6% The concentration of unsaturated fatty acids decreases with time, such as C16 and C18 acids; they are sensitive to light
Triglycerides 25% Decomposition mechanisms are particularly complex,thermal decomposition yields alkanes, alkenes, alkadienes, aromatics and carboxylic acids
Wax esters 21% Wax esters are saturated lipids, further research is required to explore their degradation products
Squalene 14.6% Squalene decreases rapidly over time,it decays more faster in ambient light conditions
Cholesterol 3.8% The concentration decreases over time, the rate of reduction is affected by the substrate
图1 指纹遗留时间评估的步骤图:A)用365 nm光照射的指纹的自发荧光图像。 B)Tryp和FOX荧光发射光谱。蓝线:283 nm激发,红线:365 nm激发。 阴影区域:FOXfl区域的积分面积。C)将B)中测量的Tryp荧光发射光谱(蓝线)进行拟合。D) ?:老化指纹Trypfl/FOXfl的比例,黑线:拟合老化曲线[49]
Fig. 1 Fingermark age-estimation procedure . A) Autofluorescence image of a fingermark illuminated with 365 nm light. B) Tryp and FOX fluorescence emission spectra. Blue line: excitation at 283 nm, red line: excitation at 365 nm. Shaded area: integrated area for FOXfl determination. C) Fit of reference fluorescence emission spectrum (lavender line) to the measured Tryp fluorescence emission spectrum (blue line) as shown in (B). D)?: Trypfl/FOXfl ratio of an aging fingermark, black line: fitted aging curve. Reprinted with permission from ref 49. Copyright 2014 Wiley.
图2 皮肤、皮脂和汗液的FTIRM光谱及其相应的光学显微照片[18]
Fig. 2 FTIRM spectra of skin, sebum, and sweat with their corresponding light micrographs. Scale bar: 20 μm. Reprinted with permission from ref 18. Copyright 2010 Wiley.
图3 新鲜的(红线)和老化一个月的(蓝线)指纹的拉曼光谱[53]
Fig. 3 Raman spectra from a freshly deposited fingermark(red) and after one month of aging(blue). Reprinted with permission from ref 53. Copyright 2017 Wiley.
图4 标准油酸(OA)的MALDI-MS分析[58]
Fig. 4 MALDI-MS analysis of standard oleic acid(OA). Reprinted with permission from ref 58. Copyright 2009 Wiley.
图5 (a) 9天酯交换反应指纹提取物的GC-MS/MS谱图;(b) 显示了四个不同供体(A,B,C,D)指纹样品的SQ/C15:0比率随光照和时间的变化(短轴:0-没有暴露在光条件下的新鲜指纹) [59]
Fig. 5 (a) GC-MS/MS chromatograms of a 9-day-old transesterified fingermark extract;(b) The SQ/C15:0 ratio change dependence on time and light exposure in fingerprint samples of four different donors A, B, C, D(minor axis: 0-fresh fingerprint without exposure to light). Reprinted with permission from ref 59. Copyright 2017 Springer.
图6 (a)指纹的TOF-SIMS离子图像,显示C16H31O2-(棕榈酸)离子在裸硅晶片的分布,红色矩形部分用于(b)图中的线性扫描;(b)指纹边缘的棕榈酸强度随时间的变化[21]
Fig. 6 (a) TOF-SIMS ion images of the fingerprint, showing the distribution of the C16H31O2- ion(palmitic acid) on top of a bare silicon wafer, the red rectangle shows the region of interest(150 pixels wide) that was used to obtain a portion of the linescans shown in part b;(b) the intensity of palmitic acid from the edge of the fingermark as a function of time. Reprinted with permission from ref 21. Copyright 2015 ACS.
图7 光照和分泌类型条件下随时间推移指纹表现出不同的降解结果[60]
Fig. 7 Different degradation outcomes of powder-developed fingermarks on different surfaces, light exposure, and secretion types over time. Reprinted with permission from ref 60. Copyright 2016 Wiley.
表2 遗留时间测定方法的总结及其优缺点
Table 2 Summary of age determination methods together with their advantages and disadvantages
Method Target Age
estimation		 Advantage Disadvantage ref
Fluorescence Tryp / FOX Three weeks Non-contact; partially solving variations in
composition between donors		 The oxidation process is very sensitive to
environmental factors such as temperature and light		 49
FTIR Aliphatic CH3,
aliphatic CH2, and
carbonyl ester		 Four weeks High spatial resolution; quantitative and
non-invasive; examining individual
fingerprint components separately		 No account for variations between genders 18
UV-Vis Eccrine, sebaceous Three days Reproducible; providing opportunity to
address the strong influence of different
sweat compositions on the aging behavior		 Fresh prints with a low aging speed as well as aged
prints are hard to distinguish		 52
RS Carotenoids, squalene,
unsaturated fatty
acids, proteins		 One month Non-destructive; providinglarger data sets
for future statistical analysis		 More data will be needed
to gain further insight into the different
decay mechanisms		 53
GC
/MS		 Relative peak areas of
squalene to cholesterol;PA(Wax esters) / [PA(cholesterol) +PA
(squalene)]		 One month Reproducible; reducing partly intra- and
inter-variability of fingermark composition		 The technique is destructive for the fingermarks 53
MALDI-MS Oleic acid(OA) Seven days Non-destructive; high resolution imaging No account for variations in more
environmental factors		 58
GC-MS/MS SQ/C15:0 Nine days Detecting two age different samples on
a glass surface from the same donor		 Initial component cannot be determined 59
TOF
-SIMS		 Palmitic acid Four days Detecting and identifing multiple
chemical species simultaneously; High
resolution and sensitivity		 Molecules can degrade or become oxidized upon
exposuring to various environmental factors		 21
High-
resolution imaging		 Minutiae count;
color contrast
between ridges and
furrows;discontinuity index;ridge width		 Six months Non-destructive; quantitative,
high resolution and sensitivity		 It is not suitable for multiple individuals to study simultaneously 60~63
Ridge height One year Non-destructive, contactless, reobservation, inexpensive cost, without pretreatment, lower error, large area of analysis Detection limit(insensitive to very thin layers); slow data acquisition times at very high resolutions 66
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摘要

指纹遗留时间的研究方法