使用高分辨率MALDI质谱分析理解人体组织生化降解的整体方法

IF 3.3 3区 化学 Q2 CHEMISTRY, ANALYTICAL
Analyst Pub Date : 2025-07-18 DOI:10.1039/d5an00588d
Jerika Ho, Naomi Stock, Vaughn Mangal, Shari Forbes, Theresa Stotesbury
{"title":"使用高分辨率MALDI质谱分析理解人体组织生化降解的整体方法","authors":"Jerika Ho, Naomi Stock, Vaughn Mangal, Shari Forbes, Theresa Stotesbury","doi":"10.1039/d5an00588d","DOIUrl":null,"url":null,"abstract":"Estimating the postmortem interval (PMI) is crucial in medico-legal death investigations, but existing methods are highly influenced by environmental and physiological factors. This study proposes a novel biochemical strategy for PMI estimation using Matrix-Assisted Laser Desorption/Ionization Mass Spectrometry (MALDI MS) to detect molecular changes in decomposing human soft tissues. Samples from the quadriceps and shoulder were collected from 13 human donors at the Research in Experimental and Social Thanatology (REST) facility in Quebec, Canada, spanning accumulated degree days (ADD) ranging from 9.75 to 11,455.86. Tissues (14 µm) were cryosectioned, mounted on carbon tape, dried under nitrogen gas, and coated with a 2,5-dihydroxybenzoic acid matrix solution. Hematoxylin and eosin staining provided histological context for the sampled tissues. MALDI MS data were acquired using a Bruker SolariX XR Fourier-transform Ion Cyclotron Resonance MS. Van Krevelen diagrams and principal component analysis revealed decomposition-linked trends, with shifts in biochemical profiles over time. N/C and N/O ratios increased, reflecting protein and peptide degradation and microbial activity, while O/C ratios declined, likely due to the loss of oxygen-rich compounds. Mixed-effects models showed moderate associations (R² marginal = 0.06–0.49) between elemental ratios and ADD, with conditional R² values up to 0.55. Spearman’s rank correlation identified compounds significantly associated with ADD. Six candidate biomarkers were identified, with variable model fit (R² marginal = 0.003–0.80) and unresolved donor-level effects. This study demonstrates the novel application of MALDI MS for PMI biomarker discovery and contributes one of the largest datasets in forensic decomposition chemistry research.","PeriodicalId":63,"journal":{"name":"Analyst","volume":"7 1","pages":""},"PeriodicalIF":3.3000,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"A holistic approach to understanding biochemical degradation of human tissues using high resolution MALDI MS\",\"authors\":\"Jerika Ho, Naomi Stock, Vaughn Mangal, Shari Forbes, Theresa Stotesbury\",\"doi\":\"10.1039/d5an00588d\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Estimating the postmortem interval (PMI) is crucial in medico-legal death investigations, but existing methods are highly influenced by environmental and physiological factors. This study proposes a novel biochemical strategy for PMI estimation using Matrix-Assisted Laser Desorption/Ionization Mass Spectrometry (MALDI MS) to detect molecular changes in decomposing human soft tissues. Samples from the quadriceps and shoulder were collected from 13 human donors at the Research in Experimental and Social Thanatology (REST) facility in Quebec, Canada, spanning accumulated degree days (ADD) ranging from 9.75 to 11,455.86. Tissues (14 µm) were cryosectioned, mounted on carbon tape, dried under nitrogen gas, and coated with a 2,5-dihydroxybenzoic acid matrix solution. Hematoxylin and eosin staining provided histological context for the sampled tissues. MALDI MS data were acquired using a Bruker SolariX XR Fourier-transform Ion Cyclotron Resonance MS. Van Krevelen diagrams and principal component analysis revealed decomposition-linked trends, with shifts in biochemical profiles over time. N/C and N/O ratios increased, reflecting protein and peptide degradation and microbial activity, while O/C ratios declined, likely due to the loss of oxygen-rich compounds. Mixed-effects models showed moderate associations (R² marginal = 0.06–0.49) between elemental ratios and ADD, with conditional R² values up to 0.55. Spearman’s rank correlation identified compounds significantly associated with ADD. Six candidate biomarkers were identified, with variable model fit (R² marginal = 0.003–0.80) and unresolved donor-level effects. This study demonstrates the novel application of MALDI MS for PMI biomarker discovery and contributes one of the largest datasets in forensic decomposition chemistry research.\",\"PeriodicalId\":63,\"journal\":{\"name\":\"Analyst\",\"volume\":\"7 1\",\"pages\":\"\"},\"PeriodicalIF\":3.3000,\"publicationDate\":\"2025-07-18\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Analyst\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1039/d5an00588d\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, ANALYTICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Analyst","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1039/d5an00588d","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, ANALYTICAL","Score":null,"Total":0}
引用次数: 0

摘要

尸检时间估算是法医死亡调查的重要内容,但现有方法受环境和生理因素的影响较大。本研究提出了一种新的生化策略来估计PMI使用基质辅助激光解吸/电离质谱(MALDI MS)来检测分解人体软组织中的分子变化。在加拿大魁北克的实验和社会病理学研究(REST)设施中,从13名人类供体中收集了股四头肌和肩部的样本,累积度(ADD)从9.75到11,455.86不等。组织(14µm)冷冻切片,安装在碳带上,在氮气下干燥,并涂有2,5-二羟基苯甲酸基质溶液。苏木精和伊红染色提供了样本组织的组织学背景。MALDI质谱数据是使用Bruker SolariX XR傅里叶变换离子回旋共振质谱获取的,Van Krevelen图和主成分分析揭示了分解相关的趋势,随着时间的推移,生物化学特征发生了变化。N/C和N/O比率增加,反映了蛋白质和肽的降解和微生物活性,而O/C比率下降,可能是由于富氧化合物的损失。混合效应模型显示元素比与ADD之间存在适度关联(R²边际= 0.06-0.49),条件R²值最高可达0.55。Spearman等级相关鉴定出与ADD显著相关的化合物。鉴定出6个候选生物标志物,模型拟合变量(R²边际= 0.003-0.80),供体水平效应未得到解决。该研究展示了MALDI质谱在PMI生物标志物发现中的新应用,并为法医分解化学研究提供了最大的数据集之一。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
A holistic approach to understanding biochemical degradation of human tissues using high resolution MALDI MS
Estimating the postmortem interval (PMI) is crucial in medico-legal death investigations, but existing methods are highly influenced by environmental and physiological factors. This study proposes a novel biochemical strategy for PMI estimation using Matrix-Assisted Laser Desorption/Ionization Mass Spectrometry (MALDI MS) to detect molecular changes in decomposing human soft tissues. Samples from the quadriceps and shoulder were collected from 13 human donors at the Research in Experimental and Social Thanatology (REST) facility in Quebec, Canada, spanning accumulated degree days (ADD) ranging from 9.75 to 11,455.86. Tissues (14 µm) were cryosectioned, mounted on carbon tape, dried under nitrogen gas, and coated with a 2,5-dihydroxybenzoic acid matrix solution. Hematoxylin and eosin staining provided histological context for the sampled tissues. MALDI MS data were acquired using a Bruker SolariX XR Fourier-transform Ion Cyclotron Resonance MS. Van Krevelen diagrams and principal component analysis revealed decomposition-linked trends, with shifts in biochemical profiles over time. N/C and N/O ratios increased, reflecting protein and peptide degradation and microbial activity, while O/C ratios declined, likely due to the loss of oxygen-rich compounds. Mixed-effects models showed moderate associations (R² marginal = 0.06–0.49) between elemental ratios and ADD, with conditional R² values up to 0.55. Spearman’s rank correlation identified compounds significantly associated with ADD. Six candidate biomarkers were identified, with variable model fit (R² marginal = 0.003–0.80) and unresolved donor-level effects. This study demonstrates the novel application of MALDI MS for PMI biomarker discovery and contributes one of the largest datasets in forensic decomposition chemistry research.
求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
Analyst
Analyst 化学-分析化学
CiteScore
7.80
自引率
4.80%
发文量
636
审稿时长
1.9 months
期刊介绍: "Analyst" journal is the home of premier fundamental discoveries, inventions and applications in the analytical and bioanalytical sciences.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信