An Automated Methodology for Non-targeted Compositional Analysis of Small Molecules in High Complexity Environmental Matrices Using Coupled Ultra Performance Liquid Chromatography Orbitrap Mass Spectrometry

TY - JOUR

T1 - An Automated Methodology for Non-targeted Compositional Analysis of Small Molecules in High Complexity Environmental Matrices Using Coupled Ultra Performance Liquid Chromatography Orbitrap Mass Spectrometry

AU - Pereira, Kelly L.

AU - Ward, Martyn W.

AU - Wilkinson, John L.

AU - Sallach, Jonathan Brett

AU - Bryant, Daniel J.

AU - Dixon, William J.

AU - Hamilton, Jacqueline F.

AU - Lewis, Alastair C.

N1 - © 2021, The Author(s).

PY - 2021/5/18

Y1 - 2021/5/18

N2 - The life-critical matrices of air and water are among the most complex chemical mixtures that are ever encountered. Ultrahigh-resolution mass spectrometers, such as the Orbitrap, provide unprecedented analytical capabilities to probe the molecular composition of such matrices, but the extraction of non-targeted chemical information is impractical to perform via manual data processing. Automated non-targeted tools rapidly extract the chemical information of all detected compounds within a sample dataset. However, these methods have not been exploited in the environmental sciences. Here, we provide an automated and (for the first time) rigorously tested methodology for the non-targeted compositional analysis of environmental matrices using coupled liquid chromatography-mass spectrometric data. First, the robustness and reproducibility was tested using authentic standards, evaluating performance as a function of concentration, ionization potential, and sample complexity. The method was then used for the compositional analysis of particulate matter and surface waters collected from worldwide locations. The method detected >9600 compounds in the individual environmental samples, arising from critical pollutant sources, including carcinogenic industrial chemicals, pesticides, and pharmaceuticals among others. This methodology offers considerable advances in the environmental sciences, providing a more complete assessment of sample compositions while significantly increasing throughput.

AB - The life-critical matrices of air and water are among the most complex chemical mixtures that are ever encountered. Ultrahigh-resolution mass spectrometers, such as the Orbitrap, provide unprecedented analytical capabilities to probe the molecular composition of such matrices, but the extraction of non-targeted chemical information is impractical to perform via manual data processing. Automated non-targeted tools rapidly extract the chemical information of all detected compounds within a sample dataset. However, these methods have not been exploited in the environmental sciences. Here, we provide an automated and (for the first time) rigorously tested methodology for the non-targeted compositional analysis of environmental matrices using coupled liquid chromatography-mass spectrometric data. First, the robustness and reproducibility was tested using authentic standards, evaluating performance as a function of concentration, ionization potential, and sample complexity. The method was then used for the compositional analysis of particulate matter and surface waters collected from worldwide locations. The method detected >9600 compounds in the individual environmental samples, arising from critical pollutant sources, including carcinogenic industrial chemicals, pesticides, and pharmaceuticals among others. This methodology offers considerable advances in the environmental sciences, providing a more complete assessment of sample compositions while significantly increasing throughput.

KW - Compound Discoverer

KW - liquid chromatography−mass spectrometry

KW - non-targeted analysis

KW - ultrahigh-resolution mass spectrometry

UR - http://www.scopus.com/inward/record.url?scp=85107390614&partnerID=8YFLogxK

U2 - 10.1021/acs.est.0c08208

DO - 10.1021/acs.est.0c08208

M3 - Article

C2 - 34006107

AN - SCOPUS:85107390614

SN - 0013-936X

VL - 55

SP - 7365

EP - 7375

JO - Environmental Science and Technology

JF - Environmental Science and Technology

IS - 11

ER -