{"title":"青藏高原东南部新粒子形成过程中重萜烯和人为相互作用的关键作用","authors":"Yuliang Liu, Wei Nie, Ximeng Qi, Yuanyuan Li, Tao Xu, Chong Liu, Dafeng Ge, Liangduo Chen, Guangdong Niu, Jinbo Wang, Liwen Yang, Lei Wang, Caijun Zhu, Jiaping Wang, Yuxuan Zhang, Tengyu Liu, Qiaozhi Zha, Chao Yan, Chunxiang Ye, Guoxian Zhang, Renzhi Hu, Ru-Jin Huang, Xuguang Chi, Tong Zhu, Aijun Ding","doi":"10.1021/acs.est.4c04112","DOIUrl":null,"url":null,"abstract":"Aerosol particles originating from the Qinghai-Tibet Plateau (QTP) readily reach the free troposphere, potentially affecting global radiation and climate. Although new particle formation (NPF) is frequently observed at such high altitudes, its precursors and their underlying chemistry remain poorly understood. This study presents direct observational evidence of anthropogenic influences on biogenic NPF on the southeastern QTP, near the Himalayas. The mean particle nucleation rate (<i>J</i><sub>1.7</sub>) is 2.6 cm<sup>–3</sup> s<sup>–1</sup>, exceeding the kinetic limit of sulfuric acid (SA) nucleation (mean SA: 2.4 × 10<sup>5</sup> cm<sup>–3</sup>). NPF is predominantly driven by highly oxygenated organic molecules (HOMs), possibly facilitated by low SA levels. We identified 1538 ultralow-volatility HOMs driving particle nucleation and 764 extremely low-volatility HOMs powering initial particle growth, with mean total concentrations of 1.5 × 10<sup>6</sup> and 3.7 × 10<sup>6</sup> cm<sup>–3</sup>, respectively. These HOMs are formed by atmospheric oxidation of biogenic precursors, unexpectedly including sesquiterpenes and diterpenes alongside the commonly recognized monoterpenes. Counterintuitively, over half of HOMs are organic nitrates, mainly produced by interacting with anthropogenic NO<sub><i>x</i></sub> via RO<sub>2</sub>+NO terminations or NO<sub>3</sub>-initiated oxidations. These findings advance our understanding of NPF mechanisms in this climate-sensitive region and underscore the importance of heavy terpene and NO<sub><i>x</i></sub>-influenced chemistry in assessing anthropogenic-biogenic interactions with climate feedbacks.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8000,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"The Pivotal Role of Heavy Terpenes and Anthropogenic Interactions in New Particle Formation on the Southeastern Qinghai-Tibet Plateau\",\"authors\":\"Yuliang Liu, Wei Nie, Ximeng Qi, Yuanyuan Li, Tao Xu, Chong Liu, Dafeng Ge, Liangduo Chen, Guangdong Niu, Jinbo Wang, Liwen Yang, Lei Wang, Caijun Zhu, Jiaping Wang, Yuxuan Zhang, Tengyu Liu, Qiaozhi Zha, Chao Yan, Chunxiang Ye, Guoxian Zhang, Renzhi Hu, Ru-Jin Huang, Xuguang Chi, Tong Zhu, Aijun Ding\",\"doi\":\"10.1021/acs.est.4c04112\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Aerosol particles originating from the Qinghai-Tibet Plateau (QTP) readily reach the free troposphere, potentially affecting global radiation and climate. Although new particle formation (NPF) is frequently observed at such high altitudes, its precursors and their underlying chemistry remain poorly understood. This study presents direct observational evidence of anthropogenic influences on biogenic NPF on the southeastern QTP, near the Himalayas. The mean particle nucleation rate (<i>J</i><sub>1.7</sub>) is 2.6 cm<sup>–3</sup> s<sup>–1</sup>, exceeding the kinetic limit of sulfuric acid (SA) nucleation (mean SA: 2.4 × 10<sup>5</sup> cm<sup>–3</sup>). NPF is predominantly driven by highly oxygenated organic molecules (HOMs), possibly facilitated by low SA levels. We identified 1538 ultralow-volatility HOMs driving particle nucleation and 764 extremely low-volatility HOMs powering initial particle growth, with mean total concentrations of 1.5 × 10<sup>6</sup> and 3.7 × 10<sup>6</sup> cm<sup>–3</sup>, respectively. These HOMs are formed by atmospheric oxidation of biogenic precursors, unexpectedly including sesquiterpenes and diterpenes alongside the commonly recognized monoterpenes. Counterintuitively, over half of HOMs are organic nitrates, mainly produced by interacting with anthropogenic NO<sub><i>x</i></sub> via RO<sub>2</sub>+NO terminations or NO<sub>3</sub>-initiated oxidations. These findings advance our understanding of NPF mechanisms in this climate-sensitive region and underscore the importance of heavy terpene and NO<sub><i>x</i></sub>-influenced chemistry in assessing anthropogenic-biogenic interactions with climate feedbacks.\",\"PeriodicalId\":36,\"journal\":{\"name\":\"环境科学与技术\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":10.8000,\"publicationDate\":\"2024-09-26\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"环境科学与技术\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.est.4c04112\",\"RegionNum\":1,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"环境科学与技术","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.est.4c04112","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
The Pivotal Role of Heavy Terpenes and Anthropogenic Interactions in New Particle Formation on the Southeastern Qinghai-Tibet Plateau
Aerosol particles originating from the Qinghai-Tibet Plateau (QTP) readily reach the free troposphere, potentially affecting global radiation and climate. Although new particle formation (NPF) is frequently observed at such high altitudes, its precursors and their underlying chemistry remain poorly understood. This study presents direct observational evidence of anthropogenic influences on biogenic NPF on the southeastern QTP, near the Himalayas. The mean particle nucleation rate (J1.7) is 2.6 cm–3 s–1, exceeding the kinetic limit of sulfuric acid (SA) nucleation (mean SA: 2.4 × 105 cm–3). NPF is predominantly driven by highly oxygenated organic molecules (HOMs), possibly facilitated by low SA levels. We identified 1538 ultralow-volatility HOMs driving particle nucleation and 764 extremely low-volatility HOMs powering initial particle growth, with mean total concentrations of 1.5 × 106 and 3.7 × 106 cm–3, respectively. These HOMs are formed by atmospheric oxidation of biogenic precursors, unexpectedly including sesquiterpenes and diterpenes alongside the commonly recognized monoterpenes. Counterintuitively, over half of HOMs are organic nitrates, mainly produced by interacting with anthropogenic NOx via RO2+NO terminations or NO3-initiated oxidations. These findings advance our understanding of NPF mechanisms in this climate-sensitive region and underscore the importance of heavy terpene and NOx-influenced chemistry in assessing anthropogenic-biogenic interactions with climate feedbacks.
期刊介绍:
Environmental Science & Technology (ES&T) is a co-sponsored academic and technical magazine by the Hubei Provincial Environmental Protection Bureau and the Hubei Provincial Academy of Environmental Sciences.
Environmental Science & Technology (ES&T) holds the status of Chinese core journals, scientific papers source journals of China, Chinese Science Citation Database source journals, and Chinese Academic Journal Comprehensive Evaluation Database source journals. This publication focuses on the academic field of environmental protection, featuring articles related to environmental protection and technical advancements.