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

IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL
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
{"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}
引用次数: 0

摘要

源自青藏高原的气溶胶颗粒很容易进入自由对流层,从而对全球辐射和气候产生潜在影响。虽然在这样的高海拔地区经常能观测到新粒子的形成(NPF),但人们对其前体及其基本化学成分仍然知之甚少。本研究提供了直接观测证据,证明人类活动对喜马拉雅山脉附近东南部 QTP 的生物源 NPF 产生了影响。平均颗粒成核率(J1.7)为 2.6 cm-3 s-1,超过了硫酸(SA)成核的动力学极限(平均 SA:2.4 × 105 cm-3)。NPF 主要由高含氧有机分子(HOMs)驱动,这可能是由于 SA 水平较低的缘故。我们确定了 1538 个超低挥发性 HOMs 驱动粒子成核,764 个极低挥发性 HOMs 驱动初始粒子生长,其平均总浓度分别为 1.5 × 106 和 3.7 × 106 cm-3。这些 HOMs 是由生物前体在大气中氧化形成的,除了常见的单萜之外,还意外地包括倍半萜和二萜。与直觉相反的是,超过一半的 HOMs 是有机硝酸盐,主要是通过 RO2+NO 终止或 NO3 引发的氧化作用与人为 NOx 相互作用而产生的。这些发现加深了我们对这一气候敏感区域 NPF 机制的理解,并强调了重萜和受氮氧化物影响的化学在评估人为-生物相互作用与气候反馈中的重要性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

The Pivotal Role of Heavy Terpenes and Anthropogenic Interactions in New Particle Formation on the Southeastern Qinghai-Tibet Plateau

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.
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
环境科学与技术
环境科学与技术 环境科学-工程:环境
CiteScore
17.50
自引率
9.60%
发文量
12359
审稿时长
2.8 months
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.
×
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:481959085
Book学术官方微信