{"title":"“特洛伊木马”型内化增加了硫化汞纳米颗粒的生物利用度和细胞内溶解后的甲基化","authors":"Yingying Guo, Yuping Xiang, Guangliang Liu, Ying Chen, Yanwei Liu, Maoyong Song, Yanbin Li, Jianbo Shi, Ligang Hu, Yongguang Yin*, Yong Cai and Guibin Jiang, ","doi":"10.1021/acsnano.2c05657","DOIUrl":null,"url":null,"abstract":"<p >Mercury sulfide nanoparticles (HgS<sub>NP</sub>), as natural metal-containing nanoparticles, are the dominant Hg species in anoxic zones. Although the microbial Hg methylation of HgS<sub>NP</sub> has been previously reported, the importance of this process in Hg methylation has yet to be clarified due to the lack of knowledge on the internalization and transformation of HgS<sub>NP</sub>. Here, we investigated the internalization and transformation of HgS<sub>NP</sub> in microbial methylator <i>Geobacter sulfurreducens</i> PCA through total Hg analysis and different Hg species quantification in medium and cytoplasm. We found that the microbial uptake of HgS<sub>NP</sub>, via a passive diffusion pathway, was significantly higher than that of the Hg<sup>2+</sup>-dissolved organic matter (Hg<sup>2+</sup>-DOM) complex. Internalized HgS<sub>NP</sub> were dissolved to Hg<sup>2+</sup> in cytoplasm with a maximal dissolution of 41%, suggesting a “Trojan horse” mechanism. The intracellular Hg<sup>2+</sup> from HgS<sub>NP</sub> exposure at the initial stage (8 h) was higher than that in Hg<sup>2+</sup>-DOM group, which led to higher methylation of HgS<sub>NP</sub>. Furthermore, no differences in methylmercury (MeHg) production from HgS<sub>NP</sub> were observed between the <i>hgcAB</i> gene knockout (Δ<i>hgcAB</i>) and wild-type strains, suggesting that HgS<sub>NP</sub> methylation may occur through HgcAB-independent pathways. Considering the possibility of a broad range of <i>hgcAB</i>-lacking microbes serving as methylators for HgS<sub>NP</sub> and the ubiquity of HgS<sub>NP</sub> in anoxic environments, this study highlights the importance of HgS<sub>NP</sub> internalization and methylation in MeHg production and demonstrates the necessity of understanding the assimilation and transformation of nutrient and toxic metal nanoparticles in general.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"17 3","pages":"1925–1934"},"PeriodicalIF":15.8000,"publicationDate":"2023-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"4","resultStr":"{\"title\":\"“Trojan Horse” Type Internalization Increases the Bioavailability of Mercury Sulfide Nanoparticles and Methylation after Intracellular Dissolution\",\"authors\":\"Yingying Guo, Yuping Xiang, Guangliang Liu, Ying Chen, Yanwei Liu, Maoyong Song, Yanbin Li, Jianbo Shi, Ligang Hu, Yongguang Yin*, Yong Cai and Guibin Jiang, \",\"doi\":\"10.1021/acsnano.2c05657\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Mercury sulfide nanoparticles (HgS<sub>NP</sub>), as natural metal-containing nanoparticles, are the dominant Hg species in anoxic zones. Although the microbial Hg methylation of HgS<sub>NP</sub> has been previously reported, the importance of this process in Hg methylation has yet to be clarified due to the lack of knowledge on the internalization and transformation of HgS<sub>NP</sub>. Here, we investigated the internalization and transformation of HgS<sub>NP</sub> in microbial methylator <i>Geobacter sulfurreducens</i> PCA through total Hg analysis and different Hg species quantification in medium and cytoplasm. We found that the microbial uptake of HgS<sub>NP</sub>, via a passive diffusion pathway, was significantly higher than that of the Hg<sup>2+</sup>-dissolved organic matter (Hg<sup>2+</sup>-DOM) complex. Internalized HgS<sub>NP</sub> were dissolved to Hg<sup>2+</sup> in cytoplasm with a maximal dissolution of 41%, suggesting a “Trojan horse” mechanism. The intracellular Hg<sup>2+</sup> from HgS<sub>NP</sub> exposure at the initial stage (8 h) was higher than that in Hg<sup>2+</sup>-DOM group, which led to higher methylation of HgS<sub>NP</sub>. Furthermore, no differences in methylmercury (MeHg) production from HgS<sub>NP</sub> were observed between the <i>hgcAB</i> gene knockout (Δ<i>hgcAB</i>) and wild-type strains, suggesting that HgS<sub>NP</sub> methylation may occur through HgcAB-independent pathways. Considering the possibility of a broad range of <i>hgcAB</i>-lacking microbes serving as methylators for HgS<sub>NP</sub> and the ubiquity of HgS<sub>NP</sub> in anoxic environments, this study highlights the importance of HgS<sub>NP</sub> internalization and methylation in MeHg production and demonstrates the necessity of understanding the assimilation and transformation of nutrient and toxic metal nanoparticles in general.</p>\",\"PeriodicalId\":21,\"journal\":{\"name\":\"ACS Nano\",\"volume\":\"17 3\",\"pages\":\"1925–1934\"},\"PeriodicalIF\":15.8000,\"publicationDate\":\"2023-01-23\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"4\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Nano\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acsnano.2c05657\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Nano","FirstCategoryId":"88","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsnano.2c05657","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
“Trojan Horse” Type Internalization Increases the Bioavailability of Mercury Sulfide Nanoparticles and Methylation after Intracellular Dissolution
Mercury sulfide nanoparticles (HgSNP), as natural metal-containing nanoparticles, are the dominant Hg species in anoxic zones. Although the microbial Hg methylation of HgSNP has been previously reported, the importance of this process in Hg methylation has yet to be clarified due to the lack of knowledge on the internalization and transformation of HgSNP. Here, we investigated the internalization and transformation of HgSNP in microbial methylator Geobacter sulfurreducens PCA through total Hg analysis and different Hg species quantification in medium and cytoplasm. We found that the microbial uptake of HgSNP, via a passive diffusion pathway, was significantly higher than that of the Hg2+-dissolved organic matter (Hg2+-DOM) complex. Internalized HgSNP were dissolved to Hg2+ in cytoplasm with a maximal dissolution of 41%, suggesting a “Trojan horse” mechanism. The intracellular Hg2+ from HgSNP exposure at the initial stage (8 h) was higher than that in Hg2+-DOM group, which led to higher methylation of HgSNP. Furthermore, no differences in methylmercury (MeHg) production from HgSNP were observed between the hgcAB gene knockout (ΔhgcAB) and wild-type strains, suggesting that HgSNP methylation may occur through HgcAB-independent pathways. Considering the possibility of a broad range of hgcAB-lacking microbes serving as methylators for HgSNP and the ubiquity of HgSNP in anoxic environments, this study highlights the importance of HgSNP internalization and methylation in MeHg production and demonstrates the necessity of understanding the assimilation and transformation of nutrient and toxic metal nanoparticles in general.
期刊介绍:
ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.