ACS Central Science最新文献_第5页

Elucidating Phosphate and Cadmium Cosorption Mechanisms on Mineral Surfaces with Direct Spectroscopic and Modeling Evidence 用直接光谱和模型证据阐明矿物表面的磷酸盐和镉共吸附机理

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-10-31 DOI: 10.1021/acs.est.4c0884710.1021/acs.est.4c08847

Wantong Zhao, Yun Xu, Liting Gu, Mengqiang Zhu, Peng Yang, Chunhao Gu, Zhe Liu, Xionghan Feng, Wenfeng Tan, Qiaoyun Huang and Xiaoming Wang*,

{"title":"Elucidating Phosphate and Cadmium Cosorption Mechanisms on Mineral Surfaces with Direct Spectroscopic and Modeling Evidence","authors":"Wantong Zhao, Yun Xu, Liting Gu, Mengqiang Zhu, Peng Yang, Chunhao Gu, Zhe Liu, Xionghan Feng, Wenfeng Tan, Qiaoyun Huang and Xiaoming Wang*, ","doi":"10.1021/acs.est.4c0884710.1021/acs.est.4c08847","DOIUrl":"https://doi.org/10.1021/acs.est.4c08847https://doi.org/10.1021/acs.est.4c08847","url":null,"abstract":"The simultaneous sorption of cations and anions at the mineral–water interface can substantially alter their individual sorption characteristics; however, this phenomenon lacks a mechanistic understanding. Our study provides direct spectroscopic and modeling evidence of the molecular cosorption mechanisms of the cadmium ion (Cd2+) and phosphate (P) on goethite and layered manganese (Mn) oxide of birnessite, through in situ attenuated total reflection Fourier-transform infrared (ATR-FTIR), P K-edge X-ray absorption near-edge structure (XANES) spectroscopy, and surface complexation modeling. Phosphate synergistically cosorbed with Cd on goethite predominantly through P-bridged ternary complexes (≡Fe–P–Cd) and electrostatic interactions at wide pH conditions. Likewise, P and Cd exhibited synergistic cosorption on birnessite by forming P-bridged ternary complexes (≡Mn–P–Cd) and weak competitive sorption at the layer edge sites. As pH and Cd loading increased, the surface P species transitioned from a binary complex to a ternary complex and/or Cd3(PO4)2 precipitate for both goethite and birnessite. Compared to that in solution at pH 8, the formation of Cd3(PO4)2 was inhibited by the presence of goethite and birnessite, ascribed to the specific adsorption of P and Cd, more pronounced in birnessite due to the stronger sorption of Cd at its vacant sites. The discovered cosorption mechanisms of P and Cd have important implications for understanding and predicting their mobility and availability in Cd-contaminated settings.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"20211–20223 20211–20223"},"PeriodicalIF":10.8,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609722","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Eureka Moments Shared by Chemists. Hints at Enhancing One's Own Creativity (and Even One's Joy).

IF 12.7 1区化学

ACS Central Science Pub Date : 2024-10-31 eCollection Date: 2024-11-27 DOI: 10.1021/acscentsci.4c00802

Jeffrey I Seeman, Judy I Wu

引用次数: 0

Trends of Benzotriazoles and Benzothiazoles in Australian Pooled Urine Samples from 2012 to 2023 2012 年至 2023 年澳大利亚尿液样本中苯并三唑和苯并噻唑类化合物的变化趋势

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-10-30 DOI: 10.1021/acs.est.4c0882410.1021/acs.est.4c08824

Danielle E. Que*, Xianyu Wang, Sandra Nilsson, Ian Zammit, Derek C. G. Muir, Cassandra Rauert, Leisa-Maree L. Toms, Pritesh Prasad, Ryan G. Shiels, Geoff Eaglesham, Peter Hobson, Daman Langguth and Jochen F. Mueller,

{"title":"Trends of Benzotriazoles and Benzothiazoles in Australian Pooled Urine Samples from 2012 to 2023","authors":"Danielle E. Que*, Xianyu Wang, Sandra Nilsson, Ian Zammit, Derek C. G. Muir, Cassandra Rauert, Leisa-Maree L. Toms, Pritesh Prasad, Ryan G. Shiels, Geoff Eaglesham, Peter Hobson, Daman Langguth and Jochen F. Mueller, ","doi":"10.1021/acs.est.4c0882410.1021/acs.est.4c08824","DOIUrl":"https://doi.org/10.1021/acs.est.4c08824https://doi.org/10.1021/acs.est.4c08824","url":null,"abstract":"Benzotriazoles (BZTs) and benzothiazoles (BTs) are high-production-volume chemicals utilized in many different commercial products and industrial processes, such as metal corrosion inhibitors, vulcanization accelerators, plastic-associated UV stabilizers, and pharmaceutical precursors. This study assessed age, gender, and temporal trends of BZTs and BTs in deidentified surplus pathology urine samples, pooled and stratified by age, gender, and sample collection year from a general Australian population (168 pools representing 16,800 individuals). Tolyltriazole (TTri), 5,6-dimethyl-1H-benzotriazole (DMBZT), 1,3-benzothiazole (BTH), 2-hydroxybenzothiazole (2-OH-BTH), and 2-aminobenzothiazole (2-amino-BTH) were detected in >50% of the pools. TTri was frequently detected in pooled samples representing ≤45-year-olds (both genders). Concentrations of DMBZT, BTH (females), 2-OH-BTH, and 2-amino-BTH (females) increased with age significantly, with adults (>15 years old) showing higher levels than children (≤15 years old). Gender differences in DMBZT concentrations (females > males) were observed across all sampling years and only in some for TTri (males > females: >45 years old), BTH (females > males), and 2-amino-BTH (males > females). A temporal increase in BTH, 2-OH-BTH, and 2-amino-BTH levels within the studied period (2012–2023) has been observed. Our findings suggest ongoing exposure of the Australian general population to BZTs and BTs, highlighting age, gender, and temporal trends of these compounds as measured via their urinary concentrations.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"19960–19969 19960–19969"},"PeriodicalIF":10.8,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609719","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Legacy and Novel Per- and Polyfluoroalkyl Substances in Surface Soils across China: Source Tracking and Main Drivers for the Spatial Variation 中国地表土壤中的遗留和新型全氟和多氟烷基物质：来源追踪和空间变化的主要驱动因素

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-10-30 DOI: 10.1021/acs.est.4c0591310.1021/acs.est.4c05913

Danfan Wang, Xiangyu Liu, Zhefei Guo, Wenyu Shan, Zilin Yang, Yinjuan Chen, Feng Ju and Yanyan Zhang*,

{"title":"Legacy and Novel Per- and Polyfluoroalkyl Substances in Surface Soils across China: Source Tracking and Main Drivers for the Spatial Variation","authors":"Danfan Wang, Xiangyu Liu, Zhefei Guo, Wenyu Shan, Zilin Yang, Yinjuan Chen, Feng Ju and Yanyan Zhang*, ","doi":"10.1021/acs.est.4c0591310.1021/acs.est.4c05913","DOIUrl":"https://doi.org/10.1021/acs.est.4c05913https://doi.org/10.1021/acs.est.4c05913","url":null,"abstract":"China aims to actively control the contamination of globally concerning per- and polyfluoroalkyl substances (PFASs). Evaluation of the current situation can provide a critical reference point for tracking the effectiveness of ongoing progress. Herein, we present the first comprehensive assessment of the spatial variations of 20 legacy and 54 novel PFASs in Chinese background soils in 2021. Novel PFASs were extensively detected in 98.4% of the samples, with 21 species being first reported, which greatly facilitated the appointment of diverse emission sources that aligned with local industrial structures. However, legacy PFASs still dominated the ∑74PFAS profile (median 0.51 ng/g, 0.050–8.33 ng/g). The spatial heterogeneity of soil PFASs was positively driven by economic development and atmospheric deposition, enabling the establishment of predictive models to project the national distribution and temporal trends. Elevated PFAS levels were predominantly distributed in the more industrialized eastern and southern regions, as well as other coastal areas with greater precipitation. ∑74PFAS in surface soils was estimated to increase by 12.9 pg/(g year) over 2002–2021, which would continue alongside economic growth, albeit with greater contributions from novel alternatives. Our work provides comprehensive baseline and predictive data to inform policies toward PFAS control in China.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"20160–20171 20160–20171"},"PeriodicalIF":10.8,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609314","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

The Global Threat from the Irreversible Accumulation of Trifluoroacetic Acid (TFA) 三氟乙酸（TFA）不可逆转的累积对全球造成的威胁

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-10-30 DOI: 10.1021/acs.est.4c0618910.1021/acs.est.4c06189

Hans Peter H. Arp*, Andrea Gredelj, Juliane Glüge, Martin Scheringer and Ian T. Cousins,

{"title":"The Global Threat from the Irreversible Accumulation of Trifluoroacetic Acid (TFA)","authors":"Hans Peter H. Arp*, Andrea Gredelj, Juliane Glüge, Martin Scheringer and Ian T. Cousins, ","doi":"10.1021/acs.est.4c0618910.1021/acs.est.4c06189","DOIUrl":"https://doi.org/10.1021/acs.est.4c06189https://doi.org/10.1021/acs.est.4c06189","url":null,"abstract":"Trifluoroacetic acid (TFA) is a persistent and mobile substance that has been increasing in concentration within diverse environmental media, including rain, soils, human serum, plants, plant-based foods, and drinking water. Currently, TFA concentrations are orders of magnitude higher than those of other per- and polyfluoroalkyl substances (PFAS). This accumulation is due to many PFAS having TFA as a transformation product, including several fluorinated gases (F-gases), pesticides, pharmaceuticals, and industrial chemicals, in addition to direct release of industrially produced TFA. Due to TFA’s extreme persistence and ongoing emissions, concentrations are increasing irreversibly. What remains less clear are the thresholds where irreversible effects on local or global scales occur. There are indications from mammalian toxicity studies that TFA is toxic to reproduction and that it exhibits liver toxicity. Ecotoxicity data are scarce, with most data being for aquatic systems; fewer data are available for terrestrial plants, where TFA bioaccumulates most readily. Collectively, these trends imply that TFA meets the criteria of a planetary boundary threat for novel entities because of increasing planetary-scale exposure, where potential irreversible disruptive impacts on vital earth system processes could occur. The rational response to this is to instigate binding actions to reduce the emissions of TFA and its many precursors.Rapidly increasing TFA concentrations, coupled with TFA’s extreme persistence, mobility and the possibility of irreversible impacts, should prompt action to reduce emissions of TFA and its precursors.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"19925–19935 19925–19935"},"PeriodicalIF":10.8,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.est.4c06189","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609315","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Ultra-efficient Ru and Nb Co-Modified CeO2 Catalysts for Catalytic Oxidation of 1,2-Dichloroethane 用于 1,2-二氯乙烷催化氧化的超高效 Ru 和 Nb 共修饰 CeO2 催化剂

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-10-30 DOI: 10.1021/acs.est.4c0677610.1021/acs.est.4c06776

Aiyong Wang*, Min Ding, Yuang Cai, Li Wang, Yun Guo, Yanglong Guo and Wangcheng Zhan*,

{"title":"Ultra-efficient Ru and Nb Co-Modified CeO2 Catalysts for Catalytic Oxidation of 1,2-Dichloroethane","authors":"Aiyong Wang*, Min Ding, Yuang Cai, Li Wang, Yun Guo, Yanglong Guo and Wangcheng Zhan*, ","doi":"10.1021/acs.est.4c0677610.1021/acs.est.4c06776","DOIUrl":"https://doi.org/10.1021/acs.est.4c06776https://doi.org/10.1021/acs.est.4c06776","url":null,"abstract":"The oxidation of chlorinated volatile organic compounds on CeO2 is hindered by its high susceptibility to chlorine poisoning, resulting in a reduced efficiency and stability. In this study, Ru- and Nb-co-modified CeO2 catalysts were designed to achieve excellent activity, stability, and CO2 selectivity in the catalytic oxidation of 1,2-dichloroethane (EDC). The formation of Nb–O–Ce bonds was observed to enhance the surface acidic sites, thereby improving HCl selectivity and reducing the production of chlorinated byproducts. Meanwhile, it inhibits the formation of Ru–O–Ce and promotes the generation of highly dispersed RuO2 particles on the surface, enhancing the redox properties and mobility of the surface oxygen, thus increasing CO2 selectivity. In situ diffuse reflectance infrared Fourier transform spectroscopy results revealed that chlorine species preferentially attach to Nb species rather than to oxygen vacancies on the Ru/Nb/CeO2 catalyst. This allows more alkane groups to oxidize to formate on the oxygen vacancies, reducing byproduct concentration. Additionally, the oxidation of alkane groups to carboxylic acids is initiated on the Nb species, completing a comprehensive oxidation process under the synergistic effect of RuO2.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"20300–20312 20300–20312"},"PeriodicalIF":10.8,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609583","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Waste to Wealth: Discarded Cigarette Butt-Derived Metal-Free N-Rich Carbon Catalysts for the Selective Catalytic Oxidation of Hydrogen Sulfide to Sulfur 变废为宝：废弃烟头衍生的无金属富 N 碳催化剂用于选择性催化硫化氢氧化成硫

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-10-30 DOI: 10.1021/acs.est.4c0646110.1021/acs.est.4c06461

Jintao Yang, Shuo Cui, Fei Zhao, Fang Wang, Jiayu Feng*, Ping Ning* and Lijuan Jia*,

{"title":"Waste to Wealth: Discarded Cigarette Butt-Derived Metal-Free N-Rich Carbon Catalysts for the Selective Catalytic Oxidation of Hydrogen Sulfide to Sulfur","authors":"Jintao Yang, Shuo Cui, Fei Zhao, Fang Wang, Jiayu Feng*, Ping Ning* and Lijuan Jia*, ","doi":"10.1021/acs.est.4c0646110.1021/acs.est.4c06461","DOIUrl":"https://doi.org/10.1021/acs.est.4c06461https://doi.org/10.1021/acs.est.4c06461","url":null,"abstract":"The selective catalytic oxidation of toxic gas H2S to elemental sulfur (H2S-SCO) is a promising desulfurization process known for its dual benefits of recovering valuable sulfur resources and mitigating environmental pollution. Nevertheless, developing cost-effective and efficient catalysts for H2S-SCO remains a significant challenge. In this study, we synthesized a low-cost and metal-free nitrogen-rich carbon catalyst (NrCC) by copyrolyzing discarded cigarette butts (organic solid wastes that are difficult to degrade naturally) with urea for the continuous H2S-SCO process at a relatively low temperature. The NrCC exhibited exceptional catalytic performance, achieving complete H2S conversion to sulfur at 180 °C, and demonstrated excellent stability in humid (RH = 80%) and high CO2 concentration environments. The catalyst succeeded due to its developed pore structure (specific surface area as high as 2267.77 m2·g–1) and abundant pyridine-N sites. DFT calculations showed that the pyridine-N neighbor carbon sites were the active sites promoting H2S adsorption and dissociation. This study presents a novel “waste control by waste” strategy that integrates the utilization of organic solid waste resources with air pollution control measures, showcasing the potential for sustainable environmental solutions.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"20267–20276 20267–20276"},"PeriodicalIF":10.8,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609584","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Chlorination of Biopterin in Water: Deciphering the Kinetics, Disinfection Byproducts, and Toxicity 水中生物蝶呤的氯化：解密动力学、消毒副产物和毒性

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-10-30 DOI: 10.1021/acs.est.4c0484410.1021/acs.est.4c04844

Yanting Zuo, Shi Cheng, Yuze Han, Liangtao Pu, Erdeng Du, Mingguo Peng, Aimin Li* and Wentao Li*,

{"title":"Chlorination of Biopterin in Water: Deciphering the Kinetics, Disinfection Byproducts, and Toxicity","authors":"Yanting Zuo, Shi Cheng, Yuze Han, Liangtao Pu, Erdeng Du, Mingguo Peng, Aimin Li* and Wentao Li*, ","doi":"10.1021/acs.est.4c0484410.1021/acs.est.4c04844","DOIUrl":"https://doi.org/10.1021/acs.est.4c04844https://doi.org/10.1021/acs.est.4c04844","url":null,"abstract":"Pterins, including biopterin prevalent during cyanobacterial blooms, are nitrogen-containing heterocyclic compounds ubiquitous in both natural and engineered environments. However, their roles and associated human risks in water treatment remain poorly understood. This study systematically investigated the kinetics, disinfection byproducts (DBPs), and toxicity of biopterin in chlorination. For deciphering the reaction kinetics, 1,3,5-trimethoxybenzene proved to be a more effective chlorine quencher than the commonly used reducing agents, as it preserved N-chlorinated intermediates without reversing them back to biopterin. The pH-dependent kinetics demonstrated that both chlorine and biopterin species had a significant influence on the reaction rates, with deprotonated biopterin exhibiting a markedly higher reactivity toward HClO/ClO–. Based on time-of-flight mass spectrometry, ten transformation products (TPs) including seven halogenated N–Cl ones, have been identified for the first time. These cyclic TPs were transformed into various aliphatic carbonaceous and nitrogenous DBPs during the subsequent chlorination process. Notably, theoretical predictions and the luminescent bacteria assay confirmed potential higher toxicities of these products than biopterin. These findings highlight the potential risks of pterins during water disinfection and provide a reference framework for accurately revealing the chlorination behavior of emerging nitrogenous chemicals.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"20137–20146 20137–20146"},"PeriodicalIF":10.8,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609720","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Estro-Androgenic Disrupting Effects of Halogenated Disinfection Byproducts: A Comprehensive Evaluation and Comparison 卤代消毒副产物的雌激素干扰效应：综合评估与比较

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-10-30 DOI: 10.1021/acs.est.4c0722310.1021/acs.est.4c07223

Xueyao Chen, Yaoming Ge, Wei Shi, Mengting Yang, Qing Zhou and Yang Pan*,

{"title":"Estro-Androgenic Disrupting Effects of Halogenated Disinfection Byproducts: A Comprehensive Evaluation and Comparison","authors":"Xueyao Chen, Yaoming Ge, Wei Shi, Mengting Yang, Qing Zhou and Yang Pan*, ","doi":"10.1021/acs.est.4c0722310.1021/acs.est.4c07223","DOIUrl":"https://doi.org/10.1021/acs.est.4c07223https://doi.org/10.1021/acs.est.4c07223","url":null,"abstract":"Drinking water halogenated disinfection byproducts (DBPs) have become an increasing health concern. However, the endocrine-disrupting effects of DBPs have not been well evaluated, and the limited available data have inhibited a comprehensive understanding of their health risks. In this study, a total of 43 DBPs were evaluated for their estro-androgenic effects using two types of human breast cancer cells. Among the tested DBPs, 16 exhibited estrogenic/antiestrogenic/androgenic/antiandrogenic effects, and the effects could be observed even at concentrations typically detected in drinking water. Iodinated and polyhalogenated DBPs generally showed higher effects than other species. For a broader comparison, DBP endocrine-disrupting effect data from this study and previous studies were summarized. It was found that the endocrine disruption efficacy of DBPs followed the rank order of iodinated > brominated > chlorinated species, and halophenolic DBPs were potential endocrine-disrupting compounds. Moreover, molecular docking results demonstrated that the binding of DBPs to estro-androgenic receptors was dominated by hydrophobic bonding, hydrogen bonding, halogen bonding, and van der Waals forces. The force strength and molecular volume were related to the magnitude of the estro-androgenic effects. Iodinated DBPs and polyhalogenated DBPs tended to have larger binding forces than other analogues and thus exhibited stronger effects.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"20190–20200 20190–20200"},"PeriodicalIF":10.8,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609721","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Understanding Trace Iron and Chromium Incorporation During Gibbsite Crystallization and Effects on Mineral Dissolution 了解吉布斯岩结晶过程中痕量铁和铬的掺入及其对矿物溶解的影响

IF 10.8 1区化学

ACS Central Science Pub Date : 2024-10-29 DOI: 10.1021/acs.est.4c0448310.1021/acs.est.4c04483

Yatong Zhao, Micah P. Prange, Meirong Zong, Yining Wang, Eric D. Walter, Ying Chen, Zihua Zhu, Mark H. Engelhard, Xiang Wang, Xiaodong Zhao, Carolyn I. Pearce, Aijun Miao*, Zheming Wang*, Kevin M. Rosso* and Xin Zhang*,

{"title":"Understanding Trace Iron and Chromium Incorporation During Gibbsite Crystallization and Effects on Mineral Dissolution","authors":"Yatong Zhao, Micah P. Prange, Meirong Zong, Yining Wang, Eric D. Walter, Ying Chen, Zihua Zhu, Mark H. Engelhard, Xiang Wang, Xiaodong Zhao, Carolyn I. Pearce, Aijun Miao*, Zheming Wang*, Kevin M. Rosso* and Xin Zhang*, ","doi":"10.1021/acs.est.4c0448310.1021/acs.est.4c04483","DOIUrl":"https://doi.org/10.1021/acs.est.4c04483https://doi.org/10.1021/acs.est.4c04483","url":null,"abstract":"Incorporation of pollutants, e.g., heavy metals, or critical elements, e.g., lithium, as impurities in mineral phases can significantly affect their mobility or sequestration in the environment. Even when present at low concentrations, impurities can alter the solubility and reactivity of the host mineral. In this study, we investigate the incorporation of trace amounts of iron (Fe3+) and chromium (Cr3+) during the crystal growth of the aluminum (Al3+) hydroxide, gibbsite, a major component of bauxite ores, an important soil mineral, and a dominant mineral phase in stored radioactive wastes. Using a comprehensive suite of analytical techniques, we show that both Cr3+ and Fe3+ can be incorporated into the gibbsite lattice during coprecipitation by replacing Al3+ in octahedral sites. These small amounts are consistent with limited to no structural isomorphism shared between Al3+ and Cr3+/Fe3+ hydroxide precipitates, nor room temperature miscibility of their isostructural M2O3 oxide forms, in contrast with oxyhydroxide forms where Al3+ and Fe3+ share similar structural topologies. Despite the limited uptake of Cr3+/Fe3+, we show that these impurities have significant implications for gibbsite dissolution behavior. The limited uptake of Cr3+/Fe3+ (e.g. 0.43% Cr3+ and 0.4% Fe3+), we show that these impurities have significant implications for gibbsite dissolution behavior and subsequent reactivity in complex environments.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"58 45","pages":"20125–20136 20125–20136"},"PeriodicalIF":10.8,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608961","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0