Insight into the model quinone compound AQDS mediated the Mn(II) abiotic oxidation and mineral mineralization on hematite surface under oxic and neutral conditions

Zhang, Hanyue1,2,3; Zheng, Lirong6; Yang, Yang4; Zhou, Wenjing5; Shen, Xinyue5; Hu, Shiwen4,5; Liu, Chongxuan5

2023-05-01

10.1016/j.apgeochem.2023.105658

APPLIED GEOCHEMISTRY   影响因子和分区

0883-2927

1872-9134

Oxidation of Mn(II) and the subsequent mineral mineralization can significantly influence the transport and fate of trace metals and organic pollutants in the soil and sediment environments. Abiotic oxidation of Mn(II) on the surface of Fe mineral in the open air is a vital formation pathway of Mn (oxyhydr)oxides; however, the impact of electron shuttle substances at neutral pH has seldomly been reported. Anthraquinone-2, 6-disulfonate (AQDS) is a typical electron shuttle and might affect the abiotic oxidation of Mn(II). In this study, abiotic oxidation of Mn (II) on the surface of a hematite substrate and mineralization of oxidation product in the presence of AQDS (0-1 mM) were investigated at pH 7.5 in the open air. In the Mn(II)-AQDS treatments, most Mn(II) remained in so-lution, suggesting that AQDS shows little catalytic activity in the abiotic oxidation of Mn(II) without hematite present. By contrast, Mn(II) was rapidly oxidized, and oxidation rates increased from 4.2 x 10-2 to 8.8 x 10-2 h-1 with increasing AQDS concentration from 0 to 1 mM in the hematite-Mn(II)-AQDS treatments. Abiotic oxidation of Mn(II) produced granular-like Mn3O4, fibrous-like beta-MnOOH, and rod-like gamma-MnOOH, and no other secondary Fe minerals were found. The proposed mechanism of the AQDS-mediated abiotic oxidation of Mn(II) on a hematite surface is the AQDS serving as an electronic medium with semiconductor hematite as a foreign substrate, promoting electron transfer between oxygen and Mn(II) on its surface. Our results revealed that electron mediators impart crucial control on not only the rate but also the compositions of Mn(II) oxidation product. The findings of this study provide new insights into the geochemical functions of electron shuttles on the dynamics of redox-sensitive elements under oxic and neutral conditions and expand the understanding of interfacial heterogeneous nucleation reactions at the molecular scale.

Mn(II) oxidation Hematite Mineral mineralization Electronic mediator Interfacial heterogeneous nucleation

SCI ; EI

英语

通讯

National Natural Science Foundation of China["42207249","41830861"] ; China Postdoctoral Science Foundation[2021M701561] ; Guangdong Basic and Applied Basic Research Foundation[2021A1515110904] ; Program for Guangdong Introducing Innovative and Entrepreneurial Teams[2017ZT07Z479]

Geochemistry & Geophysics

Geochemistry & Geophysics

WOS:000985209600001

PERGAMON-ELSEVIER SCIENCE LTD

20231613896426

Catalyst activity ; Electrons ; Hematite ; Ketones ; Manganese oxide ; Mineralogy ; Nucleation ; Organic pollutants ; Redox reactions ; Substrates ; Trace elements

Mineralogy:482 ; Minerals:482.2 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Crystal Growth:933.1.2

GEOSCIENCES

Web of Science

1.Chinese Acad Sci, Chengdu Inst Biol, CAS Key Lab Mt Ecol Restorat & Bioresource Utiliza, Chengdu 610041, Peoples R China
2.Chinese Acad Sci, Chengdu Inst Biol, Ecol Restorat & Biodivers Conservat Key Lab Sichua, Chengdu 610041, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
4.Guangdong Acad Sci, Inst Eco Environm & Soil Sci, Natl Reg Joint Engn Res Ctr Soil Pollut Control &, Guangdong Key Lab Integrated Agro Environm Pollut, Guangzhou 510650, Peoples R China
5.Southern Univ Sci & Technol, Sch Environm Sci & Engn, State Environm Protect Key Lab Integrated Surface, Shenzhen 518055, Peoples R China
6.Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil BSRF, Beijing 100049, Peoples R China

Zhang, Hanyue,Zheng, Lirong,Yang, Yang,et al. Insight into the model quinone compound AQDS mediated the Mn(II) abiotic oxidation and mineral mineralization on hematite surface under oxic and neutral conditions[J]. APPLIED GEOCHEMISTRY,2023,152.

Zhang, Hanyue.,Zheng, Lirong.,Yang, Yang.,Zhou, Wenjing.,Shen, Xinyue.,...&Liu, Chongxuan.(2023).Insight into the model quinone compound AQDS mediated the Mn(II) abiotic oxidation and mineral mineralization on hematite surface under oxic and neutral conditions.APPLIED GEOCHEMISTRY,152.

Zhang, Hanyue,et al."Insight into the model quinone compound AQDS mediated the Mn(II) abiotic oxidation and mineral mineralization on hematite surface under oxic and neutral conditions".APPLIED GEOCHEMISTRY 152(2023).