Driving forces of Ce(III) oxidation to Ce(IV) onto goethite

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F60460709%3A41330%2F23%3A97527" target="_blank" >RIV/60460709:41330/23:97527 - isvavai.cz</a>

Výsledek na webu

<a href="http://dx.doi.org/10.1016/j.chemgeo.2023.121547" target="_blank" >http://dx.doi.org/10.1016/j.chemgeo.2023.121547</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1016/j.chemgeo.2023.121547" target="_blank" >10.1016/j.chemgeo.2023.121547</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Driving forces of Ce(III) oxidation to Ce(IV) onto goethite

Popis výsledku v původním jazyce

Iron (Fe) oxyhydroxides are major phases that may control the cerium (Ce) behavior in the Earth's Critical Zone. However, understanding Ce behavior with Fe oxyhydroxides remains uncompleted. Especially, if thermodynamic calculations suggest that Fe(III) is not a sufficiently strong oxidant, several studies reported the presence of Ce (IV) onto Fe oxyhydroxides. In this study, multiple approaches, including modeling and X-ray absorption spectroscopy, deciphered the driving forces of Ce(III) oxidation to Ce(IV) onto goethite. Results showed that oxidized Ce occurred onto goethite with a Ce(III)/Ce(IV) ratio depending on the Ce concentration in the solution ([Ce]tot). The percentage of Ce(IV) onto goethite ranged from 20% to 50%, linearly increasing with [Ce]tot. Comparable observation with a redox-inert Al-hydroxide (gibbsite), allowed to rule out the importance of Fe(III) redox reactivity as the main driver of Ce(III) oxidation. Instead, thermodynamic calculations suggested that surface precipitation of Ce(IV)-hydroxides, whose formation is favored with increasing [Ce]tot, was an important driving force of the redox reaction. Because the goethite surface seemed to stabilize more strongly Ce(IV) than Ce (III) surface species than does gibbsite, differences in binding mechanisms of Ce(III) and Ce(IV) onto different mineral surfaces have been suggested to play a role on Ce redox speciation.

Název v anglickém jazyce

Driving forces of Ce(III) oxidation to Ce(IV) onto goethite

Popis výsledku anglicky

Iron (Fe) oxyhydroxides are major phases that may control the cerium (Ce) behavior in the Earth's Critical Zone. However, understanding Ce behavior with Fe oxyhydroxides remains uncompleted. Especially, if thermodynamic calculations suggest that Fe(III) is not a sufficiently strong oxidant, several studies reported the presence of Ce (IV) onto Fe oxyhydroxides. In this study, multiple approaches, including modeling and X-ray absorption spectroscopy, deciphered the driving forces of Ce(III) oxidation to Ce(IV) onto goethite. Results showed that oxidized Ce occurred onto goethite with a Ce(III)/Ce(IV) ratio depending on the Ce concentration in the solution ([Ce]tot). The percentage of Ce(IV) onto goethite ranged from 20% to 50%, linearly increasing with [Ce]tot. Comparable observation with a redox-inert Al-hydroxide (gibbsite), allowed to rule out the importance of Fe(III) redox reactivity as the main driver of Ce(III) oxidation. Instead, thermodynamic calculations suggested that surface precipitation of Ce(IV)-hydroxides, whose formation is favored with increasing [Ce]tot, was an important driving force of the redox reaction. Because the goethite surface seemed to stabilize more strongly Ce(IV) than Ce (III) surface species than does gibbsite, differences in binding mechanisms of Ce(III) and Ce(IV) onto different mineral surfaces have been suggested to play a role on Ce redox speciation.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10511 - Environmental sciences (social aspects to be 5.7)

Projekt

—

Návaznosti

S - Specificky vyzkum na vysokych skolach

Rok uplatnění

2023

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

CHEMICAL GEOLOGY

ISSN

0009-2541

e-ISSN

0009-2541

Svazek periodika

633

Číslo periodika v rámci svazku

121547

Stát vydavatele periodika

CZ - Česká republika

Počet stran výsledku

9

Strana od-do

1-9

Kód UT WoS článku

001009269600001

EID výsledku v databázi Scopus

2-s2.0-85162240699