A surface-promoted redox reaction occurs spontaneously on solvating inorganic aerosol surfaces

Xiangrui Kong; Dimitri Castarède; Erik S. Thomson; Anthony Boucly; Luca Artiglia; Markus Ammann; Ivan Gladich; Jan B.C. Pettersson

doi:10.1126/science.abc5311

A surface-promoted redox reaction occurs spontaneously on solvating inorganic aerosol surfaces

Xiangrui Kong^*, Dimitri Castarède, Erik S. Thomson, Anthony Boucly, Luca Artiglia, Markus Ammann, Ivan Gladich^*, Jan B.C. Pettersson^*

^*Corresponding author for this work

QEERI - Energy Center

Research output: Contribution to journal › Article › peer-review

37 Citations (Scopus)

Abstract

A surface-promoted sulfate-reducing ammonium oxidation reaction was discovered to spontaneously take place on common inorganic aerosol surfaces undergoing solvation. Several key intermediate species-including elemental sulfur (S0), bisulfide (HS-), nitrous acid (HONO), and aqueous ammonia [NH3(aq)]-were identified as reaction components associated with the solvation process. Depth profiles of relative species abundance showed the surface propensity of key species. The species assignments and depth profile features were supported by classical and first-principles molecular dynamics calculations, and a detailed mechanism was proposed to describe the processes that led to unexpected products during salt solvation. This discovery revealed chemistry that is distinctly linked to a solvating surface and has great potential to illuminate current puzzles within heterogeneous chemistry.

Original language	English
Pages (from-to)	747-752
Number of pages	6
Journal	Science
Volume	374
Issue number	6568
DOIs	https://doi.org/10.1126/science.abc5311
Publication status	Published - 5 Nov 2021

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abstract = "A surface-promoted sulfate-reducing ammonium oxidation reaction was discovered to spontaneously take place on common inorganic aerosol surfaces undergoing solvation. Several key intermediate species-including elemental sulfur (S0), bisulfide (HS-), nitrous acid (HONO), and aqueous ammonia [NH3(aq)]-were identified as reaction components associated with the solvation process. Depth profiles of relative species abundance showed the surface propensity of key species. The species assignments and depth profile features were supported by classical and first-principles molecular dynamics calculations, and a detailed mechanism was proposed to describe the processes that led to unexpected products during salt solvation. This discovery revealed chemistry that is distinctly linked to a solvating surface and has great potential to illuminate current puzzles within heterogeneous chemistry.",

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AU - Kong, Xiangrui

AU - Castarède, Dimitri

AU - Thomson, Erik S.

AU - Boucly, Anthony

AU - Artiglia, Luca

AU - Ammann, Markus

AU - Gladich, Ivan

AU - Pettersson, Jan B.C.

PY - 2021/11/5

Y1 - 2021/11/5

N2 - A surface-promoted sulfate-reducing ammonium oxidation reaction was discovered to spontaneously take place on common inorganic aerosol surfaces undergoing solvation. Several key intermediate species-including elemental sulfur (S0), bisulfide (HS-), nitrous acid (HONO), and aqueous ammonia [NH3(aq)]-were identified as reaction components associated with the solvation process. Depth profiles of relative species abundance showed the surface propensity of key species. The species assignments and depth profile features were supported by classical and first-principles molecular dynamics calculations, and a detailed mechanism was proposed to describe the processes that led to unexpected products during salt solvation. This discovery revealed chemistry that is distinctly linked to a solvating surface and has great potential to illuminate current puzzles within heterogeneous chemistry.

AB - A surface-promoted sulfate-reducing ammonium oxidation reaction was discovered to spontaneously take place on common inorganic aerosol surfaces undergoing solvation. Several key intermediate species-including elemental sulfur (S0), bisulfide (HS-), nitrous acid (HONO), and aqueous ammonia [NH3(aq)]-were identified as reaction components associated with the solvation process. Depth profiles of relative species abundance showed the surface propensity of key species. The species assignments and depth profile features were supported by classical and first-principles molecular dynamics calculations, and a detailed mechanism was proposed to describe the processes that led to unexpected products during salt solvation. This discovery revealed chemistry that is distinctly linked to a solvating surface and has great potential to illuminate current puzzles within heterogeneous chemistry.

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A surface-promoted redox reaction occurs spontaneously on solvating inorganic aerosol surfaces

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