Interconversion of hydrated protons at the interface between liquid water and platinum

Physical Chemistry Chemical Physics : PCCP
Peter S RiceP Hu

Abstract

Hydrogen transfer is the fundamental step in electrochemistry involved in water splitting and the hydrogen evolution reaction (HER). However, the nature of this process at the solid-liquid interface has been little studied at the atomic level. In this work, we use ab initio molecular dynamics (AIMD) and umbrella sampling (US), giving us an accurate description of the dynamic processes associated with the solid-liquid environment. Based on this method, the free energy barriers were calculated at the H2O/Pt(111) interface, and a multistep mechanism has been proposed. We find that proton transfer is dictated by the strength of the solid-liquid interaction and the configuration of water molecules above the reaction site. In particular, we show that the surface adsorbed cations, which are confined to the interface above the top site position, act as vessels for enhanced hydrogen transfer to and from the surface. Our results could lead to significant mechanistic consequences for the HER, water splitting and solid-liquid reactions in general.

References

Mar 1, 1985·Physical Review A: General Physics·W G Hoover
Dec 15, 1994·Physical Review. B, Condensed Matter·P E Blöchl
Oct 15, 1996·Physical Review. B, Condensed Matter·G Kresse, J Furthmüller
Nov 1, 1993·Physical Review. B, Condensed Matter·G Kresse, J Hafner
Oct 28, 1996·Physical Review Letters·J P PerdewM Ernzerhof
Oct 6, 2000·Physical Review Letters·A K Soper, M A Ricci
Jul 18, 2001·Journal of the American Chemical Society·A Michaelides, P Hu
Nov 20, 2001·Nature·M S Dresselhaus, I L Thomas
Jan 5, 2002·Science·Peter J Feibelman
Aug 4, 2006·The Journal of Physical Chemistry. B·Matthew P Hyman, J Will Medlin
Oct 27, 2006·The Journal of Physical Chemistry. B·Jan RossmeislMatthew Neurock
Dec 3, 2008·The Journal of Chemical Physics·Fátima González SánchezLarryn W Diamond
Aug 27, 2009·Proceedings of the National Academy of Sciences of the United States of America·C HuangA Nilsson
Mar 4, 2011·Journal of Computational Chemistry·Stefan GrimmeLars Goerigk
Apr 26, 2011·The Journal of Chemical Physics·Ikutaro Hamada, Yoshitada Morikawa
Jun 15, 2011·Physical Chemistry Chemical Physics : PCCP·Matthew WatkinsAlexander L Shluger
Jul 25, 2012·Nature Materials·Javier CarrascoAngelos Michaelides
Nov 7, 2012·The Journal of Chemical Physics·Sigrídur GudmundsdóttirEgill Skúlason
Jan 17, 2013·The Journal of Chemical Physics·Javier CarrascoAngelos Michaelides
May 15, 2015·Angewandte Chemie·Youngsoon KimHeon Kang
Mar 5, 2016·ACS Central Science·Luca BellarosaNúria López
Sep 8, 2010·Science and Technology of Advanced Materials·Takeshi Fukuma
Feb 9, 2017·Proceedings of the National Academy of Sciences of the United States of America·Tao ChengWilliam A Goddard
Sep 20, 2017·Chemistry : a European Journal·Youngsoon KimHeon Kang

❮ Previous
Next ❯

Citations

Nov 17, 2019·The Journal of Chemical Physics·Peter S Rice, P Hu
Jun 9, 2021·Journal of Chemical Theory and Computation·Jiayan XuP Hu
Jul 21, 2021·The Journal of Physical Chemistry Letters·Jun LongJianping Xiao
Sep 10, 2021·The Journal of Physical Chemistry Letters·Jia-Bo LeJun Cheng
Oct 28, 2021·The Journal of Physical Chemistry Letters·Peter S RiceP Hu

❮ Previous
Next ❯

Methods Mentioned

BETA
atomic
X-ray
neutron diffraction

Software Mentioned

AIMD
VASP
Vienna ab initio simulation package ( VASP )

Related Concepts

Trending Feeds

COVID-19

Coronaviruses encompass a large family of viruses that cause the common cold as well as more serious diseases, such as the ongoing outbreak of coronavirus disease 2019 (COVID-19; formally known as 2019-nCoV). Coronaviruses can spread from animals to humans; symptoms include fever, cough, shortness of breath, and breathing difficulties; in more severe cases, infection can lead to death. This feed covers recent research on COVID-19.

Blastomycosis

Blastomycosis fungal infections spread through inhaling Blastomyces dermatitidis spores. Discover the latest research on blastomycosis fungal infections here.

Nuclear Pore Complex in ALS/FTD

Alterations in nucleocytoplasmic transport, controlled by the nuclear pore complex, may be involved in the pathomechanism underlying multiple neurodegenerative diseases including Amyotrophic Lateral Sclerosis and Frontotemporal Dementia. Here is the latest research on the nuclear pore complex in ALS and FTD.

Applications of Molecular Barcoding

The concept of molecular barcoding is that each original DNA or RNA molecule is attached to a unique sequence barcode. Sequence reads having different barcodes represent different original molecules, while sequence reads having the same barcode are results of PCR duplication from one original molecule. Discover the latest research on molecular barcoding here.

Chronic Fatigue Syndrome

Chronic fatigue syndrome is a disease characterized by unexplained disabling fatigue; the pathology of which is incompletely understood. Discover the latest research on chronic fatigue syndrome here.

Evolution of Pluripotency

Pluripotency refers to the ability of a cell to develop into three primary germ cell layers of the embryo. This feed focuses on the mechanisms that underlie the evolution of pluripotency. Here is the latest research.

Position Effect Variegation

Position Effect Variagation occurs when a gene is inactivated due to its positioning near heterochromatic regions within a chromosome. Discover the latest research on Position Effect Variagation here.

STING Receptor Agonists

Stimulator of IFN genes (STING) are a group of transmembrane proteins that are involved in the induction of type I interferon that is important in the innate immune response. The stimulation of STING has been an active area of research in the treatment of cancer and infectious diseases. Here is the latest research on STING receptor agonists.

Microbicide

Microbicides are products that can be applied to vaginal or rectal mucosal surfaces with the goal of preventing, or at least significantly reducing, the transmission of sexually transmitted infections. Here is the latest research on microbicides.