A fundamental viewpoint on the hydrogen spillover phenomenon of electrocatalytic hydrogen evolution.

Nature Communications
Jiayuan LiYuanyuan Ma

Abstract

Hydrogen spillover phenomenon of metal-supported electrocatalysts can significantly impact their activity in hydrogen evolution reaction (HER). However, design of active electrocatalysts faces grand challenges due to the insufficient understandings on how to overcome this thermodynamically and kinetically adverse process. Here we theoretically profile that the interfacial charge accumulation induces by the large work function difference between metal and support (∆Φ) and sequentially strong interfacial proton adsorption construct a high energy barrier for hydrogen transfer. Theoretical simulations and control experiments rationalize that small ∆Φ induces interfacial charge dilution and relocation, thereby weakening interfacial proton adsorption and enabling efficient hydrogen spillover for HER. Experimentally, a series of Pt alloys-CoP catalysts with tailorable ∆Φ show a strong ∆Φ-dependent HER activity, in which PtIr/CoP with the smallest ∆Φ = 0.02 eV delivers the best HER performance. These findings have conclusively identified ∆Φ as the criterion in guiding the design of hydrogen spillover-based binary HER electrocatalysts.

References

Dec 15, 1996·Physical Review. B, Condensed Matter·J P PerdewY Wang
Nov 20, 2001·Nature·M S Dresselhaus, I L Thomas
Aug 18, 2004·Science·John A Turner
Oct 18, 2006·Proceedings of the National Academy of Sciences of the United States of America·Nathan S Lewis, Daniel G Nocera
Dec 5, 2006·Nature Materials·Anderson Janotti, Chris G Van de Walle
Jun 19, 2009·ACS Nano·Abhishek K SinghBoris I Yakobson
Oct 15, 2009·Journal of the American Chemical Society·Dongping ZhanMichael V Mirkin
Apr 23, 2011·Journal of the American Chemical Society·Yanguang LiHongjie Dai
Feb 14, 2012·Chemical Reviews·R Prins
Aug 17, 2012·Nature·Steven Chu, Arun Majumdar
Feb 8, 2013·Nano Letters·Desheng KongYi Cui
Feb 11, 2015·Journal of the American Chemical Society·Charles C L McCroryThomas F Jaramillo
Feb 13, 2015·Chemical Society Reviews·Yan JiaoShi Zhang Qiao
Nov 1, 2016·Journal of the American Chemical Society·Gong ZhangJinghong Li
Dec 3, 2016·Nature Communications·Niancai ChengXueliang Sun
Jan 6, 2017·Nature·Waiz KarimJeroen A van Bokhoven
Nov 10, 2017·Angewandte Chemie·Zechao ZhuangLiqiang Mai
Jun 1, 2021·ACS Energy Letters·Johannes Novak HansenIb Chorkendorff

❮ Previous
Next ❯

Software Mentioned

Materials Studio
CASTEP

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.