Visualization of atomic scale reaction dynamics of supported nanocatalysts during oxidation and ammonia synthesis using in-situ environmental (scanning) transmission electron microscopy

TY - JOUR

T1 - Visualization of atomic scale reaction dynamics of supported nanocatalysts during oxidation and ammonia synthesis using in-situ environmental (scanning) transmission electron microscopy

AU - Ward, Michael R.

AU - Mitchell, Robert W.

AU - Boyes, Edward D.

AU - Gai, Pratibha L.

N1 - © 2020 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. This is an author-produced version of the published paper. Uploaded in accordance with the publisher’s self-archiving policy.

PY - 2021/6

Y1 - 2021/6

N2 - Reaction dynamics in gases at operating temperatures at the atomic level are the basis of heterogeneous gas–solid catalyst reactions and are crucial to the catalyst function. Supported noble metal nanocatalysts such as platinum are of interest in fuel cells and as diesel oxidation catalysts for pollution control, and practical ruthenium nanocatalysts are explored for ammonia synthesis. Graphite and graphitic carbons are of interest as supports for the nanocatalysts. Despite considerable literature on the catalytic processes on graphite and graphitic supports, reaction dynamics of the nanocatalysts on the supports in different reactive gas environments and operating temperatures at the single atom level are not well understood. Here we present real time in-situ observations and analyses of reaction dynamics of Pt in oxidation, and practical Ru nanocatalysts in ammonia synthesis, on graphite and related supports under controlled reaction environments using a novel in-situ environmental (scanning) transmission electron microscope with single atom resolution. By recording snapshots of the reaction dynamics, the behaviour of the catalysts is imaged. The images reveal single metal atoms, clusters of a few atoms on the graphitic supports and the support function. These all play key roles in the mobility, sintering and growth of the catalysts. The experimental findings provide new structural insights into atomic scale reaction dynamics, morphology and stability of the nanocatalysts.

AB - Reaction dynamics in gases at operating temperatures at the atomic level are the basis of heterogeneous gas–solid catalyst reactions and are crucial to the catalyst function. Supported noble metal nanocatalysts such as platinum are of interest in fuel cells and as diesel oxidation catalysts for pollution control, and practical ruthenium nanocatalysts are explored for ammonia synthesis. Graphite and graphitic carbons are of interest as supports for the nanocatalysts. Despite considerable literature on the catalytic processes on graphite and graphitic supports, reaction dynamics of the nanocatalysts on the supports in different reactive gas environments and operating temperatures at the single atom level are not well understood. Here we present real time in-situ observations and analyses of reaction dynamics of Pt in oxidation, and practical Ru nanocatalysts in ammonia synthesis, on graphite and related supports under controlled reaction environments using a novel in-situ environmental (scanning) transmission electron microscope with single atom resolution. By recording snapshots of the reaction dynamics, the behaviour of the catalysts is imaged. The images reveal single metal atoms, clusters of a few atoms on the graphitic supports and the support function. These all play key roles in the mobility, sintering and growth of the catalysts. The experimental findings provide new structural insights into atomic scale reaction dynamics, morphology and stability of the nanocatalysts.

KW - Ammonia synthesis

KW - Atomic scale reaction dynamics

KW - In-situ environmental scanning transmission electron microscopy with single atom resolution

KW - In-situ visualization

KW - Oxidation reactions

KW - Supported nanoparticles

UR - http://www.scopus.com/inward/record.url?scp=85092159216&partnerID=8YFLogxK

U2 - 10.1016/j.jechem.2020.08.069

DO - 10.1016/j.jechem.2020.08.069

M3 - Article

AN - SCOPUS:85092159216

SN - 2095-4956

VL - 57

SP - 281

EP - 290

JO - Journal of Energy Chemistry

JF - Journal of Energy Chemistry

ER -