Linking Enhanced Kinetics of Electrocatalytic Oxygen Reduction Reaction with Increased Utilization of Active Sites in a Hierarchical Single-Atom Catalyst

Li，Lei1,2; Xu，Ming3; Wang，Yameng4; Zhang，Yanan2; Li，Yanyan1; Li，Fayan1; Zeng，Lin4; Zhang，Xinyu1; Zheng，Jiaxin3; Zheng，Zhiping1

2022

10.1002/smll.202205743

Small   影响因子和分区

1613-6810

1613-6829

Single-atom catalysts (SACs) are of tremendous current research due to maximized use of metal atoms and enhanced activity and selectivity for a great variety of chemical reactions. Hierarchically structured SACs have been explored to further increase the number and accessibility of active sites to realize the full potentials of SACs. However, though plausible-sounding, these supposed advantages of hierarchically structured SACs are largely untested. The assumed enhancing effects on the formation of intermediates on and the overall reaction kinetics remain largely unknown. Herein is reported a Fe-SAC with a hierarchical hollow structure (Fe/HH) that showed excellent activity in oxygen reduction reaction and proton exchange membrane fuel cell. Comparative experimental and computational studies with respect to Fe/SS—the counterpart of Fe/HH with a compact primary structure—reveal a significantly increased number of active sites and their utilization in Fe/HH as reflected by the facilitated formation of the rate-determining-step intermediate Fe-OOH*. This work thus establishes unambiguously the connection between the increased utilization of active sites and the enhanced kinetics of the electrocatalytic reduction of oxygen.

active site utilization hierarchical structures oxygen reduction reactions reaction kinetics single-atom catalysts

SCI ; EI

英语

第一 ; 通讯

Shenzhen Nobel Prize Scientists Laboratory Project[C17783101] ; Guangdong Provincial Key Laboratory of Catalysis[2020B121201002] ; Guangdong Provincial Key Laboratory of Energy Materials for Electric Power[2018B030322001] ; SUSTech["Y01216127","Y01216227"] ; Post-doctorate Scientific Research Fund for staying (coming to) Shenzhen[K21217502]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:000882541200001

WILEY-V C H VERLAG GMBH

20224713142224

Association reactions ; Atoms ; Catalyst activity ; Catalyst selectivity ; Electrolytic reduction ; Kinetics ; Oxygen ; Proton exchange membrane fuel cells (PEMFC) ; Reaction intermediates

Ore Treatment:533.1 ; Fluid Flow, General:631.1 ; Fuel Cells:702.2 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Classical Physics; Quantum Theory; Relativity:931 ; Atomic and Molecular Physics:931.3

2-s2.0-85142076152

Scopus

1.Department of Chemistry,Guangdong Provincial Key Laboratory of Energy Materials for Electric Power,and Key Laboratory of Energy Conversion and Storage Technologies (Ministry of Education),Southern University of Science and Technology,Shenzhen,518055,China
2.College of Chemistry & Chemical Engineering,Shaanxi Key Laboratory of Chemical Additives for Industry,Shaanxi University of Science and Technology,Xi'an,Shaanxi,710021,China
3.School of Advanced Materials,Peking University Shenzhen Graduate School,Shenzhen,518055,China
4.Department of Mechanical and Energy Engineering,Southern University of Science and Technology,Shenzhen,518055,China

Li，Lei,Xu，Ming,Wang，Yameng,et al. Linking Enhanced Kinetics of Electrocatalytic Oxygen Reduction Reaction with Increased Utilization of Active Sites in a Hierarchical Single-Atom Catalyst[J]. Small,2022,19(1).

Li，Lei.,Xu，Ming.,Wang，Yameng.,Zhang，Yanan.,Li，Yanyan.,...&Zheng，Zhiping.(2022).Linking Enhanced Kinetics of Electrocatalytic Oxygen Reduction Reaction with Increased Utilization of Active Sites in a Hierarchical Single-Atom Catalyst.Small,19(1).

Li，Lei,et al."Linking Enhanced Kinetics of Electrocatalytic Oxygen Reduction Reaction with Increased Utilization of Active Sites in a Hierarchical Single-Atom Catalyst".Small 19.1(2022).