Study on the Structure-Activity Relationship Between Single-Atom, Cluster and Nanoparticle Catalysts in a Hierarchical Structure for the Oxygen Reduction Reaction

Li, Yanyan1,2; Zhu, Xiaorong3; Li, Lei1,2; Li, Fayan1,2; Zhang, Xinyu1,2; Li, Yafei3; Zheng, Zhiping1,2

2021-12-01

10.1002/smll.202105487

Small   影响因子和分区

1613-6810

1613-6829

Literature reports have shown that in primary structures, single-atom catalysts exhibit better performance than cluster and nanoparticles due to their maximum atom utilization and the fine-tuning of the electronic structure of the active sites. Hierarchical structures have recently been extensively studied because of increased active sites and orderliness of channels significantly improves the catalytic performance compare to primary structures especially in nanoparticles, however, the different sized effect of catalysts research has not been reported. Herein, a unique hollow double-shell structure (a distinct cavity-containing) is used as a hierarchical model to study the possible difference between single atom, cluster, and nanoparticle and to establish the corresponding structure-activity relationship. Three Co catalysts are prepared: single atoms (Co-Catalyst-1), clusters (Co-Catalyst-2, 0.5-1 nm), and nanoparticles (Co-Catalyst-3, approximate to 5 nm) and their oxygen-reduction capacity is evaluated. The unique electronic interactions, the strong electron-withdrawing ability of N in Co-N-4 (Co-Catalyst-1), attract electrons from the electrode to Co, specifically by expediting the generation and transformation of the rate-determining step intermediates *OOH. The variant spatial structure which is caused by Co atom aggregation, and led to surface area, pore size, and carbon disorder, is a distinct, therefore significant variation in mass and charge transport efficiency, and activities.

electrocatalysts hierarchical structure oxygen reduction reaction structure-activity relationship

SCI ; EI

英语

第一 ; 通讯

Shenzhen Nobel Prize Scientists Laboratory Project[C17213101] ; Guangdong Provincial Key Laboratory of Catalysis[2020B121201002] ; Guangdong Provincial Key Laboratory of Energy Materials for Electric Power[2018B030322001] ; 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:000726285500001

WILEY-V C H VERLAG GMBH

20214911278386

Atoms ; Catalyst activity ; Electrocatalysts ; Electrolytic reduction ; Electronic structure ; Hierarchical systems ; Nanocatalysts ; Oxygen ; Pore size

Ore Treatment:533.1 ; Nanotechnology:761 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Physical Properties of Gases, Liquids and Solids:931.2 ; Atomic and Molecular Physics:931.3 ; Solid State Physics:933 ; Materials Science:951 ; Systems Science:961

Web of Science

1.Southern Univ Sci & Technol, Minist Educ, Guangdong Prov Key Lab Energy Mat Elect Power, Dept Chem, Shenzhen 518055, Peoples R China
2.Southern Univ Sci & Technol, Minist Educ, Key Lab Energy Convers & Storage Technol, Shenzhen 518055, Peoples R China
3.Nanjing Normal Univ, Sch Chem & Mat Sci, Jiangsu Collaborat Innovat Ctr Biomed Funct Mat, Nanjing 210023, Peoples R China

Li, Yanyan,Zhu, Xiaorong,Li, Lei,et al. Study on the Structure-Activity Relationship Between Single-Atom, Cluster and Nanoparticle Catalysts in a Hierarchical Structure for the Oxygen Reduction Reaction[J]. Small,2021,18.

Li, Yanyan.,Zhu, Xiaorong.,Li, Lei.,Li, Fayan.,Zhang, Xinyu.,...&Zheng, Zhiping.(2021).Study on the Structure-Activity Relationship Between Single-Atom, Cluster and Nanoparticle Catalysts in a Hierarchical Structure for the Oxygen Reduction Reaction.Small,18.

Li, Yanyan,et al."Study on the Structure-Activity Relationship Between Single-Atom, Cluster and Nanoparticle Catalysts in a Hierarchical Structure for the Oxygen Reduction Reaction".Small 18(2021).