Regulating Morphological Features of Nickel Single-Atom Catalysts for Selective and Enhanced Electroreduction of CO2

Li, Lei1,2; Jiang, Zhan3; Li, Yanyan1,2; Li, Fayan1,2; Pan, Yingying1,2; Zhang, Xinyu1,2; Liang, Yongye3; Zheng, Zhiping1,2

2022-12-01

10.1002/smtd.202201213

Small Methods   影响因子和分区

2366-9608

Single-atom catalysts (SACs) are of interest for chemical transformations of significant energy and environmental relevance because of the envisioned efficient use of active sites and the flexibility in tuning their coordination environment. Future advancement in this vein hinges upon the ability to further increase the number and accessibility of active sites in addition to fine-tuning their chemical environment. In this work, a Ni SAC is reported with a unique hierarchical hollow structure (Ni/HH) that allows increased accessibility of the active sites. The successful obtainment of such a uniquely structured catalyst was enabled by the judiciously chosen solvent mixtures for the preparation of the precursor whose hierarchical feature is maintained during the subsequent pyrolysis and etching of the pyrolysis product. Comparative catalytic and mechanistic studies with reference to three closely related but more compact Ni SACs established the superior performance of Ni/HH for selective electroreduction of CO2 to CO. Experimental analyses by in situ attenuated total reflection surface-enhanced infrared spectroscopy reveal that it is the facilitated formation of the *COOH intermediate in the rate-determining step that leads to the enhanced reaction kinetics and the overall catalytic performance.

CO2 reduction reaction diverse geometric structures intermediate monitoring mechanistic insights 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[K21217502]

Chemistry ; Science & Technology - Other Topics ; Materials Science

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:000900150900001

WILEY-V C H VERLAG GMBH

20225213287126

Atoms ; Catalysis ; Catalyst activity ; Coordination reactions ; Electrolytic reduction ; Etching ; Infrared spectroscopy ; Nickel ; Nickel compounds ; Reaction intermediates ; Reaction kinetics ; Surface reactions ; Tuning

Ore Treatment:533.1 ; Nickel:548.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Atomic and Molecular Physics:931.3

Web of Science

1.Southern Univ Sci & Technol, Dept Chem, Guangdong Prov Key Lab Energy Mat Elect Power, Shenzhen 518055, Peoples R China
2.Southern Univ Sci & Technol, Key Lab Energy Convers & Storage Technol, Minist Educ, Shenzhen 518055, Peoples R China
3.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China

Li, Lei,Jiang, Zhan,Li, Yanyan,et al. Regulating Morphological Features of Nickel Single-Atom Catalysts for Selective and Enhanced Electroreduction of CO2[J]. Small Methods,2022,7(1).

Li, Lei.,Jiang, Zhan.,Li, Yanyan.,Li, Fayan.,Pan, Yingying.,...&Zheng, Zhiping.(2022).Regulating Morphological Features of Nickel Single-Atom Catalysts for Selective and Enhanced Electroreduction of CO2.Small Methods,7(1).

Li, Lei,et al."Regulating Morphological Features of Nickel Single-Atom Catalysts for Selective and Enhanced Electroreduction of CO2".Small Methods 7.1(2022).