journal article·2018-09-20Open access

One-Pot Pyrolysis Method to Fabricate Carbon Nanotube Supported Ni Single-Atom Catalysts with Ultrahigh Loading

Shiyong Zhao, Yi Cheng, Jean-Pierre Veder, Bernt Johannessen, Martin Saunders, Lianji Zhang, Chang Liu, Matthew F. Chisholm, Roland De Marco, Jian Liu, Shi-Ze Yang, San Ping Jiang

Abstract

The practical application of single atom catalysts (SACs) is constrained by the low achievable loading of single metal atoms. Here, nickel SACs stabilized on a nitrogen-doped carbon nanotube structure (NiSA-N-CNT) with ultrahigh Ni atomic loading up to 20.3 wt % have been successfully synthesized using a new one-pot pyrolysis method employing Ni acetylacetonate (Ni(acac)2) and dicyandiamide (DCD) as precursors. The yield and formation of NiSA-N-CNT depends strongly on the Ni(acac)2/DCD ratio and annealing temperature. Pyrolysis at 350 and 650 °C led to the formation of Ni single atom dispersed melem and graphitic carbon nitride (Ni-melem and Ni-g-C3N4). Transition from a stacked and layered Ni-g-C3N4 structure to a bamboo-shaped tubular NiSA-N-CNT structure most likely occurs via a solid-to-solid curling or rolling-up mechanism, thermally activated at temperatures of 700–900 °C. Extended X-ray absorption fine structure (EXAFS) experiments and simulations show that Ni single atoms are stabilized in the N-CNT structure through nitrogen coordination, forming a structure with four nearest N coordination shell surrounded by two carbon shells, Ni–N4. The NiSA-N-CNT catalysts show an excellent activity and selectivity for the electrochemical reduction of CO2, achieving a turnover frequency (TOF) of 11.7 s–1 at −0.55 V (vs RHE), but a low activity for the O2 reduction and O2 evolution reactions, as compared to Ni nanoparticles supported on N-CNTs.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Electrocatalysts for Energy Conversion · Supercapacitor Materials and Fabrication · Catalytic Processes in Materials Science

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Fuels and Energy Technology Institute & Western Australia School of Mines: Minerals, Energy and Chemical Engineering, Curtin University, Perth, Western Australia 6102, Australia

John de Laeter Centre, Curtin University, Perth, Western Australia 6102, Australia

Australian Synchrotron, Clayton, Victoria 3168, Australia

Centre for Microscopy, Characterization and Analysis (CMCA) and School of Molecular Sciences, The University of Western Australia, Perth, Western Australia 6009, Australia

Engineering Alloys Division, Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, Liaoning 110016, China

Advanced Carbon Division, Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, Liaoning 110016, China

Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States

Faculty of Science, Health, Education and Engineering, University of Sunshine Coast, Maroochydore DC, Queensland 4558, Australia

School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane, Queensland 4072, Australia

Department of Chemical and Process Engineering and Advanced Technology Institute, University of Surry, Guildford, Surry GU2 7XH, U.K.

Funding

Australian Research Council · National Natural Science Foundation of China

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