Partial Thermal Condensation Mediated Synthesis of High-Density Nickel Single Atom Sites on Carbon Nitride for Selective Photooxidation of Methane into Methanol

Pawan Kumar, Peter Antal, Xiyang Wang, Jiu Wang, Dhwanil Trivedi, Ondřej František Fellner, Yimin A. Wu, Ivan Nemec, Vinicius Tadeu Santana, Josef Kopp, Petr Neugebauer, Jinguang Hu, Md Golam Kibria, Subodh Kumar

Research output: Contribution to journalArticlepeer-review

Abstract

Direct selective transformation of greenhouse methane (CH4) to liquid oxygenates (methanol) can substitute energy-intensive two-step (reforming/Fischer–Tropsch) synthesis while creating environmental benefits. The development of inexpensive, selective, and robust catalysts that enable room temperature conversion will decide the future of this technology. Single-atom catalysts (SACs) with isolated active centers embedded in support have displayed significant promises in catalysis to drive challenging reactions. Herein, high-density Ni single atoms are developed and stabilized on carbon nitride (NiCN) via thermal condensation of preorganized Ni-coordinated melem units. The physicochemical characterization of NiCN with various analytical techniques including HAADF-STEM and X-ray absorption fine structure (XAFS) validate the successful formation of Ni single atoms coordinated to the heptazine-constituted CN network. The presence of uniform catalytic sites improved visible absorption and carrier separation in densely populated NiCN SAC resulting in 100% selective photoconversion of (CH4) to methanol using H2O2 as an oxidant. The superior catalytic activity can be attributed to the generation of high oxidation (NiIII═O) sites and selective C─H bond cleavage to generate •CH3 radicals on Ni centers, which can combine with •OH radicals to generate CH3OH.

Original languageEnglish
JournalSmall
Early online date27 Nov 2023
DOIs
StateE-pub ahead of print - 27 Nov 2023
Externally publishedYes

Bibliographical note

Publisher Copyright:
© 2023 The Authors. Small published by Wiley-VCH GmbH.

Keywords

  • Ni single atom catalysts
  • carbon nitride
  • heterogeneous catalysts
  • methane oxidation
  • photocatalysis

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