4.8 Article

Stable and Antisintering Tungsten Carbides with Controllable Active Phase for Selective Cleavage of Aryl Ether C-O Bonds

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 7, Pages 8274-8284

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c19599

Keywords

transition-metal carbides; stability; aromatic ethers; C-O bond cleavage; phase control; antisintering

Funding

  1. National Key Research and Development Program of China [2017YFA0206801, 2018YFB0604701]
  2. National Natural Science Foundation of China [21972113]
  3. Program for Innovative Research Team in Chinese Universities [IRT_14R31]

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A comprehensive strategy was developed to synthesize stable and well-defined tungsten carbide nanoparticles, which exhibited high stability and catalytic activity for selective cleavage of the aryl ether C-O bonds in lignin-derived aromatic ethers.
Transition-metal carbides are important materials in heterogeneous catalysis. It remains challenging yet attractive in nanoscience to construct the active phase of carbide catalysts in a controllable manner and keep a sintering-resistant property in redox reactions, especially hydroprocessing. In this work, an integrated strategy was presented to synthesize stable and well-defined tungsten carbide nanoparticles (NPs) by assembling the metal precursor onto carbon nanotubes (CNTs), wrapping a thin polymeric layer, and following a controlled carburization. The polymer served as a soft carbon source to modulate the metal/carbon ratio in the carbides and introduced amorphous carbons around the carbides to prevent the NPs from sintering. The as-built p-WxC/CNT displayed high stability in the hydrogenolysis of aryl ether C-O bond in guaiacol for more than 150 h. Its activity was more than two and six times higher than those prepared via typical temperature-programmed reduction with gaseous carbon (WxC/CNT-TPR) and carbothermal reduction with intrinsic carbon support (WxC/CNT-CTR), respectively. Our p-WxC/CNT catalyst also achieved high efficiency for selective cleavage of the aryl ether C-O bonds in lignin-derived aromatic ethers, including anisole, dimethoxylphenol, and diphenyl ether, with a robust lifespan.

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