Zisheng Zhang

All Publications

• Synthesis and characterization of low-dimensional N-heterocyclic carbene lattices SCIENCE Qie, B., Wang, Z., Jiang, J., Zhang, Z., Jacobse, P. H., Lu, J., Li, X., Liu, F., Alexandrova, A. N., Louie, S. G., Crommie, M. F., Fischer, F. R. 2024; 384 (6698): 895-901

  Abstract

  The covalent interaction of N-heterocyclic carbenes (NHCs) with transition metal atoms gives rise to distinctive frontier molecular orbitals (FMOs). These emergent electronic states have spurred the widespread adoption of NHC ligands in chemical catalysis and functional materials. Although formation of carbene-metal complexes in self-assembled monolayers on surfaces has been explored, design and electronic structure characterization of extended low-dimensional NHC-metal lattices remains elusive. Here we demonstrate a modular approach to engineering one-dimensional (1D) metal-organic chains and two-dimensional (2D) Kagome lattices using the FMOs of NHC-Au-NHC junctions to create low-dimensional molecular networks exhibiting intrinsic metallicity. Scanning tunneling spectroscopy and first-principles density functional theory reveal the contribution of C-Au-C π-bonding states to dispersive bands that imbue 1D- and 2D-NHC lattices with exceptionally small work functions.

  View details for DOI 10.1126/science.adm9814

  View details for Web of Science ID 001253631400002

  View details for PubMedID 38781380

• Tracking Active Phase Behavior on Boron Nitride during the Oxidative Dehydrogenation of Propane Using Operando X-ray Raman Spectroscopy. Journal of the American Chemical Society Cendejas, M. C., Paredes Mellone, O. A., Kurumbail, U., Zhang, Z., Jansen, J. H., Ibrahim, F., Dong, S., Vinson, J., Alexandrova, A. N., Sokaras, D., Bare, S. R., Hermans, I. 2023

  Abstract

  Hexagonal boron nitride (hBN) is a highly selective catalyst for the oxidative dehydrogenation of propane (ODHP) to propylene. Using a variety of ex situ characterization techniques, the activity of the catalyst has been attributed to the formation of an amorphous boron oxyhydroxide surface layer. The ODHP reaction mechanism proceeds via a combination of surface mediated and gas phase propagated radical reactions with the relative importance of both depending on the surface-to-void-volume ratio. Here we demonstrate the unique capability of operando X-ray Raman spectroscopy (XRS) to investigate the oxyfunctionalization of the catalyst under reaction conditions (1 mm outer diameter reactor, 500 to 550 °C, P = 30 kPa C3H8, 15 kPa O2, 56 kPa He). We probe the effect of a water cofeed on the surface of the activated catalyst and find that water removes boron oxyhydroxide from the surface, resulting in a lower reaction rate when the surface reaction dominates and an enhanced reaction rate when the gas phase contribution dominates. Computational description of the surface transformations at an atomic-level combined with high precision XRS spectra simulations with the OCEAN code rationalize the experimental observations. This work establishes XRS as a powerful technique for the investigation of light element-containing catalysts under working conditions.

  View details for DOI 10.1021/jacs.3c08679

  View details for PubMedID 37931025

• Molecular engineering of dispersed nickel phthalocyanines on carbon nanotubes for selective CO(2)reduction NATURE ENERGY Zhang, X., Wang, Y., Gu, M., Wang, M., Zhang, Z., Pan, W., Jiang, Z., Zheng, H., Lucero, M., Wang, H., Sterbinsky, G. E., Ma, Q., Wang, Y., Feng, Z., Li, J., Dai, H., Liang, Y. 2020

  View details for DOI 10.1038/s41560-020-0667-9

  View details for Web of Science ID 000558156800001