Developing negative differential resistance (NDR) devices that simultaneously exhibit high conductance and a large peak-to-valley current ratio (PVCR) remains a critical challenge for the realization of molecular-scale logic circuits. The electronic transport properties of 4,4',-(pyrene-1,6-diylbis(ethyne-2,1-diyl)) dianiline (PDE) molecular devices were studied using density functional theory combined with first principles calculations of non-equilibrium Green's functions, exploring the regulatory mechanism of electrode materials and anchoring groups on NDR effects. We first fully optimizes the geometric structure of isolated molecules and electrode cells, with the convergence standard of residual force on each atom set to be less than 0.02 eV/Å. The exchange and correlations were described by the Perdew-Burke-Ernzerhof (PBE) functional under the generalized gradient approximation (GGA). The research results indicate that the PDE molecular devices using gold electrodes has a continuous and high density of states, and strong hybridization with molecular orbitals leads to broadening of the transport peak, exhibiting only monotonically increasing current voltage characteristics. Due to the low density of states near the Fermi level, PDE molecular devices using zigzag graphene nanoribbon (ZGNR) electrodes do not cause hybridization or broadening of molecular orbitals, maintaining the sharp resonance state of molecular orbitals and achieving significant NDR effects. The interface coupling changes caused by anchoring groups can regulate the alignment relationship between the frontier molecular orbitals and the electrode Fermi level, playing a decisive regulatory role in the NDR effect. The amide group forms strong π-π conjugated coupling with the molecular skeleton and ZGNR electrode through carbonyl groups, constructing efficient and continuous electron transport channels. The amino anchoring group triggers destructive interference at the coupling interface between the molecule and the electrode, significantly reducing the conductivity of the device, resulting in a significant attenuation of the peak current of the devices. These findings not only deepen our understanding of the quantum transport mechanism at carbon based molecular interfaces, but also provide clear theoretical guidance and material design paradigms for the future development of low-power, high-performance molecular switches, logic gates, and high-frequency oscillators.