• 文献标题:   One-Pot Synthesis of Ruthenium-Based Nanocatalyst Using Reduced Graphene Oxide as Matrix for Electrochemical Synthesis of Ammonia
  • 文献类型:   Article
  • 作  者:   SUN W, SAHIN NE, SUN D, WU X, MUNOZ C, THAKARE J, AULICH T, ZHANG J, HOU XD, ONCEL N, PIERCE D, ZHAO JX
  • 作者关键词:   nanocatalyst, rutheniumbased nanoparticles rubasednps, reduced graphene oxide rgo, electrocatalysi, electrochemical nitrogen reduction reaction enrr, electrochemical synthesis of nh3, ambient condition
  • 出版物名称:   ACS APPLIED MATERIALS INTERFACES
  • ISSN:   1944-8244 EI 1944-8252
  • 通讯作者地址:  
  • 被引频次:   1
  • DOI:   10.1021/acsami.2c18413 EA DEC 2022
  • 出版年:   2023

▎ 摘  要

Conventional ammonia production consumes significant energy and causes enormous carbon dioxide (CO2) emissions globally. To lower energy consumption and mitigate CO2 emissions, a facile, environmentally friendly, and cost-effective one-pot method for the synthesis of a ruthenium-based nitrogen reduction nanocatalyst has been developed using reduced graphene oxide (rGO) as a matrix. The nanocatalyst synthesis was based on a single-step simultaneous reduction of RuCl3 into ruthenium-based nanoparticles (Ru-based NPs) and graphene oxide (GO) into rGO using glucose as the reducing agent and stabilizer. The obtained ruthenium-based nanocatalyst with rGO as a matrix (Runano-based/ rGO) has shown much higher catalytic activity at lower temperatures and pressures for ammonia synthesis than conventional iron catalysts. The rGO worked as a promising promoter for the electrochemical synthesis of ammonia due to its excellent electrical and thermal conductivity. The developed Runano-based/rGO nanocatalyst was characterized using transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), scanning electron microscopy (SEM), energy-dispersive spectroscopy (EDS), ultraviolet-visible (UV-vis) absorption spectroscopy, X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FT-IR), dynamic light scattering (DLS), inductively coupled plasma mass spectrometry (ICP-MS), and X-ray photoelectron spectroscopy (XPS). The results demonstrated that the size of the Ru-based NPs on the surface of rGO was 1.9 +/- 0.2 nm and the ruthenium content was 25.03 wt %. Bulk electrolysis measurements were conducted on thin-layer electrodes at various cathodic potentials in a N2-saturated 0.1 M H2SO4 electrolyte at room temperature. From the chronoamperometric measurements, the maximum faradic efficiency (F.E.) of 2.1% for ammonia production on the nanostructured Runano-based/rGO electrocatalyst was achieved at a potential of -0.20 V vs reversible hydrogen electrode (RHE). This electrocatalyst has attained a superior ammonia production rate of 9.14 mu gmiddoth-1middotmgcat.-1. The results demonstrate the feasibility of reducing N2 into ammonia under ambient conditions and warrant further exploration of the nanostructured Runano-based/rGO for electrochemical ammonia synthesis.