Chinese Journal of Applied Chemistry ›› 2020, Vol. 37 ›› Issue (10): 1187-1194.DOI: 10.11944/j.issn.1000-0518.2020.10.200088

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Promotion Effect of Functionalized Carbon Nitride on Pd-Based Catalyst for Hydrogen Generation from Formic Acid

SUN Zhiconga,b, MENG Qingleia,b, MA Rongpenga,b, GE Junjiea,b, LIU Changpenga,b*, XING Weia,b*   

  1. aLaboratory of Advanced Power Sources,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,China;
    bUniversity of Science and Technology of China,Hefei 230026,China
  • Received:2020-03-23 Published:2020-10-01 Online:2020-09-30
  • Contact: LIU Changpeng, professor; Tel:0431-85262225; E-mail:liuchp@ciac.ac.cn; Research interests:water electrolysis, formic acid decomposition, and fuel cell
    Co-rresponding author:XING Wei, professor; Tel:0431-85262225; E-mail:xingwei@ciac.ac.cn; Research interests:water electrolysis, formic acid decomposition, and fuel cell
  • Supported by:
    Supported by the National Natural Science Foundation of China(No.21633008, No.21433003), Jilin Province Science and Technology Development Program(No.20170203003SF), and the National Science and Technology Major Project(No.2017YFB0102900)

Abstract: The supported Pd-based catalyst is one of the most effective catalysts for the decomposition of formic acid into hydrogen, in which the N content of the carbon nitride support is relatively high. The carbon nitride prepared by one-step pyrolysis method is usually bulk, which makes it difficult to effectively disperse surface metal nanoparticles (NPs). Functionalized carbon nitride was obtained by pyrolyzing the urea precursor after solvation and used as a support. A functional carbon nitride-supported Pd-based catalyst (Pd/C3N4-F) was prepared by anion exchange and sodium borohydride direct reduction. The structure of the material was characterized by scanning electron microscope (SEM), transmission electron microscope (TEM) and X-ray photoelectron spectroscopy (XPS), and the performance of the catalyst was tested by gas mass flow meter. Pd/C3N4-F has excellent catalytic performance for hydrogen production from formic acid decomposition and its initial TOF (total conversion frequency) value and mass specific activity at 30 ℃ are 1824 h-1 and 17.14 molH2/(gPd·h), respectively. The analysis of the product by gas chromatography (GS) shows that no by-product CO is formed, indicating that it has excellent selectivity. With the increase of temperature (30~40 ℃), the catalyst performance gradually improves

Key words: functionalized carbon nitride, decomposition of formic acid to produce hydrogen, heterogeneous catalysis, Pd nanoparticle, low loading