Journal
ACS CATALYSIS
Volume 7, Issue 9, Pages 6120-6127Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.7b01067
Keywords
covalent organic polymer (COP); hydrogen evolution reaction (HER); metal-free electrocatalyst; volcano plot; Tafel slope; density functional theory (DFT)
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Funding
- DST
- Science and Engineering Research Board (SERB), New Delhi, India [SB/S1/IC-15/2013]
- Department of Organic Chemistry, IACS, Kolkata through the DBT [BT/01/CEIB/11/V/13]
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Metal-free catalysis for electrocatalytic hydrogen evolution from water is very demanding for the production of sustainable and clean fuel. Herein, we report the synthesis of a porphyrin-based metal-free covalent organic polymer (TpPAM) through a simple condensation between triformyl phloroglucinol (Tp) and 5,10,15,20-tetra-(4-amino-phenyl)-21H,23H-porphyrin (PAM). The as-prepared porous TpPAM exhibited superior activity for the hydrogen evolution reaction (HER) current density of 10 mA cm(-2) at a low overpotential of 250 mV and a small Tafel slope of 106 mV decade(-1), which are better than those of related metal-free electrocatalysts. The high HER activity of TpPAM was investigated in-depth via theoretical density functional theory (DFT) calculations. The theoretical findings were correlated with the experimental results, and these were in good agreement for high HER catalytic efficiency of the porous TpPAM polymer. The Faradaic efficiency of the TpPAM-based electrode was found to be 98%, which is very close to the ideal value of 100%, reflecting its potential for practical implementation. Moreover, the as-synthesized catalyst showed good stability by retaining 91% of the initial current density after 1000 cycles.
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