CO2 Overall Splitting by a Bifunctional Metal‐Free Electrocatalyst
- 20 August 2018
- journal article
- research article
- Published by Wiley in Angewandte Chemie International Edition
- Vol. 57 (40) , 13135-13139
Abstract
Photo/electrochemical CO2 splitting is impeded by the low cost‐effective catalysts for key reactions: CO2 reduction (CDRR) and water oxidation. A porous silicon and nitrogen co‐doped carbon (SiNC) nanomaterial by a facile pyrolyzation was developed as a metal‐free bifunctional electrocatalyst. CO2‐to‐CO and oxygen evolution (OER) partial current density under neutral conditions were enhanced by two orders of magnitude in the Tafel regime on SiNC relative to single‐doped comparisons beyond their specific area gap. The photovoltaic‐driven CO2 splitting device with SiNC electrodes imitating photosynthesis yielded an overall solar‐to‐chemical efficiency of advanced 12.5 % (by multiplying energy efficiency of CO2 splitting cell and photovoltaic device) at only 650 mV overpotential. Mechanism studies suggested the elastic electron structure of −Si(O)−C−N− unit in SiNC as the highly active site for CDRR and OER simultaneously by lowering the free energy of CDRR and OER intermediates adsorption.Keywords
This publication has 33 references indexed in Scilit:
- The role of reticular chemistry in the design of CO2 reduction catalystsNature Materials, 2018
- Technical photosynthesis involving CO2 electrolysis and fermentationNature Catalysis, 2018
- Theory-driven design of high-valence metal sites for water oxidation confirmed using in situ soft X-ray absorptionNature Chemistry, 2017
- Solar thermochemical splitting of CO2 into separate streams of CO and O2 with high selectivity, stability, conversion, and efficiencyEnergy & Environmental Science, 2017
- Materials for solar fuels and chemicalsNature Materials, 2016
- Water splitting–biosynthetic system with CO 2 reduction efficiencies exceeding photosynthesisScience, 2016
- Efficient electrolyzer for CO 2 splitting in neutral water using earth-abundant materialsProceedings of the National Academy of Sciences, 2016
- Simultaneous Reduction of CO2 and Splitting of H2O by a Single Immobilized Cobalt Phthalocyanine ElectrocatalystACS Catalysis, 2016
- Future ocean hypercapnia driven by anthropogenic amplification of the natural CO2 cycleNature, 2016
- Influence of Vibrational States on CO2 Splitting by Dielectric Barrier DischargesThe Journal of Physical Chemistry C, 2012