Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 31, Pages 9640-9644Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201802055
Keywords
CO2 reduction; density functional calculations; energy conversion; fluorine; nanocatalysis
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Funding
- One Hundred Talents Program of the Chinese Academy of Sciences
- National Natural Science Foundation of China [51342009, 21501173]
- Natural Science Foundation of Fujian Province [2014J05027]
- Science and Technology Planning Project of Fujian Province [2014H2008]
- National Key R&D Program of China [2016YFB0100100]
- Strategic Priority Research Program, CAS [XDB20000000]
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The electrochemical CO2 reduction (ECDRR), as a key reaction in artificial photosynthesis to implement renewable energy conversion/storage, has been inhibited by the low efficiency and high costs of the electrocatalysts. Herein, we synthesize a fluorine-doped carbon (FC) catalyst by pyrolyzing commercial BP2000 with a fluorine source, enabling a highly selective CO2-to-CO conversion with a maximum Faradaic efficiency of 90% at a low overpotential of 510mV and a small Tafel slope of 81mVdec(-1), outcompeting current metal-free catalysts. Moreover, the higher partial current density of CO and lower partial current density of H-2 on FC relative to pristine carbon suggest an enhanced inherent activity towards ECDRR as well as a suppressed hydrogen evolution by fluorine doping. Fluorine doping activates the neighbor carbon atoms and facilitates the stabilization of the key intermediate COOH* on the fluorine-doped carbon material, which are also blocked for competing hydrogen evolution, resulting in superior CO2-to-CO conversion.
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