Enhanced electrocatalytic CO2 reduction via field-induced reagent concentration View Full Text


Ontology type: schema:ScholarlyArticle     


Article Info

DATE

2016-09

AUTHORS

Min Liu, Yuanjie Pang, Bo Zhang, Phil De Luna, Oleksandr Voznyy, Jixian Xu, Xueli Zheng, Cao Thang Dinh, Fengjia Fan, Changhong Cao, F. Pelayo García de Arquer, Tina Saberi Safaei, Adam Mepham, Anna Klinkova, Eugenia Kumacheva, Tobin Filleter, David Sinton, Shana O. Kelley, Edward H. Sargent

ABSTRACT

Electrochemical reduction of carbon dioxide (CO2) to carbon monoxide (CO) is the first step in the synthesis of more complex carbon-based fuels and feedstocks using renewable electricity. Unfortunately, the reaction suffers from slow kinetics owing to the low local concentration of CO2 surrounding typical CO2 reduction reaction catalysts. Alkali metal cations are known to overcome this limitation through non-covalent interactions with adsorbed reagent species, but the effect is restricted by the solubility of relevant salts. Large applied electrode potentials can also enhance CO2 adsorption, but this comes at the cost of increased hydrogen (H2) evolution. Here we report that nanostructured electrodes produce, at low applied overpotentials, local high electric fields that concentrate electrolyte cations, which in turn leads to a high local concentration of CO2 close to the active CO2 reduction reaction surface. Simulations reveal tenfold higher electric fields associated with metallic nanometre-sized tips compared to quasi-planar electrode regions, and measurements using gold nanoneedles confirm a field-induced reagent concentration that enables the CO2 reduction reaction to proceed with a geometric current density for CO of 22 milliamperes per square centimetre at -0.35 volts (overpotential of 0.24 volts). This performance surpasses by an order of magnitude the performance of the best gold nanorods, nanoparticles and oxide-derived noble metal catalysts. Similarly designed palladium nanoneedle electrocatalysts produce formate with a Faradaic efficiency of more than 90 per cent and an unprecedented geometric current density for formate of 10 milliamperes per square centimetre at -0.2 volts, demonstrating the wider applicability of the field-induced reagent concentration concept. More... »

PAGES

382

Identifiers

URI

http://scigraph.springernature.com/pub.10.1038/nature19060

DOI

http://dx.doi.org/10.1038/nature19060

DIMENSIONS

https://app.dimensions.ai/details/publication/pub.1018432986

PUBMED

https://www.ncbi.nlm.nih.gov/pubmed/27487220


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