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High carbon utilization in CO2 reduction to multi-carbon products in acidic media
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Journal Article
High carbon utilization in CO2 reduction to multi-carbon products in acidic media
2022
Overview
Renewable electricity-powered CO
2
reduction to multi-carbon (C
2+
) products offers a promising route to realization of low-carbon-footprint fuels and chemicals. However, a major fraction of input CO
2
(>85%) is consumed by the electrolyte through reactions with hydroxide to form carbonate/bicarbonate in both alkaline and neutral reactors. Acidic conditions offer a solution to overcoming this limitation, but also promote the hydrogen evolution reaction. Here we report a design strategy that suppresses hydrogen evolution reaction activity by maximizing the co-adsorption of CO and CO
2
on Cu-based catalysts to weaken H* binding. Using density functional theory studies, we found Pd–Cu promising for selective C
2+
production over C
1
, with the lowest ∆
G
OCCOH*
and ∆
G
OCCOH*
- ∆
G
CHO*
. We synthesized Pd–Cu catalysts and report a crossover-free system (liquid product crossover <0.05%) with a Faradaic efficiency of 89 ± 4% for CO
2
to C
2+
at 500 mA cm
−2
, simultaneous with single-pass CO
2
utilization of 60 ± 2% to C
2+
.
Acidic conditions present a solution to carbonate formation in CO
2
electrolysis but create a selectivity issue through competing H
2
evolution. Here, theoretical methods are used to optimize acidity and select Pd–Cu as a selective electrocatalyst for acidic CO
2
reduction with negligible carbonate crossover and high single-pass carbon efficiency.
Publisher
Nature Publishing Group UK,Nature Publishing Group
Subject
