ja7b04892_si_001.pdf (2 MB)
Tunable Cu Enrichment Enables Designer Syngas Electrosynthesis from CO2
journal contribution
posted on 2017-06-28, 20:30 authored by Michael
B. Ross, Cao Thang Dinh, Yifan Li, Dohyung Kim, Phil De Luna, Edward H. Sargent, Peidong YangUsing renewable energy to recycle
CO2 provides an opportunity
to both reduce net CO2 emissions and synthesize fuels and
chemical feedstocks. It is of central importance to design electrocatalysts
that both are efficient and can access a tunable spectrum of products.
Syngas, a mixture of carbon monoxide (CO) and hydrogen (H2), is an important chemical precursor that can be converted downstream
into small molecules or larger hydrocarbons by fermentation or thermochemistry.
Many processes that utilize syngas require different syngas compositions:
we therefore pursued the rational design of a family of electrocatalysts
that can be programmed to synthesize different designer syngas ratios.
We utilize in situ surface-enhanced Raman spectroscopy
and first-principles density functional theory calculations to develop
a systematic picture of CO* binding on Cu-enriched Au surface model
systems. Insights from these model systems are then translated to
nanostructured electrocatalysts, whereby controlled Cu enrichment
enables tunable syngas production while maintaining current densities
greater than 20 mA/cm2.