TY - JOUR
T1 - Electrochemical CO2-to-ethylene conversion on polyamine-incorporated Cu electrodes
AU - Chen, Xinyi
AU - Chen, Junfeng
AU - Alghoraibi, Nawal M.
AU - Henckel, Danielle A.
AU - Zhang, Ruixian
AU - Nwabara, Uzoma O.
AU - Madsen, Kenneth E.
AU - Kenis, Paul J.A.
AU - Zimmerman, Steven C.
AU - Gewirth, Andrew A.
N1 - Funding Information:
The authors gratefully acknowledge the support of the International Institute for Carbon Neutral Energy Research (WPI-I2CNER), sponsored by the Japanese Ministry of Education, Culture, Sports, Science and Technology. D.A.H., U.O.N. and P.J.A.K. gratefully acknowledge Shell’s New Energy Research and Technology (NERT) programme for providing funding. J.C. and S.C.Z. acknowledge support of the National Science Foundation (NSF CHE-1709718). We thank the School of Chemical Sciences, University of Illinois Mass Spectrometry Laboratory (especially F. Sun and X. Mao) for performing gas chromatography mass spectrometry measurements. We thank R.T. Haasch for performing XPS and the School of Chemical Sciences, University of Illinois Machine Shop for their help in designing the in situ flow cell for the Raman measurements. We also thank the School of Chemical Sciences, University of Illinois NMR Laboratory for their help with the NMR measurements.
Publisher Copyright:
© 2020, The Author(s), under exclusive licence to Springer Nature Limited.
PY - 2021/1/1
Y1 - 2021/1/1
N2 - Electrochemical conversion of CO2 into value-added chemicals holds promise to enable the transition to carbon neutrality. Enhancing selectivity for a specific hydrocarbon product is challenging, however, due to numerous possible reaction pathways of CO2 electroreduction. Here we present a Cu–polyamine hybrid catalyst, developed through co-electroplating, that significantly increases the selectivity for ethylene production. The Faradaic efficiency for ethylene production is 87% ± 3% at −0.47 V versus reversible hydrogen electrode, with full-cell energetic efficiency reaching 50% ± 2%. Raman measurements indicate that the polyamine entrained on the Cu electrode results in higher surface pH, higher CO content and higher stabilization of intermediates compared with entrainment of additives containing little or no amine functionality. More broadly, this work shows that polymer incorporation can alter surface reactivity and lead to enhanced product selectivity at high current densities. [Figure not available: see fulltext.]
AB - Electrochemical conversion of CO2 into value-added chemicals holds promise to enable the transition to carbon neutrality. Enhancing selectivity for a specific hydrocarbon product is challenging, however, due to numerous possible reaction pathways of CO2 electroreduction. Here we present a Cu–polyamine hybrid catalyst, developed through co-electroplating, that significantly increases the selectivity for ethylene production. The Faradaic efficiency for ethylene production is 87% ± 3% at −0.47 V versus reversible hydrogen electrode, with full-cell energetic efficiency reaching 50% ± 2%. Raman measurements indicate that the polyamine entrained on the Cu electrode results in higher surface pH, higher CO content and higher stabilization of intermediates compared with entrainment of additives containing little or no amine functionality. More broadly, this work shows that polymer incorporation can alter surface reactivity and lead to enhanced product selectivity at high current densities. [Figure not available: see fulltext.]
UR - http://www.scopus.com/inward/record.url?scp=85097243897&partnerID=8YFLogxK
U2 - 10.1038/s41929-020-00547-0
DO - 10.1038/s41929-020-00547-0
M3 - Article
AN - SCOPUS:85097243897
SN - 2520-1158
VL - 4
SP - 20
EP - 27
JO - Nature Catalysis
JF - Nature Catalysis
IS - 1
ER -