Efficient electrochemical CO2 conversion powered by renewable energy

Kauffman, Douglas R.; Thakkar, Jay; Siva, Rajan; Matranga, Christopher; Ohodnicki, Paul R.; Zeng, Chenjie; Jin, Rongchao

doi:10.1021/acsami.5b04393

Title: Efficient electrochemical CO₂ conversion powered by renewable energy

Journal Article · Mon Jun 29 00:00:00 EDT 2015 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.5b04393· OSTI ID:1240139

Kauffman, Douglas R. ^[1]; Thakkar, Jay ^[1]; Siva, Rajan ^[1]; Matranga, Christopher ^[1]; Ohodnicki, Paul R. ^[1]; Zeng, Chenjie ^[2]; Jin, Rongchao ^[2]

National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
Carnegie Mellon Univ., Pittsburgh, PA (United States)

Here, the catalytic conversion of CO₂ into industrially relevant chemicals is one strategy for mitigating greenhouse gas emissions. Along these lines, electrochemical CO₂ conversion technologies are attractive because they can operate with high reaction rates at ambient conditions. However, electrochemical systems require electricity, and CO₂ conversion processes must integrate with carbon-free, renewable-energy sources to be viable on larger scales. We utilize Au₂₅ nanoclusters as renewably powered CO₂ conversion electrocatalysts with CO₂ → CO reaction rates between 400 and 800 L of CO₂ per gram of catalytic metal per hour and product selectivities between 80 and 95%. These performance metrics correspond to conversion rates approaching 0.8–1.6 kg of CO₂ per gram of catalytic metal per hour. We also present data showing CO₂ conversion rates and product selectivity strongly depend on catalyst loading. Optimized systems demonstrate stable operation and reaction turnover numbers (TONs) approaching 6 × 10⁶ mol CO₂ molcatalyst–1 during a multiday (36 hours total hours) CO₂electrolysis experiment containing multiple start/stop cycles. TONs between 1 × 10⁶ and 4 × 10⁶ molCO₂ molcatalyst–1 were obtained when our system was powered by consumer-grade renewable-energy sources. Daytime photovoltaic-powered CO₂ conversion was demonstrated for 12 h and we mimicked low-light or nighttime operation for 24 h with a solar-rechargeable battery. This proof-of-principle study provides some of the initial performance data necessary for assessing the scalability and technical viability of electrochemical CO₂ conversion technologies. Specifically, we show the following: (1) all electrochemical CO₂ conversion systems will produce a net increase in CO₂ emissions if they do not integrate with renewable-energy sources, (2) catalyst loading vs activity trends can be used to tune process rates and product distributions, and (3) state-of-the-art renewable-energy technologies are sufficient to power larger-scale, tonne per day CO₂ conversion systems.

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Research Organization:: National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)

Sponsoring Organization:: USDOE Office of Fossil Energy (FE)

OSTI ID:: 1240139

Report Number(s):: NETL-PUB-1221

Journal Information:: ACS Applied Materials and Interfaces, Vol. 7, Issue 28; ISSN 1944-8244

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 171 works

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30 DIRECT ENERGY CONVERSION
electrocatalysis
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environmental

Title: Efficient electrochemical CO2 conversion powered by renewable energy

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Title: Efficient electrochemical CO₂ conversion powered by renewable energy