Steering post-C–C coupling selectivity enables high efficiency electroreduction of carbon dioxide to multi-carbon alcohols

Zhuang, Tao‐Tao; Liang, Zhiqin; Seifitokaldani, Ali; Li, Yang; Luna, Phil De; Burdyny, Thomas; Che, Fanglin; Meng, Fancheng; Min, Yimeng; Quintero-Bermúdez, Rafael; Dinh, Cao-Thang; Pang, Yuanjie; Zhong, Miao; Zhang, Bo; Li, Jun; Chen, Peining; Zheng, Xueli; Liang, Hongyan; Ge, Wenna; Ye, Bangjiao; Sinton, David; Yu, Shu‐Hong

doi:10.1038/s41929-018-0084-7

Cited by 563 publications

(463 citation statements)

References 55 publications

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“…To the best of our knowledge, this is one of the most selective catalyst for producing multi-carbon products reported to date (Supporting Information, Table S1). 11,24,[47][48][49][50][51][52] We have recently proposed that the Cu surface roughness factor (RF) is a good descriptor for selectivity to multi-carbon product formed via the CO 2 RR over Cu. 53 Higher surface roughness increases the exposure of undercoordinated Cu surface sites that strongly bind adsorbed CO, thereby promoting the reduction of adsorbed CO rather than its desorption, and creating square sites next to steps that stabilize intermediates (e.g., OC-CO, OC-CHO) involved in the formation of C 2 products (C 2 H 4 and C 2 H 5 OH).…”

Section: Resultsmentioning

confidence: 99%

Production of C₂/C₃ Oxygenates from Planar Copper Nitride-Derived Mesoporous Copper via Electrochemical Reduction of CO₂

et al. 2020

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Electrochemical reduction of CO 2 provides an opportunity to produce fuels and chemicals in a carbon-neutral manner, assuming that CO 2 can be captured from the atmosphere. To do so, requires efficient, selective, and stable catalysts. In this study, we report a highly mesoporous metallic Cu catalyst prepared by electrochemical reduction of thermally nitrided Cu foil.Under aqueous saturated CO 2 reduction conditions, the Cu 3 N-derived Cu electrocatalyst produces virtually no CH 4 , very little CO, and exhibits a Faradaic efficiency of 68% to C 2+ products (C 2 H 4 , C 2 H 5 OH, and C 3 H 7 OH) at a current density of ~18.5 mA cm -2 and a cathode potential of -1.0 V vs. the reversible hydrogen electrode (RHE). Under these conditions, the catalyst produces more oxygenated products than hydrocarbons. We show that surface roughness is a good descriptor of catalytic performance. The roughest surface reached 98% CO utilization efficiency for C 2+ product formation from CO 2 reduction and the ratio of oxygenated to hydrocarbon products correlates with the degree of surface roughness. These effects of surface roughness are attributed to the high population of under-coordinated sites as well as a high pH environment within the mesopores and adjacent to the surface of the catalyst.

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Section: Resultsmentioning

confidence: 99%

Production of C₂/C₃ Oxygenates from Planar Copper Nitride-Derived Mesoporous Copper via Electrochemical Reduction of CO₂

et al. 2020

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“…Defects of electrocatalysts, such as atom vacancies and dopants, show the possibility of adsorbing unconventional ECR intermediates and, thus, selectively enhancing the corresponding pathway toward oxygenates (29,43,100). Taking *C 2 H 3 O as an example, which is the potential penultimate intermediate for ethylene and ethanol production, Sargent and co-workers (43) studied the role of defects in a core-shell Cu electrocatalyst in detail.…”

Section: Multicarbon Oxygenatesmentioning

confidence: 99%

Strategies in catalysts and electrolyzer design for electrochemical CO ₂ reduction toward C ₂₊ products

et al. 2020

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In light of environmental concerns and energy transition, electrochemical CO 2 reduction (ECR) to value-added multicarbon (C 2+ ) fuels and chemicals, using renewable electricity, presents an elegant long-term solution to close the carbon cycle with added economic benefits as well. However, electrocatalytic C─C coupling in aqueous electrolytes is still an open challenge due to low selectivity, activity, and stability. Design of catalysts and reactors holds the key to addressing those challenges. We summarize recent progress in how to achieve efficient C─C coupling via ECR, with emphasis on strategies in electrocatalysts and electrocatalytic electrode/reactor design, and their corresponding mechanisms. In addition, current bottlenecks and future opportunities for C 2+ product generation is discussed. We aim to provide a detailed review of the state-of-the-art C─C coupling strategies to the community for further development and inspiration in both fundamental understanding and technological applications.

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“…Of important note, the commercial viability of CO 2 RR to different products depends on a series of factors including not only the market demand of the product, but also the material, manufacturing, and separation costs. Although it is intuitively more desirable to control the selectivity toward higher‐valued products such as ethylene, ethanol, acetate, n ‐propanol, or even C 4 products, recent technoeconomic analysis unambiguously points out that the two‐electron electrochemical CO 2 RR to CO or formic acid is the most economically viable, whereas those C 2 –C 4 products other than propanol are not even profitable . This is understandable because the electricity cost is the major contributor to the operation cost of CO 2 electrolyzer.…”

Section: Fundamentals Of Electrochemical Co2 Reductionmentioning

confidence: 99%

Promises of Main Group Metal–Based Nanostructured Materials for Electrochemical CO₂ Reduction to Formate

Han

Pan

et al. 2019

Advanced Energy Materials

417

355

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Selective CO2 reduction to formic acid or formate is the most technologically and economically viable approach to realize electrochemical CO2 valorization. Main group metal–based (Sn, Bi, In, Pb, and Sb) nanostructured materials hold great promise, but are still confronted with several challenges. Here, the current status, challenges, and future opportunities of main group metal–based nanostructured materials for electrochemical CO2 reduction to formate are reviewed. Firstly, the fundamentals of electrochemical CO2 reduction are presented, including the technoeconomic viability of different products, possible reaction pathways, standard experimental procedure, and performance figures of merit. This is then followed by detailed discussions about different types of main group metal–based electrocatalyst materials, with an emphasis on underlying material design principles for promoting the reaction activity, selectivity, and stability. Subsequently, recent efforts on flow cells and membrane electrode assembly cells are reviewed so as to promote the current density as well as mechanistic studies using in situ characterization techniques. To conclude a short perspective is offered about the future opportunities and directions of this exciting field.

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Steering post-C–C coupling selectivity enables high efficiency electroreduction of carbon dioxide to multi-carbon alcohols

Cited by 563 publications

References 55 publications

Production of C₂/C₃ Oxygenates from Planar Copper Nitride-Derived Mesoporous Copper via Electrochemical Reduction of CO₂

Production of C₂/C₃ Oxygenates from Planar Copper Nitride-Derived Mesoporous Copper via Electrochemical Reduction of CO₂

Strategies in catalysts and electrolyzer design for electrochemical CO ₂ reduction toward C ₂₊ products

Promises of Main Group Metal–Based Nanostructured Materials for Electrochemical CO₂ Reduction to Formate

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Steering post-C–C coupling selectivity enables high efficiency electroreduction of carbon dioxide to multi-carbon alcohols

Cited by 563 publications

References 55 publications

Production of C2/C3 Oxygenates from Planar Copper Nitride-Derived Mesoporous Copper via Electrochemical Reduction of CO2

Production of C2/C3 Oxygenates from Planar Copper Nitride-Derived Mesoporous Copper via Electrochemical Reduction of CO2

Strategies in catalysts and electrolyzer design for electrochemical CO 2 reduction toward C 2+ products

Promises of Main Group Metal–Based Nanostructured Materials for Electrochemical CO2 Reduction to Formate

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Product

Resources

About

Production of C₂/C₃ Oxygenates from Planar Copper Nitride-Derived Mesoporous Copper via Electrochemical Reduction of CO₂

Production of C₂/C₃ Oxygenates from Planar Copper Nitride-Derived Mesoporous Copper via Electrochemical Reduction of CO₂

Strategies in catalysts and electrolyzer design for electrochemical CO ₂ reduction toward C ₂₊ products

Promises of Main Group Metal–Based Nanostructured Materials for Electrochemical CO₂ Reduction to Formate