High efficiency electrochemical reduction of CO<sub>2</sub> beyond the two-electron transfer pathway on grain boundary rich ultra-small SnO<sub>2</sub> nanoparticles

Liang, Chenglu; Kim, Byoungsu; Yang, Shize; Liu, Yang; Woellner, Cristiano F.; Li, Zhengyuan; Vajtai, Róbert; Yang, Wei; Wu, Jingjie; Kenis, Paul J. A.; Ajayan, Pulickel M.

doi:10.1039/c8ta01367e

Cited by 98 publications

(63 citation statements)

References 57 publications

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“…363 The tendency of smaller SnO 2 nanoparticles being more active has also been observed by the interconnected SnO 2 NPs (<5 nm) that significantly suppressed hydrogen evolution and promoted formate production. 364 Various morphologies of Sn oxides have also shown to be promising for CO 2 electroreduction. SnO 2 nanosheets grown on carbon cloth (Figure 21c) exhibited formate FE of 87% at moderate overpotentials (880 mV) with a high current density of 50 mA cm −2 , which was enabled by the high density of sheets grown on individual carbon fibers providing a large surface area.…”

Section: Chemical Reviewsmentioning

confidence: 99%

“…369,370 The origin of catalytic enhancement observed in SnO 2 -based nanomaterials remains unclear. While there are some proposed hypotheses, such as the high density of grain boundaries present on these nanomaterials, 364,366 a more suitable explanation that could apply broadly to the SnO 2 -based catalysts would be the presence of oxidized Sn under reductive bias conditions to perform as the active site, 272,371 as stated earlier. In this regard, tin sulfide catalysts have shown to exhibit high catalytic activity toward formate.…”

Section: Chemical Reviewsmentioning

confidence: 99%

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Surface and Interface Control in Nanoparticle Catalysis

et al. 2019

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The surface and interfaces of heterogeneous catalysts are essential to their performance as they are often considered to be active sites for catalytic reactions. With the development of nanoscience, the ability to tune surface and interface of nanostructures has provided a versatile tool for the development and optimization of a heterogeneous catalyst. In this Review, we present the surface and interface control of nanoparticle catalysts in the context of oxygen reduction reaction (ORR), electrochemical CO2 reduction reaction (CO2 RR), and tandem catalysis in three sections. In the first section, we start with the activity of ORR on the nanoscale surface and then focus on the approaches to optimize the performance of Pt-based catalyst including using alloying, core–shell structure, and high surface area open structures. In the section of CO2 RR, where the surface composition of the catalysts plays a dominant role, we cover its reaction fundamentals and the performance of different nanosized metal catalysts. For tandem catalysis, where adjacent catalytic interfaces in a single nanostructure catalyze sequential reactions, we describe its concept and principle, catalyst synthesis methodology, and application in different reactions.

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Section: Chemical Reviewsmentioning

confidence: 99%

Section: Chemical Reviewsmentioning

confidence: 99%

Surface and Interface Control in Nanoparticle Catalysis

et al. 2019

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“…1,2 CO 2 reduction to compressible and/or liquid fuels is particularly attractive, yet solar or electrochemical generation of carbon-containing fuels has been hindered by poor efficiency and selectivity of the catalysts reported to date, prompting the need to search for new catalysts. [3][4][5][6][7] Here we present a material characterization instrument designed to quantitatively evaluate the efficiency and selectivity of novel catalysts for the direct conversion of carbon dioxide into transportation fuels under conditions commensurate with commercially viable solar fuel generators.…”

Section: Introductionmentioning

confidence: 99%

Reactor design and integration with product detection to accelerate screening of electrocatalysts for carbon dioxide reduction

Jones

Wang

Lai

et al. 2018

Review of Scientific Instruments

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Identifying new catalyst materials for complex reactions such as the electrochemical reduction of CO 2 poses substantial instrumentation challenges due to the need to integrate reactor control with electrochemical and analytical instrumentation. Performing accelerated screening to enable exploration of a broad span of catalyst materials poses additional challenges due to the long time scales associated with accumulation of reaction products and the detection of the reaction products with traditional separation-based analytical methods. The catalyst screening techniques that have been reported for combinatorial studies of (photo)electrocatalysts do not meet the needs of CO 2 reduction catalyst research, prompting our development of a new electrochemical cell design and its integration to gas and liquid chromatography instruments. To enable rapid chromatography measurements while maintaining sensitivity to minor products, the electrochemical cell features low electrolyte and head space volumes compared to the catalyst surface area. Additionally, the cell is operated as a batch reactor with electrolyte recirculation to rapidly concentrate reaction products, which serves the present needs for rapidly detecting minor products and has additional implications for enabling product separations in industrial CO 2 electrolysis systems. To maintain near-saturation of CO 2 in aqueous electrolytes, we employ electrolyte nebulization through a CO 2 -rich headspace, achieving similar gas-liquid equilibration as vigorous CO 2 bubbling but without gas flow. The instrument is demonstrated with a series of electrochemical experiments on an Au-Pd combinatorial library, revealing non-monotonic variations in product distribution with respect to catalyst composition. The highly integrated analytical electrochemistry system is engineered to enable automation for rapid catalyst screening as well as deployment for a broad range of electrochemical reactions where product distribution is critical to the assessment of catalyst performance. Published by AIP Publishing. https://doi.

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“…Typically, Wang and co‐workers adopt lithium electrochemical tuning method to gradually reduce ZnO nanoparticle into Zn nanoparticle with interconnected GBs, finding much more enriched GBs could be created than that of traditional in situ reduction during electrolysis (Figure c). This enhanced GB density also led to dramatic improvement for electroreduction of CO 2 to CO. Other works with “GB‐enriched strategy” have been reported by Kenis and co‐workers and Spurgeon and co‐workers as well.…”

Section: Recent Advances Of Electrocatalysts For Improved Performancementioning

confidence: 83%

Electrochemical Reduction of CO₂ over Heterogeneous Catalysts in Aqueous Solution: Recent Progress and Perspectives

Long

Guo³

et al. 2018

Small Methods

176

119

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Electrochemical reduction of CO2 into value‐added chemicals or fuels, driven by renewable energy, presents a promising solution to depletion of fossil fuels and greenhouse effects caused by excessive carbon emissions. In the past few years, great efforts have been dedicated to promote research in this field. Herein, this review focuses on the recent advances of the underlying mechanistic studies and novel heterogeneous catalyst constructions for electrochemical reduction of CO2 in aqueous media, targeting at presenting a full landscape at the current stage. The outlook for the future development is also included at the end of this review.

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High efficiency electrochemical reduction of CO₂ beyond the two-electron transfer pathway on grain boundary rich ultra-small SnO₂ nanoparticles

Abstract: Grain boundary rich ultra-small SnO2 nanoparticles exhibited high total FEs towards electrochemical reduction of CO2 with products beyond CO and HCOO−.

Cited by 98 publications

References 57 publications

Surface and Interface Control in Nanoparticle Catalysis

Surface and Interface Control in Nanoparticle Catalysis

Reactor design and integration with product detection to accelerate screening of electrocatalysts for carbon dioxide reduction

Electrochemical Reduction of CO₂ over Heterogeneous Catalysts in Aqueous Solution: Recent Progress and Perspectives

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High efficiency electrochemical reduction of CO2 beyond the two-electron transfer pathway on grain boundary rich ultra-small SnO2 nanoparticles

Abstract: Grain boundary rich ultra-small SnO2 nanoparticles exhibited high total FEs towards electrochemical reduction of CO2 with products beyond CO and HCOO−.

Cited by 98 publications

References 57 publications

Surface and Interface Control in Nanoparticle Catalysis

Surface and Interface Control in Nanoparticle Catalysis

Reactor design and integration with product detection to accelerate screening of electrocatalysts for carbon dioxide reduction

Electrochemical Reduction of CO2 over Heterogeneous Catalysts in Aqueous Solution: Recent Progress and Perspectives

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High efficiency electrochemical reduction of CO₂ beyond the two-electron transfer pathway on grain boundary rich ultra-small SnO₂ nanoparticles

Electrochemical Reduction of CO₂ over Heterogeneous Catalysts in Aqueous Solution: Recent Progress and Perspectives