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A high-performance oxygen evolution catalyst in neutral-pH for sunlight-driven CO₂ reduction.

ABSTRACT: The efficiency of sunlight-driven reduction of carbon dioxide (CO₂), a process mimicking the photosynthesis in nature that integrates the light harvester and electrolysis cell to convert CO₂ into valuable chemicals, is greatly limited by the sluggish kinetics of oxygen evolution in pH-neutral conditions. Current non-noble metal oxide catalysts developed to drive oxygen evolution in alkaline solution have poor performance in neutral solutions. Here we report a highly active and stable oxygen evolution catalyst in neutral pH, Brownmillerite Sr₂GaCoO₅, with the specific activity about one order of magnitude higher than that of widely used iridium oxide catalyst. Using Sr₂GaCoO₅ to catalyze oxygen evolution, the integrated CO₂ reduction achieves the average solar-to-CO efficiency of 13.9% with no appreciable performance degradation in 19 h of operation. Our results not only set a record for the efficiency in sunlight-driven CO₂ reduction, but open new opportunities towards the realization of practical CO₂ reduction systems.

SUBMITTER: Zhou LQ

PROVIDER: S-EPMC6733866 | biostudies-literature | 2019 Sep

REPOSITORIES: biostudies-literature

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A high-performance oxygen evolution catalyst in neutral-pH for sunlight-driven CO2 reduction.

Zhou Li Qin LQ Ling Chen C Zhou Hui H Wang Xiang X Liao Joseph J Reddy Gunugunuri K GK Deng Liangzi L Peck Torin C TC Zhang Ruigang R Whittingham M Stanley MS Wang Chongmin C Chu Ching-Wu CW Yao Yan Y Jia Hongfei H

Nature communications 20190909 1

The efficiency of sunlight-driven reduction of carbon dioxide (CO2), a process mimicking the photosynthesis in nature that integrates the light harvester and electrolysis cell to convert CO2 into valuable chemicals, is greatly limited by the sluggish kinetics of oxygen evolution in pH-neutral conditions. Current non-noble metal oxide catalysts developed to drive oxygen evolution in alkaline solution have poor performance in neutral solutions. Here we report a highly active ...[more]

PMID: 31501446

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Project description:Polymer electrolyte membrane fuel cells (PEMFCs) have reached the commercialization phase, representing a promising approach to curbing carbon emissions. However, greater durability of PEMFCs is of paramount importance to ensure their long-term viability and effectiveness, and catalyst development has become a focal point of research. Pt nanoparticles supported on carbon materials (Pt/C) are the primary catalysts used in PEMFCs. Accomplishing both a high dispersion of uniform metal particles on the carbon support and robust adhesion between the metal particles and the carbon support is imperative for superior stability, and will thereby, advance the practical applications of PEMFCs in sustainable energy solutions. Ultrasound-assisted polyol synthesis (UPS) has emerged as a suitable method for synthesizing catalysts with a well-defined metal-support structure, characterized by the high dispersion and uniformity of metal nanoparticles. In this study, we focused on the effect of ultrasound on the synthesis of Pt/C via UPS and the resulting enhanced stability of Pt/C catalysts. Therefore, we compared Pt/C synthesized using a conventional polyol synthesis (Pt/C_P) and Pt/C synthesized via UPS (Pt/C_U) under similar synthesis conditions. The two catalysts had a similar Pt content and the average particle size of the Pt nanoparticles was similar; however, the uniformity and dispersion of Pt nanoparticles in Pt/C_U were better than those of Pt/C_P. Moreover, ex/in-situ analyses performed in a high-temperature environment, in which nanoparticles tend to agglomerate, have revealed that Pt/C_U exhibited a notable improvement in the adhesion of Pt particles to the carbon support compared with that of Pt/C_P. The enhanced adhesion is crucial for maintaining the stability of the catalyst, ultimately contributing to a better durability in practical applications. Ultrasound was applied to the carbon support without the Pt precursor under the same UPS conditions used to synthesize Pt/C_U to identify the reason for the increased adhesion between the Pt particles and the carbon support in Pt/C_U, and we discovered that oxygen functional groups (C-O, C = O, and O-C = O) for anchoring site of Pt particles were generated in the carbon support. Pt/C_U displayed an increase in stability in an electrochemical accelerated stress test (AST) in an acidic electrolyte. The physical and chemical effects of ultrasound on the synthesis of Pt/C via UPS were identified, and we concluded that UPS is suitable for synthesizing carbon supported electrocatalysts with high stability.

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A high-performance oxygen evolution catalyst in neutral-pH for sunlight-driven CO₂ reduction.

Publications

A high-performance oxygen evolution catalyst in neutral-pH for sunlight-driven CO<sub>2</sub> reduction.

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