4.8 Article

Exploring dopant effects in stannic oxide nanoparticles for CO2 electro-reduction to formate

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NATURE COMMUNICATIONS
卷 13, 期 1, 页码 -

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NATURE PORTFOLIO
DOI: 10.1038/s41467-022-29783-7

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资金

  1. Korea Institute of Science and Technology
  2. Carbon to X Project through the National Research Foundation (NRF) - Ministry of Science and ICT, Republic of Korea [2020M3H7A1098229]
  3. National Research Council of Science & Technology (NST) - Korean government (MSIT) [NRF-2021R1A2C2093467]
  4. National Supercomputing Center [KSC-2021-CRE-0284]
  5. National Research Foundation of Korea [2020M3H7A1098229] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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The authors investigated the performance of fluorine-doped tin oxide catalyst for electrochemical synthesis of formate from carbon dioxide and achieved stable and efficient results. This finding provides a simple and effective approach for designing active and durable electrocatalysts.
Though stannic oxides can catalyze CO2 electroreduction to formate, the stability of these catalysts has been limited. Here, the authors demonstrate stable fluorine-doped SnO2 materials toward formate production at current densities of >300 mA/cm(2). The electrosynthesis of formate from CO2 can mitigate environmental issues while providing an economically valuable product. Although stannic oxide is a good catalytic material for formate production, a metallic phase is formed under high reduction overpotentials, reducing its activity. Here, using a fluorine-doped tin oxide catalyst, a high Faradaic efficiency for formate (95% at 100 mA cm(-2)) and a maximum partial current density of 330 mA cm(-2) (at 400 mA cm(-2)) is achieved for the electroreduction of CO2. Furthermore, the formate selectivity (approximate to 90%) is nearly constant over 7 days of operation at a current density of 100 mA cm(-2). In-situ/operando spectroscopies reveal that the fluorine dopant plays a critical role in maintaining the high oxidation state of Sn, leading to enhanced durability at high current densities. First-principle calculation also suggests that the fluorine-doped tin oxide surface could provide a thermodynamically stable environment to form HCOO* intermediate than tin oxide surface. These findings suggest a simple and efficient approach for designing active and durable electrocatalysts for the electrosynthesis of formate from CO2.

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