Journal
CARBON
Volume 195, Issue -, Pages 199-206Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.carbon.2022.04.026
Keywords
N-2 electroreduction; Local environment; Ruthenium; SnO2; Carbon cloth
Funding
- National Natural Science Foundation of China [52071171]
- Liaoning Revitalization Talents Program-Pan Deng Scholars [XLYC1802005]
- Liaoning BaiQianWan Talents Program [LNBQW2018B0048]
- Natural Science Fund of Liaoning Province for Excellent Young Scholars [2019-YQ-04]
- Key Project of Scientific Research of the Education Department of Liaoning Province [LZD201902]
- Shenyang Science and Technology Project [21-108-9-04]
- Young Scientific and Technological Talents Project of the Department of Education of Liaoning Province [LQN202008]
- Foundation for Young Scholars of Liaoning University [LDQN2019007]
- Australian Research Council (ARC) through Future Fellowship [FT210100298, FT210100806]
- Discovery Project [DP220100603]
- Linkage Project [LP210100467, LP210200504, LP210200345]
- Industrial Transformation Training Centre [IC180100005]
- CSIRO Energy Centre
- Kick-Start Project
- Victorian Government through Study Melbourne
- Australian Research Council [LP210200504, LP210200345, LP210100467] Funding Source: Australian Research Council
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Electrocatalytic N-2 reduction reaction (NRR) holds promise as a sustainable and alternative technique for NH3 production. This study successfully synthesized ruthenium-doped defect-rich SnO2 nanoparticles as an efficient electrocatalyst for NRR under ambient conditions.
Electrocatalytic N-2 reduction reaction (NRR) is of great potential as a sustainable and alternative technique to the energy-intensive Haber-Bosch process for NH3 production. However, its practical applications are impeded by the low NH3 yield and Faradaic efficiency (FE) mainly due to the inert N equivalent to N triple bond and the competing hydrogen evolution reaction (HER). Herein, ruthenium-doped defect-rich SnO2 nanoparticles on carbon cloth (Ru-SnO2/CC) are synthesized for efficient electrocatalytic NRR under ambient conditions. The catalysts exhibit an NH(3 )yield of 4.83 mg h(-1) cm(-2) with a FE of 17.01% at -0.2 V vs. reversible hydrogen electrode in 0.1 M Na2SO4. The integration of Ru species, SnO2 and oxygen vacancies leads a synergistic catalytic system, in which the semiconducting SnO2 particles not only stabilize the Ru active centers but also suppress the HER, while the oxygen vacancies in SnO2 lattice help to promote the N-2 adsorption and enhance the activity of the Ru active centers. Overall, this synergy result in a unique local environment around the Ru active sites that favors the NRR process, which is further reinforced by the binder-free and facile electron transfer nature of CC, leading to the outstanding NRR catalytic activity and durability. These results outperform majority of the noble-metals-based electrocatalysts under similar conditions. This metal-doping tuned local environment manipulation may open up a promising avenue to the design and fabrication of efficient catalysts for N-2 electroreduction. (C) 2022 Elsevier Ltd. All rights reserved.
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