Ammonia has attracted considerable interest as a hydrogen carrier that can help decarbonize global energy networks. Key to realizing this is the development of low temperature ammonia fuel cells for the on-demand generation of electricity. However, the efficiency of such systems is significantly impaired by the sluggish ammonia oxidation reaction (AOR) and oxygen reduction reaction (ORR). Here, we report the design of a bifunctional AgPtTiS electrocatalyst that facilitates both reactions at mass activities exceeding that of commercial Pt/C. Through comprehensive density functional theory calculations, we identify that active site motifs composed of Pt and Ti atoms work cooperatively to catalyze ORR and AOR. Notably, in situ shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) experiments indicate a decreased propensity for *NO formation and hence an increased resistance toward catalyst poisoning for AOR. Employing AgPtTiS as both the cathode and anode, we constructed a low temperature ammonia fuel cell with a high peak power density of 8.71 mW cm and low Pt loading of 0.45 mg cm. Our findings demonstrate a pathway towards the rational design of effective electrocatalysts with multi-element active sites that work cooperatively.
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http://dx.doi.org/10.1002/anie.202418691 | DOI Listing |
Sci Total Environ
January 2025
Yunnan Key Laboratory of Internal Combustion Engine, Kunming University of Science and Technology, Kunming 650500, China.
Ammonia is a highly promising carbon-neutral fuel. The use of ammonia as a fuel for internal combustion engines can reduce fossil energy consumption and greenhouse gas emissions. However, the high ignition energy required for ammonia and the slow flame propagation rate result in low combustion efficiency when ammonia is used directly in internal combustion engines.
View Article and Find Full Text PDFACS Nano
January 2025
College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215006, China.
Low-temperature direct ammonia fuel cell (DAFC) stands out as a more secure technology than the hydrogen fuel cell system, while there is still a lack of elegant bottom-up synthesis procedures for efficient ammonia oxidation reaction (AOR) electrocatalysts. The widely accepted d-band center, even with consideration of the d-band width, usually fails to describe variations in AOR reactivity in many practical conditions, and a more accurate activity descriptor is necessary for a less empirical synthesis path. Herein, the upper d-band edge, ε, derived from the d-band model, is identified as an effective descriptor for accurately establishing the descriptor-activity relationship.
View Article and Find Full Text PDFJ Phys Chem A
January 2025
Department of Mechanical Engineering, The Hong Kong Polytechnic University, Kowloon, Hong Kong SAR 999077, China.
An adequate understanding of the NO interacting chemistry is a prerequisite for a smoother transition to carbon-lean and carbon-free fuels such as ammonia and hydrogen. In this regard, this study presents a comprehensive study on the H atom abstraction by NO from C to C alkynes, dienes, and trienes forming 3 HNO isomers (i.e.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2024
Institute of Chemistry, Federal University of Mato Grosso do Sul, Avenida Senador Filinto Muller 1555, Campo Grande, Mato Grosso do Sul 79074-460, Brazil.
There has been huge interest among chemical scientists in the electrochemical reduction of nitrate (NO) to ammonia (NH) due to the useful application of NH in nitrogen fertilizers and fuel. To conduct such a complex reduction reaction, which involves eight electrons and eight protons, one needs to develop high-performance (and stable) electrocatalysts that favor the formation of reaction intermediates that are selective toward ammonia production. In the present study, we developed and applied CoO/graphene nanoribbon (GNR) electrocatalysts with excellent properties for the effective reduction of NO to NH, where NH yield rate of 42.
View Article and Find Full Text PDFNanomaterials (Basel)
December 2024
The Key Laboratory of Fuel Cell Technology of Guangdong Province, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510641, China.
Developing highly active and durable non-noble metal catalysts is crucial for energy conversion and storage, especially for proton exchange membrane fuel cells (PEMFCs) and lithium-oxygen (Li-O) batteries. Non-noble metal catalysts are considered the greatest potential candidates to replace noble metal catalysts in PEMFCs and Li-O batteries. Herein, we propose a novel type of non-noble metal catalyst (Fe-Hf/N/C) doped with Hf into a mesoporous carbon material derived from Hf-ZIF-8 and co-doping with Fe and N, which greatly enhanced the activity and durability of the catalyst.
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