Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 676, P. 323 - 330
Published: July 17, 2024
Language: Английский
Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: 147(9), P. 8012 - 8023
Published: Feb. 18, 2025
The electrocatalytic nitrite reduction (NO2RR) converts nitrogen-containing pollutants to high-value ammonia (NH3) under ambient conditions. However, its multiple intermediates and multielectron coupled proton transfer process lead low activity NH3 selectivity for the existing electrocatalysts. Herein, we synthesize a solid-solution copper-zinc cyanamide (Cu0.8Zn0.2NCN) with localized structure distortion tailored surface electrostatic potential, allowing asymmetric binding of NO2-. It exhibits outstanding NO2RR performance Faradaic efficiency ∼100% an yield 22 mg h-1 cm-2, among best such process. Theoretical calculations in situ spectroscopic measurements demonstrate that Cu-Zn sites coordinated linear polarized [NCN]2- could transform symmetric [Cu-O-N-O-Cu] CuNCN-NO2- [Cu-N-O-Zn] configuration Cu0.8Zn0.2NCN-NO2-, thus enhancing adsorption bond cleavage. A paired electro-refinery Cu0.8Zn0.2NCN cathode reaches 2000 mA cm-2 at 2.36 V remains fully operational industrial-level 400 >140 h production rate ∼30 mgNH3 cm-2. Our work opens new avenue tailoring potentials using strategy advanced electrocatalysis.
Language: Английский
Citations
1
Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)
Published: March 4, 2025
Atomically dispersed Ru-Cu dual-atom catalysts (DACs) with asymmetric coordination are critical for sustainable ammonia production via electrochemical nitrate reduction (NO3RR), but their rational synthesis remains challenging. Here, we report a pulsed discharge strategy that injects microsecond pulse current into ruthenium (Ru) and copper (Cu) precursors supported by nitrogen-doped graphene aerogels (NGA). The atomically Ru Cu dual atoms anchor onto nanopore defects of NGA (RuCu DAs/NGA) through explosive decomposition the metal salt nanocrystals. catalyst achieves 95.7% Faraday efficiency 3.1 mg h-1 cm-2 NH3 yield at -0.4 V vs. RHE. In situ studies reveal an RuN2-CuN3 active-site dynamic evolution during NO3RR. Density functional theory calculations demonstrate RuN2CuN3/C structure synergistically optimizes intermediate adsorption reduces energy barriers key steps. enables ultrafast various DACs (e.g., PtCu, AgCu, PdCu, FeCu, CoCu, NiCu) tailored environments, offering general-purpose precise preparation catalysts, which traditionally challenging to synthesize.
Language: Английский
Citations
1
ACS Energy Letters, Journal Year: 2024, Volume and Issue: 9(9), P. 4414 - 4440
Published: Aug. 17, 2024
Electrochemical reactions, including water splitting, oxygen reduction, hydrogen oxidation, carbon dioxide nitrogen oxide etc., are critical for sustainable energy conversion and storage. Achieving high efficiency in these reactions requires catalysts with superior activity, selectivity, stability, often realized through nanostructured metal catalysts. However, practical challenges such as low selectivity catalytic degradation persist. In situ operando characterization techniques offer real-time insights into catalyst behavior under reaction conditions, enabling a deeper understanding of structure–performance relationships and, therefore, guiding the design optimization electro-catalysts. This review discusses common situ/operando techniques, highlights their applications model catalysts, single-atom single-crystal further explores combinational analysis to study complex nanocatalysts. Finally, we provide suggestions perspectives on development advance field electrochemical catalysis.
Language: Английский
Citations
8
Joule, Journal Year: 2024, Volume and Issue: 8(7), P. 1890 - 1918
Published: July 1, 2024
Language: Английский
Citations
7
Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 676, P. 323 - 330
Published: July 17, 2024
Language: Английский
Citations
7