ACS Materials Letters, Journal Year: 2024, Volume and Issue: 6(10), P. 4801 - 4809
Published: Sept. 24, 2024
Language: Английский
ACS Materials Letters, Journal Year: 2024, Volume and Issue: 6(10), P. 4801 - 4809
Published: Sept. 24, 2024
Language: Английский
Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(45)
Published: May 28, 2024
Abstract The past decades have seen considerable imbalances in the nitrogen cycle due to excessive use of nitrate agriculture and industry. Electrocatalytic reduction (NO 3 RR) (N 2 ) holds significant potential for addressing pollution wastewater but suffers from nitrite formation sluggish hydrogeneration process. Here a single atom alloy (SAA) catalyst featuring atomically dispersed Ru on 2D Ni metal (Ru 1 Ni), proving remarkable performance − –N conversion (≈93%) N selectivity (≈99%)) through co‐catalytic metal‐support interactions (CMSI) effect is reported. Significantly, SAA achieves NO RR removal capacity as high 11.1 mg L −1 h cm −2 with 20 cycles stability (9 per cycle), surpassing most previously reported works. core boosting lies synergistically promoted activation accelerated hydrogenation oxide intermediates site substrate, respectively, revealed by various situ experiments theoretical simulations. DFT calculations indicate electron transfer substrate more robust interaction between Ru–Ni comparison that Ni–Ni. This work offers resilient methodology rational design highly efficient electrocatalysts CMSI modulation RR, illuminating arena treatment cycle.
Language: Английский
Citations
18Advanced Materials, Journal Year: 2024, Volume and Issue: unknown
Published: Oct. 22, 2024
Abstract Reconstruction of catalysts is now well recognized as a common phenomenon in electrocatalysis. As the reconstructed structure may promote or hamper electrochemical performance, how to achieve designed active surface for highly enhanced catalytic activity through reconstruction needs be carefully investigated. In this review, genesis and effects various processes, such hydrogen evolution reaction (HER), oxygen (OER), carbon dioxide reduction (CO 2 RR), nitrate (NO 3 RR) are first described. Then, strategies optimizing reconstruction, valence states control, phase retention, engineering, poisoning prevention comprehensively discussed. Finally, general rules optimization summarized give perspectives future study. It believed that review shall provide deep insights into electrocatalytic mechanisms guide design pre‐catalysts with improved activity.
Language: Английский
Citations
17Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)
Published: Jan. 21, 2025
Renewable energy-driven electrocatalytic nitrate reduction reaction presents a low-carbon and sustainable route for ammonia synthesis under mild conditions. Yet, the practical application of this process is currently hindered by unsatisfactory activity long-term stability. Herein we achieve high-rate electrosynthesis using stable amorphous/crystalline dual-phase Cu catalyst. The partial current density formation rate reach 3.33 ± 0.005 A cm-2 15.5 0.02 mmol h-1 at low cell voltage 2.6 0.01 V, respectively. Remarkably, catalyst can maintain production with Faradaic efficiency around 90% high 1.5 up to 300 h. scale-up demonstration an electrode size 100 cm2 achieves as 11.9 0.5 g total 160 A. impressive performance ascribed presence amorphous domains which promote adsorption hydrogenation nitrogen-containing intermediates, thus improving kinetics formation. This work underscores importance stabilizing metastable structures reactivity
Language: Английский
Citations
4Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 485, P. 149876 - 149876
Published: Feb. 20, 2024
Language: Английский
Citations
15Journal of Hazardous Materials, Journal Year: 2024, Volume and Issue: 472, P. 134522 - 134522
Published: May 3, 2024
Language: Английский
Citations
9Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown
Published: Feb. 10, 2025
Abstract Electrochemically promoted nitrate reduction reaction (NITRR) holds great potential for the “green” synthesis of ammonia (NH 3 ). However, NITRR in neutral media, though close to practical scenario, is often limited by an insufficient supply active hydrogen (*H) due sluggish water cleavage. In this work, it demonstrated that a bimetallic alloy FeIr can optimize trade‐off between and *H formation media. As result, exhibits excellent catalytic performance toward with Faradaic efficiency NH up 97.3% high yield rate 11.67 mg h −1 cm −2 at low working −0.6 V (versus reversible electrode (RHE)), surpassing monometallic catalysts as well majority Fe‐based state‐of‐the‐art. It also found displays remarkable electron rearrangement hetero‐atoms their significant orbital hybridization, which benefits not only but process. Moreover, coupling FeIr‐based methanol oxidation (MOR) results sustainable productions formate combined FE nearly 200% cell‐voltage 2 V. This work thus demonstrates promising strategy designing efficient NITRR.
Language: Английский
Citations
1Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown
Published: Feb. 28, 2025
Electrochemical nitrate reduction reaction (eNO3-RR) to ammonia (NH3) holds great promise for the green treatment of NO3- and ambient NH3 synthesis. Although Fe-based electrocatalysts have emerged as promising alternatives, their excellent eNO3-RR-to-NH3 activity is usually limited harsh alkaline electrolytes or alloying noble metals with Fe in sustainable neutral electrolytes. Herein, we demonstrate an unusual self-triggering localized alkalinity Co4Fe6 electrocatalyst efficient media, which breaks down conventional pH-dependent kinetics restrictions shows a 98.6% Faradaic efficiency (FE) 99.9% selectivity at -0.69 V vs RHE. The synergetic Co-Fe dual sites were demonstrated enable optimal free energies species balance water dissociation protonation adsorbed NO2-. Notably, can attain high current density 100 mA cm-2 FE surpassing 96% long-term stability over 500 h membrane electrode assembly (MEA) electrolyzer. This work provides insight into tailoring self-reinforced local-alkalinity on alloy thus avoids practical upcycling technology.
Language: Английский
Citations
1International Journal of Hydrogen Energy, Journal Year: 2024, Volume and Issue: 80, P. 586 - 598
Published: July 17, 2024
Language: Английский
Citations
8Chem Catalysis, Journal Year: 2024, Volume and Issue: 4(9), P. 101060 - 101060
Published: July 23, 2024
Language: Английский
Citations
8Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown
Published: Oct. 2, 2024
Electrochemical reduction of nitrate to ammonia (NRA) offers a sustainable approach for NH
Language: Английский
Citations
5