The electrochemical reduction reaction of nitrate (NORR) to ammonia is an environmentally friendly approach that can treat wastewater as well as find an alternative to the energy-intensive Haber-Bosch process. The use of adhesives partially to adhere to the NORR electrocatalysts, leading to sluggish kinetics, poor stability and poor scalability. Herein, we report the synthesis of PdCu alloy catalysts via a direct laser writing method, demonstrating their exceptional performance in the electrochemical reduction of nitrate. The PdCu alloy exhibited a remarkable ammonia production rate of 30.55 mg h cm under neutral electrolyte conditions and maintained stable operation for over 1500 h. Density functional theory (DFT) calculations and experimental analyses revealed that the PdCu alloy's enhanced activity stems from its lower energy barrier for the rate-determining step (*NO → *NOH) and improved mass transfer capabilities. The alloy's electronic properties and geometric configuration, fine-tuned by the laser-induced synthesis method, facilitate the conversion of NO and suppress the hydrogen evolution reaction (HER), thereby significantly enhancing the selectivity and activity of the NORR process. This study provides a sustainable and efficient pathway for ammonia synthesis and offers insights into the design of advanced catalysts for environmental and energy applications.
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http://dx.doi.org/10.1016/j.jcis.2025.02.210 | DOI Listing |
J Colloid Interface Sci
February 2025
College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, Jiangsu 215123, China; Advanced Water Technology Laboratory, National University of Singapore (Suzhou) Research Institute, Suzhou, Jiangsu 215123, China. Electronic address:
The electrochemical reduction reaction of nitrate (NORR) to ammonia is an environmentally friendly approach that can treat wastewater as well as find an alternative to the energy-intensive Haber-Bosch process. The use of adhesives partially to adhere to the NORR electrocatalysts, leading to sluggish kinetics, poor stability and poor scalability. Herein, we report the synthesis of PdCu alloy catalysts via a direct laser writing method, demonstrating their exceptional performance in the electrochemical reduction of nitrate.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
March 2025
State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China.
Tailoring local environments of active sites to match targeted configuration of key species is significant for controlling reaction pathways in selective hydrogenations. Herein, differently typed Pd sites are introduced onto Cu catalysts to tune the local environment of Cu sites for controlling the configuration of semi-hydrogenation pathway of propyne hydrogenation used in production of polymer-grade propylene. Detailed structure characterizations demonstrate the controllable construction of Pd single-atom and Pd ensemble sites modified Cu surfaces and PdCu alloy via fine tuning the Pd/Cu ratios.
View Article and Find Full Text PDFNat Commun
February 2025
State Key Joint Laboratory of Environment Simulation and Pollution Control, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing, China.
Enhancing selectivity towards specific products remains a pivotal challenge in energy catalysis. Herein, we present a strategy to refine selectivity via pathway optimization, exemplified by the rational design of catalysts for methanol steam reforming. Over traditional Pd/ZnO catalysts, the direct decomposition of key intermediates CHO* into CO and H on PdZn alloys competes with the oxidation of CHO* to CO, leading to inferior selectivity in product distribution.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2025
Department of Chemistry, Capital Normal University, Beijing, 100048, P. R. China.
Whether the catalyst can realize the non-CO pathway is the key to greatly improve the catalytic activity and stability of methanol oxidation reaction (MOR). It is feasible to optimize the reaction path selectivity by modifying organic ligands and constructing single-atom systems. At the same time, heterogeneous metal nanosheets with atomic thickness have been shown to significantly enhance the catalytic activity of materials due to their ultra-high exposure of active sites and synergistic effects.
View Article and Find Full Text PDFInt J Mol Sci
November 2024
Research Institute of Hydrogen Energy, Kuban State University, Krasnodar 350040, Russia.
Thin-film membranes of Pd-Ag and Pd-Cu alloys capable of releasing hydrogen in a wide temperature range have been developed. The surface activation of the membranes with a nanostructured coating made it possible to intensify hydrogen transport through Pd-containing membranes at low temperatures. This effect was achieved by accelerating limiting surface processes by increasing the active area of the membrane.
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