Nitrate and nitrite (NO) are widespread contaminants in industrial wastewater and groundwater. Sustainable ammonia (NH) production via NO electroreduction provides a prospective alternative to the energy-intensive industrialized Haber-Bosch process. However, selectively regulating the reaction pathway, which involves complicated electron/proton transfer, toward NH generation relies on the robust catalyst. A specific consideration in designing selective NO-to-NH catalysts should meet the criteria to suppress competing hydrogen evolution and avoid the presence of neighboring active sites that are in favor of adverse N-N coupling. Nevertheless, efforts in this regard are still inadequate. Herein, we demonstrate that isolated ruthenium sites can selectively reduce NO into NH, with maximal Faradaic efficiencies of 97.8% (NO reduction) and 72.8% (NO reduction) at -0.6 and -0.4 V, respectively. Density functional theory calculations simulated the reaction mechanisms and identified the *NO → *NOH as the potential rate-limiting step for NO-to-NH conversion on single-atom Ru sites.
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http://dx.doi.org/10.1021/acsnano.2c09691 | DOI Listing |
ChemSusChem
January 2025
University of Electronic Science and Technology of China, School of Material and Energy, Qingshuihe Campus:No.2006, Xiyuan Ave, West Hi-Tech Zone, 611731, Chengdu, CHINA.
Modulating the oxidation state of copper (Cu) is crucial for enhancing the electrocatalytic CO2 reduction reaction (CO2RR), particularly for facilitating deep reductions to produce methane (CH4) or multi-carbon (C2+) products. However, Cuδ+ sites are thermodynamically unstable, fluctuating their oxidation states under reaction conditions, which complicates their functionality. Incorporating interfacial metal oxides has emerged as an effective strategy for stabilizing these oxidation states.
View Article and Find Full Text PDFAdv Mater
January 2025
State Key Laboratory of Petroleum Molecular & Process Engineering, Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200062, China.
Copper-based electrocatalysts are recognized as crucial catalysts for CO electroreduction into multi-carbon products. However, achieving copper-based electrocatalysts with adjustable valences via one-step facile synthesis remains a challenge. In this study, Cu/CuO heterostructure is constructed by adjusting the anion species of the Cu ions-containing electrolyte during electrodeposition synthesis.
View Article and Find Full Text PDFPolymers (Basel)
December 2024
Department of Fiber System Engineering, Yeungnam University, Gyeongbuk 38541, Republic of Korea.
The development of innovative, cost effective, and biocompatible sensor materials for rapid and efficient practical applications is a key area of focus in electroanalytical chemistry. In this research, we report on a novel biocompatible sensor, made using a unique polybenzoxazine-based carbon combined with amino cellulose and hyaluronic acid to produce a bio-polymer complex (PBC-ACH) (polybenzoxazine-based carbon with amino cellulose and hyaluronic acid). This sensor material is fabricated for the first time to enable the electroreduction of the herbicide, metribuzin (MTZ).
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Hunan University, College of Materials Science and Engineering, South Lushan Road 2#, 410082, China, 410082, Changsha, CHINA.
Renewable electricity-driven electrochemical reduction of CO2 offers a promising route for production of high-value ethanol. However, the current state of this technology is hindered by low selectivity and productivity, primarily due to limited understanding of the atomic-level active sites involved in ethanol formation. Herein, we identify that the interfacial oxygen vacancy-neighboring Cu (Ov-Cu) pair sites are the active sites for CO2 electroreduction to ethanol.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
School of Chemistry and Chemical Engineering, Chongqing Key Laboratory of Chemical Theory and Mechanism, Chongqing University, Chongqing 401331, China.
Atomically precise metal nanoclusters (NCs) have emerged as an intriguing class of model catalysts for electrochemical CO reduction reactions (CORR). However, the interplay between the interface environment (e.g.
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