Electrocatalytic acetylene semi-hydrogenation to ethylene powered by renewable electricity represents a sustainable pathway, but the inadequate current density and single-pass yield greatly impedes the production efficiency and industrial application. Herein, we develop a F-modified Cu catalyst that shows an industrial partial current density up to 0.76 A cm with an ethylene Faradic efficiency surpass 90%, and the maximum single-pass yield reaches a notable 78.5%. Furthermore, the Cu-F showcase the capability to directly convert acetylene into polymer-grade ethylene in a tandem flow cell, almost no acetylene residual in the production. Combined characterizations and calculations reveal that the Cu (near fluorine) enhances the water dissociation, and the generated active hydrogen are immediately transferred to Cu (away from fluorine) and react with the locally adsorbed acetylene. Therefore, the hydrogen evolution reaction is surpassed and the overall acetylene semi-hydrogenation performance is boosted. Our findings provide new opportunity towards rational design of catalysts for large-scale electrosynthesis of ethylene and other important industrial raw.
Download full-text PDF |
Source |
---|---|
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC10725425 | PMC |
http://dx.doi.org/10.1038/s41467-023-44171-5 | DOI Listing |
Adv Mater
October 2024
Department of Chemical Sciences, University of Padova, Via F. Marzolo 1, Padova, 35131, Italy.
The semi-hydrogenation of acetylene in ethylene-rich gas streams is a high-priority industrial chemical reaction for producing polymer-grade ethylene. Traditional thermocatalytic routes for acetylene reduction to ethylene, despite progress, still require high temperatures and high H consumption, possess relatively low selectivity, and use a noble metal catalyst. Light-powered strategies are starting to emerge, given that they have the potential to use directly the abundant and sustainable solar irradiation, but are ineffective.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2024
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, 155 Yangqiao Road West, Fuzhou, Fujian, 350002, People's Republic of China.
Angew Chem Int Ed Engl
October 2024
State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China.
Catalytic removal of alkynes is essential in industry for producing polymer-grade alkenes from steam cracking processes. Non-noble Ni-based catalysts hold promise as effective alternatives to industrial Pd-based catalysts but suffer from low activity. Here we report embedding of single-atom Pd onto the NiGa intermetallic surface with replacing Ga atoms via a well-defined synthesis strategy to design Pd-NiGa catalyst for alkyne semi-hydrogenation.
View Article and Find Full Text PDFInorg Chem
June 2024
School of Chemistry and Chemical Engineering, Chongqing University, Chongqing 400044, PR China.
Removing trace acetylene from the ethylene stream through selective hydrogenation is a crucial process in the production of polymer-grade ethylene. However, achieving high selectivity while maintaining high activity remains a significant challenge, especially for nonprecious metal catalysts. Herein, the trade-off between activity and selectivity is solved by synergizing enhanced dispersion and hydrogen spillover.
View Article and Find Full Text PDFChem Sci
March 2024
Institute for Catalysis, Hokkaido University Sapporo 001-0021 Japan
The development of an efficient catalytic system for low-temperature acetylene semihydrogenation using nonnoble metals is important for the cost-effective production of polymer-grade pure ethylene. However, it remains challenging owing to the intrinsic low activity. Herein, we report a flexibly tunable catalyst design concept based on a pseudo-binary alloy, which enabled a remarkable enhancement in the catalytic activity, selectivity, and durability of a Ni-based material.
View Article and Find Full Text PDFEnter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!