Promoting Electrochemical Reactions with Dual‐Atom Catalysts for High‐Rate Lithium–Sulfur Batteries
Abstract
Abstract Sulfur cathodes offer a promising solution for high‐energy‐density, cost‐effective, and sustainable energy storage. However, their practical application is limited by sluggish and complex multistep sulfur redox reactions (SRRs), involving both electrochemical and chemical processes. Herein, it is demonstrated that accelerating electrochemical processes, particularly Li 2 S nucleation, over competing chemical pathways is fundamental to minimizing sulfur loss and achieving high‐rate performance. To this end, a scalable and cost‐effective strategy is presented for synthesizing a series of 3d transition metal–bismuth (TM–Bi) atomic pairs anchored on carbon nitride (CN) and investigate their potential to activate SRRs in lithium‐sulfur batteries (LSBs). An initial screening identifies Ni–Bi/CN and Co–Bi/CN as highly effective in improving rate performance. Detailed analysis shows these catalysts promote direct electrochemical transitions and rapid Li 2 S nucleation over competing chemical reactions, enabling high charge–discharge rates while preventing active material loss and enhancing stability. Electrochemical analysis, density functional theory, and operando spectroscopy reveal that TM‐Bi pairing shifts d‐band states closer to the Fermi level and modulates HOMO–LUMO levels, promoting lithium polysulfide (LiPS) interaction and facilitating efficient charge transfer. These findings offer valuable insights for designing advanced catalysts for LSBs and broader electrocatalytic applications.
Article Details
Authors (20)
Jing Yu
Institute for Digital Molecular Analytics and Science (IDMxS), Nanyang Technological University, 59 Nanyang Drive, Singapore 636921, Singapore
Oleg Usoltsev
CELLS‐ALBA Synchrotron Cerdanyola del Vallès Carrer de la Llum, 2, 26 Barcelona Catalonia 08290 Spain
Irina Martynova
Catalonia Institute for Energy Research (IREC) Sant Adrià de Besòs Barcelona Catalonia 08930 Spain
Chen Huang
Catalonia Institute for Energy Research-IREC, Sant Adrià de Besòs, Barcelona 08930, Spain
Zhifu Liang
College of Ocean Science and Engineering Shanghai Maritime University Shanghai 201306 China
Ivan Pinto‐Huguet
Catalan Institute of Nanoscience and Nanotechnology – ICN2 (CSIC and BIST) Campus UAB Bellaterra Barcelona 08193 Catalonia Spain
Canhuang Li
Catalonia Institute for Energy Research-IREC, Sant Adrià de Besòs, Barcelona 08930, Spain
Liqiang Lu
Helmholtz‐Zentrum Berlin für Materialien und Energie Hahn‐Meitner‐Platz 1 14109 Berlin Germany
Chaoqi Zhang
Shanghai University , , ,
Xuan Lu
Kapil Gupta
Marc Botifoll
Laura Simonelli
CELLS─ALBA Synchrotron Radiation Facility, Carrer de la Llum 2-26, Cerdanyola del Vallès 08290, Spain
Francois Fauth
CELLS-ALBA Synchrotron, Cerdanyola del Vallès, E-08290 Barcelona, Spain
Jin Yuan Zhou
School of Physical Science & Technology
Jordi Llorca
Department of Chemical Engineering and Center for Research in Multiscale Science and Engineering, Universitat Politècnica de Catalunya, UPC-EEBE, Eduard Maristany 10-14, 08019 Barcelona, Spain
Yan Lu
Chao Yue Zhang
Department of Chemistry and Biochemistry
Jordi Arbiol
Catalan Institute of Nanoscience and Nanotechnology − ICN2 (CSIC and BIST), Campus UAB, Bellaterra, Barcelona, Catalonia 08193, Spain
Andreu Cabot
Catalonia Institute for Energy Research-IREC, Sant Adrià de Besòs, Barcelona 08930, Spain