Intermetallic-driven highly reversible electrocatalysis in Li–CO2 battery over nanoporous Ni3Al/Ni heterostructure
Tianzhen Jian,
Wenqing Ma,
Caixia Xu,
Hong Liu,
John Wang
Affiliations
Tianzhen Jian
Institute for Advanced Interdisciplinary Research (iAIR), School of Chemistry and Chemical Engineering, Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of Shandong, University of Jinan, Jinan, 250022, China
Wenqing Ma
Institute for Advanced Interdisciplinary Research (iAIR), School of Chemistry and Chemical Engineering, Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of Shandong, University of Jinan, Jinan, 250022, China; Corresponding authors.
Caixia Xu
Institute for Advanced Interdisciplinary Research (iAIR), School of Chemistry and Chemical Engineering, Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of Shandong, University of Jinan, Jinan, 250022, China; Corresponding authors.
Hong Liu
Institute for Advanced Interdisciplinary Research (iAIR), School of Chemistry and Chemical Engineering, Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of Shandong, University of Jinan, Jinan, 250022, China
John Wang
Department of Materials Science and Engineering, National University of Singapore, Singapore, 117574, Singapore; Institute of Materials Research and Engineering, A∗Star, Singapore, 138634, Singapore
Li–CO2 batteries, which integrate CO2 utilization and electrochemical energy storage, offer the prospect of utilizing a greenhouse gas and providing an alternative to the well-established lithium-ion batteries. However, they still suffer from rather limited reversibility, low energy efficiency, and sluggish CO2 redox reaction kinetics. To address these key issues, a nanoporous Ni3Al intermetallic/Ni heterojunction (NP–Ni3Al/Ni) is purposely engineered here via an alloying–etching protocol, whereby the unique interactions between Al and Ni in Ni3Al endow NP-Ni3Al/Ni with optimum reactant/product adsorption and thus unique catalytic performance for the CO2 redox reaction. Furthermore, the nanoporous spongy structure benefits mass transport as well as discharge product storage and enables a rich multiphase reaction interface. In situ Raman studies and theoretical simulations reveal that both CO2 reduction and the co-decomposition of Li2CO3 and C are distinctly promoted by NP-Ni3Al/Ni, thereby greatly improving catalytic activity and stability. NP-Ni3Al/Ni offers promising application potential in Li–CO2 batteries, with its scalable fabrication, low production cost, and superior catalytic performance.
