DataVXAdvanced MaterialsPaper
journal article·2024-01Open access

Energy Band Engineering Guided Design of Bidirectional Catalyst for Reversible Li–CO2 Batteries

Bingyi Lu, Xinru Wu, Xiao Xiao, Biao Chen, Weihao Zeng, Yingqi Liu, Zhoujie Lao, Xian‐Xiang Zeng, Guangmin Zhou, Jinlong Yang

Advanced Materials· Volume 36· Issue 1
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Source abstract

Abstract

Abstract Li–CO2 batteries arouse great interest in the context of carbon neutralization, but their practicability is severely hindered by the sluggish CO2 redox reaction kinetics at the cathode, which brings about formidable challenges such as high overpotential and low Coulombic efficiency. For the complex multi‐electron transfer process, the design of catalysts at the molecular or atomic level and the understanding of the relationship between electron state and performance are essential for the CO2 redox. However, little attention is paid to it. In this work, using Co3S4 as a model system, density functional theory (DFT) calculations reveal that the adjusted d‐band and p‐band centers of Co3S4 with the introduction of Cu and sulfur vacancies are hybridized between CO2 and Li species, respectively, which is conducive to the adsorption of reactants and the decomposition of Li2CO3, and the experimental results further verify the effectiveness of energy band engineering. As a result, a highly efficient bidirectional catalyst is produced and shows an ultra‐small voltage gap of 0.73 V and marvelous Coulombic efficiency of 92.6%, surpassing those of previous catalysts under similar conditions. This work presents an effective catalyst design and affords new insight into the high‐performance cathode catalyst materials for Li–CO2 batteries.
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Research context

Energy storageCatalysis & surfaces

OpenAlex topics: Advancements in Battery Materials · Advanced Battery Materials and Technologies · Inorganic Chemistry and Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Shenzhen Key Laboratory of Energy Electrocatalytic Materials Guangdong Research Center for Interfacial Engineering of Functional Materials College of Materials Science and Engineering Shenzhen University Shenzhen 518060 China

College of Physics and Optoelectronic Engineering, Shenzhen University Shenzhen 518060 China

Tsinghua–Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518055 China

School of Materials Science and Engineering and Tianjin Key Laboratory of Composite and Functional Materials Tianjin University Tianjin 300350 China

State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China

School of Chemistry and Materials Science Hunan Agricultural University Changsha 410128 China

Funding

National Key Research and Development Program of China · National Natural Science Foundation of China · Natural Science Foundation of Guangdong Province · Guangdong Innovative and Entrepreneurial Research Team Program · Shenzhen Science and Technology Innovation Program

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