Can single-atom precision rewire the electrochemical logic of Li–S chemistry? A comprehensive review of single-atom catalysts as agents of precise modulation

Single-atom catalysts (SACs) present a compelling strategy to overcome the persistent challenges in lithium–sulfur batteries, such as polysulfide shuttling and sluggish redox kinetics. Their atomically dispersed nature and tunable coordination structures enable selective modulation of intermediate s...

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Veröffentlicht in:Chemical science (Cambridge) Jg. 16; H. 46; S. 21677 - 2174
Hauptverfasser: Wang, Yue, Song, Haobin, Zhao, Nan, Cheng, Xi, Li, Dong-Sheng, Yang, Hui Ying
Format: Journal Article
Sprache:Englisch
Veröffentlicht: England Royal Society of Chemistry 26.11.2025
Schlagworte:
Adsorption
Catalysis
Coordination
Functional integration
Lithium
Lithium sulfur batteries
Modulation
Polysulfides
Single atom catalysts
Sulfur
ISSN:2041-6520, 2041-6539
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Abstract Single-atom catalysts (SACs) present a compelling strategy to overcome the persistent challenges in lithium–sulfur batteries, such as polysulfide shuttling and sluggish redox kinetics. Their atomically dispersed nature and tunable coordination structures enable selective modulation of intermediate species and catalytic interfaces. Despite rapid progress, SAC design remains largely empirical, lacking a unified mechanistic framework. In this review, we outline a precision catalysis paradigm for SACs in lithium–sulfur systems. The discussion is organized along three core dimensions: spatial configuration, reaction pathway control, and functional integration. We summarize how coordination asymmetry, charge redistribution, and interfacial electronic coupling influence the adsorption and transformation of lithium polysulfides and Li 2 S. These insights are supported by spectroscopic characterization and theoretical calculations. Beyond conventional activity descriptors, we uncover structure–activity correlations involving d-band shifts, orbital hybridization, and electronic field effects. The concluded framework is further applied to sodium–sulfur, potassium–sulfur, and solid-state lithium–sulfur systems, demonstrating broad applicability. This review advances the understanding of SACs from passive adsorption sites toward programmable redox regulation. It provides conceptual and design guidance for future catalyst development based on adaptive coordination environments and data-driven optimization strategies. Single-atom precision rewires Li–S electrochemical logic via spatial configuration, pathway programming, and functional coupling; the paradigm extends to Na/K/Mg–S and solid-state systems.
AbstractList Single-atom catalysts (SACs) present a compelling strategy to overcome the persistent challenges in lithium–sulfur batteries, such as polysulfide shuttling and sluggish redox kinetics. Their atomically dispersed nature and tunable coordination structures enable selective modulation of intermediate species and catalytic interfaces. Despite rapid progress, SAC design remains largely empirical, lacking a unified mechanistic framework. In this review, we outline a precision catalysis paradigm for SACs in lithium–sulfur systems. The discussion is organized along three core dimensions: spatial configuration, reaction pathway control, and functional integration. We summarize how coordination asymmetry, charge redistribution, and interfacial electronic coupling influence the adsorption and transformation of lithium polysulfides and Li2S. These insights are supported by spectroscopic characterization and theoretical calculations. Beyond conventional activity descriptors, we uncover structure–activity correlations involving d-band shifts, orbital hybridization, and electronic field effects. The concluded framework is further applied to sodium–sulfur, potassium–sulfur, and solid-state lithium–sulfur systems, demonstrating broad applicability. This review advances the understanding of SACs from passive adsorption sites toward programmable redox regulation. It provides conceptual and design guidance for future catalyst development based on adaptive coordination environments and data-driven optimization strategies.
Single-atom catalysts (SACs) present a compelling strategy to overcome the persistent challenges in lithium–sulfur batteries, such as polysulfide shuttling and sluggish redox kinetics. Their atomically dispersed nature and tunable coordination structures enable selective modulation of intermediate species and catalytic interfaces. Despite rapid progress, SAC design remains largely empirical, lacking a unified mechanistic framework. In this review, we outline a precision catalysis paradigm for SACs in lithium–sulfur systems. The discussion is organized along three core dimensions: spatial configuration, reaction pathway control, and functional integration. We summarize how coordination asymmetry, charge redistribution, and interfacial electronic coupling influence the adsorption and transformation of lithium polysulfides and Li 2 S. These insights are supported by spectroscopic characterization and theoretical calculations. Beyond conventional activity descriptors, we uncover structure–activity correlations involving d-band shifts, orbital hybridization, and electronic field effects. The concluded framework is further applied to sodium–sulfur, potassium–sulfur, and solid-state lithium–sulfur systems, demonstrating broad applicability. This review advances the understanding of SACs from passive adsorption sites toward programmable redox regulation. It provides conceptual and design guidance for future catalyst development based on adaptive coordination environments and data-driven optimization strategies. Single-atom precision rewires Li–S electrochemical logic via spatial configuration, pathway programming, and functional coupling; the paradigm extends to Na/K/Mg–S and solid-state systems.
Single-atom catalysts (SACs) present a compelling strategy to overcome the persistent challenges in lithium–sulfur batteries, such as polysulfide shuttling and sluggish redox kinetics. Their atomically dispersed nature and tunable coordination structures enable selective modulation of intermediate species and catalytic interfaces. Despite rapid progress, SAC design remains largely empirical, lacking a unified mechanistic framework. In this review, we outline a precision catalysis paradigm for SACs in lithium–sulfur systems. The discussion is organized along three core dimensions: spatial configuration, reaction pathway control, and functional integration. We summarize how coordination asymmetry, charge redistribution, and interfacial electronic coupling influence the adsorption and transformation of lithium polysulfides and Li 2 S. These insights are supported by spectroscopic characterization and theoretical calculations. Beyond conventional activity descriptors, we uncover structure–activity correlations involving d-band shifts, orbital hybridization, and electronic field effects. The concluded framework is further applied to sodium–sulfur, potassium–sulfur, and solid-state lithium–sulfur systems, demonstrating broad applicability. This review advances the understanding of SACs from passive adsorption sites toward programmable redox regulation. It provides conceptual and design guidance for future catalyst development based on adaptive coordination environments and data-driven optimization strategies.
Single-atom catalysts (SACs) present a compelling strategy to overcome the persistent challenges in lithium-sulfur batteries, such as polysulfide shuttling and sluggish redox kinetics. Their atomically dispersed nature and tunable coordination structures enable selective modulation of intermediate species and catalytic interfaces. Despite rapid progress, SAC design remains largely empirical, lacking a unified mechanistic framework. In this review, we outline a precision catalysis paradigm for SACs in lithium-sulfur systems. The discussion is organized along three core dimensions: spatial configuration, reaction pathway control, and functional integration. We summarize how coordination asymmetry, charge redistribution, and interfacial electronic coupling influence the adsorption and transformation of lithium polysulfides and Li S. These insights are supported by spectroscopic characterization and theoretical calculations. Beyond conventional activity descriptors, we uncover structure-activity correlations involving d-band shifts, orbital hybridization, and electronic field effects. The concluded framework is further applied to sodium-sulfur, potassium-sulfur, and solid-state lithium-sulfur systems, demonstrating broad applicability. This review advances the understanding of SACs from passive adsorption sites toward programmable redox regulation. It provides conceptual and design guidance for future catalyst development based on adaptive coordination environments and data-driven optimization strategies.
Single-atom catalysts (SACs) present a compelling strategy to overcome the persistent challenges in lithium-sulfur batteries, such as polysulfide shuttling and sluggish redox kinetics. Their atomically dispersed nature and tunable coordination structures enable selective modulation of intermediate species and catalytic interfaces. Despite rapid progress, SAC design remains largely empirical, lacking a unified mechanistic framework. In this review, we outline a precision catalysis paradigm for SACs in lithium-sulfur systems. The discussion is organized along three core dimensions: spatial configuration, reaction pathway control, and functional integration. We summarize how coordination asymmetry, charge redistribution, and interfacial electronic coupling influence the adsorption and transformation of lithium polysulfides and Li2S. These insights are supported by spectroscopic characterization and theoretical calculations. Beyond conventional activity descriptors, we uncover structure-activity correlations involving d-band shifts, orbital hybridization, and electronic field effects. The concluded framework is further applied to sodium-sulfur, potassium-sulfur, and solid-state lithium-sulfur systems, demonstrating broad applicability. This review advances the understanding of SACs from passive adsorption sites toward programmable redox regulation. It provides conceptual and design guidance for future catalyst development based on adaptive coordination environments and data-driven optimization strategies.Single-atom catalysts (SACs) present a compelling strategy to overcome the persistent challenges in lithium-sulfur batteries, such as polysulfide shuttling and sluggish redox kinetics. Their atomically dispersed nature and tunable coordination structures enable selective modulation of intermediate species and catalytic interfaces. Despite rapid progress, SAC design remains largely empirical, lacking a unified mechanistic framework. In this review, we outline a precision catalysis paradigm for SACs in lithium-sulfur systems. The discussion is organized along three core dimensions: spatial configuration, reaction pathway control, and functional integration. We summarize how coordination asymmetry, charge redistribution, and interfacial electronic coupling influence the adsorption and transformation of lithium polysulfides and Li2S. These insights are supported by spectroscopic characterization and theoretical calculations. Beyond conventional activity descriptors, we uncover structure-activity correlations involving d-band shifts, orbital hybridization, and electronic field effects. The concluded framework is further applied to sodium-sulfur, potassium-sulfur, and solid-state lithium-sulfur systems, demonstrating broad applicability. This review advances the understanding of SACs from passive adsorption sites toward programmable redox regulation. It provides conceptual and design guidance for future catalyst development based on adaptive coordination environments and data-driven optimization strategies.
Author Zhao, Nan
Wang, Yue
Cheng, Xi
Li, Dong-Sheng
Yang, Hui Ying
Song, Haobin
AuthorAffiliation National University of Singapore
The UWCSEA Dover Campus
College of Design and Engineering
Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials
College of Materials and Chemical Engineering
Pillar of Engineering Product Development
Department of Materials Science and Engineering
Singapore University of Technology and Design
China Three Gorges University
AuthorAffiliation_xml – name: Pillar of Engineering Product Development
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– name: Singapore University of Technology and Design
– name: National University of Singapore
– name: Department of Materials Science and Engineering
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  surname: Wang
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  surname: Yang
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BackLink https://www.ncbi.nlm.nih.gov/pubmed/41210283$$D View this record in MEDLINE/PubMed
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Notes Energy & Environmental Science
Yue Wang is a research fellow in Professor Hui Ying Yang's group at the National University of Singapore. He received his Ph.D. in Materials Science from Nanjing University and previously worked at the Singapore University of Technology and Design. His research lies in electrochemical energy storage, with particular focus on sodium- and potassium-ion batteries, sodium–sulfur chemistry, and solid-state sodium–sulfur batteries. He has published in journals including
and
H
index 100) and international recognition including the NRF Investigatorship and ACS Nano Impact Award.
contributing theoretical and experimental insights toward next-generation energy devices.
Angewandte Chemie International Edition
ACS Nano
Advanced Materials
,
Hui Ying Yang is a Professor in the Department of Materials Science and Engineering at the National University of Singapore. She received her Ph.D. from Nanyang Technological University and previously held faculty appointments at the Singapore University of Technology and Design and visiting assistant professor at the Massachusetts Institute of Technology. Her research focuses on advanced nanomaterials for energy storage and water treatment, leading to over 400 publications with more than 30 000 citations
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Snippet Single-atom catalysts (SACs) present a compelling strategy to overcome the persistent challenges in lithium–sulfur batteries, such as polysulfide shuttling and...
Single-atom catalysts (SACs) present a compelling strategy to overcome the persistent challenges in lithium-sulfur batteries, such as polysulfide shuttling and...
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SubjectTerms Adsorption
Catalysis
Coordination
Functional integration
Lithium
Lithium sulfur batteries
Modulation
Polysulfides
Single atom catalysts
Sulfur
Title Can single-atom precision rewire the electrochemical logic of Li–S chemistry? A comprehensive review of single-atom catalysts as agents of precise modulation
URI https://www.ncbi.nlm.nih.gov/pubmed/41210283
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