Pub Date : 2025-07-01DOI: 10.1016/j.esci.2025.100375
Zhi-Xiang Yuan , Yingjie Gao , Shan-Qing Li , Jie Xuan , Xin-Yu Sheng , Fei Zhang , Yao Zheng , Ping Chen
The electrochemical oxidation of small molecules is a promising approach in chemical synthesis, but catalyst deactivation due to the accumulation of poorly soluble products on the surface remains a significant challenge. To address this, we propose an in situ cleaning method using an additional oxygen evolution reaction (OER) to regenerate degraded catalysts. The OER facilitates the removal of insoluble products, thereby restoring active sites. Taking the electrochemical oxidation of tetrahydroisoquinoline (THIQ) to dihydroisoquinoline (DHIQ) as an example, we develop a highly active γ-Ni(Co)OOH anode. The OER generates oxygen, promoting the oxidation of DHIQ to IQ, which is more soluble, thus effectively removing DHIQ from the catalyst surface. After 120 cycles in a small-scale pilot test, the current stability exceeds 98%, and the product selectivity reaches 95%. This method demonstrates the highest stability to date, outperforming previous catalysts 15-fold, and can be applied to other electrocatalytic systems facing similar deactivation issues.
{"title":"A versatile catalyst in situ self-cleaning method for excellent cycling and operational stability in small-molecule electrooxidation","authors":"Zhi-Xiang Yuan , Yingjie Gao , Shan-Qing Li , Jie Xuan , Xin-Yu Sheng , Fei Zhang , Yao Zheng , Ping Chen","doi":"10.1016/j.esci.2025.100375","DOIUrl":"10.1016/j.esci.2025.100375","url":null,"abstract":"<div><div>The electrochemical oxidation of small molecules is a promising approach in chemical synthesis, but catalyst deactivation due to the accumulation of poorly soluble products on the surface remains a significant challenge. To address this, we propose an <em>in situ</em> cleaning method using an additional oxygen evolution reaction (OER) to regenerate degraded catalysts. The OER facilitates the removal of insoluble products, thereby restoring active sites. Taking the electrochemical oxidation of tetrahydroisoquinoline (THIQ) to dihydroisoquinoline (DHIQ) as an example, we develop a highly active γ-Ni(Co)OOH anode. The OER generates oxygen, promoting the oxidation of DHIQ to IQ, which is more soluble, thus effectively removing DHIQ from the catalyst surface. After 120 cycles in a small-scale pilot test, the current stability exceeds 98%, and the product selectivity reaches 95%. This method demonstrates the highest stability to date, outperforming previous catalysts 15-fold, and can be applied to other electrocatalytic systems facing similar deactivation issues.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 4","pages":"Article 100375"},"PeriodicalIF":42.9,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144633402","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-07-01DOI: 10.1016/j.esci.2024.100353
Lingao Deng , Liming Jin , Luyu Yang , Chenchen Feng , An Tao , Xianlin Jia , Zhen Geng , Cunman Zhang , Xiangzhi Cui , Jianlin Shi
It is anticipated that alkaline water electrolysis (AWE) technology will assume a significant role in the future energy sector, facilitating the integration of renewable energy and hydrogen production. Regrettably, the efficiency of AWE is not yet optimal. In particular, the inefficiency caused by bubbles at increased current density is often overlooked, necessitating a detailed understanding of the intricate relationship between bubble evolution and electrolytic reactions. This paper presents a comprehensive review of the fundamental theory and recent research on bubbles, and outlines the primary challenges and research directions for bubble dynamics in AWE. First, the theory of bubble nucleation, growth, and detachment is reviewed and summarized. Subsequently, the impact of bubbles on the diverse processes occurring during the electrolysis reaction is meticulously delineated and examined. The following section presents a thorough compilation and categorization of the methods employed to remove bubbles, with a detailed analysis of the strategies deployed to mitigate the impact of gas bubble traffic. Additionally, an in-depth exploration of the research methodology employed at each stage of the bubble evolution process is provided. Finally, the review concludes with a summary and outlook on the opportunities and challenges associated with studying bubble dynamics in AWE, offering insights into innovative avenues for efficient electrolytic hydrogen production.
{"title":"Bubble evolution dynamics in alkaline water electrolysis","authors":"Lingao Deng , Liming Jin , Luyu Yang , Chenchen Feng , An Tao , Xianlin Jia , Zhen Geng , Cunman Zhang , Xiangzhi Cui , Jianlin Shi","doi":"10.1016/j.esci.2024.100353","DOIUrl":"10.1016/j.esci.2024.100353","url":null,"abstract":"<div><div>It is anticipated that alkaline water electrolysis (AWE) technology will assume a significant role in the future energy sector, facilitating the integration of renewable energy and hydrogen production. Regrettably, the efficiency of AWE is not yet optimal. In particular, the inefficiency caused by bubbles at increased current density is often overlooked, necessitating a detailed understanding of the intricate relationship between bubble evolution and electrolytic reactions. This paper presents a comprehensive review of the fundamental theory and recent research on bubbles, and outlines the primary challenges and research directions for bubble dynamics in AWE. First, the theory of bubble nucleation, growth, and detachment is reviewed and summarized. Subsequently, the impact of bubbles on the diverse processes occurring during the electrolysis reaction is meticulously delineated and examined. The following section presents a thorough compilation and categorization of the methods employed to remove bubbles, with a detailed analysis of the strategies deployed to mitigate the impact of gas bubble traffic. Additionally, an in-depth exploration of the research methodology employed at each stage of the bubble evolution process is provided. Finally, the review concludes with a summary and outlook on the opportunities and challenges associated with studying bubble dynamics in AWE, offering insights into innovative avenues for efficient electrolytic hydrogen production.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 4","pages":"Article 100353"},"PeriodicalIF":42.9,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144633400","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-07-01DOI: 10.1016/j.esci.2024.100368
Huan Li , Jinchao Xu , Liyuan Yang , Wanying Wang , Bin Shao , Fangyi Cheng , Chunning Zhao , Weichao Wang
Developing transition metal compound (TMC) catalysts is complicated by the intricate relationship between their crystal and electronic structures and their catalytic performance. To address this challenge, we propose the “from active unit to catalyst” (FAUC) strategy starting with optimizing the physical property of a Mn-centered [MnO6] entity to ensure its catalytic performance. These entities are then arranged to reveal how their assembly influences the electronic structures. Notably, a two-dimensional (2D) entity-formed lattice shows a promising low theoretical overpotential (0.08 V) for oxygen reduction reaction due to the optimal occupied orbital position. According to the catalytic requirements of an individual entity and its stacking modes, we further developed a search algorithm to identify three-dimensional (3D) structures from 154,718 candidates, pinpointing CaMnO3 as the most effective one among the screened candidates. This FAUC approach provides a comprehensive framework for designing catalysts from basic units to complex assemblies.
{"title":"Advancing Mn-based electrocatalysts: Evolving from Mn-centered octahedral entities to bulk forms","authors":"Huan Li , Jinchao Xu , Liyuan Yang , Wanying Wang , Bin Shao , Fangyi Cheng , Chunning Zhao , Weichao Wang","doi":"10.1016/j.esci.2024.100368","DOIUrl":"10.1016/j.esci.2024.100368","url":null,"abstract":"<div><div>Developing transition metal compound (TMC) catalysts is complicated by the intricate relationship between their crystal and electronic structures and their catalytic performance. To address this challenge, we propose the “from active unit to catalyst” (FAUC) strategy starting with optimizing the physical property of a Mn-centered [MnO<sub>6</sub>] entity to ensure its catalytic performance. These entities are then arranged to reveal how their assembly influences the electronic structures. Notably, a two-dimensional (2D) entity-formed lattice shows a promising low theoretical overpotential (0.08 V) for oxygen reduction reaction due to the optimal occupied <span><math><mrow><msub><mi>d</mi><msup><mi>z</mi><mn>2</mn></msup></msub></mrow></math></span> orbital position. According to the catalytic requirements of an individual entity and its stacking modes, we further developed a search algorithm to identify three-dimensional (3D) structures from 154,718 candidates, pinpointing CaMnO<sub>3</sub> as the most effective one among the screened candidates. This FAUC approach provides a comprehensive framework for designing catalysts from basic units to complex assemblies.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 4","pages":"Article 100368"},"PeriodicalIF":42.9,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144633401","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-07-01DOI: 10.1016/j.esci.2024.100334
Zichen Xu , Zhong-Shuai Wu
Electrochemical water splitting is a pivotal technology in the large-scale production of green hydrogen for sustainable future energy provisions. Highly active, stable electrocatalysts have been extensively explored, but the majority suffer from low current densities and small sizes, rendering them unsuitable for industrial applications. Recently, however, the scalable production of electrocatalysts with high performance at large current densities has made tremendous progress. In this review, the current achievements in developing outstanding large electrocatalysts for high-current-density water electrolysis are described in detail. First, we introduce the fundamentals of water electrolysis, the criteria for performance evaluation, and the requirements for producing electrocatalysts at scale under large current densities. Second, we summarize the key approaches for realizing large-sized electrocatalysts with excellent performance, including electrodeposition, corrosion engineering, and thermal treatment, as well as combinations of these methods. Finally, we offer perspectives on research challenges and propose directions for mass-producing high-performance electrocatalysts with large current densities for water electrolysis, to guide the further industrialization of water-electrolysis catalysts.
{"title":"Scalable production of high-performance electrocatalysts for electrochemical water splitting at large current densities","authors":"Zichen Xu , Zhong-Shuai Wu","doi":"10.1016/j.esci.2024.100334","DOIUrl":"10.1016/j.esci.2024.100334","url":null,"abstract":"<div><div>Electrochemical water splitting is a pivotal technology in the large-scale production of green hydrogen for sustainable future energy provisions. Highly active, stable electrocatalysts have been extensively explored, but the majority suffer from low current densities and small sizes, rendering them unsuitable for industrial applications. Recently, however, the scalable production of electrocatalysts with high performance at large current densities has made tremendous progress. In this review, the current achievements in developing outstanding large electrocatalysts for high-current-density water electrolysis are described in detail. First, we introduce the fundamentals of water electrolysis, the criteria for performance evaluation, and the requirements for producing electrocatalysts at scale under large current densities. Second, we summarize the key approaches for realizing large-sized electrocatalysts with excellent performance, including electrodeposition, corrosion engineering, and thermal treatment, as well as combinations of these methods. Finally, we offer perspectives on research challenges and propose directions for mass-producing high-performance electrocatalysts with large current densities for water electrolysis, to guide the further industrialization of water-electrolysis catalysts.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 4","pages":"Article 100334"},"PeriodicalIF":42.9,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144633548","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-06-18DOI: 10.1016/j.esci.2025.100434
Yichuan Dou , Lanling Zhao , Jun Wang , Songze Li , Yiming Zhang , Ruifeng Li , Mingzhu Gao , Ce Zhang , Zaiping Guo
MnMoO4 holds great promise as a cathode material for lithium–oxygen batteries (LOBs), but its poor conductivity and weak interaction with oxygenated intermediates substantially impede its electrocatalytic properties. Herein, electron-deficient P atoms were incorporated with MnMoO4 hollow nanospheres (P-doped MnMoO4) to realize internal orbital interactions between Mo 4d and P 3p, activating external orbital hybridization between catalysts and LiO2 during cycling. This relay orbital hybridization not only promoted charge transfer but also optimized the adsorption and desorption abilities of catalysts toward LiO2, thereby reducing the reaction energy barriers. Consequently, LOBs with P-doped MnMoO4 cathode catalysts sustained steady operation for 380 cycles under 1000 mA g−1, which is even better than some of their noble metal counterparts and points to their commercial promise for use in future large-scale applications. This work provides general guidance for constructing relay orbital hybridization through P doping on catalysts for LOBs and other electrocatalytic systems.
作为锂氧电池（lob）的正极材料，MnMoO4具有很大的前景，但其导电性差和与含氧中间体的弱相互作用极大地阻碍了其电催化性能。本文将缺电子的P原子与MnMoO4空心纳米球（P掺杂MnMoO4）结合，实现了mo4d和p3p之间的内轨道相互作用，激活了催化剂与LiO2在循环过程中的外轨道杂化。这种接力轨道杂化不仅促进了电荷转移，而且优化了催化剂对LiO2的吸附和解吸能力，从而降低了反应能垒。因此，掺杂p的MnMoO4阴极催化剂的lob在1000 mA g−1下持续稳定运行380个循环，甚至比一些贵金属催化剂更好，并指出其在未来大规模应用中的商业前景。这项工作为通过在lob和其他电催化体系催化剂上掺杂P来构建接力轨道杂化提供了一般指导。
{"title":"Relay orbital hybridization on MnMoO4 catalysts for durable lithium–oxygen batteries","authors":"Yichuan Dou , Lanling Zhao , Jun Wang , Songze Li , Yiming Zhang , Ruifeng Li , Mingzhu Gao , Ce Zhang , Zaiping Guo","doi":"10.1016/j.esci.2025.100434","DOIUrl":"10.1016/j.esci.2025.100434","url":null,"abstract":"<div><div>MnMoO<sub>4</sub> holds great promise as a cathode material for lithium–oxygen batteries (LOBs), but its poor conductivity and weak interaction with oxygenated intermediates substantially impede its electrocatalytic properties. Herein, electron-deficient P atoms were incorporated with MnMoO<sub>4</sub> hollow nanospheres (P-doped MnMoO<sub>4</sub>) to realize internal orbital interactions between Mo 4d and P 3p, activating external orbital hybridization between catalysts and LiO<sub>2</sub> during cycling. This relay orbital hybridization not only promoted charge transfer but also optimized the adsorption and desorption abilities of catalysts toward LiO<sub>2</sub>, thereby reducing the reaction energy barriers. Consequently, LOBs with P-doped MnMoO<sub>4</sub> cathode catalysts sustained steady operation for 380 cycles under 1000 mA g<sup>−1</sup>, which is even better than some of their noble metal counterparts and points to their commercial promise for use in future large-scale applications. This work provides general guidance for constructing relay orbital hybridization through P doping on catalysts for LOBs and other electrocatalytic systems.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"6 2","pages":"Article 100434"},"PeriodicalIF":36.6,"publicationDate":"2025-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146039159","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-06-14DOI: 10.1016/j.esci.2025.100437
Zixian Wang , Fan Liu , Yuqing Meng , Wenjuan Bian , Haiyan Zhao , Chuancheng Duan , Michael T. Benson , Meng Li , Bin Liu , Dong Ding
Protonic ceramic cells (PCCs) have emerged as a promising technology for power generation, energy storage, and value-added chemical synthesis, offering benefits such as fuel flexibility, low emissions, and efficient operation at intermediate temperatures (300–600 °C). Recently, significant breakthroughs in materials and manufacturing methods have markedly enhanced the performance of PCCs. However, establishing a fundamental understanding of their electrocatalytic reactions has gained less attention. As a fast and cost-effective method for physicochemical fingerprinting, diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) has proven to be a surface-sensitive analytical tool for structural and functional studies. This review critically examines the most up-to-date applications of DRIFTS for characterizing key components of PCCs, including oxygen electrodes, protonic electrolytes, and hydrogen electrodes for different applications, with a focus on revealing hydration properties and catalytic reactions, and guiding rational material design. The challenges for advancing DRIFTS, including quantitative capabilities and operando applications for PCC investigations, are highlighted and strategies to tackle these challenges are discussed. Ultimately, this review underscores the critical role of DRIFTS in accelerating the development of high-performance and durable PCCs for next-generation energy solutions, offering methodologies and insights broadly applicable to a wide range of electrochemical energy conversion and storage technologies.
{"title":"A comprehensive review of diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) techniques in protonic ceramic cells (PCCs): Current status and future perspective","authors":"Zixian Wang , Fan Liu , Yuqing Meng , Wenjuan Bian , Haiyan Zhao , Chuancheng Duan , Michael T. Benson , Meng Li , Bin Liu , Dong Ding","doi":"10.1016/j.esci.2025.100437","DOIUrl":"10.1016/j.esci.2025.100437","url":null,"abstract":"<div><div>Protonic ceramic cells (PCCs) have emerged as a promising technology for power generation, energy storage, and value-added chemical synthesis, offering benefits such as fuel flexibility, low emissions, and efficient operation at intermediate temperatures (300–600 °C). Recently, significant breakthroughs in materials and manufacturing methods have markedly enhanced the performance of PCCs. However, establishing a fundamental understanding of their electrocatalytic reactions has gained less attention. As a fast and cost-effective method for physicochemical fingerprinting, diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) has proven to be a surface-sensitive analytical tool for structural and functional studies. This review critically examines the most up-to-date applications of DRIFTS for characterizing key components of PCCs, including oxygen electrodes, protonic electrolytes, and hydrogen electrodes for different applications, with a focus on revealing hydration properties and catalytic reactions, and guiding rational material design. The challenges for advancing DRIFTS, including quantitative capabilities and <em>operando</em> applications for PCC investigations, are highlighted and strategies to tackle these challenges are discussed. Ultimately, this review underscores the critical role of DRIFTS in accelerating the development of high-performance and durable PCCs for next-generation energy solutions, offering methodologies and insights broadly applicable to a wide range of electrochemical energy conversion and storage technologies.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 5","pages":"Article 100437"},"PeriodicalIF":36.6,"publicationDate":"2025-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144887357","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-06-05DOI: 10.1016/j.esci.2025.100436
Yun Ke , Tong Li , Jun Li , Mingliang Pei , Xinming Wang , Weichang Xie , Shuting Zhuang , Xiaofeng Ye , Zhou Li , Zuankai Wang , Fan Yang
Cardiovascular diseases remain the leading cause of global morbidity and mortality, underscoring the urgent need for advanced technologies capable of continuous, noninvasive, and intelligent monitoring. Piezoelectric sensors, owing to their inherent electromechanical transduction, high sensitivity, and self-powered operation, offer a compelling pathway for next-generation cardiovascular health monitoring. In this review, we summarize recent advances in piezoelectric materials, from zero-to three-dimensional architectures, and their integration into wearable and implantable platforms. Key applications include the assessment of arterial health via pulse wave velocity and vascular stiffness, cuffless blood pressure estimation, and the monitoring of cardiopulmonary functions such as heart rate, respiratory rhythm, and cardiac acoustics. We also highlight emerging strategies such as passive wireless communication enabled by surface acoustic wave principles, and the development of multimodal systems that concurrently capture mechanical, optical, and chemical signals. The convergence of piezoelectric technologies with artificial intelligence and Internet of Things frameworks enables real-time signal processing, remote access, and personalized medical interventions. Finally, we discuss current challenges in material biocompatibility, encapsulation, signal fidelity, and clinical translation, and outline future directions for advancing high-performance piezoelectric systems for intelligent cardiovascular diagnostics and connected healthcare.
{"title":"Heartbeat electro-language: Exploring piezoelectric technologies for cardiovascular health monitoring","authors":"Yun Ke , Tong Li , Jun Li , Mingliang Pei , Xinming Wang , Weichang Xie , Shuting Zhuang , Xiaofeng Ye , Zhou Li , Zuankai Wang , Fan Yang","doi":"10.1016/j.esci.2025.100436","DOIUrl":"10.1016/j.esci.2025.100436","url":null,"abstract":"<div><div>Cardiovascular diseases remain the leading cause of global morbidity and mortality, underscoring the urgent need for advanced technologies capable of continuous, noninvasive, and intelligent monitoring. Piezoelectric sensors, owing to their inherent electromechanical transduction, high sensitivity, and self-powered operation, offer a compelling pathway for next-generation cardiovascular health monitoring. In this review, we summarize recent advances in piezoelectric materials, from zero-to three-dimensional architectures, and their integration into wearable and implantable platforms. Key applications include the assessment of arterial health via pulse wave velocity and vascular stiffness, cuffless blood pressure estimation, and the monitoring of cardiopulmonary functions such as heart rate, respiratory rhythm, and cardiac acoustics. We also highlight emerging strategies such as passive wireless communication enabled by surface acoustic wave principles, and the development of multimodal systems that concurrently capture mechanical, optical, and chemical signals. The convergence of piezoelectric technologies with artificial intelligence and Internet of Things frameworks enables real-time signal processing, remote access, and personalized medical interventions. Finally, we discuss current challenges in material biocompatibility, encapsulation, signal fidelity, and clinical translation, and outline future directions for advancing high-performance piezoelectric systems for intelligent cardiovascular diagnostics and connected healthcare.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"6 1","pages":"Article 100436"},"PeriodicalIF":36.6,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145842682","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-05-29DOI: 10.1016/j.esci.2025.100435
Yijun Song , Bo Wang , Yongpeng Cui , Pengyun Liu , Xiuli Gao , Xuejin Li , Lei Zhu , Qingzhong Xue , Yongfu Tang , Wei Xing
Layered oxide cathodes play a crucial role in developing high-energy-density Li-ion batteries. However, limited by weak interlayer support and poor oxygen stability, the ordered structure is easily transformed into a dense disordered structure, thus limiting their cycle life. Here we show that constructing a localized cation disorder (LCD) structure by chemically inducing treatment can radically address the mechanical-chemical coupling-induced structural degradation in ultrahigh-Ni cathodes. The LCD structure is proved to function as a steady-state supporting nanodomain, not only effectively enhancing the collective mechanical stability, especially avoiding the collapse of the Li-ion diffusion channel, but also enhancing the lattice oxygen framework stability by reducing charge compensation and improving electronic conductivity. As a result, the ultrahigh-Ni cathode with an LCD structure demonstrates remarkable capacity retention and excellent rate performance. This work highlights the effectiveness of localized structural design in addressing the mechanical and chemical instabilities for advanced oxide cathodes.
{"title":"Mechanically and chemically robust ultrahigh-Ni cathodes enabled by localized cation disorder design","authors":"Yijun Song , Bo Wang , Yongpeng Cui , Pengyun Liu , Xiuli Gao , Xuejin Li , Lei Zhu , Qingzhong Xue , Yongfu Tang , Wei Xing","doi":"10.1016/j.esci.2025.100435","DOIUrl":"10.1016/j.esci.2025.100435","url":null,"abstract":"<div><div>Layered oxide cathodes play a crucial role in developing high-energy-density Li-ion batteries. However, limited by weak interlayer support and poor oxygen stability, the ordered structure is easily transformed into a dense disordered structure, thus limiting their cycle life. Here we show that constructing a localized cation disorder (LCD) structure by chemically inducing treatment can radically address the mechanical-chemical coupling-induced structural degradation in ultrahigh-Ni cathodes. The LCD structure is proved to function as a steady-state supporting nanodomain, not only effectively enhancing the collective mechanical stability, especially avoiding the collapse of the Li-ion diffusion channel, but also enhancing the lattice oxygen framework stability by reducing charge compensation and improving electronic conductivity. As a result, the ultrahigh-Ni cathode with an LCD structure demonstrates remarkable capacity retention and excellent rate performance. This work highlights the effectiveness of localized structural design in addressing the mechanical and chemical instabilities for advanced oxide cathodes.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"6 1","pages":"Article 100435"},"PeriodicalIF":36.6,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145842683","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-05-26DOI: 10.1016/j.esci.2025.100431
Xin Zhao , Zhonghan Zhang , Chenfei Li , Lizhen Liu , Yonghao Xiao , Zihao Wang , Shuzhou Li , Han Sen Soo
One solution to the intermittency of renewable energy sources is energy storage in fuels such as hydrogen produced by water electrolysis. However, current water electrolysis systems are plagued by high costs. Here, a co-electrolysis system for biomass-derived glucose and water is shown to achieve green hydrogen generation of over 500 μmol h−1 cm−2 using a membrane-free undivided cell with electrocatalysts comprising only earth-abundant elements, driven by a triple-junction photovoltaic. Glucose is selectively electrooxidized to formate with high yields of up to 80%, instead of water being oxidized into oxygen; the former circumvents the need for costly membranes to separate the hydrogen and oxygen gaseous products. High selectivity is achieved through cascade carbon–carbon bond oxidation by regulating the adsorption mode and moderating the oxidation state of cobalt with copper doping. The overall electrolysis potential is lowered by ∼400 mV compared to water splitting. The revenue from the formate co-product can lower the levelized cost of hydrogen from water electrolysis by $4.63/kg of hydrogen produced, making it competitive with grey hydrogen generation.
{"title":"Steering the adsorption modes and oxidation state of Co oxyhydroxide active sites to unlock selective glucose oxidation to formate for efficient solar reforming of biomass to green hydrogen","authors":"Xin Zhao , Zhonghan Zhang , Chenfei Li , Lizhen Liu , Yonghao Xiao , Zihao Wang , Shuzhou Li , Han Sen Soo","doi":"10.1016/j.esci.2025.100431","DOIUrl":"10.1016/j.esci.2025.100431","url":null,"abstract":"<div><div>One solution to the intermittency of renewable energy sources is energy storage in fuels such as hydrogen produced by water electrolysis. However, current water electrolysis systems are plagued by high costs. Here, a co-electrolysis system for biomass-derived glucose and water is shown to achieve green hydrogen generation of over 500 μmol h<sup>−1</sup> cm<sup>−2</sup> using a membrane-free undivided cell with electrocatalysts comprising only earth-abundant elements, driven by a triple-junction photovoltaic. Glucose is selectively electrooxidized to formate with high yields of up to 80%, instead of water being oxidized into oxygen; the former circumvents the need for costly membranes to separate the hydrogen and oxygen gaseous products. High selectivity is achieved through cascade carbon–carbon bond oxidation by regulating the adsorption mode and moderating the oxidation state of cobalt with copper doping. The overall electrolysis potential is lowered by ∼400 mV compared to water splitting. The revenue from the formate co-product can lower the levelized cost of hydrogen from water electrolysis by $4.63/kg of hydrogen produced, making it competitive with grey hydrogen generation.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 6","pages":"Article 100431"},"PeriodicalIF":36.6,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145366117","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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