Pub Date : 2025-07-01Epub Date: 2025-01-25DOI: 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 : 2025-07-01Epub Date: 2024-12-24DOI: 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 : 2025-07-01Epub Date: 2024-12-14DOI: 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 : 2025-07-01Epub Date: 2024-11-14DOI: 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 : 2025-07-01Epub Date: 2025-02-13DOI: 10.1016/j.esci.2025.100379
Lei Li , Siqi Liu , Jie Luo , Xunan Hou , Junhua Kong , Qichong Zhang , Wenyong Lai , Chaobin He
Affordable, easily recycled organics with electroactive centers have drawn attention in the pursuit of high-performance aqueous zinc organic batteries (AZOBs). However, intrinsic barriers such as high solubility, undesirable potential, and inferior conductivity hinder their further development. To this end, we have designed an advanced cathode material for AZOBs, comprising an n-type polymer with a three-dimensional (3D) building block (HAT-TP) formed by polymerizing 2,3,6,7,10,11-hexacyano-1,4,5,8,9,12-hexazepenanthrene (HAT-CN) and 3D 2,3,6,7,14,15-hexaaminotriptycene (THA-NH2). The introduction of a 3D architecture not only bolsters the insolubility but also exposes redox-active sites for cation coordination, while the material's extended conjugated system promotes electronic delocalization to increase the redox potential and conductivity. As a result, a HAT-TP battery exhibits a notable initial discharge voltage of 1.32 V at 0.1 A g−1, followed by a midpoint voltage of 1.17 V. Remarkably, an ultrastable capacity retention ratio of up to 93.4% is achieved, even after 40,000 cycles at 5 A g−1. Theoretical simulations reveal that the elevated discharge potential results from the strong electronic delocalization of HAT-TP, which improves the affinity with cations. Ex situ characterizations and theoretical calculations verify that the reversible Zn2+/H+ co-storage mechanism involves only electroactive C=N sites and the best possible coordination paths between them.
{"title":"Three-dimensional architecture design enables hexaazatriphenylene-based polymers as high-voltage, long-lifespan cathodes for aqueous zinc–organic batteries","authors":"Lei Li , Siqi Liu , Jie Luo , Xunan Hou , Junhua Kong , Qichong Zhang , Wenyong Lai , Chaobin He","doi":"10.1016/j.esci.2025.100379","DOIUrl":"10.1016/j.esci.2025.100379","url":null,"abstract":"<div><div>Affordable, easily recycled organics with electroactive centers have drawn attention in the pursuit of high-performance aqueous zinc organic batteries (AZOBs). However, intrinsic barriers such as high solubility, undesirable potential, and inferior conductivity hinder their further development. To this end, we have designed an advanced cathode material for AZOBs, comprising an n-type polymer with a three-dimensional (3D) building block (HAT-TP) formed by polymerizing 2,3,6,7,10,11-hexacyano-1,4,5,8,9,12-hexazepenanthrene (HAT-CN) and 3D 2,3,6,7,14,15-hexaaminotriptycene (THA-NH<sub>2</sub>). The introduction of a 3D architecture not only bolsters the insolubility but also exposes redox-active sites for cation coordination, while the material's extended conjugated system promotes electronic delocalization to increase the redox potential and conductivity. As a result, a HAT-TP battery exhibits a notable initial discharge voltage of 1.32 V at 0.1 A g<sup>−1</sup>, followed by a midpoint voltage of 1.17 V. Remarkably, an ultrastable capacity retention ratio of up to 93.4% is achieved, even after 40,000 cycles at 5 A g<sup>−1</sup>. Theoretical simulations reveal that the elevated discharge potential results from the strong electronic delocalization of HAT-TP, which improves the affinity with cations. <em>Ex situ</em> characterizations and theoretical calculations verify that the reversible Zn<sup>2+</sup>/H<sup>+</sup> co-storage mechanism involves only electroactive C=N sites and the best possible coordination paths between them.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 4","pages":"Article 100379"},"PeriodicalIF":42.9,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144308024","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 : 2025-05-01Epub Date: 2024-11-13DOI: 10.1016/j.esci.2024.100332
Yijian Song , Chao Han , Weijie Li , Xiufeng Yi , Qing Liao , Ji Zhou , Yaqin Zhou , Yitao Ouyang , Yingping Zhang , Qingqing Zheng , Anqiang Pan
Integrating single atoms and clusters into a unified catalytic system represents a novel strategy for enhancing catalytic performance. Compared to single-atom catalysts, those incorporating both single atoms and clusters exhibit superior catalytic activity. However, the co-construction of these systems and the mechanisms of their catalytic efficacy remain challenging and poorly understood. In this study, we synthesized a Mn–N–C catalyst featuring MnY clusters and Mn single atoms via a straightforward two-step sintering method. Y doping facilitated the formation of Mn clusters and optimized the d-band center of Mn through a unique synergy effect, thereby reducing energy barriers and enhancing the reaction kinetics. Additionally, the electron-donating ability of Y single atoms promoted the formation of unsaturated Mn–N₃ coordination structures, resulting in excellent oxygen reduction reaction (ORR) performance. Consequently, the MnY/NC catalyst demonstrated a half-wave potential (E₁/₂) of 0.90 V and maintained stability in 0.1 M KOH, outperforming both Mn/NC and Pt/C. This work underscores the potential of rare earth metal doping in transition metals to create stable single-atom and cluster systems, effectively leveraging their synergy effect for superior catalytic performance and validating the concept of the “remote synergy effect” in heterogeneous catalysis.
将单个原子和簇整合到一个统一的催化系统中代表了一种提高催化性能的新策略。与单原子催化剂相比，那些结合单原子和簇的催化剂表现出更好的催化活性。然而，这些系统的共同构建及其催化效果的机制仍然具有挑战性且知之甚少。在这项研究中，我们通过简单的两步烧结法合成了一种具有MnY簇和Mn单原子的Mn - n - c催化剂。Y掺杂通过独特的协同效应促进了Mn簇的形成，优化了Mn的d带中心，从而降低了能垒，提高了反应动力学。此外，Y单原子的给电子能力促进了不饱和Mn-N₃配位结构的形成，从而获得了优异的氧还原反应（ORR）性能。因此，MnY/NC催化剂的半波电位（E₁/ 2）为0.90 V，在0.1 M KOH下保持稳定性，优于Mn/NC和Pt/C。这项工作强调了稀土金属在过渡金属中掺杂的潜力，可以创建稳定的单原子和簇体系，有效地利用它们的协同效应来获得卓越的催化性能，并验证了多相催化中“远程协同效应”的概念。
{"title":"Engineering bimetallic cluster architectures: Harnessing unique “remote synergy effect” between Mn and Y for enhanced electrocatalytic oxygen reduction reaction","authors":"Yijian Song , Chao Han , Weijie Li , Xiufeng Yi , Qing Liao , Ji Zhou , Yaqin Zhou , Yitao Ouyang , Yingping Zhang , Qingqing Zheng , Anqiang Pan","doi":"10.1016/j.esci.2024.100332","DOIUrl":"10.1016/j.esci.2024.100332","url":null,"abstract":"<div><div>Integrating single atoms and clusters into a unified catalytic system represents a novel strategy for enhancing catalytic performance. Compared to single-atom catalysts, those incorporating both single atoms and clusters exhibit superior catalytic activity. However, the co-construction of these systems and the mechanisms of their catalytic efficacy remain challenging and poorly understood. In this study, we synthesized a Mn–N–C catalyst featuring MnY clusters and Mn single atoms via a straightforward two-step sintering method. Y doping facilitated the formation of Mn clusters and optimized the <em>d</em>-band center of Mn through a unique synergy effect, thereby reducing energy barriers and enhancing the reaction kinetics. Additionally, the electron-donating ability of Y single atoms promoted the formation of unsaturated Mn–N₃ coordination structures, resulting in excellent oxygen reduction reaction (ORR) performance. Consequently, the MnY/NC catalyst demonstrated a half-wave potential (E₁/₂) of 0.90 V and maintained stability in 0.1 M KOH, outperforming both Mn/NC and Pt/C. This work underscores the potential of rare earth metal doping in transition metals to create stable single-atom and cluster systems, effectively leveraging their synergy effect for superior catalytic performance and validating the concept of the “remote synergy effect” in heterogeneous catalysis.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 3","pages":"Article 100332"},"PeriodicalIF":42.9,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143931609","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 : 2025-05-01Epub Date: 2024-09-10DOI: 10.1016/j.esci.2024.100309
Ruo-Bei Huang , Meng-Yin Wang , Jian-Feng Xiong , Hua Zhang , Jing-Hua Tian , Jian-Feng Li
With issues of energy security and environmental crisis intensifying, we urgently need to develop energy storage systems with high energy density and high safety. Zinc–air batteries have attracted extensive attention for their energy density, safety, and low cost, but problems with the zinc anode—such as hydrogen evolution, corrosion, passivation, dendrite proliferation, and deformation—have led to zinc–air batteries with low Coulombic efficiency and short cycle life; these remain the key obstacles hindering the batteries’ further development. In this review paper, we briefly describe the reaction mechanism of zinc–air batteries, then summarize the strategies for solving the key issues in zinc anodes. These approaches are divided into three aspects: structural designs for the zinc anode; interface engineering; and electrolyte selection and optimization. We finish by offering some suggestions for future research directions to improve the zinc anode in zinc–air batteries.
{"title":"Anode optimization strategies for zinc–air batteries","authors":"Ruo-Bei Huang , Meng-Yin Wang , Jian-Feng Xiong , Hua Zhang , Jing-Hua Tian , Jian-Feng Li","doi":"10.1016/j.esci.2024.100309","DOIUrl":"10.1016/j.esci.2024.100309","url":null,"abstract":"<div><div>With issues of energy security and environmental crisis intensifying, we urgently need to develop energy storage systems with high energy density and high safety. Zinc–air batteries have attracted extensive attention for their energy density, safety, and low cost, but problems with the zinc anode—such as hydrogen evolution, corrosion, passivation, dendrite proliferation, and deformation—have led to zinc–air batteries with low Coulombic efficiency and short cycle life; these remain the key obstacles hindering the batteries’ further development. In this review paper, we briefly describe the reaction mechanism of zinc–air batteries, then summarize the strategies for solving the key issues in zinc anodes. These approaches are divided into three aspects: structural designs for the zinc anode; interface engineering; and electrolyte selection and optimization. We finish by offering some suggestions for future research directions to improve the zinc anode in zinc–air batteries.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 3","pages":"Article 100309"},"PeriodicalIF":42.9,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143931431","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 : 2025-05-01Epub Date: 2024-10-22DOI: 10.1016/j.esci.2024.100330
Bo Liu , Zhibin Xu , Cong Wei , Zixuan Zhu , Yanyan Fang , Xin Lei , Ya Zhou , Chongyang Tang , Shiyi Ni , Hongge Pan , Gongming Wang
Interfacial H2 release severely limits the reversibility and feasibility of aqueous Zn metal batteries for large-scale energy storage. Different from the conventional perception that H2 release mainly originates from the competition between hydrogen evolution reaction and Zn plating process, we herein surprisingly find that non-negligible H2 is also generated during stripping due to the accelerated chemical corrosion of the newly exposed Zn surface. To address this issue, we systematically screened the organic additives with different molecular structures and functional groups. Interestingly, a positive correlation between the adsorption strength of additives and the ability to inhibit the interfacial hydrogen release is found. Taking cysteamine (MEA) as a model additive, a gradient solid electrolyte interphase (SEI) is in situ formed at the Zn surface, acting as a chemical “barrier” to isolate interfacial water molecules from electrode surface consequently enable a higher Coulombic efficiency (> 99.5%, 4000 cycles) compared with that of MEA-free electrolyte (98.1%, 189 cycles). This work provides a new understanding of the interfacial hydrogen release mechanism and the criteria for selecting additives for aqueous Zn metal anodes.
{"title":"Re-understanding and mitigating hydrogen release chemistry toward reversible aqueous zinc metal batteries","authors":"Bo Liu , Zhibin Xu , Cong Wei , Zixuan Zhu , Yanyan Fang , Xin Lei , Ya Zhou , Chongyang Tang , Shiyi Ni , Hongge Pan , Gongming Wang","doi":"10.1016/j.esci.2024.100330","DOIUrl":"10.1016/j.esci.2024.100330","url":null,"abstract":"<div><div>Interfacial H<sub>2</sub> release severely limits the reversibility and feasibility of aqueous Zn metal batteries for large-scale energy storage. Different from the conventional perception that H<sub>2</sub> release mainly originates from the competition between hydrogen evolution reaction and Zn plating process, we herein surprisingly find that non-negligible H<sub>2</sub> is also generated during stripping due to the accelerated chemical corrosion of the newly exposed Zn surface. To address this issue, we systematically screened the organic additives with different molecular structures and functional groups. Interestingly, a positive correlation between the adsorption strength of additives and the ability to inhibit the interfacial hydrogen release is found. Taking cysteamine (MEA) as a model additive, a gradient solid electrolyte interphase (SEI) is <em>in situ</em> formed at the Zn surface, acting as a chemical “barrier” to isolate interfacial water molecules from electrode surface consequently enable a higher Coulombic efficiency (> 99.5%, 4000 cycles) compared with that of MEA-free electrolyte (98.1%, 189 cycles). This work provides a new understanding of the interfacial hydrogen release mechanism and the criteria for selecting additives for aqueous Zn metal anodes.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 3","pages":"Article 100330"},"PeriodicalIF":42.9,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143931433","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 : 2025-05-01Epub Date: 2024-10-10DOI: 10.1016/j.esci.2024.100323
Yu Wang , Haijing Yan , Honggang Fu
Proton exchange membrane water electrolyzer (PEMWE) technology is regarded as one of the most promising methods for green hydrogen generation. The oxygen evolution reaction (OER) at the anode is the primary bottleneck preventing the industrial-scale application of PEMWEs due to its sluggish kinetics, and it presently relies upon electrocatalysts that use scarce, costly Ru and Ir. In addition, most of the Ru- and Ir-based electrocatalysts developed to date need high noble metal loading and present good activity only at low current density for a short period. In this review, we systematically elaborate upon various effective strategies for modulating Ru- and Ir-based catalysts to achieve large current density, high stability, and high atom economy, including single-atom designs, heteroatom doping, defect/vacancy creation, alloying, and heterojunction engineering. The structure–performance relationships of OER catalysts synthesized using different strategies are elucidated, along with the importance of substrate materials. We conclude by discussing the remaining challenges and future prospects for OER electrocatalysts in acid.
{"title":"Recent advances and modulation tactics in Ru- and Ir-based electrocatalysts for PEMWE anodes at large current densities","authors":"Yu Wang , Haijing Yan , Honggang Fu","doi":"10.1016/j.esci.2024.100323","DOIUrl":"10.1016/j.esci.2024.100323","url":null,"abstract":"<div><div>Proton exchange membrane water electrolyzer (PEMWE) technology is regarded as one of the most promising methods for green hydrogen generation. The oxygen evolution reaction (OER) at the anode is the primary bottleneck preventing the industrial-scale application of PEMWEs due to its sluggish kinetics, and it presently relies upon electrocatalysts that use scarce, costly Ru and Ir. In addition, most of the Ru- and Ir-based electrocatalysts developed to date need high noble metal loading and present good activity only at low current density for a short period. In this review, we systematically elaborate upon various effective strategies for modulating Ru- and Ir-based catalysts to achieve large current density, high stability, and high atom economy, including single-atom designs, heteroatom doping, defect/vacancy creation, alloying, and heterojunction engineering. The structure–performance relationships of OER catalysts synthesized using different strategies are elucidated, along with the importance of substrate materials. We conclude by discussing the remaining challenges and future prospects for OER electrocatalysts in acid.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 3","pages":"Article 100323"},"PeriodicalIF":42.9,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143931434","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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