Pub Date : 2025-05-01Epub Date: 2024-12-03DOI: 10.1016/j.esci.2024.100351
Ximei Lv , Jie Liu , Chenkun Li , Fengjiao Yu , Dengji Xiao , Shulin Zhao , Yuping Wu , Yuhui Chen
The solid electrolyte interphase (SEI) layer is crucial for lithium-ion batteries and has a significant impact on the electrochemical performance of negative electrodes, particularly for conversion-type materials with large volume changes and metallic lithium anode. However, the SEI layer has not yet been well understood. In this work, we used redox mediators of various sizes to probe the SEI layer that formed in carbonate-based electrolytes. The SEI layer has diffusion channels that allow the mediators smaller than benzoquinone (5.7 Å) to pass, suggesting that lithium ions have to partially de-solvate to pass through. Additionally, due to partial desolvation, the diffusion coefficient in the diffusion channels was higher than that in the bulk electrolytes. Both lithium salts and solvents influenced the size and areal density of channels. Herein, we aim to enhance comprehension of SEI structure and provide a method to study porous SEI layers using mediators, which can be extended to other electrochemical systems.
{"title":"Probing a solid electrolyte interphase layer with sub-nanometer pores using redox mediators","authors":"Ximei Lv , Jie Liu , Chenkun Li , Fengjiao Yu , Dengji Xiao , Shulin Zhao , Yuping Wu , Yuhui Chen","doi":"10.1016/j.esci.2024.100351","DOIUrl":"10.1016/j.esci.2024.100351","url":null,"abstract":"<div><div>The solid electrolyte interphase (SEI) layer is crucial for lithium-ion batteries and has a significant impact on the electrochemical performance of negative electrodes, particularly for conversion-type materials with large volume changes and metallic lithium anode. However, the SEI layer has not yet been well understood. In this work, we used redox mediators of various sizes to probe the SEI layer that formed in carbonate-based electrolytes. The SEI layer has diffusion channels that allow the mediators smaller than benzoquinone (5.7 Å) to pass, suggesting that lithium ions have to partially de-solvate to pass through. Additionally, due to partial desolvation, the diffusion coefficient in the diffusion channels was higher than that in the bulk electrolytes. Both lithium salts and solvents influenced the size and areal density of channels. Herein, we aim to enhance comprehension of SEI structure and provide a method to study porous SEI layers using mediators, which can be extended to other electrochemical systems.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 3","pages":"Article 100351"},"PeriodicalIF":42.9,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143931611","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: 2024-12-14DOI: 10.1016/j.esci.2024.100354
Jingzhao Cheng , Bei Cheng , Jingsan Xu , Jiaguo Yu , Shaowen Cao
Since the concept was introduced in 2019, step-scheme (S-scheme) heterojunctions have emerged as an important subclass of heterojunction technology and attracted much attention for solar energy conversion. S-scheme heterojunctions are capable of maximizing redox ability through conferring enhanced photocatalytic performance by addressing the problem of rapid electron–hole recombination. In particular, the organic–inorganic S-scheme heterojunction (OI-SHJ) can integrate atomic long-range ordered inorganic semiconductors with tailored organic materials using diverse organic molecular building blocks and integration methods, offering brilliant prospects for innovation. Here, we review the state-of-the-art progress in OI-SHJ photocatalysts by introducing their charge transfer mechanism, design criteria, preparation approaches, and applications. We also highlight the synergistic role of organic and inorganic materials in S-scheme heterojunctions and what is understood so far about their structure–activity relationship. We conclude by summarizing the existing challenges and emphasizing the current outlook for the future development of OI-SHJ photocatalysts.
{"title":"Organic–inorganic S-scheme heterojunction photocatalysts: Design, synthesis, applications, and challenges","authors":"Jingzhao Cheng , Bei Cheng , Jingsan Xu , Jiaguo Yu , Shaowen Cao","doi":"10.1016/j.esci.2024.100354","DOIUrl":"10.1016/j.esci.2024.100354","url":null,"abstract":"<div><div>Since the concept was introduced in 2019, step-scheme (S-scheme) heterojunctions have emerged as an important subclass of heterojunction technology and attracted much attention for solar energy conversion. S-scheme heterojunctions are capable of maximizing redox ability through conferring enhanced photocatalytic performance by addressing the problem of rapid electron–hole recombination. In particular, the organic–inorganic S-scheme heterojunction (OI-SHJ) can integrate atomic long-range ordered inorganic semiconductors with tailored organic materials using diverse organic molecular building blocks and integration methods, offering brilliant prospects for innovation. Here, we review the state-of-the-art progress in OI-SHJ photocatalysts by introducing their charge transfer mechanism, design criteria, preparation approaches, and applications. We also highlight the synergistic role of organic and inorganic materials in S-scheme heterojunctions and what is understood so far about their structure–activity relationship. We conclude by summarizing the existing challenges and emphasizing the current outlook for the future development of OI-SHJ photocatalysts.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 3","pages":"Article 100354"},"PeriodicalIF":42.9,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143931607","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}
Mobility, environmental adaptability, and functionality are essential attributes of robots, but these become challenging for small-scale on-water robots, also referred to as S-aquabots. Herein, we propose a programmable Marangoni motor (PM-motor) to propel centimeter-scale S-aquabots with high maneuverability and adaptability. Lightweight, compact, flexible hybrid electronics are used to precisely release ethanol to achieve controllable propulsion, smart sensing, and wireless communication functions. The PM-motor utilizes the surface tension gradient generated by the ethanol, which is released from leaf-inspired veins and improves fuel efficiency by 3.5 times when compared with traditional Marangoni effect-propelled robots. As a result, the device’s endurance is up to ∼226 s for a navigation distance of ∼5 m with just 1.2 mL ethanol. Benefiting from the leaf-like shape and negligible noise production, the S-aquabots can also blend well with their surroundings. Autonomous response capability is demonstrated by guiding an S-aquabot with laser spots to complete a butterfly-shaped trajectory. Equipped with a mini-camera or digital sensors, untethered S-aquabots deployed on an outdoor pool can capture real-time videos or monitor long-term environmental conditions. This work is beneficial for inspiring insightful design strategies to develop S-aquabots with high practical potential.
{"title":"Bio-inspired and programmable Marangoni motor for highly maneuverable and adaptable S-aquabots","authors":"Yexi Zhou , Xiao Guan , Dazhe Zhao , Kaijun Zhang , YongAn Huang , Junwen Zhong","doi":"10.1016/j.esci.2024.100335","DOIUrl":"10.1016/j.esci.2024.100335","url":null,"abstract":"<div><div>Mobility, environmental adaptability, and functionality are essential attributes of robots, but these become challenging for small-scale on-water robots, also referred to as S-aquabots. Herein, we propose a programmable Marangoni motor (PM-motor) to propel centimeter-scale S-aquabots with high maneuverability and adaptability. Lightweight, compact, flexible hybrid electronics are used to precisely release ethanol to achieve controllable propulsion, smart sensing, and wireless communication functions. The PM-motor utilizes the surface tension gradient generated by the ethanol, which is released from leaf-inspired veins and improves fuel efficiency by 3.5 times when compared with traditional Marangoni effect-propelled robots. As a result, the device’s endurance is up to ∼226 s for a navigation distance of ∼5 m with just 1.2 mL ethanol. Benefiting from the leaf-like shape and negligible noise production, the S-aquabots can also blend well with their surroundings. Autonomous response capability is demonstrated by guiding an S-aquabot with laser spots to complete a butterfly-shaped trajectory. Equipped with a mini-camera or digital sensors, untethered S-aquabots deployed on an outdoor pool can capture real-time videos or monitor long-term environmental conditions. This work is beneficial for inspiring insightful design strategies to develop S-aquabots with high practical potential.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 3","pages":"Article 100335"},"PeriodicalIF":42.9,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143931615","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: 2024-08-20DOI: 10.1016/j.esci.2024.100306
Juxia Xiong , Jiapeng Ji , Qiong Lei , Xinchun Yang , Yang Bai , Xiaolong Zhang , Hui-Ming Cheng
Converting CO2 into fuel or chemicals using renewable energy is a promising strategy for closing the anthropogenic carbon cycle. However, due to the highly stable C=O bond, CO2 activation requires a significant energy input to elevate the reactant to a higher energy state, plus an efficient catalyst to surmount the activation energy barrier. Despite significant advancements in catalytic methods using a single energy input for CO2 reduction, the catalytic efficiency and economic viability have yet to be improved. However, integrating multiple energy sources in catalysis has shown significant potential for improving catalytic efficiency. These energy-coupled systems demonstrate a synergistic effect, stemming from the multiple excitation modes of the reactants, the reaction intermediates, or even the catalysts. To our knowledge, there has not been a systematic review addressing synergetic energy-coupled catalysis for CO2 reduction. Herein, we aim to offer a comprehensive overview of recent advances in CO2 reduction driven by synergetic energy-coupled catalysis. Furthermore, we explore the technological challenges and prospects associated with the synergistic effect in energy-coupled catalytic systems, presenting our insights on potential breakthrough directions.
{"title":"Synergetic energy coupled thermal catalytic systems for CO2 reduction","authors":"Juxia Xiong , Jiapeng Ji , Qiong Lei , Xinchun Yang , Yang Bai , Xiaolong Zhang , Hui-Ming Cheng","doi":"10.1016/j.esci.2024.100306","DOIUrl":"10.1016/j.esci.2024.100306","url":null,"abstract":"<div><div>Converting CO<sub>2</sub> into fuel or chemicals using renewable energy is a promising strategy for closing the anthropogenic carbon cycle. However, due to the highly stable C=O bond, CO<sub>2</sub> activation requires a significant energy input to elevate the reactant to a higher energy state, plus an efficient catalyst to surmount the activation energy barrier. Despite significant advancements in catalytic methods using a single energy input for CO<sub>2</sub> reduction, the catalytic efficiency and economic viability have yet to be improved. However, integrating multiple energy sources in catalysis has shown significant potential for improving catalytic efficiency. These energy-coupled systems demonstrate a synergistic effect, stemming from the multiple excitation modes of the reactants, the reaction intermediates, or even the catalysts. To our knowledge, there has not been a systematic review addressing synergetic energy-coupled catalysis for CO<sub>2</sub> reduction. Herein, we aim to offer a comprehensive overview of recent advances in CO<sub>2</sub> reduction driven by synergetic energy-coupled catalysis. Furthermore, we explore the technological challenges and prospects associated with the synergistic effect in energy-coupled catalytic systems, presenting our insights on potential breakthrough directions.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 3","pages":"Article 100306"},"PeriodicalIF":42.9,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143931606","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: 2024-12-27DOI: 10.1016/j.esci.2024.100370
Zhaoqiang Wang , Guixiang Ding , Hongwei Huang , Juntao Zhang , Qi Lv , Li Shuai , Yonghao Ni , Guangfu Liao
Piezo-photocatalysis is capable of concerting mechanical vibration into chemical energy, portraying a promising alternative technology for H2O2 production. However, low mechanical energy conversion efficiency and constrained surface active sites hinder its practical application. Herein, ultrathin porous carbon nitride nanosheets with controlled carbon vacancies and oxygen doping (OCN-X, where X represents the calcination temperature) are synthesized by thermal oxidation etching to achieve unprecedented piezo-photocatalytic H2O2 production. The carbon vacancies and oxygen doping cause the formation of asymmetric structure of triazine unit with a strong dipole field, which creates spontaneous polarization field to speed up directional electron transfer to the nitrogen active sites for effective piezo-photocatalysis. Meanwhile, the ultrathin and porous structure formed by hot-oxygen etching enhances the mechanical energy conversion efficiency and collaboratively induces adsorbed oxygen via indirect two-electron oxygen reduction reaction (ORR) transfer pathway to effectively produce H2O2. Consequently, without any co-catalysts, the as-prepared OCN-460 displays record-high piezo-photocatalytic H2O2 production rate of 19.30 mmol g−1 h−1, far outdistancing those previously reported for piezo-photocatalysts. Furthermore, it also still maintains a notable piezo-photocatalytic activity of 2.87 mmol g−1 h−1 in the pure water system. This work offers some new insights for the future design of an effective piezo-photocatalytic H2O2 production system.
{"title":"Unraveling the dipole field in ultrathin, porous, and defective carbon nitride nanosheets for record-high piezo-photocatalytic H2O2 production","authors":"Zhaoqiang Wang , Guixiang Ding , Hongwei Huang , Juntao Zhang , Qi Lv , Li Shuai , Yonghao Ni , Guangfu Liao","doi":"10.1016/j.esci.2024.100370","DOIUrl":"10.1016/j.esci.2024.100370","url":null,"abstract":"<div><div>Piezo-photocatalysis is capable of concerting mechanical vibration into chemical energy, portraying a promising alternative technology for H<sub>2</sub>O<sub>2</sub> production. However, low mechanical energy conversion efficiency and constrained surface active sites hinder its practical application. Herein, ultrathin porous carbon nitride nanosheets with controlled carbon vacancies and oxygen doping (OCN-X, where X represents the calcination temperature) are synthesized by thermal oxidation etching to achieve unprecedented piezo-photocatalytic H<sub>2</sub>O<sub>2</sub> production. The carbon vacancies and oxygen doping cause the formation of asymmetric structure of triazine unit with a strong dipole field, which creates spontaneous polarization field to speed up directional electron transfer to the nitrogen active sites for effective piezo-photocatalysis. Meanwhile, the ultrathin and porous structure formed by hot-oxygen etching enhances the mechanical energy conversion efficiency and collaboratively induces adsorbed oxygen via indirect two-electron oxygen reduction reaction (ORR) transfer pathway to effectively produce H<sub>2</sub>O<sub>2</sub>. Consequently, without any co-catalysts, the as-prepared OCN-460 displays record-high piezo-photocatalytic H<sub>2</sub>O<sub>2</sub> production rate of 19.30 mmol g<sup>−1</sup> h<sup>−1</sup>, far outdistancing those previously reported for piezo-photocatalysts. Furthermore, it also still maintains a notable piezo-photocatalytic activity of 2.87 mmol g<sup>−1</sup> h<sup>−1</sup> in the pure water system. This work offers some new insights for the future design of an effective piezo-photocatalytic H<sub>2</sub>O<sub>2</sub> production system.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 3","pages":"Article 100370"},"PeriodicalIF":42.9,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143931614","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: 2024-12-27DOI: 10.1016/j.esci.2024.100369
Yang Li , Guining Shao , Xinyu Zheng , Yansong Jia , Yanghong Xia , Yuhai Dou , Ming Huang , Chaohua Gu , Jianfeng Shi , Jinyang Zheng , Shixue Dou
As an important component in electrochemical energy conversion and storage systems, electrochemical reactors (ECRs) are widely used for commodity chemical synthesis, including electrolytic H2 production, NH3 synthesis, and high-value CO2 utilization. However, ECRs pose challenges related to low energy efficiency and selectivity due to the low solubility of their gaseous reactants, slow kinetics, and limitations in mass transfer. It is thus imperative to develop advanced high-pressure (HP) ECRs to address these issues. In this review, we start by presenting a comprehensive analysis of the fundamental mechanisms of HP ECRs. Then, we summarize the state-of-the-art HP ECR applications for water electrolysis, the N2 reduction reaction, and the CO2 reduction reaction. We also demonstrate that mathematical simulations are valuable tools for digital validation and guidance to accelerate the design of better reactors. Finally, we make recommendations on developing relevant specifications and standards for the industrial application of HP ECRs.
{"title":"Cutting-edge advances in pressurized electrocatalytic reactors","authors":"Yang Li , Guining Shao , Xinyu Zheng , Yansong Jia , Yanghong Xia , Yuhai Dou , Ming Huang , Chaohua Gu , Jianfeng Shi , Jinyang Zheng , Shixue Dou","doi":"10.1016/j.esci.2024.100369","DOIUrl":"10.1016/j.esci.2024.100369","url":null,"abstract":"<div><div>As an important component in electrochemical energy conversion and storage systems, electrochemical reactors (ECRs) are widely used for commodity chemical synthesis, including electrolytic H<sub>2</sub> production, NH<sub>3</sub> synthesis, and high-value CO<sub>2</sub> utilization. However, ECRs pose challenges related to low energy efficiency and selectivity due to the low solubility of their gaseous reactants, slow kinetics, and limitations in mass transfer. It is thus imperative to develop advanced high-pressure (HP) ECRs to address these issues. In this review, we start by presenting a comprehensive analysis of the fundamental mechanisms of HP ECRs. Then, we summarize the state-of-the-art HP ECR applications for water electrolysis, the N<sub>2</sub> reduction reaction, and the CO<sub>2</sub> reduction reaction. We also demonstrate that mathematical simulations are valuable tools for digital validation and guidance to accelerate the design of better reactors. Finally, we make recommendations on developing relevant specifications and standards for the industrial application of HP ECRs.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 3","pages":"Article 100369"},"PeriodicalIF":42.9,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143931608","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: 2025-01-11DOI: 10.1016/j.esci.2025.100372
Jiabao Li , Jialong Duan , Chenlong Zhang , Ziting Qi , Ya Liu , Xingxing Duan , Yueji Liu , Jie Dou , Qiyao Guo , Benlin He , Yuanyuan Zhao , Peizhi Yang , Qunwei Tang
Persistent operation inevitably elevates the temperature of perovskite solar cells (PSCs), posing a challenge for maximizing their power output and stability even after effective defect passivation and encapsulation techniques have been implemented. Regulating the thermal conductivity of halide perovskites by additive engineering is now a mainstream strategy for achieving self-cooling devices, but our fundamental understanding of how perovskites with atomic disorder function remains insufficient. This theoretical study unveils the underlying mechanism of facet-dependent thermodynamic properties in mixed-cation perovskites. The results demonstrate that the (100) facet has higher thermal conductivity than the (110) and (111) facets. By carefully controlling the (100) crystallographic orientation through buried and bulk modification, the thermal conductivity of the target perovskite film can be increased from 1.005 to 1.068 W m−1 K−1, which lowers the PSC's equilibrium temperature 5.25 °C by accelerating heat transport and dissipation. Consequently, we achieve an inverted PSC with an excellent efficiency of 25.12%, accompanied by a significantly reduced temperature coefficient and better long-term stability: a conservation rate exceeding 90% after aging at 85 °C and exposure to persistent light irradiation for 1100 h. This work elucidates a previously unidentified outcome of crystal facet engineering: the achievement of thermal management in high-performance PSCs.
持续工作不可避免地会提高钙钛矿太阳能电池（PSCs）的温度，即使在实施了有效的缺陷钝化和封装技术之后，也对其功率输出和稳定性的最大化提出了挑战。通过增材工程调节卤化物钙钛矿的热导率是目前实现自冷器件的主流策略，但我们对具有原子无序功能的钙钛矿的基本理解仍然不足。这一理论研究揭示了混合阳离子钙钛矿的面依赖热力学性质的潜在机制。结果表明，（100）面的导热系数高于（110）和（111）面的导热系数。通过埋埋改性和块状改性控制（100）晶体取向，可以将目标钙钛矿膜的导热系数从1.005提高到1.068 W m−1 K−1，通过加速热传递和耗散，降低PSC的平衡温度5.25℃。因此，我们实现了倒置的PSC，效率为25.12%，同时温度系数显著降低，长期稳定性更好：在85°C老化和持续光照1100小时后，保存率超过90%。这项工作阐明了以前未确定的晶体面工程的结果：实现高性能psc的热管理。
{"title":"Facet-orientation-enhanced thermal transfer for temperature-insensitive and stable p-i-n perovskite solar cells","authors":"Jiabao Li , Jialong Duan , Chenlong Zhang , Ziting Qi , Ya Liu , Xingxing Duan , Yueji Liu , Jie Dou , Qiyao Guo , Benlin He , Yuanyuan Zhao , Peizhi Yang , Qunwei Tang","doi":"10.1016/j.esci.2025.100372","DOIUrl":"10.1016/j.esci.2025.100372","url":null,"abstract":"<div><div>Persistent operation inevitably elevates the temperature of perovskite solar cells (PSCs), posing a challenge for maximizing their power output and stability even after effective defect passivation and encapsulation techniques have been implemented. Regulating the thermal conductivity of halide perovskites by additive engineering is now a mainstream strategy for achieving self-cooling devices, but our fundamental understanding of how perovskites with atomic disorder function remains insufficient. This theoretical study unveils the underlying mechanism of facet-dependent thermodynamic properties in mixed-cation perovskites. The results demonstrate that the (100) facet has higher thermal conductivity than the (110) and (111) facets. By carefully controlling the (100) crystallographic orientation through buried and bulk modification, the thermal conductivity of the target perovskite film can be increased from 1.005 to 1.068 W m<sup>−1</sup> K<sup>−1</sup>, which lowers the PSC's equilibrium temperature 5.25 °C by accelerating heat transport and dissipation. Consequently, we achieve an inverted PSC with an excellent efficiency of 25.12%, accompanied by a significantly reduced temperature coefficient and better long-term stability: a conservation rate exceeding 90% after aging at 85 °C and exposure to persistent light irradiation for 1100 h. This work elucidates a previously unidentified outcome of crystal facet engineering: the achievement of thermal management in high-performance PSCs.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 3","pages":"Article 100372"},"PeriodicalIF":42.9,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143931612","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: 2024-11-30DOI: 10.1016/j.esci.2024.100350
Junchao Yu , Zichao Xi , Jinhui Su , Peng Jing , Xuan Xu , Baocang Liu , Yu Wang , Jun Zhang
Electrochemical nitrate reduction reaction in alkaline condition involves two reactants, the nitrate () and the water (H2O). Although the significance of the active ∗H species produced from the dissociation of H2O has been proved, the correlation between the reaction pathways and the ∗H species is often overlooked. Herein, Co(OH)2–CoP supported Ru nanoclusters is designed for electrocatalytic nitrate reduction and shows a record-high faradaic efficiency of 99.7% at an ultralow potential of 0.1 V versus reversible hydrogen electrode. Experiments and theoretical calculations reveal that in addition to the faster proton transfer kinetics, the reaction pathway is strongly correlated with ∗H supply with the aid of CoP, that is, the direct hydrogenation of ∗NOH instead of deprotonation over Ru sites with the lowest energy barrier is promoted with the moderate production of ∗H species. This work provides new insights into the impact of ∗H species on the thermodynamics and kinetics of electrocatalytic nitrate reduction.
{"title":"Influence of active hydrogen on pathway selection in electrochemical nitrate reduction","authors":"Junchao Yu , Zichao Xi , Jinhui Su , Peng Jing , Xuan Xu , Baocang Liu , Yu Wang , Jun Zhang","doi":"10.1016/j.esci.2024.100350","DOIUrl":"10.1016/j.esci.2024.100350","url":null,"abstract":"<div><div>Electrochemical nitrate reduction reaction in alkaline condition involves two reactants, the nitrate (<span><math><mrow><msup><msub><mtext>NO</mtext><mn>3</mn></msub><mo>−</mo></msup></mrow></math></span>) and the water (H<sub>2</sub>O). Although the significance of the active ∗H species produced from the dissociation of H<sub>2</sub>O has been proved, the correlation between the reaction pathways and the ∗H species is often overlooked. Herein, Co(OH)<sub>2</sub>–CoP supported Ru nanoclusters is designed for electrocatalytic nitrate reduction and shows a record-high faradaic efficiency of 99.7% at an ultralow potential of 0.1 V versus reversible hydrogen electrode. Experiments and theoretical calculations reveal that in addition to the faster proton transfer kinetics, the reaction pathway is strongly correlated with ∗H supply with the aid of CoP, that is, the direct hydrogenation of ∗NOH instead of deprotonation over Ru sites with the lowest energy barrier is promoted with the moderate production of ∗H species. This work provides new insights into the impact of ∗H species on the thermodynamics and kinetics of electrocatalytic nitrate reduction.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 3","pages":"Article 100350"},"PeriodicalIF":42.9,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143931610","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: 2025-01-13DOI: 10.1016/j.esci.2025.100371
Chun Wu , Wenjie Huang , Yinghao Zhang , Qinghang Chen , Li Li , Yajun Zhang , Xingqiao Wu , Shu-Lei Chou
Hard carbon (HC) anodes in sodium-ion batteries (SIBs) are prized for their high capacity, durability, cost-efficiency, environmental sustainability, and safety. The metallic ash elements in HCs inevitably affect the overall performance of SIBs, however, the unclear role of metallic ash elements during carbonization and the electrochemical sodium storage process presents challenges for advancing HC design concepts. In this review, the traditional role of metallic ash element realized in the past and the deep understanding by a new sight from the view of intrinsic types in precursor matrix are initially introduced. Subsequently, the effect of catalyzing graphitization degree, constructing pore structure, tuning SEI formation and tailoring defects of the HCs regulated by extrinsic factors introduced through experimental conditions in recent years are comprehensively summarized. Additionally, future development prospects and perspectives on the research about metallic ash element in HC are also briefly outlined. It is believed that this review can deliver noteworthy viewpoints by introducing metallic ash elements, for the continued development of adjusting the microstructure of HCs at the nanoscale to actualize high-performance SIBs.
{"title":"Revisiting the critical role of metallic ash elements in the development of hard carbon for advancing sodium-ion battery applications","authors":"Chun Wu , Wenjie Huang , Yinghao Zhang , Qinghang Chen , Li Li , Yajun Zhang , Xingqiao Wu , Shu-Lei Chou","doi":"10.1016/j.esci.2025.100371","DOIUrl":"10.1016/j.esci.2025.100371","url":null,"abstract":"<div><div>Hard carbon (HC) anodes in sodium-ion batteries (SIBs) are prized for their high capacity, durability, cost-efficiency, environmental sustainability, and safety. The metallic ash elements in HCs inevitably affect the overall performance of SIBs, however, the unclear role of metallic ash elements during carbonization and the electrochemical sodium storage process presents challenges for advancing HC design concepts. In this review, the traditional role of metallic ash element realized in the past and the deep understanding by a new sight from the view of intrinsic types in precursor matrix are initially introduced. Subsequently, the effect of catalyzing graphitization degree, constructing pore structure, tuning SEI formation and tailoring defects of the HCs regulated by extrinsic factors introduced through experimental conditions in recent years are comprehensively summarized. Additionally, future development prospects and perspectives on the research about metallic ash element in HC are also briefly outlined. It is believed that this review can deliver noteworthy viewpoints by introducing metallic ash elements, for the continued development of adjusting the microstructure of HCs at the nanoscale to actualize high-performance SIBs.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 3","pages":"Article 100371"},"PeriodicalIF":42.9,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143931432","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 : 2025-03-01Epub Date: 2024-04-15DOI: 10.1016/j.esci.2024.100270
Xuan Liu , Gang Wu , Qing Li
Platinum group metal (PGM) electrocatalysts play an irreplaceable role in many electrochemical reactions for sustainable energy conversion. In the past few decades, the electronic orbital modulation methods have emerged as an important way to produce high-performance electrocatalysts, often by adjusting surface reactivity and enhancing structural stability. In this review, we first systematically elaborate on the basic principles and strategies of orbital modulation for PGM-based catalysts, mainly from the perspective of improving activity and stability, in which we highlight some exploratory theoretical studies over the past few decades. Then we describe a series of representative works to elucidate the specific approaches used to realize precise orbital modulation in PGM catalysts. Finally, we clarify the existing challenges and propose some perspectives for the development of related theories and practical applications.
{"title":"Orbital modulation in platinum-group-metal (PGM) electrocatalysts: An effective approach to boost catalytic performance","authors":"Xuan Liu , Gang Wu , Qing Li","doi":"10.1016/j.esci.2024.100270","DOIUrl":"10.1016/j.esci.2024.100270","url":null,"abstract":"<div><div>Platinum group metal (PGM) electrocatalysts play an irreplaceable role in many electrochemical reactions for sustainable energy conversion. In the past few decades, the electronic orbital modulation methods have emerged as an important way to produce high-performance electrocatalysts, often by adjusting surface reactivity and enhancing structural stability. In this review, we first systematically elaborate on the basic principles and strategies of orbital modulation for PGM-based catalysts, mainly from the perspective of improving activity and stability, in which we highlight some exploratory theoretical studies over the past few decades. Then we describe a series of representative works to elucidate the specific approaches used to realize precise orbital modulation in PGM catalysts. Finally, we clarify the existing challenges and propose some perspectives for the development of related theories and practical applications.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 2","pages":"Article 100270"},"PeriodicalIF":42.9,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140795924","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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