Pub Date : 2025-02-01DOI: 10.1016/j.nanoen.2024.110564
Shuhan Qiang , Zhiyong Li , Siqi He , Hu Zhou , Yu Zhang , Xia Cao , Aihua Yuan , Jiasheng Zou , Jianchun Wu , Yanxin Qiao
To rationally fabricate efficient nonprecious-metal electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is essential for developing the sustainable electrolytic water system but still remain a great challenge. The Fe-doped CoS2 (Fe-CoS2) nanorods are proposed and synthesized in this work by a heteroatomic doping strategy. Compared with single CoS2 and FeS2, the Fe-CoS2 catalyst requires an overpotential of 217 mV for HER and 280 mV for OER at 10 mA cm−2, along with a robust durability in alkaline electrolyte. Remarkably, the water electrolytic cell assembled with Fe-CoS2 delivers a voltage of 1.62 V at 10 mA cm−2. Experimental characterizations and theoretical calculations cooperatively reveal that the promoted bifunctional catalytic performances of Fe-CoS2 can be ascribed to the intriguing nanorod-like morphology and the modulation of electronic structure. This work not only highlights the heteroatom doping strategy to regulate the electronic structure, but also offers a straightforward protocol for constructing advanced metal sulfides as bifunctional electrocatalysts for overall water splitting.
合理制备高效的析氢、析氧非贵金属电催化剂是发展可持续电解水系统的必要条件，但仍是一个巨大的挑战。本文采用杂原子掺杂策略合成了Fe-CoS2 （Fe-CoS2）纳米棒。与单一的CoS2和FeS2相比，Fe-CoS2催化剂在10 mA cm-2下的HER过电位为217 mV， OER过电位为280 mV，并且在碱性电解质中具有较强的耐久性。值得注意的是，用Fe-CoS2组装的水电解池在10 mA cm-2时可提供1.62 V的电压。实验表征和理论计算共同表明，Fe-CoS2的双功能催化性能的提高可归因于其纳米棒状的形态和电子结构的调制。这项工作不仅突出了杂原子掺杂策略来调节电子结构，而且为构建先进的金属硫化物作为双功能电催化剂来全面分解水提供了一个简单的方案。
{"title":"Modulating electronic structure of CoS2 nanorods by Fe doping for efficient electrocatalytic overall water splitting","authors":"Shuhan Qiang , Zhiyong Li , Siqi He , Hu Zhou , Yu Zhang , Xia Cao , Aihua Yuan , Jiasheng Zou , Jianchun Wu , Yanxin Qiao","doi":"10.1016/j.nanoen.2024.110564","DOIUrl":"10.1016/j.nanoen.2024.110564","url":null,"abstract":"<div><div>To rationally fabricate efficient nonprecious-metal electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is essential for developing the sustainable electrolytic water system but still remain a great challenge. The Fe-doped CoS<sub>2</sub> (Fe-CoS<sub>2</sub>) nanorods are proposed and synthesized in this work by a heteroatomic doping strategy. Compared with single CoS<sub>2</sub> and FeS<sub>2</sub>, the Fe-CoS<sub>2</sub> catalyst requires an overpotential of 217 mV for HER and 280 mV for OER at 10 mA cm<sup>−2</sup>, along with a robust durability in alkaline electrolyte. Remarkably, the water electrolytic cell assembled with Fe-CoS<sub>2</sub> delivers a voltage of 1.62 V at 10 mA cm<sup>−2</sup>. Experimental characterizations and theoretical calculations cooperatively reveal that the promoted bifunctional catalytic performances of Fe-CoS<sub>2</sub> can be ascribed to the intriguing nanorod-like morphology and the modulation of electronic structure. This work not only highlights the heteroatom doping strategy to regulate the electronic structure, but also offers a straightforward protocol for constructing advanced metal sulfides as bifunctional electrocatalysts for overall water splitting.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"134 ","pages":"Article 110564"},"PeriodicalIF":16.8,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797499","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.nanoen.2024.110562
Lingyi Liao, Qingsong Mei, Zihao Chen, Yuqi Peng, Yuanyuan Tan
Contact electrification (CE) is known as the charge transfer between two surfaces upon contacting and separating, which has been exploited for the development of triboelectric nanogenerator (TENG). It is generally understood that CE is dependent on the difference of the charge affinity of dissimilar polymers, which is considered as an intrinsic property of polymers, i.e., CE is expected to be minor between identical materials. Here, abnormally evident CE behavior between identical polymers that are subjected to mechanical deformation (MD) to the plastic strain level is observed. Meanwhile, a unique correlation between the dynamic variation of coefficient of friction and friction electrification output is revealed as a result of the MD effect on CE. Analysis demonstrates that the observed MD effect on CE can be attributed to the strain-induced reconstruction of molecular structures of polymers. The present results indicate that CE/TENG is highly prone to the dynamic structure evolutions induced by contact-separation/friction, providing a new perspective to understand the intrinsic correlation between friction and CE behaviors between materials, as well as a potential way to modulate CE by MD.
{"title":"Abnormal contact electrification induced by mechanical deformation between identical materials","authors":"Lingyi Liao, Qingsong Mei, Zihao Chen, Yuqi Peng, Yuanyuan Tan","doi":"10.1016/j.nanoen.2024.110562","DOIUrl":"10.1016/j.nanoen.2024.110562","url":null,"abstract":"<div><div>Contact electrification (CE) is known as the charge transfer between two surfaces upon contacting and separating, which has been exploited for the development of triboelectric nanogenerator (TENG). It is generally understood that CE is dependent on the difference of the charge affinity of dissimilar polymers, which is considered as an intrinsic property of polymers, i.e., CE is expected to be minor between identical materials. Here, abnormally evident CE behavior between identical polymers that are subjected to mechanical deformation (MD) to the plastic strain level is observed. Meanwhile, a unique correlation between the dynamic variation of coefficient of friction and friction electrification output is revealed as a result of the MD effect on CE. Analysis demonstrates that the observed MD effect on CE can be attributed to the strain-induced reconstruction of molecular structures of polymers. The present results indicate that CE/TENG is highly prone to the dynamic structure evolutions induced by contact-separation/friction, providing a new perspective to understand the intrinsic correlation between friction and CE behaviors between materials, as well as a potential way to modulate CE by MD.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"134 ","pages":"Article 110562"},"PeriodicalIF":16.8,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793262","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.nanoen.2024.110543
Zihao Zhai , Jieyi Chen , Xiang Li , Qingyue Jiang , Jie Bao , Yongqi Wang , Qi Liu , Yufang Li , Xuemei Li
Integration of solar steam production and water-evaporation-induced electricity generation has become a promising strategy to optimize the existing water-energy nexus. However, owing to the different requirement of material design for water management, satisfying solar steam and water-evaporation-induced electricity cogeneration at high efficiency with a facile and controllable material construction still faces a great challenge. Herein, oxygen-doped vertical graphene (OVG), which possesses vertical structure with high light absorption and abundant nanoconfined channels, was directly deposited on macroporous carbon cloth (CC) by plasma-enhanced chemical vapor deposition (PECVD) to induce strong electrokinetic effect and ensure rapid water evaporation. The creative OVG/CC with different conformal graphene skinned was controllably constructed in PECVD system with the change of deposition temperature and the aid of in-situ carbon-dioxide plasma post-treatment. Benefited from the favorable structure prepared at 800 ℃ with intense light absorption on surface and strong electrical interaction at solid-water interface, the OVG/CC-based device presented efficient outputs with an evaporation rate of 2.78 kg m−2 h−1, a voltage of 0.75 V and a current of 2.67 μA in DI water, and with an evaporation rate of 2.69 kg m−2 h−1, a voltage of 0.52 V and a current of 24.11 μA in real seawater respectively, accompanied with the good cycling stability and long-term durability. Moreover, the device could also purify various water sources and drive electron components for practical applications. This work provides a promising CVD strategy for constructing carbon-based composite materials toward efficient clean water and electricity cogeneration.
太阳能蒸汽生产和水蒸发发电的整合已成为优化现有水能关系的一种有前途的策略。然而，由于水管理对材料设计的不同要求，用一种易于控制的材料结构来满足太阳能蒸汽和水蒸发发电的高效热电联产仍然面临着很大的挑战。本文采用等离子体增强化学气相沉积（PECVD）技术将垂直结构、高光吸收和丰富纳米限制通道的氧掺杂垂直石墨烯（OVG）直接沉积在大孔碳布（CC）上，以诱导强电动力学效应并保证水分快速蒸发。通过改变沉积温度和原位二氧化碳等离子后处理，在PECVD系统中可控地构建了具有不同适形石墨烯表皮的创新型OVG/CC。基于OVG/ cc的器件在800℃下制备的良好结构，具有表面强光吸收和固水界面强电相互作用，在去离子水中蒸发量为2.78 kg m-2 h-1，电压为0.75 V，电流为2.67 μA，在真实海水中蒸发量为2.69 kg m-2 h-1，电压为0.52 V，电流为24.11 μA。具有良好的循环稳定性和长期耐用性。此外，该装置还可以净化各种水源和驱动电子元件，具有实际应用价值。这项工作为构建高效清洁水和电热电联产的碳基复合材料提供了一种有前途的CVD策略。
{"title":"PECVD-derived oxygen-doped vertical graphene-skinned carbon cloth toward efficient solar steam and water-evaporation-induced electricity cogeneration","authors":"Zihao Zhai , Jieyi Chen , Xiang Li , Qingyue Jiang , Jie Bao , Yongqi Wang , Qi Liu , Yufang Li , Xuemei Li","doi":"10.1016/j.nanoen.2024.110543","DOIUrl":"10.1016/j.nanoen.2024.110543","url":null,"abstract":"<div><div>Integration of solar steam production and water-evaporation-induced electricity generation has become a promising strategy to optimize the existing water-energy nexus. However, owing to the different requirement of material design for water management, satisfying solar steam and water-evaporation-induced electricity cogeneration at high efficiency with a facile and controllable material construction still faces a great challenge. Herein, oxygen-doped vertical graphene (OVG), which possesses vertical structure with high light absorption and abundant nanoconfined channels, was directly deposited on macroporous carbon cloth (CC) by plasma-enhanced chemical vapor deposition (PECVD) to induce strong electrokinetic effect and ensure rapid water evaporation. The creative OVG/CC with different conformal graphene skinned was controllably constructed in PECVD system with the change of deposition temperature and the aid of in-situ carbon-dioxide plasma post-treatment. Benefited from the favorable structure prepared at 800 ℃ with intense light absorption on surface and strong electrical interaction at solid-water interface, the OVG/CC-based device presented efficient outputs with an evaporation rate of 2.78 kg m<sup>−2</sup> h<sup>−1</sup>, a voltage of 0.75 V and a current of 2.67 μA in DI water, and with an evaporation rate of 2.69 kg m<sup>−2</sup> h<sup>−1</sup>, a voltage of 0.52 V and a current of 24.11 μA in real seawater respectively, accompanied with the good cycling stability and long-term durability. Moreover, the device could also purify various water sources and drive electron components for practical applications. This work provides a promising CVD strategy for constructing carbon-based composite materials toward efficient clean water and electricity cogeneration.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"134 ","pages":"Article 110543"},"PeriodicalIF":16.8,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793263","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.nanoen.2024.110561
Zhenhui Jin , Yang Fu , Hongfa Zhao , Wenbo Ding , Yi-Cheng Wang
Humidity can significantly impact the quality of food. In the case of low-moisture foods – a category characterized by its low water activity – humidity can cause undesirable physical and chemical changes. In this study, we developed intelligent packaging for such foods based around versatile triboelectric nanogenerators (TENGs) that incorporated triboelectric layers fabricated from a carbohydrate polymer, pectin, and glycerol. We found that such TENGs generated their highest electrical output, making them suitable for use as energy harvesters, when the glycerol content of such a layer was 70 % of its pectin content. We further demonstrated that such energy harvesters could successfully convert mechanical energy into sufficient electricity to power small electronic devices such as a hygrometer and a calculator. However, when the pectin-containing triboelectric layer’s glycerol content was reduced to 50 % of its pectin content, the resulting TENG-based sensors exhibited distinctive behaviors during sorption and desorption processes. Those behaviors were leveraged to create a triboelectric food-quality sensor (TFQS) that we integrated into food packaging for food-quality monitoring. Testing of the TFQS indicated that it could effectively measure a key quality attribute, hardness, of our target low-moisture food, crackers. These findings illustrated not only how altering their compositions can endow triboelectric devices with multifunctionality, but also such devices’ potential to help reduce food waste by providing consumers with accurate, dynamic quality information. As such, they could address a core limitation of the current pre-printed food-date label system, which does not account for storage conditions.
{"title":"Carbohydrate polymer-based triboelectric devices for energy harvesting and intelligent packaging for food-quality monitoring","authors":"Zhenhui Jin , Yang Fu , Hongfa Zhao , Wenbo Ding , Yi-Cheng Wang","doi":"10.1016/j.nanoen.2024.110561","DOIUrl":"10.1016/j.nanoen.2024.110561","url":null,"abstract":"<div><div>Humidity can significantly impact the quality of food. In the case of low-moisture foods – a category characterized by its low water activity – humidity can cause undesirable physical and chemical changes. In this study, we developed intelligent packaging for such foods based around versatile triboelectric nanogenerators (TENGs) that incorporated triboelectric layers fabricated from a carbohydrate polymer, pectin, and glycerol. We found that such TENGs generated their highest electrical output, making them suitable for use as energy harvesters, when the glycerol content of such a layer was 70 % of its pectin content. We further demonstrated that such energy harvesters could successfully convert mechanical energy into sufficient electricity to power small electronic devices such as a hygrometer and a calculator. However, when the pectin-containing triboelectric layer’s glycerol content was reduced to 50 % of its pectin content, the resulting TENG-based sensors exhibited distinctive behaviors during sorption and desorption processes. Those behaviors were leveraged to create a triboelectric food-quality sensor (TFQS) that we integrated into food packaging for food-quality monitoring. Testing of the TFQS indicated that it could effectively measure a key quality attribute, hardness, of our target low-moisture food, crackers. These findings illustrated not only how altering their compositions can endow triboelectric devices with multifunctionality, but also such devices’ potential to help reduce food waste by providing consumers with accurate, dynamic quality information. As such, they could address a core limitation of the current pre-printed food-date label system, which does not account for storage conditions.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"134 ","pages":"Article 110561"},"PeriodicalIF":16.8,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797501","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.nanoen.2024.110589
Pan An , Yujia Lv , Hao Xiu , Jingyi Chen , Panxing Ren , Yuan Bai , Chuanchao Tao , Chang Ao , Chunhao Yang , Jiaxing Wu , Dan Luo , Yajun Wang
Photoelectrocatalysis, an advanced oxidation method that combines photocatalysis and electrochemistry, typically requires substantial external energy. This study introduces a hybrid approach that combines efficient semiconductor light-harvesting with the superior energy collection and conversion capabilities of a self-powered system. We enhanced visible light absorption in a Cu2O/Bi2MoO6 photoanode using a type-II heterojunction structure. A triboelectric-electromagnetic nanogenerator (TENG-EMG) acts as a self-powered energy source, promoting electron and hole separation during the photoelectrocatalytic process. The empirical results show that under light irradiation, electrons move from Cu2O to Bi2MoO6, whereas holes move in opposite directions. As the TENG-EMG rotational speed increased from 100 to 400 r/min, the tetracycline hydrochloride (TCH) degradation rate of the TENG-EMG-Cu2O/Bi2MoO6 system increased from 49.2 % to 92.4 %. The use of the TENG-EMGs significantly enhanced the efficacy of organic wastewater treatment. This paper presents a new, eco-friendly, and cost-effective method for wastewater treatment that combines self-powered advanced oxidation technology with a TENG-EMG and a heterojunction photoanode.
{"title":"Triboelectric-electromagnetic nanogenerator coupled type-II heterojunction enhancing photoelectrocatalysis for wastewater degradation","authors":"Pan An , Yujia Lv , Hao Xiu , Jingyi Chen , Panxing Ren , Yuan Bai , Chuanchao Tao , Chang Ao , Chunhao Yang , Jiaxing Wu , Dan Luo , Yajun Wang","doi":"10.1016/j.nanoen.2024.110589","DOIUrl":"10.1016/j.nanoen.2024.110589","url":null,"abstract":"<div><div>Photoelectrocatalysis, an advanced oxidation method that combines photocatalysis and electrochemistry, typically requires substantial external energy. This study introduces a hybrid approach that combines efficient semiconductor light-harvesting with the superior energy collection and conversion capabilities of a self-powered system. We enhanced visible light absorption in a Cu<sub>2</sub>O/Bi<sub>2</sub>MoO<sub>6</sub> photoanode using a type-II heterojunction structure. A triboelectric-electromagnetic nanogenerator (TENG-EMG) acts as a self-powered energy source, promoting electron and hole separation during the photoelectrocatalytic process. The empirical results show that under light irradiation, electrons move from Cu<sub>2</sub>O to Bi<sub>2</sub>MoO<sub>6</sub>, whereas holes move in opposite directions. As the TENG-EMG rotational speed increased from 100 to 400 r/min, the tetracycline hydrochloride (TCH) degradation rate of the TENG-EMG-Cu<sub>2</sub>O/Bi<sub>2</sub>MoO<sub>6</sub> system increased from 49.2 % to 92.4 %. The use of the TENG-EMGs significantly enhanced the efficacy of organic wastewater treatment. This paper presents a new, eco-friendly, and cost-effective method for wastewater treatment that combines self-powered advanced oxidation technology with a TENG-EMG and a heterojunction photoanode.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"134 ","pages":"Article 110589"},"PeriodicalIF":16.8,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142823094","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.nanoen.2024.110535
Fobao Huang , Yong Chao , Qingyuan Yang , Minjiang Dan , Qiao Chen , Gongwei Hu , Wei Huang
Piezotronic strain sensors that convert mechanical deformation into electrical signals are becoming increasingly important in artificial intelligence, human-machine interfaces, and robotic technologies. These applications require piezotronic sensor with the integration of high-sensitivity, high-stability, and versatile-functionality, which are limited by the single conductivity mechanism. In this study, we propose a piezotronic strain sensor with uniform and switchable sensitivity in a short channel field-effect junction. The strain-induced piezo-potential can be used to switch the conductivity between Schottky and Ohmic regime, leading to an exponential (linear) piezotronic modulation in Schottky (Ohmic) conductivity elucidated by Fermi occupation theory. Local gauge factor reaches a high value of 1330 in Schottky conductivity and a low value of 320 in Ohmic regime, yielding a higher ratio of 4.2. The stable conductivity makes these high and low sensitivity uniform over a wide strain range. This study gives a deep insight into the correlation of strain-sensing performance and conductive mechanism in piezotronic sensors, and offers a new avenue to develop multifunctional and high-sensitivity sensors.
{"title":"Piezotronic strain sensor with uniform and switchable sensitivity by conductivity transformation","authors":"Fobao Huang , Yong Chao , Qingyuan Yang , Minjiang Dan , Qiao Chen , Gongwei Hu , Wei Huang","doi":"10.1016/j.nanoen.2024.110535","DOIUrl":"10.1016/j.nanoen.2024.110535","url":null,"abstract":"<div><div>Piezotronic strain sensors that convert mechanical deformation into electrical signals are becoming increasingly important in artificial intelligence, human-machine interfaces, and robotic technologies. These applications require piezotronic sensor with the integration of high-sensitivity, high-stability, and versatile-functionality, which are limited by the single conductivity mechanism. In this study, we propose a piezotronic strain sensor with uniform and switchable sensitivity in a short channel field-effect junction. The strain-induced piezo-potential can be used to switch the conductivity between Schottky and Ohmic regime, leading to an exponential (linear) piezotronic modulation in Schottky (Ohmic) conductivity elucidated by Fermi occupation theory. Local gauge factor reaches a high value of 1330 in Schottky conductivity and a low value of 320 in Ohmic regime, yielding a higher ratio of 4.2. The stable conductivity makes these high and low sensitivity uniform over a wide strain range. This study gives a deep insight into the correlation of strain-sensing performance and conductive mechanism in piezotronic sensors, and offers a new avenue to develop multifunctional and high-sensitivity sensors.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"134 ","pages":"Article 110535"},"PeriodicalIF":16.8,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142777206","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Li-rich Mn-based layered oxides (LLOs) are promising cathode materials due to their high capacity derived from the unique cation and anion redox couples. However, the poor cycling stability and drastic voltage decay impede their practical application. Despite the covalency theory is proposed to understand the redox activity of LLOs, comprehensive design guidelines are still lacking. Inspired by the covalency theory of polyanion cathodes, high-performance LLOs are developed through an in-situ surface reconstruction strategy of near-surface doping and surface coating. Density function theory (DFT) calculations show that through the introduction of Ni2+ and PO43-, the energy bands of the transition metal (TM) 3d-O 2p and non-bonding O-2p shift to lower energy, resulting in the elevated working potential, reduced activity of lattice oxygen, and enhanced reversibility of redox oxygen. Meanwhile, the Li3PO4 coating can prevent electrolyte corrosion and mitigate surface degradation of LLOs upon cycling. As a result, the capacity retention of the modified LLOs is increased from 35.9 % to 77 %, and the voltage retention is raised from 68.6 % to 75.1 % after 700 cycles at 1 C. Furthermore, at 55 °C the capacity retention of the modified LLOs is also elevated from 32.1 % to 85.9 %, and the voltage retention is improved from 67.9 % to 82.3 % after 120 cycles at 1 C. The proposed strategy could advance the application of high-performance LLOs and their high-energy-density Li-ion batteries.
富锂锰基层状氧化物（LLOs）由于其独特的阳离子和阴离子氧化还原对而产生的高容量，是一种很有前途的正极材料。然而，循环稳定性差和电压衰减剧烈阻碍了它们的实际应用。尽管提出了共价理论来理解LLOs的氧化还原活性，但仍然缺乏全面的设计指南。受聚阴离子阴极共价理论的启发，通过近表面掺杂和表面涂层的原位表面重建策略，开发了高性能的LLOs。密度泛函理论（DFT）计算表明，通过Ni2+和PO43-的引入，过渡金属（TM） 3d-O -2p和非成键O-2p的能带向较低能量转移，导致工作电位升高，晶格氧活度降低，氧化还原氧的可逆性增强。同时，Li3PO4涂层可以防止电解液的腐蚀，减轻LLOs在循环过程中的表面降解。结果,能力保留修改LLOs从35.9%上升到77%,与电压保留从68.6%提高到75.1%,700年周期在1 c。此外,在55摄氏度的能力保留修改LLOs也从32.1%升高到85.9%,保留从67.9%提高到82.3%,电压在1 c . 120次后提出的策略可以促进高性能LLOs和高能量密度锂离子电池的应用。
{"title":"Tailoring redox couples of Li-rich Mn-based cathode materials by in-situ surface reconstruction for high-performance lithium-ion batteries","authors":"Xutao Zhu, Xujia Xie, Jie Lin, Yuanyuan Liu, Guiyang Gao, Yong Yang, Yinggan Zhang, Weicheng Xiong, Yidi Jiang, Qiyuan Li, Dong-Liang Peng","doi":"10.1016/j.nanoen.2024.110588","DOIUrl":"10.1016/j.nanoen.2024.110588","url":null,"abstract":"<div><div>Li-rich Mn-based layered oxides (LLOs) are promising cathode materials due to their high capacity derived from the unique cation and anion redox couples. However, the poor cycling stability and drastic voltage decay impede their practical application. Despite the covalency theory is proposed to understand the redox activity of LLOs, comprehensive design guidelines are still lacking. Inspired by the covalency theory of polyanion cathodes, high-performance LLOs are developed through an in-situ surface reconstruction strategy of near-surface doping and surface coating. Density function theory (DFT) calculations show that through the introduction of Ni<sup>2+</sup> and PO<sub>4</sub><sup>3-</sup>, the energy bands of the transition metal (TM) 3d-O 2p and non-bonding O-2p shift to lower energy, resulting in the elevated working potential, reduced activity of lattice oxygen, and enhanced reversibility of redox oxygen. Meanwhile, the Li<sub>3</sub>PO<sub>4</sub> coating can prevent electrolyte corrosion and mitigate surface degradation of LLOs upon cycling. As a result, the capacity retention of the modified LLOs is increased from 35.9 % to 77 %, and the voltage retention is raised from 68.6 % to 75.1 % after 700 cycles at 1 C. Furthermore, at 55 °C the capacity retention of the modified LLOs is also elevated from 32.1 % to 85.9 %, and the voltage retention is improved from 67.9 % to 82.3 % after 120 cycles at 1 C. The proposed strategy could advance the application of high-performance LLOs and their high-energy-density Li-ion batteries.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"134 ","pages":"Article 110588"},"PeriodicalIF":16.8,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816406","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.nanoen.2024.110579
Daijie Deng , Wei Zhang , Junchao Qian , Yun Chen , Chen Pu , Huaming Li , Henan Li , Li Xu
Atomically dispersed tungsten-nitrogen-carbon with W−N4 sites acts as a highly efficient catalyst for oxygen reactions. However, the symmetrical charge distribution of W−N4 sites results in strong binding with oxygen-containing intermediates, leading to unsatisfactory catalytic activities. Here, an axially coordinated sulfur (S) atom is integrated into the atomically dispersed W−N4 site and anchored onto multi-walled carbon nanotubes (S1−W1N4−MWCNTs) for oxygen reduction/oxygen evolution reactions (ORR/OER). The axial S atom, with significantly different electronegativity and outer electronic structure compared to nitrogen atom, induces localized charge redistribution around W−N4 site. This change optimizes the adsorption/desorption capabilities of oxygen-containing intermediates on W−N4 site, thereby enhancing the overall oxygen reaction activities. The S1−W1N4−MWCNTs demonstrates excellent ORR/OER activity with the half-wave potential of 0.916 V for ORR and the potential of 1.644 V (at 10 mA cm−2) for OER. At −20 °C, S1−W1N4−MWCNTs-based zinc-air batteries demonstrate increased specific capacity and an extended charging-discharging cycle life of 420 h, surpassing performance at room temperature. Regulating the charge distribution of W−N4 sites with axial S atoms provides an effective strategy to boost the oxygen reaction activities of tungsten-nitrogen-carbon catalysts.
{"title":"Charge delocalization regulation of atomically dispersed tungsten sites by axial sulfur atoms for highly active oxygen reactions in low-temperature zinc-air batteries","authors":"Daijie Deng , Wei Zhang , Junchao Qian , Yun Chen , Chen Pu , Huaming Li , Henan Li , Li Xu","doi":"10.1016/j.nanoen.2024.110579","DOIUrl":"10.1016/j.nanoen.2024.110579","url":null,"abstract":"<div><div>Atomically dispersed tungsten-nitrogen-carbon with W−N<sub>4</sub> sites acts as a highly efficient catalyst for oxygen reactions. However, the symmetrical charge distribution of W−N<sub>4</sub> sites results in strong binding with oxygen-containing intermediates, leading to unsatisfactory catalytic activities. Here, an axially coordinated sulfur (S) atom is integrated into the atomically dispersed W−N<sub>4</sub> site and anchored onto multi-walled carbon nanotubes (S<sub>1</sub>−W<sub>1</sub>N<sub>4</sub>−MWCNTs) for oxygen reduction/oxygen evolution reactions (ORR/OER). The axial S atom, with significantly different electronegativity and outer electronic structure compared to nitrogen atom, induces localized charge redistribution around W−N<sub>4</sub> site. This change optimizes the adsorption/desorption capabilities of oxygen-containing intermediates on W−N<sub>4</sub> site, thereby enhancing the overall oxygen reaction activities. The S<sub>1</sub>−W<sub>1</sub>N<sub>4</sub>−MWCNTs demonstrates excellent ORR/OER activity with the half-wave potential of 0.916 V for ORR and the potential of 1.644 V (at 10 mA cm<sup>−2</sup>) for OER. At −20 °C, S<sub>1</sub>−W<sub>1</sub>N<sub>4</sub>−MWCNTs-based zinc-air batteries demonstrate increased specific capacity and an extended charging-discharging cycle life of 420 h, surpassing performance at room temperature. Regulating the charge distribution of W−N<sub>4</sub> sites with axial S atoms provides an effective strategy to boost the oxygen reaction activities of tungsten-nitrogen-carbon catalysts.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"134 ","pages":"Article 110579"},"PeriodicalIF":16.8,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816412","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.nanoen.2024.110537
Seyed Masoud Parsa , Zhijie Chen , Siran Feng , Yuanying Yang , Li Luo , Huu Hao Ngo , Wei Wei , Bing-Jie Ni , Wenshan Guo
One of the major obstacles to microbial fuel cell (MFC) development is the design of high-performance, durable, and cost-effective electrocatalysts for the oxygen reduction reaction (ORR) to improve system performance during the electrochemical process. Accordingly, metal-free nitrogen-doped carbon-based electrocatalysts, in different forms/families, have been brought into the spotlight as a promising alternative to address this challenge. In this critical review, we comprehensively focus on recent advances in the design of this type of electrocatalyst for application in MFCs. We discuss the main drawbacks in applying metal-free nitrogen-doped carbon-based electrocatalysts through different angles, from nano-scale challenges like the interaction of nitrogen species during the ORR process and identifying the main active sites in various nitrogen species, to macro-scale issues such as different synthesizing methods during electrode preparation, MFC experiment conditions, and long-term operation, economic and cost assessment, just to name a few, that bridge lab-scale experiments to future real-world prototypes. Indeed, this review aims to open new windows for applying metal-free nitrogen-doped carbon-based catalysts in MFCs by addressing the gaps between fundamental understanding of fabrication of this type of catalyst to applied engineering point of view for practical applications. Finally, by discussing the most important remaining challenges, we outline a conceptual framework for future researches.
{"title":"Metal-free nitrogen-doped carbon-based electrocatalysts for oxygen reduction reaction in microbial fuel cells: Advances, challenges, and future directions","authors":"Seyed Masoud Parsa , Zhijie Chen , Siran Feng , Yuanying Yang , Li Luo , Huu Hao Ngo , Wei Wei , Bing-Jie Ni , Wenshan Guo","doi":"10.1016/j.nanoen.2024.110537","DOIUrl":"10.1016/j.nanoen.2024.110537","url":null,"abstract":"<div><div>One of the major obstacles to microbial fuel cell (MFC) development is the design of high-performance, durable, and cost-effective electrocatalysts for the oxygen reduction reaction (ORR) to improve system performance during the electrochemical process. Accordingly, metal-free nitrogen-doped carbon-based electrocatalysts, in different forms/families, have been brought into the spotlight as a promising alternative to address this challenge. In this critical review, we comprehensively focus on recent advances in the design of this type of electrocatalyst for application in MFCs. We discuss the main drawbacks in applying metal-free nitrogen-doped carbon-based electrocatalysts through different angles, from nano-scale challenges like the interaction of nitrogen species during the ORR process and identifying the main active sites in various nitrogen species, to macro-scale issues such as different synthesizing methods during electrode preparation, MFC experiment conditions, and long-term operation, economic and cost assessment, just to name a few, that bridge lab-scale experiments to future real-world prototypes. Indeed, this review aims to open new windows for applying metal-free nitrogen-doped carbon-based catalysts in MFCs by addressing the gaps between fundamental understanding of fabrication of this type of catalyst to applied engineering point of view for practical applications. Finally, by discussing the most important remaining challenges, we outline a conceptual framework for future researches.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"134 ","pages":"Article 110537"},"PeriodicalIF":16.8,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142763347","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.nanoen.2024.110532
Zhenyang Li , Chenyu Li , Yue Xiao , Shuzheng Liu , Gang Qin , Jia Yang , Qiang Chen , Aiguo Zhou
Triboelectric nanogenerator (TENG) is widely used in the fields of sustainable green energy harvesting, self-powered motion parameter and tactile sensing, However, it still fails to meet the requirements under various complex conditions, such as low temperatures, self healing after destruction, punching, long-term placement, soaking in acid or alkali solution, scorch, continuous work. Herein, based on metal coordination, Zr4 + ions are introduced to enhance the first network k-carrageenan (k-CG) for achieving double enhancement in mechanics and electricity of the gel electrode layer, poly (N-hydroxyl acrylamide)/k-CG (PKZ) double network organic conductive gel enhanced by multiple hydrogen bonds and metal coordination bond is designed, and the gel exhibits high tensile strength, high conductivity, fast self-recovery, excellent self-repairing and low-temperature resistance. Based on simple sandpaper templates with different mesh numbers Ecoflex film with rough surfaces is designed for efficient triboelectric contact interface, and TENG with PKZ double network organic conductive gel as electrode layer is constructed, and possesses excellent resistant to multiple complex conditions. With high short-circuit current, open-circuit voltage and output power, the TENG is capable of powering electronic devices, and it can also be sensitive and stable sensing in writing recognition, real-time monitoring of motion parameters involving acceleration, speed and distance. The TENG is stable and reliable for sustainable green energy harvesting, motion parameter and tactile sensing in multiple complex environments. Thus, we provide novel ideas for designing energy harvesting and sensing for future wearable electronics under multiple complex conditions.
{"title":"Metal coordination bond and rough interface enhanced triboelectric nanogenerator aiming for multiple complex conditions","authors":"Zhenyang Li , Chenyu Li , Yue Xiao , Shuzheng Liu , Gang Qin , Jia Yang , Qiang Chen , Aiguo Zhou","doi":"10.1016/j.nanoen.2024.110532","DOIUrl":"10.1016/j.nanoen.2024.110532","url":null,"abstract":"<div><div>Triboelectric nanogenerator (TENG) is widely used in the fields of sustainable green energy harvesting, self-powered motion parameter and tactile sensing, However, it still fails to meet the requirements under various complex conditions, such as low temperatures, self healing after destruction, punching, long-term placement, soaking in acid or alkali solution, scorch, continuous work. Herein, based on metal coordination, Zr<sup>4 +</sup> ions are introduced to enhance the first network <em>k</em>-carrageenan (<em>k</em>-CG) for achieving double enhancement in mechanics and electricity of the gel electrode layer, poly (<em>N</em>-hydroxyl acrylamide)/<em>k</em>-CG (PKZ) double network organic conductive gel enhanced by multiple hydrogen bonds and metal coordination bond is designed, and the gel exhibits high tensile strength, high conductivity, fast self-recovery, excellent self-repairing and low-temperature resistance. Based on simple sandpaper templates with different mesh numbers Ecoflex film with rough surfaces is designed for efficient triboelectric contact interface, and TENG with PKZ double network organic conductive gel as electrode layer is constructed, and possesses excellent resistant to multiple complex conditions. With high short-circuit current, open-circuit voltage and output power, the TENG is capable of powering electronic devices, and it can also be sensitive and stable sensing in writing recognition, real-time monitoring of motion parameters involving acceleration, speed and distance. The TENG is stable and reliable for sustainable green energy harvesting, motion parameter and tactile sensing in multiple complex environments. Thus, we provide novel ideas for designing energy harvesting and sensing for future wearable electronics under multiple complex conditions.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"134 ","pages":"Article 110532"},"PeriodicalIF":16.8,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142756375","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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