Pub Date : 2024-02-01DOI: 10.1016/j.esci.2023.100188
Lidong Sun , Yong Wang , Lingchen Kong , Shaoshan Chen , Cong Peng , Jiahui Zheng , Yu Li , Wei Feng
As high-energy cathode materials, conversion-type metal fluorides provide a prospective pathway for developing next-generation lithium-ion batteries. However, they suffer from severe performance decay owing to continuous structural destruction and active material dissolution upon cycling, which worsen at elevated temperatures. Here, we design a novel FeF2 cathode with in situ polymerized solid-state electrolyte systems to enhance the cycling ability of metal fluorides at 60 °C. Novel FeF2 with a mesoporous structure (meso-FeF2) improves Li+ diffusion and relieves the volume change that typically occurs during the alternating conversion reactions. The structural stability of the meso-FeF2 cathode is strengthened by an in situ polymerized solid-state electrolyte, which prevents the pulverization and ion dissolution that are inevitable for conventional liquid electrolytes. Under the double action of this in situ polymerized solid-state electrolyte and the meso-FeF2's mesoporous structure, the active material maintains an intact SEI layer and part of the mesoporous structure after long charge–discharge cycling, showing excellent cycling stability at high temperatures.
作为高能正极材料,转换型金属氟化物为开发下一代锂离子电池提供了一条前景广阔的途径。然而,由于在循环过程中结构持续破坏和活性材料溶解,它们的性能衰减严重,在温度升高时情况更加恶化。在此,我们设计了一种新型 FeF2 阴极,并采用原位聚合固态电解质系统,以增强金属氟化物在 60 °C 下的循环能力。具有介孔结构(meso-FeF2)的新型 FeF2 改善了 Li+ 的扩散,缓解了通常在交替转换反应中发生的体积变化。原位聚合固态电解质增强了介孔 FeF2 阴极的结构稳定性,防止了传统液态电解质不可避免的粉碎和离子溶解现象。在这种原位聚合固态电解质和介质 FeF2 的介孔结构的双重作用下,活性材料在长时间充放电循环后仍能保持完整的 SEI 层和部分介孔结构,在高温下表现出优异的循环稳定性。
{"title":"Designing mesostructured iron (II) fluorides with a stable in situ polymer electrolyte interface for high-energy-density lithium-ion batteries","authors":"Lidong Sun , Yong Wang , Lingchen Kong , Shaoshan Chen , Cong Peng , Jiahui Zheng , Yu Li , Wei Feng","doi":"10.1016/j.esci.2023.100188","DOIUrl":"10.1016/j.esci.2023.100188","url":null,"abstract":"<div><p>As high-energy cathode materials, conversion-type metal fluorides provide a prospective pathway for developing next-generation lithium-ion batteries. However, they suffer from severe performance decay owing to continuous structural destruction and active material dissolution upon cycling, which worsen at elevated temperatures. Here, we design a novel FeF<sub>2</sub> cathode with <em>in situ</em> polymerized solid-state electrolyte systems to enhance the cycling ability of metal fluorides at 60 °C. Novel FeF<sub>2</sub> with a mesoporous structure (meso-FeF<sub>2</sub>) improves Li<sup>+</sup> diffusion and relieves the volume change that typically occurs during the alternating conversion reactions. The structural stability of the meso-FeF<sub>2</sub> cathode is strengthened by an <em>in situ</em> polymerized solid-state electrolyte, which prevents the pulverization and ion dissolution that are inevitable for conventional liquid electrolytes. Under the double action of this <em>in situ</em> polymerized solid-state electrolyte and the meso-FeF<sub>2</sub>'s mesoporous structure, the active material maintains an intact SEI layer and part of the mesoporous structure after long charge–discharge cycling, showing excellent cycling stability at high temperatures.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"4 1","pages":"Article 100188"},"PeriodicalIF":0.0,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667141723001283/pdfft?md5=0dbd161a4b3d9986b41b7b53f20710b5&pid=1-s2.0-S2667141723001283-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135434450","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}
Pub Date : 2024-02-01DOI: 10.1016/j.esci.2023.100140
Hon Ho Wong , Mingzi Sun , Tong Wu , Cheuk Hei Chan , Lu Lu , Qiuyang Lu , Baian Chen , Bolong Huang
Although single-atom catalysts (SACs) have attracted enormous attention for their applications in the electrochemical reduction of CO2 (CO2RR) due to their extraordinary catalytic activity and well-defined active centers, neighboring effects and their influence on the electrochemical performance of SACs have not been well investigated. In this review, we present a summary of the neighboring effects on SACs for the CO2RR process, where the surrounding atoms not only induce electronic modulation of the metal atom but also participate in the CO2RR. Both theoretical and experimental studies have pointed out that the neighboring sites of the anchored metal center can provide second active/adsorption locations during the catalytic process, enhancing CO2RR performance tremendously. This review supplies advanced insights into the significant roles and impacts of neighboring effects on the catalytic process, which also benefit the development of advanced SACs to achieve efficient electrocatalysis.
{"title":"Neighboring effect in single-atom catalysts for the electrochemical carbon dioxide reduction reaction","authors":"Hon Ho Wong , Mingzi Sun , Tong Wu , Cheuk Hei Chan , Lu Lu , Qiuyang Lu , Baian Chen , Bolong Huang","doi":"10.1016/j.esci.2023.100140","DOIUrl":"10.1016/j.esci.2023.100140","url":null,"abstract":"<div><p>Although single-atom catalysts (SACs) have attracted enormous attention for their applications in the electrochemical reduction of CO<sub>2</sub> (CO<sub>2</sub>RR) due to their extraordinary catalytic activity and well-defined active centers, neighboring effects and their influence on the electrochemical performance of SACs have not been well investigated. In this review, we present a summary of the neighboring effects on SACs for the CO<sub>2</sub>RR process, where the surrounding atoms not only induce electronic modulation of the metal atom but also participate in the CO<sub>2</sub>RR. Both theoretical and experimental studies have pointed out that the neighboring sites of the anchored metal center can provide second active/adsorption locations during the catalytic process, enhancing CO<sub>2</sub>RR performance tremendously. This review supplies advanced insights into the significant roles and impacts of neighboring effects on the catalytic process, which also benefit the development of advanced SACs to achieve efficient electrocatalysis.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"4 1","pages":"Article 100140"},"PeriodicalIF":0.0,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667141723000654/pdfft?md5=434077aa5799f09e9b05a582ec478729&pid=1-s2.0-S2667141723000654-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"76581058","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}
Pub Date : 2024-01-25DOI: 10.1016/j.esci.2024.100243
Hee Jung Kim , Gill Sang Han , Hyun Suk Jung
Perovskite solar cells (PSCs) have shown remarkable advancements and achieved impressive power conversion efficiencies since their initial introduction in 2012. However, challenges regarding stability, quality, and sustainability must be addressed for their successful commercial use. This review analyses the recent studies and challenges related to the operating life and end-of-life utilization of PSCs. Strategies to enhance the stability and mitigate the toxic Pb leakage in operational and recycling approaches of discarded PSCs post their end-of-life are examined to establish a viable and sustainable PSC industry. Additionally, future research directions are proposed for the advancements in the PSC industry. The goal is to ensure high efficiency as well as economic and environmental sustainability throughout the lifecycle of PSCs.
{"title":"Managing the lifecycle of perovskite solar cells: Addressing stability and environmental concerns from utilization to end-of-life","authors":"Hee Jung Kim , Gill Sang Han , Hyun Suk Jung","doi":"10.1016/j.esci.2024.100243","DOIUrl":"10.1016/j.esci.2024.100243","url":null,"abstract":"<div><p>Perovskite solar cells (PSCs) have shown remarkable advancements and achieved impressive power conversion efficiencies since their initial introduction in 2012. However, challenges regarding stability, quality, and sustainability must be addressed for their successful commercial use. This review analyses the recent studies and challenges related to the operating life and end-of-life utilization of PSCs. Strategies to enhance the stability and mitigate the toxic Pb leakage in operational and recycling approaches of discarded PSCs post their end-of-life are examined to establish a viable and sustainable PSC industry. Additionally, future research directions are proposed for the advancements in the PSC industry. The goal is to ensure high efficiency as well as economic and environmental sustainability throughout the lifecycle of PSCs.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"4 2","pages":"Article 100243"},"PeriodicalIF":0.0,"publicationDate":"2024-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667141724000211/pdfft?md5=9af375c34e24f08f7ef6b4770783ac17&pid=1-s2.0-S2667141724000211-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139562337","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}
Pub Date : 2023-12-10DOI: 10.1016/j.esci.2023.100221
Aodong Zhu , Lin Chen , Ao Zhang , Chenpu Zhu , Xinxin Zhang , Jie Zhong , Fuzhi Huang , Yi-Bing Cheng , Junyan Xiao
Carbon-based perovskite solar cells (C-PSCs) are promising candidates for large-scale photovoltaic applications due to their theoretical low cost and high stability. However, the fabrication of high-performance C-PSCs with large-area electrodes remains challenging. In this work, we propose a novel playdough-like graphite putty as top electrode in the perovskite devices. This electrode with soft nature can form good contact with the hole-transporting layer and the conductive substrate at room temperature by a simple pressing technique, which facilitates the fabrication of both small-area devices and perovskite solar modules. In this preliminary research, the corresponding small devices and modules can achieve efficiencies of 20.29% (∼0.15 cm2) and 16.01% (∼10 cm2), respectively. Moreover, we analyze the limitations of the optical and electrical properties of this playdough-like graphite electrode on the device performance, suggesting a direction for further improvement of C-PSCs in the future.
{"title":"Playdough-like carbon electrode: A promising strategy for high efficiency perovskite solar cells and modules","authors":"Aodong Zhu , Lin Chen , Ao Zhang , Chenpu Zhu , Xinxin Zhang , Jie Zhong , Fuzhi Huang , Yi-Bing Cheng , Junyan Xiao","doi":"10.1016/j.esci.2023.100221","DOIUrl":"10.1016/j.esci.2023.100221","url":null,"abstract":"<div><p>Carbon-based perovskite solar cells (C-PSCs) are promising candidates for large-scale photovoltaic applications due to their theoretical low cost and high stability. However, the fabrication of high-performance C-PSCs with large-area electrodes remains challenging. In this work, we propose a novel playdough-like graphite putty as top electrode in the perovskite devices. This electrode with soft nature can form good contact with the hole-transporting layer and the conductive substrate at room temperature by a simple pressing technique, which facilitates the fabrication of both small-area devices and perovskite solar modules. In this preliminary research, the corresponding small devices and modules can achieve efficiencies of 20.29% (∼0.15 cm<sup>2</sup>) and 16.01% (∼10 cm<sup>2</sup>), respectively. Moreover, we analyze the limitations of the optical and electrical properties of this playdough-like graphite electrode on the device performance, suggesting a direction for further improvement of C-PSCs in the future.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"4 2","pages":"Article 100221"},"PeriodicalIF":0.0,"publicationDate":"2023-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667141723001751/pdfft?md5=581b2051f0552172b41c70cb0f765139&pid=1-s2.0-S2667141723001751-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138560609","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}
Pub Date : 2023-12-10DOI: 10.1016/j.esci.2023.100223
Xingkai Ju , Jiao Kong , Guohua Qi , Shuping Hou , Bo Wang , Xingkang Diao , Shaojun Dong , Yongdong Jin
Developing the high biosafety, effective and wearable devices for fast wound healing is highly desired but remains a challenge. Here, we propose a “win–win co-operation” strategy to potentiate effective skin wound healing at the wound site by constructing robust and ecofriendly composite patch under opto-electric stimulation. The wearable patch is composed of ionic gel doped with Ti3C2Tx (MXene), which possesses good photothermal response to kill the bacteria via effective inhibition of the expression of inflammatory factors, preventing wound infection. Importantly, the composite ionogel patch is capable of providing green and on-demand electrical stimulation for wound site, guiding cell migration and proliferation by improved bioenergy and expression up-regulation of growth factor. In mice wound models, the treatment group healed ∼31% more rapidly. Mechanistically, the wearable devices could enable visual and real-time supervising treatment effect due to their good transmittance. The proposed strategy would be promising for future clinical treatment of wound healing.
{"title":"Photoelectric-driven conductive composite ionogel patch for effective wound healing","authors":"Xingkai Ju , Jiao Kong , Guohua Qi , Shuping Hou , Bo Wang , Xingkang Diao , Shaojun Dong , Yongdong Jin","doi":"10.1016/j.esci.2023.100223","DOIUrl":"10.1016/j.esci.2023.100223","url":null,"abstract":"<div><p>Developing the high biosafety, effective and wearable devices for fast wound healing is highly desired but remains a challenge. Here, we propose a “win–win co-operation” strategy to potentiate effective skin wound healing at the wound site by constructing robust and ecofriendly composite patch under opto-electric stimulation. The wearable patch is composed of ionic gel doped with Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> (MXene), which possesses good photothermal response to kill the bacteria via effective inhibition of the expression of inflammatory factors, preventing wound infection. Importantly, the composite ionogel patch is capable of providing green and on-demand electrical stimulation for wound site, guiding cell migration and proliferation by improved bioenergy and expression up-regulation of growth factor. In mice wound models, the treatment group healed ∼31% more rapidly. Mechanistically, the wearable devices could enable visual and real-time supervising treatment effect due to their good transmittance. The proposed strategy would be promising for future clinical treatment of wound healing.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"4 2","pages":"Article 100223"},"PeriodicalIF":0.0,"publicationDate":"2023-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667141723001775/pdfft?md5=12a01699ebde0f655eda4a436e12f70a&pid=1-s2.0-S2667141723001775-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138560597","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}
Pub Date : 2023-11-08DOI: 10.1016/j.esci.2023.100209
Mengjun Wang , Jun Jia , Hao Yan , Guang Li , Qiming Hong , Yuzheng Guo , Yong Xu , Xiaoqing Huang
Phase modulation of noble metal alloys (NMAs) is critically important in nanoscience since the distinct atomic arrangements can largely determine their physicochemical properties. However, the precise modulation of NMAs is formidably challenging, because thermodynamically stable phases are generally preferential compared to those metastable ones. Herein, we proposed a potential energy trapping strategy for phase modulation of Pd–Te alloys with solvents. Thereinto, ethylene glycol can increase the energy barrier for both Pd leaching and Te introduction, forming metastable Pd20Te7 phase. Inversely, N, N-dimethylformamide is unable to trap metastable phase, inducing the phase evolution to thermodynamically stable PdTe phase, and the precise phase modulation was realized including Pd20Te7, PdTe and PdTe2 phases. The Pd–Te alloys displayed phase-dependent formic acid oxidation catalytic performance with PdTe phase showing the best. This work proposes a strategy for creating metastable phase with potential energy trap, which may deepen the understanding of phase engineering for noble metal-based nanocrystals.
{"title":"Phase engineering of Pd–Te nanoplates via potential energy trapping","authors":"Mengjun Wang , Jun Jia , Hao Yan , Guang Li , Qiming Hong , Yuzheng Guo , Yong Xu , Xiaoqing Huang","doi":"10.1016/j.esci.2023.100209","DOIUrl":"10.1016/j.esci.2023.100209","url":null,"abstract":"<div><p>Phase modulation of noble metal alloys (NMAs) is critically important in nanoscience since the distinct atomic arrangements can largely determine their physicochemical properties. However, the precise modulation of NMAs is formidably challenging, because thermodynamically stable phases are generally preferential compared to those metastable ones. Herein, we proposed a potential energy trapping strategy for phase modulation of Pd–Te alloys with solvents. Thereinto, ethylene glycol can increase the energy barrier for both Pd leaching and Te introduction, forming metastable Pd<sub>20</sub>Te<sub>7</sub> phase. Inversely, N, N-dimethylformamide is unable to trap metastable phase, inducing the phase evolution to thermodynamically stable PdTe phase, and the precise phase modulation was realized including Pd<sub>20</sub>Te<sub>7</sub>, PdTe and PdTe<sub>2</sub> phases. The Pd–Te alloys displayed phase-dependent formic acid oxidation catalytic performance with PdTe phase showing the best. This work proposes a strategy for creating metastable phase with potential energy trap, which may deepen the understanding of phase engineering for noble metal-based nanocrystals.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"4 2","pages":"Article 100209"},"PeriodicalIF":0.0,"publicationDate":"2023-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667141723001556/pdfft?md5=34aee37357daca6bebf346fe5ec9f4b7&pid=1-s2.0-S2667141723001556-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135515079","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}
Pub Date : 2023-11-02DOI: 10.1016/j.esci.2023.100208
Shijie Li , Kexin Dong , Mingjie Cai , Xinyu Li , Xiaobo Chen
Present photocatalysts for the synchronous cleanup of pharmaceuticals and heavy metals have several drawbacks, including inadequate reactive sites, inefficient electron–hole disassociation, and insufficient oxidation and reduction power. In this research, we sought to address these issues by using a facile solvothermal-photoreduction route to develop an innovative plasmonic S-scheme heterojunction, Au/MIL-101(Fe)/BiOBr. The screened-out Au/MIL-101(Fe)/BiOBr (AMB-2) works in a durable and high-performance manner for both Cr(VI) and norfloxacin (NOR) eradication under visible light, manifesting up to 53.3 and 2 times greater Cr(VI) and NOR abatement rates, respectively, than BiOBr. Remarkably, AMB-2's ability to remove Cr(VI) in a Cr(VI)-NOR co-existence system is appreciably better than in a sole-Cr(VI) environment; the synergy among Cr(VI), NOR, and AMB-2 results in the better utilization of photo-induced carriers, yielding a desirable capacity for decontaminating Cr(VI) and NOR synchronously. The integration of MOF-based S-scheme heterojunctions and a plasmonic effect contributes to markedly reinforced photocatalytic ability by increasing the number of active sites, augmenting the visible-light absorbance, boosting the efficient disassociation and redistribution of powerful photo-carriers, and elevating the generation of reactive substances. We provide details of the photocatalytic mechanism, NOR decomposition process, and bio-toxicity of the intermediates. This synergistic strategy of modifying S-scheme heterojunctions with a noble metal opens new horizons for devising excellent MOF-based photosystems with a plasmonic effect for environment purification.
目前用于同步净化药物和重金属的光催化剂存在几个缺点,包括反应位点不足、电子-空穴解离效率低以及氧化和还原能力不足。在这项研究中,我们试图利用一种简便的溶热-光诱导路线来开发一种创新的等离子体 S 型异质结 Au/MIL-101(Fe)/BiOBr,从而解决这些问题。筛选出的金/MIL-101(Fe)/BiOBr(AMB-2)可在可见光下持久、高效地消除六价铬和诺氟沙星(NOR),其六价铬和 NOR 的消除率分别是 BiOBr 的 53.3 倍和 2 倍。值得注意的是,AMB-2 在六价铬-NOR 共存系统中去除六价铬的能力明显优于在单一六价铬环境中;六价铬、NOR 和 AMB-2 之间的协同作用使光诱导载体得到了更好的利用,从而产生了同步去除六价铬和 NOR 的理想能力。基于 MOF 的 S 型异质结与等离子体效应相结合,增加了活性位点的数量,提高了可见光吸收率,促进了强力光载体的有效解离和再分配,并提高了反应物质的生成,从而显著增强了光催化能力。我们详细介绍了光催化机理、NOR 分解过程以及中间产物的生物毒性。这种用贵金属修饰 S 型异质结的协同策略为设计出具有质子效应、用于环境净化的卓越 MOF 基光电系统开辟了新天地。
{"title":"A plasmonic S-scheme Au/MIL-101(Fe)/BiOBr photocatalyst for efficient synchronous decontamination of Cr(VI) and norfloxacin antibiotic","authors":"Shijie Li , Kexin Dong , Mingjie Cai , Xinyu Li , Xiaobo Chen","doi":"10.1016/j.esci.2023.100208","DOIUrl":"10.1016/j.esci.2023.100208","url":null,"abstract":"<div><p>Present photocatalysts for the synchronous cleanup of pharmaceuticals and heavy metals have several drawbacks, including inadequate reactive sites, inefficient electron–hole disassociation, and insufficient oxidation and reduction power. In this research, we sought to address these issues by using a facile solvothermal-photoreduction route to develop an innovative plasmonic S-scheme heterojunction, Au/MIL-101(Fe)/BiOBr. The screened-out Au/MIL-101(Fe)/BiOBr (AMB-2) works in a durable and high-performance manner for both Cr(VI) and norfloxacin (NOR) eradication under visible light, manifesting up to 53.3 and 2 times greater Cr(VI) and NOR abatement rates, respectively, than BiOBr. Remarkably, AMB-2's ability to remove Cr(VI) in a Cr(VI)-NOR co-existence system is appreciably better than in a sole-Cr(VI) environment; the synergy among Cr(VI), NOR, and AMB-2 results in the better utilization of photo-induced carriers, yielding a desirable capacity for decontaminating Cr(VI) and NOR synchronously. The integration of MOF-based S-scheme heterojunctions and a plasmonic effect contributes to markedly reinforced photocatalytic ability by increasing the number of active sites, augmenting the visible-light absorbance, boosting the efficient disassociation and redistribution of powerful photo-carriers, and elevating the generation of reactive substances. We provide details of the photocatalytic mechanism, NOR decomposition process, and bio-toxicity of the intermediates. This synergistic strategy of modifying S-scheme heterojunctions with a noble metal opens new horizons for devising excellent MOF-based photosystems with a plasmonic effect for environment purification.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"4 2","pages":"Article 100208"},"PeriodicalIF":0.0,"publicationDate":"2023-11-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667141723001544/pdfft?md5=40dae6d8b3f22e4bcb724dd6a23addc0&pid=1-s2.0-S2667141723001544-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135410663","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}
Pub Date : 2023-10-19DOI: 10.1016/j.esci.2023.100205
Lei Zhang , Jin Xiao , Xilin Xiao , Wenli Xin , Yaheng Geng , Zichao Yan , Zhiqiang Zhu
Stabilizing the Zn anode under high utilization rates is highly applauded yet very challenging in aqueous Zn batteries. Here, we rationally design a zincophilic short-chain aromatic molecule, 4-mercaptopyridine (4Mpy), to construct self-assembled monolayers (SAMs) on a copper substrate to achieve highly utilized Zn anodes. We reveal that 4Mpy could be firmly bound on the Cu substrate via Cu–S bond to form compact and uniform SAMs, which could effectively isolate the water on the electrode surface and thus eliminate the water-related side reactions. In addition, the short-chain aromatic ring structure of 4Mpy could not only ensure the ordered arrangement of zincophilic pyridine N but also facilitate charge transfer, thus enabling uniform and rapid Zn deposition. Consequently, the Zn/4Mpy/Cu electrode not only enables the symmetric cell to stably cycle for over 180 h at 10 mA cm−2 under a high depth-of-discharge of 90%, but also allows the MnO2-paired pouch cell to survive for 100 cycles under a high Zn utilization rate of 78.8%. An anode-free 4Mpy/Cu||graphite cell also operates for 150 cycles without obvious capacity fading at 0.1 A g−1. This control of interfacial chemistry via SAMs to achieve high utilization rates of metal anodes provides a new paradigm for developing high-energy metal-based batteries.
{"title":"Molecular engineering of self-assembled monolayers for highly utilized Zn anodes","authors":"Lei Zhang , Jin Xiao , Xilin Xiao , Wenli Xin , Yaheng Geng , Zichao Yan , Zhiqiang Zhu","doi":"10.1016/j.esci.2023.100205","DOIUrl":"10.1016/j.esci.2023.100205","url":null,"abstract":"<div><p>Stabilizing the Zn anode under high utilization rates is highly applauded yet very challenging in aqueous Zn batteries. Here, we rationally design a zincophilic short-chain aromatic molecule, 4-mercaptopyridine (4Mpy), to construct self-assembled monolayers (SAMs) on a copper substrate to achieve highly utilized Zn anodes. We reveal that 4Mpy could be firmly bound on the Cu substrate via Cu–S bond to form compact and uniform SAMs, which could effectively isolate the water on the electrode surface and thus eliminate the water-related side reactions. In addition, the short-chain aromatic ring structure of 4Mpy could not only ensure the ordered arrangement of zincophilic pyridine N but also facilitate charge transfer, thus enabling uniform and rapid Zn deposition. Consequently, the Zn/4Mpy/Cu electrode not only enables the symmetric cell to stably cycle for over 180 h at 10 mA cm<sup>−2</sup> under a high depth-of-discharge of 90%, but also allows the MnO<sub>2</sub>-paired pouch cell to survive for 100 cycles under a high Zn utilization rate of 78.8%. An anode-free 4Mpy/Cu||graphite cell also operates for 150 cycles without obvious capacity fading at 0.1 A g<sup>−1</sup>. This control of interfacial chemistry via SAMs to achieve high utilization rates of metal anodes provides a new paradigm for developing high-energy metal-based batteries.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"4 2","pages":"Article 100205"},"PeriodicalIF":0.0,"publicationDate":"2023-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667141723001507/pdfft?md5=11125af729dee09f1a1add11d8fdf975&pid=1-s2.0-S2667141723001507-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135963788","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}
Pub Date : 2023-10-04DOI: 10.1016/j.esci.2023.100201
Lu-Kang Zhao , Xuan-Wen Gao , Qinfen Gu , Xiaochen Ge , Zhimin Ding , Zhaomeng Liu , Wen-Bin Luo
Potassium metal batteries (PMBs) have become a paramount alternative energy storage technology to lithium-ion batteries, due to their low cost and potential energy density. However, uncontrolled dendrite growth interferes with the stability of the interfacial anode, leading to significant capacity degradation and safety hazards. Herein, a facile reactive prewetting strategy is proposed to discourage dendrite growth by constructing a functional KF/Zn-rich hybrid interface layer on K metal. The KF/Zn@K anode design functions like an interconnected paddy field, stabilizing the anode interface through the preferential redistribution of K+ flux/electrons, continuous transport paths, and enhanced transport dynamics. As anticipated, symmetrical batteries exhibit an extended cycling lifetime of over 2000 h, with reduced voltage hysteresis at 0.5 mA cm−2 and 0.5 mAh cm−2. Furthermore, when the KF/Zn@K anode is applied to full batteries coupled with PTCDA, a boosted reversible capacity of 61.6 mAh g−1 at 5 C is present over 3000 cycles. This interfacial control creates rational possibilities for constructing high-efficiency, stable K metal anodes.
钾金属电池(PMB)因其低成本和潜在的能量密度,已成为锂离子电池的重要替代储能技术。然而,不受控制的枝晶生长会干扰界面阳极的稳定性,导致容量显著下降并带来安全隐患。本文提出了一种简便的反应性预湿策略,通过在 K 金属上构建富含 KF/Zn 的功能性混合界面层来阻止枝晶的生长。KF/Zn@K 阳极设计就像一个相互连接的稻田,通过优先重新分配 K+ 通量/电子、连续传输路径和增强传输动力学来稳定阳极界面。正如预期的那样,对称电池的循环寿命延长了 2000 多小时,在 0.5 mA cm-2 和 0.5 mAh cm-2 时的电压滞后也有所减少。此外,当 KF/Zn@K 阳极与 PTCDA 结合应用于全电池时,在 5 C 条件下,经过 3000 次循环后,可逆容量提高到 61.6 mAh g-1。这种界面控制为构建高效、稳定的 K 金属阳极提供了合理的可能性。
{"title":"Realizing a dendrite-free metallic-potassium anode using reactive prewetting chemistry","authors":"Lu-Kang Zhao , Xuan-Wen Gao , Qinfen Gu , Xiaochen Ge , Zhimin Ding , Zhaomeng Liu , Wen-Bin Luo","doi":"10.1016/j.esci.2023.100201","DOIUrl":"10.1016/j.esci.2023.100201","url":null,"abstract":"<div><p>Potassium metal batteries (PMBs) have become a paramount alternative energy storage technology to lithium-ion batteries, due to their low cost and potential energy density. However, uncontrolled dendrite growth interferes with the stability of the interfacial anode, leading to significant capacity degradation and safety hazards. Herein, a facile reactive prewetting strategy is proposed to discourage dendrite growth by constructing a functional KF/Zn-rich hybrid interface layer on K metal. The KF/Zn@K anode design functions like an interconnected paddy field, stabilizing the anode interface through the preferential redistribution of K<sup>+</sup> flux/electrons, continuous transport paths, and enhanced transport dynamics. As anticipated, symmetrical batteries exhibit an extended cycling lifetime of over 2000 h, with reduced voltage hysteresis at 0.5 mA cm<sup>−2</sup> and 0.5 mAh cm<sup>−2</sup>. Furthermore, when the KF/Zn@K anode is applied to full batteries coupled with PTCDA, a boosted reversible capacity of 61.6 mAh g<sup>−1</sup> at 5 C is present over 3000 cycles. This interfacial control creates rational possibilities for constructing high-efficiency, stable K metal anodes.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"4 2","pages":"Article 100201"},"PeriodicalIF":0.0,"publicationDate":"2023-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667141723001465/pdfft?md5=5de5ce2336f30cbd0f3281e0e41a5574&pid=1-s2.0-S2667141723001465-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"134935419","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}
Pub Date : 2023-10-01DOI: 10.1016/j.esci.2023.100159
Xiaohui Rong , Dongdong Xiao , Qinghao Li , Yaoshen Niu , Feixiang Ding , Xueyan Hou , Qiyu Wang , Juping Xu , Chenglong Zhao , Dong Zhou , Ruijuan Xiao , Xiqian Yu , Wen Yin , Lin Gu , Hong Li , Xuejie Huang , Liquan Chen , Yong-Sheng Hu
The anionic redox reaction (ARR) is a promising charge contributor to improve the reversible capacity of layered-oxide cathodes for Na-ion batteries; however, some practical bottlenecks still need to be eliminated, including a low capacity retention, large voltage hysteresis, and low rate capability. Herein, we proposed a high-Na content honeycomb-ordered cathode, P2–Na5/6[Li1/6Cu1/6Mn2/3]O2 (P2-NLCMO), with combined cationic/anionic redox. Neutron powder diffraction and X-ray diffraction of P2-NLCMO suggested P2-type stacking with rarely found P6322 symmetry. In addition, advanced spectroscopy techniques and density functional theory calculations confirmed the synergistic stabilizing relationship between the Li/Cu dual honeycomb centers, achieving fully active Cu3+/Cu2+ redox and stabilized ARR with interactively suppressed local distortion. With a meticulously regulated charge/discharge protocol, both the cycling and rate capability of P2-NLCMO were significantly improved, demonstrating reasonable capacity and eliminating voltage hysteresis. Overall, this work contributes a well-defined layered oxide cathode with combined cationic/anionic redox towards rational designing advanced Na-ion batteries.
{"title":"Boosting reversible anionic redox reaction with Li/Cu dual honeycomb centers","authors":"Xiaohui Rong , Dongdong Xiao , Qinghao Li , Yaoshen Niu , Feixiang Ding , Xueyan Hou , Qiyu Wang , Juping Xu , Chenglong Zhao , Dong Zhou , Ruijuan Xiao , Xiqian Yu , Wen Yin , Lin Gu , Hong Li , Xuejie Huang , Liquan Chen , Yong-Sheng Hu","doi":"10.1016/j.esci.2023.100159","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100159","url":null,"abstract":"<div><p>The anionic redox reaction (ARR) is a promising charge contributor to improve the reversible capacity of layered-oxide cathodes for Na-ion batteries; however, some practical bottlenecks still need to be eliminated, including a low capacity retention, large voltage hysteresis, and low rate capability. Herein, we proposed a high-Na content honeycomb-ordered cathode, P2–Na<sub>5/6</sub>[Li<sub>1/6</sub>Cu<sub>1/6</sub>Mn<sub>2/3</sub>]O<sub>2</sub> (P2-NLCMO), with combined cationic/anionic redox. Neutron powder diffraction and X-ray diffraction of P2-NLCMO suggested P2-type stacking with rarely found <em>P</em>6<sub>3</sub>22 symmetry. In addition, advanced spectroscopy techniques and density functional theory calculations confirmed the synergistic stabilizing relationship between the Li/Cu dual honeycomb centers, achieving fully active Cu<sup>3+</sup>/Cu<sup>2+</sup> redox and stabilized ARR with interactively suppressed local distortion. With a meticulously regulated charge/discharge protocol, both the cycling and rate capability of P2-NLCMO were significantly improved, demonstrating reasonable capacity and eliminating voltage hysteresis. Overall, this work contributes a well-defined layered oxide cathode with combined cationic/anionic redox towards rational designing advanced Na-ion batteries.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"3 5","pages":"Article 100159"},"PeriodicalIF":0.0,"publicationDate":"2023-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"50203460","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}