Han Liu, Yaqi Liao, Chihon Leung, Yangqian Zhang, Yuewen Yang, Fangyan Liu, Ying Wei, Che Fan, Shuoxiao Zhang, Donghai Wang, Jie Yan, Qi Liu, Chiyuen Chung, Yang Ren, Yunhui Huang, Jiayi Yang
Polyacrylonitrile (PAN) is a promising polymer for solid-state lithium (Li) metal batteries (SSLMBs). However, the low ionic conductivity of PAN-based solid polymer electrolytes (SPEs) and unstable Li/PAN interface hinder the applications of PAN in SSLMBs. Herein, a strategy of ring-opening polymerization is proposed to reconfigure the PAN-based SPE network. Triggered by the alkaline species from Li6.4La3Zr1.4Ta0.6O12 nanoparticles, ethylene carbonate (EC) undergoes nucleophilic ring-opening reaction, and subsequently forms dipole–dipole interaction with the PAN chain. This polymerization process consequently reconfigures PAN segment, endowing the SPE with rapid Li+ transport channels and enhanced interfacial stability with Li metal. As a result, the designed PAN-based SPE demonstrates high ionic conductivity of 2.96 × 10−4 S cm−1 and Li+ transference number of 0.56 at 25 °C. The Li/Li symmetric cells with the reconfigured PAN network deliver a high critical current density of 1.8 mA cm−2 and maintain stable Li plating/stripping for 1200 h. A high-capacity retention of 90.1% after 1000 cycles at 2 C is achieved in LiFePO4 (LFP)/Li solid-state cells with PAN-based SPEs. Moreover, the LFP/Li and LiNi0.8Co0.1Co0.1O2/Graphite pouch batteries both present good cycling and safety performances. This strategy provides new insights into designing high-performance PAN-based SPE for SSLMBs.
聚丙烯腈（PAN）是一种用于固态锂（Li）金属电池（SSLMB）的前景广阔的聚合物。然而，PAN 基固体聚合物电解质（SPE）的低离子电导率和不稳定的 Li/PAN 界面阻碍了 PAN 在 SSLMB 中的应用。本文提出了一种开环聚合策略来重构 PAN 基固态聚合物电解质网络。在来自 Li6.4La3Zr1.4Ta0.6O12 纳米粒子的碱性物质的触发下，碳酸乙烯（EC）发生亲核开环反应，随后与 PAN 链形成偶极-偶极相互作用。这一聚合过程使 PAN 链段发生重构，从而使 SPE 具有快速的 Li+ 传输通道，并增强了与锂金属的界面稳定性。因此，所设计的基于 PAN 的固相萃取剂在 25 °C 时具有 2.96 × 10-4 S cm-1 的高离子电导率和 0.56 的 Li+ 传输数。使用重构 PAN 网络的锂/锂对称电池可提供 1.8 mA cm-2 的高临界电流密度，并可在 1200 小时内保持稳定的锂镀层/剥离。此外，LFP/锂电池和 LiNi0.8Co0.1Co0.1O2/Graphite 袋式电池都具有良好的循环和安全性能。这一策略为设计用于 SSLMB 的高性能 PAN 基固相萃取剂提供了新的思路。
{"title":"Ring-Opening Polymerization Reconfigures Polyacrylonitrile Network for Ultra Stable Solid-State Lithium Metal Batteries","authors":"Han Liu, Yaqi Liao, Chihon Leung, Yangqian Zhang, Yuewen Yang, Fangyan Liu, Ying Wei, Che Fan, Shuoxiao Zhang, Donghai Wang, Jie Yan, Qi Liu, Chiyuen Chung, Yang Ren, Yunhui Huang, Jiayi Yang","doi":"10.1002/aenm.202402795","DOIUrl":"https://doi.org/10.1002/aenm.202402795","url":null,"abstract":"Polyacrylonitrile (PAN) is a promising polymer for solid-state lithium (Li) metal batteries (SSLMBs). However, the low ionic conductivity of PAN-based solid polymer electrolytes (SPEs) and unstable Li/PAN interface hinder the applications of PAN in SSLMBs. Herein, a strategy of ring-opening polymerization is proposed to reconfigure the PAN-based SPE network. Triggered by the alkaline species from Li<sub>6.4</sub>La<sub>3</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>12</sub> nanoparticles, ethylene carbonate (EC) undergoes nucleophilic ring-opening reaction, and subsequently forms dipole–dipole interaction with the PAN chain. This polymerization process consequently reconfigures PAN segment, endowing the SPE with rapid Li<sup>+</sup> transport channels and enhanced interfacial stability with Li metal. As a result, the designed PAN-based SPE demonstrates high ionic conductivity of 2.96 × 10<sup>−4</sup> S cm<sup>−1</sup> and Li<sup>+</sup> transference number of 0.56 at 25 °C. The Li/Li symmetric cells with the reconfigured PAN network deliver a high critical current density of 1.8 mA cm<sup>−2</sup> and maintain stable Li plating/stripping for 1200 h. A high-capacity retention of 90.1% after 1000 cycles at 2 C is achieved in LiFePO<sub>4</sub> (LFP)/Li solid-state cells with PAN-based SPEs. Moreover, the LFP/Li and LiNi<sub>0.8</sub>Co<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub>/Graphite pouch batteries both present good cycling and safety performances. This strategy provides new insights into designing high-performance PAN-based SPE for SSLMBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142369902","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}
Monolayer atomic crystals show significant advantages in improving charge storage kinetics for electrode materials. While notable progress is made, challenges remain in producing nanocrystals with desirable configurations, dimensions, and crystallographic properties. Here, 1D single-crystal nanobelts assembled from monolayer sodium titanate nanobelts are reported with highly exposed active sites as anode materials for sodium-ion batteries (SIBs). The unique structural properties of the 1D single-crystal nanobelts offer excellent electrochemical activity, electrochemo-mechanical stability, and well-maintained structural integrity, leading to highly efficient sodium ion storage performance. Insights into the electrochemical reaction processes, as revealed by in situ transmission electron microscopy, in situ synchrotron X-ray diffraction, and theoretical calculations, indicate that the 1D single-crystal nanobelts enable favorable sodium ion storage kinetics and a low-strain characteristic. This facilitates fast charge/discharge capability and long-term cycling stability for up to 5000 cycles at 20 C. Moreover, the 1D single-crystal nanobelts demonstrate practical applicability. A pouch cell assembled with the 1D single-crystal nanobelts anode and iron-based Prussian blue cathode exhibits highly stable cycling, achieving a low capacity fading ratio of ≈0.05% per cycle over 150 cycles. This study provides an innovative design principle to enhance the charge storage capability of electrode materials through intelligent structural nanoengineering.
单层原子晶体在改善电极材料的电荷储存动力学方面具有显著优势。虽然取得了显著进展，但在生产具有理想构型、尺寸和晶体学特性的纳米晶体方面仍存在挑战。本文报告了由单层钛酸钠纳米颗粒组装而成的一维单晶纳米颗粒，其活性位点高度暴露，可作为钠离子电池（SIB）的负极材料。一维单晶纳米颗粒的独特结构特性提供了优异的电化学活性、电化学机械稳定性和良好的结构完整性，从而实现了高效的钠离子存储性能。原位透射电子显微镜、原位同步辐射 X 射线衍射和理论计算对电化学反应过程的深入研究表明，一维单晶纳米颗粒具有良好的钠离子存储动力学和低应变特性。此外，一维单晶纳米颗粒还证明了其实用性。由一维单晶纳米颗粒阳极和铁基普鲁士蓝阴极组装而成的袋式电池具有高度稳定的循环性能，在 150 个循环周期内，每个循环的容量衰减率低至≈0.05%。这项研究为通过智能结构纳米工程增强电极材料的电荷存储能力提供了一种创新的设计原理。
{"title":"Monolayer Sodium Titanate Nanobelts as a Highly Efficient Anode Material for Sodium-Ion Batteries","authors":"Qingbing Xia, Yaru Liang, Emily R. Cooper, Cheng-Lin Ko, Zhe Hu, Weijie Li, Shulei Chou, Ruth Knibbe","doi":"10.1002/aenm.202400929","DOIUrl":"https://doi.org/10.1002/aenm.202400929","url":null,"abstract":"Monolayer atomic crystals show significant advantages in improving charge storage kinetics for electrode materials. While notable progress is made, challenges remain in producing nanocrystals with desirable configurations, dimensions, and crystallographic properties. Here, 1D single-crystal nanobelts assembled from monolayer sodium titanate nanobelts are reported with highly exposed active sites as anode materials for sodium-ion batteries (SIBs). The unique structural properties of the 1D single-crystal nanobelts offer excellent electrochemical activity, electrochemo-mechanical stability, and well-maintained structural integrity, leading to highly efficient sodium ion storage performance. Insights into the electrochemical reaction processes, as revealed by in situ transmission electron microscopy, in situ synchrotron X-ray diffraction, and theoretical calculations, indicate that the 1D single-crystal nanobelts enable favorable sodium ion storage kinetics and a low-strain characteristic. This facilitates fast charge/discharge capability and long-term cycling stability for up to 5000 cycles at 20 C. Moreover, the 1D single-crystal nanobelts demonstrate practical applicability. A pouch cell assembled with the 1D single-crystal nanobelts anode and iron-based Prussian blue cathode exhibits highly stable cycling, achieving a low capacity fading ratio of ≈0.05% per cycle over 150 cycles. This study provides an innovative design principle to enhance the charge storage capability of electrode materials through intelligent structural nanoengineering.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142369904","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}
Aqueous nickel-based batteries, particularly nickel-organic batteries, are promising candidates for large-scale energy storage applications owing to their environmental friendliness, abundant resources, and intrinsic safety. However, organic anode materials suffer from serious dissolution in electrolytes during discharge/charge processes and ampere-hour-scale nickel-organic batteries are still absent. Here, phenazine (PZ) is screened as the anode and utilizes 10 m KOH as the electrolyte to construct ampere-hour-scale PZ/Ni(OH)2 batteries to demonstrate the practicability. In situ, UV–vis and molecular dynamics simulations demonstrate the inhibited dissolution of PZ in high-concentration of 10 m KOH. The PZ anode can provide a high initial specific capacity of 281.6 mAh g−1 at 0.5 C with a Coulombic efficiency of 98.6% and ultralong cycle life with a capacity retention of 74.3% after 14 000 cycles at 30 C. Moreover, the fabricated pouch-type PZ/Ni(OH)2 battery with a high PZ mass-loading of 48 mg cm−2 delivers a capacity of 1.23 Ah and achieves a high energy density of 50 Wh kg−1 (based on the total mass of the cell). The abundant resources, excellent stability, and cost-effectiveness of phenazine endow nickel-organic batteries with promising potential for large-scale energy storage applications.
{"title":"Ampere-Hour-Scale Aqueous Nickel–Organic Batteries based on Phenazine Anode","authors":"Xiaomeng Liu, Youxuan Ni, Zhuo Yang, Yong Lu, Weiwei Xie, Zhenhua Yan, Jun Chen","doi":"10.1002/aenm.202403628","DOIUrl":"https://doi.org/10.1002/aenm.202403628","url":null,"abstract":"Aqueous nickel-based batteries, particularly nickel-organic batteries, are promising candidates for large-scale energy storage applications owing to their environmental friendliness, abundant resources, and intrinsic safety. However, organic anode materials suffer from serious dissolution in electrolytes during discharge/charge processes and ampere-hour-scale nickel-organic batteries are still absent. Here, phenazine (PZ) is screened as the anode and utilizes 10 <span>m</span> KOH as the electrolyte to construct ampere-hour-scale PZ/Ni(OH)<sub>2</sub> batteries to demonstrate the practicability. In situ, UV–vis and molecular dynamics simulations demonstrate the inhibited dissolution of PZ in high-concentration of 10 <span>m</span> KOH. The PZ anode can provide a high initial specific capacity of 281.6 mAh g<sup>−1</sup> at 0.5 C with a Coulombic efficiency of 98.6% and ultralong cycle life with a capacity retention of 74.3% after 14 000 cycles at 30 C. Moreover, the fabricated pouch-type PZ/Ni(OH)<sub>2</sub> battery with a high PZ mass-loading of 48 mg cm<sup>−2</sup> delivers a capacity of 1.23 Ah and achieves a high energy density of 50 Wh kg<sup>−1</sup> (based on the total mass of the cell). The abundant resources, excellent stability, and cost-effectiveness of phenazine endow nickel-organic batteries with promising potential for large-scale energy storage applications.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142360432","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}
Giovanni Ferro, Camille Roiron, Hanson Wang, Jonathan Braaten, Björn M. Stühmeier, Christina Johnston, Lei Cheng, Iryna V. Zenyuk, Plamen Atanassov
For global deployment of proton exchange membrane fuel cells, achieving optimal interaction between the components of the cathode active layer remains challenging. Studies addressing the effect of nanoparticle location (inside vs outside of pores) on performance and durability mostly compare porous and nonporous carbon supports, thus coming short of decoupling nanoparticle locality from carbon support effects. To address the influence of nanoparticle locality on performance and durability, new carbon-supported electrocatalysts with designed and distinct nanoparticle localities are presented. The developed methodology allows to place Pt nanoparticles preferentially inside or outside of the mesopores of conductive carbon supports from materials under development at Cabot Corporation. Synthesis protocols are tuned to control nanoparticle size, crystallinity, and loading; this way the effect of Pt locality can be studied for two experimental carbon supports in isolation from all other parameters. For one carbon support, Pt active surface area and activity are significantly lower when nanoparticles are placed inside the pores. In contrast, for another, more graphitic carbon support, placing nanoparticles inside or outside of the carbon pores produces no appreciable difference in active surface area and performance rotating disk electrode measurements. Given their carefully tailored structure, these catalysts provide a framework for evaluating locality-performance-durability relationships.
{"title":"Designer Electrocatalysts for the Oxygen Reduction Reaction with Controlled Platinum Nanoparticle Locality","authors":"Giovanni Ferro, Camille Roiron, Hanson Wang, Jonathan Braaten, Björn M. Stühmeier, Christina Johnston, Lei Cheng, Iryna V. Zenyuk, Plamen Atanassov","doi":"10.1002/aenm.202403165","DOIUrl":"https://doi.org/10.1002/aenm.202403165","url":null,"abstract":"For global deployment of proton exchange membrane fuel cells, achieving optimal interaction between the components of the cathode active layer remains challenging. Studies addressing the effect of nanoparticle location (inside vs outside of pores) on performance and durability mostly compare porous and nonporous carbon supports, thus coming short of decoupling nanoparticle locality from carbon support effects. To address the influence of nanoparticle locality on performance and durability, new carbon-supported electrocatalysts with designed and distinct nanoparticle localities are presented. The developed methodology allows to place Pt nanoparticles preferentially inside or outside of the mesopores of conductive carbon supports from materials under development at Cabot Corporation. Synthesis protocols are tuned to control nanoparticle size, crystallinity, and loading; this way the effect of Pt locality can be studied for two experimental carbon supports in isolation from all other parameters. For one carbon support, Pt active surface area and activity are significantly lower when nanoparticles are placed inside the pores. In contrast, for another, more graphitic carbon support, placing nanoparticles inside or outside of the carbon pores produces no appreciable difference in active surface area and performance rotating disk electrode measurements. Given their carefully tailored structure, these catalysts provide a framework for evaluating locality-performance-durability relationships.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142360573","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}
Chuanjun Zhang, Ruihao Jiang, Yonghui Zheng, Yaozhen Li, Zenghua Cai, Chunlan Ma, Yan Cheng, Junhao Chu, Jiahua Tao
Quasi-1D antimony selenide (Sb2Se3) is known for its stable phase structure and excellent light absorption coefficient, making it a promising material for high-efficiency light harvesting. However, the (Sb4Se6)n ribbons align horizontally, increasing defect interference and limiting vertical carrier transport. Herein, a novel strategy of burying selenium (Se) seed layers to reduce lattice mismatch at the heterojunction interface, promote crystal orientation, mitigate deep donor defects, increase P-type carrier concentration, and purify the PN junction, is proposed. Admittance spectroscopy reveals that Sb2Se3 solar cells with Se seed layers have higher activation energies for defect states and significantly lower defect densities (1.2 × 1014, 2.7 × 1014, and 1.3 × 1015 cm−3 for D1, D2, and D3) compared to an order of magnitude higher densities in Sb2Se3 solar cells without a Se seed layer. First-principles calculations support these findings, showing that Se seed layers create a Se-rich environment, reducing selenium vacancies (VSe), antimony on selenium sites (SbSe), and interface defects. This dual passivation mechanism suppresses defect formation and activation, increasing carrier concentration and open-circuit voltage (VOC). Ultimately, employing this novel method, a VOC of 498.3 mV and an efficiency of 8.42%, the highest performance reported for Sb2Se3 solar cells prepared via vapor transport deposition (VTD), are achieved.
{"title":"Mechanism of Defect Passivation in Sb2Se3 Solar Cells via Buried Selenium Seed Layer","authors":"Chuanjun Zhang, Ruihao Jiang, Yonghui Zheng, Yaozhen Li, Zenghua Cai, Chunlan Ma, Yan Cheng, Junhao Chu, Jiahua Tao","doi":"10.1002/aenm.202403352","DOIUrl":"https://doi.org/10.1002/aenm.202403352","url":null,"abstract":"Quasi-1D antimony selenide (Sb<sub>2</sub>Se<sub>3</sub>) is known for its stable phase structure and excellent light absorption coefficient, making it a promising material for high-efficiency light harvesting. However, the (Sb<sub>4</sub>Se<sub>6</sub>)<sub>n</sub> ribbons align horizontally, increasing defect interference and limiting vertical carrier transport. Herein, a novel strategy of burying selenium (Se) seed layers to reduce lattice mismatch at the heterojunction interface, promote crystal orientation, mitigate deep donor defects, increase P-type carrier concentration, and purify the PN junction, is proposed. Admittance spectroscopy reveals that Sb<sub>2</sub>Se<sub>3</sub> solar cells with Se seed layers have higher activation energies for defect states and significantly lower defect densities (1.2 × 10<sup>14</sup>, 2.7 × 10<sup>14</sup>, and 1.3 × 10<sup>15</sup> cm<sup>−3</sup> for D1, D2, and D3) compared to an order of magnitude higher densities in Sb<sub>2</sub>Se<sub>3</sub> solar cells without a Se seed layer. First-principles calculations support these findings, showing that Se seed layers create a Se-rich environment, reducing selenium vacancies (<i>V</i><sub>Se</sub>), antimony on selenium sites (<i>Sb</i><sub>Se</sub>), and interface defects. This dual passivation mechanism suppresses defect formation and activation, increasing carrier concentration and open-circuit voltage (<i>V</i><sub>OC</sub>). Ultimately, employing this novel method, a <i>V</i><sub>OC</sub> of 498.3 mV and an efficiency of 8.42%, the highest performance reported for Sb<sub>2</sub>Se<sub>3</sub> solar cells prepared via vapor transport deposition (VTD), are achieved.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142330280","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}
Na metal batteries (NMBs) stand at the forefront of advancing energy storage technologies, but are severely hampered by Na dendrite issues, especially when using carbonate electrolytes. Suppressing the growth of Na dendrites through constructing NaF-rich solid-electrolyte-interphase (SEI) is a commonly-used strategy to prolong the lifespan of NMBs. In contrast, fluorinated organic SEI components are often underutilized. Inspired by unveiling the adsorption configuration of fluorinated organic compounds on the surface of Na metal, an optimized SEI architecture for stabilizing NMBs is proposed by investigating the C4H9SO2F-/C4F9SO2F-treated Na metal anodes. It is revealed that the SEI built on a fluorinated inorganic/organic hybrid layer exhibit favorable Na passivation capability, significantly improving Na deposition behavior. As a result, the NMB with a high-loading cathode (15 mg cm−2) and a negative/positive capacity ratio (N/P) ratio of 4 shows a long-term life span over 1000 cycles with 92.8% capacity retention at 2 C. This work opens a new pathway for developing robust and high-energy-density NMBs.
镍金属电池（NMB）是先进储能技术的前沿，但却受到镍枝晶问题的严重阻碍，尤其是在使用碳酸盐电解质时。通过构建富含 NaF 的固态电解质间相（SEI）来抑制 Na 树枝的生长，是延长 NMB 寿命的常用策略。相比之下，含氟有机 SEI 成分往往未得到充分利用。受揭示含氟有机化合物在 Na 金属表面吸附构型的启发，通过研究 C4H9SO2F-/C4F9SO2F 处理过的 Na 金属阳极，提出了一种用于稳定 NMB 的优化 SEI 结构。研究表明，建立在含氟无机/有机杂化层上的 SEI 具有良好的 Na 钝化能力，可显著改善 Na 沉积行为。因此，高负载阴极（15 mg cm-2）和负/正容量比（N/P）为 4 的 NMB 在 2 C 条件下可长期使用 1000 次，容量保持率达 92.8%。
{"title":"Highly Stable Sodium Metal Batteries Enabled by Manipulating the Fluorinated Organic Components of Solid-Electrolyte-Interphase","authors":"Chaozhi Wang, Shuqi Dai, Kaihang Wu, Shuchang Liu, Jingqin Cui, Yu Shi, Xinrui Cao, Qiulong Wei, Xiaoliang Fang, Nanfeng Zheng","doi":"10.1002/aenm.202402711","DOIUrl":"https://doi.org/10.1002/aenm.202402711","url":null,"abstract":"Na metal batteries (NMBs) stand at the forefront of advancing energy storage technologies, but are severely hampered by Na dendrite issues, especially when using carbonate electrolytes. Suppressing the growth of Na dendrites through constructing NaF-rich solid-electrolyte-interphase (SEI) is a commonly-used strategy to prolong the lifespan of NMBs. In contrast, fluorinated organic SEI components are often underutilized. Inspired by unveiling the adsorption configuration of fluorinated organic compounds on the surface of Na metal, an optimized SEI architecture for stabilizing NMBs is proposed by investigating the C<sub>4</sub>H<sub>9</sub>SO<sub>2</sub>F-/C<sub>4</sub>F<sub>9</sub>SO<sub>2</sub>F-treated Na metal anodes. It is revealed that the SEI built on a fluorinated inorganic/organic hybrid layer exhibit favorable Na passivation capability, significantly improving Na deposition behavior. As a result, the NMB with a high-loading cathode (15 mg cm<sup>−2</sup>) and a negative/positive capacity ratio (N/P) ratio of 4 shows a long-term life span over 1000 cycles with 92.8% capacity retention at 2 C. This work opens a new pathway for developing robust and high-energy-density NMBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329953","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}
Tianchi Zhang, Tiantian Liu, Xingtao Wang, Yuhan Zhou, Yehui Wen, Junhang Li, Chunqiong Bao, Li Wan, Xuegong Yu, Weihua Ning, Yong Wang, Deren Yang
State-of-the-art inverted perovskite solar cells (PSCs) have exhibited considerable promise for commercialization due to their prospective stability. However, the intricate crystallization of halide perovskite, especially for multi-component perovskites, not only distorts the surface lattice from its ideal form but also introduces numerous unsaturated dangling bonds to form surface defects, which can easily lead to reduced stability and poor performance. Herein, a surface lattice engineering is developed by coupling surface unsaturated ions and regulating ion bonding lengths/angles to achieve efficient and stable inverted PSCs. The renovated surface lattice not only eliminates shallow/deep level defects on the surface of perovskite, but also enhances photo/thermal stability of the materials. Moreover, the surface lattice engineering contributes to uniform potential surface, and improves energy-level alignment at the interfaces of the perovskite and C60 carrier transport layer, enhancing charge carrier extraction and transportation. Finally, the champion PSC delivers an impressive efficiency of 25.82% (certified 25.5%). Moreover, these PSCs exhibit excellent operational stability, retaining 94% initial efficiency after more than ≈1 000h maximum power point test.
{"title":"Surface Lattice Engineering Enables Efficient Inverted Perovskite Solar Cells","authors":"Tianchi Zhang, Tiantian Liu, Xingtao Wang, Yuhan Zhou, Yehui Wen, Junhang Li, Chunqiong Bao, Li Wan, Xuegong Yu, Weihua Ning, Yong Wang, Deren Yang","doi":"10.1002/aenm.202403554","DOIUrl":"https://doi.org/10.1002/aenm.202403554","url":null,"abstract":"State-of-the-art inverted perovskite solar cells (PSCs) have exhibited considerable promise for commercialization due to their prospective stability. However, the intricate crystallization of halide perovskite, especially for multi-component perovskites, not only distorts the surface lattice from its ideal form but also introduces numerous unsaturated dangling bonds to form surface defects, which can easily lead to reduced stability and poor performance. Herein, a surface lattice engineering is developed by coupling surface unsaturated ions and regulating ion bonding lengths/angles to achieve efficient and stable inverted PSCs. The renovated surface lattice not only eliminates shallow/deep level defects on the surface of perovskite, but also enhances photo/thermal stability of the materials. Moreover, the surface lattice engineering contributes to uniform potential surface, and improves energy-level alignment at the interfaces of the perovskite and C<sub>60</sub> carrier transport layer, enhancing charge carrier extraction and transportation. Finally, the champion PSC delivers an impressive efficiency of 25.82% (certified 25.5%). Moreover, these PSCs exhibit excellent operational stability, retaining 94% initial efficiency after more than ≈1 000h maximum power point test.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142330281","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}
Jianhui Zhu, Jie Tai, Tao Liu, Yanyi Wang, Yinyin Li, Ming Yang, Dingtao Ma, Libo Deng, Jingting Luo, Peixin Zhang
The development of high energy/power density and long lifespan device is always the frontier direction and attracts great research attention in the energy storage fields. Zinc-ion capacitors (ZICs), as an integration of zinc-ion batteries and supercapacitors, have been widely regarded as one of the viable future options for energy storage, owing to their variable system assembly method and potential performance improvement. However, the research of ZICs still locate at initial stage until now, and how to construct the suitable systems for different condition is still challenging. Herein, the recent advance in the rational design of ZICs is reviewed in order to construct related theory including compatible principle and design paradigm. It starts with a systematically summary of the fundamental theory as well as the motivation. Then, the electrode materials are classified into capacitor-type and battery-type based on the storage mechanism, and the design strategies and progress of these two-type candidates are comprehensively discussed, aiming to reveal the inherent relationship between the performance of devices and the component as well as architecture of electrode materials. Beyond that, the future perspectives in this emerging field are also given, expecting to guide the construction of high-performance ZICs for practical applications and boost its development.
{"title":"Emerging Zinc-Ion Capacitor Science: Compatible Principle, Design Paradigm, and Frontier Applications","authors":"Jianhui Zhu, Jie Tai, Tao Liu, Yanyi Wang, Yinyin Li, Ming Yang, Dingtao Ma, Libo Deng, Jingting Luo, Peixin Zhang","doi":"10.1002/aenm.202403739","DOIUrl":"https://doi.org/10.1002/aenm.202403739","url":null,"abstract":"The development of high energy/power density and long lifespan device is always the frontier direction and attracts great research attention in the energy storage fields. Zinc-ion capacitors (ZICs), as an integration of zinc-ion batteries and supercapacitors, have been widely regarded as one of the viable future options for energy storage, owing to their variable system assembly method and potential performance improvement. However, the research of ZICs still locate at initial stage until now, and how to construct the suitable systems for different condition is still challenging. Herein, the recent advance in the rational design of ZICs is reviewed in order to construct related theory including compatible principle and design paradigm. It starts with a systematically summary of the fundamental theory as well as the motivation. Then, the electrode materials are classified into capacitor-type and battery-type based on the storage mechanism, and the design strategies and progress of these two-type candidates are comprehensively discussed, aiming to reveal the inherent relationship between the performance of devices and the component as well as architecture of electrode materials. Beyond that, the future perspectives in this emerging field are also given, expecting to guide the construction of high-performance ZICs for practical applications and boost its development.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142330243","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}
Qi Tang, Qi Hao, Qian Zhu, Junxiu Wu, Keke Huang, Kai Liu, Jun Lu
The metal–metal (M1–M2) interactions in heteronuclear dual-atom catalysts (HNDACs) significantly optimize the electronic properties of the active sites, resulting in the promotion of the reaction kinetics in electrocatalysis. However, the regulation mechanisms in these M1–M2 dual-atom sites still remain unclear. Herein, the intrinsic electron transfer in Fe–Zn dual-atom sites are revealed for facilitating electrocatalytic carbon dioxide reduction (ECO2R) to carbon monoxide (CO). The electronegativity difference between the Fe and Zn centers induces the specific electron transfer from Zn to Fe, which regulates the electron structures of the active Zn sites, leading to the optimized reaction pathway of CO2-to-CO conversion on these sites. The Fe–Zn HNDAC (FeZnNC) exhibits superior ECO2R performances than the single-atom Fe/Zn catalysts (FeNC and ZnNC) in the typical H-cell system, the maximum CO partial current density on FeZnNC reaches more than 3.3 and 1.8 folds of those on FeNC and ZnNC, respectively. More importantly, in a strongly acidic medium (pH = 1), FeZnNC achieves CO Faradaic efficiencies greater than 94% in the current density range of 100–400 mA cm−2. This work uncovers the intrinsic electron transfer at the heteronuclear diatomic sites, providing new insights for the rational design of high-performance HNDACs toward industrial electrocatalysis.
异核双原子催化剂（HNDACs）中的金属-金属（M1-M2）相互作用极大地优化了活性位点的电子特性，从而促进了电催化反应动力学。然而，这些 M1-M2 双原子位点的调节机制仍不清楚。本文揭示了铁锌双原子位点的内在电子传递，以促进电催化二氧化碳还原（ECO2R）为一氧化碳（CO）的反应。铁和锌中心的电负性差异诱导了特定的电子从锌转移到铁，从而调节了活性锌位点的电子结构，优化了这些位点上 CO2 到 CO 的转化反应途径。与单原子铁/锌催化剂（FeNC 和 ZnNC）相比，FeZn HNDAC（FeZnNC）在典型的氢电池体系中表现出更优越的 ECO2R 性能，FeZnNC 上的最大 CO 部分电流密度分别达到 FeNC 和 ZnNC 上的 3.3 倍和 1.8 倍以上。更重要的是，在强酸性介质（pH = 1）中，FeZnNC 在 100-400 mA cm-2 的电流密度范围内实现了超过 94% 的 CO 法拉第效率。这项工作揭示了异核二原子位点的内在电子传递，为合理设计高性能 HNDACs 实现工业电催化提供了新的见解。
{"title":"Intrinsic Electron Transfer in Heteronuclear Dual-Atom Sites Facilitates Selective Electrocatalytic Carbon Dioxide Reduction","authors":"Qi Tang, Qi Hao, Qian Zhu, Junxiu Wu, Keke Huang, Kai Liu, Jun Lu","doi":"10.1002/aenm.202403778","DOIUrl":"https://doi.org/10.1002/aenm.202403778","url":null,"abstract":"The metal–metal (M<sub>1</sub>–M<sub>2</sub>) interactions in heteronuclear dual-atom catalysts (HNDACs) significantly optimize the electronic properties of the active sites, resulting in the promotion of the reaction kinetics in electrocatalysis. However, the regulation mechanisms in these M<sub>1</sub>–M<sub>2</sub> dual-atom sites still remain unclear. Herein, the intrinsic electron transfer in Fe–Zn dual-atom sites are revealed for facilitating electrocatalytic carbon dioxide reduction (ECO<sub>2</sub>R) to carbon monoxide (CO). The electronegativity difference between the Fe and Zn centers induces the specific electron transfer from Zn to Fe, which regulates the electron structures of the active Zn sites, leading to the optimized reaction pathway of CO<sub>2</sub>-to-CO conversion on these sites. The Fe–Zn HNDAC (FeZnNC) exhibits superior ECO<sub>2</sub>R performances than the single-atom Fe/Zn catalysts (FeNC and ZnNC) in the typical H-cell system, the maximum CO partial current density on FeZnNC reaches more than 3.3 and 1.8 folds of those on FeNC and ZnNC, respectively. More importantly, in a strongly acidic medium (pH = 1), FeZnNC achieves CO Faradaic efficiencies greater than 94% in the current density range of 100–400 mA cm<sup>−2</sup>. This work uncovers the intrinsic electron transfer at the heteronuclear diatomic sites, providing new insights for the rational design of high-performance HNDACs toward industrial electrocatalysis.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142330282","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}
Wei Li, Ying Xu, Guanhua Wang, Ting Xu, Chuanling Si
Silicon/carbon (Si/C) composites present great potential as anode materials for rechargeable batteries since the materials integrate the high specific capacity and the preferable cycling stability from Si and C components, respectively. Functional Si/C composites based on lignocellulose have attracted wide attention due to the advantages from lignocellulose, including sustainability property, flexible structural tunability, and diverse physicochemical functionality. Although the flourishing development of rechargeable batteries boosts the studies on lignocellulose-derived Si/C materials with high electrochemical performance, the publications that comprehensively clarify the design and functionalization of these high-profile materials are still scarce. Accordingly, this review first systematically summarizes the recent advances in the structural design of lignocellulose-derived Si/C composites after a brief clarification about the Si selection sources based on self and extraneous sources. Afterward, the functionalization strategies, including nanosizing, porosification, and magnesiothermic reduction of Si material as well as heteroatom modification of C material, are specifically highlighted. Besides, the applications of lignocellulose-derived Si/C-based materials in rechargeable batteries are elaborated. Finally, this review discusses the challenges and prospects of the application of lignocellulose-derived Si/C composites for energy storage and provides a nuanced viewpoint regarding this topic.
{"title":"Design and Functionalization of Lignocellulose-Derived Silicon-Carbon Composites for Rechargeable Batteries","authors":"Wei Li, Ying Xu, Guanhua Wang, Ting Xu, Chuanling Si","doi":"10.1002/aenm.202403593","DOIUrl":"https://doi.org/10.1002/aenm.202403593","url":null,"abstract":"Silicon/carbon (Si/C) composites present great potential as anode materials for rechargeable batteries since the materials integrate the high specific capacity and the preferable cycling stability from Si and C components, respectively. Functional Si/C composites based on lignocellulose have attracted wide attention due to the advantages from lignocellulose, including sustainability property, flexible structural tunability, and diverse physicochemical functionality. Although the flourishing development of rechargeable batteries boosts the studies on lignocellulose-derived Si/C materials with high electrochemical performance, the publications that comprehensively clarify the design and functionalization of these high-profile materials are still scarce. Accordingly, this review first systematically summarizes the recent advances in the structural design of lignocellulose-derived Si/C composites after a brief clarification about the Si selection sources based on self and extraneous sources. Afterward, the functionalization strategies, including nanosizing, porosification, and magnesiothermic reduction of Si material as well as heteroatom modification of C material, are specifically highlighted. Besides, the applications of lignocellulose-derived Si/C-based materials in rechargeable batteries are elaborated. Finally, this review discusses the challenges and prospects of the application of lignocellulose-derived Si/C composites for energy storage and provides a nuanced viewpoint regarding this topic.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142330278","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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