ZnIn2S4 (ZIS) has garnered significant interest in photocatalytic energy conversion and environmental remediation due to its tunable band gap, strong visible-light response, and facile synthesis. However, its practical application is severely hindered by inherent limitations, including low charge carrier separation efficiency and sluggish surface reaction kinetics. Constructing heterojunctions has emerged as an effective strategy to enhance ZIS performance by leveraging precise band alignment and interface engineering to optimize charge separation. While excellent reviews on ZIS-based photocatalysis have been published, comprehensive reviews focusing specifically on the design and evaluation of ZIS-based heterojunctions remain scarce. This review systematically summarizes recent advances in ZIS-based heterojunctions, providing a detailed discussion of heterojunction types and key synthesis strategies. Multi-scale modification strategies for synergistically enhancing photocatalytic activity are also examined. Furthermore, the charge separation mechanisms and surface reaction pathways are elucidated through advanced in situ characterization techniques and density functional theory (DFT) calculations. ZIS-based heterojunctions demonstrate great potential across various photocatalytic applications, including H2 evolution, CO2 reduction, H2O2 production, N2 fixation, pollutant degradation, and emerging fields such as plastic reforming and tumor therapy. Finally, future research directions are outlined, encompassing crystal phase regulation, adaptive heterojunction design, and AI-driven screening, thereby providing theoretical guidance for the development of highly efficient ZIS-based photocatalysts.
{"title":"Unveiling Cutting-Edge Advancements in ZnIn2S4-Based Heterojunctions for Photocatalysis","authors":"Jipeng Fan, Yueting Zhang, Jing Zou, Haitao Wang","doi":"10.1002/cnl2.70081","DOIUrl":"https://doi.org/10.1002/cnl2.70081","url":null,"abstract":"<p>ZnIn<sub>2</sub>S<sub>4</sub> (ZIS) has garnered significant interest in photocatalytic energy conversion and environmental remediation due to its tunable band gap, strong visible-light response, and facile synthesis. However, its practical application is severely hindered by inherent limitations, including low charge carrier separation efficiency and sluggish surface reaction kinetics. Constructing heterojunctions has emerged as an effective strategy to enhance ZIS performance by leveraging precise band alignment and interface engineering to optimize charge separation. While excellent reviews on ZIS-based photocatalysis have been published, comprehensive reviews focusing specifically on the design and evaluation of ZIS-based heterojunctions remain scarce. This review systematically summarizes recent advances in ZIS-based heterojunctions, providing a detailed discussion of heterojunction types and key synthesis strategies. Multi-scale modification strategies for synergistically enhancing photocatalytic activity are also examined. Furthermore, the charge separation mechanisms and surface reaction pathways are elucidated through advanced in situ characterization techniques and density functional theory (DFT) calculations. ZIS-based heterojunctions demonstrate great potential across various photocatalytic applications, including H<sub>2</sub> evolution, CO<sub>2</sub> reduction, H<sub>2</sub>O<sub>2</sub> production, N<sub>2</sub> fixation, pollutant degradation, and emerging fields such as plastic reforming and tumor therapy. Finally, future research directions are outlined, encompassing crystal phase regulation, adaptive heterojunction design, and AI-driven screening, thereby providing theoretical guidance for the development of highly efficient ZIS-based photocatalysts.</p>","PeriodicalId":100214,"journal":{"name":"Carbon Neutralization","volume":"5 1","pages":""},"PeriodicalIF":12.0,"publicationDate":"2025-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cnl2.70081","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145739897","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}
Electrochromic (EC) fabrics exhibiting tunable optical and thermal modulation have attracted extensive attention in both active camouflage and wearable electronic. However, the lack of compatibility among the basic components of an EC device for flexible EC fabrics remains a challenge, hindering its future application. Herein, a highly integrated all-in-one EC fabric (AECF) is developed by assembling all the essential components into a piece of fabric, which is based on the dual-band EC polyaniline (PANI), Au collector, and a gel electrolyte filled into the fabric matrix. Benefiting from such a highly integrated configuration, the AECF possesses an ultrathin thickness of 82.0 μm and high flexibility, which could endow it with good conformity on arbitrarily shaped surfaces, further enhancing the applicability of the intrinsically non-stretchable EC fabrics device. Stemming from the optical modulation of the PANI EC layers, the AECF exhibits a color switch between golden yellow and dark green, with both visible and infrared reflectance modulation. Considering the excellent conformability and active optical-thermal modulation, the AECF is further developed into an environmental adaptive camouflage prototype system by integrating with a model car, which exhibits a fast color blending with dynamic environment background. This study is anticipated to provide new insights into developing high-performance EC fabrics toward the applications in wearable displays and active military camouflage.
{"title":"Robust Electrochromic Fabrics Compatible With Arbitrary Surface for Active Optical and Thermal Modulations","authors":"Yuhao Wang, Wanzhong Li, Hui Gong, Ang Li, Mingyu Ding, Jingbing Liu, Zilong Zheng, Hao Wang, Qianqian Zhang","doi":"10.1002/cnl2.70090","DOIUrl":"https://doi.org/10.1002/cnl2.70090","url":null,"abstract":"<p>Electrochromic (EC) fabrics exhibiting tunable optical and thermal modulation have attracted extensive attention in both active camouflage and wearable electronic. However, the lack of compatibility among the basic components of an EC device for flexible EC fabrics remains a challenge, hindering its future application. Herein, a highly integrated all-in-one EC fabric (AECF) is developed by assembling all the essential components into a piece of fabric, which is based on the dual-band EC polyaniline (PANI), Au collector, and a gel electrolyte filled into the fabric matrix. Benefiting from such a highly integrated configuration, the AECF possesses an ultrathin thickness of 82.0 μm and high flexibility, which could endow it with good conformity on arbitrarily shaped surfaces, further enhancing the applicability of the intrinsically non-stretchable EC fabrics device. Stemming from the optical modulation of the PANI EC layers, the AECF exhibits a color switch between golden yellow and dark green, with both visible and infrared reflectance modulation. Considering the excellent conformability and active optical-thermal modulation, the AECF is further developed into an environmental adaptive camouflage prototype system by integrating with a model car, which exhibits a fast color blending with dynamic environment background. This study is anticipated to provide new insights into developing high-performance EC fabrics toward the applications in wearable displays and active military camouflage.</p>","PeriodicalId":100214,"journal":{"name":"Carbon Neutralization","volume":"5 1","pages":""},"PeriodicalIF":12.0,"publicationDate":"2025-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cnl2.70090","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145739663","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}
The pursuit of highly efficient energy storage technique represents the key drive for the global energy structure transformation towards future renewable society. The state-of-the-art Li/Na-ion secondary battery that relies on the intercalation reaction is now well-established as the primary technology by the virtue of high energy and power density as well as the environmental benign. Despite the advantage, tremendous effects have been made for the improvement of the electrochemical performance of Li/Na-ion battery to mitigate the huddle between existing technology and increasing application demand. One of the major challenges lies in the further improvement of the energy efficiency, which is closely related to the voltage hysteresis behavior. The existence of voltage hysteresis could reduce energy output efficiency and accelerates capacity fading thus hindering the practical applications. Due to the voltage hysteresis between charging and discharging, it may induce the part of the energy lost, which decreases the energy conversion efficiency, increases polarization at high rates, intensifies side reactions at high potentials, and reduces the cycle life. At the same time, it also leads to the dendrite growth, promotes gas generation, and increases the risk of thermal runaway. In this review, we systematical outline the previous research on the topic which would contribute to the fundamental understanding of the origination and mechanism of voltage hysteresis. Critical assessments of battery behavior upon cycling are presented in combination with summaries of multiple modification strategies to mitigate the hysteresis in both Li/Na-ion battery. The remaining problems and future prospectives are also proposed which are expected to facilitate for the rational design of advanced electrode materials. This, in our point of view, could inspire the novel insight into future battery development towards practical application as well.
{"title":"Fundamental Understanding of the Origin of Voltage Hysteresis and the Modification Strategy Towards the Development of Advanced Li/Na-Ion Batteries","authors":"Dianwu Kang, Tao Wang, Shuai Tong, Wenbo Li, Chao Zhu, Tianshu Yang, Zhijiang Zhou, Jianxin Yang, Xin Guo, Min Jia, Xiaoyu Zhang","doi":"10.1002/cnl2.70094","DOIUrl":"https://doi.org/10.1002/cnl2.70094","url":null,"abstract":"<p>The pursuit of highly efficient energy storage technique represents the key drive for the global energy structure transformation towards future renewable society. The state-of-the-art Li/Na-ion secondary battery that relies on the intercalation reaction is now well-established as the primary technology by the virtue of high energy and power density as well as the environmental benign. Despite the advantage, tremendous effects have been made for the improvement of the electrochemical performance of Li/Na-ion battery to mitigate the huddle between existing technology and increasing application demand. One of the major challenges lies in the further improvement of the energy efficiency, which is closely related to the voltage hysteresis behavior. The existence of voltage hysteresis could reduce energy output efficiency and accelerates capacity fading thus hindering the practical applications. Due to the voltage hysteresis between charging and discharging, it may induce the part of the energy lost, which decreases the energy conversion efficiency, increases polarization at high rates, intensifies side reactions at high potentials, and reduces the cycle life. At the same time, it also leads to the dendrite growth, promotes gas generation, and increases the risk of thermal runaway. In this review, we systematical outline the previous research on the topic which would contribute to the fundamental understanding of the origination and mechanism of voltage hysteresis. Critical assessments of battery behavior upon cycling are presented in combination with summaries of multiple modification strategies to mitigate the hysteresis in both Li/Na-ion battery. The remaining problems and future prospectives are also proposed which are expected to facilitate for the rational design of advanced electrode materials. This, in our point of view, could inspire the novel insight into future battery development towards practical application as well.</p>","PeriodicalId":100214,"journal":{"name":"Carbon Neutralization","volume":"5 1","pages":""},"PeriodicalIF":12.0,"publicationDate":"2025-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cnl2.70094","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145739664","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}
Aqueous electrolytes, while conferring inherent safety advantages, inevitably induce hydrogen-evolution corrosion, resulting in nonuniform Zn deposition and shortened cycle life. Herein, a novel electrolyte with buffering function is designed to modulate ion behavior and stabilize interface pH. The introduced additive acts as a cushion maskant (CM) that spontaneously adsorbs onto the Zn metal surface, displacing interfacial water molecules and thereby suppressing corrosion. Simultaneously, its coordination with Zn2+ homogenizes the Zn2+ flux to promote uniform deposition. Moreover, the protonation/deprotonation equilibria of CM within the electrolyte buffer local pH fluctuations, stabilizing the interfacial microenvironment. Consequently, a beneficial solid electrolyte interphase (SEI) is established, which further shields the Zn anode, enhances interfacial stability, and markedly improves cycling durability. Accordingly, Zn//Zn symmetrical cells in CM-containing electrolyte can realize exceptional lifespan for 2800 h at 2 mA cm−2 and 970 h even at 10 mA cm−2. In addition, CM demonstrates the superior practical applicability in Zn//I2 full cells for long-term and rate tests. Zn//I2 pouch full cell can operate for 150 mAh with CM. This study offers a distinctive and comprehensive strategy for stabilizing the Zn anode.
水溶液虽然具有固有的安全优势,但不可避免地会引起析氢腐蚀,导致锌沉积不均匀,缩短循环寿命。本文设计了一种具有缓冲功能的新型电解质,以调节离子行为并稳定界面ph。引入的添加剂作为缓冲质(CM),自发吸附在Zn金属表面,取代界面水分子,从而抑制腐蚀。同时,它与Zn2+的配位使Zn2+通量均匀化,促进沉积均匀。此外,CM的质子化/去质子化平衡可以缓冲电解质内的局部pH波动,稳定界面微环境。因此,建立了有益的固体电解质界面相(SEI),进一步屏蔽了Zn阳极,增强了界面稳定性,并显着提高了循环耐久性。因此,在含cm的电解液中,锌/锌对称电池在2 mA cm - 2下的寿命为2800 h,在10 mA cm - 2下的寿命为970 h。此外,CM在Zn//I2全电池的长期和倍率测试中具有优越的实用性。锌//I2袋全电池可在CM下工作150毫安时。该研究为稳定锌阳极提供了一种独特而全面的策略。
{"title":"Cushion-Maskant-Regulated Interfacial Chemistry Enables Durable Zinc Metal Anodes","authors":"Qiwen Zhao, Ying Chen, Wen Liu, Antai Zhu, Zikun Li, Hanwei He, Bingang Xu, Yuejiao Chen, Libao Chen","doi":"10.1002/cnl2.70088","DOIUrl":"https://doi.org/10.1002/cnl2.70088","url":null,"abstract":"<p>Aqueous electrolytes, while conferring inherent safety advantages, inevitably induce hydrogen-evolution corrosion, resulting in nonuniform Zn deposition and shortened cycle life. Herein, a novel electrolyte with buffering function is designed to modulate ion behavior and stabilize interface pH. The introduced additive acts as a cushion maskant (CM) that spontaneously adsorbs onto the Zn metal surface, displacing interfacial water molecules and thereby suppressing corrosion. Simultaneously, its coordination with Zn<sup>2+</sup> homogenizes the Zn<sup>2+</sup> flux to promote uniform deposition. Moreover, the protonation/deprotonation equilibria of CM within the electrolyte buffer local pH fluctuations, stabilizing the interfacial microenvironment. Consequently, a beneficial solid electrolyte interphase (SEI) is established, which further shields the Zn anode, enhances interfacial stability, and markedly improves cycling durability. Accordingly, Zn//Zn symmetrical cells in CM-containing electrolyte can realize exceptional lifespan for 2800 h at 2 mA cm<sup>−2</sup> and 970 h even at 10 mA cm<sup>−2</sup>. In addition, CM demonstrates the superior practical applicability in Zn//I<sub>2</sub> full cells for long-term and rate tests. Zn//I<sub>2</sub> pouch full cell can operate for 150 mAh with CM. This study offers a distinctive and comprehensive strategy for stabilizing the Zn anode.</p>","PeriodicalId":100214,"journal":{"name":"Carbon Neutralization","volume":"5 1","pages":""},"PeriodicalIF":12.0,"publicationDate":"2025-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cnl2.70088","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145739659","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}
The practical application of solid polymer electrolytes (SPE) is limited due to notorious high crystallinity and low ionic conductivity. Existing research concentrated on reducing crystallinity and increasing Li salt concentration have made certain process. However, the segmentation and isolation effects of large and numerous grains on amorphous region have always been overlooked and the effect of grain size remains largely unexplored. Herein, take polyethylene oxide (PEO) as an example, “grain size refinement” strategy is adopted to improve the related room-temperature ionic conductivity by simply placing PEO based SPE on Li sheets coated with ester monomers and conducting in-situ polymerization. During these processes, in addition to reducing the interaction force between polymer chains and decreasing the driving force for crystallization, ester monomers are conducive to form interface with polymer clusters, which serves as additional nucleation sites and promotes the formation of refined grains. Then instantaneous high-temperature provided by muffle furnace triggers rapid solidification of monomers, leading to the locking of refined grain structure and the formation of more interconnected amorphous regions. Time-of-flight secondary ion mass spectrometry and polarization microscope confirm these processes, while small-angle X-ray scattering results indicate that the grain size reduces to one-third of its original size. Then the room-temperature conductivity increased by at least two orders of magnitude for PEO-based SPE.
{"title":"Grain Size Control Toward Room-Temperature Operable Solid Polymer Electrolytes","authors":"Yanrui Pan, Zhaokun Wang, Chen Li, Zuohang Li, Yue Ma, Mingfu Ye, Xixi Shi, Hongzhou Zhang, Dawei Song, Lianqi Zhang","doi":"10.1002/cnl2.70085","DOIUrl":"https://doi.org/10.1002/cnl2.70085","url":null,"abstract":"<p>The practical application of solid polymer electrolytes (SPE) is limited due to notorious high crystallinity and low ionic conductivity. Existing research concentrated on reducing crystallinity and increasing Li salt concentration have made certain process. However, the segmentation and isolation effects of large and numerous grains on amorphous region have always been overlooked and the effect of grain size remains largely unexplored. Herein, take polyethylene oxide (PEO) as an example, “grain size refinement” strategy is adopted to improve the related room-temperature ionic conductivity by simply placing PEO based SPE on Li sheets coated with ester monomers and conducting in-situ polymerization. During these processes, in addition to reducing the interaction force between polymer chains and decreasing the driving force for crystallization, ester monomers are conducive to form interface with polymer clusters, which serves as additional nucleation sites and promotes the formation of refined grains. Then instantaneous high-temperature provided by muffle furnace triggers rapid solidification of monomers, leading to the locking of refined grain structure and the formation of more interconnected amorphous regions. Time-of-flight secondary ion mass spectrometry and polarization microscope confirm these processes, while small-angle X-ray scattering results indicate that the grain size reduces to one-third of its original size. Then the room-temperature conductivity increased by at least two orders of magnitude for PEO-based SPE.</p>","PeriodicalId":100214,"journal":{"name":"Carbon Neutralization","volume":"5 1","pages":""},"PeriodicalIF":12.0,"publicationDate":"2025-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cnl2.70085","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145739662","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}
Wearable heaters with multifunctional capabilities and high performance are in high demand for future personal thermal management. However, the development of such devices remains challenging due to limitations in flexibility, complex fabrication, inadequate Joule heating efficiency, insufficient electromagnetic interference (EMI) shielding, and poor antibacterial performance. Here, Ag@PEDOT heterostructures were decorated on laser-induced graphene (LIG) through a simple spray-coating process followed by a facile chemical synthetic method to deposit silver nanoparticles (AgNPs) onto the PEDOT layers. The resulting composite retains the intrinsic flexibility and comfort of the original graphene matrices, while demonstrating exceptional Joule heating characteristics—achieving a broad temperature range (30°C–100°C) at low operating voltages (0.8–2.6 V) and a rapid photothermal response (reaching 89.6°C within 180 s at 1.5 sun irradiation). Moreover, the material exhibits superior electromagnetic shielding effectiveness (33 dB in the X-band) and outstanding antibacterial activity, with an inhibition rate exceeding 95% against Escherichia coli and Staphylococcus aureus. This study offers a promising strategy for designing multifunctional wearable heaters suited for personal healthcare and thermal management applications.
{"title":"Multifunctional and Flexible Ag@PEDOT Heterostructure-Decorated Laser-Induced Graphene Film for Body Thermal Therapy","authors":"Qinhua Zhou, Jing He, Xinmeng Hu, Zhengying Tu, Junwen Xie, Qingbin Zheng, Lin Lin, Yinhang Zhang","doi":"10.1002/cnl2.70092","DOIUrl":"https://doi.org/10.1002/cnl2.70092","url":null,"abstract":"<p>Wearable heaters with multifunctional capabilities and high performance are in high demand for future personal thermal management. However, the development of such devices remains challenging due to limitations in flexibility, complex fabrication, inadequate Joule heating efficiency, insufficient electromagnetic interference (EMI) shielding, and poor antibacterial performance. Here, Ag@PEDOT heterostructures were decorated on laser-induced graphene (LIG) through a simple spray-coating process followed by a facile chemical synthetic method to deposit silver nanoparticles (AgNPs) onto the PEDOT layers. The resulting composite retains the intrinsic flexibility and comfort of the original graphene matrices, while demonstrating exceptional Joule heating characteristics—achieving a broad temperature range (30°C–100°C) at low operating voltages (0.8–2.6 V) and a rapid photothermal response (reaching 89.6°C within 180 s at 1.5 sun irradiation). Moreover, the material exhibits superior electromagnetic shielding effectiveness (33 dB in the X-band) and outstanding antibacterial activity, with an inhibition rate exceeding 95% against <i>Escherichia coli</i> and <i>Staphylococcus aureus</i>. This study offers a promising strategy for designing multifunctional wearable heaters suited for personal healthcare and thermal management applications.</p>","PeriodicalId":100214,"journal":{"name":"Carbon Neutralization","volume":"5 1","pages":""},"PeriodicalIF":12.0,"publicationDate":"2025-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cnl2.70092","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145750658","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}
Iron-based Prussian blue analogs (PBAs) represent promising, facile-to-prepare, and low-cost positive electrode materials for sodium-ion batteries. However, their practical application is hindered by the markedly irreversible three-phase transitions and severe lattice distortion that occur during sodium ion storage, leading to capacity limitations and diminished cycling stability. Herein, a simple pyrrole-induced phase transition engineering strategy is proposed to successfully transform monoclinic PBAs into cubic polypyrrole-PBAs (PPy-PBAs). In situ X-ray diffraction (XRD) testing and density functional theory (DFT) calculations reveal that the phase transition mechanism transforms from an unfavorable three-phase process to a highly reversible two-phase transition. Compared to complex three-phase transition (PBAs), the efficient two-phase transition (PPy-PBAs) exhibits smaller lattice volume contraction/expansion and less Fe-C/Fe-N bond length stretching/shrinking, demonstrating remarkable structural stability. Moreover, this strategy effectively reduced the energy barrier for sodium-ion (Na+) migration, with the density of states crossing the Fermi level, significantly enhancing electronic conductivity, and thereby facilitating redox reactions and Na+ transport kinetics within the material. The reversible two-phase transition enables sustainable sodium-ion storage through phase-transition engineering. Compared with PBAs that undergo structural distortion and significant lattice strain, the optimized positive electrode material demonstrates a discharge capacity of 136 mAh/g and an ultralong stable cycling lifespan of 1700 cycles, establishing new possibilities for advanced sodium-ion batteries.
{"title":"Pyrrole-Driven Structural Phase Engineering of Prussian Blue Analogs for Ultrastable and Highly Efficient Na-Ion Storage","authors":"Jiazhuo Li, Shuai Wang, Ying Sun, Minghui Liu, Hanyu Wen, Hui Li, Meiyan Sun, Siwen Zhang, Bosi Yin, Zhenbo Wang, Tianyi Ma","doi":"10.1002/cnl2.70091","DOIUrl":"https://doi.org/10.1002/cnl2.70091","url":null,"abstract":"<p>Iron-based Prussian blue analogs (PBAs) represent promising, facile-to-prepare, and low-cost positive electrode materials for sodium-ion batteries. However, their practical application is hindered by the markedly irreversible three-phase transitions and severe lattice distortion that occur during sodium ion storage, leading to capacity limitations and diminished cycling stability. Herein, a simple pyrrole-induced phase transition engineering strategy is proposed to successfully transform monoclinic PBAs into cubic polypyrrole-PBAs (PPy-PBAs). In situ X-ray diffraction (XRD) testing and density functional theory (DFT) calculations reveal that the phase transition mechanism transforms from an unfavorable three-phase process to a highly reversible two-phase transition. Compared to complex three-phase transition (PBAs), the efficient two-phase transition (PPy-PBAs) exhibits smaller lattice volume contraction/expansion and less Fe-C/Fe-N bond length stretching/shrinking, demonstrating remarkable structural stability. Moreover, this strategy effectively reduced the energy barrier for sodium-ion (Na<sup>+</sup>) migration, with the density of states crossing the Fermi level, significantly enhancing electronic conductivity, and thereby facilitating redox reactions and Na<sup>+</sup> transport kinetics within the material. The reversible two-phase transition enables sustainable sodium-ion storage through phase-transition engineering. Compared with PBAs that undergo structural distortion and significant lattice strain, the optimized positive electrode material demonstrates a discharge capacity of 136 mAh/g and an ultralong stable cycling lifespan of 1700 cycles, establishing new possibilities for advanced sodium-ion batteries.</p>","PeriodicalId":100214,"journal":{"name":"Carbon Neutralization","volume":"5 1","pages":""},"PeriodicalIF":12.0,"publicationDate":"2025-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cnl2.70091","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145739666","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}
Min Zheng, Qian Sun, Zeheng Lin, Joe, Yanzhao Zhang, Yifan Bao, Jiakang You, Kai Wang, Huihui Li, Shuhao Wang, Yan Nie, Yuhan Xie, Dazhi Yao, Shuai Bi
Electrochemical CO2 reduction (CO2RR) holds promise for sustainable fuel and chemical production but faces fundamental challenges rooted in limited CO2 availability and high activation reaction barriers. These issues manifest as slow kinetics, low selectivity, and poor stability under industrial operational conditions. While the catalyst/electrolyte interface engineering plays a decisive role in modulating the local microenvironment, which directly influences the kinetics and thermodynamics of CO2RR, current understanding remains fragmented due to the complex interplay of interfacial factors. Herein, in this review, we address this gap by moving beyond conventional categorization by materials or products. We present a unified mechanism-oriented framework that directly links interfacial design strategies for tackling the core challenges of CO2 availability, site accessibility, and reaction affordability. We systematically decouple the interface interactions and survey interfacial engineering strategies for CO2 reduction, including mass-transport control, electrostatic microenvironment tuning, molecular functionalization, and device–interface engineering. By elucidating the mechanistic principles behind these strategies and their interconnections, this review provides actionable guidelines for engineering robust interfaces that break inherent trade-offs among activity, selectivity, and stability. We aim for this perspective to not only advance understanding of microenvironment modulation but also accelerate the development of scalable, carbon-neutral energy conversion technologies.
{"title":"Interfacial Engineering Toward Local Environment Modulation for Selective CO2 Electroreduction","authors":"Min Zheng, Qian Sun, Zeheng Lin, Joe, Yanzhao Zhang, Yifan Bao, Jiakang You, Kai Wang, Huihui Li, Shuhao Wang, Yan Nie, Yuhan Xie, Dazhi Yao, Shuai Bi","doi":"10.1002/cnl2.70073","DOIUrl":"https://doi.org/10.1002/cnl2.70073","url":null,"abstract":"<p>Electrochemical CO<sub>2</sub> reduction (CO<sub>2</sub>RR) holds promise for sustainable fuel and chemical production but faces fundamental challenges rooted in limited CO<sub>2</sub> availability and high activation reaction barriers. These issues manifest as slow kinetics, low selectivity, and poor stability under industrial operational conditions. While the catalyst/electrolyte interface engineering plays a decisive role in modulating the local microenvironment, which directly influences the kinetics and thermodynamics of CO<sub>2</sub>RR, current understanding remains fragmented due to the complex interplay of interfacial factors. Herein, in this review, we address this gap by moving beyond conventional categorization by materials or products. We present a unified mechanism-oriented framework that directly links interfacial design strategies for tackling the core challenges of CO<sub>2</sub> availability, site accessibility, and reaction affordability. We systematically decouple the interface interactions and survey interfacial engineering strategies for CO<sub>2</sub> reduction, including mass-transport control, electrostatic microenvironment tuning, molecular functionalization, and device–interface engineering. By elucidating the mechanistic principles behind these strategies and their interconnections, this review provides actionable guidelines for engineering robust interfaces that break inherent trade-offs among activity, selectivity, and stability. We aim for this perspective to not only advance understanding of microenvironment modulation but also accelerate the development of scalable, carbon-neutral energy conversion technologies.</p>","PeriodicalId":100214,"journal":{"name":"Carbon Neutralization","volume":"5 1","pages":""},"PeriodicalIF":12.0,"publicationDate":"2025-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cnl2.70073","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145739661","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}
Jie Yang, Haidong Zhong, Chunbiao Li, Qian Zhang, Zhihao Wu, Zuohua Liu, Zihan Yang, Jiaxing Li
This study explored thermal and electrodeposition impacts of distinct chaotic current waveforms to enhance current efficiency and reduce heat loss through the regulation of electrode interfacial reaction dynamics, advancing current efficiency, energy conservation, and carbon neutrality. Two universal control methodology was developed to achieve independent amplitude and offset boosting of arbitrary chaotic signals, implemented through a specially designed chaotic circuit. Three distinct waveforms (w-, F-, and G-signals) were systematically investigated for their thermal and electrochemical effects. Experimental and COMSOL simulation results demonstrated that Joule heating was governed by both fluctuation amplitude and frequency characteristics, following the sequence w < F < G. When the current density was about 1500 A/m2, the corresponding optimal voltage fluctuations were identified as 2.8 V (w), 0.51 V (F), and 0.23 V (G), yielding current efficiency improvements of 2.2%, 0.7%, and 5.1%, respectively, based on the electrodeposition experiments. Combining experiments on electrolytes at different temperatures with corresponding SEM characterization revealed that chaotic current suppresses manganese nodules not only through Joule heating-induced temperature rise, but also via effective regulation of the interfacial electrochemical environment, thus allowing effective inhibition even at lower temperatures. These findings provide both theoretical insights and practical methodologies for implementing chaotic currents in industrial electrodeposition processes.
本研究探讨了不同混沌电流波形对热和电沉积的影响,通过调节电极界面反应动力学,提高电流效率,减少热损失,提高电流效率,节能和碳中和。开发了两种通用控制方法,通过特殊设计的混沌电路实现任意混沌信号的独立幅度和偏移增强。系统地研究了三种不同的波形(w-, F-和g -信号)的热效应和电化学效应。实验和COMSOL模拟结果表明,焦耳加热受波动幅度和频率特性的共同控制,并遵循w <; F <; G的顺序。当电流密度约为1500 A/m2时,确定了相应的最佳电压波动为2.8 V (w)、0.51 V (F)和0.23 V (G),根据电沉积实验,电流效率分别提高2.2%、0.7%和5.1%。结合不同温度下电解质的实验和相应的SEM表征表明,混沌电流不仅通过焦耳加热引起的温升抑制锰结核,而且通过有效调节界面电化学环境,从而在较低温度下也能有效抑制锰结核。这些发现为在工业电沉积过程中实现混沌电流提供了理论见解和实践方法。
{"title":"Chaotic Current Waveforms in Electrodeposition: Modulating Joule Heating and Current Efficiency Toward Carbon Neutrality","authors":"Jie Yang, Haidong Zhong, Chunbiao Li, Qian Zhang, Zhihao Wu, Zuohua Liu, Zihan Yang, Jiaxing Li","doi":"10.1002/cnl2.70089","DOIUrl":"https://doi.org/10.1002/cnl2.70089","url":null,"abstract":"<p>This study explored thermal and electrodeposition impacts of distinct chaotic current waveforms to enhance current efficiency and reduce heat loss through the regulation of electrode interfacial reaction dynamics, advancing current efficiency, energy conservation, and carbon neutrality. Two universal control methodology was developed to achieve independent amplitude and offset boosting of arbitrary chaotic signals, implemented through a specially designed chaotic circuit. Three distinct waveforms (<i>w</i>-, <i>F</i>-, and <i>G</i>-signals) were systematically investigated for their thermal and electrochemical effects. Experimental and COMSOL simulation results demonstrated that Joule heating was governed by both fluctuation amplitude and frequency characteristics, following the sequence <i>w</i> < <i>F</i> < <i>G</i>. When the current density was about 1500 A/m<sup>2</sup>, the corresponding optimal voltage fluctuations were identified as 2.8 V (<i>w</i>), 0.51 V (<i>F</i>), and 0.23 V (<i>G</i>), yielding current efficiency improvements of 2.2%, 0.7%, and 5.1%, respectively, based on the electrodeposition experiments. Combining experiments on electrolytes at different temperatures with corresponding SEM characterization revealed that chaotic current suppresses manganese nodules not only through Joule heating-induced temperature rise, but also via effective regulation of the interfacial electrochemical environment, thus allowing effective inhibition even at lower temperatures. These findings provide both theoretical insights and practical methodologies for implementing chaotic currents in industrial electrodeposition processes.</p>","PeriodicalId":100214,"journal":{"name":"Carbon Neutralization","volume":"5 1","pages":""},"PeriodicalIF":12.0,"publicationDate":"2025-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cnl2.70089","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145739660","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}
Tao Zhou, Teng Wang, Changqing Chu, Peng Shi, Guo Gao
V-based materials, with the high specific capacity and multi-electron redox reactions, are considered as preferred cathodes for low-cost and high-safety aqueous zinc-ion batteries. Nevertheless, poor electronic conductivity, sluggish kinetics, vanadium dissolution, and unstable structure pose severe challenges for the further practical applications. To address these issues, in this study, transition metal ions Mo6+ and polyaniline were incorporated into V2O5 derived from vanadium acetylacetonate via a one-step hydrothermal method (MPVO). The results reveal that MPVO exhibits a unique three-dimensional (3D) sea urchin-like morphology with a satisfactory specific surface area and high concentration of oxygen vacancies. These characteristics offer more reaction sites for Zn2+ and adjust the electronic conductivity. Moreover, kinetic analysis and density-functional-theory calculations indicate that MPVO performs metallic behavior, with the lowest Zn2+ diffusion barrier and outstanding pseudocapacitive storage capacity. Hence, the MPVO cathode delivers a reversible capacity of approximately 457.5 mAh g−1 at 0.1 A g−1. Moreover, it demonstrates remarkable high-rate capacity and robust long-cycle performance. This study realizes a triple-strategy approach of enlarging the interlayer spacing, evolving from a zero-dimensional (0D) to 3D sea urchin-like morphology, and introducing abundant defects. These synergistic strategies significantly enhance the rapid kinetics and high stability of the MPVO cathode and provide new insights for designing V-based cathodes.
v基材料具有高比容量和多电子氧化还原反应,被认为是低成本、高安全的水性锌离子电池的首选阴极材料。然而,电导率差、动力学缓慢、钒溶解和结构不稳定等问题对进一步的实际应用构成了严峻的挑战。为了解决这些问题,本研究通过一步水热法(MPVO)将过渡金属离子Mo6+和聚苯胺掺入由乙酰丙酮钒制备的V2O5中。结果表明,MPVO具有独特的三维(3D)海胆样形态,具有令人满意的比表面积和高浓度的氧空位。这些特性为Zn2+提供了更多的反应位点,并调节了电子导电性。此外,动力学分析和密度泛函理论计算表明,MPVO具有金属行为,具有最低的Zn2+扩散势垒和优异的赝电容存储容量。因此,MPVO阴极在0.1 a g−1时提供约457.5 mAh g−1的可逆容量。此外,它还具有显著的高速率容量和稳健的长周期性能。本研究实现了扩大层间间距、从零维(0D)形态向三维海胆形态演化、引入丰富缺陷的三重策略。这些协同策略显著提高了MPVO阴极的快速动力学和高稳定性,为v基阴极的设计提供了新的见解。
{"title":"Unlocking Ultra-Fast Kinetics in Vanadium Oxides via the Synergistic Intercalation of Mo6+ and PANI for Superior Zinc-Ion Storage","authors":"Tao Zhou, Teng Wang, Changqing Chu, Peng Shi, Guo Gao","doi":"10.1002/cnl2.70095","DOIUrl":"https://doi.org/10.1002/cnl2.70095","url":null,"abstract":"<p>V-based materials, with the high specific capacity and multi-electron redox reactions, are considered as preferred cathodes for low-cost and high-safety aqueous zinc-ion batteries. Nevertheless, poor electronic conductivity, sluggish kinetics, vanadium dissolution, and unstable structure pose severe challenges for the further practical applications. To address these issues, in this study, transition metal ions Mo<sup>6+</sup> and polyaniline were incorporated into V<sub>2</sub>O<sub>5</sub> derived from vanadium acetylacetonate via a one-step hydrothermal method (MPVO). The results reveal that MPVO exhibits a unique three-dimensional (3D) sea urchin-like morphology with a satisfactory specific surface area and high concentration of oxygen vacancies. These characteristics offer more reaction sites for Zn<sup>2+</sup> and adjust the electronic conductivity. Moreover, kinetic analysis and density-functional-theory calculations indicate that MPVO performs metallic behavior, with the lowest Zn<sup>2+</sup> diffusion barrier and outstanding pseudocapacitive storage capacity. Hence, the MPVO cathode delivers a reversible capacity of approximately 457.5 mAh g<sup>−1</sup> at 0.1 A g<sup>−1</sup>. Moreover, it demonstrates remarkable high-rate capacity and robust long-cycle performance. This study realizes a triple-strategy approach of enlarging the interlayer spacing, evolving from a zero-dimensional (0D) to 3D sea urchin-like morphology, and introducing abundant defects. These synergistic strategies significantly enhance the rapid kinetics and high stability of the MPVO cathode and provide new insights for designing V-based cathodes.</p>","PeriodicalId":100214,"journal":{"name":"Carbon Neutralization","volume":"5 1","pages":""},"PeriodicalIF":12.0,"publicationDate":"2025-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cnl2.70095","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145739665","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}