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}
Wide-bandgap (WBG) perovskite solar cells (PSCs) are critical for tandem architectures but suffer from light-induced halide segregation and non-radiative recombination. Although conventional rare-earth doping passivates defects, it concurrently introduces vacancies and lattice strain that exacerbate halogen migration. Herein, we report a thermally induced doping strategy where Pr3+/Sm3+ ions pre-embedded in MeO-4PACz diffuse into the perovskite during annealing. Through combined tolerance factor analysis, structural characterization, and DFT calculations, we identify a dual doping mechanism: predominant interstitial incorporation with minor B-site substitution. This approach reduces defect density, increases iodine migration energy barriers (from 0.85 to 0.94 and 1.12 eV), and minimizes lattice distortion. Consequently, the experimental results show that the open-circuit voltage increases from 1.198 V to 1.230 V (Pr3+) and 1.233 V (Sm3+), and the fill factor increases from 83% to 86%. Finally, the PCE reached 23.04% (Pr3+) and 23.39% (Sm3+) (20.12% for control) with > 90% stability retention after 1500 h. In addition, the optimized semitransparent WBG device PCE was 19.48% (Pr3+) and 19.85% (Sm3+), and the PCE of 4-T perovskite was 27.05% (Pr3+) and 27.56% (Sm3+). This method will be beneficial for the development and application of WBG PSCs and TSCs.
宽带隙钙钛矿太阳能电池(PSCs)对于串联结构至关重要,但受到光诱导卤化物偏析和非辐射复合的影响。传统稀土掺杂虽然钝化了缺陷,但同时引入了空位和晶格应变,加剧了卤素迁移。本文报道了一种热诱导掺杂策略,即预先嵌入在MeO-4PACz中的Pr3+/Sm3+离子在退火过程中扩散到钙钛矿中。通过综合耐受因子分析、结构表征和DFT计算,我们确定了双重掺杂机制:主要的间隙掺入和少量的b位取代。这种方法降低了缺陷密度,增加了碘迁移能垒(从0.85到0.94和1.12 eV),并最大限度地减少了晶格畸变。因此,实验结果表明,开路电压从1.198 V增加到1.230 V (Pr3+)和1.233 V (Sm3+),填充因子从83%增加到86%。PCE分别为23.04% (Pr3+)和23.39% (Sm3+)(对照组为20.12%),1500 h后PCE稳定保持率为90%。此外,优化后的半透明WBG器件PCE分别为19.48% (Pr3+)和19.85% (Sm3+), 4-T钙钛矿的PCE分别为27.05% (Pr3+)和27.56% (Sm3+)。该方法将有利于WBG psscs和tsscs的开发和应用。
{"title":"Thermally Driven Lanthanide Dual-Site Doping Enables High Performance Perovksite Solar Cells via Halide Migration Suppression","authors":"Mengni Zhou, Tao Wang, Fashe Li, Kunpeng Li, Xinlong Zhao, Zhongming Cai, Xue Lu, Shichao Sun, Zhishan Li, Dongfang Li, Huicong Zhang, Xing Zhu, Hua Wang, Tao Zhu","doi":"10.1002/cnl2.70087","DOIUrl":"https://doi.org/10.1002/cnl2.70087","url":null,"abstract":"<p>Wide-bandgap (WBG) perovskite solar cells (PSCs) are critical for tandem architectures but suffer from light-induced halide segregation and non-radiative recombination. Although conventional rare-earth doping passivates defects, it concurrently introduces vacancies and lattice strain that exacerbate halogen migration. Herein, we report a thermally induced doping strategy where Pr<sup>3+</sup>/Sm<sup>3+</sup> ions pre-embedded in MeO-4PACz diffuse into the perovskite during annealing. Through combined tolerance factor analysis, structural characterization, and DFT calculations, we identify a dual doping mechanism: predominant interstitial incorporation with minor B-site substitution. This approach reduces defect density, increases iodine migration energy barriers (from 0.85 to 0.94 and 1.12 eV), and minimizes lattice distortion. Consequently, the experimental results show that the open-circuit voltage increases from 1.198 V to 1.230 V (Pr<sup>3+</sup>) and 1.233 V (Sm<sup>3+</sup>), and the fill factor increases from 83% to 86%. Finally, the PCE reached 23.04% (Pr<sup>3+</sup>) and 23.39% (Sm<sup>3+</sup>) (20.12% for control) with > 90% stability retention after 1500 h. In addition, the optimized semitransparent WBG device PCE was 19.48% (Pr<sup>3+</sup>) and 19.85% (Sm<sup>3+</sup>), and the PCE of 4-T perovskite was 27.05% (Pr<sup>3+</sup>) and 27.56% (Sm<sup>3+</sup>). This method will be beneficial for the development and application of WBG PSCs and TSCs.</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/cnl2.70087","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145750659","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}
SnSe2 is a promising thermoelectric (TE) material with intrinsic n-type characteristics and a high theoretical ZT value of 2.95 along the a-axis. However, its densely packed crystal lattice in the plane perpendicular to the c-axis leads to weak phonon scattering, limiting improvements through conventional defect or nanostructure-based strategies. In this study, the rare-earth element Yb is introduced into tin-rich SnSe2, predominantly segregating at grain boundaries and enhancing phonon scattering, while a small fraction incorporates into the lattice and modifies the electronic structure, simultaneously tuning both electrical and thermal transport behaviors. Yb incorporation enhances multiple phonon scattering mechanisms, significantly reducing lattice thermal conductivity, reaching a minimum of ~0.48 W·m−1·K−1. Meanwhile, it modulates the electronic structure by introducing impurity states, altering band alignment, and enhancing band degeneracy, collectively increasing the density-of-states (DOS) effective mass and Seebeck coefficient, contributing to a maximum power factor of 436.47 μW·m−1·K−2 at 773 K. As a result, the Yb-doped SnSe2 sample with 1.0 wt% achieves a peak ZTmax of ~0.53 at 773 K along the direction parallel to the pressing direction, representing an ~95.3% enhancement over the undoped sample. This study presents a synergistic and effective strategy for optimizing SnSe2-based TE materials via rare-earth doping, paving the way for next-generation high-performance TE devices.
{"title":"Phonon Scattering Engineering via Yb Doping in SnSe2 for Substantially Lowered Thermal Conductivity and Enhanced Thermoelectric Performance","authors":"Zhuoming Xu, Wenning Qin, Mohammad Nisar, Mazhar Hussain Danish, Suniya Siddique, Fu Li, Guangxing Liang, Jingting Luo, Zhuanghao Zheng, Yue-Xing Chen","doi":"10.1002/cnl2.70083","DOIUrl":"https://doi.org/10.1002/cnl2.70083","url":null,"abstract":"<p>SnSe<sub>2</sub> is a promising thermoelectric (TE) material with intrinsic n-type characteristics and a high theoretical ZT value of 2.95 along the <i>a</i>-axis. However, its densely packed crystal lattice in the plane perpendicular to the <i>c</i>-axis leads to weak phonon scattering, limiting improvements through conventional defect or nanostructure-based strategies. In this study, the rare-earth element Yb is introduced into tin-rich SnSe<sub>2</sub>, predominantly segregating at grain boundaries and enhancing phonon scattering, while a small fraction incorporates into the lattice and modifies the electronic structure, simultaneously tuning both electrical and thermal transport behaviors. Yb incorporation enhances multiple phonon scattering mechanisms, significantly reducing lattice thermal conductivity, reaching a minimum of ~0.48 W·m<sup>−1</sup>·K<sup>−1</sup>. Meanwhile, it modulates the electronic structure by introducing impurity states, altering band alignment, and enhancing band degeneracy, collectively increasing the density-of-states (DOS) effective mass and Seebeck coefficient, contributing to a maximum power factor of 436.47 μW·m<sup>−1</sup>·K<sup>−2</sup> at 773 K. As a result, the Yb-doped SnSe<sub>2</sub> sample with 1.0 wt% achieves a peak <i>ZT</i><sub>max</sub> of ~0.53 at 773 K along the direction parallel to the pressing direction, representing an ~95.3% enhancement over the undoped sample. This study presents a synergistic and effective strategy for optimizing SnSe<sub>2</sub>-based TE materials via rare-earth doping, paving the way for next-generation high-performance TE devices.</p>","PeriodicalId":100214,"journal":{"name":"Carbon Neutralization","volume":"5 1","pages":""},"PeriodicalIF":12.0,"publicationDate":"2025-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cnl2.70083","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145618975","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}
Zhaodi Tang, Xi Zhang, Dongmei Huang, Bin Wang, Jionghui Wang
For decades, the industry has believed that spherical graphite (SG) yield correlates strongly with graphite flake size. To clarify natural graphite (NG) spheroidization mechanisms, a comprehensive evaluation was conducted by extracting intermediate products from an industrial production line and utilizing separated jet mills to simulate continuous processing in the study. Focused ion beam-scanning electron microscope (FIB-SEM) cross-sectional analysis and nanocomputed tomography (Nano-CT) imaging revealed that flakes of different thicknesses underwent distinct morphological changes (folding, bending, or fragmentation) under mechanical force, with only flakes above a critical thickness (∼2 μm) forming SG cores. Statistical correlation between thickness (measured via statistical method under SEM) and yield demonstrated that thickness—not only size—is the dominant factor, redefining “effective SG flakes” to include small but thick flakes. Therefore, prioritizing thickness protection over size preservation in grinding-flotation and spheroidization processes increased SG yield by 7% in industrial validation. The work provides new insights for high-efficiency SG production.
{"title":"Critical Thickness and Its Role in the Spheroidization of Natural Flake Graphite","authors":"Zhaodi Tang, Xi Zhang, Dongmei Huang, Bin Wang, Jionghui Wang","doi":"10.1002/cnl2.70079","DOIUrl":"https://doi.org/10.1002/cnl2.70079","url":null,"abstract":"<p>For decades, the industry has believed that spherical graphite (SG) yield correlates strongly with graphite flake size. To clarify natural graphite (NG) spheroidization mechanisms, a comprehensive evaluation was conducted by extracting intermediate products from an industrial production line and utilizing separated jet mills to simulate continuous processing in the study. Focused ion beam-scanning electron microscope (FIB-SEM) cross-sectional analysis and nanocomputed tomography (Nano-CT) imaging revealed that flakes of different thicknesses underwent distinct morphological changes (folding, bending, or fragmentation) under mechanical force, with only flakes above a critical thickness (∼2 μm) forming SG cores. Statistical correlation between thickness (measured via statistical method under SEM) and yield demonstrated that thickness—not only size—is the dominant factor, redefining “effective SG flakes” to include small but thick flakes. Therefore, prioritizing thickness protection over size preservation in grinding-flotation and spheroidization processes increased SG yield by 7% in industrial validation. The work provides new insights for high-efficiency SG production.</p>","PeriodicalId":100214,"journal":{"name":"Carbon Neutralization","volume":"5 1","pages":""},"PeriodicalIF":12.0,"publicationDate":"2025-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cnl2.70079","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145626859","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 zinc-ion batteries (AZIBs) have gained great attention due to their nontoxicity, low-cost, and high theoretical capacity. However, the scarcity of suitable cathode materials with excellent performance limits the practical application of AZIBs. Herein, we develop a conducting polymer (polyaniline) and divalent ions (Ca2+) co-intercalated method to synergistically regulate the property of V2O5 to enhance Zn2+ storage performance. The synergistic effect of co-insertion Ca2+ and polyaniline (PANI) not only enlarges the interlayer spacing but also regulates multiple oxidation states of vanadium, which dramatically improves the conductivity, diffusion kinetics, and structural stability of host V2O5. Consequently, the resultant Ca/PANI/V2O5•nH2O (CPVO) as AZIBs cathodes exhibits extraordinary specific capacity of 512 mAh g–1 (0.5 A g–1) and cycling stability with an outstanding coulombic efficiency of around 100% after 2000 cycles (25 A g–1). Moreover, the Zn2+ storage mechanism is elaborated by combining comprehensive characterizations and DFT calculations.
水基锌离子电池(azib)因其无毒性、低成本和高理论容量而受到广泛关注。然而,性能优良的正极材料的缺乏限制了azib的实际应用。在此,我们开发了一种导电聚合物(聚苯胺)和二价离子(Ca2+)共插的方法来协同调节V2O5的性能,以提高Zn2+的存储性能。共插入Ca2+和聚苯胺(PANI)的协同作用不仅扩大了层间距,还调节了钒的多种氧化态,从而显著提高了宿主V2O5的电导率、扩散动力学和结构稳定性。因此,所得到的Ca/PANI/V2O5•nH2O (CPVO)作为AZIBs阴极具有非凡的512 mAh g-1 (0.5 A g-1)比容量和循环稳定性,在2000次循环(25 A g-1)后具有出色的库仑效率,约为100%。并结合综合表征和DFT计算阐述了Zn2+的存储机理。
{"title":"Tuning Interlayer and Mixed Vanadium Valences of V2O5 via Organic and Inorganic Guests Co-Intercalation Enables Boosted Aqueous Zinc-Ion Storage","authors":"Xiaoteng Yan, Junjie Qi, Honghai Wang, Zhiying Wang, Chunli Li, Wenchao Peng, Jiapeng Liu","doi":"10.1002/cnl2.70082","DOIUrl":"https://doi.org/10.1002/cnl2.70082","url":null,"abstract":"<p>Aqueous zinc-ion batteries (AZIBs) have gained great attention due to their nontoxicity, low-cost, and high theoretical capacity. However, the scarcity of suitable cathode materials with excellent performance limits the practical application of AZIBs. Herein, we develop a conducting polymer (polyaniline) and divalent ions (Ca<sup>2+</sup>) co-intercalated method to synergistically regulate the property of V<sub>2</sub>O<sub>5</sub> to enhance Zn<sup>2+</sup> storage performance. The synergistic effect of co-insertion Ca<sup>2+</sup> and polyaniline (PANI) not only enlarges the interlayer spacing but also regulates multiple oxidation states of vanadium, which dramatically improves the conductivity, diffusion kinetics, and structural stability of host V<sub>2</sub>O<sub>5</sub>. Consequently, the resultant Ca/PANI/V<sub>2</sub>O<sub>5</sub>•nH<sub>2</sub>O (CPVO) as AZIBs cathodes exhibits extraordinary specific capacity of 512 mAh g<sup>–1</sup> (0.5 A g<sup>–1</sup>) and cycling stability with an outstanding coulombic efficiency of around 100% after 2000 cycles (25 A g<sup>–1</sup>). Moreover, the Zn<sup>2+</sup> storage mechanism is elaborated by combining comprehensive characterizations and DFT calculations.</p>","PeriodicalId":100214,"journal":{"name":"Carbon Neutralization","volume":"4 6","pages":""},"PeriodicalIF":12.0,"publicationDate":"2025-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cnl2.70082","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145580941","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}
Jixin Shi, Peipei Zhang, Fawang Liu, Tiantian Su, Jingsan Xu, Chao Lin, Xiaopeng Li, Wei Luo
The development of advanced catalytic technologies for the combustion of low-concentration methane is crucial for minimizing unburned CH4 emissions, consequently improving the eco-efficiency of natural gas vehicles and power plants. The integration of effective catalysts into existing systems with minimal modifications is of paramount importance. Porous ceramic composites offer a promising alternative to traditional powder catalysts due to their high surface area, excellent thermal stability, adjustable porosity, and prolonged catalytic durability. This study introduces a trace Pd–incorporated SnO2 porous ceramic catalyst (Pd/SnO2) fabricated using the spark plasma sintering (SPS) technique. The synthesis process uses a NaCl salt template to create a porous structure and graphite to improve Pd loading and dispersion on the SnO2 surface. An optimized 10 wt.% graphite-decorated Pd/SnO2 porous ceramic catalyst, containing a trace Pd loading of 0.17 wt.%, achieved a low T90 of 427°C during methane reforming tests and maintained stable catalytic performance after multiple temperature cycling and over 900 min of continuous operation. Enhanced activity stems from two synergies: first, graphite-mediated uniform PdO dispersion boosting active site accessibility and second, PdO–SnO2 interfacial charge transfer generating oxygen-deficient sites, accelerating CH4 dissociation and stabilizing Pd2+ against deactivation. These findings highlight the potential of this approach for use in the development of durable and efficient ceramic composite–based catalysts for environmental applications.
{"title":"Trace Pd–Functionalized SnO2 Porous Ceramic for Enhanced Catalytic Combustion of Low-Concentration Methane","authors":"Jixin Shi, Peipei Zhang, Fawang Liu, Tiantian Su, Jingsan Xu, Chao Lin, Xiaopeng Li, Wei Luo","doi":"10.1002/cnl2.70080","DOIUrl":"https://doi.org/10.1002/cnl2.70080","url":null,"abstract":"<p>The development of advanced catalytic technologies for the combustion of low-concentration methane is crucial for minimizing unburned CH<sub>4</sub> emissions, consequently improving the eco-efficiency of natural gas vehicles and power plants. The integration of effective catalysts into existing systems with minimal modifications is of paramount importance. Porous ceramic composites offer a promising alternative to traditional powder catalysts due to their high surface area, excellent thermal stability, adjustable porosity, and prolonged catalytic durability. This study introduces a trace Pd–incorporated SnO<sub>2</sub> porous ceramic catalyst (Pd/SnO<sub>2</sub>) fabricated using the spark plasma sintering (SPS) technique. The synthesis process uses a NaCl salt template to create a porous structure and graphite to improve Pd loading and dispersion on the SnO<sub>2</sub> surface. An optimized 10 wt.% graphite-decorated Pd/SnO<sub>2</sub> porous ceramic catalyst, containing a trace Pd loading of 0.17 wt.%, achieved a low T<sub>90</sub> of 427°C during methane reforming tests and maintained stable catalytic performance after multiple temperature cycling and over 900 min of continuous operation. Enhanced activity stems from two synergies: first, graphite-mediated uniform PdO dispersion boosting active site accessibility and second, PdO–SnO<sub>2</sub> interfacial charge transfer generating oxygen-deficient sites, accelerating CH<sub>4</sub> dissociation and stabilizing Pd<sup>2+</sup> against deactivation. These findings highlight the potential of this approach for use in the development of durable and efficient ceramic composite–based catalysts for environmental applications.</p>","PeriodicalId":100214,"journal":{"name":"Carbon Neutralization","volume":"4 6","pages":""},"PeriodicalIF":12.0,"publicationDate":"2025-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cnl2.70080","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145521531","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}
Hongtian Ning, Jinxuan Zou, Yangyang Dong, Meiling Shu, Shuo Yang, Xuemei Zhou, Huagui Nie, Dong Cai, Zhanshuang Jin, Zhi Yang
Lithium–sulfur (Li–S) batteries face significant commercialization hurdles, predominantly due to challenges in promoting sulfur conversion reactions and simultaneously stabilizing cathode/electrolyte/anode interfaces. To tackle these issues, Fluoroisatin (FRN), as an electrolyte additive, was introduced in Li–S batteries, which dissolves in the electrolyte, undergoes partial deprotonation, and reacts with LiTFSI/lithium polysulfides. Consequently, it can regulate sulfur conversion pathways, accelerate reaction kinetics, and construct a LiF-rich solid-state electrolyte interface. The Li–S battery, with merely 0.5 wt% FRN additive and operating at −20°C, shows a high initial discharge capacity of 912 mAh g−1 at 0.2 C, and it is maintained at 830 mAh g−1 after 120 cycles. The potential of FRN, as a versatile electrolyte modifier, has potential for using in high-performance Li–S batteries.
锂硫电池面临着巨大的商业化障碍,主要是由于在促进硫转化反应和同时稳定阴极/电解质/阳极界面方面的挑战。为了解决这些问题,氟isatin (FRN)作为电解质添加剂被引入到Li-S电池中,它溶解在电解质中,经历部分去质子化,并与LiTFSI/锂多硫化物反应。因此,它可以调节硫转化途径,加速反应动力学,构建富liff固态电解质界面。仅添加0.5 wt% FRN且在- 20°C下工作的Li-S电池在0.2 C下显示出912 mAh g - 1的高初始放电容量,并且在120次循环后保持在830 mAh g - 1。FRN作为一种多用途的电解液改进剂,在高性能锂硫电池中具有应用潜力。
{"title":"Fluoroisatin Mediation Unlocks Durable Lithium–Sulfur Batteries Via Self-Regulating Solvation Engineering and SEI Reinforcement","authors":"Hongtian Ning, Jinxuan Zou, Yangyang Dong, Meiling Shu, Shuo Yang, Xuemei Zhou, Huagui Nie, Dong Cai, Zhanshuang Jin, Zhi Yang","doi":"10.1002/cnl2.70078","DOIUrl":"https://doi.org/10.1002/cnl2.70078","url":null,"abstract":"<p>Lithium–sulfur (Li–S) batteries face significant commercialization hurdles, predominantly due to challenges in promoting sulfur conversion reactions and simultaneously stabilizing cathode/electrolyte/anode interfaces. To tackle these issues, Fluoroisatin (FRN), as an electrolyte additive, was introduced in Li–S batteries, which dissolves in the electrolyte, undergoes partial deprotonation, and reacts with LiTFSI/lithium polysulfides. Consequently, it can regulate sulfur conversion pathways, accelerate reaction kinetics, and construct a LiF-rich solid-state electrolyte interface. The Li–S battery, with merely 0.5 wt% FRN additive and operating at −20°C, shows a high initial discharge capacity of 912 mAh g<sup>−1</sup> at 0.2 C, and it is maintained at 830 mAh g<sup>−1</sup> after 120 cycles. The potential of FRN, as a versatile electrolyte modifier, has potential for using in high-performance Li–S batteries.</p>","PeriodicalId":100214,"journal":{"name":"Carbon Neutralization","volume":"4 6","pages":""},"PeriodicalIF":12.0,"publicationDate":"2025-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cnl2.70078","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145521535","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}
Jiaxuan Zhu, Lin Zhao, Zhongkai Yu, Yue Xu, Jae Su Yu, Yongbin Hua
Thermal quenching has long plagued rare-earth-doped luminescent materials as an inherent limitation, severely hampering their practical deployment in complex environments. Herein, novel orange-red-emitting K3Sc(PO4)2:Sm3+ phosphors with anti-thermal quenching behavior have been successfully synthesized. The resultant samples have a trigonal crystal structure with space group P