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Unveiling Na-ion storage mechanism and interface property of layered perovskite Bi2TiO4F2@rGO anode in ether-based electrolyte 揭示醚基电解质中层状过氧化物 Bi2TiO4F2@rGO 阳极的钠离子存储机理和界面特性
Pub Date : 2024-08-13 DOI: 10.1002/cnl2.163
Miao Yan, Qi Fang, Rui Ding, Yi Li, Jian Guo, Jinmei Xie, Yuzhen Zhang, Yuming He, Ziyang Yan, Zhiqiang Chen, Xiujuan Sun, Enhui Liu

To unveil the charge storage mechanisms and interface properties of electrode materials is very challenging for Na-ion storage. In this work, we report that the novel layered perovskite Bi2TiO4F2@reduced graphene oxides (BTOF@rGO) serves as a promising anode for Na-ion storage in an ether-based electrolyte, which exhibits much better electrochemical performance than in an ester-based electrolyte. Interestingly, BTOF@rGO possesses a prominent specific capacity of 458.3–102 mAh g−1/0.02–1 A g−1 and a high initial coulombic efficiency (ICE) of 70.3%. Cross-sectional morphology and depth profile surface chemistry indicate not only a denser reactive interfacial layer but also a superior solid electrolyte interface film containing a higher proportion of inorganic components, which accelerates Na+ migration and is an essential factor for the improvement of ICE and other electrochemical properties. Electrochemical tests and ex situ measurements demonstrate the triple hybridization Na-ion storage mechanism of conversion, alloying, and intercalation for BTOF@rGO in the ether-based electrolyte. Furthermore, the Na-ion batteries assembled with the BTOF@rGO anode and the commercial Na3V2(PO4)2F3@C cathode exhibit remarkable energy densities and power densities. Overall, the work shows deep insights on developing advanced electrode materials for efficient Na-ion storage.

要揭示电极材料的电荷存储机制和界面特性,对于瑙离子存储来说非常具有挑战性。在这项工作中,我们报告了新型层状包晶Bi2TiO4F2@还原石墨烯氧化物(BTOF@rGO)在醚基电解质中作为瑙离子存储阳极的前景,其电化学性能远远优于酯基电解质。有趣的是,BTOF@rGO 的比容量高达 458.3-102 mAh g-1/0.02-1 A g-1,初始库仑效率高达 70.3%。横截面形貌和深度剖面表面化学性质表明,不仅反应界面层更致密,而且固体电解质界面膜更优异,含有更高比例的无机成分,这加速了 Na+ 迁移,是提高 ICE 和其他电化学性能的重要因素。电化学测试和原位测量证明了 BTOF@rGO 在醚基电解质中的转化、合金化和插层三重杂化 Na 离子存储机制。此外,用 BTOF@rGO 阳极和商用 Na3V2(PO4)2F3@C 阴极组装的瑙离子电池表现出显著的能量密度和功率密度。总之,该研究成果对开发用于高效氖离子存储的先进电极材料具有深刻的启示。
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引用次数: 0
A systematic study of switching, optoelectronics, and gas-sensitive properties of PCF-graphene-based nanodevices: Insights from DFT study 对 PCF 石墨烯基纳米器件的开关、光电和气敏特性的系统研究:DFT 研究的启示
Pub Date : 2024-08-09 DOI: 10.1002/cnl2.156
Wenhao Yang, Tong Chen, Luzhen Xie, Yang Yu, Mengqiu Long, Liang Xu

Two-dimensional materials exhibit significant potential and wide-ranging application prospects owing to their remarkable tunability, pronounced quantum confinement effects, and notable surface sensitivity. The switching, optoelectronics, and gas-sensitive properties of the new carbon material poly-cyclooctatetraene framework (PCF)-graphene were systematically studied using density functional theory combined with the nonequilibrium Green's function method. First, the diode device based on PCF-graphene monolayer exhibited an impressive switching ratio of 106, demonstrating excellent diode characteristics. Moreover, in the investigation of the pin junction utilizing monolayer PCF-graphene, it is noteworthy that significant photocurrent responses were observed in both the zigzag and armchair directions, specifically within the visible and ultraviolet regions. Finally, gas sensors employing monolayer and bilayer PCF-graphene demonstrate significant chemical adsorption capabilities for NO and NO2. Notably, the maximum gas sensitivity for NO is achieved in monolayer PCF-graphene, reaching 322% at a bias voltage of 1.0 V. Meanwhile, for bilayer PCF-graphene-based gas sensor, the maximum gas sensitivity reaches 52% at a bias voltage of 0.4 V. In addition, the study also examined the influence of various environmental conditions, specifically H2O, O, and OH, on the system under investigation. The obtained results emphasize the multifunctional properties of PCF-graphene, exhibiting significant potential for various applications, including switching devices, optoelectronic devices, and gas sensors.

二维材料因其显著的可调谐性、明显的量子约束效应和明显的表面敏感性而展现出巨大的潜力和广泛的应用前景。本研究采用密度泛函理论结合非平衡格林函数方法,系统地研究了新型碳材料聚环辛四烯框架(PCF)-石墨烯的开关、光电和气敏特性。首先,基于 PCF-石墨烯单层的二极管器件的开关比达到了惊人的 106,显示出优异的二极管特性。此外,在研究利用单层 PCF 石墨烯的引脚结时,值得注意的是在之字形和扶手椅方向都观察到了显著的光电流响应,特别是在可见光和紫外线区域。最后,采用单层和双层 PCF 石墨烯的气体传感器对 NO 和 NO2 具有显著的化学吸附能力。值得注意的是,单层 PCF 石墨烯对 NO 的气体灵敏度最高,在偏置电压为 1.0 V 时达到 322%。同时,对于基于双层 PCF 石墨烯的气体传感器,在偏置电压为 0.4 V 时,最大气体灵敏度达到 52%。此外,研究还考察了各种环境条件(特别是 H2O、O 和 OH)对所研究系统的影响。研究结果表明,PCF-石墨烯具有多功能特性,在开关器件、光电器件和气体传感器等各种应用领域具有巨大潜力。
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引用次数: 0
Emerging strategies for the improvement of modifications in aqueous rechargeable zinc–iodine batteries: Cathode, anode, separator, and electrolyte 改进锌碘水性充电电池改性的新策略:阴极、阳极、隔膜和电解液
Pub Date : 2024-08-05 DOI: 10.1002/cnl2.155
Yuwei Zhao, Xinyu Chen, Weina Guo, Chenyang Zha

Aqueous rechargeable zinc–iodine batteries have gained traction as a promising solution due to their suitable theoretical energy density, cost-effectiveness, eco-friendliness, and safety features. However, challenges such as the polyiodide shuttle effect, low iodine cathode conductivity, zinc anode dendritic growth, and the requirement for efficient separators and electrolytes hinder their commercial prospects. Hence, this review highlights recent progress in refining the core optimization strategies of zinc–iodine batteries, focusing on enhancements to the cathode, anode, separator, and electrolyte. Cathode improvements involve the addition of inorganic, organic, and hybrid materials to counteract the shuttle effect and boost redox kinetics, where these functional materials also are applied in anode modifications to curb dendritic growth and enhance cycling stability. Meanwhile, cell separator design approaches that effectively block polyiodide shuttle while promoting uniform zinc deposition are also discussed, while electrolyte innovations target zinc corrosion and polyiodide dissolution. Ultimately, the review aims to map out a strategy for developing zinc–iodine batteries that are efficient, safe, and economical, aligning with the demands of contemporary energy storage.

锌碘水溶液可充电电池因其合适的理论能量密度、成本效益、生态友好性和安全特性,作为一种有前途的解决方案而备受关注。然而,聚碘穿梭效应、低碘阴极电导率、锌阳极树枝状生长以及对高效分离器和电解质的要求等挑战阻碍了其商业前景。因此,本综述着重介绍了在完善锌碘电池核心优化策略方面的最新进展,重点关注阴极、阳极、隔膜和电解液的改进。阴极的改进包括添加无机、有机和混合材料,以抵消穿梭效应并提高氧化还原动力学,这些功能性材料还可用于阳极改造,以抑制树枝状生长并提高循环稳定性。同时,还讨论了在促进锌均匀沉积的同时有效阻止多碘化物穿梭的电池分离器设计方法,以及针对锌腐蚀和多碘化物溶解的电解质创新。最后,本综述旨在为开发高效、安全、经济的锌碘电池制定战略,以满足当代能源存储的需求。
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引用次数: 0
Front Cover: Carbon Neutralization, Volume 3, Issue 4, July 2024 封面:碳中和》,第 3 卷第 4 期,2024 年 7 月
Pub Date : 2024-07-29 DOI: 10.1002/cnl2.159

Front cover image: By serving as conductive binders, active material hosts, current collectors, and even as components of separators and interlayers, MXenes have demonstrated their adaptability and multifunctionality in different battery chemistries. Their ability to mitigate issues like dendrite growth, shuttle effects, and poor mechanical stability have significant implications for extending battery lifespan, increasing energy density, and ensuring operational safety.

封面图片:通过充当导电粘合剂、活性材料宿主、电流收集器,甚至作为隔膜和夹层的成分,MXenes 已证明了其在不同电池化学成分中的适应性和多功能性。它们能够缓解枝晶生长、穿梭效应和机械稳定性差等问题,对延长电池寿命、提高能量密度和确保操作安全具有重要意义。
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引用次数: 0
Back Cover Image: Carbon Neutralization, Volume 3, Issue 4, July 2024 封底图片:碳中和》,第 3 卷第 4 期,2024 年 7 月
Pub Date : 2024-07-29 DOI: 10.1002/cnl2.161

Back cover image: Currently, developing advanced energy storage and conversion systems is of great significance. In the review, the strategies for realizing high-performance anode-free rechargeable batteries enabled by interfacial regulation engineering are summarized, mainly including designing of current collector, introducing of surface coating layers, modification of electrolyte, separators engineering and cathode materials regulation.

封底图片:当前,开发先进的能量存储和转换系统意义重大。本综述总结了通过界面调控工程实现高性能无阳极充电电池的策略,主要包括集流体设计、表面涂层引入、电解质改性、隔膜工程和阴极材料调控。
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引用次数: 0
Inside Front Cover Image: Carbon Neutralization, Volume 3, Issue 4, July 2024 封面内页图片:碳中和》,第 3 卷第 4 期,2024 年 7 月
Pub Date : 2024-07-29 DOI: 10.1002/cnl2.160

Inside front cover image: The image is related to the recycling of chicken feathers, aiming to state the energy and environmental applications of materials derived from chicken feathers. In this image, the applications, such as battery, catalysis and architectural field, surround a chicken feather, demonstrating the application potential of chicken feather waste. Besides, the clear water and beautiful environment indicate the effectiveness of recycled chicken feathers in energy and environmental fields.

封面内页图片:该图片与鸡毛的回收利用有关,旨在说明从鸡毛中提取的材料在能源和环境方面的应用。在这幅图中,电池、催化和建筑领域等应用围绕着一根鸡毛,展示了鸡毛废弃物的应用潜力。此外,清澈的水和优美的环境也表明了回收鸡毛在能源和环境领域的有效性。
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引用次数: 0
Modulation of the multiphase phosphorus/sulfide heterogeneous interface via rare earth for solar-enhanced water splitting at industrial-level current densities 通过稀土调制多相磷/硫化物异质界面,在工业级电流密度下实现太阳能增强型水分离
Pub Date : 2024-07-28 DOI: 10.1002/cnl2.157
Yikun Cheng, Pengjie Fu, Zhipeng Yu, Xiaodong Yang, Yangrui Zhang, Aojie Yuan, Huan Liu, Jianhao Du, Long Chen

Photoelectrically coupling water splitting at high current density is a promising approach for the acquisition of green hydrogen energy. However, it places significant demands on the photo/electrocatalysts. Herein, rare earth elements doping NiMoO4-based phosphorus/sulfide heterostructure nanorod arrays (RE-NiMo-PS@NF [RE = Y, Er, La, and Sc]) are obtained for solar-enhanced electrocatalytic water splitting at high current densities. The results of the experiment and density-functional theory studies illustrate that the Y element as a dopant not only makes the NiMoP2/NiMo3S4/NiMoO4 heterostructure exhibit excellent solar-enhanced electrocatalytic activity (hydrogen evolution reaction [HER]: η1000 = 211 mV, oxygen evolution reaction [OER]: η1000 = 367 mV) but also optimizes the heterostructure interfacial electron density distributions and HER free energy. In addition, Y-NiMo-PS@NF achieves 18.64% solar-to-hydrogen efficiency. This study not only provides a new way to synthesize heterostructure electrocatalysts but also inspires the application of solar enhancement strategies for high current density water splitting.

在高电流密度下进行光电耦合水分裂是获得绿色氢能的一种前景广阔的方法。然而,这对光电催化剂提出了很高的要求。本文研究了掺杂稀土元素的基于 NiMoO4 的磷/硫化物异质结构纳米棒阵列(RE-NiMo-PS@NF [RE = Y、Er、La 和 Sc]),用于在高电流密度下进行太阳能增强电催化水分离。实验和密度泛函理论研究结果表明,Y 元素作为掺杂剂不仅使 NiMoP2/NiMo3S4/NiMoO4 异质结构表现出优异的太阳能增强电催化活性(氢进化反应 [HER]:η1000 = 211 mV,氧进化反应 [OER]:η1000 = 367 mV),而且优化了异质结构界面电子密度分布和氢进化反应自由能。此外,Y-NiMo-PS@NF 还实现了 18.64% 的太阳能制氢效率。这项研究不仅为合成异质结构电催化剂提供了一种新方法,而且还为应用太阳能增强策略实现高电流密度水分离提供了灵感。
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引用次数: 0
Bismuth-based metal-organic frameworks and derivatives for photocatalytic applications in energy and environment: Advances and challenges 铋基金属有机框架及其衍生物在能源和环境领域的光催化应用:进展与挑战
Pub Date : 2024-07-04 DOI: 10.1002/cnl2.153
Yankun Wang, He Sun, Zhuxian Yang, Yanqiu Zhu, Yongde Xia

Photocatalysis is an environmentally friendly technology for the utilizations of solar energy and has garnered significant attention in both scientific and industrial sectors. Developing cost-effective semiconductive materials is the core issue in photocatalysis. Bismuth-based metal-organic frameworks (Bi-MOFs) have emerged as attractive candidates in various photocatalytic applications, and Bi-MOFs derivatives further expand and consolidate their promising potential in the realm of photocatalysis. Various modification strategies including in-situ tailoring or external doping, as well as meticulous design and selection of metal nodes and organic linkers allow for fine control over the surface multifunctionality in Bi-MOF-based and derived photocatalytic composites with adjustable energy band structures and enhanced photocatalytic performance. In this review, the recent progress in the synthesis of diverse Bi-MOFs-based materials, Bi-MOFs derivatives, and their Bi-containing semiconductive composites were systemically analyzed and reviewed. The state-of-the-art research progresses in the applications of Bi-MOFs and derivatives, as well as composites in photocatalytic water splitting for hydrogen production, photodegradation of organic pollutants, and photocatalytic carbon dioxide reduction are comprehensively summarized. The relationships between structures, properties, and photocatalytic performance of Bi-based semiconductive composites are discussed in detail. In addition, the perspectives and future challenges on Bi-MOFs-based and derived materials for photocatalytic applications are also offered.

光催化是一种利用太阳能的环保技术,在科学界和工业界都备受关注。开发具有成本效益的半导体材料是光催化技术的核心问题。铋基金属有机框架(Bi-MOFs)已成为各种光催化应用中极具吸引力的候选材料,Bi-MOFs 衍生物进一步拓展和巩固了其在光催化领域的巨大潜力。各种改性策略,包括原位定制或外部掺杂,以及金属节点和有机连接体的精心设计和选择,使得基于 Bi-MOF 及其衍生光催化复合材料的表面多功能性得到精细控制,能带结构可调,光催化性能增强。在这篇综述中,系统分析和综述了最近在合成各种基于 Bi-MOFs 的材料、Bi-MOFs 衍生物及其含 Bi- 半导体复合材料方面取得的进展。全面总结了 Bi-MOFs 及其衍生物和复合材料在光催化水分离制氢、光降解有机污染物和光催化还原二氧化碳等方面的最新研究进展。详细讨论了 Bi 基半导体复合材料的结构、性能和光催化性能之间的关系。此外,还对基于 Bi-MOFs 的光催化应用及其衍生材料的前景和未来挑战进行了展望。
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引用次数: 0
Research progress of electrocatalysts for hydrogen oxidation reaction in alkaline media 碱性介质中氢氧化反应电催化剂的研究进展
Pub Date : 2024-06-25 DOI: 10.1002/cnl2.152
Youze Zeng, Xue Wang, Yang Hu, Wei Qi, Zhuoqi Wang, Meiling Xiao, Changpeng Liu, Wei Xing, Jianbing Zhu

Anion exchange membrane fuel cells (AEMFCs) have been hailed as a promising hydrogen energy technology due to high energy conversion efficiency, zero carbon emission and the potential independence on scare and expensive noble metal electrocatalysts. A variety of platinum group metal (PGM)-free catalysts has been developed with superior catalytic performance to noble metal benchmarks toward cathodic oxygen reduction reactions (ORR). However, PGM electrocatalysts still dominate the anodic catalyst research because the kinetics of hydrogen oxidation reaction (HOR) are two or three orders of magnitude slower than in that acidic media. Therefore, it is urgently desirable to improve noble metal utilization efficiency and/or develop high-performance PGM-free electrocatalysts for HOR, thus promoting the real-world implementation of AEMFCs. In this review, the current research progress of electrocatalysts for HOR in alkaline media is summarized. We start with the discussion on the current HOR reaction mechanisms and existing controversies. Then, methodologies to improve the HOR performance are reviewed. Following these principles, the recently developed HOR electrocatalysts including PGM and PGM-free HOR electrocatalysts in alkaline media are systematically introduced. Finally, we put forward the challenges and prospects in the field of HOR catalysis.

阴离子交换膜燃料电池(AEMFCs)具有高能量转换效率、零碳排放以及独立于昂贵的贵金属电催化剂的潜力,因此被誉为前景广阔的氢能技术。目前已开发出多种不含铂族金属(PGM)的催化剂,其阴极氧还原反应(ORR)的催化性能优于贵金属基准。然而,由于氢氧化反应(HOR)的动力学比在酸性介质中慢两到三个数量级,因此铂族金属电催化剂仍然在阳极催化剂研究中占主导地位。因此,当务之急是提高贵金属的利用效率和/或开发高性能的不含 PGM 的氢氧化反应电催化剂,从而促进 AEMFCs 在现实世界中的应用。本综述总结了目前碱性介质中 HOR 电催化剂的研究进展。我们首先讨论了当前的 HOR 反应机理和存在的争议。然后,回顾了提高 HOR 性能的方法。根据这些原则,系统介绍了最近开发的 HOR 电催化剂,包括碱性介质中的 PGM 和无 PGM HOR 电催化剂。最后,我们提出了 HOR 催化领域的挑战和前景。
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引用次数: 0
Recent advances in robust and ultra-thin Li metal anode 坚固超薄锂金属阳极的最新进展
Pub Date : 2024-06-17 DOI: 10.1002/cnl2.147
Zheng Luo, Yang Cao, Guobao Xu, Wenrui Sun, Xuhuan Xiao, Hui Liu, Shanshan Wang

Li metal batteries have been widely expected to break the energy-density limits of current Li-ion batteries, showing impressive prospects for the next-generation electrochemical energy storage system. Although much progress has been achieved in stabilizing the Li metal anode, the current Li electrode still lacks efficiency and safety. Moreover, a practical Li metal battery requires a thickness-controllable Li electrode to maximally balance the energy density and stability. However, due to the stickiness and fragile nature of Li metal, manufacturing Li ingot into thin electrodes from conventional approaches has historically remained challenging, limiting the sufficient utilization of energy density in Li metal batteries. Aiming at the practical application of Li metal anode, the current issues and their initiation mechanism are comprehensively summarized from the stability and processability perspectives. Recent advances in robust and ultra-thin Li metal anode are outlined from methodology innovation to provide an overall insight. Finally, challenges and prospective developments regarding this burgeoning field are critically discussed to afford future outlooks. With the development of advanced processing and modification technology, we are optimistic that a truly great leap will be achieved in the foreseeable future toward the industrial application of Li metal batteries.

人们普遍期待锂金属电池能够突破目前锂离子电池的能量密度极限,为下一代电化学储能系统展现出令人瞩目的前景。虽然在稳定锂金属阳极方面取得了很大进展,但目前的锂电极仍然缺乏效率和安全性。此外,实用的金属锂电池需要厚度可控的锂电极,以最大限度地平衡能量密度和稳定性。然而,由于锂金属的粘性和易碎性,用传统方法将锂锭制成薄电极一直是个挑战,限制了锂金属电池能量密度的充分发挥。针对锂金属负极的实际应用,本文从稳定性和可加工性的角度全面总结了当前存在的问题及其引发机制。此外,还从方法创新的角度概述了坚固超薄锂金属阳极的最新进展,以提供全面的见解。最后,批判性地讨论了这一新兴领域所面临的挑战和发展前景,以展望未来。随着先进加工和改性技术的发展,我们相信在可预见的未来,锂金属电池的工业应用将实现真正的飞跃。
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引用次数: 0
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