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Metal chloride-graphite intercalation compounds for rechargeable metal-ion batteries 用于可充电金属离子电池的金属氯石墨插层化合物
IF 19.5 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-06 DOI: 10.1002/cey2.600
Anbang Lu, Fei Wang, Zhendong Liu, Yuchen Wang, Yue Gu, Shuang Wang, Chong Ye, Quanbing Liu, Chengzhi Zhang, Jun Tan

The typical metal chloride-graphite intercalation compounds (MC-GICs) inherit intercalation capacity, high charge conductivity, and high tap density from graphite, and these are considered as one of the promising alternatives of graphite anode in rechargeable metal-ion batteries (MIBs). Notably, the special interlayer decoupling effects and the introduction of extra conversion capacity by metal chloride could greatly break the capacity limitation of graphite anodes and achieve higher energy density in MIBs. The optimization of both graphite host and metal chloride species with specific structures endows MC-GICs with design feasibility for different application requirements of different MIBs, such as several times the actual capacity compared to graphite anodes, rapid migration of large carriers, and other properties. Herein, a brief review has been provided with the latest understanding of conductivity characteristics and energy storage mechanisms of MC-GICs and their interesting performance features of full potential application in rechargeable MIBs. Based on the existing research of MC-GICs, necessary improvements and prospects in the near future have been put forward.

典型的金属氯化物-石墨插层化合物(MC-GICs)继承了石墨的插层容量、高电荷传导性和高点密度,被认为是可充电金属离子电池(MIBs)中石墨负极的理想替代品之一。值得注意的是,特殊的层间退耦效应和金属氯化物引入的额外转换能力可大大打破石墨阳极的容量限制,并在 MIB 中实现更高的能量密度。通过对石墨母体和具有特定结构的金属氯化物的优化,MC-GICs 具有设计可行性,可满足不同 MIB 的不同应用要求,如实际容量是石墨阳极的数倍、大载流子的快速迁移等特性。本文简要回顾了对 MC-GIC 的电导特性和储能机制的最新理解,以及它们在可充电 MIB 中具有充分应用潜力的有趣性能特点。在现有 MC-GICs 研究的基础上,提出了必要的改进措施,并展望了不久的将来。
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引用次数: 0
Rationalizing the catalytic surface area of oxygen vacancy-enriched layered perovskite LaSrCrO4 nanowires on oxygen electrocatalyst for enhanced performance of Li–O2 batteries 合理利用氧电催化剂上富含氧空位的层状过氧化物 LaSrCrO4 纳米线的催化表面积,提高二氧化锰锂电池的性能
IF 19.5 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-06 DOI: 10.1002/cey2.550
Myeong-Chang Sung, Chan Ho Kim, Byoungjoon Hwang, Dong-Wan Kim

Efficient electrocatalysis at the cathode is crucial to addressing the limited stability and low rate capability of Li−O2 batteries. This study examines the kinetic behavior of Li−O2 batteries utilizing layered perovskite LaSrCrO4 nanowires (NWs) composed of lower oxidation states. Layered perovskite LaSrCrO4 NWs exhibited improved rate capability over a wide range of current densities and longer cycle life in Li−O2 batteries than V-based layered perovskite (LaSrVO4) and simple perovskite (La0.8Sr0.2CrO3) NWs. X-ray photoelectron spectroscopy and electrochemical surface area analyses showed that the observed performance variations primarily stemmed from active sites such as oxygen vacancies. In situ Raman analysis showed that these active sites significantly modulate the kinetics of oxygen reduction and evolution, which are related to LiO2 intermediate adsorption. Electrochemical impedance spectroscopy showed that the active sites in layered perovskite LaSrCrO4 NWs contributed to their high charge transfer capability and reduced polarization. This study presents an appealing method for the precise fabrication and analysis of Cr-based layered perovskites, aimed at achieving highly efficient and stable bifunctional oxygen electrocatalysis.

阴极的高效电催化对于解决二氧化锰锂电池的有限稳定性和低速率能力至关重要。本研究利用由低氧化态组成的层状过氧化物 LaSrCrO4 纳米线(NWs)研究了二氧化锰锂电池的动力学行为。与基于 V 的层状包晶体(LaSrVO4)和简单包晶体(La0.8Sr0.2CrO3)纳米线相比,层状包晶体 LaSrCrO4 纳米线在锂-O2 电池中表现出更高的电流密度范围内的速率能力和更长的循环寿命。X 射线光电子能谱和电化学表面积分析表明,观察到的性能变化主要源于氧空位等活性位点。原位拉曼分析表明,这些活性位点极大地调节了氧还原和进化的动力学,这与二氧化锂中间体的吸附有关。电化学阻抗光谱显示,层状包晶体 LaSrCrO4 纳米晶中的活性位点有助于提高电荷转移能力和降低极化。这项研究为精确制备和分析铬基层状包晶石提供了一种极具吸引力的方法,旨在实现高效稳定的双功能氧电催化。
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引用次数: 0
Determining materials for energy conversion across scales: The alkaline oxygen evolution reaction 确定跨尺度能量转换材料:碱性氧进化反应
IF 20.5 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-06 DOI: 10.1002/cey2.608
Philipp Gerschel, Steven Angel, Mohaned Hammad, André Olean-Oliveira, Blaž Toplak, Vimanshu Chanda, Ricardo Martínez-Hincapié, Sebastian Sanden, Ali Raza Khan, Da Xing, Amin Said Amin, Hartmut Wiggers, Harry Hoster, Viktor Čolić, Corina Andronescu, Christof Schulz, Ulf-Peter Apfel, Doris Segets
Despite considerable efforts to develop electrolyzers for energy conversion, progress has been hindered during the implementation stage by different catalyst development requirements in academic and industrial research. Herein, a coherent workflow for the efficient transition of electrocatalysts from basic research to application readiness for the alkaline oxygen evolution reaction is proposed. To demonstrate this research approach, La0.8Sr0.2CoO3 is selected as a catalyst, and its electrocatalytic performance is compared with that of the benchmark material NiFe2O4. The La0.8Sr0.2CoO3 catalyst with the desired dispersity is successfully synthesized by scalable spray-flame synthesis. Subsequently, inks are formulated using different binders (Nafion®, Naf; Sustainion®, Sus), and nickel substrates are spray coated, ensuring a homogeneous catalyst distribution. Extensive electrochemical evaluations, including several scale-bridging techniques, highlight the efficiency of the La0.8Sr0.2CoO3 catalyst. Experiments using the scanning droplet cell (SDC) indicate good lateral homogeneity for La0.8Sr0.2CoO3 electrodes and NiFe2O4-Sus, while the NiFe2O4-Naf film suffers from delamination. Among the various half-cell techniques, SDC proves to be a valuable tool to quickly check whether a catalyst layer is suitable for full-cell-level testing and will be used for the fast-tracking of catalysts in the future. Complementary compression and flow cell experiments provide valuable information on the electrodes' behavior upon exposure to chemical and mechanical stress. Finally, parameters and conditions simulating industrial settings are applied using a zero-gap cell. Findings from various research fields across different scales obtained based on the developed coherent workflow contribute to a better understanding of the electrocatalytic system at the early stages of development and provide important insights for the evaluation of novel materials that are to be used in large-scale industrial applications.
尽管在开发用于能源转换的电解槽方面做出了巨大努力,但在实施阶段,学术研究和工业研究对催化剂开发的不同要求阻碍了进展。在此,我们提出了一个连贯的工作流程,以实现碱性氧进化反应电催化剂从基础研究到应用准备的高效过渡。为了展示这种研究方法,我们选择了 La0.8Sr0.2CoO3 作为催化剂,并将其电催化性能与基准材料 NiFe2O4 进行了比较。通过可扩展的喷雾火焰合成法成功合成了具有理想分散性的 La0.8Sr0.2CoO3 催化剂。随后,使用不同的粘合剂(Nafion®,Naf;Sustainion®,Sus)配制油墨,并对镍基底进行喷涂,以确保催化剂的均匀分布。广泛的电化学评估,包括几种尺度桥接技术,凸显了 La0.8Sr0.2CoO3 催化剂的效率。使用扫描液滴池(SDC)进行的实验表明,La0.8Sr0.2CoO3 电极和 NiFe2O4-Sus 具有良好的横向均匀性,而 NiFe2O4-Naf 薄膜则存在分层现象。在各种半电池技术中,SDC 被证明是快速检查催化剂层是否适合全电池测试的重要工具,并将在未来用于催化剂的快速跟踪。压缩和流动池实验为电极暴露于化学和机械应力时的行为提供了有价值的信息。最后,使用零间隙电池模拟了工业环境的参数和条件。根据所开发的连贯工作流程从不同研究领域获得的不同规模的研究结果,有助于更好地了解处于开发早期阶段的电催化系统,并为评估将用于大规模工业应用的新型材料提供了重要见解。
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引用次数: 0
Unraveling reaction discrepancy and electrolyte stabilizing effects of auto-oxygenated porphyrin catalysts in lithium–oxygen and lithium–air cells 揭示锂-氧电池和锂-空气电池中自氧卟啉催化剂的反应差异和电解质稳定作用
IF 20.5 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-06 DOI: 10.1002/cey2.587
Boran Kim, Hyunyoung Park, Hyun-Soo Kim, Jun Seo Lee, Jongsoon Kim, Won-Hee Ryu
Lithium–oxygen (Li–O2) batteries are an emerging energy storage alternative with the potential to meet the recent increase in demand for high-energy-density batteries. From a practical viewpoint, lithium–air (Li–Air) batteries using ambient air instead of pure oxygen could be the final goal. However, the slow oxygen reduction and evolution reactions interfere with reversible cell operation during cycling. Therefore, research continues to explore various catalyst materials. The present study attempts to improve the performance of Li–Air batteries by using porphyrin-based materials known to have catalytic effects in Li–O2 batteries. The results confirm that the iron phthalocyanine (FePc) catalyst not only exhibits a catalytic effect in an air atmosphere with a low oxygen fraction but also suppresses electrolyte decomposition by stabilizing superoxide radical ions (O2) at a high voltage range. Density functional theory calculations are used to gain insight into the exact FePc-mediated catalytic mechanism in Li–Air batteries, and various ex situ and in situ analyses reveal the reversible reactions and structural changes in FePc during electrochemical reaction. This study provides a practical solution to ultimately realize an air-breathing battery using nature-friendly catalyst materials.
锂-氧(Li-O2)电池是一种新兴的储能替代品,有望满足近年来对高能量密度电池需求的增长。从实用角度来看,使用环境空气代替纯氧的锂-空气(Li-Air)电池可能是最终目标。然而,在循环过程中,缓慢的氧气还原和进化反应会干扰电池的可逆操作。因此,研究人员继续探索各种催化剂材料。本研究试图通过使用已知在锂-氧电池中具有催化作用的卟啉基材料来提高锂-空气电池的性能。研究结果证实,铁酞菁(FePc)催化剂不仅能在含氧量较低的空气环境中发挥催化作用,还能在高电压范围内通过稳定超氧自由基离子(O2-)抑制电解质分解。通过密度泛函理论计算,深入了解了 FePc 在锂空气电池中介导的确切催化机理,各种原位和原位分析揭示了 FePc 在电化学反应过程中的可逆反应和结构变化。这项研究为使用自然友好型催化剂材料最终实现空气呼吸电池提供了一种实用的解决方案。
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引用次数: 0
Back Cover Image, Volume 6, Number 8, August 2024 封底图片,第 6 卷第 8 号,2024 年 8 月
IF 19.5 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-29 DOI: 10.1002/cey2.653
Jundong Zhong, Tingting Xu, Hongyan Qi, Weibo Sun, Shuang Zhao, Zhe Zhao, Yirong Sun, Youliang Zhu, Jianxin Mu, Haibo Zhang, Xuanbo Zhu, Zhenhua Jiang, Lei Jiang

Back cover image: The ion transport properties of porous membrane materials are essential in numerous applications, and achieving synergistic enhancement of both permeability and selectivity remains a significant challenge. In the article number cey2.458, Zhu and co-workers reported a strategy to address this challenge by developing a charge-tunable nanofluidic membrane. Inserting chargetunable copolymers into GO membranes, effectively matches the charge density of the membrane with the pore size. This synergistic enhancement strategy led to a nearly 10-fold increase in osmotic energy generation, and it was expected to optimize the energy structure and promote the utilization and conversion of clean energy in the future.

封底图片:多孔膜材料的离子传输特性在众多应用中至关重要,而实现渗透性和选择性的协同增强仍是一项重大挑战。在cey2.458号文章中,Zhu及其合作者报告了一种通过开发电荷可调纳米流体膜来应对这一挑战的策略。在 GO 膜中插入电荷可调共聚物,可有效地使膜的电荷密度与孔径相匹配。这种协同增强策略使渗透能的产生增加了近10倍,有望在未来优化能源结构,促进清洁能源的利用和转化。
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引用次数: 0
Cover Image, Volume 6, Number 8, August 2024 封面图片,第 6 卷第 8 号,2024 年 8 月
IF 19.5 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-29 DOI: 10.1002/cey2.652
Wei Zhang, Hui Li, Daming Feng, Chenglin Wu, Chenghua Sun, Baohua Jia, Xue Liu, Tianyi Ma

Front cover image: Electrocatalytic CO2 reduction to syngas (CO and H2) offers an efficient way to mitigate carbon emissions and store intermittent renewable energy in chemicals. However, it is tricky to produce an adjustable ratio of syngas due to the difficulty of maintaining a balance between CO2 reduction reaction (CO2RR) and the competing hydrogen evolution reaction (HER). In article number cey2.461, Zhang et al. prepare hierarchical one-dimensional/three-dimensional nitrogen-doped porous carbon (1D/3D NPC) by carbonizing the composite of Zn-MOF-74 crystals in situ grown on a commercial melamine sponge (MS). Benefiting from the unique spatial environment of 1D/3D NPC, the reaction kinetics is significantly improved by increasing specific surface areas, CO2 adsorption, mass transport, and facilitating electron transfer from the 3D N-doped carbon framework to 1D porous carbon. The bifunctional activity of N-doped carbon materials for CO2RR and HER is beneficial for regulating the balance between CO2RR and HER. The carbonizing temperatures can affect the distribution of N species and further dominate syngas composition ratios.

封面图片:电催化二氧化碳还原为合成气(CO 和 H2)为减少碳排放和将间歇性可再生能源储存在化学品中提供了一种有效方法。然而,由于难以保持二氧化碳还原反应(CO2RR)和竞争性氢进化反应(HER)之间的平衡,要生产出比例可调的合成气十分困难。在cey2.461号文章中,Zhang等人通过对在商用三聚氰胺海绵(MS)上原位生长的Zn-MOF-74晶体复合材料进行碳化,制备了分层的一维/三维掺氮多孔碳(1D/3D NPC)。得益于 1D/3D NPC 独特的空间环境,通过增加比表面积、二氧化碳吸附、质量传输以及促进电子从三维掺氮碳框架转移到一维多孔碳,反应动力学得到了显著改善。掺杂 N 的碳材料对 CO2RR 和 HER 的双功能活性有利于调节 CO2RR 和 HER 之间的平衡。碳化温度会影响 N 物种的分布,并进一步主导合成气成分比。
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引用次数: 0
Enhancing the electrochemical performance of semicoke-based hard carbon anode through oxidation-crosslinking strategy for low-cost sodium-ion batteries 通过氧化-交联策略提高半焦基硬碳阳极的电化学性能,用于低成本钠离子电池
IF 20.5 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-26 DOI: 10.1002/cey2.584
Huizhen Ma, Yakun Tang, Bin Tang, Yue Zhang, Limin Deng, Lang Liu, Sen Dong, Yuliang Cao
Semicoke, a coal pyrolysis product, is a cost-effective and high-yield precursor for hard carbon used as anode in sodium-ion batteries (SIBs). However, as a thermoplastic precursor, semicoke inevitably graphitizes during high-temperature carbonization, so it is not easy to form the hard carbon structure. Herein, we propose an oxidation-crosslinking strategy to realize fusion-to-solid-state pyrolysis of semicoke. The semicoke is first preoxidized using a modified alkali-oxygen oxidation method to enrich its surface with carboxyl groups, which are localization points and the cross-linking reactions occur with citric acid to build the semicoke precursor with homogeneous and abundant -C-(O)–O- groups (up to 21 at% oxygen content). The -C-(O)–O- groups effectively prevent the rearrangement of carbon microcrystals in semicoke during carbonization, resulting in the formation of an abundant pseudographite structure with larger carbon interlayer spacing and micropores. The optimized semicoke-based hard carbon shows both a high initial Coulombic efficiency of 81% and a specific capacity of 307 mAh g−1, with low-voltage plateau capacity increased to 2.5 times, compared to that of the unmodified semicoke carbon. By the combination of detailed discharge curves and in situ X-ray diffraction analysis, the plateau capacity of semicoke-based hard carbon is mainly derived from interlayer intercalation of Na+ ion. The proposed oxidation-crosslinking strategy can contribute to the usage of low-cost and high-performance hard carbons in advanced SIBs.
Semicoke 是一种煤热解产物,是钠离子电池(SIB)中用作负极的硬质碳的一种低成本、高产出的前驱体。然而,作为一种热塑性前驱体,半焦在高温碳化过程中不可避免地会发生石墨化,因此不易形成硬碳结构。在此,我们提出了一种氧化-交联策略,以实现半焦的熔融-固态热解。首先使用改良的碱氧氧化法对半焦进行预氧化,使其表面富含作为定位点的羧基,然后与柠檬酸发生交联反应,形成具有均匀而丰富的 -C-(O)-O- 基团(氧含量高达 21%)的半焦前驱体。在碳化过程中,-C-(O)-O-基团可有效阻止半焦中碳微晶的重新排列,从而形成具有较大碳层间距和微孔的丰富假象石结构。优化后的半焦基硬质碳的初始库仑效率高达 81%,比容量为 307 mAh g-1,与未改性的半焦碳相比,低电压高原容量提高了 2.5 倍。结合详细的放电曲线和原位 X 射线衍射分析,半焦基硬质碳的高原容量主要来源于 Na+ 离子的层间插层。所提出的氧化-交联策略有助于在先进的 SIB 中使用低成本、高性能的硬质碳。
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引用次数: 0
Interfacial chemistry and structural engineering modified carbon fibers for stable sodium metal anodes 用于稳定钠金属阳极的界面化学和结构工程改性碳纤维
IF 20.5 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-23 DOI: 10.1002/cey2.601
Chenxiao Chu, Chunting Wang, Weisong Meng, Feipeng Cai, Bo Wang, Nana Wang, Jian Yang, Zhongchao Bai
Sodium (Na) metal stands out as a highly promising anode material for high-energy-density Na batteries owing to its abundant resources and exceptional theoretical capacity at low redox potential. Nevertheless, the uncontrolled growth of Na dendrites and the accompanying volumetric changes during the plating/stripping process lead to safety concerns and poor electrochemical performances. This study introduces nitrogen and oxygen co-doped carbon nanofiber networks wrapped carbon felt (NO-CNCF), serving as Na deposition skeletons to facilitate a highly reversible Na metal anode. The NO-CNCF framework with uniformly distributed “sodiophilic” functional groups, nanonetwork protuberances, and cross-linked network scaffold structure can avoid charge accumulation and facilitate the dendrite-free Na deposition. Benefiting from these features, the NO-CNCF@Na symmetrical cells demonstrate notable enhancements in cycling stability, achieving 4000 h cycles at 1 mA cm−2 for 1 mAh cm−2 and 2400 h cycles at 2 mA cm−2 for 2 mAh cm−2 with voltage overpotential of approximately 6 and 10 mV, respectively. Furthermore, the NVP//NO-CNCF@Na full cells achieve stable cycling performance and favorable rate capability. This investigation offers novel insights into fabricating a “sodiophilic” matrix with a multistage structure toward high-performance Na metal batteries.
金属钠(Na)资源丰富,在低氧化还原电位下具有超强的理论容量,是极具潜力的高能量密度钠电池阳极材料。然而,在电镀/剥离过程中,Na 树枝状突起的不可控生长和随之而来的体积变化会导致安全问题和较差的电化学性能。本研究引入氮氧共掺杂碳纳米纤维网络包裹碳毡(NO-CNCF)作为 Na 沉积骨架,以促进高度可逆的 Na 金属阳极。NO-CNCF骨架具有均匀分布的 "亲钠 "官能团、纳米网络突起和交联网络支架结构,可避免电荷积累,促进无树枝状的Na沉积。得益于这些特点,NO-CNCF@Na 对称电池的循环稳定性显著提高,1 mAh cm-2 的电池在 1 mA cm-2 下可循环 4000 小时,2 mAh cm-2 的电池在 2 mA cm-2 下可循环 2400 小时,过电位电压分别约为 6 mV 和 10 mV。此外,NVP//NO-CNCF@Na 全电池实现了稳定的循环性能和良好的速率能力。这项研究为制造具有多级结构的 "亲钠 "基质以实现高性能镍金属电池提供了新的见解。
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引用次数: 0
Rich electron delocalization structure in carbon nitride inducing radical transfer for high-performance photocatalytic uranyl reduction 氮化碳中诱导自由基转移的丰富电子致焦结构可实现高性能光催化铀酰还原
IF 20.5 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-23 DOI: 10.1002/cey2.636
Zhangmeng Liu, Yayao Li, Shuaiqi Yao, Runchao Zhou, Guiting Lin, Yunzhi Fu, Qixin Zhou, Wei Wang, Weijie Chi
Investigating the activation of the persulfate process through heterogeneous carbonaceous catalysts to expedite the reduction of uranyl ions (U(VI)) is imperative. The primary hurdle involves understanding the transfer and distribution of photogenerated carriers during the reduction process in this intricate system and deciphering the role of activated groups in promoting reduction efficiency. In this study, we strategically regulate the structure of polymeric carbon nitride to promote the N-doped state, thereby facilitating delocalization electron enrichment. The resulting active sites effectively activate peroxyl disulfate (PDS), generating radicals that expedite the selective reduction of U(VI). This strategic approach mitigates the inherent disadvantage of the short half-life of free radicals in persulfate-based advanced oxidation processes. As a consequence of our endeavors and with the simultaneous presence of PDS and hydrogen peroxide, we achieve an exceptional photoreduction efficiency of 100% within a remarkably short period of 20 min. This breakthrough presents a high-efficiency application with significant potential for addressing the pollution associated with uranyl-containing wastewater. Our findings not only contribute to the fundamental understanding of AOPs but also offer a practical solution with implications for environmental remediation.
研究通过异质碳质催化剂激活过硫酸盐过程以加快铀酰离子(U(VI))的还原过程势在必行。首要的障碍是了解光生载流子在这一错综复杂的系统中还原过程中的转移和分布,并破译活化基团在促进还原效率方面的作用。在这项研究中,我们对聚合氮化碳的结构进行了策略性调节,以促进 N 掺杂状态,从而促进电子富集。由此产生的活性位点可有效激活过氧二硫酸盐(PDS),产生自由基,从而加速 U(VI)的选择性还原。这种策略性方法缓解了基于过硫酸盐的高级氧化过程中自由基半衰期短的固有缺点。经过努力,在 PDS 和过氧化氢同时存在的情况下,我们在极短的 20 分钟内实现了 100% 的卓越光还原效率。这一突破为解决含铀废水污染问题提供了一种具有巨大潜力的高效应用。我们的研究成果不仅有助于从根本上理解 AOPs,还为环境修复提供了实用的解决方案。
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引用次数: 0
Ion-sieving MXene flakes with quantum dots enable high plating capacity for dendrite-free Zn anodes 带有量子点的离子筛MXene薄片可实现无枝晶锌阳极的高电镀能力
IF 19.5 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-23 DOI: 10.1002/cey2.603
Xinlong Liu, Bingang Xu, Shenzhen Deng, Jing Han, Yongling An, Jingxin Zhao, Qingjun Yang, Yana Xiao, Cuiqin Fang

The commercial utilization of Zn metal anodes with high plating capacity is significantly hindered by the uncontrolled growth of dendrites and associated side reactions. Herein, a robust artificial ion-sieving MXene flake (MXF)-coating layer, with abundant polar terminated groups, is constructed to regulate the interfacial Zn2+ deposition behavior. In particular, the fragmented MXF coupled with in situ generated quantum dots not only has strong Zn affinity to homogenize electric fields but also generates numerous zincophilic sites to reduce nucleation energy, thus securing a uniform dendrite-free surface. Additionally, the porous coating layer with polar groups allows the downward diffusion of Zn2+ to achieve bottom-up deposition and repels the excessive free water and anions to prevent parasitic reactions. The ion-sieving effect of MXF is firmly verified in symmetric cells with high areal capacity of 10–40 mAh cm−2 (1.0 mA cm−2) and depth of discharge of 15%–60%. Therefore, the functional MXF-coated anode manifests long-term cycling with 2700 h of stable plating/stripping in Zn||Zn cell. Such rational design of MXF protective layer breaks new ground in developing high plating capacity zinc anodes for practical applications.

具有高电镀能力的锌金属阳极的商业利用受到枝晶生长失控和相关副反应的严重阻碍。在此,我们构建了一种具有丰富极性终止基团的坚固人造离子筛分 MXene 片(MXF)涂层,以调节界面 Zn2+ 沉积行为。特别是,碎化的 MXF 与原位生成的量子点相结合,不仅具有很强的锌亲和力以均化电场,还能产生大量亲锌位点以降低成核能量,从而确保表面均匀无树枝状突起。此外,带有极性基团的多孔涂层允许 Zn2+ 向下扩散,实现自下而上的沉积,并能排斥过多的自由水和阴离子,防止寄生反应。MXF 的离子筛分效应在对称电池中得到了充分验证,其电池容量高达 10-40 mAh cm-2(1.0 mA cm-2),放电深度为 15%-60%。因此,在 Zn||Zn 电池中,功能性 MXF 涂层阳极可实现 2700 小时的稳定电镀/剥离长期循环。这种 MXF 保护层的合理设计为开发高电镀能力锌阳极的实际应用开辟了新天地。
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引用次数: 0
期刊
Carbon Energy
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