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Reconciling electrolyte donicity and polarity for lithium carbon fluoride batteries 协调氟化碳锂电池的电解质同源性和极性
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-19 DOI: 10.1039/d4ee01793e
Xingxing Wang, Ziyu Song, Hao Wu, Jiayi Chen, Wenfang Feng, Michel Armand, Zhi-Bin Zhou, Heng Zhang
Among existing electrochemical energy storage technologies, lithium carbon fluoride (Li°||CFx) batteries have captured enormous attention owing to their surprisingly high energy density and low self-discharge rate. The features of nonaqueous electrolytes play an essential role in determining the electrochemical reactions of CFx cathode, and subsequently impacting the electrochemical performances of the Li°||CFx batteries. Herein, differing from previous stereotypical perceptions, the fascinatingly entangled parameters of non-aqueous electrolytes, enlisting permittivity, donicity, and polarity, are comprehensively investigated and reconciled, adopting the solution mixtures of 1,2-dimethoxyethane (DME) and propylene carbonate (PC). The results demonstrate that a higher donicity and moderate polarity of nonaqueous electrolytes (e.g., DME-rich electrolytes) favor the heterolytic dissociation of carbon-fluorine bonds, resulting in more complete electrochemical conversions of CFx cathode. This work not only brings a fresh mechanism understanding on the electrochemical reaction paths of CFx cathode, but also spurs the electrolyte design for high-energy batteries with other conversion-type electrode materials (e.g., sulfur, oxygen).
在现有的电化学储能技术中,氟化碳锂(Li°||CFx)电池因其惊人的高能量密度和低自放电率而备受关注。非水电解质的特性对碳氟化合物阴极的电化学反应起着至关重要的作用,并进而影响锂碳氟化合物电池的电化学性能。本文有别于以往的陈旧观念,采用 1,2 二甲基乙烷(DME)和碳酸丙烯酯(PC)的溶液混合物,全面研究和协调了非水电解质的介电常数、唐氏常数和极性等令人着迷的纠缠参数。结果表明,非水电解质(如富含二甲醚的电解质)中较高的别离度和适度的极性有利于碳-氟键的异解,从而使 CFx 阴极的电化学转化更加完全。这项工作不仅为 CFx 阴极的电化学反应路径带来了全新的机理认识,还推动了使用其他转换型电极材料(如硫、氧)的高能电池的电解质设计。
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引用次数: 0
Regulating electron spin orbital by sulfur atoms-doped Ti vacancies to manipulate spin flip for enhancing PEC water splitting 通过掺杂硫原子的钛空位调节电子自旋轨道,操纵自旋翻转以提高 PEC 水分离效果
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-19 DOI: 10.1039/d4ee02674h
Yixuan Gao, Min Zhang, Qi Zhao, Wen Liu, Lirong Zheng, Jin Ouyang, Na Na
Titanium dioxide (TiO2) as semiconductor photocatalysis has been broadly investigated due to its high chemical stability, nontoxicity and low cost. Nevertheless, TiO2 still suffers from low visible-light response and rapid photogenerated charge carrier recombination. Herein, to overcome the limitation of TiO2, the incorporation of different sulfur sources in Ti vacancy defects was constructed by vacancy capture strategy. Compared to oxygen vacancies, the Ti vacancies (VTi) on TiO2 can induce the transfer of electrons from electron spin-down orbital (↓) in valence band to electron spin-up orbital (↑) in conduction band. The excited electrons are forbidden to spin-down orbital in valence band due to spin pinning effect, which inhibits recombination of electron-hole pairs for enhancing PEC water splitting performance. More significantly, the sulfur dopants can manipulate electron spin flip to regulate the electron spin direction and increase the number of charge carriers. This can solve pretty key problem of the common doping strategy, which is high recombination rate of electron-hole pairs due to the reduced band gap through doping p state above the valence band. This work provides an efficient pathway to improve PEC activity by manipulating spin flip through cationic vacancy modification technology.
二氧化钛(TiO2)具有化学稳定性高、无毒、成本低等特点,因此作为半导体光催化材料已被广泛研究。然而,二氧化钛仍然存在可见光响应低和光生电荷载流子快速重组的问题。在此,为了克服 TiO2 的局限性,我们采用空位捕获策略在 Ti 空位缺陷中掺入了不同的硫源。与氧空位相比,TiO2 上的钛空位(VTi)能诱导电子从价带的电子自旋下降轨道(↓)转移到导带的电子自旋上升轨道(↑)。由于自旋锁定效应,受激电子被禁止进入价带的自旋下降轨道,从而抑制了电子-空穴对的重组,提高了 PEC 水分离性能。更重要的是,硫掺杂剂可以操纵电子自旋翻转,从而调节电子自旋方向,增加电荷载流子的数量。这可以解决普通掺杂策略的关键问题,即通过在价带上方掺杂 p 态而降低带隙导致的电子-空穴对高重组率。这项工作通过阳离子空位修饰技术操纵自旋翻转,为提高 PEC 活性提供了一条有效途径。
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引用次数: 0
Deciphering the dynamic interfacial chemistry of calcium metal anodes 解读钙金属阳极的动态界面化学性质
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-18 DOI: 10.1039/d4ee01257g
Huijun Lin, Jiayi Meng, Weihua Guo, Renjie Li, Yuyang Yi, Yiyuan Ma, Chi Fai Cheung, Doron Aurbach, Zheng-Long Xu
Calcium (Ca) metal batteries, due to the high crustal abundance and potential for dendrite-free cycling of Ca, are promising alternative to current lithium battery chemistry. Ca deposition in aprotic organic electrolytes had been stalled by ion-blocking passivation layers on Ca metal. This limitation was recently overcome by using borate-based electrolyte solutions, but the electrode/electrolyte interfacial chemistry enabling reversible Ca metal deposition remains unclear. This study elucidates the formation and dynamic evolution of passivation layers upon immersion of Ca metal electrodes and during electrochemical Ca deposition/dissolution processes in a representative calcium tetrakis(hexafluoroisopropyloxy)-borate (Ca[B(hfip)4]2) and glyme electrolyte solution. Upon ageing, a native passivation layer comprising porous Ca metal and Ca ion conducting solid-electrolyte interphase is formed. In subsequent electrochemical cycles, the pre-passivated Ca metal shows superior activities compared to fresh Ca electrodes. Nevertheless, the electrolyte solution can penetrate the passivating layer to further corrode Ca metal to form secondary passivation layers, compromising cyclic stability. The native passivation layer, on the other hand, can facilitate Ca metal reversibility in otherwise incompatible electrolyte solutions, such as Ca(TFSI)2 in glyme. New insights related to the interfacial chemistry of Ca metal can spur the advancement of anticorrosion interphases or electrolyte systems for rechargeable Ca metal batteries.
钙(Ca)金属电池因其地壳丰度高和无枝晶循环的潜力,有望成为当前锂电池化学的替代品。钙金属上的离子阻挡钝化层阻碍了钙在非沸腾有机电解质中的沉积。最近,通过使用基于硼酸盐的电解质溶液克服了这一限制,但使钙金属可逆沉积的电极/电解质界面化学仍不清楚。本研究阐明了钙金属电极浸泡时以及在代表性四(六氟异丙基氧基)硼酸钙(Ca[B(hfip)4]2)和甘油醚电解质溶液中电化学钙沉积/溶解过程中钝化层的形成和动态演化。在老化过程中,会形成由多孔钙金属和钙离子导电固态电解质间相组成的原生钝化层。在随后的电化学循环中,预钝化钙金属的活性优于新鲜的钙电极。然而,电解质溶液会渗透钝化层,进一步腐蚀钙金属,形成二次钝化层,从而影响循环稳定性。另一方面,原生钝化层可以促进钙金属在其他不相容的电解质溶液中的可逆性,例如甘氨中的 Ca(TFSI)2。有关钙金属界面化学的新见解可促进可充电钙金属电池的防腐蚀中间层或电解质系统的发展。
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引用次数: 0
Cosolvent Occupied Solvation Tuned Anti-Oxidation Therapy Toward Highly Safe 4.7V-Class NCM811 Battery 共溶剂占有溶解调谐抗氧化疗法实现高度安全的 4.7V 级 NCM811 电池
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-18 DOI: 10.1039/d4ee02074j
Yuqing Chen, Yun Zhao, Aiping Wang, Daozhen Zhang, Baohua Li, Xiangming He, Xiulin Fan, Jilei Liu
Fluorinated electrolytes are promising for stabilizing the interfacial chemistry in high-voltage LiNi0.8Co0.1Mn0.1O2 (NCM811) batteries. However, previous fluorinated electrolytes overlooked the essential role of the cathode-electrolyte interface (CEI) on de-solvation, relying heavily on weak solvation. Theoretically, the cosolvent occupied solvation structure characteristic of highly antioxidative cosolvent and the easily oxidized salt additive in the first solvation shell, is highly desirable to both widen electrochemical window and promote anion-enriched CEI to facilitate the de-solvation. The key challenges lie in identifying ideal cosolvents that are highly polar, antioxidative, and with stronger interaction with anions, to replace the solvation site of the main solvents without oxidation of itself and promote the oxidation of additive anions. Herein sulfone (SL) and DFOB- are screened out following developed rules, the interaction relationships are: i) Li+ - cosolvent > Li+- main solvent; ii) DFOB- - cosolvent > DFOB- - main solvent; iii) DFOB- - cosolvent > DFOB- - Li+. And optimized fluorinated electrolyte composed of 10% SL and 0.02 M LiDFOB is therefore successfully developed. This occupied solvation design promotes both interfacial/ anodic stability and de-solvation under an aggressive 4.7 V. Consequently, ~400 Wh kg-1 NCM811/Li cells at 4.7 V demonstrate an 82% capacity retention after 200 cycles. Commercial NCM811/Gr pouch cells at 4.5 V achieve 92% capacity retention over 500 cycles, concurrently with unexpectedly high safety performance in terms of thermal, mechanical, and electrical abuse. This work underscores the critical impact of solvation site-occupied cosolvent on the CEI modification and kinetics optimization, opening a new avenue for high voltage electrolyte design.
氟化电解质有望稳定高压镍钴锰锂电池(NCM811)的界面化学。然而,以往的含氟电解质忽视了阴极-电解质界面(CEI)对去溶解的重要作用,而严重依赖于弱溶解。从理论上讲,具有高抗氧化性的共溶剂和第一溶壳中易氧化的盐添加剂所构成的共溶剂占位溶解结构是非常理想的,既能拓宽电化学窗口,又能促进阴离子富集的阴极-电解质界面(CEI),从而促进去溶解。关键的挑战在于找到极性强、抗氧化、与阴离子相互作用更强的理想助溶剂,以取代主溶剂的溶解位点而不使其本身氧化,并促进添加剂阴离子的氧化。在此,根据制定的规则筛选出砜(SL)和 DFOB-,其相互作用关系为:i) Li+ - 助溶剂 > Li+ - 主溶剂;ii) DFOB- - 助溶剂 > DFOB- - 主溶剂;iii) DFOB- - 助溶剂 > DFOB- - Li+。因此,由 10% SL 和 0.02 M LiDFOB 组成的优化含氟电解质研制成功。这种占位溶解设计既能提高界面/阳极稳定性,又能在苛刻的 4.7 V 电压下去溶解。因此,在 4.7 V 电压下,约 400 Wh kg-1 的 NCM811/Li 电池在 200 次循环后显示出 82% 的容量保持率。4.5 V 的商用 NCM811/Gr 袋式电池在 500 次循环后的容量保持率达到 92%,同时在热滥用、机械滥用和电气滥用方面具有出乎意料的高安全性能。这项工作强调了溶解位点共溶剂对 CEI 改性和动力学优化的关键影响,为高压电解液的设计开辟了一条新途径。
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引用次数: 0
Doping engineering of Cu-based catalysts for electrocatalytic CO2 reduction to multi-carbon products 用于电催化二氧化碳还原为多碳产品的铜基催化剂掺杂工程
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-18 DOI: 10.1039/d4ee01325e
Shiya You, Jiewen Xiao, Shuyu Liang, Wenfu Xie, Tianyu Zhang, Min Li, Ziyi Zhong, Qiang Wang, Hong He
Electrocatalytic carbon dioxide reduction (CO2RR) is a promising technology that uses renewable energy sources to convert excess atmospheric CO2 into high-value multi-carbon (C2+) products. In the CO2RR mechanism, adsorbed *CO is recognized as a crucial intermediate, playing a pivotal role in facilitating the formation of C2+ products. Currently, Cu-based materials are the most effective catalysts in producing the *CO and further coupling it to form C2+ products. However, mono-component Cu catalysts still face some challenges, such as low activity, selectivity, and poor stability. Doping engineering has emerged as a valuable strategy for enhancing the performance of Cu-based catalysts in CO2 electroreduction into C2+ products. This comprehensive review presents the recent advancements in CO2 electroreduction into C2+ products over heteroatom-doped Cu-based catalysts, encompassing metallic heteroatoms such as Pd, Au and Ag, as well as non-metallic heteroatoms like P, B and F. The mechanism of enhanced performance through heteroatom doping is specifically highlighted, providing helpful guidance and avenues for the rational design of Cu-based catalysts. Additionally, the review discusses the challenges and prospects associated with CO2RR into C2+ products, offering a nuanced perspective on this subject.
电催化二氧化碳还原(CO2RR)是一项前景广阔的技术,它利用可再生能源将大气中过剩的二氧化碳转化为高价值的多碳(C2+)产品。在 CO2RR 机制中,吸附的 *CO 被认为是一个关键的中间体,在促进 C2+ 产品的形成方面发挥着举足轻重的作用。目前,铜基材料是产生 *CO 并进一步偶联形成 C2+ 产物的最有效催化剂。然而,单组分铜催化剂仍然面临着一些挑战,如活性低、选择性差、稳定性差等。掺杂工程已成为提高铜基催化剂在 CO2 电还原成 C2+ 产物过程中性能的重要策略。本综述介绍了杂原子掺杂的 Cu 基催化剂将 CO2 电还原成 C2+ 产物的最新进展,包括 Pd、Au 和 Ag 等金属杂原子以及 P、B 和 F 等非金属杂原子。此外,综述还讨论了将 CO2RR 转化为 C2+ 产品所面临的挑战和前景,为这一主题提供了一个细致入微的视角。
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引用次数: 0
Subnano confinement in robust MoS2-based membranes for high-performance osmotic energy conversion 在基于 MoS2 的坚固膜中实现亚纳米约束,实现高性能渗透能量转换
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-18 DOI: 10.1039/d4ee01381f
Xuying Wang, Zhaoyi Wang, Zhiwei Xue, Yiyi Fan, Jing Yang, Naitao Yang, Qingxiao Zhang, Xiuxia Meng, Yun Jin, Shaomin Liu
Osmotic energy harvesting from salinity gradients shows great potential for sustainable electricity generation, which can be fulfilled using two-dimensional ion-selective nanofluidic devices. Metal dichalcogenide membranes like MoS2 exhibit good anti-swelling properties in aqueous solution and can be applied in nanofluidic device development. However, conventional MoS2-based membranes encounter the major issue of low ion selectivity, reducing the electricity generation efficiency. In this paper, we propose the strategy of subnano confinement using the environmentally benign hydrophilic bacterial nanocellulose (BNC) with negative charges to create high ion-selectivity channels in robust MoS2-based membranes. The developed membrane exhibited the interlayer spacing of 9.8 Å with desirable negativity in nanochannels, thus generating a favorable confinement for enhancing Na+ transport but blocking Cl-. The tested membrane provided the area of 0.78 mm2, exceeding other reported macroscopic-scale membranes. The electrochemical device delivered the power density of 73 and 233 W m-2 at ambient temperature and 343 K, respectively, in a 50-fold concentration gradient, outperforming previously reported 2D nanofluidic membranes by a factor up to 70. Furthermore, the membrane exhibited exceptional long-term stability up to 40 days without performance decay. The current work makes a breakthrough in developing 2D nanofluidic membranes for harvesting osmotic energy.
从盐度梯度中收集渗透能显示了可持续发电的巨大潜力,可利用二维离子选择性纳米流体装置来实现。二卤化金属膜(如 MoS2)在水溶液中具有良好的抗溶胀特性,可用于纳米流体装置的开发。然而,传统的 MoS2 基膜存在离子选择性低的主要问题,从而降低了发电效率。在本文中,我们提出了亚纳米限制策略,利用带负电荷的环保亲水性细菌纳米纤维素(BNC)在坚固的 MoS2 基膜中创建高离子选择性通道。所开发的膜具有 9.8 Å 的层间间距和理想的负电荷纳米通道,从而产生了有利于增强 Na+ 运输而阻止 Cl- 运输的封闭性。测试膜的面积为 0.78 平方毫米,超过了其他已报道的宏观尺度膜。在环境温度和 343 K 条件下,该电化学装置在 50 倍浓度梯度下的功率密度分别为 73 W m-2 和 233 W m-2,比之前报道的二维纳米流体膜高出 70 倍。此外,该膜还表现出卓越的长期稳定性,可持续 40 天而无性能衰减。目前的研究工作在开发用于收集渗透能的二维纳米流体膜方面取得了突破性进展。
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引用次数: 0
Lithium−sulfur pouch cells with 99% capacity retention for 1000 cycles 锂硫袋电池 1000 次循环后容量保持率达 99
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-17 DOI: 10.1039/d4ee02149e
Huangwei Zhang, Yidan Zhang, Chen Cao, Wanli Zhao, Kai Huang, Yi Zhang, Yue Shen, Zhen Li, Yunhui Huang
Lithium−sulfur (Li−S) battery is a highly promising candidate for the next−generation battery system. However, the shuttle effect of polysulfides or the dendrites and side reactions of lithium metal anodes limit the cycle life of batteries. Especially at the pouch cell level, achieving the long cycle stability is extremely challenging. Here, we have constructed a Li−S pouch cell with sulfurized pyrolyzed poly(acrylonitrile) (SPAN) as the cathode and graphite (Gr) as the anode, introducing lithium−ions through a facile in−situ pre−lithiation method. In carbonate−based electrolytes, the SPAN cathode can avoid the shuttle effect, while the Gr anode can exclude the interference of lithium metal. By rationally controlling the cycling conditions to suppress the loss of active lithium and the increase in resistance, a SPAN||Gr pouch cell with 1000 cycles and 99% capacity retention rate can be ultimately obtained. The Ah−level pouch cell can stably cycle for 1031 times with 82% capacity retention rate and pass multiple safety tests. This design is expected to fundamentally improve the long cycle stability of the Li−S pouch cells and it has great potential in the field of large scale energy storage due to its absence of transition metal elements.
锂硫(Li-S)电池是下一代电池系统中极具潜力的候选电池。然而,多硫化物的穿梭效应或锂金属阳极的枝晶和副反应限制了电池的循环寿命。特别是在袋式电池层面,实现长循环稳定性极具挑战性。在此,我们构建了一种以硫化热解聚丙烯腈(SPAN)为阴极、石墨(Gr)为阳极的锂-S 袋式电池,并通过简便的原位预硫化方法引入了锂离子。在碳酸盐基电解质中,SPAN 阴极可以避免穿梭效应,而 Gr 阳极则可以排除金属锂的干扰。通过合理控制循环条件,抑制活性锂的损失和电阻的增加,最终可获得循环 1000 次、容量保持率达 99% 的 SPAN||Gr 袋式电池。Ah 级袋装电池可稳定循环 1031 次,容量保持率达 82%,并通过了多项安全测试。这种设计有望从根本上提高锂-S 袋式电池的长循环稳定性,而且由于不含过渡金属元素,它在大规模储能领域具有巨大潜力。
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引用次数: 0
H-buffer effects boosting H-spillover for efficient hydrogen evolution reaction 氢缓冲效应促进氢溢出,实现高效氢进化反应
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-17 DOI: 10.1039/d4ee01858c
Yuanyuan Yan, Junyi Du, Chenyang Li, Jin Yang, Yike Xu, Meiling Wang, Yapeng Li, Tian Wang, Xiaosong Li, Xianming Zhang, Huang Zhou, Xun Hong, Yuen Wu, Lixing Kang
The hydrogen (H) spillover effect on metal/support electrocatalysts plays a significant role in facilitating hydrogen evolution reaction (HER). However, the gradual accumulated hydrogen migration barrier during H-spillover processes leads to sluggish H-migration kinetics. Therefore, building an effective hydrogen transport channel to impede the interface H accumulation is highly expected for H-spillover. Herein, we design a multi-shell H-buffer chain by exploiting the oxygen diversity of confined polyoxometalates (POMs) to accelerate H-spillover on Pt in HER. A series of dual-confinement systems (Pt1@POMs@PC) are built by confining single Pt atoms within POMs that are restricted by sub-1-nm pores of porous carbon (PC), and they achieve superior HER activities (η10 = 3.8 ~ 8.3 mV) and long-term durability properties. Experiments and calculations co-reveal a typical H-spillover pathway from Pt to the support via the H-buffer chains (Pt→Obr→O3H→Mo/W→Oc→PCsub-1-nm), which strikingly mitigate the H-migration barriers. We believe the H-buffer chain introduced by this work provides operative guidance for the rational design of metal/support catalysts in various H-spillover-related reactions.
金属/支撑物电催化剂上的氢(H)溢出效应在促进氢进化反应(HER)方面发挥着重要作用。然而,氢溢出过程中逐渐积累的氢迁移障碍导致氢迁移动力学缓慢。因此,建立一个有效的氢迁移通道来阻碍界面上的氢积累是氢溢出所亟需的。在此,我们利用封闭聚氧金属盐(POMs)的氧多样性设计了一种多壳氢缓冲链,以加速 HER 中铂上的氢溢出。通过将单个铂原子限制在受亚 1 纳米多孔碳(PC)孔隙限制的 POMs 中,建立了一系列双限制系统(Pt1@POMs@PC),并获得了优异的 HER 活性(η10 = 3.8 ~ 8.3 mV)和长期耐久性能。实验和计算共同揭示了通过 H 缓冲链(Pt→Obr→O3H→Mo/W→Oc→PCsub-1-nm)从铂到支撑物的典型 H 溢出途径,这显著减轻了 H 迁移障碍。我们相信,这项工作引入的 H 缓冲链为在各种 H 溢出相关反应中合理设计金属/支撑催化剂提供了可操作的指导。
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引用次数: 0
Ultra-low Lattice Thermal-conductivity Realizes Ultra-High Performance Bi0.48Sb1.52Te3-Based Thermoelectric Material and Module 超低晶格热导率实现了基于 Bi0.48Sb1.52Te3 的超高性能热电材料和模块
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-16 DOI: 10.1039/d4ee02008a
Hongtao Li, Lidong Chen, Zhe Guo, Gang Wu, Xiaojian Tan, Qiang Zhang, Jianfeng Cai, Qianqian Sun, Jacques G. Noudem, Jiehua Wu, Peng Sun, Guoqiang Liu, Jun Jiang
The component regulation in Bi2Te3-based materials usually simultaneously decreases the lattice thermal conductivity and carrier mobility, which make it difficult to improve the thermoelectric performance. In this work, we aim to improve the zT of p-type Bi0.48Sb1.52Te3 by adding Sn1/3Ge1/3Pb1/3Te and Cu to introduce differentiated electro-phonon scattering centres to reduce the lattice thermal conductivity while maintaining the carrier mobility as much as possible. The Sn1/3Ge1/3Pb1/3Te alloying produces many point defects and a Te-poor characteristic, thus induces twin and low-angle grain boundaries to effectively strengthen the phonon scattering, and realizes an ultralow lattice thermal conductivity of 0.42 W m−1 K−1 at 300 K. Simultaneously, the Cu doping optimizes the hole concentration, boosting the power factor overall to an average value of 32.1 μW cm−1 K−2 within 300-500 K. These synergistic effects yield a peak zT of 1.45 at 375 K and an average zT of 1.32 (300–500 K) in the Bi0.48Sb1.516Cu0.004Te3 + 0.50 wt% Sn1/3Ge1/3Pb1/3Te sample. The integrated 17-pair thermoelectric module achieves a conversion efficiency of 6.8% at ΔT = 200 K when coupled with n-type zone-melted Bi2Te2.7Se0.3. More importantly, the output performance of the fabricated module has not weakened after 100 cycles in 500 hours aging test.
Bi2Te3 基材料中的组分调节通常会同时降低晶格热导率和载流子迁移率,从而难以改善热电性能。在这项工作中,我们旨在通过添加 Sn1/3Ge1/3Pb1/3Te 和 Cu 来改善 p 型 Bi0.48Sb1.52Te3 的 zT,从而引入差异化的电声散射中心,在尽可能保持载流子迁移率的同时降低晶格热导率。Sn1/3Ge1/3Pb1/3Te 合金产生了许多点缺陷和贫Te特性,从而诱发了孪晶和低角度晶界,有效地加强了声子散射,实现了 300 K 时 0.42 W m-1 K-1 的超低晶格热导率。这些协同效应使 Bi0.48Sb1.516Cu0.004Te3 + 0.50 wt% Sn1/3Ge1/3Pb1/3Te 样品在 375 K 时的 zT 峰值达到 1.45,平均 zT 值为 1.32(300-500 K)。当与 n 型区熔 Bi2Te2.7Se0.3 相耦合时,集成的 17 对热电模块在 ΔT = 200 K 时的转换效率达到 6.8%。更重要的是,在经过 500 小时老化试验的 100 次循环后,所制造模块的输出性能并未减弱。
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引用次数: 0
Ultra-Thin Amphiphilic Hydrogel Electrolyte for Flexible Zinc-ion Paper Batteries 用于柔性锌离子纸电池的超薄两亲水凝胶电解质
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-16 DOI: 10.1039/d4ee01993h
Huan Xia, Wei Zhang, Chunyang Miao, Hao Chen, Chengjie Yi, Yihan Shang, Tao Shui, Xin Cao, Jiacheng Liu, Song-Zhu Kure-Chu, Feifei Liang, Nosipho Moloto, Yipeng Xiong, Takehiko Hihara, Wei Bing Lu, Zhengming Sun
Hydrogel electrolytes are the ideal platform to construct flexible zinc-ion batteries. However, they usually require immersion in salt solutions to the swollen state for high ion transportation, resulting in a decreased energy density and poor interface adhesion. Herein, we developed a hydrophobic-hydrophilic dual phase stabilization strategy to crosslink polymer membranes into hydrogels based on solvent displacement. The hydrophobic and rigid polyacrylonitrile (PAN) network effectively restricts the swelling behavior of the hydrophilic polyvinyl alcohol (PVA) network, forming an interconnected amphiphilic hydrogel (C-PVA/PAN) with a thickness of only 20 μm even after swelling. The Zn||C-PVA/PAN||Zn symmetric cell cycling tests demonstrate stable performance exceeding 3500 hours without zinc dendrite formation. Molecular dynamics (MD) simulations also corroborate the ability of the C-PVA/PAN hydrogel electrolyte to facilitate uniform zinc deposition. Additionally, paper-like Zn||C-PVA/PAN||NH4V4O10 batteries with a thickness of only 82 μm exhibit remarkable cycling performance (180 mAh g⁻¹ after 3000 cycles at 20 A g⁻¹) and can be folded using the Miura folding technique, significantly enhancing areal energy density. This work presents a facile strategy for designing ultra-thin hydrogel electrolytes, paving the way for powering next-generation flexible electronics through paper-like batteries.
水凝胶电解质是构建柔性锌离子电池的理想平台。然而,它们通常需要在盐溶液中浸泡至膨胀状态才能实现高离子传输,从而导致能量密度降低和界面粘附性差。在此,我们开发了一种疏水-亲水双相稳定策略,基于溶剂置换将聚合物膜交联成水凝胶。疏水性刚性聚丙烯腈(PAN)网络有效限制了亲水性聚乙烯醇(PVA)网络的溶胀行为,形成了一种相互连接的两亲水凝胶(C-PVA/PAN),即使在溶胀后厚度也只有 20 μm。Zn||C-PVA/PAN||Zn对称电池循环测试表明,该产品的性能稳定,超过3500小时无锌枝晶形成。分子动力学(MD)模拟也证实了 C-PVA/PAN 水凝胶电解质促进锌均匀沉积的能力。此外,厚度仅为 82 μm 的纸状 Zn||C-PVA/PAN||NH4V4O10电池表现出卓越的循环性能(在 20 A g-¹ 的条件下循环 3000 次后可达到 180 mAh g-¹),并可使用三浦折叠技术进行折叠,从而显著提高能量密度。这项研究提出了一种设计超薄水凝胶电解质的简便策略,为通过纸质电池为下一代柔性电子产品供电铺平了道路。
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引用次数: 0
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Energy & Environmental Science
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