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Co-production of hydrogen, oxygen, and electricity via an integrated solar-driven system with decoupled water electrolyzer and Na-Zn ion battery 通过带有解耦水电解器和纳-锌离子电池的太阳能驱动集成系统联合生产氢气、氧气和电力
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-11 DOI: 10.1016/j.jechem.2024.08.062
Fei Lv, Longjie Liu, Jiazhe Wu, Pengfei Wang, Lixia Pan, Dengwei Jing, Yubin Chen
Combining water electrolysis and rechargeable battery technologies into a single system holds great promise for the co-production of hydrogen (H2) and electricity. However, the design and development of such systems is still in its infancy. Herein, an integrated hydrogen-oxygen (O2)-electricity co-production system featuring a bipolar membrane-assisted decoupled electrolyzer and a Na-Zn ion battery was established with sodium nickelhexacyanoferrate (NaNiHCF) and Zn2+/Zn as dual redox electrodes. The decoupled electrolyzer enables to produce H2 and O2 in different time and space with almost 100% Faradaic efficiency at 100 mA cm−2. Then, the charged NaNiHCF and Zn electrodes after the electrolysis processes formed a Na-Zn ion battery, which can generate electricity with an average cell voltage of 1.75 V at 10 mA cm−2. By connecting Si photovoltaics with the modular electrochemical device, a well-matched solar driven system was built to convert the intermittent solar energy into hydrogen and electric energy with a solar to hydrogen-electricity efficiency of 16.7%, demonstrating the flexible storage and conversion of renewables.
将水电解和可充电电池技术结合到一个系统中,为氢气(H2)和电力的联合生产带来了巨大希望。然而,此类系统的设计和开发仍处于起步阶段。在此,我们建立了一个氢-氧(O2)-电一体化联合生产系统,该系统以双极膜辅助解耦电解槽和镍-锌离子电池为特色,以镍六氰基铁酸钠(NaNiHCF)和 Zn2+/Zn 作为双氧化还原电极。解耦电解器能够在不同的时间和空间产生 H2 和 O2,在 100 mA cm-2 的条件下,法拉第效率几乎达到 100%。然后,NaNiHCF 和 Zn 电极经过电解过程后形成 Na-Zn 离子电池,在 10 mA cm-2 的条件下,电池平均电压为 1.75 V。通过将硅光伏与模块化电化学装置连接,建立了一个匹配良好的太阳能驱动系统,可将间歇性太阳能转化为氢能和电能,太阳能转化为氢能的效率为 16.7%,展示了可再生能源的灵活存储和转化。
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引用次数: 0
Interfacial Zn2+-solvation regulator towards reversible and stable Zn anode 实现可逆和稳定锌阳极的表面 Zn2+-溶解调节器
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-11 DOI: 10.1016/j.jechem.2024.08.061
Miao Zhou , Xiongbin Luo , Hang Li , Shan Guo , Zhuang Tong , Xiaotao Zhou , Xu Li , Zhaohui Hou , Shuquan Liang , Guozhao Fang
Aqueous zinc-ion batteries (AZIBs) are fundamentally challenged by the instability of the electrode/electrolyte interface, predominantly due to irreversible zinc (Zn) deposition and hydrogen evolution. Particularly, the intricate mechanisms behind the electrochemical discrepancies induced by interfacial Zn2+-solvation and deposition behavior demand comprehensive investigation. Organic molecules endowed with special functional groups (such as hydroxyl, carboxyl, etc.) have the potential to significantly optimize the solvation structure of Zn2+ and regulate the interfacial electric double layer (EDL). By increasing nucleation overpotential and decreasing interfacial free energy, these functional groups facilitate a lower critical nucleation radius, thereby forming an asymptotic nucleation model to promote uniform Zn deposition. Herein, this study presents a pioneering approach by introducing trace amounts of n-butanol as solvation regulators to engineer the homogenized Zn (H-Zn) anode with a uniform and dense structure. The interfacial reaction and structure evolution are explored by in/ex-situ experimental techniques, indicating that the H-Zn anode exhibits dendrite-free growth, no by-products, and weak hydrogen evolution, in sharp contrast to the bare Zn. Consequently, the H-Zn anode achieves a remarkable Zn utilization rate of approximately 20% and simultaneously sustains a prolonged cycle life exceeding 500 h. Moreover, the H-Zn//NH4V4O10 (NVO) full battery showcases exceptional cycle stability, retaining 95.04% capacity retention after 400 cycles at a large current density of 5 A g−1. This study enlightens solvation-regulated additives to develop Zn anode with superior utilization efficiency and extended operational lifespan.
锌离子水电池(AZIBs)面临着电极/电解质界面不稳定的根本挑战,这主要是由于不可逆的锌(Zn)沉积和氢演化造成的。尤其需要全面研究界面 Zn2+ 溶解和沉积行为所引起的电化学差异背后的复杂机制。具有特殊官能团(如羟基、羧基等)的有机分子有可能显著优化 Zn2+ 的溶解结构并调节界面电双层(EDL)。通过提高成核过电位和降低界面自由能,这些官能团可降低临界成核半径,从而形成渐近成核模型,促进 Zn 的均匀沉积。本研究开创性地引入微量正丁醇作为溶解调节剂,设计出具有均匀致密结构的匀化锌(H-Zn)阳极。通过原位/离位实验技术对界面反应和结构演化进行了探索,结果表明 H-Zn 阳极呈现出无枝晶生长、无副产物和弱氢演化的特点,与裸锌形成鲜明对比。此外,H-Zn//NH4V4O10(NVO)全电池显示出卓越的循环稳定性,在 5 A g-1 的大电流密度下循环 400 次后仍能保持 95.04% 的容量。这项研究为开发具有更高的利用效率和更长的运行寿命的锌阳极提供了溶解调节添加剂的启示。
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引用次数: 0
Design of a cationic accelerator enabling ultrafast ion diffusion kinetics in aqueous zinc-ion batteries 设计阳离子加速器,实现锌离子水电池中的超快离子扩散动力学
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-11 DOI: 10.1016/j.jechem.2024.09.002
Yawei Xiao , Qianqian Gu , Haoyu Li , Mengyao Li , Yude Wang

Aqueous zinc-ion batteries are highly favored for grid-level energy storage owing to their low cost and high safety, but their practical application is limited by slow ion migration. To address this, a strategy has been developed to create a cation-accelerating electric field on the surface of the cathode to achieve ultrafast Zn2+ diffusion kinetics. By employing electrodeposition to coat MoS2 on the surface of BaV6O16·3H2O nanowires, the directional built-in electric field generated at the heterointerface acts as a cation accelerator, continuously accelerating Zn2+ diffusion into the active material. The optimized Zn2+ diffusion coefficient in CC@BaV6O16·3H2O@MoS2 (7.5 × 10−8 cm2 s−1) surpasses that of most reported V-based cathodes. Simultaneously, MoS2 serving as a cathodic armor extends the cycling life of the Zn-CC@BaV6O16·3H2O@MoS2 full batteries to over 10000 cycles. This work provides valuable insights into optimizing ion diffusion kinetics for high-performance energy storage devices.

锌离子水电池因其低成本和高安全性而备受电网级储能技术的青睐,但其实际应用却因离子迁移缓慢而受到限制。为了解决这个问题,我们开发了一种策略,在阴极表面形成阳离子加速电场,以实现超快的 Zn2+ 扩散动力学。通过电沉积将 MoS2 涂覆在 BaV6O16-3H2O 纳米线表面,在异质表面产生的定向内置电场就像阳离子加速器一样,不断加速 Zn2+ 向活性材料的扩散。CC@BaV6O16-3H2O@MoS2 中优化的 Zn2+ 扩散系数(7.5 × 10-8 cm2 s-1)超过了大多数已报道的 V 基阴极。同时,作为阴极铠甲的 MoS2 将 Zn-CC@BaV6O16-3H2O@MoS2 全电池的循环寿命延长至 10000 次以上。这项研究为优化高性能储能设备的离子扩散动力学提供了宝贵的见解。
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引用次数: 0
Micro-strain regulation strategy to stabilize perovskite lattice based on the categories and impact of strain on perovskite solar cells 基于应变类别及其对包晶石太阳能电池影响的稳定包晶石晶格的微应变调节策略
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-11 DOI: 10.1016/j.jechem.2024.08.063
Caixia Li, Wenwu Liu, Shiji Da, Lingbin Kong, Fen Ran
Photovoltaic metal halide perovskite solar cells (PSCs) convert light to electricity more efficiently than crystalline silicon cells, and the cost of materials used to make them is lower than that of silicon cells. Conversion efficiency is not a core issue affecting the application of perovskite solar cells in special scenarios. At present, stability is the major technical encounters that hinders its further commercial development. Micro-strain in PSCs is currently a significant factor responsible for the device’s instability. Strain-induced ion migration is widely believed to accelerate perovskite degradation even when external stimuli are excluded. Undoubtedly, it is imperative to study strain to enhance the stability of PSCs. This paper reviews recent developments to understand strain’s origin and effect mechanisms on performance of PSCs, including ion migration, failure behavior, defect formation, and its effect on photoelectric properties, stability, and reliability. Additionally, several well-known strain management strategies are systematically introduced based on the strain effect mechanism and strain engineering on the film, providing more clues for further preparation with increased stability. The manipulation of external physical strain applied from films to entire devices has been extensively studied. Furthermore, recommendations for future research directions and chemical approaches have been provided. It is emphasized that strain engineering plays a crucial role in improving the efficiency and longevity of PSCs. Tensile strain causes rapid degradation, while moderate compressive strain and external strain control could improve properties and stability. Efforts should focus on controlling compressive strain to mitigate residual tensile strain and introducing it in a controlled manner. Future research endeavors may focus on exploring these pathways to improve the efficiency and lifespan of PSCs.
与晶体硅电池相比,光伏金属卤化物包晶体太阳能电池(PSCs)能更有效地将光转换为电能,而且其材料成本也低于硅电池。转换效率并不是影响包晶体太阳能电池在特殊情况下应用的核心问题。目前,稳定性是阻碍其进一步商业化发展的主要技术问题。目前,PSCs 中的微应变是导致设备不稳定的重要因素。人们普遍认为,即使在排除外部刺激的情况下,应变引起的离子迁移也会加速包晶体的降解。毫无疑问,研究应变以提高 PSCs 的稳定性势在必行。本文回顾了了解应变的起源及其对 PSC 性能影响机制的最新进展,包括离子迁移、失效行为、缺陷形成及其对光电特性、稳定性和可靠性的影响。此外,根据薄膜的应变效应机制和应变工程学,系统地介绍了几种著名的应变管理策略,为进一步制备稳定性更高的薄膜提供了更多线索。此外,还广泛研究了从薄膜到整个器件的外部物理应变操作。此外,还对未来的研究方向和化学方法提出了建议。研究强调,应变工程在提高 PSC 的效率和寿命方面起着至关重要的作用。拉伸应变会导致快速降解,而适度的压缩应变和外部应变控制则可以改善性能和稳定性。应集中精力控制压缩应变,以减轻残余拉伸应变,并以可控的方式引入压缩应变。未来的研究工作可能会侧重于探索这些途径,以提高 PSC 的效率和寿命。
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引用次数: 0
Conversion-type cathode materials for high energy density solid-state lithium batteries 用于高能量密度固态锂电池的转换型正极材料
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-11 DOI: 10.1016/j.jechem.2024.09.001
Yuhao Ma , Shihong Qing , Hongyu Liu , Chuntao Ma , Yuan Yu , Chuang Yu , Liping Wang

Solid-state lithium batteries (SSLBs) are regarded as an essential growth path in energy storage systems due to their excellent safety and high energy density. In particular, SSLBs using conversion-type cathode materials have received widespread attention because of their high theoretical energy densities, low cost, and sustainability. Despite the great progress in research and development of SSLBs based on conversion-type cathodes, their practical applications still face challenges such as blocked ionic-electronic migration pathways, huge volume change, interfacial incompatibility, and expensive processing costs. This review focuses on the advantages and critical issues of coupling conversion-type cathodes with solid-state electrolytes (SSEs), as well as state-of-the-art progress in various promising cathodes (e.g., FeS2, CuS, FeF3, FeF2, and S) in SSLBs. Furthermore, representative research on conversion-type solid-state full cells is discussed to offer enlightenment for their practical application. Significantly, the energy density exhibited by the S cathode stands out impressively, while sulfide SSEs and halide SSEs have demonstrated immense potential for coupling with conversion-type cathodes. Finally, perspectives on conversion-type cathodes are provided at the material, interface, composite electrode, and battery levels, with a view to accelerating the development of conversion-type cathodes for high-energy–density SSLBs.

固态锂电池(SSLB)因其出色的安全性和高能量密度,被视为能源存储系统的重要发展方向。其中,使用转换型正极材料的固态锂电池因其理论能量密度高、成本低和可持续性强而受到广泛关注。尽管基于转换型阴极的 SSLB 的研究和开发取得了巨大进展,但其实际应用仍面临着离子电子迁移途径受阻、体积变化巨大、界面不兼容和加工成本昂贵等挑战。本综述重点介绍了转换型阴极与固态电解质(SSE)耦合的优势和关键问题,以及 SSLB 中各种有前途的阴极(如 FeS2、CuS、FeF3、FeF2 和 S)的最新进展。此外,还讨论了转换型固态全电池的代表性研究,为其实际应用提供启示。值得注意的是,S 阴极表现出的能量密度令人印象深刻,而硫化物 SSE 和卤化物 SSE 则在与转换型阴极耦合方面展现出巨大的潜力。最后,从材料、界面、复合电极和电池等层面对转换型阴极进行了展望,以期加快高能量密度 SSLB 转换型阴极的开发。
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引用次数: 0
Rational modulation of fluorophosphate cathode by anionic groups to reduce the polarization behavior for fast-charging sodium-ion batteries 用阴离子基团合理调节氟磷酸盐阴极以减少钠离子电池快速充电时的极化行为
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-11 DOI: 10.1016/j.jechem.2024.08.064
Xinyuan Wang, Fan Zhang, Xingyu Zhou, Qian Wang, Changyu Liu, Yangyang Liu, Hui Wang, Xiaojie Liu
Na3V2(PO4)2O2F (VP) is recognized as a promising cathode material for sodium-ion batteries due to its stable structural framework and high specific capacity. Density functional theory (DFT) and finite element simulations show that incorporating SO42− into VP decreases its band gap, lowers the migration energy barrier, and ensures a uniform Na+ concentration gradient and stress distribution during charge and discharge cycles. Consequently, the average Na+ diffusion coefficient of Na3V2(PO4)1.95(SO4)0.05O2F (VPS-1) is roughly double that of VP, leading to enhanced rate capability (80 C, 75.5 mAh g−1) and cycling stability (111.0 mAh g−1 capacity after 1000 cycles at 10 C current density) for VPS-1. VPS-1 exhibits outstanding fast-charging capabilities, achieving an 80% state of charge in just 8.1 min. The assembled VPS-1//SbSn/NPC full cell demonstrated stable cycling over 200 cycles at a high 5 C current, maintaining an average coulombic efficiency of 95.35%.
Na3V2(PO4)2O2F(VP)因其稳定的结构框架和高比容量而被认为是一种很有前途的钠离子电池阴极材料。密度泛函理论(DFT)和有限元模拟表明,在 VP 中加入 SO42- 会减小其带隙,降低迁移能垒,并确保充放电循环过程中 Na+ 浓度梯度和应力分布均匀。因此,Na3V2(PO4)1.95(SO4)0.05O2F(VPS-1)的平均 Na+ 扩散系数大约是 VP 的两倍,从而提高了 VPS-1 的速率能力(80 C、75.5 mAh g-1)和循环稳定性(10 C 电流密度下 1000 次循环后容量为 111.0 mAh g-1)。VPS-1 具有出色的快速充电能力,仅需 8.1 分钟即可达到 80% 的充电状态。组装后的 VPS-1//SbSn/NPC 全电池在 5 C 大电流下稳定循环 200 次,平均库仑效率保持在 95.35%。
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引用次数: 0
Ru doping triggering reconstruction of cobalt phosphide for coupling glycerol electrooxidation with seawater electrolysis 掺杂 Ru 触发磷化钴重构,实现甘油电氧化与海水电解耦合
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-07 DOI: 10.1016/j.jechem.2024.08.056
Binglu Deng , Jie Shen , Jinxing Lu , Chuqiang Huang , Zhuoyuan Chen , Feng Peng , Yunpeng Liu

Seawater electrolysis is a promising approach for sustainable energy without relying on precious freshwater. However, the large-scale seawater electrolysis is hindered by low catalytic efficiency and severe anode corrosion caused by the harmful chlorine. In contrast to the oxygen evolution reaction (OER) and chlorin ion oxidation reaction (ClOR), glycerol oxidation reaction (GOR) is more thermodynamically and kinetically favorable alternative. Herein, a Ru doping cobalt phosphide (Ru-CoP2) is proposed as a robust bifunctional electrocatalyst for seawater electrolysis and GOR, for the concurrent productions of hydrogen and value-added formate. The in situ and ex situ characterization analyses demonstrated that Ru doping featured in the dynamic reconstruction process from Ru-CoP2 to Ru-CoOOH, accounting for the superior GOR performance. Further coupling GOR with hydrogen evolution was realized by employing Ru-CoP2 as both anode and cathode, requiring only a low voltage of 1.43 V at 100 mA cm−2, which was 250 mV lower than that in alkaline seawater. This work guides the design of bifunctional electrocatalysts for energy-efficient seawater electrolysis coupled with biomass resource upcycling.

海水电解是一种无需依赖珍贵淡水即可实现可持续能源的可行方法。然而,催化效率低和有害氯造成的阳极严重腐蚀阻碍了大规模海水电解。与氧进化反应(OER)和氯离子氧化反应(ClOR)相比,甘油氧化反应(GOR)是热力学和动力学上更为有利的替代反应。在此,我们提出了一种掺杂 Ru 的磷化钴(Ru-CoP2),作为海水电解和甘油氧化反应的强效双功能电催化剂,可同时产生氢气和增值的甲酸盐。原位和非原位表征分析表明,在 Ru-CoP2 到 Ru-CoOOH 的动态重构过程中掺入了 Ru,这也是 GOR 性能优越的原因。通过将 Ru-CoP2 同时用作阳极和阴极,进一步实现了 GOR 与氢进化的耦合,在 100 mA cm-2 的条件下仅需 1.43 V 的低电压,比碱性海水中的电压低 250 mV。这项工作为设计双功能电催化剂提供了指导,可用于高效节能的海水电解以及生物质资源的循环利用。
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引用次数: 0
A self-adaptive inorganic in-situ separator by particle crosslinking for nonflammable lithium-ion batteries 用于不可燃锂离子电池的颗粒交联自适应无机原位隔膜
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-07 DOI: 10.1016/j.jechem.2024.08.054
Jiarui Yang , Jiuzhou Liu , Wenrui Cai, Ziyu Zhao, Shan Wang, Lu He, Shanshan Lv, Zhiwei Zhu, Zhongfeng Ji, Guojiang Wen, Hua Li, Yuanming Zhai, Xuewei Fu, Wei Yang, Yu Wang
All-safe liquid-state lithium-ion batteries (ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional liquid-state LIBs. However, the practical success of ASLS-LIBs is bottlenecked by the lack of advanced separator technology that can simultaneously realize high performances in puncturing-tolerability, fire-resistance, and importantly, wetting-capability with non-flammable liquid-electrolytes. Here, we propose a concept of inorganic in-situ separator (IISS) by hybrid-sol physical crosslinking directly onto the electrode surface to address the above challenges. Particularly, the hybrid-sol is designed with silica nanoparticles as the building block and poly(vinylidene difluoride) nanoparticles as the crosslinking agent. The critical factors for controlling the IISS microstructures and properties have been systematically investigated. The advantages of the IISS have been confirmed by its fast wetting with various fire-resistant liquid-electrolytes, customizable thickness and porous structures, robust interface with planar or three-dimensional (3D)-structured electrodes, and importantly, unexpected self-adaptability against puncturing. Enabled by the above merits, a fire-resistant ASLS-LIB is successfully assembled and demonstrated with stable electrochemical performance. This sol-crosslinked IISS may open an avenue for the studies on the next-generation separator technology, cell assembling, solid electrolyte processing as well as non-flammable secondary batteries.
全安全液态锂离子电池(ASLS-LIBs)可将全固态电池的安全性与传统液态锂离子电池的高性能和低制造成本结合起来,因此备受关注。然而,由于缺乏先进的隔膜技术,ASLS-LIB 无法同时实现耐穿刺性、耐火性以及重要的非易燃液态电解质润湿性等方面的高性能,从而制约了其实际应用的成功。在此,我们提出了一种无机原位分离器(IISS)的概念,通过将混合溶胶直接物理交联到电极表面来解决上述难题。其中,混合溶胶的设计以二氧化硅纳米颗粒为构件,聚偏二氟乙烯纳米颗粒为交联剂。系统地研究了控制 IISS 微结构和性能的关键因素。IISS 的优势已得到证实,它能快速润湿各种耐火液态电解质,可定制厚度和多孔结构,能与平面或三维(3D)结构电极牢固对接,更重要的是,它具有意想不到的抗穿刺自适应能力。在上述优点的支持下,一种耐火 ASLS-LIB 被成功组装,并展示了其稳定的电化学性能。这种溶胶交联 IISS 可为下一代隔膜技术、电池组装、固体电解质加工以及不易燃二次电池的研究开辟一条途径。
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引用次数: 0
High-temperature-tolerant flexible supercapacitors: Gel polymer electrolytes and electrode materials 耐高温柔性超级电容器:凝胶聚合物电解质和电极材料
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-07 DOI: 10.1016/j.jechem.2024.08.051
Chong Peng , Xinyi Huang , Mingwei Zhao , Shuling Liao , Quanhong Yang , Nianjun Yang , Siyu Yu

The development of flexible supercapacitors (FSCs) capable of operating at high temperatures is crucial for expanding the application areas and operating conditions of supercapacitors. Gel polymer electrolytes and electrode materials stand as two key components that significantly impact the efficacy of high-temperature-tolerant FSCs (HT-FSCs). They should not only exhibit high electrochemical performance and excellent flexibility, but also withstand intense thermal stress. Considerable efforts have been devoted to enhancing their thermal stability while maintaining high electrochemical and mechanical performance. In this review, the fundamentals of HT-FSCs are outlined. A comprehensive overview of state-of-the-art progress and achievements in HT-FSCs, with a focus on thermally stable gel polymer electrolytes and electrode materials is provided. Finally, challenges and future perspectives regarding HT-FSCs are discussed, alongside strategies for elevating operational temperatures and performance. This review offers both theoretical foundations and practical guidelines for designing and manufacturing HT-FSCs, further promoting their widespread adoption across diverse fields.

开发能够在高温下工作的柔性超级电容器(FSC)对于扩大超级电容器的应用领域和工作条件至关重要。凝胶聚合物电解质和电极材料是对耐高温柔性超级电容器(HT-FSCs)的功效产生重大影响的两个关键部件。它们不仅要表现出高电化学性能和出色的柔韧性,还要能承受强烈的热应力。在保持高电化学和机械性能的同时,人们一直致力于提高它们的热稳定性。本综述概述了 HT-FSC 的基本原理。全面概述了 HT-FSCs 的最新进展和成就,重点介绍了热稳定凝胶聚合物电解质和电极材料。最后,讨论了 HT-FSCs 面临的挑战和未来展望,以及提高工作温度和性能的策略。本综述为设计和制造高温固态电容器提供了理论基础和实践指南,进一步推动了其在各个领域的广泛应用。
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引用次数: 0
Electrochemical conversion of methane to bridge the gap in the artificial carbon cycle 电化学转化甲烷,弥补人工碳循环的缺口
IF 13.1 1区 化学 Q1 Energy Pub Date : 2024-09-07 DOI: 10.1016/j.jechem.2024.08.050
Yuhao Peng , Yuefeng Song , Ihar Razanau , Juanxiu Xiao , Wei Xiao , Di Hu , Guoxiong Wang

Methane, an abundant one-carbon (C1) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy- and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO2 emissions and coke deposition. Electrochemical conversion of methane (ECM) using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4 conversion rates, and minimization of CO2 emission.

甲烷是一种丰富的一碳(C1)资源,被广泛用于重要燃料和增值化学品的工业生产。然而,目前的工业甲烷转化技术是能源和碳密集型的,主要原因是打破惰性 C-H 键所需的活化能高、选择性低以及副反应问题多,包括二氧化碳排放和焦炭沉积。利用间歇性可再生能源进行甲烷电化学转化(ECM)提供了一种极具吸引力的解决方案,因为它采用模块化反应器设计,可在广泛的温度和压力范围内灵活操作。本综述强调了甲烷在各种反应系统中的转化途径,突出了 ECM 在促进可持续人工碳循环方面的意义和优势。这项研究全面概述了传统的甲烷活化机制,并勾勒出甲烷在电解环境中的完整转化途径。基于表面/界面化学,本研究系统地分析了拟议的反应途径和相应的策略,以提高电解甲烷转化为各种目标产品(包括合成气、碳氢化合物、含氧化合物和先进碳材料)的效率。讨论还涵盖了 ECM 过程的机遇和挑战,包括对 ECM 途径的见解、合理的电催化剂设计、基准协议的建立、电解质工程、CH4 转化率的提高以及二氧化碳排放的最小化。
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引用次数: 0
期刊
Journal of Energy Chemistry
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