eScience最新文献_第10页

Cation-inspired polyhedral distortion boosting moisture/electrolyte stability of iron sulfate cathode for durable high-temperature sodium-ion storage 阳离子激发多面体畸变提高硫酸铁阴极的水分/电解质稳定性，用于持久高温钠离子储存

IF 42.9 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-03-01 Epub Date: 2024-09-25 DOI: 10.1016/j.esci.2024.100313

Longfei Wen , Jiyu Zhang , Jian Zhang , Lingfei Zhao , Xin Wang , Sen Wang , Siyu Ma , Wenbin Li , Jun Luo , Junmin Ge , Weihua Chen

Alluaudite-type iron-based sulfates are prospective positive-electrode active materials for sodium-ion batteries given their low-cost and high operation voltage, yet suffer from poor intrinsic ionic conductivity and (electro) chemical instability at high temperatures. Herein, a cation-modified Na_2.466Fe_1.724Mg_0.043(SO₄)₃ with micron-sized spherical structure was reported. The substitutive MgO₆ octahedron featured stronger covalent bonding interactions and enriched the ion transfer pathways within the crystals, facilitating the ionic kinetics in bulk. Using in situ mass spectrometry and quartz crystal microbalance techniques, Mg cations were demonstrated to lower the electron density around O atoms and surficial nucleophilicity of materials, which effectively suppressed their side reactions with H₂O in air and active ester molecule in electrolyte. This interaction enables an inorganic-rich and uniform interphase to stabilize the cathode/electrolyte interface at high voltage (4.5 V vs. Na⁺/Na). The as-prepared cathode exhibits a high discharge capacity of 102.2 mAh g⁻¹ (voltage platform at 3.74 V), remarkable reaction reversibility (average Coulomb efficiency of 99.3 % over 300 cycles) at high loading (9.0−9.6 mg cm⁻²) and temperature (60 °C), as well as long-lasting cyclability (70.8 %, 5000 cycles). Its application was verified in assembled sodium-ion full cells with a hard carbon negative electrode, showing a long cycling lifetime over 190 cycles.

冲积型铁基硫酸盐具有低成本和高工作电压的优点，是钠离子电池极具前景的正极活性材料，但其固有离子电导率差，且在高温下存在（电）化学不稳定性。本文报道了一种具有微米级球形结构的阳离子改性Na2.466Fe1.724Mg0.043(SO4)3。取代的MgO6八面体具有更强的共价键相互作用，丰富了晶体内的离子转移途径，有利于整体离子动力学。利用原位质谱法和石英晶体微天平技术，证明了Mg阳离子可以降低材料O原子周围的电子密度和表面亲核性，从而有效抑制材料与空气中的H2O和电解质中的活性酯分子的副反应。这种相互作用使富无机和均匀的界面相能够在高压下稳定阴极/电解质界面（4.5 V vs. Na+/Na）。制备的阴极在高负载（9.0 ~ 9.6 mg cm−2）和温度（60°C）下具有102.2 mAh g−1的高放电容量（电压平台为3.74 V），显著的反应可逆性（平均库仑效率为99.3%，超过300次循环），以及持久的可循环性（70.8%，5000次循环）。在硬碳负极组装钠离子电池中验证了其应用，显示出超过190次的长循环寿命。

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引用次数: 0

Delithiation-accelerating and self-healing strategies realizes high-capacity and high-rate black phosphorus anode in wide temperature range 加速衰减和自愈策略实现了宽温度范围内高容量、高速率黑磷阳极

IF 42.9 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-03-01 Epub Date: 2024-10-18 DOI: 10.1016/j.esci.2024.100328

Shaojie Zhang , Yanhua Wan , Yu Cao , Yiming Zhang , Haochen Gong , Xu Liang , Baoshan Zhang , Xiaoyi Wang , Siyu Fang , Jiahong Wang , Wei Li , Jie Sun

Black phosphorus (BP) anode with high capacity (2596 mAh g⁻¹) and suitable lithiation potential (0.7 V vs. Li⁺/Li) is an ideal candidate for high-energy-density and high-safety lithium-ion batteries, however, the practical implementation is greatly limited by its slow reaction kinetics and huge volume expansion. Here, inspired by nature, liquid metal (LM) is explored as a self-heal agent, which can well stabilize the BP anode through buffering the volumetric expansion and re-activating “dead P and Li_xP”. Moreover, LM also acts as a good catalyst, which can adjust Li ion concentration and reduce the activation energy of delithiation reaction, thus prolonging the cycling life. Therefore, the LM modified BP/graphite (G) composite delivers an excellent high-rate performance of 1123 mAh g⁻¹ at 4 C with 80.0 % capacity retention after 200 cycles, a superior wide-temperature performance of 1547.5 mAh g⁻¹ and 569.0 mAh g⁻¹ at 50 °C and −20 °C, respectively.

黑磷（BP）阳极具有高容量（2596 mAh g−1）和适宜的锂化电位（0.7 V vs. Li+/Li），是高能量密度和高安全性锂离子电池的理想阳极，但其反应动力学缓慢和体积膨胀大，极大地限制了其实际应用。在这里，受大自然的启发，探索液态金属（LM）作为一种自愈剂，通过缓冲体积膨胀和重新激活“死P和LixP”，可以很好地稳定BP阳极。同时，LM也是一种很好的催化剂，可以调节Li离子浓度，降低降解反应的活化能，从而延长循环寿命。因此，LM改性的BP/石墨(G)复合材料在4℃下具有1123 mAh G - 1的优异性能，200次循环后容量保持率为80.0%，在50℃和- 20℃下分别具有1547.5 mAh G - 1和569.0 mAh G - 1的优异宽温性能。

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引用次数: 0

Accelerated commercial battery electrode-level degradation diagnosis via only 11-point charging segments 仅通过11点充电段加速商用电池电极级退化诊断

IF 42.9 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-01-01 Epub Date: 2024-10-05 DOI: 10.1016/j.esci.2024.100325

Yu Tian , Cheng Lin , Xiangfeng Meng , Xiao Yu , Hailong Li , Rui Xiong

Accelerated and accurate degradation diagnosis is imperative for the management and reutilization of commercial lithium-ion batteries in the upcoming TWh era. Different from traditional methods, this work proposes a hybrid framework for rapid and accurate degradation diagnosis at the electrode level combining both deep learning, which is used to rapidly and robustly predict polarization-free incremental capacity analysis (ICA) curves in minutes, and physical modeling, which is used to quantitatively reveal the electrode-level degradation modes by decoupling them from the ICA curves. Only measured charging current and voltage signals are used. Results demonstrates that 11 points collected at any starting state-of-charge (SOC) in a minimum of 2.5 minutes are sufficient to obtain reliable ICA curves with a mean root mean square error (RMSE) of 0.2774 Ah/V. Accordingly, battery status can be accurately elevated based on their degradation at both macro and electrode levels. Through transfer learning, such a method can also be adapted to different battery chemistries, indicating the enticing potential for wide applications.

在即将到来的太瓦时时代，加速和准确的降解诊断对于商用锂离子电池的管理和再利用至关重要。与传统方法不同，本工作提出了一个混合框架，用于在电极水平上快速准确地进行降解诊断，结合深度学习和物理建模，深度学习用于在几分钟内快速和稳健地预测无极化增量容量分析（ICA）曲线，物理建模用于通过将它们与ICA曲线解耦来定量揭示电极水平的降解模式。仅使用测量的充电电流和电压信号。结果表明，在任何启动荷电状态（SOC）下在至少2.5分钟内收集的11个点足以获得可靠的ICA曲线，平均均方根误差（RMSE）为0.2774 Ah/V。因此，可以根据电池在宏观和电极水平上的退化准确地提高电池状态。通过迁移学习，这种方法也可以适应不同的电池化学性质，表明了广泛应用的诱人潜力。

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引用次数: 0

Atomic Ni-catalyzed cathode and stabilized Li metal anode for high-performance Li–O2 batteries 高性能锂氧电池的原子镍催化阴极和稳定锂金属阳极

IF 42.9 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-01-01 Epub Date: 2024-09-12 DOI: 10.1016/j.esci.2024.100310

Tiansheng Bai , Jiaxian Wang , Hongqiang Zhang , Fengjun Ji , Wei Song , Shenyi Xiao , Dandan Gao , Jingyu Lu , Lijie Ci , Deping Li

The Li–O₂ battery (LOB) has attracted growing interest, including for its great potential in next-generation energy storage systems due to its extremely high theoretical specific capacity. However, a series of challenges have seriously hindered LOB development, such as sluggish kinetics during the oxygen reduction and oxygen evolution reactions (ORR/OER) at the cathode, the formation of lithium dendrites, and undesirable corrosion at the lithium metal anode. Herein, we propose a strategy based on the ultra-low loading of atomic Ni catalysts to simultaneously boost the ORR/OER at the cathode while stabilizing the Li metal anode. The resultant LOB delivers a superior discharge capacity (> 16,000 mAh g⁻¹), excellent long-term cycling stability (> 200 cycles), and enhanced high rate capability (> 300 cycles @ 500 mA g⁻¹). The working mechanisms of these atomic Ni catalysts are revealed through carefully designed in situ experiments and theoretical calculations. This work provides a novel research paradigm for designing high-performance LOBs that are useable in practical applications.

由于其极高的理论比容量，锂氧电池（LOB）在下一代储能系统中具有巨大的潜力，因此引起了人们越来越多的兴趣。然而，一系列挑战严重阻碍了LOB的发展，例如阴极氧还原和析氧反应（ORR/OER）动力学缓慢，锂枝晶的形成以及锂金属阳极的不良腐蚀。在此，我们提出了一种基于超低负载镍原子催化剂的策略，以同时提高阴极的ORR/OER，同时稳定锂金属阳极。由此产生的LOB提供了卓越的放电能力(>；16,000 mA h g−1)，优异的长期循环稳定性(>；200个周期)，以及增强的高速率能力(>；300个周期@ 500 mA g−1)。通过精心设计的原位实验和理论计算，揭示了这些Ni原子催化剂的工作机理。这项工作为设计可用于实际应用的高性能lob提供了一种新的研究范式。

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引用次数: 0

Understanding multi-scale ion-transport in solid-state lithium batteries 了解固态锂电池中的多尺度离子传输

IF 42.9 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-01-01 Epub Date: 2024-05-11 DOI: 10.1016/j.esci.2024.100278

Wen Yu , Nanping Deng , Yang Feng , Xiaofan Feng , Hengying Xiang , Lu Gao , Bowen Cheng , Weimin Kang , Kai Zhang

Solid-state lithium battery (SSLB) is considered as one of the promising candidates for next-generation power batteries due to high safety, unprecedented energy density and favorable adaptability to high pression and temperature. However, the system of solid electrolyte (SE), as one of the most important components in SSLB, is usually plagued by clumsy ionic transport, leading to poor rate performance of the SSLBs. Herein, a unique perspective is proposed to re-examine the ion-transport behavior in lithium conductors by tracing Li⁺ at multi-scale, including microscopic, mesoscopic and macroscopic scales. The multi-scale ion-transport mechanisms and corresponding characterization techniques are analyzed in depth. Furthermore, some strategies of structure design to improve ion-transport kinetics at corresponding scales are elaborated systematically, involving the modulation of microscopic homogeneous structure, mesoscopic heterogeneous structure and macroscopic structures, etc. The proposed generalized rules for SEs are expected to construct a close link from mechanism−structure−characterization to high performances for SSLBs.

固态锂电池（SSLB）具有极高的安全性、前所未有的能量密度以及对高压和高温的良好适应性，被认为是下一代动力电池的理想选择之一。然而，作为SSLB中最重要的组成部分之一的固体电解质（SE）体系，由于其离子输运笨拙，导致SSLB的倍率性能较差。本文提出了一个独特的视角，通过在多尺度（包括微观、介观和宏观尺度）上追踪Li+来重新研究锂导体中的离子输运行为。深入分析了多尺度离子输运机制及其表征技术。此外，系统阐述了相应尺度下改善离子输运动力学的结构设计策略，包括微观均相结构、介观非均相结构和宏观结构的调节等。所提出的广义规则有望建立从机制-结构-表征到sslb高性能的密切联系。

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引用次数: 0

Heterogeneous structure design for stable Li/Na metal batteries: Progress and prospects 稳定锂/钽金属电池的异质结构设计：进展与前景

IF 42.9 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-01-01 Epub Date: 2024-05-23 DOI: 10.1016/j.esci.2024.100281

Hongyang Chen , Junxiong Wu , Manxian Li , Jingyue Zhao , Zulin Li , Manxi Wang , Xuan Li , Chuanping Li , Xiaochuan Chen , Xiaoyan Li , Yiu-Wing Mai , Yuming Chen

The growth of dendrites in Li/Na metal batteries is a multifaceted process that is controlled by several factors such as electric field, ion transportation, temperature, and pressure. Rational design of battery components has become a viable approach to address this challenge. Among the various design strategies, heterogeneous structures have been demonstrated to be effective in mitigating uneven metal deposition by reducing the local current density and regulating the deposition sites. In this review, we discuss comprehensively the underlying principles and factors that influence dendrite growth, as well as the synthesis approaches for heterogeneous structures. Furthermore, we provide an overview of the diverse applications of heterogeneous structures in battery components. Finally, we highlight existing challenges and future directions for the use of heterogeneous structures in regulating metal deposition.

锂/钠金属电池中枝晶的生长是一个多方面的过程，受电场、离子输运、温度和压力等多种因素的控制。合理设计电池组件已成为解决这一挑战的可行方法。在各种设计策略中，非均质结构已被证明可以通过降低局部电流密度和调节沉积位置来有效减轻金属沉积的不均匀性。本文综述了影响枝晶生长的基本原理和因素，以及非均相结构的合成方法。此外，我们还概述了异质结构在电池组件中的各种应用。最后，我们强调了在调节金属沉积中使用非均质结构存在的挑战和未来的方向。

引用次数: 0

Energetic disorder dominates optical properties and recombination dynamics in tin-lead perovskite nanocrystals 能量无序主导锡铅过氧化物纳米晶体的光学特性和重组动力学

IF 42.9 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-01-01 Epub Date: 2024-05-11 DOI: 10.1016/j.esci.2024.100279

Dandan Wang , Yusheng Li , Yongge Yang , Chao Ding , Yuyao Wei , Dong Liu , Hua Li , Huan Bi , Shikai Chen , Sujun Ji , Boyu Zhang , Yao Guo , Huiyun Wei , Hongshi Li , Shuzi Hayase , Qing Shen

Tin-lead alloyed perovskite nanocrystals (PNCs) offer a promising pathway toward low-toxicity and air-stable light-emitting devices. However, substantial energetic disorder has thus far hindered their lighting applications compared to pure lead-based PNCs. A fundamental understanding of this disorder and its impact on optical properties is crucial for overcoming this limitation. Here, using temperature-dependent static and transient absorption spectroscopy, we meticulously distinguish the contributions of static disorder (including defects, impurities, etc.) and dynamic disorder (carrier–phonon interactions). We reveal how these disorders shape band-tail structure and ultimately influence inter-band carrier recombination behaviors. Surprisingly, we find that static and dynamic disorder primarily control band-tail defect states and bandgap renormalization, respectively, which together modulate fast carrier trapping and slow band-band recombination rates. Furthermore, we link these disorders to the tin-induced symmetry-lowering distortions in tin-lead alloyed PNCs. These findings illuminate critical design principles for highly luminescent, low-toxicity tin-lead PNCs, accelerating their adoption in optoelectronic applications.

锡铅合金钙钛矿纳米晶体（PNCs）为低毒性和空气稳定的发光器件提供了一条有前途的途径。然而，与纯铅基pnc相比，大量的能量紊乱迄今为止阻碍了它们的照明应用。对这种无序及其对光学性质的影响的基本理解对于克服这一限制至关重要。在这里，使用温度相关的静态和瞬态吸收光谱，我们仔细区分了静态无序（包括缺陷，杂质等）和动态无序（载流子-声子相互作用）的贡献。我们揭示了这些紊乱如何形成带尾结构并最终影响带间载流子重组行为。令人惊讶的是，我们发现静态无序和动态无序分别主要控制带尾缺陷状态和带隙重整化，它们共同调节快速载波捕获和缓慢的带复合速率。此外，我们将这些失调与锡铅合金pnc中锡引起的对称性降低畸变联系起来。这些发现阐明了高发光、低毒性锡铅pnc的关键设计原则，加速了它们在光电应用中的采用。

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引用次数: 0

Tailoring the electron redistribution of RuO2 by constructing a Ru-O-La asymmetric configuration for efficient acidic oxygen evolution 通过构建Ru-O-La不对称结构来调整RuO2的电子再分配，以实现高效的酸性氧演化

IF 42.9 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-01-01 Epub Date: 2024-08-28 DOI: 10.1016/j.esci.2024.100307

Cong-Hui Li , Cheng-Zong Yuan , Xiaolei Huang , Hongrui Zhao , Fuling Wu , Lei Xin , Xiaomeng Zhang , Shufeng Ye , Yunfa Chen

Stabilizing the highly active RuO₂ electrocatalyst for the oxygen evolution reaction (OER) is critical for the application of proton exchange membrane water electrolysis, but this remains challenging due to the inevitable over-oxidation of Ru in harsh oxidative environments. Herein, we describe constructing Ru-O-La asymmetric configurations into RuO₂ via a facile sol-gel method to tailor electron redistribution and thereby eliminate the over-oxidation of Ru centers. Specifically, the as-prepared optimal La_0.1Ru_0.9O₂ shows a low overpotential of 188 mV at 10 mA cm⁻², a high mass activity of 251 A

{g_{Ru}}^{- 1}

at 1.6 V vs. reversible hydrogen electrode (RHE), and a long-lasting durability of 63 h, far superior to the 8 h achieved by standard RuO₂. Experiments and density functional theory calculations jointly reveal that the Ru-O-La asymmetric configuration could trigger electron redistribution in RuO₂. More importantly, electron transfer from La to Ru via the Ru-O-La configuration could lead to increased electron density around Ru, thus preventing the over-oxidation of Ru. In addition, electron redistribution tunes the Ru 4d band center’s energy level, which optimizes the adsorption and desorption of oxygen intermediates. This work offers an effective strategy for regulating electronic structure to synergistically boost the activity and stability of RuO₂-based acidic OER electrocatalysts.

稳定出氧反应（OER）的高活性RuO2电催化剂对于质子交换膜电解的应用至关重要，但由于Ru在恶劣的氧化环境中不可避免的过度氧化，这仍然具有挑战性。在这里，我们描述了通过简单的溶胶-凝胶方法构建Ru- o - la不对称构型到RuO2中，以调整电子再分配，从而消除Ru中心的过度氧化。具体而言，制备的最佳La0.1Ru0.9O2在10 mA cm−2下的过电位为188 mV，与可逆氢电极（RHE）相比，在1.6 V下的质量活性高达251 a gRu−1，持久寿命为63 h，远远优于标准RuO2的8 h。实验和密度泛函理论计算共同表明，Ru-O-La的不对称构型可以引发RuO2中的电子重分布。更重要的是，电子通过Ru- o -La结构从La转移到Ru，可以增加Ru周围的电子密度，从而防止Ru的过度氧化。此外，电子重分配调节了Ru 4d带中心的能级，从而优化了氧中间体的吸附和解吸。本研究提供了一种有效的策略来调节电子结构，以协同提高基于ruo2的酸性OER电催化剂的活性和稳定性。

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引用次数: 0

Cryogenic and in situ characterization techniques for electrode interphase analysis 低温和原位表征技术的电极间相分析

IF 42.9 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-01-01 Epub Date: 2024-06-17 DOI: 10.1016/j.esci.2024.100291

Shuang Xiang , Lin Zhu , Liang Fu , Miaomiao Wang , Xianbi Zhang , Yougen Tang , Dan Sun , Haiyan Wang

There is an urgent need to develop innovative electrochemical energy storage devices that can offer high energy density, long lifespan, excellent rate capability, and improved security. For the electrochemical system, the electrode interphase, namely the cathode electrolyte interphase (CEI) and solid electrolyte interphase (SEI) play crucial roles in the operating mechanism, kinetics, and overall performance of the battery. However, the in-depth investigation of the unstable and complex electrode interphase is limited by the unavoidable air and moisture contact during the material transfer process and probable high-energy radiation damage in the characterization procedure. Recently, cryogenic techniques and in situ techniques have been developed and applied in the electrode interphase research to settle the radiation damage and air erosion, respectively. However, there has not been a special review that summarizes the relevant methods, so a systematic review is very important to accelerate the development. In this review, we summarize these two state-of-the-art methods, including their working principle, characterization process, advantages, and applications in electrode interphase analysis. And the integrative techniques, which are considered as the future development perspectives, are also discussed. This review can provide important directions for next-generation characterization techniques and strategies to effectively analyze the electrode interphase for advanced batteries.

迫切需要开发具有高能量密度、长寿命、高速率性能和高安全性的新型电化学储能装置。对于电化学系统而言，电极间相，即阴极电解质间相（CEI）和固体电解质间相（SEI）对电池的运行机理、动力学和整体性能起着至关重要的作用。然而，由于材料传递过程中不可避免的空气和水分接触以及表征过程中可能出现的高能辐射损伤，限制了对不稳定和复杂电极界面的深入研究。近年来，低温技术和原位技术分别被应用于电极界面研究，以解决辐射损伤和空气侵蚀问题。然而，目前还没有专门的综述对相关方法进行总结，因此系统的综述对于加快发展非常重要。本文综述了这两种方法的工作原理、表征过程、优点及其在电极间相分析中的应用。并对综合技术进行了展望，认为这是未来的发展方向。这一综述为下一代表征技术和策略的发展提供了重要的方向，以有效地分析先进电池的电极界面。

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引用次数: 0

Electrochemical conversion of small organic molecules to value-added chemicals and hydrogen/electricity without CO2 emission: Electrocatalysts, devices and mechanisms 电化学将小分子有机物转化为高附加值化学品和氢气/电力而不排放二氧化碳：电催化剂、装置和机制

IF 42.9 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-01-01 Epub Date: 2024-03-30 DOI: 10.1016/j.esci.2024.100267

Jianwen Liu , Guodong Fu , Yuanfeng Liao , Wangji Zhang , Xiuan Xi , Fengzhan Si , Lei Wang , Jiujun Zhang , Xian-Zhu Fu , Jing-Li Luo

The electrochemical conversion of small organic molecules to value-added chemicals and hydrogen/electricity without CO₂ emissions integrates efficient energy conversions (hydrogen energy or electricity) and value-added chemical productions in one reaction system, which is essentially competitive in the carbon-neutral era. However, the activity, stability, and cost-effectiveness of electrocatalysts, as well as the safety, durability, and scalability of devices, are still challenging for their industrial applications. In addition, a lack of knowledge about relevant and detailed mechanisms restricts the further development of electrocatalysts and devices. A timely review of the electrocatalysts, devices, and mechanisms is essential to shed lights on the correct direction towards further development. In this review, the advances in the design of electrocatalysts, fabrication of devices, and understanding of reaction mechanisms are comprehensively summarized and analyzed. The major challenges are also discussed as well as the potential approaches to overcoming them. The insights for further development are provided to offer a sustainable and environmentally friendly approach to cogeneration of energy and chemicals production.

小有机分子的电化学转化为增值化学品和氢/电而不排放二氧化碳，将高效的能源转换（氢能或电）和增值化学品生产集成在一个反应系统中，这在碳中和时代具有本质上的竞争力。然而，电催化剂的活性、稳定性和成本效益，以及设备的安全性、耐用性和可扩展性，仍然是其工业应用的挑战。此外，缺乏对相关机理的详细了解限制了电催化剂和器件的进一步发展。及时回顾电催化剂、装置和机制对进一步发展的正确方向至关重要。本文对电催化剂的设计、器件的制备以及反应机理的研究进展进行了综述和分析。还讨论了主要挑战以及克服这些挑战的潜在方法。提供进一步发展的见解，为能源和化学品生产的热电联产提供可持续和环境友好的方法。

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引用次数: 0