eScience最新文献

30 years of AI for electrocatalysis: Where we are and what’s next? 人工智能电催化30年：我们在哪里，下一步是什么？

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-12-17 DOI: 10.1016/j.esci.2025.100515

Haotian Chen , Enno Kätelhön , Yuanyuan Lu , Jun Cheng , Zhong-Qun Tian , Richard G. Compton

Artificial Intelligence (AI) has evolved over the past three decades from the initial pioneering stage to become a transformative force in electrocatalytic research yet is far from realizing its full potential. This review traces foundational applications of AI to electrocatalysis in the 1990s to highlight the integration of AI into the full catalyst development workflow in the last five years, from material design and synthesis to characterization and performance evaluation, and ultimately to knowledge extraction. Emphasis is placed on critical but often partially recognized or neglected bottlenecks: the scale gap between atomistic simulations and macroscopic performance, inverse electrocatalyst design, physical consistency and interpretability of machine learning models, automated experiments, and the scarcity of high-quality, well validated experimental data. Cutting edge solutions such as exascale computing, machine learning interatomic potentials (MLIPs), physics-informed machine learning (PIML), generative models (variational autoencoders, diffusion models, and large language models), and FAIR-compliant data are discussed. This review highlights that the progress of AI for electrocatalysis is inherently data-centric, driven by advances in data-quality, FAIR-compliant infrastructure, and data-driven workflows that connect experiment, simulations, and machine learning. Beyond technical perspectives, this review also emphasizes the importance of interdisciplinary collaboration, industrial relevance, and cautions in respect of hyping. By identifying challenges and highlighting emerging breakthroughs, this work offers a roadmap for advancing AI-driven electrocatalysis towards more predictive, interpretable, and scalable discovery.

人工智能（AI）在过去三十年中从最初的先驱阶段发展成为电催化研究的变革力量，但远未充分发挥其潜力。本文回顾了20世纪90年代人工智能在电催化领域的基础应用，重点介绍了过去五年人工智能在催化剂开发工作流程中的整合，从材料设计和合成到表征和性能评估，最终到知识提取。重点放在关键但经常被部分认识或忽视的瓶颈上：原子模拟和宏观性能之间的尺度差距，反电催化剂设计，机器学习模型的物理一致性和可解释性，自动化实验，以及高质量，良好验证的实验数据的稀缺性。讨论了诸如百亿亿次计算、机器学习原子间势（MLIPs）、物理信息机器学习（PIML）、生成模型（变分自编码器、扩散模型和大型语言模型）和fair兼容数据等前沿解决方案。这篇综述强调了人工智能在电催化方面的进展本质上是以数据为中心的，这是由数据质量、符合fair标准的基础设施以及连接实验、模拟和机器学习的数据驱动工作流程的进步所驱动的。除了技术角度，这篇综述还强调了跨学科合作、工业相关性的重要性，并在炒作方面提出了警告。通过识别挑战和突出新兴突破，这项工作为推动人工智能驱动的电催化向更具预测性、可解释性和可扩展性的发现方向发展提供了路线图。

{"title":"30 years of AI for electrocatalysis: Where we are and what’s next?","authors":"Haotian Chen , Enno Kätelhön , Yuanyuan Lu , Jun Cheng , Zhong-Qun Tian , Richard G. Compton","doi":"10.1016/j.esci.2025.100515","DOIUrl":"10.1016/j.esci.2025.100515","url":null,"abstract":"<div><div>Artificial Intelligence (AI) has evolved over the past three decades from the initial pioneering stage to become a transformative force in electrocatalytic research yet is far from realizing its full potential. This review traces foundational applications of AI to electrocatalysis in the 1990s to highlight the integration of AI into the full catalyst development workflow in the last five years, from material design and synthesis to characterization and performance evaluation, and ultimately to knowledge extraction. Emphasis is placed on critical but often partially recognized or neglected bottlenecks: the scale gap between atomistic simulations and macroscopic performance, inverse electrocatalyst design, physical consistency and interpretability of machine learning models, automated experiments, and the scarcity of high-quality, well validated experimental data. Cutting edge solutions such as exascale computing, machine learning interatomic potentials (MLIPs), physics-informed machine learning (PIML), generative models (variational autoencoders, diffusion models, and large language models), and FAIR-compliant data are discussed. This review highlights that the progress of AI for electrocatalysis is inherently data-centric, driven by advances in data-quality, FAIR-compliant infrastructure, and data-driven workflows that connect experiment, simulations, and machine learning. Beyond technical perspectives, this review also emphasizes the importance of interdisciplinary collaboration, industrial relevance, and cautions in respect of hyping. By identifying challenges and highlighting emerging breakthroughs, this work offers a roadmap for advancing AI-driven electrocatalysis towards more predictive, interpretable, and scalable discovery.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"6 2","pages":"Article 100515"},"PeriodicalIF":36.6,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145957650","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Regulating lower hubbard band for tandem electrocatalytic lithium polysulfides conversion 串联电催化锂多硫化物转化的调节下轨带

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-11-11 DOI: 10.1016/j.esci.2025.100497

Pan Zeng , Wanhai Zhou , Bin Su , Yinqi Hu , ChengWei Du , Xiaoqin Li , Cheng Yuan , Genlin Liu , Xiaofeng Zhao , Wei Luo , Rajeev Ahuja , Qingyuan Wang , Dongliang Chao , Liang Zhang

Catalytic conversion of lithium polysulfides (LiPSs) is a promising avenue to suppress the shuttle effect and enhance the redox kinetics of lithium–sulfur (Li–S) batteries. However, the consecutive multiple LiPSs redox reactions make the activity prediction of electrocatalysts elusive. Herein, we propose a lower Hubbard band (LHB) descriptor to regulate tandem electrocatalytic LiPSs conversion for fast and robust Li–S batteries. Combined with theoretical calculations, the catalytic activity is jointly determined by the balance between LHB center position (Ɛ_LHB) and LHB width (ꞷ_LHB). As a proof of concept, Fe₃O₄@FeP shows a balance of possessing a close Ɛ_LHB to the Fermi level and a wide ꞷ_LHB simultaneously. An accelerated tandem electrocatalytic LiPSs conversion is achieved, where a close Ɛ_LHB to Fermi level (with Fe₃O₄ as the active center) benefits the adsorption of long-chain LiPSs and catalyzes S₈-to-Li₂S₄ process, while a wide ꞷ_LHB (with FeP as the active center) subsequently contributes to catalyze the Li₂S₄-to-Li₂S reaction. Consequently, the elaborate Li–S batteries deliver outstanding cycle stability over 1000 cycles and superior rate performance over 10C. Further, the constructed Ah-scale pouch cell delivers notable energy density of 360.6 Wh kg⁻¹. This work demonstrates the great promise of LHB regulation strategy for designing high-efficient electrocatalysts for Li–S batteries and beyond.

多硫化物锂（LiPSs）的催化转化是抑制穿梭效应和提高锂硫电池氧化还原动力学的一种很有前途的途径。然而，连续的多个LiPSs氧化还原反应使得电催化剂的活性难以预测。在此，我们提出了一个低哈伯德带（LHB）描述子来调节串联电催化lips转化，以实现快速和坚固的Li-S电池。结合理论计算，催化活性由LHB中心位置（ƐLHB）和LHB宽度（ꞷLHB）之间的平衡共同决定。作为概念证明，Fe3O4@FeP显示了同时拥有接近ƐLHB的费米能级和宽ꞷ的LHB的平衡。实现了一个加速的串联电催化LiPSs转化，其中接近ƐLHB费米能级（以Fe3O4为活性中心）有利于长链LiPSs的吸附并催化s8到li2s4的过程，而宽ꞷLHB（以FeP为活性中心）随后有助于催化li2s4到li2s的反应。因此，精心制作的Li-S电池在1000次循环以上提供出色的循环稳定性，在10C以上提供卓越的倍率性能。此外，构建的ah级袋状电池提供了360.6 Wh kg−1的显著能量密度。这项工作证明了LHB调节策略在设计Li-S电池及其他领域的高效电催化剂方面的巨大前景。

{"title":"Regulating lower hubbard band for tandem electrocatalytic lithium polysulfides conversion","authors":"Pan Zeng , Wanhai Zhou , Bin Su , Yinqi Hu , ChengWei Du , Xiaoqin Li , Cheng Yuan , Genlin Liu , Xiaofeng Zhao , Wei Luo , Rajeev Ahuja , Qingyuan Wang , Dongliang Chao , Liang Zhang","doi":"10.1016/j.esci.2025.100497","DOIUrl":"10.1016/j.esci.2025.100497","url":null,"abstract":"<div><div>Catalytic conversion of lithium polysulfides (LiPSs) is a promising avenue to suppress the shuttle effect and enhance the redox kinetics of lithium–sulfur (Li–S) batteries. However, the consecutive multiple LiPSs redox reactions make the activity prediction of electrocatalysts elusive. Herein, we propose a lower Hubbard band (LHB) descriptor to regulate tandem electrocatalytic LiPSs conversion for fast and robust Li–S batteries. Combined with theoretical calculations, the catalytic activity is jointly determined by the balance between LHB center position (Ɛ<sub>LHB</sub>) and LHB width (ꞷ<sub>LHB</sub>). As a proof of concept, Fe<sub>3</sub>O<sub>4</sub>@FeP shows a balance of possessing a close Ɛ<sub>LHB</sub> to the Fermi level and a wide ꞷ<sub>LHB</sub> simultaneously. An accelerated tandem electrocatalytic LiPSs conversion is achieved, where a close Ɛ<sub>LHB</sub> to Fermi level (with Fe<sub>3</sub>O<sub>4</sub> as the active center) benefits the adsorption of long-chain LiPSs and catalyzes S<sub>8</sub>-to-Li<sub>2</sub>S<sub>4</sub> process, while a wide ꞷ<sub>LHB</sub> (with FeP as the active center) subsequently contributes to catalyze the Li<sub>2</sub>S<sub>4</sub>-to-Li<sub>2</sub>S reaction. Consequently, the elaborate Li–S batteries deliver outstanding cycle stability over 1000 cycles and superior rate performance over 10C. Further, the constructed Ah-scale pouch cell delivers notable energy density of 360.6 Wh kg<sup>−1</sup>. This work demonstrates the great promise of LHB regulation strategy for designing high-efficient electrocatalysts for Li–S batteries and beyond.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"6 1","pages":"Article 100497"},"PeriodicalIF":36.6,"publicationDate":"2025-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145842606","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Site-specific stabilizing effect of single atoms on spinel oxides for acidic oxygen evolution 单原子对尖晶石氧化物酸性析氧的定点稳定作用

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-11-01 DOI: 10.1016/j.esci.2025.100402

Zhirong Zhang , Peiyu Ma , Chuanyi Jia , Wenting Gao , Mingkai Liu , Kwun Nam Hui , Ming Zuo , Shiming Zhou , Jie Zeng

Developing efficient and economical non-precious metal electrocatalysts for acidic oxygen evolution reaction (OER) is crucial for proton exchange membrane water electrolyzers (PEMWE). Spinel oxides are considered promising non-precious acidic OER catalysts due to their excellent activities. However, the structure dissolution of spinel oxides in acidic conditions severely limits their applications in PEMWE. Introducing acid-resistant heteroatoms into spinel oxides is an available strategy to enhance their stability. Herein, by anchoring Ir single atoms at different sites of spinel oxide Co₃O₄, we demonstrated that the stabilizing effect strongly depends on the single-atom anchoring site. Electrochemical measurements and in situ spectroscopic characterization revealed that the Ir single atoms anchored at lattice sites significantly enhanced the stability of Co₃O₄ during acidic OER in comparison with ones at three-fold hollow sites. The long-term durability test showed that the Ir single atoms at lattice sites stabilized Co₃O₄ during a 200 h continuous operation at a current density of 10 mA cm⁻². Moreover, the resultant PEMWE device fabricated by the catalyst achieved a stability time of about 60 h at a current density of 1 A cm⁻². Mechanistic studies revealed that Ir single atoms at lattice sites enhanced the covalency between Co and O atoms, thereby suppressing their migration and improving the stability of spinel oxides. The discovery of the site-specific stabilizing effect of single atoms provides essential guidance for the rational design of highly stable electrocatalysts for PEMWE.

开发高效、经济的非贵金属酸性析氧电催化剂是质子交换膜水电解槽（PEMWE）发展的关键。尖晶石氧化物因其优异的活性被认为是很有前途的非贵重酸性OER催化剂。然而，尖晶石氧化物在酸性条件下的结构溶解严重限制了其在PEMWE中的应用。在尖晶石氧化物中引入耐酸杂原子是提高其稳定性的一种有效策略。本文通过将Ir单原子锚定在尖晶石氧化物Co3O4的不同位点，证明了稳定效果强烈依赖于单原子锚定位点。电化学测量和原位光谱表征表明，在酸性OER中，固定在晶格位置的Ir单原子比固定在三层空心位置的Ir单原子显著提高了Co3O4的稳定性。长期耐久性测试表明，在10 mA cm−2的电流密度下，晶格位置的Ir单原子在200 h的连续工作中稳定了Co3O4。此外，该催化剂制备的PEMWE器件在电流密度为1 a cm−2时的稳定时间约为60 h。机制研究表明，晶格位置的Ir单原子增强了Co和O原子之间的共价，从而抑制了Co和O原子的迁移，提高了尖晶石氧化物的稳定性。单原子的定点稳定效应的发现，为合理设计高稳定性的PEMWE电催化剂提供了重要的指导。

{"title":"Site-specific stabilizing effect of single atoms on spinel oxides for acidic oxygen evolution","authors":"Zhirong Zhang , Peiyu Ma , Chuanyi Jia , Wenting Gao , Mingkai Liu , Kwun Nam Hui , Ming Zuo , Shiming Zhou , Jie Zeng","doi":"10.1016/j.esci.2025.100402","DOIUrl":"10.1016/j.esci.2025.100402","url":null,"abstract":"<div><div>Developing efficient and economical non-precious metal electrocatalysts for acidic oxygen evolution reaction (OER) is crucial for proton exchange membrane water electrolyzers (PEMWE). Spinel oxides are considered promising non-precious acidic OER catalysts due to their excellent activities. However, the structure dissolution of spinel oxides in acidic conditions severely limits their applications in PEMWE. Introducing acid-resistant heteroatoms into spinel oxides is an available strategy to enhance their stability. Herein, by anchoring Ir single atoms at different sites of spinel oxide Co<sub>3</sub>O<sub>4</sub>, we demonstrated that the stabilizing effect strongly depends on the single-atom anchoring site. Electrochemical measurements and <em>in situ</em> spectroscopic characterization revealed that the Ir single atoms anchored at lattice sites significantly enhanced the stability of Co<sub>3</sub>O<sub>4</sub> during acidic OER in comparison with ones at three-fold hollow sites. The long-term durability test showed that the Ir single atoms at lattice sites stabilized Co<sub>3</sub>O<sub>4</sub> during a 200 h continuous operation at a current density of 10 mA cm<sup>−</sup><sup>2</sup>. Moreover, the resultant PEMWE device fabricated by the catalyst achieved a stability time of about 60 h at a current density of 1 A cm<sup>−</sup><sup>2</sup>. Mechanistic studies revealed that Ir single atoms at lattice sites enhanced the covalency between Co and O atoms, thereby suppressing their migration and improving the stability of spinel oxides. The discovery of the site-specific stabilizing effect of single atoms provides essential guidance for the rational design of highly stable electrocatalysts for PEMWE.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 6","pages":"Article 100402"},"PeriodicalIF":36.6,"publicationDate":"2025-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145528416","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Design of dual-electrode interfacial kinetics regulator for long-lasting Ah-level zinc-iodine batteries 长效ah级锌碘电池双电极界面动力学调节器的设计

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-11-01 DOI: 10.1016/j.esci.2025.100455

Xueting Hu , Guojun Lai , Yangyang Liu , Peng Zhou , Bingan Lu , Zeinhom M. El-Bahy , Manal S. Ebaid , Lina Chen , Jiang Zhou

Zinc-iodine (Zn–I₂) batteries hold great promise for large-scale applications, yet their practical deployment is constrained by uncontrollable iodine conversion, polyiodide shuttling, and unpredictable zinc (Zn) depositional morphology. Furthermore, the mismatched kinetics of its interfacial reactions demand significant attention. Herein, we introduce a betaine (Bet) additive as a dual-electrode interfacial regulator to synergistically address the challenges faced at both the anode and cathode interface. Specifically, the hydrophilic group (–COO) of Bet preferentially adsorbs on the Zn anode surface, modulating Zn²⁺ solvation and electrodeposition dynamics to enable highly uniform Zn plating, extending the Zn–Zn symmetric cell lifespan beyond 7000 h at 1 mA cm⁻². Moreover, Bet's lipophilic group (–N–R₃) interacts with polyiodides, suppressing their migration and accelerating iodine redox kinetics, thereby mitigating cathodic side reactions. Consequently, Zn–I₂ full-cell demonstrates exceptional cycle life, maintaining capacity with an ultralow decay rate of 0.007‰ per cycle over 15,500 cycles at 10 mA cm⁻². Furthermore, an Ah-level pouch cell of ∼1.15 Ah can deliver a competitive capacity retention of 92.1% after 600 cycles, highlighting the scalability of this approach. This cost-effective and efficient interfacial modulation strategy offers a new perspective for realizing long-cycle Zn–I₂ batteries and advancing their practical applications.

锌-碘（Zn - i2）电池具有大规模应用的巨大前景，但其实际部署受到不可控的碘转化、多碘化物穿梭和不可预测的锌（Zn）沉积形态的限制。此外，其界面反应的不匹配动力学值得重视。在此，我们引入甜菜碱（Bet）添加剂作为双电极界面调节剂，以协同解决阳极和阴极界面面临的挑战。具体来说，Bet的亲水性基团（-COO）优先吸附在Zn阳极表面，调节Zn2+的溶剂化和电沉积动力学，实现高度均匀的Zn电镀，延长Zn - Zn对称电池在1 mA cm - 2下的寿命超过7000小时。此外，Bet的亲脂基团（-N-R3）与多碘化物相互作用，抑制它们的迁移并加速碘氧化还原动力学，从而减轻阴极副反应。因此，锌- i2全电池表现出优异的循环寿命，在10 mA cm - 2下，在15,500次循环中，每循环保持0.007‰的超低衰减率。此外，约1.15 Ah的Ah级袋状电池在600次循环后可提供92.1%的竞争容量保留，突出了该方法的可扩展性。这种经济高效的界面调制策略为实现长周期锌- i2电池和推进其实际应用提供了新的前景。

{"title":"Design of dual-electrode interfacial kinetics regulator for long-lasting Ah-level zinc-iodine batteries","authors":"Xueting Hu , Guojun Lai , Yangyang Liu , Peng Zhou , Bingan Lu , Zeinhom M. El-Bahy , Manal S. Ebaid , Lina Chen , Jiang Zhou","doi":"10.1016/j.esci.2025.100455","DOIUrl":"10.1016/j.esci.2025.100455","url":null,"abstract":"<div><div>Zinc-iodine (Zn–I<sub>2</sub>) batteries hold great promise for large-scale applications, yet their practical deployment is constrained by uncontrollable iodine conversion, polyiodide shuttling, and unpredictable zinc (Zn) depositional morphology. Furthermore, the mismatched kinetics of its interfacial reactions demand significant attention. Herein, we introduce a betaine (Bet) additive as a dual-electrode interfacial regulator to synergistically address the challenges faced at both the anode and cathode interface. Specifically, the hydrophilic group (–COO) of Bet preferentially adsorbs on the Zn anode surface, modulating Zn<sup>2+</sup> solvation and electrodeposition dynamics to enable highly uniform Zn plating, extending the Zn–Zn symmetric cell lifespan beyond 7000 h at 1 mA cm<sup>−2</sup>. Moreover, Bet's lipophilic group (–N–R<sub>3</sub>) interacts with polyiodides, suppressing their migration and accelerating iodine redox kinetics, thereby mitigating cathodic side reactions. Consequently, Zn–I<sub>2</sub> full-cell demonstrates exceptional cycle life, maintaining capacity with an ultralow decay rate of 0.007‰ per cycle over 15,500 cycles at 10 mA cm<sup>−2</sup>. Furthermore, an Ah-level pouch cell of ∼1.15 Ah can deliver a competitive capacity retention of 92.1% after 600 cycles, highlighting the scalability of this approach. This cost-effective and efficient interfacial modulation strategy offers a new perspective for realizing long-cycle Zn–I<sub>2</sub> batteries and advancing their practical applications.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 6","pages":"Article 100455"},"PeriodicalIF":36.6,"publicationDate":"2025-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145425511","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Noble metal-free single-atom electrocatalysts and reactor engineering for enhanced hydrogen peroxide generation via two-electron oxygen reduction reaction 无贵金属单原子电催化剂及通过双电子氧还原反应增强过氧化氢生成的反应器工程

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-07-25 DOI: 10.1016/j.esci.2025.100456

Jingqin Ji , Hui Wang , Yanlan Zhao , Yan Wang , Kaifeng Wang , Yuexin Cui , Ridha Djellabi , Chuan Xia , Xu Zhao , Xiangming He

The generation of hydrogen peroxide (H₂O₂), a compound with diverse applications, via the two-electron (2e⁻) oxygen reduction reaction (ORR) has garnered extensive attention in both laboratory research and industrial settings. The integration of non-noble metals such as Co, Fe, Ni, Zn, Mn, Mo, or Bi into nitrogen-doped carbon (M–N–C) matrices with defined structures and active metal center sites has emerged as a promising approach for fabricating electrocatalysts for the ORR. This review uncovers the latest advancements in the development of noble metal-free single-atom electrocatalysts (M–N–C SAECs) and electrochemical reactors aimed at enhancing and stabilizing H₂O₂ production from the 2e⁻ ORR. Firstly, the review explores the basics of the ORR for H₂O₂ production and the impact of electrochemical conditions. Subsequently, the synthesis strategies and characterization methods of various M–N–C SAECs are examined in depth. In addition, the structural attributes of both conventional and altered M–N–C SAECs are meticulously investigated, and the importance of engineering and optimizing reactors to elevate H₂O₂ yields is highlighted. This review identifies the challenges and technological hurdles in bridging the gap between laboratory-scale research and practical, real-world applications.

过氧化氢（H2O2）是一种应用广泛的化合物，通过双电子（2e−）氧还原反应（ORR）生成过氧化氢（H2O2）在实验室研究和工业环境中都得到了广泛的关注。将Co， Fe, Ni, Zn, Mn， Mo或Bi等非贵金属整合到具有明确结构和活性金属中心位置的氮掺杂碳（M-N-C）基体中，已成为制造ORR电催化剂的一种有前途的方法。本文综述了无贵金属单原子电催化剂（M-N-C saec）和旨在提高和稳定2e - ORR产生H2O2的电化学反应器的最新进展。首先，综述了ORR生产H2O2的基本原理和电化学条件的影响。随后，深入研究了各种M-N-C saec的合成策略和表征方法。此外，本文还详细研究了常规和改进型M-N-C saec的结构特性，并强调了提高H2O2产率的工程和优化反应器的重要性。这篇综述指出了在弥合实验室规模研究和实际应用之间的差距方面面临的挑战和技术障碍。

{"title":"Noble metal-free single-atom electrocatalysts and reactor engineering for enhanced hydrogen peroxide generation via two-electron oxygen reduction reaction","authors":"Jingqin Ji , Hui Wang , Yanlan Zhao , Yan Wang , Kaifeng Wang , Yuexin Cui , Ridha Djellabi , Chuan Xia , Xu Zhao , Xiangming He","doi":"10.1016/j.esci.2025.100456","DOIUrl":"10.1016/j.esci.2025.100456","url":null,"abstract":"<div><div>The generation of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>), a compound with diverse applications, via the two-electron (2e<sup>−</sup>) oxygen reduction reaction (ORR) has garnered extensive attention in both laboratory research and industrial settings. The integration of non-noble metals such as Co, Fe, Ni, Zn, Mn, Mo, or Bi into nitrogen-doped carbon (M–N–C) matrices with defined structures and active metal center sites has emerged as a promising approach for fabricating electrocatalysts for the ORR. This review uncovers the latest advancements in the development of noble metal-free single-atom electrocatalysts (M–N–C SAECs) and electrochemical reactors aimed at enhancing and stabilizing H<sub>2</sub>O<sub>2</sub> production from the 2e<sup>−</sup> ORR. Firstly, the review explores the basics of the ORR for H<sub>2</sub>O<sub>2</sub> production and the impact of electrochemical conditions. Subsequently, the synthesis strategies and characterization methods of various M–N–C SAECs are examined in depth. In addition, the structural attributes of both conventional and altered M–N–C SAECs are meticulously investigated, and the importance of engineering and optimizing reactors to elevate H<sub>2</sub>O<sub>2</sub> yields is highlighted. This review identifies the challenges and technological hurdles in bridging the gap between laboratory-scale research and practical, real-world applications.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"6 2","pages":"Article 100456"},"PeriodicalIF":36.6,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145981527","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Longitudinal confinement engineering in phase change materials 相变材料的纵向约束工程

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-07-23 DOI: 10.1016/j.esci.2025.100454

Yuhao Feng , Keke Chen , Panpan Liu , Jindi Zhao , Yang Li , Xiao Chen

Amidst escalating energy demands and intensifying environmental pressures, advanced phase change materials (PCMs) have emerged as highly efficient and sustainable storage solutions, owing to their unique operational principles. However, pristine PCMs encounter a multitude of challenges, including susceptibility to leakage, inferior thermal/electrical conductivity, inadequate light responsiveness, intrinsic rigidity, and limited functionality, which impede their effectiveness in addressing the complex demands of real-world applications. Longitudinal confinement of PCMs using advanced multifunctional 1D materials is accepted as a cutting-edge solution to these limitations. A corresponding comprehensive review of longitudinally confined composite PCMs is thus imperative for subsequent studies and yet is missing from the literature, unlike reviews of 0D, 2D, and 3D materials for PCMs. Herein, this review systematically highlights the diverse roles of longitudinal materials in PCMs and analyzes the relationships between their architectures and thermophysical properties, with particular emphasis on design principles and advanced multifunctional interdisciplinary applications. Additionally, we provide an in-depth understanding of thermal transfer, energy conversion mechanisms, and rationalized routes to high-efficiency energy conversion PCMs. Finally, we introduce critical considerations for current challenges and future solutions to them, hoping to offer constructive guidance and facilitate significant breakthroughs for longitudinally confined composite PCMs in both fundamental interdisciplinary research and commercial applications.

在不断升级的能源需求和不断加剧的环境压力下，先进相变材料（PCMs）由于其独特的工作原理而成为高效和可持续的存储解决方案。然而，原始pcm面临着许多挑战，包括易泄漏、导热/导电性差、光响应性不足、固有刚性和有限的功能，这些都阻碍了它们在解决实际应用的复杂需求方面的有效性。使用先进的多功能一维材料纵向约束pcm被认为是解决这些限制的前沿解决方案。因此，纵向受限复合pcm的相应综合综述对于后续研究是必要的，但与对pcm的0D， 2D和3D材料的综述不同，文献中缺少这一综述。在此，本文系统地强调了纵向材料在pcm中的不同作用，并分析了其结构与热物理性质之间的关系，特别强调了设计原则和先进的多功能跨学科应用。此外，我们还提供了对热传导，能量转换机制的深入了解，以及高效能量转换pcm的合理化路线。最后，我们介绍了当前挑战的关键考虑因素和未来的解决方案，希望为纵向受限复合材料相变材料在基础跨学科研究和商业应用方面提供建设性的指导和促进重大突破。

{"title":"Longitudinal confinement engineering in phase change materials","authors":"Yuhao Feng , Keke Chen , Panpan Liu , Jindi Zhao , Yang Li , Xiao Chen","doi":"10.1016/j.esci.2025.100454","DOIUrl":"10.1016/j.esci.2025.100454","url":null,"abstract":"<div><div>Amidst escalating energy demands and intensifying environmental pressures, advanced phase change materials (PCMs) have emerged as highly efficient and sustainable storage solutions, owing to their unique operational principles. However, pristine PCMs encounter a multitude of challenges, including susceptibility to leakage, inferior thermal/electrical conductivity, inadequate light responsiveness, intrinsic rigidity, and limited functionality, which impede their effectiveness in addressing the complex demands of real-world applications. Longitudinal confinement of PCMs using advanced multifunctional 1D materials is accepted as a cutting-edge solution to these limitations. A corresponding comprehensive review of longitudinally confined composite PCMs is thus imperative for subsequent studies and yet is missing from the literature, unlike reviews of 0D, 2D, and 3D materials for PCMs. Herein, this review systematically highlights the diverse roles of longitudinal materials in PCMs and analyzes the relationships between their architectures and thermophysical properties, with particular emphasis on design principles and advanced multifunctional interdisciplinary applications. Additionally, we provide an in-depth understanding of thermal transfer, energy conversion mechanisms, and rationalized routes to high-efficiency energy conversion PCMs. Finally, we introduce critical considerations for current challenges and future solutions to them, hoping to offer constructive guidance and facilitate significant breakthroughs for longitudinally confined composite PCMs in both fundamental interdisciplinary research and commercial applications.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"6 1","pages":"Article 100454"},"PeriodicalIF":36.6,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145842688","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Mutual stabilization of hybrid and inorganic perovskites for photovoltaics 光伏用杂化钙钛矿和无机钙钛矿的相互稳定

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-07-18 DOI: 10.1016/j.esci.2025.100449

Yuheng Li , Ziwei Zheng , Xin Zheng , Xiaoyuan Liu , Yingguo Yang , Yongcheng Zhu , Zaiwei Wang , Xingyu Ren , Mimi Fu , Rui Guo , Jing Guo , Zewen Xiao , Yaoguang Rong , Xiong Li

Stabilizing black-phase formamidinium lead triiodide (FAPbI₃) is critical for high-performance perovskite solar cells (PSCs). We present a stabilization strategy utilizing co-evaporated cesium lead iodide (CsPbI₃) capping layers. Enabled by favorable crystal lattice matching, cubic-phase CsPbI₃ spontaneously forms on FAPbI₃ surfaces, establishing mutual phase stabilization with the underlying black-phase FAPbI₃. When combined with ammonium salt interface modification, the CsPbI₃ interlayer effectively suppresses the ion (FA⁺ and F-PEA⁺) diffusion between the stacked perovskite layers. The FAPbI₃/CsPbI₃ bilayer structured devices exhibited a certified record reverse-scanning power-conversion efficiency of 27.17% and maintained a stabilized power output efficiency of 26.62%. Remarkably, the cells retain 93.5% of the initial efficiency after 1500 h damp-heat test, and retaining over 94.2% of its maximum PCE after about 1185 h with a linear extrapolation to a T₉₀ of 2352 h operation under continuous illumination at maximum power point tracking at 85 °C.

稳定黑相三碘化甲脒铅（FAPbI3）是高性能钙钛矿太阳能电池（PSCs）的关键。我们提出了一种利用共蒸发铯碘化铅（CsPbI3）封盖层的稳定策略。由于有利的晶格匹配，立方相CsPbI3在FAPbI3表面自发形成，与底层的黑相FAPbI3建立了相互相稳定。当与铵盐界面改性结合时，CsPbI3夹层能有效抑制钙钛矿层间离子（FA+和F-PEA+）的扩散。FAPbI3/CsPbI3双层结构器件的反向扫描功率转换效率为27.17%，稳定功率输出效率为26.62%。值得注意的是，电池在1500 h湿热测试后保持了93.5%的初始效率，在大约1185 h后保持了超过94.2%的最大PCE，线性外推到在85°C的最大功率点跟踪下连续照明下运行2352 h的T90。

{"title":"Mutual stabilization of hybrid and inorganic perovskites for photovoltaics","authors":"Yuheng Li , Ziwei Zheng , Xin Zheng , Xiaoyuan Liu , Yingguo Yang , Yongcheng Zhu , Zaiwei Wang , Xingyu Ren , Mimi Fu , Rui Guo , Jing Guo , Zewen Xiao , Yaoguang Rong , Xiong Li","doi":"10.1016/j.esci.2025.100449","DOIUrl":"10.1016/j.esci.2025.100449","url":null,"abstract":"<div><div>Stabilizing black-phase formamidinium lead triiodide (FAPbI<sub>3</sub>) is critical for high-performance perovskite solar cells (PSCs). We present a stabilization strategy utilizing co-evaporated cesium lead iodide (CsPbI<sub>3</sub>) capping layers. Enabled by favorable crystal lattice matching, cubic-phase CsPbI<sub>3</sub> spontaneously forms on FAPbI<sub>3</sub> surfaces, establishing mutual phase stabilization with the underlying black-phase FAPbI<sub>3</sub>. When combined with ammonium salt interface modification, the CsPbI<sub>3</sub> interlayer effectively suppresses the ion (FA<sup>+</sup> and F-PEA<sup>+</sup>) diffusion between the stacked perovskite layers. The FAPbI<sub>3</sub>/CsPbI<sub>3</sub> bilayer structured devices exhibited a certified record reverse-scanning power-conversion efficiency of 27.17% and maintained a stabilized power output efficiency of 26.62%. Remarkably, the cells retain 93.5% of the initial efficiency after 1500 h damp-heat test, and retaining over 94.2% of its maximum PCE after about 1185 h with a linear extrapolation to a <em>T</em><sub>90</sub> of 2352 h operation under continuous illumination at maximum power point tracking at 85 °C.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"6 1","pages":"Article 100449"},"PeriodicalIF":36.6,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145799745","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Concentration-gradient driven atom diffusion to synthesize high-loaded and sub-5 nm PtCo intermetallic compound for fuel cells 浓度梯度驱动原子扩散合成燃料电池用高负载亚5nm PtCo金属间化合物

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-07-16 DOI: 10.1016/j.esci.2025.100453

Qingqing Cheng , Tao Wang , Yihe Chen , Yongyu Pan , Yubin Chen , Bo Yang , Hui Yang

The synthesis of Pt intermetallic compounds (IMCs) typically necessitates high-temperature annealing to overcome the atom-diffusion kinetic barrier, which inevitably results in considerable nanoparticle sintering, especially for the high-loaded catalyst, thus leading to diminished performance in proton exchange membrane fuel cells. We propose a concentration-gradient-driven atom diffusion strategy to synthesize Pt intermetallic compounds (IMCs), overcoming the atom-diffusion kinetic barrier under relatively low temperature. This method efficiently transforms high-loaded Pt seeds/C into sub-5 nm L₁₀-PtCo-IMC/C (44.3 wt%) catalyst. Advanced characterizations and molecular dynamic simulations reveal that locally concentrated Co precursors accelerate atom diffusion and enhance nanoparticle anti-sintering ability. Temperature-dependent analyses further elucidate the structural transformation mechanism by tracking crystal structure and nanoparticle size evolution. Membrane electrode assembly (MEA) integrated with the optimized PtCo-IMC/C at a low Pt usage (0.1 mg cm⁻²) delivers a maximum power density of approximately 1.15 W cm⁻² and excellent stability (a 26-mV loss at 0.8 A cm⁻²) after 30000 cycles of accelerated stress testing under H₂-air conditions. This scalable synthesis pathway (20 g per batch) holds great promise for advancing high-loaded fuel cell electrocatalysts.

Pt金属间化合物（IMCs）的合成通常需要高温退火来克服原子扩散动力学屏障，这不可避免地导致大量纳米颗粒烧结，特别是对于高负载催化剂，从而导致质子交换膜燃料电池的性能下降。我们提出了一种浓度梯度驱动的原子扩散策略来合成铂金属间化合物（IMCs），克服了相对低温下原子扩散的动力学势垒。该方法有效地将高负载Pt种子/C转化为低于5 nm （44.3% wt%）的L10-PtCo-IMC/C催化剂。先进的表征和分子动力学模拟表明，局部浓缩的Co前驱体加速了原子扩散，增强了纳米颗粒的抗烧结能力。温度依赖分析通过跟踪晶体结构和纳米颗粒尺寸演变进一步阐明了结构转变机制。膜电极组件（MEA）与优化的PtCo-IMC/C集成在低铂用量（0.1 mg cm - 2）下，在h2 -空气条件下进行30000次加速应力测试后，其最大功率密度约为1.15 W cm - 2，稳定性极佳（0.8 a cm - 2时损耗26 mv）。这种可扩展的合成途径（每批20克）对推进高负荷燃料电池电催化剂具有很大的希望。

{"title":"Concentration-gradient driven atom diffusion to synthesize high-loaded and sub-5 nm PtCo intermetallic compound for fuel cells","authors":"Qingqing Cheng , Tao Wang , Yihe Chen , Yongyu Pan , Yubin Chen , Bo Yang , Hui Yang","doi":"10.1016/j.esci.2025.100453","DOIUrl":"10.1016/j.esci.2025.100453","url":null,"abstract":"<div><div>The synthesis of Pt intermetallic compounds (IMCs) typically necessitates high-temperature annealing to overcome the atom-diffusion kinetic barrier, which inevitably results in considerable nanoparticle sintering, especially for the high-loaded catalyst, thus leading to diminished performance in proton exchange membrane fuel cells. We propose a concentration-gradient-driven atom diffusion strategy to synthesize Pt intermetallic compounds (IMCs), overcoming the atom-diffusion kinetic barrier under relatively low temperature. This method efficiently transforms high-loaded Pt seeds/C into sub-5 nm L<sub>10</sub>-PtCo-IMC/C (44.3 wt%) catalyst. Advanced characterizations and molecular dynamic simulations reveal that locally concentrated Co precursors accelerate atom diffusion and enhance nanoparticle anti-sintering ability. Temperature-dependent analyses further elucidate the structural transformation mechanism by tracking crystal structure and nanoparticle size evolution. Membrane electrode assembly (MEA) integrated with the optimized PtCo-IMC/C at a low Pt usage (0.1 mg cm<sup>−2</sup>) delivers a maximum power density of approximately 1.15 W cm<sup>−2</sup> and excellent stability (a 26-mV loss at 0.8 A cm<sup>−2</sup>) after 30000 cycles of accelerated stress testing under H<sub>2</sub>-air conditions. This scalable synthesis pathway (20 g per batch) holds great promise for advancing high-loaded fuel cell electrocatalysts.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"6 1","pages":"Article 100453"},"PeriodicalIF":36.6,"publicationDate":"2025-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145842687","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Electron-funnel mediated anion confinement enables ultra-reversible interphases in solid-state batteries 电子漏斗介导的阴离子约束使固态电池中的超可逆界面成为可能

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-07-10 DOI: 10.1016/j.esci.2025.100452

Yi Chen , Ji Qian , Ke Wang , Tianyang Xue , Zhengqiang Hu , Fengling Zhang , Tong Lian , Xinhui Pan , Teng Zhao , Li Li , Feng Wu , Renjie Chen

Solid-state lithium metal batteries face challenges from irreversible interfacial degradation and sluggish ion transport. We propose an electron-funnel-mediated anion confinement strategy via atomic-level electronic field engineering. Incorporating electron-withdrawing –NO₂ groups into Zr-based frameworks induces a 0.38 eV upward d-band center shift, generating a quantum-confined electrostatic gradient that polarizes TFSI⁻ anions. This reduces TFSI⁻ decomposition energy barrier (ΔG: −0.35 → −1.22 eV), selectively promoting LiF nucleation while suppressing side reactions. Concurrently, Zr⁴⁺-PEO Lewis interactions disrupt polymer crystallinity, enhancing ionic conductivity and Li⁺ transference number. Cryo-TEM tomography and TOF-SIMS mapping reveal a fractal LiF-rich interphase enabling dendrite-free lithium plating for > 11,000 h with polarization < 40 mV. LiFePO₄ full cells achieve 86.3% capacity retention after 400 cycles at 1C (1.3 mAh cm⁻²). This work establishes anion confinement as a universal framework synchronizing ion transport and interfacial durability, advancing practical solid-state batteries with exceptional longevity.

固态锂金属电池面临着界面不可逆降解和离子传输缓慢等挑战。我们提出了一种电子通道介导的阴离子约束策略。将吸电子的-NO2基团加入到zr基框架中，诱导了0.38 eV向上的d波段中心位移，产生了量子限制的静电梯度，使TFSI -阴离子极化。这降低了TFSI -分解能垒（ΔG:−0.35→−1.22 eV），选择性地促进了LiF成核，同时抑制了副反应。同时，Zr4+-PEO路易斯相互作用破坏了聚合物的结晶度，提高了离子电导率和Li+转移数。低温tem断层扫描和TOF-SIMS图谱显示了一个分形的富liff界面，可以在极化40 mV下电镀11000 h的无枝晶锂。在1C （1.3 mAh cm−2）下循环400次后，LiFePO4全电池的容量保持率达到86.3%。这项工作建立了阴离子约束作为同步离子传输和界面耐久性的通用框架，推进了具有特殊寿命的实用固态电池。

{"title":"Electron-funnel mediated anion confinement enables ultra-reversible interphases in solid-state batteries","authors":"Yi Chen , Ji Qian , Ke Wang , Tianyang Xue , Zhengqiang Hu , Fengling Zhang , Tong Lian , Xinhui Pan , Teng Zhao , Li Li , Feng Wu , Renjie Chen","doi":"10.1016/j.esci.2025.100452","DOIUrl":"10.1016/j.esci.2025.100452","url":null,"abstract":"<div><div>Solid-state lithium metal batteries face challenges from irreversible interfacial degradation and sluggish ion transport. We propose an electron-funnel-mediated anion confinement strategy via atomic-level electronic field engineering. Incorporating electron-withdrawing –NO<sub>2</sub> groups into Zr-based frameworks induces a 0.38 eV upward d-band center shift, generating a quantum-confined electrostatic gradient that polarizes TFSI<sup>−</sup> anions. This reduces TFSI<sup>−</sup> decomposition energy barrier (ΔG: −0.35 → −1.22 eV), selectively promoting LiF nucleation while suppressing side reactions. Concurrently, Zr<sup>4+</sup>-PEO Lewis interactions disrupt polymer crystallinity, enhancing ionic conductivity and Li<sup>+</sup> transference number. Cryo-TEM tomography and TOF-SIMS mapping reveal a fractal LiF-rich interphase enabling dendrite-free lithium plating for > 11,000 h with polarization < 40 mV. LiFePO<sub>4</sub> full cells achieve 86.3% capacity retention after 400 cycles at 1C (1.3 mAh cm<sup>−2</sup>). This work establishes anion confinement as a universal framework synchronizing ion transport and interfacial durability, advancing practical solid-state batteries with exceptional longevity.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"6 1","pages":"Article 100452"},"PeriodicalIF":36.6,"publicationDate":"2025-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145842684","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Chemical inhibition of light-induced decomposition by hindered amine for efficient and stable perovskite solar cells 高效稳定钙钛矿太阳能电池中受阻胺对光诱导分解的化学抑制

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-07-05 DOI: 10.1016/j.esci.2025.100451

Yuqing Su , Jike Ding , Zuolin Zhang , Mengjia Li , Jiangzhao Chen , Jian-Xin Tang , Thierry Pauporté , Cong Chen

Despite significant advancements in improving the power-conversion efficiency (PCE) of exceeding 27% in perovskite solar cells (PSCs), the insufficient operational stability of PSCs under illumination remains a critical challenge, posing a major obstacle to their commercial viability. This paper proposes a feasible hindered amine stabilization strategy (HASS) by using a hindered amine light stabilizer for grain and surface modulation of perovskite, thereby blocking the internal and external degradation pathways of perovskite. Its piperidine ring is easily oxidized to form Nitrogen monoxide (N–O•) radicals after absorbing light energy in an aerobic environment. The free superoxide radical (

O_{2}^{\cdot -}

) radicals react with perovskite and H⁺ in the decomposition products of perovskite, thereby improving the light stability of the device. In addition, the contained triazine and morpholine functional groups can coordinate with Pb²⁺, thereby reducing the interface defects and inhibiting the non-radiative recombination. The HASS-modulated PSC could reach the champion PCE of 26.74% (certified 26.56%), which is remarkable for inverted PSCs prepared under ambient conditions. Further, the unencapsulated device could maintain 95.4% of its initial PCE after more than 1000 h of aging at maximum power point tracking.

尽管钙钛矿太阳能电池（PSCs）在提高功率转换效率（PCE）超过27%方面取得了重大进展，但PSCs在照明下的工作稳定性不足仍然是一个关键挑战，对其商业可行性构成了主要障碍。本文提出了一种可行的受阻胺稳定策略（HASS），利用受阻胺光稳定剂对钙钛矿的晶粒和表面进行调制，从而阻断钙钛矿的内部和外部降解途径。其哌啶环在有氧环境中吸收光能后容易氧化形成一氧化氮（N-O•）自由基。在钙钛矿的分解产物中，游离超氧自由基（O2·−）与钙钛矿和H+发生反应，从而提高了器件的光稳定性。此外，所含的三嗪和啉官能团可以与Pb2+配位，从而减少了界面缺陷，抑制了非辐射复合。hass调制的PSC的PCE最高可达26.74%（经认证为26.56%），这对于在环境条件下制备的倒装PSC来说是非常显著的。此外，在最大功率点跟踪超过1000小时的老化后，未封装的器件可以保持其初始PCE的95.4%。

{"title":"Chemical inhibition of light-induced decomposition by hindered amine for efficient and stable perovskite solar cells","authors":"Yuqing Su , Jike Ding , Zuolin Zhang , Mengjia Li , Jiangzhao Chen , Jian-Xin Tang , Thierry Pauporté , Cong Chen","doi":"10.1016/j.esci.2025.100451","DOIUrl":"10.1016/j.esci.2025.100451","url":null,"abstract":"<div><div>Despite significant advancements in improving the power-conversion efficiency (PCE) of exceeding 27% in perovskite solar cells (PSCs), the insufficient operational stability of PSCs under illumination remains a critical challenge, posing a major obstacle to their commercial viability. This paper proposes a feasible hindered amine stabilization strategy (HASS) by using a hindered amine light stabilizer for grain and surface modulation of perovskite, thereby blocking the internal and external degradation pathways of perovskite. Its piperidine ring is easily oxidized to form Nitrogen monoxide (N–O•) radicals after absorbing light energy in an aerobic environment. The free superoxide radical (<span><math><mrow><msubsup><mi>O</mi><mn>2</mn><mrow><mo>·</mo><mo>−</mo></mrow></msubsup></mrow></math></span>) radicals react with perovskite and H<sup>+</sup> in the decomposition products of perovskite, thereby improving the light stability of the device. In addition, the contained triazine and morpholine functional groups can coordinate with Pb<sup>2+</sup>, thereby reducing the interface defects and inhibiting the non-radiative recombination. The HASS-modulated PSC could reach the champion PCE of 26.74% (certified 26.56%), which is remarkable for inverted PSCs prepared under ambient conditions. Further, the unencapsulated device could maintain 95.4% of its initial PCE after more than 1000 h of aging at maximum power point tracking.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"6 1","pages":"Article 100451"},"PeriodicalIF":36.6,"publicationDate":"2025-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145842607","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0