首页 > 最新文献

Advanced Energy Materials最新文献

英文 中文
How Halide Segregation Governs the Ion Density Evolution and Ionic Performance Losses: From Degradation to Recovery 卤化物偏析如何控制离子密度演变和离子性能损失:从降解到恢复
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-05 DOI: 10.1002/aenm.202503866
Nikhil Kalasariya, Paria Forozi Sowmeeh, Francisco Pena‐Camargo, Francesco Vanin, Tino Lukas, Yuxin Dong, Qifan Feng, Ziwei Liu, Waqar Ali Memon, Danpeng Gao, Jianqiu Gong, Xin Wu, Andres Felipe Castro Mendez, Jan Hagenberg, Zahra Abadi, Thomas Hultzsch, Xinyi Zhao, Sahil Shah, Hui Yu, Varun Srivastava, Jianbin Xu, Ni Zhao, Felix Lang, Zonglong Zhu, Martin Stolterfoht
Halide segregation (HS) is considered to be one of the most significant hurdles for the commercialization of tandem solar cells. However, despite significant research on this matter, the exact impact of HS on the performance degradation and the ion density evolution is yet to be established. In this work, we investigate the intriguing correlation between HS, ion‐induced efficiency losses, and ion density evolution in wide‐bandgap (WBG) triple cation perovskite cells. Our results highlight that all three phenomena evolve on similar timescales and follow the same trend across all studied bandgaps. This implies that the poor energy‐lifetime product observed for devices prone to halide segregation is a result of enhanced ionic losses rather than, for instance, charge carrier funneling. Furthermore, reminiscent of the recovery of HS observed previously, we demonstrate that ionic losses also recover after light exposure and dark storage, which occurs along with a receding ion density. However, we also observe irreversible ionic losses, especially after prolonged illumination, which are critical for device operation. These findings present an important new understanding of the interplay between halide segregation and ionic processes and provide a rational explanation for the performance and stability of mixed halide WBG perovskites.
卤化物分离(HS)被认为是串联太阳能电池商业化的最大障碍之一。然而,尽管对这一问题进行了大量研究,但HS对性能下降和离子密度演变的确切影响尚未确定。在这项工作中,我们研究了宽带隙(WBG)三阳离子钙钛矿电池中HS、离子诱导效率损失和离子密度演变之间的有趣相关性。我们的研究结果强调,这三种现象在相似的时间尺度上演变,并在所有研究的带隙中遵循相同的趋势。这意味着,对于易于发生卤化物偏析的器件,观察到的较差的能量寿命产物是离子损失增强的结果,而不是电荷载流子漏斗的结果。此外,与之前观察到的HS恢复类似,我们证明了离子损失在光暴露和暗储存后也会恢复,这伴随着离子密度的下降而发生。然而,我们也观察到不可逆的离子损失,特别是在长时间照明后,这对设备操作至关重要。这些发现为卤化物偏析与离子过程之间的相互作用提供了重要的新认识,并为混合卤化物WBG钙钛矿的性能和稳定性提供了合理的解释。
{"title":"How Halide Segregation Governs the Ion Density Evolution and Ionic Performance Losses: From Degradation to Recovery","authors":"Nikhil Kalasariya, Paria Forozi Sowmeeh, Francisco Pena‐Camargo, Francesco Vanin, Tino Lukas, Yuxin Dong, Qifan Feng, Ziwei Liu, Waqar Ali Memon, Danpeng Gao, Jianqiu Gong, Xin Wu, Andres Felipe Castro Mendez, Jan Hagenberg, Zahra Abadi, Thomas Hultzsch, Xinyi Zhao, Sahil Shah, Hui Yu, Varun Srivastava, Jianbin Xu, Ni Zhao, Felix Lang, Zonglong Zhu, Martin Stolterfoht","doi":"10.1002/aenm.202503866","DOIUrl":"https://doi.org/10.1002/aenm.202503866","url":null,"abstract":"Halide segregation (HS) is considered to be one of the most significant hurdles for the commercialization of tandem solar cells. However, despite significant research on this matter, the exact impact of HS on the performance degradation and the ion density evolution is yet to be established. In this work, we investigate the intriguing correlation between HS, ion‐induced efficiency losses, and ion density evolution in wide‐bandgap (WBG) triple cation perovskite cells. Our results highlight that all three phenomena evolve on similar timescales and follow the same trend across all studied bandgaps. This implies that the poor energy‐lifetime product observed for devices prone to halide segregation is a result of enhanced ionic losses rather than, for instance, charge carrier funneling. Furthermore, reminiscent of the recovery of HS observed previously, we demonstrate that ionic losses also recover after light exposure and dark storage, which occurs along with a receding ion density. However, we also observe irreversible ionic losses, especially after prolonged illumination, which are critical for device operation. These findings present an important new understanding of the interplay between halide segregation and ionic processes and provide a rational explanation for the performance and stability of mixed halide WBG perovskites.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"15 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122286","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Effects of Mechanical Properties of Elastomeric Electrolytes for Stable Operation of Lithium Metal Batteries (Adv. Energy Mater. 5/2026) 弹性电解质力学性能对锂金属电池稳定运行的影响(能源材料,5/2026)
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-04 DOI: 10.1002/aenm.70512
Dongkyu Lee, Dongguk Kang, Chanho Yuk, Hyeri Kang, Eunji Lee, Wonho Lee, Jinseok Park, Bumjoon J. Kim
{"title":"Effects of Mechanical Properties of Elastomeric Electrolytes for Stable Operation of Lithium Metal Batteries (Adv. Energy Mater. 5/2026)","authors":"Dongkyu Lee, Dongguk Kang, Chanho Yuk, Hyeri Kang, Eunji Lee, Wonho Lee, Jinseok Park, Bumjoon J. Kim","doi":"10.1002/aenm.70512","DOIUrl":"https://doi.org/10.1002/aenm.70512","url":null,"abstract":"","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"89 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122287","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Boron Carbide Supported Ultra-Small Ruthenium Nanoparticles with High-Performance for Hydrogen and Chlor-Alkali Co-Production 碳化硼负载的高性能超小钌纳米颗粒用于氢氯碱联产
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-04 DOI: 10.1002/aenm.202506175
Abdulwahab Salah, Hong-Da Ren, Feiyang Yu, Nabilah Al-Ansi, Zhongling Lang, Yangguang Li, Yonghui Wang, Huaqiao Tan
Ruthenium (Ru) is a promising electrocatalyst for hydrogen and chlor-alkali co-production, but suffers from poor water adsorption and hydrogen desorption. To enhance its hydrogen evolution reaction (HER) performance, this study employs density functional theory (DFT) to explore how non-metallic supports (B, C, N) modulate the electronic structure of Ru via metal-support interactions (MSIs). Results reveal B4C as the optimal support, with 1.56 electrons transferred from Ru13 to B4C, shifting the Ru d-band center closer to the Fermi level and synergistically optimizing the adsorption of HER intermediates. The synthesized N-doped carbon-coated Ru/B4C catalyst (Ru/B4C@NC) exhibits outstanding alkaline HER activity, achieving overpotentials of only 5 mV at 10 mA cm−2 and 361 mV at 1 A cm−2, along with stability over 500 h. Under chlor-alkali conditions, Ru/B4C@NC also maintains high HER activity with overpotentials of 5 and 99 mV at 10 and 500 mA cm−2 and long-term stability for 300 h. A hybrid electrolysis cell with Ru/B4C@NC (−) //RuO2/IrO2-coated Ti mesh (+) achieves a record low voltage of 2.33 V at 10 mA cm−2 with long-term stability for 100 h. This work provides valuable insights for designing advanced Ru-based catalysts for integrated hydrogen and chlor-alkali production.
钌(Ru)是一种很有前途的氢氯碱联产电催化剂,但其吸水性和解吸氢性能较差。为了提高Ru的析氢反应(HER)性能,本研究采用密度泛函理论(DFT)探讨了非金属载体(B, C, N)如何通过金属-载体相互作用(msi)调节Ru的电子结构。结果表明,B4C是最佳载体,有1.56个电子从Ru13转移到B4C,使Ru带中心更接近费米能级,协同优化了HER中间体的吸附。合成的n掺杂碳包覆Ru/B4C催化剂(Ru/B4C@NC)表现出出色的碱性HER活性,在10 mA cm−2时过电位仅为5 mV,在1 A cm−2时过电位仅为361 mV,并且在500 h内稳定。Ru/B4C@NC还保持了高HER活性,在10和500 mA cm - 2下的过电位为5和99 mV,长期稳定性为300小时。Ru/B4C@NC(−)//RuO2/ iro2涂层Ti网(+)的混合电解池在10 mA cm - 2下达到了创纪录的2.33 V的低电压,长期稳定性为100小时。这项工作为设计先进的Ru基催化剂提供了宝贵的见解。
{"title":"Boron Carbide Supported Ultra-Small Ruthenium Nanoparticles with High-Performance for Hydrogen and Chlor-Alkali Co-Production","authors":"Abdulwahab Salah, Hong-Da Ren, Feiyang Yu, Nabilah Al-Ansi, Zhongling Lang, Yangguang Li, Yonghui Wang, Huaqiao Tan","doi":"10.1002/aenm.202506175","DOIUrl":"https://doi.org/10.1002/aenm.202506175","url":null,"abstract":"Ruthenium (Ru) is a promising electrocatalyst for hydrogen and chlor-alkali co-production, but suffers from poor water adsorption and hydrogen desorption. To enhance its hydrogen evolution reaction (HER) performance, this study employs density functional theory (DFT) to explore how non-metallic supports (B, C, N) modulate the electronic structure of Ru via metal-support interactions (MSIs). Results reveal B<sub>4</sub>C as the optimal support, with 1.56 electrons transferred from Ru<sub>13</sub> to B<sub>4</sub>C, shifting the Ru d-band center closer to the Fermi level and synergistically optimizing the adsorption of HER intermediates. The synthesized N-doped carbon-coated Ru/B<sub>4</sub>C catalyst (Ru/B<sub>4</sub>C@NC) exhibits outstanding alkaline HER activity, achieving overpotentials of only 5 mV at 10 mA cm<sup>−2</sup> and 361 mV at 1 A cm<sup>−2</sup>, along with stability over 500 h. Under chlor-alkali conditions, Ru/B<sub>4</sub>C@NC also maintains high HER activity with overpotentials of 5 and 99 mV at 10 and 500 mA cm<sup>−2</sup> and long-term stability for 300 h. A hybrid electrolysis cell with Ru/B<sub>4</sub>C@NC (−) //RuO<sub>2</sub>/IrO<sub>2</sub>-coated Ti mesh (+) achieves a record low voltage of 2.33 V at 10 mA cm<sup>−2</sup> with long-term stability for 100 h. This work provides valuable insights for designing advanced Ru-based catalysts for integrated hydrogen and chlor-alkali production.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"90 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116205","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Molecular Engineering of Fluorinated Hybrid Gel Polymer Electrolytes Enables Ultra-Wide-Temperature Operation of High-Voltage Lithium Metal Batteries 氟化混合凝胶聚合物电解质的分子工程实现高压锂金属电池的超宽温度运行
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-04 DOI: 10.1002/aenm.202506074
Zhenxiang Zhu, Xianbin Wu, Hong Xu, Dayao Zhang, Zhen Geng, Cunman Zhang, Stefano Passerini, Mingzhe Xue
The development of wide-temperature gel polymer electrolytes (GPEs) represents a promising strategy for enhancing the extreme environment tolerance of lithium-metal batteries (LMBs), which requires simultaneously optimizing Li+ transport kinetics at low temperatures and maintaining the thermal and mechanical stability. This work addresses the intrinsic limitations of conventional GPEs by employing a molecular engineering strategy that achieves molecular-scale hybridization of organic and inorganic units. Specifically, a fluorinated hybrid gel polymer electrolyte (FHPE) is fabricated through the in situ crosslinking polymerization of trifluoroethyl acrylate (TFEA) and acryloxypropyl polyhedral oligomeric silsesquioxane (Acry-POSS) within 2,2-difluoroethyl acetate (DFEA). The FHPE displays high Li+ conductivity (3.54 × 10−4 S cm−1 at −30°C), broad electrochemical stability window (>4.7 V), and remarkable mechanical strength (58.7 MPa). Moreover, the FHPE promotes the formation of LiF-rich interphases on the LiCoO2 cathode and lithium metal anode, thereby effectively mitigating dendrite growth and interfacial side reactions. Consequently, FHPE-based Li/Li coin cells stably cycle for 1500 h at 0.3 mA cm−2 and −30°C, while Li/LiCoO2 coin cells exhibit 86.7% capacity retention after 200 cycles at −30°C and 77.9% after 400 cycles at 60°C. Furthermore, Li/FHPE/LiCoO2 pouch cells exhibit stable operation during nail penetration tests, thereby confirming their exceptional safety.
宽温度凝胶聚合物电解质(gpe)的开发是提高锂金属电池(lmb)极端环境耐受性的一种有前景的策略,这需要同时优化Li+在低温下的传输动力学,并保持热稳定性和机械稳定性。这项工作通过采用分子工程策略实现有机和无机单元的分子尺度杂交,解决了传统gpe的内在局限性。具体而言,通过在2,2-二氟乙酸乙酯(DFEA)中原位交联聚合三氟丙烯酸乙酯(TFEA)和丙烯氧丙基多面体低聚硅氧烷(acy - poss)制备了氟化杂化凝胶聚合物电解质(FHPE)。FHPE具有较高的Li+电导率(- 30°C时为3.54 × 10−4 S cm−1)、较宽的电化学稳定窗口(>4.7 V)和显著的机械强度(58.7 MPa)。此外,FHPE促进了LiCoO2阴极和锂金属阳极上富liff界面相的形成,从而有效地减缓了枝晶生长和界面副反应。因此,基于fhpe的Li/Li硬币电池在0.3 mA cm - 2和- 30°C下稳定循环1500 h,而Li/LiCoO2硬币电池在- 30°C下循环200次后容量保持率为86.7%,在60°C下循环400次后容量保持率为77.9%。此外,Li/FHPE/LiCoO2袋状电池在指甲穿透测试中表现出稳定的运行,从而证实了它们卓越的安全性。
{"title":"Molecular Engineering of Fluorinated Hybrid Gel Polymer Electrolytes Enables Ultra-Wide-Temperature Operation of High-Voltage Lithium Metal Batteries","authors":"Zhenxiang Zhu, Xianbin Wu, Hong Xu, Dayao Zhang, Zhen Geng, Cunman Zhang, Stefano Passerini, Mingzhe Xue","doi":"10.1002/aenm.202506074","DOIUrl":"https://doi.org/10.1002/aenm.202506074","url":null,"abstract":"The development of wide-temperature gel polymer electrolytes (GPEs) represents a promising strategy for enhancing the extreme environment tolerance of lithium-metal batteries (LMBs), which requires simultaneously optimizing Li<sup>+</sup> transport kinetics at low temperatures and maintaining the thermal and mechanical stability. This work addresses the intrinsic limitations of conventional GPEs by employing a molecular engineering strategy that achieves molecular-scale hybridization of organic and inorganic units. Specifically, a fluorinated hybrid gel polymer electrolyte (FHPE) is fabricated through the in situ crosslinking polymerization of trifluoroethyl acrylate (TFEA) and acryloxypropyl polyhedral oligomeric silsesquioxane (Acry-POSS) within 2,2-difluoroethyl acetate (DFEA). The FHPE displays high Li<sup>+</sup> conductivity (3.54 × 10<sup>−4</sup> S cm<sup>−1</sup> at −30°C), broad electrochemical stability window (&gt;4.7 V), and remarkable mechanical strength (58.7 MPa). Moreover, the FHPE promotes the formation of LiF-rich interphases on the LiCoO<sub>2</sub> cathode and lithium metal anode, thereby effectively mitigating dendrite growth and interfacial side reactions. Consequently, FHPE-based Li/Li coin cells stably cycle for 1500 h at 0.3 mA cm<sup>−2</sup> and −30°C, while Li/LiCoO<sub>2</sub> coin cells exhibit 86.7% capacity retention after 200 cycles at −30°C and 77.9% after 400 cycles at 60°C. Furthermore, Li/FHPE/LiCoO<sub>2</sub> pouch cells exhibit stable operation during nail penetration tests, thereby confirming their exceptional safety.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"58 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122278","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Investigation of the Lithium Extraction Mechanism from LiNi0.6Mn0.2Co0.2O2 by Using Operando Neutron Diffraction in an All-Solid-State Battery 用全固态电池中Operando中子衍射研究LiNi0.6Mn0.2Co0.2O2萃取锂的机理
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-04 DOI: 10.1002/aenm.202506600
Sreelakshmi Anil Kumar, Dhanush Shanbhag, Ove Korjus, Prashanth Sivakumar, Laurence Croguennec, Christian Masquelier, Jean-Noël Chotard, Emmanuelle Suard
All-Solid-State Batteries (ASSBs) are promising emerging devices for meeting high-energy demands and an in-depth understanding of the reaction mechanisms occuring during their operation will help in their design for better performance. In this context, neutrons, with their high penetration depth and sensitivity to light elements such as lithium, provide a powerful tool for investigating the structural mechanisms occurring in bulk ASSBs, while the electrochemical operation of large batteries (required for neutron diffraction) remains a challenge. In this study, we demonstrate the reversible electrochemical Li+ extraction/insertion within a 2.5 mm thick ASSB system comprising 140 mg of LiNi0.6Mn0.2Co0.2O2 (NMC622) as the positive electrode material (238 mWh energy density), Li5.4PS4.4BrCl0.6 (LPSClBr) as the solid electrolyte and Li0.5In as the negative electrode. Thanks to the use of the newly-designed ILLBAT#5 electrochemical cell, we were able to perform operando neutron powder diffraction (NPD) of the system, which coupled with ex situ diffraction, allowed us to gain valuable insights into the structural evolution of NMC622 within the ASSB as well as to probe the structural stability of the Argyrodite solid electrolyte throughout the initial cycle. Herein, we report on the formation and the co-existence of H1-H2 phases in NMC622, attributed to system inhomogeneity.
全固态电池(assb)是满足高能量需求的新兴设备,深入了解其运行过程中发生的反应机制将有助于设计出更好的性能。在这种情况下,中子具有高穿透深度和对锂等轻元素的敏感性,为研究大块assb中发生的结构机制提供了有力的工具,而大型电池的电化学操作(中子衍射所需)仍然是一个挑战。在这项研究中,我们展示了在2.5 mm厚的ASSB系统中可逆的电化学Li+提取/插入,该系统由140 mg LiNi0.6Mn0.2Co0.2O2 (NMC622)作为正极材料(238 mWh能量密度),Li5.4PS4.4BrCl0.6 (LPSClBr)作为固体电解质,Li0.5In作为负极。由于使用了新设计的ILLBAT#5电化学电池,我们能够对该系统进行operando中子粉末衍射(NPD),再加上非原位衍射,使我们能够获得有关NMC622在ASSB内的结构演变的宝贵见解,并在整个初始循环中探测Argyrodite固体电解质的结构稳定性。本文报道了NMC622中由于体系不均匀性导致的H1-H2相的形成和共存。
{"title":"Investigation of the Lithium Extraction Mechanism from LiNi0.6Mn0.2Co0.2O2 by Using Operando Neutron Diffraction in an All-Solid-State Battery","authors":"Sreelakshmi Anil Kumar, Dhanush Shanbhag, Ove Korjus, Prashanth Sivakumar, Laurence Croguennec, Christian Masquelier, Jean-Noël Chotard, Emmanuelle Suard","doi":"10.1002/aenm.202506600","DOIUrl":"https://doi.org/10.1002/aenm.202506600","url":null,"abstract":"All-Solid-State Batteries (ASSBs) are promising emerging devices for meeting high-energy demands and an in-depth understanding of the reaction mechanisms occuring during their operation will help in their design for better performance. In this context, neutrons, with their high penetration depth and sensitivity to light elements such as lithium, provide a powerful tool for investigating the structural mechanisms occurring in bulk ASSBs, while the electrochemical operation of large batteries (required for neutron diffraction) remains a challenge. In this study, we demonstrate the reversible electrochemical Li<sup>+</sup> extraction/insertion within a 2.5 mm thick ASSB system comprising 140 mg of LiNi<sub>0.6</sub>Mn<sub>0.2</sub>Co<sub>0.2</sub>O<sub>2</sub> (NMC622) as the positive electrode material (238 mWh energy density), Li<sub>5.4</sub>PS<sub>4.4</sub>BrCl<sub>0.6</sub> (LPSClBr) as the solid electrolyte and Li<sub>0.5</sub>In as the negative electrode. Thanks to the use of the newly-designed ILLBAT#5 electrochemical cell, we were able to perform <i>operando</i> neutron powder diffraction (NPD) of the system, which coupled with ex situ diffraction, allowed us to gain valuable insights into the structural evolution of NMC622 within the ASSB as well as to probe the structural stability of the Argyrodite solid electrolyte throughout the initial cycle. Herein, we report on the formation and the co-existence of H1-H2 phases in NMC622, attributed to system inhomogeneity.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"235 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116207","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Interfacial Microenvironmental Engineering for Acidic CO2 Electroreduction in Proton Exchange Membrane Electrolyzers 质子交换膜电解槽酸性CO2电还原界面微环境工程
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-03 DOI: 10.1002/aenm.202506790
Shengjie Bai, Xufei Gu, Jianxin Dong, Jirui Yang, Wenyu Zheng, Cong Guo, Ya Liu, TingTing Kong, Shaohua Shen
Electrochemical CO2 reduction reaction (CO2RR) in proton exchange membrane electrolyzers offers a pathway to close the carbon cycle and produce sustainable fuels and chemicals at industrial-scale current densities. Acidic operation enables compact reactor architectures and superior single-pass carbon utilization, yet faces persistent challenges including parasitic hydrogen evolution, catalyst corrosion and deactivation, along with constrained local CO2 transport. This review highlights recent progress in interfacial microenvironmental engineering that reconcile acidic operation with selective and durable CO2 conversion. We organize strategies across four critical interfaces: (1) the gas diffusion layer-catalyst layer interface, where engineered hydrophobicity and pore structure promote CO2 delivery while maintaining a stable three-phase boundary; (2) the catalyst-electrolyte electric double layer interface, where control over interfacial fields, pH gradients, and adsorbate binding energetics suppresses the hydrogen evolution reaction while promoting CO2RR selectivity; (3) at the catalyst layer-membrane interface, where optimized ionomer distribution and tailored proton conductivity balance local proton availability, mitigating catalyst degradation; and (4) the integrated membrane-electrode assembly, where harmonized ion transport, CO2 flux, and electron conduction stabilizes the microenvironment for long-term durability. By consolidating mechanistic insights and practical design principles, this review provides a roadmap for rational interfacial engineering to realize efficient, durable, and scalable acidic CO2 electroreduction in PEM electrolyzers.
质子交换膜电解槽中的电化学CO2还原反应(CO2RR)为关闭碳循环和在工业规模电流密度下生产可持续燃料和化学品提供了一条途径。酸性操作可以实现紧凑的反应器结构和卓越的单道碳利用率,但也面临着持续的挑战,包括寄生析氢、催化剂腐蚀和失活,以及局部二氧化碳运输受限。本文综述了界面微环境工程的最新进展,将酸性操作与选择性和持久的CO2转化相结合。我们在四个关键界面上组织策略:(1)气体扩散层-催化剂层界面,其中工程疏水性和孔隙结构促进CO2传递,同时保持稳定的三相边界;(2)催化剂-电解质双电层界面,控制界面场、pH梯度和吸附质结合能抑制析氢反应,同时促进CO2RR选择性;(3)在催化剂层-膜界面,优化的离聚体分布和定制的质子电导率平衡了局部质子可用性,减轻了催化剂的降解;(4)集成膜电极组件,其中离子传输、二氧化碳通量和电子传导协调一致,稳定了微环境的长期耐用性。通过巩固机理认识和实际设计原则,本综述为合理的界面工程提供了路线图,以实现PEM电解槽中高效、耐用和可扩展的酸性CO2电还原。
{"title":"Interfacial Microenvironmental Engineering for Acidic CO2 Electroreduction in Proton Exchange Membrane Electrolyzers","authors":"Shengjie Bai, Xufei Gu, Jianxin Dong, Jirui Yang, Wenyu Zheng, Cong Guo, Ya Liu, TingTing Kong, Shaohua Shen","doi":"10.1002/aenm.202506790","DOIUrl":"https://doi.org/10.1002/aenm.202506790","url":null,"abstract":"Electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) in proton exchange membrane electrolyzers offers a pathway to close the carbon cycle and produce sustainable fuels and chemicals at industrial-scale current densities. Acidic operation enables compact reactor architectures and superior single-pass carbon utilization, yet faces persistent challenges including parasitic hydrogen evolution, catalyst corrosion and deactivation, along with constrained local CO<sub>2</sub> transport. This review highlights recent progress in interfacial microenvironmental engineering that reconcile acidic operation with selective and durable CO<sub>2</sub> conversion. We organize strategies across four critical interfaces: (1) the gas diffusion layer-catalyst layer interface, where engineered hydrophobicity and pore structure promote CO<sub>2</sub> delivery while maintaining a stable three-phase boundary; (2) the catalyst-electrolyte electric double layer interface, where control over interfacial fields, pH gradients, and adsorbate binding energetics suppresses the hydrogen evolution reaction while promoting CO<sub>2</sub>RR selectivity; (3) at the catalyst layer-membrane interface, where optimized ionomer distribution and tailored proton conductivity balance local proton availability, mitigating catalyst degradation; and (4) the integrated membrane-electrode assembly, where harmonized ion transport, CO<sub>2</sub> flux, and electron conduction stabilizes the microenvironment for long-term durability. By consolidating mechanistic insights and practical design principles, this review provides a roadmap for rational interfacial engineering to realize efficient, durable, and scalable acidic CO<sub>2</sub> electroreduction in PEM electrolyzers.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"87 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146102037","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Stability of Perovskite Indoor Photovoltaics: A Focused Review and a Call for Standardized Stability Reporting 钙钛矿室内光伏的稳定性:重点综述和对标准化稳定性报告的呼吁
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-03 DOI: 10.1002/aenm.202506091
Ivy Mawusi Asuo, Arezo Mahdavi Varposhti, Cyril Chu Fubin Kumachang, Gopal Krishnamurthy Grandhi, Vincenzo Pecunia, Thomas Meredith Brown, Paola Vivo, Nutifafa Yao Doumon
Metal halide perovskite indoor photovoltaics (IPVs) are the top contenders in terms of efficiency among emerging IPV technologies. The state-of-the-art perovskite IPVs have already achieved reported efficiencies above 44%, indicating their significant potential. However, only a small percentage of reports discuss stability measurements, with approximately 7% adopting the International Summit on Organic PV Stability (ISOS) protocol for stability evaluation. A standard for the stability assessment of emerging thin film IPVs still lags. This research area remains largely unexplored, yet it is essential to the commercialization of IPV technologies. This review focuses on perovskite-based IPVs, with an emphasis on device stability. It provides discussions of the origins of degradation in perovskite materials and their corresponding IPV devices. This is followed by an overview of various structure–property–stability strategies, including compositional, interface, and device design engineering for perovskite materials to improve their performance. Finally, the review outlines some existing stability test protocols that could apply to perovskite IPVs, including addressing mitigation issues, such as encapsulation, draws the attention of researchers in the field, and calls for the development of standardized stability test protocols for perovskite IPVs and for understanding how these tests correlate with actual indoor lifespans to enable the commercialization of perovskite IPVs.
金属卤化物钙钛矿室内光伏(IPVs)是新兴IPV技术中效率最高的竞争者。据报道,最先进的钙钛矿IPVs的效率已经达到44%以上,这表明它们具有巨大的潜力。然而,只有一小部分报告讨论了稳定性测量,大约7%的报告采用了国际有机光伏稳定性峰会(ISOS)协议进行稳定性评估。新兴薄膜IPVs的稳定性评价标准仍然滞后。这一研究领域在很大程度上仍未被探索,但它对IPV技术的商业化至关重要。本文综述了基于钙钛矿的IPVs,重点是器件稳定性。它提供了钙钛矿材料及其相应的IPV器件降解的起源的讨论。随后概述了各种结构-性能-稳定性策略,包括钙钛矿材料的成分,界面和器件设计工程,以提高其性能。最后,综述概述了一些适用于钙钛矿IPVs的现有稳定性测试协议,包括解决封装等缓解问题,引起了该领域研究人员的注意,并呼吁制定钙钛矿IPVs的标准化稳定性测试协议,并了解这些测试如何与实际室内寿命相关联,以实现钙钛矿IPVs的商业化。
{"title":"Stability of Perovskite Indoor Photovoltaics: A Focused Review and a Call for Standardized Stability Reporting","authors":"Ivy Mawusi Asuo, Arezo Mahdavi Varposhti, Cyril Chu Fubin Kumachang, Gopal Krishnamurthy Grandhi, Vincenzo Pecunia, Thomas Meredith Brown, Paola Vivo, Nutifafa Yao Doumon","doi":"10.1002/aenm.202506091","DOIUrl":"https://doi.org/10.1002/aenm.202506091","url":null,"abstract":"Metal halide perovskite indoor photovoltaics (IPVs) are the top contenders in terms of efficiency among emerging IPV technologies. The state-of-the-art perovskite IPVs have already achieved reported efficiencies above 44%, indicating their significant potential. However, only a small percentage of reports discuss stability measurements, with approximately 7% adopting the International Summit on Organic PV Stability (ISOS) protocol for stability evaluation. A standard for the stability assessment of emerging thin film IPVs still lags. This research area remains largely unexplored, yet it is essential to the commercialization of IPV technologies. This review focuses on perovskite-based IPVs, with an emphasis on device stability. It provides discussions of the origins of degradation in perovskite materials and their corresponding IPV devices. This is followed by an overview of various structure–property–stability strategies, including compositional, interface, and device design engineering for perovskite materials to improve their performance. Finally, the review outlines some existing stability test protocols that could apply to perovskite IPVs, including addressing mitigation issues, such as encapsulation, draws the attention of researchers in the field, and calls for the development of standardized stability test protocols for perovskite IPVs and for understanding how these tests correlate with actual indoor lifespans to enable the commercialization of perovskite IPVs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"21 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116066","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Thermal Stability Assessment of Sodium Solid Electrolytes 钠固体电解质的热稳定性评价
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-02 DOI: 10.1002/aenm.202506749
Bowen Wang, Yang Yang, Qianhe Xu, Xubin Wang, Lihao Tang, Xueyan Cui, Hongyue Cui, Han Tang, Hong Li, Yong-Sheng Hu, Yaxiang Lu
All-solid-state batteries (ASSBs) are widely regarded as promising nextgeneration energy storage systems due to their high energy density and enhanced safety. Na-based ASSBs, in particular, offer compelling advantages through the use of earth-abundant and low-cost materials. However, a critical knowledge gap remains regarding the thermal stability of sodium solid electrolytes (SEs)—especially their reactivity with electrode materials—hindering reliable safety assessment. Herein, we present a systematic comparison of the thermal behavior of six representative sodium SEs: Na3Zr2Si2PO12, Na3PS4, NaAlCl4, Na2ZrCl6, NaAlCl2.5O0.75, and PEO. While inorganic SEs demonstrate good intrinsic thermal stability, most exhibit significant exothermic reactions with cathode or anode materials upon heating, releasing considerable heat that could trigger thermal runaway. Notably, chloride-based SEs show markedly different reactivities—NaAlCl4 reacts violently with Na15Sn4, whereas Na2ZrCl6 remains remarkably stable, highlighting the crucial role of reaction kinetics and melting point in modulating thermal stability. The findings reveal that electrode–electrolyte compatibility under thermal stress—not just the stability of the SE alone—is a decisive factor for ASSB safety. Our work underscores the critical role of electrode-electrolyte thermal stability, offering new insights into the safety design of all-solid-state batteries.
全固态电池(assb)由于其高能量密度和增强的安全性而被广泛认为是有前途的下一代储能系统。特别是基于na的assb,通过使用地球资源丰富和低成本的材料,提供了令人信服的优势。然而,关于钠固体电解质(SEs)的热稳定性,特别是它们与电极材料的反应性,仍然存在一个关键的知识空白,这阻碍了可靠的安全性评估。本文系统比较了Na3Zr2Si2PO12、Na3PS4、NaAlCl4、Na2ZrCl6、NaAlCl2.5O0.75和PEO这六种具有代表性的se钠的热行为。虽然无机se具有良好的固有热稳定性,但大多数在加热时与阴极或阳极材料发生显著的放热反应,释放出大量的热量,可能引发热失控。值得注意的是,基于氯化物的se表现出明显不同的反应活性——naalcl4与Na15Sn4发生剧烈反应,而Na2ZrCl6保持非常稳定,这突出了反应动力学和熔点在调节热稳定性方面的关键作用。研究结果表明,在热应力下电极-电解质的相容性(而不仅仅是SE的稳定性)是ASSB安全性的决定性因素。我们的工作强调了电极-电解质热稳定性的关键作用,为全固态电池的安全设计提供了新的见解。
{"title":"Thermal Stability Assessment of Sodium Solid Electrolytes","authors":"Bowen Wang, Yang Yang, Qianhe Xu, Xubin Wang, Lihao Tang, Xueyan Cui, Hongyue Cui, Han Tang, Hong Li, Yong-Sheng Hu, Yaxiang Lu","doi":"10.1002/aenm.202506749","DOIUrl":"https://doi.org/10.1002/aenm.202506749","url":null,"abstract":"All-solid-state batteries (ASSBs) are widely regarded as promising nextgeneration energy storage systems due to their high energy density and enhanced safety. Na-based ASSBs, in particular, offer compelling advantages through the use of earth-abundant and low-cost materials. However, a critical knowledge gap remains regarding the thermal stability of sodium solid electrolytes (SEs)—especially their reactivity with electrode materials—hindering reliable safety assessment. Herein, we present a systematic comparison of the thermal behavior of six representative sodium SEs: Na<sub>3</sub>Zr<sub>2</sub>Si<sub>2</sub>PO<sub>12</sub>, Na<sub>3</sub>PS<sub>4</sub>, NaAlCl<sub>4</sub>, Na<sub>2</sub>ZrCl<sub>6</sub>, NaAlCl<sub>2.5</sub>O<sub>0.75,</sub> and PEO. While inorganic SEs demonstrate good intrinsic thermal stability, most exhibit significant exothermic reactions with cathode or anode materials upon heating, releasing considerable heat that could trigger thermal runaway. Notably, chloride-based SEs show markedly different reactivities—NaAlCl<sub>4</sub> reacts violently with Na<sub>15</sub>Sn<sub>4</sub>, whereas Na<sub>2</sub>ZrCl<sub>6</sub> remains remarkably stable, highlighting the crucial role of reaction kinetics and melting point in modulating thermal stability. The findings reveal that electrode–electrolyte compatibility under thermal stress—not just the stability of the SE alone—is a decisive factor for ASSB safety. Our work underscores the critical role of electrode-electrolyte thermal stability, offering new insights into the safety design of all-solid-state batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"58 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146102038","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Unraveling Failure Mechanism of Indium Anodes in all-Solid-State Batteries 全固态电池中铟阳极的分解失效机理
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-02 DOI: 10.1002/aenm.202504932
Haoqi Ren, Xiaoting Lin, Jiamin Fu, Yipeng Sun, Xiaozhang Yao, Yingjie Gao, Bolin Fu, Weihan Li, Changhong Wang, Xueliang Sun
Alloy-based anodes, particularly indium (In) are emerging as promising candidates for achieving long-cycle life in all-solid-state lithium batteries (ASSLBs), due to their dendrite-free characteristics and ability to stabilize the anode interface. However, their practical applications remain hindered by limitations in the failure of In anodes under high current densities and areal capacities, where the incomplete understanding of the underlying failure mechanism limits the optimization strategies. Herein, we employ advanced characterization techniques to systematically investigate the failure mechanisms of In anodes under high current densities and areal capacities. Our findings reveal that alloying and dealloying processes involve an electro-chemo-mechanical coupling failure mechanism and further exacerbate performance degradation. By elucidating these failure mechanisms, our work provides critical insights and rational surface protection strategies by ALD coating with Al2O3 layer for enhancing the interfacial stability and performance of alloy anodes in ASSLBs. The maximum cycling capacity of the Li/In asymmetric cell at 0.5 mA/cm2 was enhanced from 0.2 to 2 mAh/cm2 (>200 cycles). This work paves the way for the development of durable, high-energy-density batteries.
合金基阳极,特别是铟(In),由于其无枝晶的特性和稳定阳极界面的能力,正在成为实现全固态锂电池(ASSLBs)长循环寿命的有希望的候选者。然而,它们的实际应用仍然受到高电流密度和面积容量下in阳极失效的限制,其中对潜在失效机制的不完全理解限制了优化策略。在此,我们采用先进的表征技术系统地研究了In阳极在高电流密度和面容量下的失效机制。我们的研究结果表明,合金化和脱合金化过程涉及电化学-机械耦合失效机制,并进一步加剧了性能退化。通过阐明这些失效机制,我们的工作为ALD涂层Al2O3层提供了重要的见解和合理的表面保护策略,以提高asslb中合金阳极的界面稳定性和性能。在0.5 mA/cm2下,Li/In非对称电池的最大循环容量从0.2 mAh/cm2提高到2 mAh/cm2 (>;200次循环)。这项工作为开发耐用、高能量密度的电池铺平了道路。
{"title":"Unraveling Failure Mechanism of Indium Anodes in all-Solid-State Batteries","authors":"Haoqi Ren, Xiaoting Lin, Jiamin Fu, Yipeng Sun, Xiaozhang Yao, Yingjie Gao, Bolin Fu, Weihan Li, Changhong Wang, Xueliang Sun","doi":"10.1002/aenm.202504932","DOIUrl":"https://doi.org/10.1002/aenm.202504932","url":null,"abstract":"Alloy-based anodes, particularly indium (In) are emerging as promising candidates for achieving long-cycle life in all-solid-state lithium batteries (ASSLBs), due to their dendrite-free characteristics and ability to stabilize the anode interface. However, their practical applications remain hindered by limitations in the failure of In anodes under high current densities and areal capacities, where the incomplete understanding of the underlying failure mechanism limits the optimization strategies. Herein, we employ advanced characterization techniques to systematically investigate the failure mechanisms of In anodes under high current densities and areal capacities. Our findings reveal that alloying and dealloying processes involve an electro-chemo-mechanical coupling failure mechanism and further exacerbate performance degradation. By elucidating these failure mechanisms, our work provides critical insights and rational surface protection strategies by ALD coating with Al<sub>2</sub>O<sub>3</sub> layer for enhancing the interfacial stability and performance of alloy anodes in ASSLBs. The maximum cycling capacity of the Li/In asymmetric cell at 0.5 mA/cm<sup>2</sup> was enhanced from 0.2 to 2 mAh/cm<sup>2</sup> (&gt;200 cycles). This work paves the way for the development of durable, high-energy-density batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"32 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146102039","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Deciphering Molecular Structural Effect on Redox-Mediated CO2 Reduction Reaction Mechanisms for Aprotic Li-CO2 Batteries 非质子锂-二氧化碳电池氧化还原介导的CO2还原反应机制的分子结构解析效应
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-02 DOI: 10.1002/aenm.202506608
Tianfeng Yao, Long Pang, Yuwei Su, Limin Guo, Erkang Wang, Zhangquan Peng, Zhiwei Zhao
Redox mediators (RMs) emerge as critical enablers for unlocking the energy potentials of aprotic Li-CO2 batteries through solution-mediated CO2 reduction reaction (CO2RR). However, the structural effect of RMs on CO2RR pathways and catalytic efficiency remains insufficiently understood. Herein, through a comparative investigation of model quinone (Q)-based RMs using in situ spectroscopic techniques coupled with theoretical calculations, it is revealed that reduced Q species chemically bind with CO2 to form metastable Lin(Q-xCO2) adducts (n, x = 1 or 2), which subsequently dissociate into LiCO2 intermediates and further generate Li2CO3 and CO as discharge product while regenerating LinQ (n = 0 or 1) for sustained redox cycling. The dissociation of Lin(Q-xCO2) adducts constitutes the rate-determining step under non-polarization conditions. The introduction of electron-withdrawing groups (EWGs) into the Q moiety can enhance discharge potentials, but creates a kinetic trade-off: increased dissociation kinetics of Lin(Q-xCO2) adducts and suppressed adduct formation due to diminished CO2 binding affinity for reduced Q species. Strategic electronic modulation via optimized EWG substitution balances this CO2 affinity and adducts dissociation equilibrium, achieving simultaneous improvements in discharge potential and capacity. Our work provides fundamental guidelines for the rational design of advanced RMs in next-generation Li-CO2 batteries.
氧化还原介质(RMs)是通过溶液介导的CO2还原反应(CO2RR)释放非质子锂-CO2电池能量潜力的关键促成因素。然而,RMs对CO2RR途径和催化效率的结构影响尚不清楚。本文利用原位光谱技术结合理论计算对模型醌(Q)基RMs进行了对比研究,发现还原后的Q与CO2化学结合形成亚稳的Lin(Q- xco2)加合物(n, x = 1或2),这些加合物随后解离成LiCO2中间体,并进一步生成Li2CO3和CO作为排放产物,同时再生LinQ (n = 0或1)进行持续的氧化还原循环。在非极化条件下,Lin(Q-xCO2)加合物的离解是速率决定步骤。在Q部分引入吸电子基团(ewg)可以增强放电电位,但会产生动力学上的权衡:由于CO2对还原Q的结合亲和力降低,增加了Lin(Q- xco2)加合物的解离动力学和抑制了加合物的形成。通过优化的EWG替代,战略性电子调制平衡了这种CO2亲和力和加合物解离平衡,同时实现了放电电位和容量的改善。我们的工作为下一代锂-二氧化碳电池的先进RMs的合理设计提供了基本指导。
{"title":"Deciphering Molecular Structural Effect on Redox-Mediated CO2 Reduction Reaction Mechanisms for Aprotic Li-CO2 Batteries","authors":"Tianfeng Yao, Long Pang, Yuwei Su, Limin Guo, Erkang Wang, Zhangquan Peng, Zhiwei Zhao","doi":"10.1002/aenm.202506608","DOIUrl":"https://doi.org/10.1002/aenm.202506608","url":null,"abstract":"Redox mediators (RMs) emerge as critical enablers for unlocking the energy potentials of aprotic Li-CO<sub>2</sub> batteries through solution-mediated CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR). However, the structural effect of RMs on CO<sub>2</sub>RR pathways and catalytic efficiency remains insufficiently understood. Herein, through a comparative investigation of model quinone (Q)-based RMs using in situ spectroscopic techniques coupled with theoretical calculations, it is revealed that reduced Q species chemically bind with CO<sub>2</sub> to form metastable Li<sub>n</sub>(Q-xCO<sub>2</sub>) adducts (n, x = 1 or 2), which subsequently dissociate into LiCO<sub>2</sub> intermediates and further generate Li<sub>2</sub>CO<sub>3</sub> and CO as discharge product while regenerating Li<sub>n</sub>Q (n = 0 or 1) for sustained redox cycling. The dissociation of Li<sub>n</sub>(Q-xCO<sub>2</sub>) adducts constitutes the rate-determining step under non-polarization conditions. The introduction of electron-withdrawing groups (EWGs) into the Q moiety can enhance discharge potentials, but creates a kinetic trade-off: increased dissociation kinetics of Li<sub>n</sub>(Q-xCO<sub>2</sub>) adducts and suppressed adduct formation due to diminished CO<sub>2</sub> binding affinity for reduced Q species. Strategic electronic modulation via optimized EWG substitution balances this CO<sub>2</sub> affinity and adducts dissociation equilibrium, achieving simultaneous improvements in discharge potential and capacity. Our work provides fundamental guidelines for the rational design of advanced RMs in next-generation Li-CO<sub>2</sub> batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"19 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116209","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
期刊
Advanced Energy Materials
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1