Potassium-ion batteries (PIBs) hold great promise as low-cost and sustainable alternatives to lithium-ion batteries, yet their practical deployment is hindered by rapid capacity decay driven by irreversible potassium loss and unstable solid electrolyte interphase (SEI). Here, we present a dual-effect pre-potassiation strategy that addresses both issues simultaneously. First, it is shown that the Prussian blue analogue K2Mn[Fe(CN)6] can be overpotassiated to KxMn[Fe(CN)6] (2+ into its large interstitial sites, accompanied by K+ off-centering and Mn(II)→Mn(I) reduction, while preserving structural integrity. Subsequently, an unconventional overdischarge strategy is proposed for the K2Mn[Fe(CN)6]-graphite PIBs, which enables in-situ formation of KxMn[Fe(CN)6] to compensate the SEI-related potassium losses while induces controlled electrolyte oxidation on graphite to produce a robust SEI with high stability. This dual mechanism significantly extends the cycling lifespan of the K2Mn[Fe(CN)6]-graphite cells from less than 100 cycles to more than 2000 cycles with high specific energy. This work pioneers a scalable and effective pre-potassiation approach to redefine the energy storage mechanism of Prussian blue analogues, advancing PIBs toward lithium-ion-level performance and offering a generalizable route for other alkali-ion batteries.
{"title":"Dual-Effect Pre-Potassiation Unlocks Stable and High-Energy Potassium-Ion Batteries","authors":"Nan Li, Yixiang He, Jiacheng Zhu, Xiaofang Wang, Yifan Chen, Yusi Yang, Linlin Wang, Xiaogang Niu, Xiao Ji, Xuefeng Wang, Qianfan Zhang, Yujie Zhu","doi":"10.1039/d5ee06846k","DOIUrl":"https://doi.org/10.1039/d5ee06846k","url":null,"abstract":"Potassium-ion batteries (PIBs) hold great promise as low-cost and sustainable alternatives to lithium-ion batteries, yet their practical deployment is hindered by rapid capacity decay driven by irreversible potassium loss and unstable solid electrolyte interphase (SEI). Here, we present a dual-effect pre-potassiation strategy that addresses both issues simultaneously. First, it is shown that the Prussian blue analogue K<small><sub>2</sub></small>Mn[Fe(CN)<small><sub>6</sub></small>] can be overpotassiated to K<small><sub>x</sub></small>Mn[Fe(CN)<small><sub>6</sub></small>] (2+ into its large interstitial sites, accompanied by K+ off-centering and Mn(II)→Mn(I) reduction, while preserving structural integrity. Subsequently, an unconventional overdischarge strategy is proposed for the K<small><sub>2</sub></small>Mn[Fe(CN)<small><sub>6</sub></small>]-graphite PIBs, which enables in-situ formation of K<small><sub>x</sub></small>Mn[Fe(CN)<small><sub>6</sub></small>] to compensate the SEI-related potassium losses while induces controlled electrolyte oxidation on graphite to produce a robust SEI with high stability. This dual mechanism significantly extends the cycling lifespan of the K<small><sub>2</sub></small>Mn[Fe(CN)<small><sub>6</sub></small>]-graphite cells from less than 100 cycles to more than 2000 cycles with high specific energy. This work pioneers a scalable and effective pre-potassiation approach to redefine the energy storage mechanism of Prussian blue analogues, advancing PIBs toward lithium-ion-level performance and offering a generalizable route for other alkali-ion batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"15 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507684","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}
Electric double-layer capacitors (EDLCs) with a high energy density for ultralow-temperature use are crucial for polar and space explorations, but hindered by the lack of suitable electrolytes and electrodes. We proposed a strong-weak interaction strategy to precisely regulate the solvation structure of an ionic liquid-based electrolyte that is stable from 25 to -80 °C.Then by using activated carbon with a mesopore-rich structure, we obtain an EDLC that can be used at -80 °C and 4.5 V, and has a record energy density of 104.5 Wh kg -1 with an 89.5% capacitance retention after 10,000 cycles. Furthermore, a 300 F pouch-type EDLC was assembled and it can operate stably from 25 to -80 °C, demonstrating the practical applicability. This study provides strategic guidance for constructing EDLCs with a high energy density for use under extreme conditions.
具有超低温高能量密度的双电层电容器（edlc）对于极地和太空探索至关重要，但由于缺乏合适的电解质和电极而受到阻碍。我们提出了一种强-弱相互作用策略来精确调节离子液体基电解质的溶剂化结构，该电解质在25至-80°C范围内稳定。然后，通过使用富中孔结构的活性炭，我们获得了可在-80°C和4.5 V下使用的EDLC，其记录能量密度为104.5 Wh kg -1，经过10,000次循环后电容保持率为89.5%。此外，还组装了一个300 F的袋式EDLC，在25 ~ -80°C范围内稳定工作，证明了它的实用性。该研究为构建在极端条件下使用的高能量密度edlc提供了战略指导。
{"title":"An Electric Double-layer Capacitor with High Performance at -80 °C","authors":"Haofeng Liu, Feng Zhou, Zekai Zhang, Haodong Wang, Hanqing Liu, Zhihao Ren, Endian Yang, Zhengdong Ma, Tongle Chen, Pratteek Das, Changde Ma, Ao Leng, shihao Liao, Xiong Zhang, Yabin An, Cheng Lian, Yanwei Ma, Hui-Ming Cheng, Zhong-Shuai Wu","doi":"10.1039/d5ee06850a","DOIUrl":"https://doi.org/10.1039/d5ee06850a","url":null,"abstract":"Electric double-layer capacitors (EDLCs) with a high energy density for ultralow-temperature use are crucial for polar and space explorations, but hindered by the lack of suitable electrolytes and electrodes. We proposed a strong-weak interaction strategy to precisely regulate the solvation structure of an ionic liquid-based electrolyte that is stable from 25 to -80 °C.Then by using activated carbon with a mesopore-rich structure, we obtain an EDLC that can be used at -80 °C and 4.5 V, and has a record energy density of 104.5 Wh kg -1 with an 89.5% capacitance retention after 10,000 cycles. Furthermore, a 300 F pouch-type EDLC was assembled and it can operate stably from 25 to -80 °C, demonstrating the practical applicability. This study provides strategic guidance for constructing EDLCs with a high energy density for use under extreme conditions.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"131 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507685","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}
It is widely known that semiconductor-based solar energy conversion could power our planet. This is in part because high-quality semiconductor structures are unrivalled in their ability to separate photogenerated electrons and holes. One effective approach to achieving this photoinduced charge separation relies on a phenomenon known as “band bending”. But details to justify why band bending results in photoinduced charge separation are more complex than often appreciated. This underappreciation is an impediment to the rational, hypothesis-driven design of next-generation approaches to solar energy conversion. Herein we show, by means of derivations rooted in physical chemistry, that several phenomena – not just band bending – can facilitate photoinduced charge separation, and that each is influenced by nonequilibrium species concentration and a parameter, such as diffusion coefficient or rate coefficient, that introduces dynamics. To help visualize the impact of each phenomenon, we introduce plots that depict their contributions as free energy, force, flux, force constant, and rate. We reveal that spatial dopant distributions that define band bending are predictors of initial photogenerated species transport rates. But charge separation alone does not guarantee high-efficiency operation. A photogenerated change in energy that is freely available to do useful work is also essential, and is strongly dependent on semiconductor optical properties and reaction kinetics. Notably, this information reveals that specificity of interfacial chemical reactions – even when they are not preceded by charge separation elsewhere – can result in efficient solar energy conversion. We expect that this tutorial will guide researchers in their pursuit to uncover new mechanisms for light to perform useful work.
{"title":"A fresh perspective on the role of band bending, and related contributors, in light-driven production of electricity and chemicals","authors":"Adam C. Nielander, Matthew R. Shaner, Shane Ardo","doi":"10.1039/d4ee05115g","DOIUrl":"https://doi.org/10.1039/d4ee05115g","url":null,"abstract":"It is widely known that semiconductor-based solar energy conversion could power our planet. This is in part because high-quality semiconductor structures are unrivalled in their ability to separate photogenerated electrons and holes. One effective approach to achieving this photoinduced charge separation relies on a phenomenon known as “<em>band bending</em>”. But details to justify why <em>band bending</em> results in photoinduced charge separation are more complex than often appreciated. This underappreciation is an impediment to the rational, hypothesis-driven design of next-generation approaches to solar energy conversion. Herein we show, by means of derivations rooted in physical chemistry, that several phenomena – not just <em>band bending</em> – can facilitate photoinduced charge separation, and that each is influenced by nonequilibrium species concentration and a parameter, such as diffusion coefficient or rate coefficient, that introduces dynamics. To help visualize the impact of each phenomenon, we introduce plots that depict their contributions as free energy, force, flux, force constant, and rate. We reveal that spatial dopant distributions that define <em>band bending</em> are predictors of initial photogenerated species transport rates. But charge separation alone does not guarantee high-efficiency operation. A photogenerated change in energy that is freely available to do useful work is also essential, and is strongly dependent on semiconductor optical properties and reaction kinetics. Notably, this information reveals that specificity of interfacial chemical reactions – even when they are not preceded by charge separation elsewhere – can result in efficient solar energy conversion. We expect that this tutorial will guide researchers in their pursuit to uncover new mechanisms for light to perform useful work.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"310 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507791","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}
Anode-free sodium metal batteries (AFSBs) offer a compelling route toward high-energy and sustainable electrochemical storage by eliminating excess sodium and inactive anode hosts. Yet their practical viability is fundamentally limited by rapid and irreversible active sodium loss. In anode-free architectures, cyclable sodium is the governing "currency" of cell lifetime: any interfacial irreversibility directly translates into catastrophic capacity decay. Unlike lithium systems, sodium depletion in AFSBs is driven by Na-specific physicochemical constraints-including a large ionic radius, low melting point, extreme volumetric expansion (≈260%), and intrinsically fragile solid-electrolyte interphase (SEI) mechanics-giving rise to distinct degradation pathways spanning sparse nucleation, porous growth, dynamic SEI fracture-repassivation, thermally induced morphology collapse, and coupled cathode-anode inventory feedback. This review establishes a multiscale mechanistic framework linking intrinsic sodium properties to cell-level failure, and critically assesses emerging mitigation strategies across sodiophilic current-collector engineering, multifunctional interphase design, sodium supplementation, and operation-protocol optimization. By integrating these approaches within a "source-process-inventory-environment" regulation paradigm, we outline key design rules and future priorities required to suppress sodium depletion and accelerate the translation of AFSBs from laboratory concepts to practical high-energy batteries.
{"title":"Active Sodium Loss in Practical Anode-Free Sodium Batteries: Mechanisms, Challenges, and Strategies","authors":"Saisai Qiu, Haolin Zhu, Jia Xie, Shijie Cheng","doi":"10.1039/d6ee00760k","DOIUrl":"https://doi.org/10.1039/d6ee00760k","url":null,"abstract":"Anode-free sodium metal batteries (AFSBs) offer a compelling route toward high-energy and sustainable electrochemical storage by eliminating excess sodium and inactive anode hosts. Yet their practical viability is fundamentally limited by rapid and irreversible active sodium loss. In anode-free architectures, cyclable sodium is the governing \"currency\" of cell lifetime: any interfacial irreversibility directly translates into catastrophic capacity decay. Unlike lithium systems, sodium depletion in AFSBs is driven by Na-specific physicochemical constraints-including a large ionic radius, low melting point, extreme volumetric expansion (≈260%), and intrinsically fragile solid-electrolyte interphase (SEI) mechanics-giving rise to distinct degradation pathways spanning sparse nucleation, porous growth, dynamic SEI fracture-repassivation, thermally induced morphology collapse, and coupled cathode-anode inventory feedback. This review establishes a multiscale mechanistic framework linking intrinsic sodium properties to cell-level failure, and critically assesses emerging mitigation strategies across sodiophilic current-collector engineering, multifunctional interphase design, sodium supplementation, and operation-protocol optimization. By integrating these approaches within a \"source-process-inventory-environment\" regulation paradigm, we outline key design rules and future priorities required to suppress sodium depletion and accelerate the translation of AFSBs from laboratory concepts to practical high-energy batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"27 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147519105","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}
Electrochemical CO2 conversion is approaching industrially relevant performance, yet its practical deployment is constrained by insufficient stability under realistic operating conditions. We reframe stability as a dynamic, system-wide property rather than a fixed device performance, and establish a unified multi-scale framework linking degradation pathways, detection, and corrective strategies across hierarchical levels from the active site to full-stack operation. We identify the limitations of constant-condition testing, which often misclassifies quasi-stable operation as industrial stable, and propose new measurement concepts that bridge laboratory diagnostics with real-world operating stresses. Through analyzing reversible failure modes including catalyst degradation, salt precipitation, and flooding, we organize recovery strategies that can be integrated into operational cycles for performance restoration. Building on this foundation, we chart a progression from intrinsic stability enhancement, to adaptive dynamic regulation, to fully operando recovery, in which autonomous systems are capable of operando performance restoration without interrupting production. These pathways define a research agenda for cross-disciplinary advances that could transform CO2 electrolysis from a fragile laboratory demonstration into a self-maintaining, commercially viable technology.
{"title":"Pathways toward Operando Recoverable CO2 Electrolyzers","authors":"Xin Li, Jingyun Tian, Panpan Li, Huazhang Zhao, Bingjun Xu, Zishuai Bill Zhang","doi":"10.1039/d5ee07501g","DOIUrl":"https://doi.org/10.1039/d5ee07501g","url":null,"abstract":"Electrochemical CO2 conversion is approaching industrially relevant performance, yet its practical deployment is constrained by insufficient stability under realistic operating conditions. We reframe stability as a dynamic, system-wide property rather than a fixed device performance, and establish a unified multi-scale framework linking degradation pathways, detection, and corrective strategies across hierarchical levels from the active site to full-stack operation. We identify the limitations of constant-condition testing, which often misclassifies quasi-stable operation as industrial stable, and propose new measurement concepts that bridge laboratory diagnostics with real-world operating stresses. Through analyzing reversible failure modes including catalyst degradation, salt precipitation, and flooding, we organize recovery strategies that can be integrated into operational cycles for performance restoration. Building on this foundation, we chart a progression from intrinsic stability enhancement, to adaptive dynamic regulation, to fully operando recovery, in which autonomous systems are capable of operando performance restoration without interrupting production. These pathways define a research agenda for cross-disciplinary advances that could transform CO2 electrolysis from a fragile laboratory demonstration into a self-maintaining, commercially viable technology.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"11 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507772","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}
Cadmium-free ZnxSn1−xO (ZTO) buffer layers are an attractive alternative to conventional CdS in Cu2ZnSn(S,Se)4 (CZTSSe) thin-film solar cells, especially with advantages of Cd-related toxicity elimination and parasitic absorption mitigation at short wavelengths. However, the performance of ZTO-based CZTSSe devices has lagged behind that of CdS-involved counterparts, largely due to high-density detrimental defects and non-ideal band alignment at the CZTSSe/ZTO heterojunction. Here, we develop a junction heat-treatment process that, upon thermal activation, selectively drives Zn cations to diffuse from the ZTO buffer into the CZTSSe absorber along the chemical potential gradient. This diffusion-driven Zn incorporation compensates for intrinsic bulk defects such as CuZn and VCu, particularly in the space charge region. The cation diffusion also contributes to a more favorable conduction-band offset, prolonged minority-carrier lifetime, and extended carrier-diffusion length. Collectively, this results in optimization of carrier dynamics with simultaneously enhanced carrier separation, extraction, and transport efficiencies. As a result, we achieve an efficiency of 14.39% (certified at 13.90%) and a large-area (1.03 cm2) efficiency of 12.24%, representing the highest-to-date efficiency for Cd-free CZTSSe solar cells.
{"title":"Intrinsic defect compensation in the space charge region enables cadmium-free kesterite solar cells to achieve 13.9% certified efficiency","authors":"Yonggang Zhao, Shuo Chen, Jiangjian Shi, Shurong Wang, Jia Yang, Zhenghua Su, Zhuanghao Zheng, Hongli Ma, Xianghua Zhang, Guangxing Liang","doi":"10.1039/d6ee00550k","DOIUrl":"https://doi.org/10.1039/d6ee00550k","url":null,"abstract":"Cadmium-free Zn<small><sub><em>x</em></sub></small>Sn<small><sub>1−<em>x</em></sub></small>O (ZTO) buffer layers are an attractive alternative to conventional CdS in Cu<small><sub>2</sub></small>ZnSn(S,Se)<small><sub>4</sub></small> (CZTSSe) thin-film solar cells, especially with advantages of Cd-related toxicity elimination and parasitic absorption mitigation at short wavelengths. However, the performance of ZTO-based CZTSSe devices has lagged behind that of CdS-involved counterparts, largely due to high-density detrimental defects and non-ideal band alignment at the CZTSSe/ZTO heterojunction. Here, we develop a junction heat-treatment process that, upon thermal activation, selectively drives Zn cations to diffuse from the ZTO buffer into the CZTSSe absorber along the chemical potential gradient. This diffusion-driven Zn incorporation compensates for intrinsic bulk defects such as Cu<small><sub>Zn</sub></small> and V<small><sub>Cu</sub></small>, particularly in the space charge region. The cation diffusion also contributes to a more favorable conduction-band offset, prolonged minority-carrier lifetime, and extended carrier-diffusion length. Collectively, this results in optimization of carrier dynamics with simultaneously enhanced carrier separation, extraction, and transport efficiencies. As a result, we achieve an efficiency of 14.39% (certified at 13.90%) and a large-area (1.03 cm<small><sup>2</sup></small>) efficiency of 12.24%, representing the highest-to-date efficiency for Cd-free CZTSSe solar cells.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"97 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147496351","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}
Guangmao Yan, Fei Wang, Jieqian Liu, He Zhou, Xiong Lei, Zhijun Wu, Wubin Du, Yingxing Zhong, Jing Feng, Zhenhua Ge, Yan Zhao, Qiu He, Hongge Pan, Hanyu Huo, Yan Yu
Silicon, germanium, tin, phosphorus, metal oxides, and their related compounds have emerged as promising anode materials for lithium-ion batteries owing to their high theoretical capacities. However, their practical application is severely hindered by large volume changes during lithiation and delithiation, which lead to electrode pulverization and rapid capacity fading. In addition, their intrinsically low electrical conductivity limits rate performance. To mitigate these issues, composite strategies—such as incorporating buffering matrices and conductive carbon—are widely employed, resulting in complex contact interfaces within the electrode. Nevertheless, the static and dynamic understanding of these interfaces remains insufficient. Under substantial volume strain, these contact interfaces undergo continuous evolution: point contacts may transform into surface contacts, while established interfaces may delaminate, ultimately governing electrode failure mechanisms. In this review, we systematically examine the nature and impact of contact interfaces in anodes undergoing significant volume strain. Contact interfaces are categorized into geometric types as well as physical and chemical interfaces, with particular emphasis on their operando evolution and coupling with solid electrolyte interphase chemistry. We critically evaluate advanced characterization techniques, including operando X-ray/neutron imaging and cryogenic electron microscopy, and present a comparative matrix outlining their respective capabilities. Furthermore, we bridge the gap between qualitative understanding and quantitative design principles by highlighting emerging advances in multiscale simulations as well as AI-assisted and data-driven interface engineering. Finally, we propose a roadmap linking laboratory-scale strategies to industrial scalability, offering a forward-looking framework for the rational design of next-generation Li⁺ storage systems.
{"title":"Contact Interfaces in Anodes with Large Volume Strain for High-Performance Lithium-Ion Storage","authors":"Guangmao Yan, Fei Wang, Jieqian Liu, He Zhou, Xiong Lei, Zhijun Wu, Wubin Du, Yingxing Zhong, Jing Feng, Zhenhua Ge, Yan Zhao, Qiu He, Hongge Pan, Hanyu Huo, Yan Yu","doi":"10.1039/d6ee01264g","DOIUrl":"https://doi.org/10.1039/d6ee01264g","url":null,"abstract":"Silicon, germanium, tin, phosphorus, metal oxides, and their related compounds have emerged as promising anode materials for lithium-ion batteries owing to their high theoretical capacities. However, their practical application is severely hindered by large volume changes during lithiation and delithiation, which lead to electrode pulverization and rapid capacity fading. In addition, their intrinsically low electrical conductivity limits rate performance. To mitigate these issues, composite strategies—such as incorporating buffering matrices and conductive carbon—are widely employed, resulting in complex contact interfaces within the electrode. Nevertheless, the static and dynamic understanding of these interfaces remains insufficient. Under substantial volume strain, these contact interfaces undergo continuous evolution: point contacts may transform into surface contacts, while established interfaces may delaminate, ultimately governing electrode failure mechanisms. In this review, we systematically examine the nature and impact of contact interfaces in anodes undergoing significant volume strain. Contact interfaces are categorized into geometric types as well as physical and chemical interfaces, with particular emphasis on their operando evolution and coupling with solid electrolyte interphase chemistry. We critically evaluate advanced characterization techniques, including operando X-ray/neutron imaging and cryogenic electron microscopy, and present a comparative matrix outlining their respective capabilities. Furthermore, we bridge the gap between qualitative understanding and quantitative design principles by highlighting emerging advances in multiscale simulations as well as AI-assisted and data-driven interface engineering. Finally, we propose a roadmap linking laboratory-scale strategies to industrial scalability, offering a forward-looking framework for the rational design of next-generation Li⁺ storage systems.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"34 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507085","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}
Molecular single-atom catalysts (SACs) offer tunable and well-defined active sites, rendering them ideal model systems to explore fundamental concepts in oxygen reduction reaction (ORR). However, the high-efficiency molecular SACs are still plagued by easy aggregation, planar symmetry of active sites, suboptimal adsorption/desorption of oxygen intermediates, and poor conductivity. Herein, we propose spatial electron bridge engineering as a universal strategy to disrupt the planar configuration of Fe-N4 moieties, modulate electronic structure, and enhance interfacial coupling. Through dual-descriptor (ΔG*OH and (ΔG*O-ΔG*OH)) analysis correlating activity with theoretical overpotentials, we systematically decode structureactivity relationships in symmetry-broken X-Fe-N4 (X=O, S, N) sites. Molecular heterostructure SACs are constructed by tethering iron pyridinic hexaazacyclophane macrocycle (Fe(Phen)2) to electron bridges (phenol, thiophenol, pyridine) functionalized carbon nanotubes (CNT), forming precisely controlled CNT-X-Fe architectures. Combined spectroscopic studies and DFT calculations reveal that the phenol bridge triggers a low-to-medium spin state transition via electron bridgeto-metal charge transfer, facilitating rapid electron shuttling between Fe(Phen)2 and CNT. This optimizes the Fe d-band center occupancy and enhances antibonding orbital hybridization, yielding the best ORR performance. This work establishes spatial electron bridges as orbital-coupling hubs bridging quantum-level d-p hybridization to macroscopic catalytic performance, offering a universal design framework for molecularly precise electrocatalysts.
分子单原子催化剂（SACs）提供了可调节和定义明确的活性位点，使其成为探索氧还原反应（ORR）基本概念的理想模型系统。然而，高效分子SACs仍然存在容易聚集、活性位点平面不对称、氧中间体吸附/解吸不理想以及导电性差等问题。在此，我们提出空间电子桥工程作为一种通用策略来破坏Fe-N4基团的平面构型，调节电子结构，增强界面耦合。通过双描述子（ΔG*OH和（ΔG*O-ΔG*OH））分析活性与理论过电位的相关性，我们系统地解码了对称破缺的X- fe - n4 （X=O， S， N）位点的结构-活性关系。分子异质结构SACs是通过将铁吡啶六氮杂环大环（Fe(Phen)2）系在电子桥（苯酚、噻吩、吡啶）官能化碳纳米管（CNT）上构建的，形成精确控制的CNT- x -Fe结构。结合光谱研究和DFT计算表明，苯酚桥通过电子桥到金属的电荷转移触发了低到中自旋态的转变，促进了Fe(Phen)2和碳纳米管之间的快速电子穿梭。这优化了Fe - d波段的中心占位，增强了反键轨道杂化，获得了最佳的ORR性能。这项工作建立了空间电子桥作为轨道耦合枢纽，桥接量子级d-p杂化到宏观催化性能，为分子精密电催化剂提供了通用设计框架。
{"title":"Engineering Spatial Electron Bridge in Molecular Heterostructure Single-Atom Catalyst for Oxygen Electroreduction","authors":"Qiao Gu, Mingtao Huang, Bingyu Huang, Wenhui Jiang, Ting Hu, Dirk Lützenkirchen-Hecht, Kai Yuan, Yiwang Chen","doi":"10.1039/d6ee00888g","DOIUrl":"https://doi.org/10.1039/d6ee00888g","url":null,"abstract":"Molecular single-atom catalysts (SACs) offer tunable and well-defined active sites, rendering them ideal model systems to explore fundamental concepts in oxygen reduction reaction (ORR). However, the high-efficiency molecular SACs are still plagued by easy aggregation, planar symmetry of active sites, suboptimal adsorption/desorption of oxygen intermediates, and poor conductivity. Herein, we propose spatial electron bridge engineering as a universal strategy to disrupt the planar configuration of Fe-N4 moieties, modulate electronic structure, and enhance interfacial coupling. Through dual-descriptor (ΔG*OH and (ΔG*O-ΔG*OH)) analysis correlating activity with theoretical overpotentials, we systematically decode structureactivity relationships in symmetry-broken X-Fe-N4 (X=O, S, N) sites. Molecular heterostructure SACs are constructed by tethering iron pyridinic hexaazacyclophane macrocycle (Fe(Phen)2) to electron bridges (phenol, thiophenol, pyridine) functionalized carbon nanotubes (CNT), forming precisely controlled CNT-X-Fe architectures. Combined spectroscopic studies and DFT calculations reveal that the phenol bridge triggers a low-to-medium spin state transition via electron bridgeto-metal charge transfer, facilitating rapid electron shuttling between Fe(Phen)2 and CNT. This optimizes the Fe d-band center occupancy and enhances antibonding orbital hybridization, yielding the best ORR performance. This work establishes spatial electron bridges as orbital-coupling hubs bridging quantum-level d-p hybridization to macroscopic catalytic performance, offering a universal design framework for molecularly precise electrocatalysts.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"11 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147478684","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}
Zhipeng Yin, Beining Wang, Tianyu Huang, Zhisheng Zhou, Kang An, Zsuzsanna László, István Bíró, Ning Li, Hai-Qiao Wang, Christoph J Brabec
Inverted organic solar cells (OSCs) are recognized for their superior operational stability, yet their efficiency, when fabricated via the layer-by-layer (LBL) approach, has remained substantially behind that of conventional architectures. This limitation stems from the inherent dissolution of the initial small-molecule acceptor (SMA) layer during sequential deposition and a fundamental misalignment between the resultant vertical component distribution and the optical field. Here, we introduce a reversed LBL (r-LBL) strategy, which inverts the conventional deposition sequence. We first construct a robust polymer donor (PD) scaffold, followed by the interstitial infiltration of SMA solutions. This order strategically positions the donor at the transparent electrode side, aligning its distribution with the light intensity maximum for optimal photon harvesting. Concurrently, it prevents the dissolution of the initial layer. The resulting active layer exhibits an ideal “polymer-scaffold-with-SMA-filling” morphology, characterized by enhanced crystallinity and face-on molecular orientation. This leads to inverted OSCs with remarkable power conversion efficiencies (PCEs) of 18.44% (PM6/L8-BO), 18.71% (D18-CI/L8-BO), and 19.20% (PM6/L8-BO:BTP-eC9). These devices also demonstrate exceptional operational stability, retaining over 97% of their initial PCE after 340 hours of continuous illumination. The universality of this r-LBL strategy is further validated in small-molecule-donor:polymer-acceptor systems, establishing it as a foundational and universal processing principle to overcome the efficiency-stability trade-off in inverted OSCs.
{"title":"Breaking the Efficiency Bottleneck of Inverted Solar Cells by Reversed Sequential Deposition","authors":"Zhipeng Yin, Beining Wang, Tianyu Huang, Zhisheng Zhou, Kang An, Zsuzsanna László, István Bíró, Ning Li, Hai-Qiao Wang, Christoph J Brabec","doi":"10.1039/d5ee07561k","DOIUrl":"https://doi.org/10.1039/d5ee07561k","url":null,"abstract":"Inverted organic solar cells (OSCs) are recognized for their superior operational stability, yet their efficiency, when fabricated via the layer-by-layer (LBL) approach, has remained substantially behind that of conventional architectures. This limitation stems from the inherent dissolution of the initial small-molecule acceptor (SMA) layer during sequential deposition and a fundamental misalignment between the resultant vertical component distribution and the optical field. Here, we introduce a reversed LBL (r-LBL) strategy, which inverts the conventional deposition sequence. We first construct a robust polymer donor (PD) scaffold, followed by the interstitial infiltration of SMA solutions. This order strategically positions the donor at the transparent electrode side, aligning its distribution with the light intensity maximum for optimal photon harvesting. Concurrently, it prevents the dissolution of the initial layer. The resulting active layer exhibits an ideal “polymer-scaffold-with-SMA-filling” morphology, characterized by enhanced crystallinity and face-on molecular orientation. This leads to inverted OSCs with remarkable power conversion efficiencies (PCEs) of 18.44% (PM6/L8-BO), 18.71% (D18-CI/L8-BO), and 19.20% (PM6/L8-BO:BTP-eC9). These devices also demonstrate exceptional operational stability, retaining over 97% of their initial PCE after 340 hours of continuous illumination. The universality of this r-LBL strategy is further validated in small-molecule-donor:polymer-acceptor systems, establishing it as a foundational and universal processing principle to overcome the efficiency-stability trade-off in inverted OSCs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"13 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147478687","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}
Jae Won Kim, You-Hyun Seo, Hee Jeong Jeong, Eun Chong Chae, Helen Hejin Park, Bong Joo Kang, Kyungsik Kim, Jinho Lee, Soonil Hong, Nam Joong Jeon
Organic solar cells (OSCs) and perovskite solar cells (PSCs) are emerging as promising next-generation alternatives to conventional silicon solar cells because of their rapidly increasing power conversion efficiency (PCE); potential for low-cost manufacturing; and suitability for diverse applications, including building- and vehicle-integrated photovoltaics, space-based solar power sources, and portable power sources. With the certified PCEs of OSCs and PSCs reaching 19.2% and 27.0%, respectively, significant effort is now directed toward upscaling these cells for commercialization. However, this transition presents a critical challenge: compared with those of their small-area cell (~ 0.1 cm2) counterparts, the PCEs of large-area modules (> 10 cm2) typically decrease by 20–30%, posing a significant barrier to the replacement of silicon-based technologies. While laser scribing is a prevalent technique for producing efficient large-area modules, it frequently introduces process-induced damage and stability concerns, as well as high process costs. This review critically examines the various module designs that are used in OSC and PSC fabrication schemes, summarizes the tradeoffs among different patterning techniques, and proposes future design directions that can bridge the efficiency gap and provide enhanced long-term stability.
{"title":"Review of module designs for organic and perovskite solar cells","authors":"Jae Won Kim, You-Hyun Seo, Hee Jeong Jeong, Eun Chong Chae, Helen Hejin Park, Bong Joo Kang, Kyungsik Kim, Jinho Lee, Soonil Hong, Nam Joong Jeon","doi":"10.1039/d5ee07830j","DOIUrl":"https://doi.org/10.1039/d5ee07830j","url":null,"abstract":"Organic solar cells (OSCs) and perovskite solar cells (PSCs) are emerging as promising next-generation alternatives to conventional silicon solar cells because of their rapidly increasing power conversion efficiency (PCE); potential for low-cost manufacturing; and suitability for diverse applications, including building- and vehicle-integrated photovoltaics, space-based solar power sources, and portable power sources. With the certified PCEs of OSCs and PSCs reaching 19.2% and 27.0%, respectively, significant effort is now directed toward upscaling these cells for commercialization. However, this transition presents a critical challenge: compared with those of their small-area cell (~ 0.1 cm2) counterparts, the PCEs of large-area modules (> 10 cm2) typically decrease by 20–30%, posing a significant barrier to the replacement of silicon-based technologies. While laser scribing is a prevalent technique for producing efficient large-area modules, it frequently introduces process-induced damage and stability concerns, as well as high process costs. This review critically examines the various module designs that are used in OSC and PSC fabrication schemes, summarizes the tradeoffs among different patterning techniques, and proposes future design directions that can bridge the efficiency gap and provide enhanced long-term stability.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"89 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147478685","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}
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