High-voltage lithium metal batteries (LMBs) face a critical barrier to practical deployment: conventional electrolytes fail to stabilize both the cathode and anode interfaces, triggering rapid degradation and safety risks. To overcome this limitation, we designed 3-methoxypropanenitrile (MPN), a molecularly tailored ether-nitrile additive, and integrated it into a diluted high-concentration electrolyte (DHCE). Computational studies reveal that the ether-oxygen heteroatom in MPN redistributes electron density and fine-tunes Li+ solvation, effectively circumventing the notorious reactivity of nitrile groups with lithium metal. This molecular intervention enables dual-interphase stabilization—on the lithium anode, MPN promotes anion-derived decomposition through weak yet selective Li+ coordination, forming an inorganic-rich SEI (LiF/Li3N) that ensures 99.5% Coulombic efficiency and uniform lithium deposition. At the LiMnxFe1-xPO4 cathode operating above 4.5 V, MPN adsorbs preferentially via Mn/Fe coordination, shields the surface from oxidative attack, and participates in hydrogen-transfer reactions with FSI- anions to construct a robust inorganic CEI, substantially suppressing transition metal dissolution. As a result, the MPN-enhanced electrolyte enables Li||LMFP full cells to achieve breakthrough cycling stability, maintaining 86.4% capacity after 1,400 cycles at 0.5C while sustaining 300 cycles under lean-lithium conditions (N/P=2). This work establishes a heteroatom-functionalization strategy that transforms conventionally incompatible nitriles into bifunctional interphase regulators, thereby providing a universal platform for constructing durable high-voltage lithium metal batteries.
{"title":"Molecular Engineering of an Ether-Nitrile Constructs Robust Dual-interphases for Ultra-Stable 4.5 V Lithium Metal Batteries","authors":"Yongchuan Liu, Hengyang Zhu, Chenyu Wang, Guihuang Fang, Xiangxin Zhang, Baisheng Sa, Yuanqiang Chen, Ying Liu, Lunhui Guan, Yining Zhang","doi":"10.1039/d5ee07479g","DOIUrl":"https://doi.org/10.1039/d5ee07479g","url":null,"abstract":"High-voltage lithium metal batteries (LMBs) face a critical barrier to practical deployment: conventional electrolytes fail to stabilize both the cathode and anode interfaces, triggering rapid degradation and safety risks. To overcome this limitation, we designed 3-methoxypropanenitrile (MPN), a molecularly tailored ether-nitrile additive, and integrated it into a diluted high-concentration electrolyte (DHCE). Computational studies reveal that the ether-oxygen heteroatom in MPN redistributes electron density and fine-tunes Li+ solvation, effectively circumventing the notorious reactivity of nitrile groups with lithium metal. This molecular intervention enables dual-interphase stabilization—on the lithium anode, MPN promotes anion-derived decomposition through weak yet selective Li+ coordination, forming an inorganic-rich SEI (LiF/Li3N) that ensures 99.5% Coulombic efficiency and uniform lithium deposition. At the LiMnxFe1-xPO4 cathode operating above 4.5 V, MPN adsorbs preferentially via Mn/Fe coordination, shields the surface from oxidative attack, and participates in hydrogen-transfer reactions with FSI- anions to construct a robust inorganic CEI, substantially suppressing transition metal dissolution. As a result, the MPN-enhanced electrolyte enables Li||LMFP full cells to achieve breakthrough cycling stability, maintaining 86.4% capacity after 1,400 cycles at 0.5C while sustaining 300 cycles under lean-lithium conditions (N/P=2). This work establishes a heteroatom-functionalization strategy that transforms conventionally incompatible nitriles into bifunctional interphase regulators, thereby providing a universal platform for constructing durable high-voltage lithium metal batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"17 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146129668","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}
Yuezhang He, Hongxi Luo, Yuancheng Lin, Carl Talsma, Anna Li, Zhenqian Wang, Yujuan Fang, Pei Liu, Jesse D Jenkins, Eric Larson, Zheng Li
High costs of green hydrogen and of carbon capture, utilization, and sequestration (CCUS) have hindered policy ambition and slowed real-world deployment, despite their importance for decarbonizing hard-to-abate sectors, including cement and methanol. Given the economic challenges of adopting CCUS in cement and green hydrogen in methanol production separately, we propose a renewable-powered co-production system that couples electrolytic hydrogen and CCUS through molecule exchange. We optimize system configurations using an hourly-resolved, process-based model incorporating operational flexibility, and explore integrated strategies for plant-level deployment and CO₂ source-sink matching across China. We find that co-production could reduce CO₂ abatement costs to $41–53 per tonne by 2035, significantly lower than approximately $75 for standalone cement CCUS and over $120 for standalone renewable-based methanol. Co-production is preferentially deployed at cement plants in renewable-rich regions, potentially reshaping national CO₂ infrastructure planning. This hydrogen–CCUS coupling paradigm could accelerate industrial decarbonization and scaling for other applications.
{"title":"Scaling green hydrogen and CCUS via cement-methanol co-production in China","authors":"Yuezhang He, Hongxi Luo, Yuancheng Lin, Carl Talsma, Anna Li, Zhenqian Wang, Yujuan Fang, Pei Liu, Jesse D Jenkins, Eric Larson, Zheng Li","doi":"10.1039/d5ee07379k","DOIUrl":"https://doi.org/10.1039/d5ee07379k","url":null,"abstract":"High costs of green hydrogen and of carbon capture, utilization, and sequestration (CCUS) have hindered policy ambition and slowed real-world deployment, despite their importance for decarbonizing hard-to-abate sectors, including cement and methanol. Given the economic challenges of adopting CCUS in cement and green hydrogen in methanol production separately, we propose a renewable-powered co-production system that couples electrolytic hydrogen and CCUS through molecule exchange. We optimize system configurations using an hourly-resolved, process-based model incorporating operational flexibility, and explore integrated strategies for plant-level deployment and CO₂ source-sink matching across China. We find that co-production could reduce CO₂ abatement costs to $41–53 per tonne by 2035, significantly lower than approximately $75 for standalone cement CCUS and over $120 for standalone renewable-based methanol. Co-production is preferentially deployed at cement plants in renewable-rich regions, potentially reshaping national CO₂ infrastructure planning. This hydrogen–CCUS coupling paradigm could accelerate industrial decarbonization and scaling for other applications.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"70 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146129469","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}
Jung Geon Son, Ha-Eun Koo, Woo Jin Lee, Dongyoung Kim, Sujung Park, Jina Roe, Jongdeuk Seo, Jung Min Ha, Heunjeong Lee, Wangyeon Lee, Han Young Woo, Shinuk Cho, Dong Suk Kim, Seung-Jae Shin, Jin Young Kim
Self-assembled monolayer (SAM)-based hole-selective layers (HSLs) offer a promising route to defect-passivated and energy-aligned interfaces in perovskite organic tandem solar cells (POTSCs). However, their practical implementation remains hindered by weak anchoring to transparent conductive oxides (TCOs), leading to desorption during perovskite deposition and poor interfacial durability under polar solvent exposure. Here, we present a chemical interfacial stabilization strategy in which potassium carbonate (K2CO3) mediates the controlled deprotonation of [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2PACz), forming mixed mono- and di-deprotonated species (2PACz-K) that bind strongly to indium tin oxide (ITO). The resulting SAM exhibits superior solvent resistance, improved energy-level alignment, and enhanced buried interface quality. POTSCs incorporating 2PACz-K achieve 25.10% power conversion efficiency (PCE) with a high open-circuit voltage (VOC) of 2.230 V, while retaining 80% of their initial PCE after 220 h of maximum power point (MPP) tracking under simulated 1-sun illumination. Beyond photovoltaics, the robust 2PACz-K interface is further integrated into a perovskite/organic tandem photocathode (POT-PEC), representing the first transparent, metal-free tandem PEC architecture capable of stable operation in aqueous electrolyte, delivering a photovoltage (Vph) of 2.16 V and achieving solar-to-hydrogen (STH) conversion efficiency of 7.7%. This work establishes a versatile interfacial design paradigm that bridges photovoltaic and photoelectrochemical energy conversion.
{"title":"Deprotonated Self-Assembled Molecules as Robust Hole-Selective Layers for Perovskite/Organic Tandem Solar Cells and Photocathodes","authors":"Jung Geon Son, Ha-Eun Koo, Woo Jin Lee, Dongyoung Kim, Sujung Park, Jina Roe, Jongdeuk Seo, Jung Min Ha, Heunjeong Lee, Wangyeon Lee, Han Young Woo, Shinuk Cho, Dong Suk Kim, Seung-Jae Shin, Jin Young Kim","doi":"10.1039/d5ee07006f","DOIUrl":"https://doi.org/10.1039/d5ee07006f","url":null,"abstract":"Self-assembled monolayer (SAM)-based hole-selective layers (HSLs) offer a promising route to defect-passivated and energy-aligned interfaces in perovskite organic tandem solar cells (POTSCs). However, their practical implementation remains hindered by weak anchoring to transparent conductive oxides (TCOs), leading to desorption during perovskite deposition and poor interfacial durability under polar solvent exposure. Here, we present a chemical interfacial stabilization strategy in which potassium carbonate (K2CO3) mediates the controlled deprotonation of [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2PACz), forming mixed mono- and di-deprotonated species (2PACz-K) that bind strongly to indium tin oxide (ITO). The resulting SAM exhibits superior solvent resistance, improved energy-level alignment, and enhanced buried interface quality. POTSCs incorporating 2PACz-K achieve 25.10% power conversion efficiency (PCE) with a high open-circuit voltage (VOC) of 2.230 V, while retaining 80% of their initial PCE after 220 h of maximum power point (MPP) tracking under simulated 1-sun illumination. Beyond photovoltaics, the robust 2PACz-K interface is further integrated into a perovskite/organic tandem photocathode (POT-PEC), representing the first transparent, metal-free tandem PEC architecture capable of stable operation in aqueous electrolyte, delivering a photovoltage (Vph) of 2.16 V and achieving solar-to-hydrogen (STH) conversion efficiency of 7.7%. This work establishes a versatile interfacial design paradigm that bridges photovoltaic and photoelectrochemical energy conversion.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"17 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146129541","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}
Li-rich layered oxides (LLOs) are promising cathodes for high-energy-density Li-ion batteries, yet their practical deployment is hindered by severe voltage decay and structural degradation driven by uncontrolled lattice-oxygen activity. Here, we propose a lattice chemistry damping stabilization strategy by constructing radially graded disordered domains without disrupting the long-range layered order. The highly disordered surface evolves into spinel-like units with oxygen defects, functioning as a damping reservoir that buffers oxygen activity and accelerates Li+ diffusion, whereas the moderately disordered bulk acts as a structural damper by reinforcing TM–O bonding and alleviating strain. This spatially resolved cooperative damping enhances O 2p–TM 3d hybridization, promotes electron delocalization, and enables reversible oxygen redox. Importantly, in situ XRD and EIS–DRT jointly quantify this damping through suppressed Δc/ΔV and microstrain excursions, together with attenuated SOC-dependent polarisation/relaxation evolution under practical high-voltage operation. Benefiting from this mechanism, the optimized electrode delivers 81.3% capacity retention after 800 cycles with an ultra-low voltage decay of 0.64 mV/cycle, and Ah-level pouch cells maintain 90% capacity after 200 cycles alongside negligible voltage decay. This work provides a physically inspired, measurement-anchored pathway to suppress voltage decay and extend the lifetime of LLOs.
{"title":"Lattice Chemistry Damping Stabilization Enables Voltage Stability and Oxygen Redox Reversibility in Li-Rich Layered Oxides","authors":"Lingcai Zeng, Yaqian Wang, Tong Li, Bao Qiu, Jiajie Pan, Haoyan Liang, Junhao Li, Xiaolei Sun, Jianrong Zeng, Kaixiang Shi, Zhaoping Liu, Quanbing Liu","doi":"10.1039/d5ee06116d","DOIUrl":"https://doi.org/10.1039/d5ee06116d","url":null,"abstract":"Li-rich layered oxides (LLOs) are promising cathodes for high-energy-density Li-ion batteries, yet their practical deployment is hindered by severe voltage decay and structural degradation driven by uncontrolled lattice-oxygen activity. Here, we propose a lattice chemistry damping stabilization strategy by constructing radially graded disordered domains without disrupting the long-range layered order. The highly disordered surface evolves into spinel-like units with oxygen defects, functioning as a damping reservoir that buffers oxygen activity and accelerates Li+ diffusion, whereas the moderately disordered bulk acts as a structural damper by reinforcing TM–O bonding and alleviating strain. This spatially resolved cooperative damping enhances O 2p–TM 3d hybridization, promotes electron delocalization, and enables reversible oxygen redox. Importantly, in situ XRD and EIS–DRT jointly quantify this damping through suppressed Δc/ΔV and microstrain excursions, together with attenuated SOC-dependent polarisation/relaxation evolution under practical high-voltage operation. Benefiting from this mechanism, the optimized electrode delivers 81.3% capacity retention after 800 cycles with an ultra-low voltage decay of 0.64 mV/cycle, and Ah-level pouch cells maintain 90% capacity after 200 cycles alongside negligible voltage decay. This work provides a physically inspired, measurement-anchored pathway to suppress voltage decay and extend the lifetime of LLOs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"30 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146129470","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}
Kumar Raju, Stephen W. T. Price, Alice J. Merryweather, Aleksandar Radić, May Ching Lai, Debashis Tripathy, Daniel Lorden, Edward Saunders, Israel Temprano, Sulki Park, Caterina Ducati, Akshay Rao, Angkur Shaikeea, Clare P. Grey, Michael De Volder
The charging time of Li-ion batteries is an important bottleneck in the wider adoption of electric vehicles (EVs). A common strategy to improve the rate performance is improving ion transport by patterning the electrode. However, these patterning methods usually increase the electrode porosity, thereby decreasing the volumetric energy density. In this work, we leverage the ability of Single Crystal LiNi0.8Mn0.1Co0.1O2 (SC-NMC811) electrodes to be calendered to higher packing densities than traditional cathodes, which then allows to offset additional porosity introduced by electrode patterning. We calendar SC-NMC811 electrodes to a 25% porosity and then introduce hole patterns spaced 100 to 600 µm apart using laser processing with a goal to maintain average porosities below 30%. As expected, we found systematic improvements in the rate performance with increasing hole density and used operando charge photometry to explore the limits of mass transport in the regions surrounding the holes but interestingly, we also observe improved capacity retention when using patterned electrodes. We found that there is less cathode lattice oxygen loss when using patterned cathodes, this in turn reduces transition metal shuttling reduces anode solid electrolyte interphase (SEI) impedance growth. We demonstrated a reduction in oxygen loss by both electron energy loss spectroscopy (EELS) mapping, X-ray diffraction (XRD) mapping and X-ray diffraction computed tomography (XRD-CT). Overall, SC-NMC811 electrode's ability to withstand over-calendering offers the opportunity to introduce laser patterned holes while maintaining the average porosity below 30%. This increases both the rate performance and longevity of the electrodes.
{"title":"Enhancing power density and cycle life of NMC811 battery cathodes via combined dense calendering and laser patterning","authors":"Kumar Raju, Stephen W. T. Price, Alice J. Merryweather, Aleksandar Radić, May Ching Lai, Debashis Tripathy, Daniel Lorden, Edward Saunders, Israel Temprano, Sulki Park, Caterina Ducati, Akshay Rao, Angkur Shaikeea, Clare P. Grey, Michael De Volder","doi":"10.1039/d5ee06773a","DOIUrl":"https://doi.org/10.1039/d5ee06773a","url":null,"abstract":"The charging time of Li-ion batteries is an important bottleneck in the wider adoption of electric vehicles (EVs). A common strategy to improve the rate performance is improving ion transport by patterning the electrode. However, these patterning methods usually increase the electrode porosity, thereby decreasing the volumetric energy density. In this work, we leverage the ability of Single Crystal LiNi<small><sub>0.8</sub></small>Mn<small><sub>0.1</sub></small>Co<small><sub>0.1</sub></small>O<small><sub>2</sub></small> (SC-NMC811) electrodes to be calendered to higher packing densities than traditional cathodes, which then allows to offset additional porosity introduced by electrode patterning. We calendar SC-NMC811 electrodes to a 25% porosity and then introduce hole patterns spaced 100 to 600 µm apart using laser processing with a goal to maintain average porosities below 30%. As expected, we found systematic improvements in the rate performance with increasing hole density and used <em>operando</em> charge photometry to explore the limits of mass transport in the regions surrounding the holes but interestingly, we also observe improved capacity retention when using patterned electrodes. We found that there is less cathode lattice oxygen loss when using patterned cathodes, this in turn reduces transition metal shuttling reduces anode solid electrolyte interphase (SEI) impedance growth. We demonstrated a reduction in oxygen loss by both electron energy loss spectroscopy (EELS) mapping, X-ray diffraction (XRD) mapping and X-ray diffraction computed tomography (XRD-CT). Overall, SC-NMC811 electrode's ability to withstand over-calendering offers the opportunity to introduce laser patterned holes while maintaining the average porosity below 30%. This increases both the rate performance and longevity of the electrodes.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"89 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116089","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}
Zhenhai Shi, Suli Chen, Min Zan, Leiqian Zhang, Jiaming Gong, Yazhou Zhou, Klaus Müllen, Feili Lai, Tianxi Liu
Aqueous zinc-ion batteries are promising for large-scale energy storage due to their safety, low cost, and sustainability. Their practical application, however, is hampered by the instability of the Zn anode, primarily arising from dendritic growth and parasitic side reactions. Here, we report a surfactant-mediated mesoscopic electrolyte utilizing sophorolipid (SL), an amphiphilic surfactant that provides dual behavior. In the bulk electrolyte, SL spontaneously assembles into nanoscale micelles, creating a tailored mesoscopic environment that confines Zn2+ through multivalent dipole interactions. This weakens the solvation shell and enhances Zn2+ transport kinetics. At the same time, unassembled SL molecules selectively anchor onto the Zn surface to form a protective interfacial layer that excludes free water and promotes oriented Zn(101) deposition through electrostatic shielding and spatial confinement effects. This dual regulation mechanism effectively suppresses Zn dendrite formation, hydrogen evolution, and corrosion. Consequently, the resulting electrolyte enables a Zn//Zn symmetric cell to achieve excellent cycling stability for 2800 h at 1 mA cm−2 and 1 mAh cm−2, coupled with a high average coulombic efficiency of 99.3%. Furthermore, assembled Zn//I2 full cells demonstrate outstanding long-term cyclability, retaining nearly 100% capacity after 25 000 cycles at 5 A g−1.
水锌离子电池由于其安全、低成本和可持续性，在大规模储能方面具有很大的前景。然而，它们的实际应用受到锌阳极的不稳定性的阻碍，主要是由枝晶生长和寄生副反应引起的。在这里，我们报道了一种表面活性剂介导的介观电解质，利用槐脂（SL），一种提供双重行为的两亲表面活性剂。在散装电解质中，SL自发地组装成纳米级胶束，通过多价偶极子相互作用创造了一个定制的介孔环境，限制了Zn2+。这弱化了溶剂化壳层，增强了Zn2+输运动力学。同时，未组装的SL分子选择性地锚定在Zn表面，形成保护界面层，通过静电屏蔽和空间约束效应，排除游离水，促进取向Zn（101）沉积。这种双重调控机制有效地抑制了Zn枝晶的形成、析氢和腐蚀。因此，所得到的电解质使锌/锌对称电池能够在1 mA cm - 2和1 mAh cm - 2下实现2800 h的优异循环稳定性，并具有99.3%的高平均库仑效率。此外，组装的Zn/ I2电池表现出出色的长期可循环性，在5 A g−1下循环25000次后仍保持近100%的容量。
{"title":"Surfactant-mediated mesoscopic confinement and selective interfacial shielding for highly stable zinc anode","authors":"Zhenhai Shi, Suli Chen, Min Zan, Leiqian Zhang, Jiaming Gong, Yazhou Zhou, Klaus Müllen, Feili Lai, Tianxi Liu","doi":"10.1039/d5ee06338h","DOIUrl":"https://doi.org/10.1039/d5ee06338h","url":null,"abstract":"Aqueous zinc-ion batteries are promising for large-scale energy storage due to their safety, low cost, and sustainability. Their practical application, however, is hampered by the instability of the Zn anode, primarily arising from dendritic growth and parasitic side reactions. Here, we report a surfactant-mediated mesoscopic electrolyte utilizing sophorolipid (SL), an amphiphilic surfactant that provides dual behavior. In the bulk electrolyte, SL spontaneously assembles into nanoscale micelles, creating a tailored mesoscopic environment that confines Zn<small><sup>2+</sup></small> through multivalent dipole interactions. This weakens the solvation shell and enhances Zn<small><sup>2+</sup></small> transport kinetics. At the same time, unassembled SL molecules selectively anchor onto the Zn surface to form a protective interfacial layer that excludes free water and promotes oriented Zn(101) deposition through electrostatic shielding and spatial confinement effects. This dual regulation mechanism effectively suppresses Zn dendrite formation, hydrogen evolution, and corrosion. Consequently, the resulting electrolyte enables a Zn//Zn symmetric cell to achieve excellent cycling stability for 2800 h at 1 mA cm<small><sup>−2</sup></small> and 1 mAh cm<small><sup>−2</sup></small>, coupled with a high average coulombic efficiency of 99.3%. Furthermore, assembled Zn//I<small><sub>2</sub></small> full cells demonstrate outstanding long-term cyclability, retaining nearly 100% capacity after 25 000 cycles at 5 A g<small><sup>−1</sup></small>.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"19 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116248","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}
Longhai Zhang, Cheng Ji, Quanwei Ma, Hongbao Li, Rui Wang, Lin Zhang, Shilin Zhang, Qingyu Yan, Dongliang Chao, Chaofeng Zhang
Aqueous aluminum-ion batteries represent a promising energy storage technology, leveraging their exceptional capacity, low cost, and inherent safety. However, practical implementation has been hampered by severe performance degradation at subzero temperatures and a scarcity of cathode materials with high capacity. Here, we present a conjugated bipolar polymer poly(2,3-diaminonaphthalene-1,4-dione) (PDND) synthesized via continuous-flow organic electrosynthesis. This molecular design incorporates a quinone-amine redox system that unifies n-type (quinone) and p-type (amine) moieties, thereby enhancing charge storage capacity. The extended quinone-amine backbone enhances p-π conjugation, enabling efficient π-electron delocalization and continuous charge transport pathways along the polymer chain, resulting in high electronic conductivity. Furthermore, planar π-conjugated quinone units and arylamine linkages construct synergistic dualinteraction networks between polymer chains including dense hydrogen-bonding and strong π-π interaction, ensuring structural stability. Consequently, the Al//PDND battery delivers a high capacity of 302 mAh g⁻¹, outstanding cycling stability (≥1000 cycles), and remarkable rate capability (up to 2 A g⁻¹). Notably, it operates effectively at -25 o C using a standard aqueous electrolyte without antifreeze additives, underscoring the superior low-temperature performance endowed by PDND. Through in situ/ex situ spectroscopic studies, we elucidate a multi-ion co-storage mechanism involving the reversible insertion of Al³⁺, H⁺, and ClO₄⁻ ions.
水铝离子电池凭借其卓越的容量、低成本和固有的安全性，代表了一种很有前途的储能技术。然而，由于在零下温度下的严重性能下降和高容量正极材料的缺乏，实际实施受到了阻碍。本文采用连续流有机电合成方法合成了共轭双极性聚合物聚（2,3-二氨基萘-1,4-二酮）（pnd）。这种分子设计结合了醌-胺氧化还原系统，统一了n型（醌）和p型（胺）部分，从而提高了电荷存储能力。延伸的醌-胺主链增强了p-π共轭作用，使π-电子有效离域和沿聚合物链的连续电荷传输途径成为可能，从而获得高电子导电性。此外，平面π共轭醌单元和芳胺键在聚合物链之间构建了致密的氢键和强π-π相互作用的协同双相互作用网络，保证了结构的稳定性。因此，Al// pnd电池提供了302 mAh g⁻¹的高容量，出色的循环稳定性（≥1000次循环）和卓越的速率能力（高达2 a g⁻¹）。值得注意的是，它在-25℃下使用不含防冻添加剂的标准水性电解质有效工作，突出了pnd所赋予的优越低温性能。通过原位/非原位光谱研究，我们阐明了一种多离子共存储机制，包括Al³+、H +和clo4 +的可逆插入。
{"title":"Continuous-Flow Organic Electrosynthesis of a Conjugated Bipolar Polymer Cathode for High-Performance Low-Temperature Aqueous Aluminum-Ion Batteries","authors":"Longhai Zhang, Cheng Ji, Quanwei Ma, Hongbao Li, Rui Wang, Lin Zhang, Shilin Zhang, Qingyu Yan, Dongliang Chao, Chaofeng Zhang","doi":"10.1039/d5ee06706e","DOIUrl":"https://doi.org/10.1039/d5ee06706e","url":null,"abstract":"Aqueous aluminum-ion batteries represent a promising energy storage technology, leveraging their exceptional capacity, low cost, and inherent safety. However, practical implementation has been hampered by severe performance degradation at subzero temperatures and a scarcity of cathode materials with high capacity. Here, we present a conjugated bipolar polymer poly(2,3-diaminonaphthalene-1,4-dione) (PDND) synthesized via continuous-flow organic electrosynthesis. This molecular design incorporates a quinone-amine redox system that unifies n-type (quinone) and p-type (amine) moieties, thereby enhancing charge storage capacity. The extended quinone-amine backbone enhances p-π conjugation, enabling efficient π-electron delocalization and continuous charge transport pathways along the polymer chain, resulting in high electronic conductivity. Furthermore, planar π-conjugated quinone units and arylamine linkages construct synergistic dualinteraction networks between polymer chains including dense hydrogen-bonding and strong π-π interaction, ensuring structural stability. Consequently, the Al//PDND battery delivers a high capacity of 302 mAh g⁻¹, outstanding cycling stability (≥1000 cycles), and remarkable rate capability (up to 2 A g⁻¹). Notably, it operates effectively at -25 o C using a standard aqueous electrolyte without antifreeze additives, underscoring the superior low-temperature performance endowed by PDND. Through in situ/ex situ spectroscopic studies, we elucidate a multi-ion co-storage mechanism involving the reversible insertion of Al³⁺, H⁺, and ClO₄⁻ ions.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"42 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116065","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}
Min Jae Lee, Xuanjie Wang, Tae Han Kim, Rohith Mittapally, Won Sik Kim, Young Ko, Bong Jae Lee, Jae Hyun Song, Hyung Jun Lee, Doo Nam Moon, Seung Hwan Ko, Gang Chen
Vehicles exposed to sunlight experience rapid heating due to low thermal mass and confined space, leading to excessive HVAC energy consumption. Transparent radiative cooling (TRC) provides a passive pathway for heat mitigation, but existing TRC technologies face limitations in optical clarity, durability, and real-world validation. Here, we present a scalable transparent radiative cooling (STRC) film for vehicle windows, achieving >70% visible transmittance, strong mid-infrared emittance, and high solar reflectance. Full-scale field tests across various regions and vehicle types show substantial cabin temperature reductions of up to 6.1 °C and energy savings exceeding 20%, with a minimal winter heating penalty of 0.3%. Seasonal analysis and U.S. fleet-scale modeling further project an annual CO2 reduction of 25.4 megatons—equivalent to removing 5 million cars from the road. STRC thus provides a practical, durable, and zero-energy cooling solution for sustainable and decarbonized transportation.
{"title":"Towards decarbonization in transportation: scalable transparent radiative cooling for enhanced vehicle energy efficiency","authors":"Min Jae Lee, Xuanjie Wang, Tae Han Kim, Rohith Mittapally, Won Sik Kim, Young Ko, Bong Jae Lee, Jae Hyun Song, Hyung Jun Lee, Doo Nam Moon, Seung Hwan Ko, Gang Chen","doi":"10.1039/d5ee06609c","DOIUrl":"https://doi.org/10.1039/d5ee06609c","url":null,"abstract":"Vehicles exposed to sunlight experience rapid heating due to low thermal mass and confined space, leading to excessive HVAC energy consumption. Transparent radiative cooling (TRC) provides a passive pathway for heat mitigation, but existing TRC technologies face limitations in optical clarity, durability, and real-world validation. Here, we present a scalable transparent radiative cooling (STRC) film for vehicle windows, achieving >70% visible transmittance, strong mid-infrared emittance, and high solar reflectance. Full-scale field tests across various regions and vehicle types show substantial cabin temperature reductions of up to 6.1 °C and energy savings exceeding 20%, with a minimal winter heating penalty of 0.3%. Seasonal analysis and U.S. fleet-scale modeling further project an annual CO<small><sub>2</sub></small> reduction of 25.4 megatons—equivalent to removing 5 million cars from the road. STRC thus provides a practical, durable, and zero-energy cooling solution for sustainable and decarbonized transportation.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"236 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116158","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}
The hydrogen evolution reaction (HER) plays a pivotal role in sustainable hydrogen production and the transition to a carbon-neutral energy future. Traditionally, HER catalyst design has focused on optimizing as-synthesized structures such as composition, morphology, and electronic states, under the assumption that these features remain static during operation. However, accumulating evidence reveals that HER catalysts undergo profound reconstruction, including phase transformation, compositional change, and atomic rearrangement, which fundamentally redefine the true active states. Neglecting this dynamic evolution risks misidentifying catalytic sites, misinterpreting mechanisms, and misguiding design strategies. In this Perspective, we advocate a reconstruction-centered framework for the HER. We outline key reconstruction modes, argue that reconstruction is thermodynamically driven and shaped by intrinsic and extrinsic factors, and emphasize that catalysts should be designed as precursors engineered to evolve in situ into their most active and durable forms. Finally, we advocate for stability assessments that capture steady-state reconstructed phases instead of transient initial states. Adopting this dynamic viewpoint establishes a coherent foundation for mechanistic understanding and rational catalyst design, paving the way toward predictive control of catalytic activity and long-term durability.
{"title":"Dynamic Reconstruction Defines True Active States in the Hydrogen Evolution Reaction","authors":"Xingyu Ding, Xianbiao Fu","doi":"10.1039/d5ee06502j","DOIUrl":"https://doi.org/10.1039/d5ee06502j","url":null,"abstract":"The hydrogen evolution reaction (HER) plays a pivotal role in sustainable hydrogen production and the transition to a carbon-neutral energy future. Traditionally, HER catalyst design has focused on optimizing as-synthesized structures such as composition, morphology, and electronic states, under the assumption that these features remain static during operation. However, accumulating evidence reveals that HER catalysts undergo profound reconstruction, including phase transformation, compositional change, and atomic rearrangement, which fundamentally redefine the true active states. Neglecting this dynamic evolution risks misidentifying catalytic sites, misinterpreting mechanisms, and misguiding design strategies. In this Perspective, we advocate a reconstruction-centered framework for the HER. We outline key reconstruction modes, argue that reconstruction is thermodynamically driven and shaped by intrinsic and extrinsic factors, and emphasize that catalysts should be designed as precursors engineered to evolve in situ into their most active and durable forms. Finally, we advocate for stability assessments that capture steady-state reconstructed phases instead of transient initial states. Adopting this dynamic viewpoint establishes a coherent foundation for mechanistic understanding and rational catalyst design, paving the way toward predictive control of catalytic activity and long-term durability.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"241 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116087","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}
Dong Zhang, Baoze Liu, Xue Wang, Qi Liu, Danpeng Gao, Xianglang Sun, Xin Wu, Zexin Yu, Chunlei Zhang, Ning Wang, Yan Wang, Nikhil Kalasariya, Francesco Vanin, Weidong Tian, Shuai Li, Jianqiu Gong, Lina Wang, Yang Bai, Shuang Xiao, Bo Li, Martin Stolterfoht, Xiao Cheng Zeng, Shangfeng Yang, Zonglong Zhu
Perovskite–organic tandem solar cells (POTSCs) offer significant advantages over other perovskite-based tandem architectures owing to their straightforward processing and broad tuneability. However, the interfacial energetics disorder and resulting heterogeneous photoactive phase in wide bandgap perovskite subcells significantly undermine their long-term stability. Here, we develop a multidentate anchoring-bridging strategy that establishes a periodic passivating array that coordinates with dangling Pb2+ on the perovskite surface to reduce vacancy-mediated halide migration. The network with fluorinated chains reconfigures the interfacial dielectric landscape, significantly increasing the migration activation barrier for halide vacancies at the perovskite/electron transport layer interface, suppressing ion migration and significantly enchancing longevity. Poly-FPTS-treated tandem devices delivered a power conversion efficiency (PCE) of 26.5%, with a high open-circuit voltage of 2.178 V. A steady-state certified efficiency of 25.1% was achieved in Japan Electrical Safety & Environmental Technology Laboratories (JET), as reported in Solar Cell Efficiency Tables (version 65). Under continuous 1-sun illumination at the maximum power point (ISOS-L-1I protocol), these devices retained 92% of their initial efficiency after 1000 hours, and they exhibited an efficiency loss < 5% after 1056 hours of light–dark cycling (ISOS-LC-1). This work reveals the importance of treating the top perovskite/ETL contact for commercializing perovskite–organic tandem solar cells.
{"title":"Multidentate silane bridging for stable and efficient perovskite–organic tandem solar cells","authors":"Dong Zhang, Baoze Liu, Xue Wang, Qi Liu, Danpeng Gao, Xianglang Sun, Xin Wu, Zexin Yu, Chunlei Zhang, Ning Wang, Yan Wang, Nikhil Kalasariya, Francesco Vanin, Weidong Tian, Shuai Li, Jianqiu Gong, Lina Wang, Yang Bai, Shuang Xiao, Bo Li, Martin Stolterfoht, Xiao Cheng Zeng, Shangfeng Yang, Zonglong Zhu","doi":"10.1039/d5ee06253e","DOIUrl":"https://doi.org/10.1039/d5ee06253e","url":null,"abstract":"Perovskite–organic tandem solar cells (POTSCs) offer significant advantages over other perovskite-based tandem architectures owing to their straightforward processing and broad tuneability. However, the interfacial energetics disorder and resulting heterogeneous photoactive phase in wide bandgap perovskite subcells significantly undermine their long-term stability. Here, we develop a multidentate anchoring-bridging strategy that establishes a periodic passivating array that coordinates with dangling Pb<small><sup>2+</sup></small> on the perovskite surface to reduce vacancy-mediated halide migration. The network with fluorinated chains reconfigures the interfacial dielectric landscape, significantly increasing the migration activation barrier for halide vacancies at the perovskite/electron transport layer interface, suppressing ion migration and significantly enchancing longevity. Poly-FPTS-treated tandem devices delivered a power conversion efficiency (PCE) of 26.5%, with a high open-circuit voltage of 2.178 V. A steady-state certified efficiency of 25.1% was achieved in Japan Electrical Safety & Environmental Technology Laboratories (JET), as reported in Solar Cell Efficiency Tables (version 65). Under continuous 1-sun illumination at the maximum power point (ISOS-L-1I protocol), these devices retained 92% of their initial efficiency after 1000 hours, and they exhibited an efficiency loss < 5% after 1056 hours of light–dark cycling (ISOS-LC-1). This work reveals the importance of treating the top perovskite/ETL contact for commercializing perovskite–organic tandem solar cells.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"6 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101833","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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