The oxygen reduction reaction (ORR) lies at the heart of metal–air batteries and emerging sustainable energy technologies; however, the persistent trade-off between catalytic activity and operational durability poses a formidable challenge that impedes real-world deployment. Herein, a sulfur−doped, atomically dispersed Fe,Zr dual−site catalyst (Fe,Zr−SNC) is developed through a facile one−pot synthesis strategy to address the coupled activity−stability limitation of conventional Fe−based ORR catalysts. The catalyst features a polarized Fe coordination center represented by an FeN₃S-like asymmetric configuration adjacent to oxyphilic Zr sites, forming a cooperative dual−site microenvironment for oxygenated−intermediate regulation. Benefiting from this structure, Fe,Zr−SNC exhibits excellent ORR performance with a half−wave potential of 0.913 V, together with a peak power density of 237 mW cm−2 and exceptional long−term stability exceeding 1300 h in zinc−air batteries. Mechanistic studies reveal that the neighboring Zr site provides complementary regulation of oxygenate adsorption through its distinct affinity toward hydroxyl-related intermediates, while the sulfur-modulated Fe coordination center selectively regulates the adsorption and conversion of key oxygenated intermediates (*OOH, *O, and *OH) through a dynamically tunable electronic structure. This site-dependent oxygenate regulation within the cooperative Fe–Zr microenvironment effectively alleviates conventional adsorption coupling and breaks the linear scaling relationship, thereby enabling concurrent enhancement of ORR kinetics and durability.
{"title":"Breaking the Activity-Stability Trade-off in Oxygen Reduction via Sulfur-Modulated Fe–Zr Dual-Site Microenvironment Engineering","authors":"Siqi Qiu,Hao Wan,Yuechao Yao,Xiao Xu,Junzhao Yang,chongyang zeng,Zhangjian Li,Hongliang Wu,Lin Zeng,Jizhao Zou,Tianyi Ma","doi":"10.1039/d6ee05522b","DOIUrl":"https://doi.org/10.1039/d6ee05522b","url":null,"abstract":"The oxygen reduction reaction (ORR) lies at the heart of metal–air batteries and emerging sustainable energy technologies; however, the persistent trade-off between catalytic activity and operational durability poses a formidable challenge that impedes real-world deployment. Herein, a sulfur−doped, atomically dispersed Fe,Zr dual−site catalyst (Fe,Zr−SNC) is developed through a facile one−pot synthesis strategy to address the coupled activity−stability limitation of conventional Fe−based ORR catalysts. The catalyst features a polarized Fe coordination center represented by an FeN₃S-like asymmetric configuration adjacent to oxyphilic Zr sites, forming a cooperative dual−site microenvironment for oxygenated−intermediate regulation. Benefiting from this structure, Fe,Zr−SNC exhibits excellent ORR performance with a half−wave potential of 0.913 V, together with a peak power density of 237 mW cm−2 and exceptional long−term stability exceeding 1300 h in zinc−air batteries. Mechanistic studies reveal that the neighboring Zr site provides complementary regulation of oxygenate adsorption through its distinct affinity toward hydroxyl-related intermediates, while the sulfur-modulated Fe coordination center selectively regulates the adsorption and conversion of key oxygenated intermediates (*OOH, *O, and *OH) through a dynamically tunable electronic structure. This site-dependent oxygenate regulation within the cooperative Fe–Zr microenvironment effectively alleviates conventional adsorption coupling and breaks the linear scaling relationship, thereby enabling concurrent enhancement of ORR kinetics and durability.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"65 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148899292","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}
Yun Bai,Ting Sun,Jiawen Huang,Jian Peng,Yao Xiao,Wei Kong Pang,Hua Kun Liu,Shi Xue Dou,Chao Wu
Anode-free sodium metal batteries (AFSMBs) promise high energy density and sustainability but are substantially hindered by kinetic limitations at low temperatures, where sluggish ion transport and irreversible sodium loss rapidly cause failure. We report a solvent molecular branching strategy that directly drives the antifreezing performance and synergistic solvation of electrolytes for ultra-low temperature AFSMBs. By combining two weakly coordinating, branched ether solvents, 1,2-dimethoxypropane and dipropylene glycol dimethyl ether, we create a mixed electrolyte in which a synergistic solvation of branched solvents lowers the overall solvation free energy with a low desolvation barrier. The synergistic solvation environment significantly suppresses electrolyte freezing at low temperature. This unique solvation environment results in a high ionic conductivity down to −80 °C. As a result, sodium plating and stripping remain highly reversible at −60 °C, achieving a coulombic efficiency of 99.88% for 1000 cycles. When assembled into Ah-level anode-free full batteries, this electrolyte allows stable cycling at −40 °C with nearly no capacity decay over 100 cycles, delivering an energy density of 123.07 Wh kg−1. These results establish molecular branching-driven synergistic solvation as a general design principle for electrolytes operating at extreme temperatures and provide a pathway toward high-energy batteries for cryogenic environments.
无阳极钠金属电池（AFSMBs）承诺高能量密度和可持续性，但在低温下受到动力学限制，离子传输缓慢和不可逆的钠损失会迅速导致故障。我们报道了一种溶剂分子分支策略，该策略直接驱动了超低温afsmb的抗冻性能和电解质的协同溶剂化。通过结合两种弱配位支链醚溶剂，1,2-二甲氧基丙烷和二丙二醇二甲醚，我们创造了一种混合电解质，其中支链溶剂的协同溶剂化降低了整体溶剂化自由能，并具有低的脱溶势垒。协同溶剂化环境显著抑制了电解质在低温下的冻结。这种独特的溶剂化环境导致高离子电导率低至- 80°C。因此，镀钠和剥离在−60°C下保持高度可逆，在1000次循环中实现99.88%的库仑效率。当组装成ah级无阳极全电池时，这种电解质可以在- 40°C下稳定循环，在100次循环中几乎没有容量衰减，提供123.07 Wh kg - 1的能量密度。这些结果确立了分子分支驱动的协同溶剂化作为极端温度下电解质的一般设计原则，并为低温环境下的高能电池提供了一条途径。
{"title":"Solvent molecular branching drives synergistic solvation and antifreezing for ultra-low-temperature anode-free sodium metal batteries","authors":"Yun Bai,Ting Sun,Jiawen Huang,Jian Peng,Yao Xiao,Wei Kong Pang,Hua Kun Liu,Shi Xue Dou,Chao Wu","doi":"10.1039/d6ee03355e","DOIUrl":"https://doi.org/10.1039/d6ee03355e","url":null,"abstract":"Anode-free sodium metal batteries (AFSMBs) promise high energy density and sustainability but are substantially hindered by kinetic limitations at low temperatures, where sluggish ion transport and irreversible sodium loss rapidly cause failure. We report a solvent molecular branching strategy that directly drives the antifreezing performance and synergistic solvation of electrolytes for ultra-low temperature AFSMBs. By combining two weakly coordinating, branched ether solvents, 1,2-dimethoxypropane and dipropylene glycol dimethyl ether, we create a mixed electrolyte in which a synergistic solvation of branched solvents lowers the overall solvation free energy with a low desolvation barrier. The synergistic solvation environment significantly suppresses electrolyte freezing at low temperature. This unique solvation environment results in a high ionic conductivity down to −80 °C. As a result, sodium plating and stripping remain highly reversible at −60 °C, achieving a coulombic efficiency of 99.88% for 1000 cycles. When assembled into Ah-level anode-free full batteries, this electrolyte allows stable cycling at −40 °C with nearly no capacity decay over 100 cycles, delivering an energy density of 123.07 Wh kg−1. These results establish molecular branching-driven synergistic solvation as a general design principle for electrolytes operating at extreme temperatures and provide a pathway toward high-energy batteries for cryogenic environments.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"29 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148899293","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}
Sodium-ion batteries are widely regarded as a promising successor to lithium-ion batteries due to the element abundance in the Earth's crust. The lower energy density of sodium-ion batteries has often led to the assumption that they may offer enhanced safety; however, this may not necessarily be the case. In this study, we compared the thermal failure behavior of sodium-ion and lithium-ion batteries through calorimetric and material characterization tests to evaluate their thermal hazards. The results show that when sodium-ion batteries employ layered oxide cathodes—which are oxidative and can react with the reductive anode—the heat release exhibits a two-stage pattern: Stage I corresponds to the reaction between the anode and the electrolyte, while Stage II involves the reaction between the cathode and the anode. The thermal degradation of the layered oxide cathode follows a P3 → O3 → rock-salt phase transition, which is the driving force for Stage II. In contrast, polyanionic cathodes remain thermally stable up to 500 °C, confining the thermal runaway reaction to Stage I (anode–electrolyte reaction) and resulting in a significantly lower maximum temperature during thermal runaway. Since the cathode structure governs the thermal hazard of the full cell, sodium-ion batteries with polyanionic cathodes (110 Wh·kg⁻¹) exhibit failure temperatures (450–500 °C) comparable to those of lithium-ion batteries with layered oxide cathodes (170 Wh·kg⁻¹). Meanwhile, sodium-ion batteries with layered oxide cathodes (170 Wh·kg⁻¹) reach failure temperatures (900–1100 °C) as high as those of lithium-ion batteries with layered oxide cathodes (230 Wh·kg⁻¹). In summary, we demonstrate that sacrificing energy density does not yield improved safety in sodium-ion batteries. Unless the oxidative instability of layered cathodes is fundamentally resolved, pursuing such sodium-ion batteries offers no net advantage over lithium-ion batteries in terms of safety, energy density, and cost.
{"title":"Sacrificing Energy Density Fails to Deliver Safety: Cathode Structure Determines the Safety of Sodium-ion Batteries","authors":"Junxian Hou,Yinan Ma,Xuning Feng,Chunyan Luo,Li Wang,Xuebing Han,Chengshan Xu,Shilong Wen,Zhiwei Liu,Hui Li,Languang Lu,Yanxia Li,Xiangming He,Cheng Bao,Minggao Ouyang","doi":"10.1039/d6ee04331c","DOIUrl":"https://doi.org/10.1039/d6ee04331c","url":null,"abstract":"Sodium-ion batteries are widely regarded as a promising successor to lithium-ion batteries due to the element abundance in the Earth's crust. The lower energy density of sodium-ion batteries has often led to the assumption that they may offer enhanced safety; however, this may not necessarily be the case. In this study, we compared the thermal failure behavior of sodium-ion and lithium-ion batteries through calorimetric and material characterization tests to evaluate their thermal hazards. The results show that when sodium-ion batteries employ layered oxide cathodes—which are oxidative and can react with the reductive anode—the heat release exhibits a two-stage pattern: Stage I corresponds to the reaction between the anode and the electrolyte, while Stage II involves the reaction between the cathode and the anode. The thermal degradation of the layered oxide cathode follows a P3 → O3 → rock-salt phase transition, which is the driving force for Stage II. In contrast, polyanionic cathodes remain thermally stable up to 500 °C, confining the thermal runaway reaction to Stage I (anode–electrolyte reaction) and resulting in a significantly lower maximum temperature during thermal runaway. Since the cathode structure governs the thermal hazard of the full cell, sodium-ion batteries with polyanionic cathodes (110 Wh·kg⁻¹) exhibit failure temperatures (450–500 °C) comparable to those of lithium-ion batteries with layered oxide cathodes (170 Wh·kg⁻¹). Meanwhile, sodium-ion batteries with layered oxide cathodes (170 Wh·kg⁻¹) reach failure temperatures (900–1100 °C) as high as those of lithium-ion batteries with layered oxide cathodes (230 Wh·kg⁻¹). In summary, we demonstrate that sacrificing energy density does not yield improved safety in sodium-ion batteries. Unless the oxidative instability of layered cathodes is fundamentally resolved, pursuing such sodium-ion batteries offers no net advantage over lithium-ion batteries in terms of safety, energy density, and cost.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"50 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148893367","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}
Yang Liu,Jianfei Fu,Qinyong Tian,Huaiqing Luo,Bolin Zheng,Jiaxing Song,Zaifang Li,Jifeng Wu,Dongsheng Yu,Hai-Qiao Wang,Bin Fan,Wei Chen,Qiuju Liu
Precise control over crystallographic orientation, particularly the preferential (100) facet, is essential for enhancing the performance of perovskite photovoltaics. Here, we introduced a novel zero-dimensional (0D) perovskite based on π-stacked phenyl-1,3,5-triyltrimethanammonium (PTMA3+) cations as a crystal growth promoter. The PTMA-based 0D perovskite directs nucleation and significantly reduces the phase-transformation barrier, enabling the rapid formation of highly crystalline, preferred (100)-oriented perovskite films with superior stability. The corresponding inverted devices deliver a power conversion efficiency of 26.05% (certified, 25.78%) for 0.09 cm2 cells and 24.11% (certified, 24.09%) for 110 cm2 modules, respectively. The advanced module sets a record efficiency and demonstrates exceptional operational stability, retaining over 88% of its initial efficiency after 1200 hours of continuous maximum power point tracking at 85 °C. This work highlights the potential of 0D perovskites as crystalline promoters for producing highly ordered and stable perovskite film.
{"title":"0D Perovskite Directing Oriented Crystallization toward High-Performance Perovskite Solar Cells and Modules","authors":"Yang Liu,Jianfei Fu,Qinyong Tian,Huaiqing Luo,Bolin Zheng,Jiaxing Song,Zaifang Li,Jifeng Wu,Dongsheng Yu,Hai-Qiao Wang,Bin Fan,Wei Chen,Qiuju Liu","doi":"10.1039/d6ee04612f","DOIUrl":"https://doi.org/10.1039/d6ee04612f","url":null,"abstract":"Precise control over crystallographic orientation, particularly the preferential (100) facet, is essential for enhancing the performance of perovskite photovoltaics. Here, we introduced a novel zero-dimensional (0D) perovskite based on π-stacked phenyl-1,3,5-triyltrimethanammonium (PTMA3+) cations as a crystal growth promoter. The PTMA-based 0D perovskite directs nucleation and significantly reduces the phase-transformation barrier, enabling the rapid formation of highly crystalline, preferred (100)-oriented perovskite films with superior stability. The corresponding inverted devices deliver a power conversion efficiency of 26.05% (certified, 25.78%) for 0.09 cm2 cells and 24.11% (certified, 24.09%) for 110 cm2 modules, respectively. The advanced module sets a record efficiency and demonstrates exceptional operational stability, retaining over 88% of its initial efficiency after 1200 hours of continuous maximum power point tracking at 85 °C. This work highlights the potential of 0D perovskites as crystalline promoters for producing highly ordered and stable perovskite film.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"17 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148877537","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}
Francisco Bernal-Texca,Chiara Cortese,Mariia Kramarenko,Quan Liu,Jordi Martorell
An intrinsic limitation of the sunlight to electrical energy conversion originates from three major loss mechanisms: Thermalization, Transmission, and Boltzmann. To overcome such a major drawback in solar cell performance a large amount of effort is currently placed on the fabrication of tandem architectures to reduce transmission and thermalization losses. However, although photon emission is considered to be unavoidable, by restricting the photon angular spread, it should be possible to reduce Boltzmann losses. Here we report on a PM6:Y6 inverted solar cell where photon emission is inhibited, leading to the highest power conversion efficiency to date for solar cells based on this particular configuration. Our work sets the path for matching the photon emission and the sunlight absorption cones, which can lead to open-circuit voltage Boltzmann loss suppression, thereby pushing the efficiency in planar single-junction solar cells far beyond the detailed balance limit which assumes radiative recombination being unavoidable.
{"title":"Inhibited photon emission to overcome Boltzmann losses in a cavity configuration organic solar cell","authors":"Francisco Bernal-Texca,Chiara Cortese,Mariia Kramarenko,Quan Liu,Jordi Martorell","doi":"10.1039/d6ee03772k","DOIUrl":"https://doi.org/10.1039/d6ee03772k","url":null,"abstract":"An intrinsic limitation of the sunlight to electrical energy conversion originates from three major loss mechanisms: Thermalization, Transmission, and Boltzmann. To overcome such a major drawback in solar cell performance a large amount of effort is currently placed on the fabrication of tandem architectures to reduce transmission and thermalization losses. However, although photon emission is considered to be unavoidable, by restricting the photon angular spread, it should be possible to reduce Boltzmann losses. Here we report on a PM6:Y6 inverted solar cell where photon emission is inhibited, leading to the highest power conversion efficiency to date for solar cells based on this particular configuration. Our work sets the path for matching the photon emission and the sunlight absorption cones, which can lead to open-circuit voltage Boltzmann loss suppression, thereby pushing the efficiency in planar single-junction solar cells far beyond the detailed balance limit which assumes radiative recombination being unavoidable.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"74 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148877540","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}
Electrochemically redox-active halide (eREAL) materials are an emerging class of materials that combine high Li-ion conductivity with transition-metal redox activity, making them promising candidates for cathode or catholyte applications. As a redox-active catholyte, they could significantly increase the energy density of solid-state batteries. In this work, we perform first-principles calculations on Li–M–Cl (M = 3d transition metals) ternaries to establish such a theoretical foundation for their stability and electrochemical activity. We map the phase stability of eREAL structures with varying metal-to-Cl ratio, transition-metal species, oxidation states, and anion frameworks, and compute cation and anion redox potentials. We find that the high ionicity of metal–Cl bonds elevates cation redox potentials above those of conventional oxide cathodes, but also will promote Cl oxidation and Cl–Cl dimerization at high voltages, which may limit the stability of these materials. Anion substitution effectively tunes both cation and anion redox potentials, with F substitution standing out as a viable route to extend the reversible voltage window. Beyond the anion redox issue, eREAL compounds generally exhibit flat voltage profiles, which potentially poses an electrochemical compatibility challenge when paired with active materials that operate at different voltage values or over wider voltage ranges. Collectively, our study provides a comprehensive analysis for redox behavior of eREAL materials, paving the way for their rational design and optimization in next-generation battery applications.
{"title":"Redox-active halide materials for cathode applications","authors":"Zhuohan Li,Gerbrand Ceder","doi":"10.1039/d6ee03881f","DOIUrl":"https://doi.org/10.1039/d6ee03881f","url":null,"abstract":"Electrochemically redox-active halide (eREAL) materials are an emerging class of materials that combine high Li-ion conductivity with transition-metal redox activity, making them promising candidates for cathode or catholyte applications. As a redox-active catholyte, they could significantly increase the energy density of solid-state batteries. In this work, we perform first-principles calculations on Li–M–Cl (M = 3d transition metals) ternaries to establish such a theoretical foundation for their stability and electrochemical activity. We map the phase stability of eREAL structures with varying metal-to-Cl ratio, transition-metal species, oxidation states, and anion frameworks, and compute cation and anion redox potentials. We find that the high ionicity of metal–Cl bonds elevates cation redox potentials above those of conventional oxide cathodes, but also will promote Cl oxidation and Cl–Cl dimerization at high voltages, which may limit the stability of these materials. Anion substitution effectively tunes both cation and anion redox potentials, with F substitution standing out as a viable route to extend the reversible voltage window. Beyond the anion redox issue, eREAL compounds generally exhibit flat voltage profiles, which potentially poses an electrochemical compatibility challenge when paired with active materials that operate at different voltage values or over wider voltage ranges. Collectively, our study provides a comprehensive analysis for redox behavior of eREAL materials, paving the way for their rational design and optimization in next-generation battery applications.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"22 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148877542","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}
Hanlin Sun,Yikui Gao,Zhihao Zhao,Xiaocheng Sun,Zilou Liu,Zhiwei Li,Jing-Shan Zhao,Zhong Lin Wang,Jie Wang
Triboelectric nanogenerators (TENGs) are well-suited to high-voltage power-source design because of their high-voltage, low current characteristics. However, the reliance on simplified ideal voltage models and a limited understanding of energy cycling mechanisms have restricted the potential for optimizing output voltage and charge utilization efficiency. Building upon the intrinsic V–Q characteristics of TENGs, this paper identifies the flattening of the energy cycle curve as a key factor limiting charge utilization efficiency in practical high-voltage applications and establishes a correlation between charge utilization efficiency and the theoretical maximum open-circuit voltage. Meanwhile, a theoretical model for the open-circuit voltage of the contact–separation-mode TENGs (CS-TENGs) in practical applications was developed, considering edge effects and parasitic capacitance. Building on this model, the sensitivity of the optimized parameters was analyzed, providing valuable insights into the standardization of high-voltage power supply designs. A series of effective ways were utilized to avoid the flattening of the V–Q curve, thereby improving charge utilization efficiency. Ultimately, a record-breaking output was achieved, with an ultra-high voltage exceeding 20 kV and exceptional durability over 11 million cycles. Rapid air purification within 1 min demonstrates the effectiveness of the proposed device, highlighting its potential for self-powered high-voltage technologies in environmental and energy applications.
{"title":"Achieving ultra-high voltage triboelectric nanogenerators and improving charge utilization efficiency","authors":"Hanlin Sun,Yikui Gao,Zhihao Zhao,Xiaocheng Sun,Zilou Liu,Zhiwei Li,Jing-Shan Zhao,Zhong Lin Wang,Jie Wang","doi":"10.1039/d6ee04137j","DOIUrl":"https://doi.org/10.1039/d6ee04137j","url":null,"abstract":"Triboelectric nanogenerators (TENGs) are well-suited to high-voltage power-source design because of their high-voltage, low current characteristics. However, the reliance on simplified ideal voltage models and a limited understanding of energy cycling mechanisms have restricted the potential for optimizing output voltage and charge utilization efficiency. Building upon the intrinsic V–Q characteristics of TENGs, this paper identifies the flattening of the energy cycle curve as a key factor limiting charge utilization efficiency in practical high-voltage applications and establishes a correlation between charge utilization efficiency and the theoretical maximum open-circuit voltage. Meanwhile, a theoretical model for the open-circuit voltage of the contact–separation-mode TENGs (CS-TENGs) in practical applications was developed, considering edge effects and parasitic capacitance. Building on this model, the sensitivity of the optimized parameters was analyzed, providing valuable insights into the standardization of high-voltage power supply designs. A series of effective ways were utilized to avoid the flattening of the V–Q curve, thereby improving charge utilization efficiency. Ultimately, a record-breaking output was achieved, with an ultra-high voltage exceeding 20 kV and exceptional durability over 11 million cycles. Rapid air purification within 1 min demonstrates the effectiveness of the proposed device, highlighting its potential for self-powered high-voltage technologies in environmental and energy applications.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"43 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148877581","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}
Wide-bandgap mixed-halide perovskites are the cornerstone of next-generation perovskite/silicon tandem solar cells, yet their operational stability remains a fundamental barrier to commercial deployment. Two distinct instabilities, δ-phase impurity formation during crystallization and light-induced halide phase segregation under operation, share a common thermodynamic origin in the compositional mismatch of mixed halides, yet have so far required separate mitigation strategies. Here, we report an interface-triggered gradient doping strategy via rubidium fluoride (RbF) surface post-treatment that resolves both instabilities through a single chemical event. The exceptionally high electronegativity of F− drives preferential coordination to surface Pb2+, anchoring fluoride at the interface while liberating Rb+ to diffuse into the bulk and establish a continuous concentration gradient. This gradient distribution simultaneously raises the δ-phase formation barrier to promote α-phase purification, elevates the halide migration barrier to suppress polaron-driven phase segregation, and reconstructs the perovskite/electron-transporting layer interface into a dual-step conduction band cascade that minimizes extraction losses. The resulting single-junction device achieves a power conversion efficiency (PCE) of 23.5% with 94% retention after 1000 h under ISOS-L-2I conditions. Integrated into monolithic perovskite/silicon tandems, the strategy delivers a PCE of 32.66% (certified 31.93%) with 91% retention after 1000 h under ISOS-L-1. This work establishes surface-initiated bulk modification as a conceptually distinct and scalable route to operationally stable wide-bandgap perovskites, broadening the chemical toolkit for engineering mixed-halide systems beyond conventional bulk additive approaches.
宽禁带混合卤化物钙钛矿是下一代钙钛矿/硅串联太阳能电池的基石，但其运行稳定性仍然是商业部署的根本障碍。两种不同的不稳定性，结晶过程中的δ相杂质形成和光致卤化物相偏析，在混合卤化物的成分不匹配中具有共同的热力学根源，但迄今为止需要单独的缓解策略。在这里，我们报告了一种通过氟化铷（RbF）表面后处理的界面触发梯度掺杂策略，该策略通过单一化学事件解决了这两种不稳定性。F−异常高的电负性驱动了对Pb2+表面的优先配位，将氟化物锚定在界面上，同时释放Rb+扩散到体中并建立连续的浓度梯度。这种梯度分布同时提高了δ-相形成势垒以促进α-相净化，提高了卤化物迁移势垒以抑制极化子驱动的相偏析，并将钙钛矿/电子输运层界面重构为双阶导带级联，使萃取损失最小化。所得的单结器件在iso - l - 2i条件下，功率转换效率（PCE）达到23.5%，1000小时后保持率为94%。集成到单片钙钛矿/硅串联中，该策略提供了32.66%（认证31.93%）的PCE，在iso - l -1下1000小时后保持91%。这项工作建立了表面引发的体改性作为一种在概念上独特且可扩展的方法来稳定宽禁带钙钛矿，拓宽了工程混合卤化物系统的化学工具箱，超越了传统的体添加剂方法。
{"title":"Surface-initiated gradient doping for efficient and stable perovskite/silicon tandem solar cells","authors":"Ziyue Feng,Jungan Wang,Hongjae Shim,Mingrui He,Ziheng Liu,Robert Patterson,Xinyu Zhang,Hao Jin,Kaiwen Sun,Jan Seidel,Menglei Xu,Zhen Li,Xiaojing Hao","doi":"10.1039/d6ee04055a","DOIUrl":"https://doi.org/10.1039/d6ee04055a","url":null,"abstract":"Wide-bandgap mixed-halide perovskites are the cornerstone of next-generation perovskite/silicon tandem solar cells, yet their operational stability remains a fundamental barrier to commercial deployment. Two distinct instabilities, δ-phase impurity formation during crystallization and light-induced halide phase segregation under operation, share a common thermodynamic origin in the compositional mismatch of mixed halides, yet have so far required separate mitigation strategies. Here, we report an interface-triggered gradient doping strategy via rubidium fluoride (RbF) surface post-treatment that resolves both instabilities through a single chemical event. The exceptionally high electronegativity of F− drives preferential coordination to surface Pb2+, anchoring fluoride at the interface while liberating Rb+ to diffuse into the bulk and establish a continuous concentration gradient. This gradient distribution simultaneously raises the δ-phase formation barrier to promote α-phase purification, elevates the halide migration barrier to suppress polaron-driven phase segregation, and reconstructs the perovskite/electron-transporting layer interface into a dual-step conduction band cascade that minimizes extraction losses. The resulting single-junction device achieves a power conversion efficiency (PCE) of 23.5% with 94% retention after 1000 h under ISOS-L-2I conditions. Integrated into monolithic perovskite/silicon tandems, the strategy delivers a PCE of 32.66% (certified 31.93%) with 91% retention after 1000 h under ISOS-L-1. This work establishes surface-initiated bulk modification as a conceptually distinct and scalable route to operationally stable wide-bandgap perovskites, broadening the chemical toolkit for engineering mixed-halide systems beyond conventional bulk additive approaches.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"43 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148877627","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) exhibits a pronounced non-Nernstian pH dependence, yet its microscopic origin remains unclear. Here, we anchor Pd single atoms on grain-boundary-engineered RuO2 (Pd–GB–RuO2) as a model system, creating an atomically short spillover network to track pH-dependent pathway switching. Operando experiments and theoretical calculations reveal a pH-adaptive intermediate spillover mechanism. Varying pH rebalances competitive adsorption of intermediates and switches the dominant spillover behavior: *H spillover dominates in an acidic electrolyte, whereas coupled *H/*OH spillover operates in an alkaline electrolyte. Pd–GB–RuO2 delivers overpotentials of 13.6 mV (0.5 M H2SO4) and 9.4 mV (1 M KOH) at 10 mA cm−2, and remains stable for 3000 hours. Moreover, the Pd–GB–RuO2 catalyst achieves 1 A cm−2 at 1.60 V in a proton exchange membrane water electrolyser (PEMWE) and 1.65 V in an anion exchange membrane water electrolyser (AEMWE). These findings deepen the mechanistic understanding for the pH effect and offer a design principle for pH-universal HER catalysts.
析氢反应（HER）表现出明显的非能斯特pH依赖性，但其微观起源仍不清楚。在这里，我们将Pd单原子锚定在晶界工程的RuO2 （Pd - gb - RuO2）上作为模型系统，创建了一个原子短溢出网络来跟踪ph依赖的途径切换。实验和理论计算揭示了一种ph值自适应的中间溢出机制。不同的pH值重新平衡了中间产物的竞争性吸附，并改变了主要的溢出行为：*H溢出在酸性电解质中占主导地位，而耦合的*H/*OH溢出在碱性电解质中起作用。Pd-GB-RuO2在10 mA cm−2下可提供13.6 mV （0.5 M H2SO4）和9.4 mV （1 M KOH）的过电位，并保持稳定3000小时。此外，Pd-GB-RuO2催化剂在质子交换膜水电解槽（PEMWE）和阴离子交换膜水电解槽（AEMWE）中分别在1.60 V和1.65 V下达到1 A cm - 2。这些发现加深了对pH效应的机理理解，并提供了pH通用HER催化剂的设计原则。
{"title":"Switchable intermediate spillover illuminates the pH effect in hydrogen evolution on Pd-doped grain-boundary-engineered RuO","authors":"Jiabao Huang,Jiaqi Wan,Chengzong Yuan,Luocai Yi,Fangren Qian,Jiahui Luo,Tianjun Wu,Chengsi Hu,Xinlu Liu,Zhenhai Wen,Lei Liu,Zonghua Pu,Qingjun Chen","doi":"10.1039/d6ee02543a","DOIUrl":"https://doi.org/10.1039/d6ee02543a","url":null,"abstract":"The hydrogen evolution reaction (HER) exhibits a pronounced non-Nernstian pH dependence, yet its microscopic origin remains unclear. Here, we anchor Pd single atoms on grain-boundary-engineered RuO2 (Pd–GB–RuO2) as a model system, creating an atomically short spillover network to track pH-dependent pathway switching. Operando experiments and theoretical calculations reveal a pH-adaptive intermediate spillover mechanism. Varying pH rebalances competitive adsorption of intermediates and switches the dominant spillover behavior: *H spillover dominates in an acidic electrolyte, whereas coupled *H/*OH spillover operates in an alkaline electrolyte. Pd–GB–RuO2 delivers overpotentials of 13.6 mV (0.5 M H2SO4) and 9.4 mV (1 M KOH) at 10 mA cm−2, and remains stable for 3000 hours. Moreover, the Pd–GB–RuO2 catalyst achieves 1 A cm−2 at 1.60 V in a proton exchange membrane water electrolyser (PEMWE) and 1.65 V in an anion exchange membrane water electrolyser (AEMWE). These findings deepen the mechanistic understanding for the pH effect and offer a design principle for pH-universal HER catalysts.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"11 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148877541","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}
Haifan Li,Quan Quan,Dongchang He,Yuxuan Zhang,Boxiang Gao,Lin Su,Mengxue Chen,Dong Chen,Di Yin,Pengshan Xie,Siliang Hu,Mingqi Ding,Jianbo Wu,Chun-Yuen Wong,Johnny C Ho
Ruthenium oxide (RuO2) is commonly used as an anode material in proton exchange membrane water electrolysis (PEMWE). Still, it suffers from a trade-off between activity and stability due to excessive Ru-O covalency, which exacerbates lattice oxygen loss via the lattice oxygen mechanism (LOM). In this study, we introduce a synergistic approach by incorporating cobalt single atoms and RuO2/TiO2 heterointerfaces on RuO 2 clusters (CoSA-RuO2/TiO2) to modulate Ru-O covalency.This strategy facilitates a domainant adsorbate evolution mechanism (AEM) and regulates interfacial water dissociation, enhancing both intrinsic activity and stability.The optimized design achieves an ultralow overpotential of 151 mV at 10 mA cm-2 for acid oxygen evolution reaction (OER) and demonstrates remarkable durability of 1000 hours in a PEMWE cell under pulsed currents (0~100 mA cm-2). In situ/operando characterizations and theoretical calculations reveal that the Co-SAs and RuO2/TiO2 heterointerfaces extend the Ru-O bond and reduce the Ru oxidation state. This optimized electronic structure weakens Ru-O covalency, stabilizes lattice oxygen, and suppresses LOM, favoring a dominant AEM pathway. Moreover, the engineered interface reduces the interfacial hydrogen-bonding network, as revealed by ab initio molecular dynamics (AIMD), thus facilitating water dissociation and accelerating proton transfer kinetics. This work underscores the potential of precisely modulating metaloxygen bonds through interfacial and single-atom synergy to overcome the activitystability challenge in oxide electrocatalysis.
氧化钌（RuO2）是质子交换膜电解（PEMWE）中常用的阳极材料。然而，由于过量的Ru-O共价，它在活性和稳定性之间存在权衡，这加剧了通过晶格氧机制（LOM）的晶格氧损失。在这项研究中，我们引入了一种协同方法，通过在RuO2簇（CoSA-RuO2/TiO2）上结合钴单原子和RuO2/TiO2异质界面来调节Ru-O共价。该策略促进了domainant吸附物演化机制（AEM）并调节了界面水解离，增强了内在活性和稳定性。优化后的设计在10 mA cm-2下实现了151 mV的超低过电位，用于酸性析氧反应（OER），并且在脉冲电流（0~100 mA cm-2）下PEMWE电池中具有1000小时的显着耐久性。原位/operando表征和理论计算表明，Co-SAs和RuO2/TiO2异质界面扩展了Ru- o键，降低了Ru的氧化态。这种优化的电子结构削弱了Ru-O共价，稳定了晶格氧，抑制了LOM，有利于AEM的主导途径。此外，从头算分子动力学（AIMD）表明，工程界面减少了界面氢键网络，从而促进了水的解离和质子转移动力学的加速。这项工作强调了通过界面和单原子协同作用精确调节金属氧键的潜力，以克服氧化物电催化中活性稳定性的挑战。
{"title":"Engineering Ru-O covalency to trigger mechanism transition for fast-response proton exchange membrane water electrolysis","authors":"Haifan Li,Quan Quan,Dongchang He,Yuxuan Zhang,Boxiang Gao,Lin Su,Mengxue Chen,Dong Chen,Di Yin,Pengshan Xie,Siliang Hu,Mingqi Ding,Jianbo Wu,Chun-Yuen Wong,Johnny C Ho","doi":"10.1039/d6ee03666j","DOIUrl":"https://doi.org/10.1039/d6ee03666j","url":null,"abstract":"Ruthenium oxide (RuO2) is commonly used as an anode material in proton exchange membrane water electrolysis (PEMWE). Still, it suffers from a trade-off between activity and stability due to excessive Ru-O covalency, which exacerbates lattice oxygen loss via the lattice oxygen mechanism (LOM). In this study, we introduce a synergistic approach by incorporating cobalt single atoms and RuO2/TiO2 heterointerfaces on RuO 2 clusters (CoSA-RuO2/TiO2) to modulate Ru-O covalency.This strategy facilitates a domainant adsorbate evolution mechanism (AEM) and regulates interfacial water dissociation, enhancing both intrinsic activity and stability.The optimized design achieves an ultralow overpotential of 151 mV at 10 mA cm-2 for acid oxygen evolution reaction (OER) and demonstrates remarkable durability of 1000 hours in a PEMWE cell under pulsed currents (0~100 mA cm-2). In situ/operando characterizations and theoretical calculations reveal that the Co-SAs and RuO2/TiO2 heterointerfaces extend the Ru-O bond and reduce the Ru oxidation state. This optimized electronic structure weakens Ru-O covalency, stabilizes lattice oxygen, and suppresses LOM, favoring a dominant AEM pathway. Moreover, the engineered interface reduces the interfacial hydrogen-bonding network, as revealed by ab initio molecular dynamics (AIMD), thus facilitating water dissociation and accelerating proton transfer kinetics. This work underscores the potential of precisely modulating metaloxygen bonds through interfacial and single-atom synergy to overcome the activitystability challenge in oxide electrocatalysis.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"4 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148877535","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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