Jie Miao, Haonan Wang, Nan He, Bingsen Wang, Mengting Zhang, Dawei Tang, Lin Li
Moisture energy harvesting holds immense potential for sustained electricity generation, yet its practical deployment is hindered by the inherent instability of water–ion gradients, leading to rapid performance degradation and limited scalability. Here, we present a dual-layer hydrogel platform driven by asymmetric ionic hydration chemistries, creating persistent water–salt gradients for sustained energy harvesting. The system leverages distinct ionic hydration dynamics, where the LiCl layer maximizes ionic dissociation and water adsorption while the Li2CO3 layer stabilizes the water content through moderate ionic binding. This water–salt dual gradient design induces persistent osmotic pressure differentials, enabling synchronized water–ion migration and continuous ionic transport. Our platform shows a significant improvement in current density compared to conventional long-duration moisture energy generators (MEGs), achieving a peak current density of 96.4 µA cm−2 and a power density of 5.06 µW cm−2, while maintaining stable operation for over 500 h. Additionally, we introduce a highly scalable MEG platform, with an active surface area of 1000 cm2, enabling energy harvesting at scales previously unattainable. This work demonstrates a scalable and durable MEG platform capable of sustainable energy generation in diverse environments, paving the way for self-powered wearable electronics, environmental monitoring, and autonomous sensing technologies.
水分能量收集在持续发电方面具有巨大的潜力，但其实际部署受到水离子梯度固有的不稳定性的阻碍，导致性能迅速下降和可扩展性有限。在这里，我们提出了一个由不对称离子水化化学驱动的双层水凝胶平台，为持续的能量收集创造了持久的水盐梯度。该系统利用了独特的离子水合动力学，其中LiCl层最大限度地发挥了离子解离和水吸附作用，而Li2CO3层通过适度的离子结合稳定了水的含量。这种水盐双梯度设计诱导了持续的渗透压差，使同步的水离子迁移和连续的离子传输成为可能。与传统的长时间湿能发生器（MEG）相比，我们的平台在电流密度上有了显著的改善，实现了96.4 μ a cm - 2的峰值电流密度和5.06 μ W cm - 2的功率密度，同时保持了500小时以上的稳定运行。此外，我们引入了一个高度可扩展的MEG平台，其有效表面积为1000 cm2，能够实现以前无法实现的规模的能量收集。这项工作展示了一个可扩展和耐用的MEG平台，能够在各种环境中可持续地发电，为自供电可穿戴电子设备、环境监测和自主传感技术铺平了道路。
{"title":"An estuarine-inspired dual-gradient hydrogel for stable and scalable moisture energy harvesting up to a single-module 100 mA output","authors":"Jie Miao, Haonan Wang, Nan He, Bingsen Wang, Mengting Zhang, Dawei Tang, Lin Li","doi":"10.1039/d5ee04508h","DOIUrl":"https://doi.org/10.1039/d5ee04508h","url":null,"abstract":"Moisture energy harvesting holds immense potential for sustained electricity generation, yet its practical deployment is hindered by the inherent instability of water–ion gradients, leading to rapid performance degradation and limited scalability. Here, we present a dual-layer hydrogel platform driven by asymmetric ionic hydration chemistries, creating persistent water–salt gradients for sustained energy harvesting. The system leverages distinct ionic hydration dynamics, where the LiCl layer maximizes ionic dissociation and water adsorption while the Li<small><sub>2</sub></small>CO<small><sub>3</sub></small> layer stabilizes the water content through moderate ionic binding. This water–salt dual gradient design induces persistent osmotic pressure differentials, enabling synchronized water–ion migration and continuous ionic transport. Our platform shows a significant improvement in current density compared to conventional long-duration moisture energy generators (MEGs), achieving a peak current density of 96.4 µA cm<small><sup>−2</sup></small> and a power density of 5.06 µW cm<small><sup>−2</sup></small>, while maintaining stable operation for over 500 h. Additionally, we introduce a highly scalable MEG platform, with an active surface area of 1000 cm<small><sup>2</sup></small>, enabling energy harvesting at scales previously unattainable. This work demonstrates a scalable and durable MEG platform capable of sustainable energy generation in diverse environments, paving the way for self-powered wearable electronics, environmental monitoring, and autonomous sensing technologies.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"88 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116206","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}
Dengxu Wu, Ziqi Zhang, Lutong Wang, Lei Zhu, Hong Li, Liquan Chen, Fan Wu
All-solid-state lithium batteries (ASSLBs) face critical challenges in practical implementation due to excessive stack pressure requirements and interfacial degradation. To solve the solid-solid interfacial contact problem, we propose a dual interfacial engineering strategy combining nano-engineered Li6-xPS5-xCl1+x (LPSCl) electrolytes (D₅₀=0.36 μm) with a self-adaptive polyethylene-vinyl acetate/lithium difluoro(oxalato)borate (PEVA-LiDFOB) composite glue. This design establishes robust ionic networks while dynamically maintains interfacial integrity through viscoelastic stress accommodation. The interfacial electrochemical stability on the cathode side is significantly enhanced, and the interfacial side reactions are effectively suppressed. The optimized ASSLBs with Li metal anode achieve outstanding cyclability with 90.6% capacity retention over 1000 cycles at 1C and 61.4% after 9000 cycles at 2C under 10 MPa and RT. Practical pouch cells demonstrate 90.6% capacity retention after 100 cycles under 2 MPa pressure and RT. This work provides universal interfacial design principles for developing pressure-resilient ASSLB system.
{"title":"Self-adaptive Interfacial Glue for Low-pressure Sulfide-Based All-Solid-State Lithium Metal Batteries","authors":"Dengxu Wu, Ziqi Zhang, Lutong Wang, Lei Zhu, Hong Li, Liquan Chen, Fan Wu","doi":"10.1039/d5ee06207a","DOIUrl":"https://doi.org/10.1039/d5ee06207a","url":null,"abstract":"All-solid-state lithium batteries (ASSLBs) face critical challenges in practical implementation due to excessive stack pressure requirements and interfacial degradation. To solve the solid-solid interfacial contact problem, we propose a dual interfacial engineering strategy combining nano-engineered Li6-xPS5-xCl1+x (LPSCl) electrolytes (D₅₀=0.36 μm) with a self-adaptive polyethylene-vinyl acetate/lithium difluoro(oxalato)borate (PEVA-LiDFOB) composite glue. This design establishes robust ionic networks while dynamically maintains interfacial integrity through viscoelastic stress accommodation. The interfacial electrochemical stability on the cathode side is significantly enhanced, and the interfacial side reactions are effectively suppressed. The optimized ASSLBs with Li metal anode achieve outstanding cyclability with 90.6% capacity retention over 1000 cycles at 1C and 61.4% after 9000 cycles at 2C under 10 MPa and RT. Practical pouch cells demonstrate 90.6% capacity retention after 100 cycles under 2 MPa pressure and RT. This work provides universal interfacial design principles for developing pressure-resilient ASSLB system.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"80 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089766","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}
Shihao Duan, Shuoqing Zhang, Xiaoteng Huang, Haikuo Zhang, Ruhong Li, Long Chen, Jinze Wang, Sheng Dai, Guorong Wang, Feng Guo, Xuezhang Xiao, Huilin Pan, Lixin Chen, Tao Deng, Xiulin Fan
Ah-level anode-free Li metal batteries (AFLMBs) exhibit the highest theoretical energy density for rechargeable batteries; however, their practical application is hindered by serious electrolyte depletion and active Li consumption. The insufficiently protective solid electrolyte interphase (SEI) limits the Li retention during the prolonged cycling. Here we establish two criteria, i.e., electron resonance energy and exchange repulsion energy, using the principle of electron resonance to facilitate the formation of stable SEI with high content of anion reduction products. Based on this principle, fractional electron transfer from anions to solvent molecules helps decrease the electron density around the anions, thereby facilitating the preferential reduction of anions. This electron resonance mechanism effectively promotes the incorporation of anion-decomposition products into the SEI, mitigating electrolyte consumption and dead Li formation. Additionally, battery stability is improved through the anode-free configuration in the optimized electrolyte due to the reduced galvanic corrosion and Li metal inventory. Using an electrolyte enlighted by electron resonance effect, an anode-free Cu||LiNi0.8Mn0.1Co0.1O2 pouch cell with a 15-Ah capacity was assembled, achieving a high energy density of 500 Wh kg-1 with excellent reversibility. This study offers insights into advanced electrolyte design, focusing on anion-decomposed interphase to boost the stable application of Ah-level AFLMBs.
{"title":"Stable 15-Ah Anode-Free Li Pouch Cell Enabled by Electron Resonance Effect","authors":"Shihao Duan, Shuoqing Zhang, Xiaoteng Huang, Haikuo Zhang, Ruhong Li, Long Chen, Jinze Wang, Sheng Dai, Guorong Wang, Feng Guo, Xuezhang Xiao, Huilin Pan, Lixin Chen, Tao Deng, Xiulin Fan","doi":"10.1039/d5ee06811h","DOIUrl":"https://doi.org/10.1039/d5ee06811h","url":null,"abstract":"Ah-level anode-free Li metal batteries (AFLMBs) exhibit the highest theoretical energy density for rechargeable batteries; however, their practical application is hindered by serious electrolyte depletion and active Li consumption. The insufficiently protective solid electrolyte interphase (SEI) limits the Li retention during the prolonged cycling. Here we establish two criteria, i.e., electron resonance energy and exchange repulsion energy, using the principle of electron resonance to facilitate the formation of stable SEI with high content of anion reduction products. Based on this principle, fractional electron transfer from anions to solvent molecules helps decrease the electron density around the anions, thereby facilitating the preferential reduction of anions. This electron resonance mechanism effectively promotes the incorporation of anion-decomposition products into the SEI, mitigating electrolyte consumption and dead Li formation. Additionally, battery stability is improved through the anode-free configuration in the optimized electrolyte due to the reduced galvanic corrosion and Li metal inventory. Using an electrolyte enlighted by electron resonance effect, an anode-free Cu||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> pouch cell with a 15-Ah capacity was assembled, achieving a high energy density of 500 Wh kg<small><sup>-1</sup></small> with excellent reversibility. This study offers insights into advanced electrolyte design, focusing on anion-decomposed interphase to boost the stable application of Ah-level AFLMBs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"1 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146070661","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}
Aqueous zinc–iodine (Zn–I2) batteries are promising candidates for large-scale energy storage due to inherent safety and environmental compatibility. However, their application is hindered by serious polyiodides shuttling, limited iodine conversion kinetics, and poor Zn anode reversibility. Here, we report a water-responsive molecular strategy to simultaneously address these challenges for advanced Zn–I2 batteries. When introduced into the electrolyte, Ectoine (Ect) spontaneously establishes localized dual-polarity charge centers. The positive center immobilizes polyiodides and mitigates their shuttling, while the negative site coordinates with Zn2+ to reshape its solvation environment and markedly improve Zn reversibility. Importantly, hydrogen bonding between Ect and polyiodides modulates the iodine conversion pathway and enhances its redox kinetics, even under high iodine loadings. Consequently, the Zn–I2 coin cell with Ect exhibits record cycling stability (60,000 cycles at 50 C) and high-rate capability (139.4 mAh g−1 at 50 C). The Zn–I2 pouch cell with high I2 loading of ~20 mgiodine cm−2 and 65% Zn utilization rate retains 80% of capacity after over 1,000 cycles. This finding offers a scalable electrolyte design for next-generation aqueous batteries, advancing their potential for practical large-scale energy storage.
锌-碘（Zn-I2）水电池由于其固有的安全性和环境兼容性，是大规模储能的有希望的候选者。然而，它们的应用受到严重的多碘化物穿梭、碘转化动力学有限和锌阳极可逆性差的阻碍。在这里，我们报告了一种水响应分子策略，以同时解决先进锌- i2电池的这些挑战。当引入电解质时，Ectoine （Ect）自发地建立局部双极性电荷中心。正电荷中心固定了多碘化物并减轻了它们的穿梭，而负电荷中心与Zn2+配合，重塑了其溶剂化环境，显著提高了Zn的可逆性。重要的是，即使在高碘负荷下，Ect和多碘之间的氢键也能调节碘转化途径并增强其氧化还原动力学。因此，具有Ect的Zn-I2硬币电池具有创纪录的循环稳定性（50℃下60,000次循环）和高倍率容量（50℃下139.4 mAh g−1）。高I2负荷量为~20 mg - cm - 2，锌利用率为65%的Zn - I2袋电池在1000次循环后仍能保持80%的容量。这一发现为下一代水性电池提供了一种可扩展的电解质设计，提高了它们在实际大规模储能方面的潜力。
{"title":"Water-Responsive Molecule Realizes Stable Ah-Scale Zn–I2 Pouch Cells with High Zn Utilization","authors":"Yiyang Hu, shao-jian zhang, Han Wu, Qianru Chen, Pengfang Zhang, Junnan Hao, Shizhang Qiao","doi":"10.1039/d5ee06986f","DOIUrl":"https://doi.org/10.1039/d5ee06986f","url":null,"abstract":"Aqueous zinc–iodine (Zn–I2) batteries are promising candidates for large-scale energy storage due to inherent safety and environmental compatibility. However, their application is hindered by serious polyiodides shuttling, limited iodine conversion kinetics, and poor Zn anode reversibility. Here, we report a water-responsive molecular strategy to simultaneously address these challenges for advanced Zn–I2 batteries. When introduced into the electrolyte, Ectoine (Ect) spontaneously establishes localized dual-polarity charge centers. The positive center immobilizes polyiodides and mitigates their shuttling, while the negative site coordinates with Zn2+ to reshape its solvation environment and markedly improve Zn reversibility. Importantly, hydrogen bonding between Ect and polyiodides modulates the iodine conversion pathway and enhances its redox kinetics, even under high iodine loadings. Consequently, the Zn–I2 coin cell with Ect exhibits record cycling stability (60,000 cycles at 50 C) and high-rate capability (139.4 mAh g−1 at 50 C). The Zn–I2 pouch cell with high I2 loading of ~20 mgiodine cm−2 and 65% Zn utilization rate retains 80% of capacity after over 1,000 cycles. This finding offers a scalable electrolyte design for next-generation aqueous batteries, advancing their potential for practical large-scale energy storage.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"219 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146056968","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}
Zhenwei Li, Zhiyu Zou, Hengyuan Hu, Jie Chen, Mengchuang Liu, Ping Liu, Wenhua Zhang, Chang Lu, Zhaoxin Meng, Yongqiang Ji, Jie Yu, Meisheng Han, Yuliang Cao
Understanding and regulating the interfacial Na+-storage kinetics of MoS2 anodes remains a key challenge for sodium-ion batteries. Here, Co-doped MoS2 is employed as a model to elucidate, from the perspective of the dynamic evolution of spin-polarized electrons, a magnetoelectric coupling-dominated mechanism that accelerates interfacial Na+ storage. During the conversion reaction, Co atoms doped into the MoS2 lattice generate ~ 4 nm Co0 nanocrystals. In-situ magnetometry reveals that the spin-split bands of these magnetic Co0 nanocrystals effectively accommodate spin-polarized electrons, thereby generating a spin-polarized surface capacitive effect (“magnetic” contribution), which in turn enables ultrafast Na+ storage at the Co0/Na2S interfaces. Moreover, a portion of spin-polarized electrons stored in Co0 nanocrystals are transferred to electrolyte molecules, catalyzing their directional decomposition and promoting the formation of NaF-riched solid electrolyte interphase (“electric” contribution). Benefiting from this magnetoelectric coupling effect, the Co-doped MoS2 electrode exhibits excellent fast-charging capability in both half cells and full cells. This study not only establishes a direct link between spin-polarized electron dynamics and interfacial reaction pathways, but also provides important insights for the co-design of heterogeneous catalysis and interfacial dynamics.
{"title":"Magnetoelectric coupling drives ultrafast-charging MoS₂ anodes for sodium-ion batteries","authors":"Zhenwei Li, Zhiyu Zou, Hengyuan Hu, Jie Chen, Mengchuang Liu, Ping Liu, Wenhua Zhang, Chang Lu, Zhaoxin Meng, Yongqiang Ji, Jie Yu, Meisheng Han, Yuliang Cao","doi":"10.1039/d5ee06010a","DOIUrl":"https://doi.org/10.1039/d5ee06010a","url":null,"abstract":"Understanding and regulating the interfacial Na+-storage kinetics of MoS2 anodes remains a key challenge for sodium-ion batteries. Here, Co-doped MoS2 is employed as a model to elucidate, from the perspective of the dynamic evolution of spin-polarized electrons, a magnetoelectric coupling-dominated mechanism that accelerates interfacial Na+ storage. During the conversion reaction, Co atoms doped into the MoS2 lattice generate ~ 4 nm Co0 nanocrystals. In-situ magnetometry reveals that the spin-split bands of these magnetic Co0 nanocrystals effectively accommodate spin-polarized electrons, thereby generating a spin-polarized surface capacitive effect (“magnetic” contribution), which in turn enables ultrafast Na+ storage at the Co0/Na2S interfaces. Moreover, a portion of spin-polarized electrons stored in Co0 nanocrystals are transferred to electrolyte molecules, catalyzing their directional decomposition and promoting the formation of NaF-riched solid electrolyte interphase (“electric” contribution). Benefiting from this magnetoelectric coupling effect, the Co-doped MoS2 electrode exhibits excellent fast-charging capability in both half cells and full cells. This study not only establishes a direct link between spin-polarized electron dynamics and interfacial reaction pathways, but also provides important insights for the co-design of heterogeneous catalysis and interfacial dynamics.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"14 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146056970","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}
Layered manganese oxides (δ-MnO2) are regarded as promising cathodes for aqueous zinc-ion batteries (AZIBs), owing to their abundant resources, multiple electron transfer, and environmental benignity. However, their poor intrinsic conductivity and severe Mn dissolution significantly limit rate capability, rendering them insufficient for meeting the “fast‑charging” requirements of AZIBs. Herein, an orbital‑engineering driven strategy is proposed to enhance the intrinsic conductivity and improve the electrochemical performance of δ‑MnO2. Based on high‑throughput simulations, a theoretical framework for intelligent screening is first established. The results demonstrated that single-atom Fe-doped δ-MnO2 (FeSA-MnO2) exhibits the strongest electron delocalization effect, with a charge-transfer number of 3.54. This originates from orbital hybridization between Fe and O atoms, which introduces new electronic states, together with the degeneracy of dxz and dyz in Fe 3d orbitals. These effects collectively enhance electron delocalization around Fe atoms and electron localization around O atoms, thereby boosting intrinsic conductivity. Moreover, the Fe-O bonds formed by the FeSA injection effectively increase the Mn dissolution energy and improve structural stability. Guided by theoretical predictions and supported by in-situ/ex-situ characterization, the activated intrinsic conduction enables the synthesized FeSA-MnO2 to not only increase electron density and accelerate charge transfer but also promote H+/Zn2+ reaction kinetics, leading to significantly enhanced rate performance. Consequently, FeSA-MnO2 delivers an ultrahigh rate performance of 20 A g−1 (~15 mA cm−2), with a capacity decay rate as low as 0.00037% per cycle over 30,000 cycles in electrolyte of 2 M ZnSO4 + 0.1 M MnSO4. This orbital‑level activation of intrinsic conductivity via single‑atom doping provides a new perspective for developing highly stable Mn‑based cathodes for fast‑charging AZIBs.
层状锰氧化物（δ-MnO2）由于其丰富的资源、多重电子转移和环境友好性而被认为是水锌离子电池（AZIBs）极有前途的阴极材料。然而，它们的固有电导率差和严重的锰溶解严重限制了速率能力，使它们不足以满足azib的“快速充电”要求。本文提出了一种轨道工程驱动策略，以提高δ - MnO2的固有电导率和电化学性能。基于高通量模拟，首先建立了智能筛选的理论框架。结果表明，单原子掺铁δ-MnO2 （FeSA-MnO2）具有最强的电子离域效应，其电荷转移数为3.54。这源于Fe和O原子之间的轨道杂化，引入了新的电子态，以及Fe三维轨道中dxz和dyz的简并。这些效应共同增强了Fe原子周围的电子离域和O原子周围的电子定域，从而提高了本征电导率。此外，FeSA注入形成的Fe-O键有效地提高了Mn的溶解能，提高了结构的稳定性。在理论预测的指导下，原位/非原位表征的支持下，激活的本态传导使合成的FeSA-MnO2不仅增加了电子密度和加速了电荷转移，而且促进了H+/Zn2+反应动力学，从而显著提高了速率性能。因此，FeSA-MnO2在2 M ZnSO4 + 0.1 M MnSO4的电解液中提供了20 A g−1 （~15 mA cm−2）的超高倍率性能，在3万次循环中，每循环的容量衰减率低至0.00037%。这种通过单原子掺杂激活固有电导率的轨道水平为开发高稳定的用于快速充电azib的Mn基阴极提供了新的视角。
{"title":"Orbital Engineering Activated Intrinsic Conduction Enables Ultra-high-rate Performance Zinc Storage in Manganese Dioxide","authors":"Huihui Hu, Yanhong Feng, Zhiwei Wang, Longchao Zhuo, cejun hu, Imran Shakir, Dingsheng Wang, Xijun Liu","doi":"10.1039/d5ee05832e","DOIUrl":"https://doi.org/10.1039/d5ee05832e","url":null,"abstract":"Layered manganese oxides (δ-MnO2) are regarded as promising cathodes for aqueous zinc-ion batteries (AZIBs), owing to their abundant resources, multiple electron transfer, and environmental benignity. However, their poor intrinsic conductivity and severe Mn dissolution significantly limit rate capability, rendering them insufficient for meeting the “fast‑charging” requirements of AZIBs. Herein, an orbital‑engineering driven strategy is proposed to enhance the intrinsic conductivity and improve the electrochemical performance of δ‑MnO2. Based on high‑throughput simulations, a theoretical framework for intelligent screening is first established. The results demonstrated that single-atom Fe-doped δ-MnO2 (FeSA-MnO2) exhibits the strongest electron delocalization effect, with a charge-transfer number of 3.54. This originates from orbital hybridization between Fe and O atoms, which introduces new electronic states, together with the degeneracy of dxz and dyz in Fe 3d orbitals. These effects collectively enhance electron delocalization around Fe atoms and electron localization around O atoms, thereby boosting intrinsic conductivity. Moreover, the Fe-O bonds formed by the FeSA injection effectively increase the Mn dissolution energy and improve structural stability. Guided by theoretical predictions and supported by in-situ/ex-situ characterization, the activated intrinsic conduction enables the synthesized FeSA-MnO2 to not only increase electron density and accelerate charge transfer but also promote H+/Zn2+ reaction kinetics, leading to significantly enhanced rate performance. Consequently, FeSA-MnO2 delivers an ultrahigh rate performance of 20 A g−1 (~15 mA cm−2), with a capacity decay rate as low as 0.00037% per cycle over 30,000 cycles in electrolyte of 2 M ZnSO4 + 0.1 M MnSO4. This orbital‑level activation of intrinsic conductivity via single‑atom doping provides a new perspective for developing highly stable Mn‑based cathodes for fast‑charging AZIBs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"290 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097859","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}
Understanding the thermal origins of performance instabilities and hysteresis in perovskite solar cells (PSCs) is essential for advancing their long-term stability and reliable operation. In this perspective, we develop a novel coupled multiphysics mathematical framework that integrates layer-resolved optical absorption, non-isothermal electronic–ionic transport, and a layer-resolved, self-consistent energy balance with explicit bulk and interfacial heat-generation pathways. These pathways include hot-carrier thermalization, Joule heating, Peltier effects, radiative/non-radiative recombination, and parasitic optical absorption. This mathematical framework extends PSC characterization beyond conventional J–V analysis by introducing temperature–voltage (T–V) and heat–voltage (P–V) characteristics curves, enabling quantitative tracking of transient self-heating and its interactions with electronic–ionic dynamics. It is shown that PSCs develop internal thermal inertia that evolves on timescales comparable to ionic relaxation under bias sweeps, leading to strongly scan-rate-dependent heating. At intermediate scan rates, this thermo-electro-ionic coupling produces non-monotonic temperature evolution with dual-peak profiles during forward sweeps and pronounced T–V hysteresis, coinciding with S-shaped J–V distortions that are shifted to lower scan rates relative to isothermal predictions. The scan-rate-dependent heating can be resolved into interfacial- and bulk-dominated regimes: interfacial heating governs the temperature evolution at low-to-intermediate scan rates, bulk heating controls the profile at intermediate-to-high rates, while rapid sweeps leave insufficient time for heat to accumulate, ultimately driving the response toward an ion-frozen, quasi-isothermal limit. These distinct thermal regimes reshape carrier extraction asymmetry, internal field screening, and mobile-ion redistribution, thereby aggravating or mitigating hysteresis relative to isothermal electronic–ionic transport predictions. Neglecting thermo-electro-ionic effects underestimates transient temperature rises by >10 K and misidentify the scan-rate window associated with S-shaped J–V distortions. By integrating these multiphysics effects, the framework provides a diagnostic tool for next-generation PSC characterization and identifies design strategies such as interface engineering, nanostructural thermal management, and scan-protocol optimization to enhance device performance and stability under real-world operating conditions.
{"title":"On the role of thermo-electro-ionic dynamics in hysteresis and transient performance of perovskite solar cells","authors":"Hadi Rostamzadeh, Hamid Montazeri","doi":"10.1039/d5ee05840f","DOIUrl":"https://doi.org/10.1039/d5ee05840f","url":null,"abstract":"Understanding the thermal origins of performance instabilities and hysteresis in perovskite solar cells (PSCs) is essential for advancing their long-term stability and reliable operation. In this perspective, we develop a novel coupled multiphysics mathematical framework that integrates layer-resolved optical absorption, non-isothermal electronic–ionic transport, and a layer-resolved, self-consistent energy balance with explicit bulk and interfacial heat-generation pathways. These pathways include hot-carrier thermalization, Joule heating, Peltier effects, radiative/non-radiative recombination, and parasitic optical absorption. This mathematical framework extends PSC characterization beyond conventional <em>J</em>–<em>V</em> analysis by introducing temperature–voltage (<em>T</em>–<em>V</em>) and heat–voltage (<em>P</em>–<em>V</em>) characteristics curves, enabling quantitative tracking of transient self-heating and its interactions with electronic–ionic dynamics. It is shown that PSCs develop internal thermal inertia that evolves on timescales comparable to ionic relaxation under bias sweeps, leading to strongly scan-rate-dependent heating. At intermediate scan rates, this thermo-electro-ionic coupling produces non-monotonic temperature evolution with dual-peak profiles during forward sweeps and pronounced <em>T</em>–<em>V</em> hysteresis, coinciding with S-shaped <em>J</em>–<em>V</em> distortions that are shifted to lower scan rates relative to isothermal predictions. The scan-rate-dependent heating can be resolved into interfacial- and bulk-dominated regimes: interfacial heating governs the temperature evolution at low-to-intermediate scan rates, bulk heating controls the profile at intermediate-to-high rates, while rapid sweeps leave insufficient time for heat to accumulate, ultimately driving the response toward an ion-frozen, quasi-isothermal limit. These distinct thermal regimes reshape carrier extraction asymmetry, internal field screening, and mobile-ion redistribution, thereby aggravating or mitigating hysteresis relative to isothermal electronic–ionic transport predictions. Neglecting thermo-electro-ionic effects underestimates transient temperature rises by >10 K and misidentify the scan-rate window associated with S-shaped <em>J</em>–<em>V</em> distortions. By integrating these multiphysics effects, the framework provides a diagnostic tool for next-generation PSC characterization and identifies design strategies such as interface engineering, nanostructural thermal management, and scan-protocol optimization to enhance device performance and stability under real-world operating conditions.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"73 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146057005","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}
Bochun Liang, Xueyan Huang, Shendong Tan, Tairan Wang, Chaoyuan Ji, Ting Si, Xi-Yao Li, Hao Chen, Yaoshu Xie, Lu Jiang, Chen-Zi Zhao, Jun Fan, Tingzheng Hou, Qiang Zhang
Decoupling Li+ transport from polymer segmental dynamics is crucial for enhancing ionic conductivity (σ) and transference number (t+) in solid polymer electrolytes (SPEs). Herein, by studying four ether-based SPEs with varying oxygen density, we identify a transition from polymer relaxation-limited ion transport in poly(ethylene oxide) (PEO) to ion hopping-dominant transport in poly(tetrahydrofuran) (PTHF), poly(1,3-dioxolane) (PDOL), and poly(trioxymethylene) (PTOM). Molecular dynamics simulations and solidstate 7Li nuclear magnetic resonance reveal origins of the transition. In PTHF, weak solvation with lithium bond characteristics contributes to a less-shielded Li+ environment, while in PDOL and PTOM, the discontinuous coordination (DC) structure and multi-chain binding are pivotal. The presence of DC structures is experimentally confirmed by in situ attenuated total reflection Fourier transform infrared spectroscopy and supported by quantum chemistry calculations. As a result, PDOL and PTOM exhibit t+ values exceeding 0.5 and enhanced σ values of 4.3 × 10-3 and 8.5 × 10-3 S cm-1 at 373 K, respectively. The Li/SPEs/LiFePO4 cell with ex situ-prepared PDOL achieves a superior capacity retention of 90.8% after 50 cycles. This work underscores the significance of functional group spacing in tuning the transport mechanisms and demonstrates how the decoupling strategy can guide the bottom-up design of advanced SPEs.
聚合物节段动力学中Li+输运解耦对于提高固体聚合物电解质（spe）中的离子电导率（σ）和转移数（t+）至关重要。在此，通过研究不同氧密度的四种醚基spe，我们确定了从聚环氧乙烷（PEO）中的聚合物弛豫限制离子传输到聚四氢呋喃（PTHF）、聚1,3-二氧索烷（PDOL）和聚三氧亚甲基（PTOM）中的离子跳跃优势传输的转变。分子动力学模拟和固态7Li核磁共振揭示了转变的起源。在PTHF中，具有锂键特征的弱溶剂化有助于低屏蔽的Li+环境，而在PDOL和PTOM中，不连续配位（DC）结构和多链结合是关键。用原位衰减全反射傅立叶变换红外光谱证实了直流结构的存在，并得到了量子化学计算的支持。结果表明，在373 K时，PDOL和PTOM的t+值均超过0.5，σ值分别增大到4.3 × 10-3和8.5 × 10-3 S cm-1。经过50次循环后，原位制备PDOL的Li/ spe /LiFePO4电池的容量保持率达到90.8%。这项工作强调了功能群间距在调整传输机制中的重要性，并展示了解耦策略如何指导高级spe的自底向上设计。
{"title":"Discontinuous Coordination Boosting Ion Transport in Solid Polymer Electrolytes","authors":"Bochun Liang, Xueyan Huang, Shendong Tan, Tairan Wang, Chaoyuan Ji, Ting Si, Xi-Yao Li, Hao Chen, Yaoshu Xie, Lu Jiang, Chen-Zi Zhao, Jun Fan, Tingzheng Hou, Qiang Zhang","doi":"10.1039/d5ee05901a","DOIUrl":"https://doi.org/10.1039/d5ee05901a","url":null,"abstract":"Decoupling Li<small><sup>+</sup></small> transport from polymer segmental dynamics is crucial for enhancing ionic conductivity (σ) and transference number (t<small><sub>+</sub></small>) in solid polymer electrolytes (SPEs). Herein, by studying four ether-based SPEs with varying oxygen density, we identify a transition from polymer relaxation-limited ion transport in poly(ethylene oxide) (PEO) to ion hopping-dominant transport in poly(tetrahydrofuran) (PTHF), poly(1,3-dioxolane) (PDOL), and poly(trioxymethylene) (PTOM). Molecular dynamics simulations and solidstate <small><sup>7</sup></small>Li nuclear magnetic resonance reveal origins of the transition. In PTHF, weak solvation with lithium bond characteristics contributes to a less-shielded Li<small><sup>+</sup></small> environment, while in PDOL and PTOM, the discontinuous coordination (DC) structure and multi-chain binding are pivotal. The presence of DC structures is experimentally confirmed by in situ attenuated total reflection Fourier transform infrared spectroscopy and supported by quantum chemistry calculations. As a result, PDOL and PTOM exhibit t<small><sub>+</sub></small> values exceeding 0.5 and enhanced σ values of 4.3 × 10<small><sup>-3</sup></small> and 8.5 × 10<small><sup>-3</sup></small> S cm<small><sup>-1</sup></small> at 373 K, respectively. The Li/SPEs/LiFePO<small><sub>4</sub></small> cell with ex situ-prepared PDOL achieves a superior capacity retention of 90.8% after 50 cycles. This work underscores the significance of functional group spacing in tuning the transport mechanisms and demonstrates how the decoupling strategy can guide the bottom-up design of advanced SPEs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"179 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146048787","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}
Chuanyao Sun, Pengfei Qiu, Xinjie Yuan, Kelin Shen, Yi Wu, Xuefeng Zhao, Jiawei Zhang, Shiqi Yang, Lidong Chen, Xun Shi
Thermoelectric (TE) technology can convert human body heat into useful electricity, providing a promising solution to develop self-powered wearable electronics, in which both high output voltage density and power density are urgently required. However, the existing TE devices usually possess low voltage density in the wearing condition, greatly limiting their real applications. In this work, we propose a novel highly integrated blade structure, which can achieve ultrahigh output voltage and power densities. The finite element simulation gives the optimal geometric dimensions and integration numbers of the TE legs for the blade structure. In the experiment, we successfully fabricated the blade TE device by using the recently discovered Ag-based ductile inorganic TE materials with the TE leg density and aspect ratio of 300 cm−2 and 1250 cm−1, respectively. Such high values have not been simultaneously achieved for the TE devices reported before. An ultrahigh voltage density of up to 869.6 mV cm−2 is achieved when the blade device is worn on the human body, which is at least one order of magnitude higher than the existing TE devices. Likewise, the blade TE devices also exhibit high power density up to 114.1 µW cm−2, among the highest values reported so far. The electricity converted from body heat by the blade TE device can directly power an electronic watch, showing great potential to be used in real applications.
热电（TE）技术可以将人体热量转化为有用的电能，为开发迫切需要高输出电压密度和高功率密度的自供电可穿戴电子产品提供了一个有希望的解决方案。然而，现有的TE器件在磨损状态下通常具有较低的电压密度，极大地限制了其实际应用。在这项工作中，我们提出了一种新的高度集成的叶片结构，可以实现超高的输出电压和功率密度。有限元仿真给出了叶片结构中TE支腿的最优几何尺寸和积分数。在实验中，我们利用新发现的ag基延展性无机TE材料，成功制备了叶片TE器件，TE支腿密度为300 cm−2，长径比为1250 cm−1。如此高的数值并没有同时达到之前报道的TE设备。当叶片器件佩戴在人体上时，可实现高达869.6 mV cm−2的超高电压密度，比现有TE器件高出至少一个数量级。同样，叶片TE器件也具有高达114.1 μ W cm−2的高功率密度，是迄今为止报道的最高值之一。刀片TE装置将人体热量转化为电能，可以直接为电子表供电，在实际应用中显示出巨大的潜力。
{"title":"A highly integrated blade structure for thermoelectric devices with ultra-high output voltage and power densities","authors":"Chuanyao Sun, Pengfei Qiu, Xinjie Yuan, Kelin Shen, Yi Wu, Xuefeng Zhao, Jiawei Zhang, Shiqi Yang, Lidong Chen, Xun Shi","doi":"10.1039/d5ee06920c","DOIUrl":"https://doi.org/10.1039/d5ee06920c","url":null,"abstract":"Thermoelectric (TE) technology can convert human body heat into useful electricity, providing a promising solution to develop self-powered wearable electronics, in which both high output voltage density and power density are urgently required. However, the existing TE devices usually possess low voltage density in the wearing condition, greatly limiting their real applications. In this work, we propose a novel highly integrated blade structure, which can achieve ultrahigh output voltage and power densities. The finite element simulation gives the optimal geometric dimensions and integration numbers of the TE legs for the blade structure. In the experiment, we successfully fabricated the blade TE device by using the recently discovered Ag-based ductile inorganic TE materials with the TE leg density and aspect ratio of 300 cm<small><sup>−2</sup></small> and 1250 cm<small><sup>−1</sup></small>, respectively. Such high values have not been simultaneously achieved for the TE devices reported before. An ultrahigh voltage density of up to 869.6 mV cm<small><sup>−2</sup></small> is achieved when the blade device is worn on the human body, which is at least one order of magnitude higher than the existing TE devices. Likewise, the blade TE devices also exhibit high power density up to 114.1 µW cm<small><sup>−2</sup></small>, among the highest values reported so far. The electricity converted from body heat by the blade TE device can directly power an electronic watch, showing great potential to be used in real applications.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"72 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146056969","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}
Monolithic perovskite/silicon tandem solar cells have emerged as a compelling route, combining the certified power conversion efficiencies exceeding 34% for laboratory-scale devices with more cost-effective manufacturing compared to market-established silicon photovoltaics. Despite deployment in pilot processing lines beyond the lab stage, this technology still faces scaling challenges from perovskite sub-cells, such as the incompatibility with contemporary mass production lines and the upscaling efficiency deficit, that are expected to be resolved within a few years to achieve commercial viability. Here, we comprehensively elaborate the scalable deposition and drying methods of perovskite sub-cells on silicon substrates and review their recent advanced progress. We assess the merits and limitations of these competing methods, providing a systematic framework for achieving efficient and durable large-area perovskite/silicon tandem solar cells suitable for industrial production.
{"title":"Scalable deposition and drying methods toward large-area monolithic perovskite/silicon tandem solar cells","authors":"Chenxia Kan, Chao Luo, Yi Hou","doi":"10.1039/d5ee06772c","DOIUrl":"https://doi.org/10.1039/d5ee06772c","url":null,"abstract":"Monolithic perovskite/silicon tandem solar cells have emerged as a compelling route, combining the certified power conversion efficiencies exceeding 34% for laboratory-scale devices with more cost-effective manufacturing compared to market-established silicon photovoltaics. Despite deployment in pilot processing lines beyond the lab stage, this technology still faces scaling challenges from perovskite sub-cells, such as the incompatibility with contemporary mass production lines and the upscaling efficiency deficit, that are expected to be resolved within a few years to achieve commercial viability. Here, we comprehensively elaborate the scalable deposition and drying methods of perovskite sub-cells on silicon substrates and review their recent advanced progress. We assess the merits and limitations of these competing methods, providing a systematic framework for achieving efficient and durable large-area perovskite/silicon tandem solar cells suitable for industrial production.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"50 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146034081","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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