Zhengqing Cui,Zhongshuo Zhang,Zhenhao Wang,Zhisen Jiang,Jieshan Qiu,Jie Zeng,Ib Chorkendorff,Shaofeng Li
Gas diffusion electrodes (GDEs) are essential for continuous-flow lithium-mediated nitrogen reduction reaction (Li-NRR), where they deliver N2 directly to the cathode and maintain the gas-liquid-solid interface required for NH3 formation. Carbon paper is widely used as a GDE substrate in gas-fed electrochemistry, yet its performance in continuous-flow Li-NRR remains limited. Here we show that this limitation originates from the coupled effects of pore architecture and carbon chemistry. The narrow, tortuous fiber-derived pores of carbon paper are prone to electrolyte flooding, which restricts N2 transport to the reactive interface. In parallel, graphitic domains promote parasitic Li+ intercalation, consuming charge before metallic Li deposition is established. To address these constraints, we develop a carbon-coated Ni mesh (Ni@C) as a model GDE with a low-graphitization carbon overlayer. The macroporous Ni scaffold preserves open gas-transport pathways and resists capillary flooding, while the low-graphitization carbon overlayer suppresses Li + intercalation and enables rapid metallic Li deposition. As a result, Ni@C increases the NH 3 Faradaic efficiency from 20 ± 2% to 59 ± 3%, reaching performance comparable to benchmark stainless-steel mesh GDEs. These results reveal that the performance of GDEs with carbon surface in continuous-flow Li-NRR is governed by the interplay between pore-level gas accessibility and carbon-interfacemediated Li deposition. By separating these two factors, Ni@C provides a model platform for defining how carbon overlayers should be integrated into cathodic GDEs for efficient lithiummediated ammonia synthesis.
{"title":"Low-graphitization carbon overlayers enable efficient gas diffusion electrodes for lithium-mediated ammonia synthesis","authors":"Zhengqing Cui,Zhongshuo Zhang,Zhenhao Wang,Zhisen Jiang,Jieshan Qiu,Jie Zeng,Ib Chorkendorff,Shaofeng Li","doi":"10.1039/d6ee04435b","DOIUrl":"https://doi.org/10.1039/d6ee04435b","url":null,"abstract":"Gas diffusion electrodes (GDEs) are essential for continuous-flow lithium-mediated nitrogen reduction reaction (Li-NRR), where they deliver N2 directly to the cathode and maintain the gas-liquid-solid interface required for NH3 formation. Carbon paper is widely used as a GDE substrate in gas-fed electrochemistry, yet its performance in continuous-flow Li-NRR remains limited. Here we show that this limitation originates from the coupled effects of pore architecture and carbon chemistry. The narrow, tortuous fiber-derived pores of carbon paper are prone to electrolyte flooding, which restricts N2 transport to the reactive interface. In parallel, graphitic domains promote parasitic Li+ intercalation, consuming charge before metallic Li deposition is established. To address these constraints, we develop a carbon-coated Ni mesh (Ni@C) as a model GDE with a low-graphitization carbon overlayer. The macroporous Ni scaffold preserves open gas-transport pathways and resists capillary flooding, while the low-graphitization carbon overlayer suppresses Li + intercalation and enables rapid metallic Li deposition. As a result, Ni@C increases the NH 3 Faradaic efficiency from 20 ± 2% to 59 ± 3%, reaching performance comparable to benchmark stainless-steel mesh GDEs. These results reveal that the performance of GDEs with carbon surface in continuous-flow Li-NRR is governed by the interplay between pore-level gas accessibility and carbon-interfacemediated Li deposition. By separating these two factors, Ni@C provides a model platform for defining how carbon overlayers should be integrated into cathodic GDEs for efficient lithiummediated ammonia synthesis.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"12 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149225877","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}
Poly(vinylidene fluoride) (PVDF)-based solid-state polymer electrolytes (SPEs) are promising for high-energy-density solid-state lithium metal batteries (SSLMBs) but are hindered by the inherent trade-off between Li+ coordination for salt dissociation and decoordination for ions transport. This work decouples this dilemma by employing a poly(vinylidene fluoride-co-chlorofluoroethylene) [P(VDF-CFE)] copolymer as a novel SPE matrix. Relative to VDF units, the chlorine substitution in CFE exhibits a lower dipole moment and reduced Li+ adsorption energy, facilitating the timely detachment of Li+ from polymer chains and releasing more Li+ to form aggregated (AGG) species. Concurrently, the increased dielectric constant of P(VDF-CFE) ensures sufficient salt dissociation. In consequence, the P(VDF-CFE) SPE achieves a high room-temperature ionic conductivity (4.17 × 10-4 S/cm) and enables the formation of a LiCl-containing and LiF-rich solid electrolyte interphase (SEI) layer, which offers high ionic conductivity and robust dendrite suppression. The Li//Li symmetric cells show a high critical current density of 1.8 mA·cm-2 and stable cycles for 4000 hours under 0.10 mA cm−2, and retaining stability even at 0.6 mA cm−2. The LiNi0.8Co0.1Mn0.1O2//Li cells retain 71.2% of their capacity after 1200 cycles at 1 C. This work breaks the performance bottleneck of filler-free SPEs and advances the viability of SSLMBs.
基于聚偏氟乙烯（PVDF）的固态聚合物电解质（spe）在高能量密度固态锂金属电池（sslmb）中具有广阔的应用前景，但由于Li+配位的盐解离和离子输运的配位之间的固有平衡而受到阻碍。这项工作通过采用聚偏氟乙烯-共氯氟乙烯共聚物[P(VDF-CFE)]作为新型SPE基质来解决这一难题。相对于VDF单元，CFE中的氯取代具有较低的偶极矩和较低的Li+吸附能，有利于Li+从聚合物链上及时脱离，释放更多的Li+形成聚集态（AGG）。同时，P（VDF-CFE）介电常数的增加保证了盐的充分解离。因此，P(VDF-CFE) SPE实现了高室温离子电导率（4.17 × 10-4 S/cm），并能够形成含licl和富lif的固体电解质界面（SEI）层，该层具有高离子电导率和强大的枝晶抑制能力。Li//Li对称电池的临界电流密度高达1.8 mA·cm-2，在0.10 mA cm-2下可稳定循环4000小时，即使在0.6 mA cm-2下也能保持稳定。在高温下，经过1200次循环后，LiNi0.8Co0.1Mn0.1O2//Li电池的容量保持在71.2%，突破了无填料spe的性能瓶颈，提高了sslmb的可行性。
{"title":"Decoupling the Coordination-Decoordination Trade-off in PVDF-Based Electrolytes via Chlorine Substitution for High-Performance Solid-State Lithium Metal Batteries","authors":"Kewen Tao,Min Zuo,Yanfei Huang","doi":"10.1039/d6ee05255j","DOIUrl":"https://doi.org/10.1039/d6ee05255j","url":null,"abstract":"Poly(vinylidene fluoride) (PVDF)-based solid-state polymer electrolytes (SPEs) are promising for high-energy-density solid-state lithium metal batteries (SSLMBs) but are hindered by the inherent trade-off between Li+ coordination for salt dissociation and decoordination for ions transport. This work decouples this dilemma by employing a poly(vinylidene fluoride-co-chlorofluoroethylene) [P(VDF-CFE)] copolymer as a novel SPE matrix. Relative to VDF units, the chlorine substitution in CFE exhibits a lower dipole moment and reduced Li+ adsorption energy, facilitating the timely detachment of Li+ from polymer chains and releasing more Li+ to form aggregated (AGG) species. Concurrently, the increased dielectric constant of P(VDF-CFE) ensures sufficient salt dissociation. In consequence, the P(VDF-CFE) SPE achieves a high room-temperature ionic conductivity (4.17 × 10-4 S/cm) and enables the formation of a LiCl-containing and LiF-rich solid electrolyte interphase (SEI) layer, which offers high ionic conductivity and robust dendrite suppression. The Li//Li symmetric cells show a high critical current density of 1.8 mA·cm-2 and stable cycles for 4000 hours under 0.10 mA cm−2, and retaining stability even at 0.6 mA cm−2. The LiNi0.8Co0.1Mn0.1O2//Li cells retain 71.2% of their capacity after 1200 cycles at 1 C. This work breaks the performance bottleneck of filler-free SPEs and advances the viability of SSLMBs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"13 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149225876","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}
Zhiwei Li,Yinghong Xu,Xi Wang,Xinglong Pan,Wei Li Ong,Peng Jin,Yi Zhou,Guo Tian,Wanheng Lu,Yi Hou,Ghim Wei Wei Ho
The urban heat island effect intensifies thermal stress in cities and increases electricity demand for cooling. Although rooftop photovoltaics play a key role in decarbonizing urban energy systems, conventional thermal management either consumes additional energy or passively dissipates heat without recovery, limiting net energy benefits. Here, we report a cascade photovoltaic (C-PV) system that reconfigures energy flow within PV, enabling negative energy-consuming thermal management by converting waste heat into additional electricity. Under simulated 1.0 Sun illumination, the C-PV lowers the silicon-based PV operating temperature by ~10 °C (18.2%), enhancing power density by 14.2%. The strategy is also applicable to an emerging perovskite-based cell, where a 5 °C (11.5%) temperature reduction improves the efficiency from 23.5% to 25.1%. Unlike energy-consuming/-neutral cooling approaches, the system achieves net energy gain via ionic thermoelectric coupling and maintains stable operation over one year. These results establish ionic thermoelectric coupling as a new paradigm for solar-thermal management in urban environments.
{"title":"Negative energy-consuming thermal management guided by machine learning for year-round electricity generation","authors":"Zhiwei Li,Yinghong Xu,Xi Wang,Xinglong Pan,Wei Li Ong,Peng Jin,Yi Zhou,Guo Tian,Wanheng Lu,Yi Hou,Ghim Wei Wei Ho","doi":"10.1039/d6ee05261d","DOIUrl":"https://doi.org/10.1039/d6ee05261d","url":null,"abstract":"The urban heat island effect intensifies thermal stress in cities and increases electricity demand for cooling. Although rooftop photovoltaics play a key role in decarbonizing urban energy systems, conventional thermal management either consumes additional energy or passively dissipates heat without recovery, limiting net energy benefits. Here, we report a cascade photovoltaic (C-PV) system that reconfigures energy flow within PV, enabling negative energy-consuming thermal management by converting waste heat into additional electricity. Under simulated 1.0 Sun illumination, the C-PV lowers the silicon-based PV operating temperature by ~10 °C (18.2%), enhancing power density by 14.2%. The strategy is also applicable to an emerging perovskite-based cell, where a 5 °C (11.5%) temperature reduction improves the efficiency from 23.5% to 25.1%. Unlike energy-consuming/-neutral cooling approaches, the system achieves net energy gain via ionic thermoelectric coupling and maintains stable operation over one year. These results establish ionic thermoelectric coupling as a new paradigm for solar-thermal management in urban environments.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"395 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149225915","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}
Iodine cathodes with four-electron redox chemistry offer a promising pathway toward ultrahigh energy density in zinc–iodine (Zn–I2) batteries. However, the conventional ultrahigh-concentration chloride (Cl−) electrolytes suffer from intrinsic sluggish Zn2+ transport, while the reported low Cl− electrolytes have the issues of insufficient I+ stabilization and rampant growth of Zn dendrites, thereby severely hindering the practical deployment of four-electron Zn–I2 batteries. Herein, we explore organic quaternary ammonium chloride salts as low-chloride electrolytes and find that 3-chloro-2-hydroxypropyl trimethylammonium chloride (CHPTAC) containing both –OH and –CH3CH2Cl functional groups not only stabilizes I+ very well under low Cl− concentration, but also facilitates the reversibility of four-electron iodine conversion through the reconstruction of the electrolyte hydrogen-bond network, extending the I+ stabilization mechanism beyond the reported conventional halide coordination. Moreover, CHPTAC cations are demonstrated to enable uniform Zn2+ deposition with a preferred (002) crystal-plane orientation. Accordingly, in this low-chloride CHPTAC electrolyte, the Zn–I2 battery maintains a high specific capacity of over 320 mAh g−1 even after 2100 cycles at 2C, which is superior to the state-of-the-art Zn–I2 batteries. Furthermore, at an ultrahigh areal loading of I2 (10 mg cm−2), the assembled Ah-level pouch cell delivers a stable lifespan over 120 cycles. This work provides an effective electrolyte design strategy for durable high-energy aqueous zinc-ion batteries.
具有四电子氧化还原化学性质的碘阴极为锌-碘（Zn-I2）电池的超高能量密度提供了一条有前途的途径。然而，传统的超高浓度Cl -电解质存在固有的Zn2+传输缓慢的问题，而低Cl -电解质存在I+稳定性不足和Zn枝晶生长猖獗的问题，从而严重阻碍了四电子Zn - i2电池的实际部署。在此，我们探索了有机季铵盐作为低氯电解质，发现含有-OH和-CH3CH2Cl官能团的3-氯-2-羟丙基三甲基氯化铵（CHPTAC）不仅在低Cl−浓度下稳定I+，而且通过重构电解质氢键网络促进了四电子碘转化的可逆性。将I+稳定机制扩展到传统卤化物配位之外。此外，CHPTAC阳离子被证明能够以首选（002）晶体面取向均匀沉积Zn2+。因此，在这种低氯化物CHPTAC电解质中，即使在2C循环2100次后，Zn-I2电池仍保持超过320 mAh g - 1的高比容量，这优于最先进的Zn-I2电池。此外，在I2 （10 mg cm−2）的超高面负载下，组装的ah级袋状电池提供了超过120次循环的稳定寿命。本研究为耐用高能水锌离子电池提供了一种有效的电解质设计策略。
{"title":"Low-chloride electrolytes with dual-functional organic cations enable four-electron redox conversion in durable Ah-level zinc–iodine batteries","authors":"Kaiyi Guo,Bibo Han,Wenjie Zhang,Shanjie Cheng,Yu Qiu,Chen Wang,Jingzhen Du,Yi Peng,Xiaohui Yan,Zaichun Liu,Rui Wang,Panpan Zhang,Faxing Wang,Xinhua Zheng,Yuping Wu","doi":"10.1039/d6ee04666e","DOIUrl":"https://doi.org/10.1039/d6ee04666e","url":null,"abstract":"Iodine cathodes with four-electron redox chemistry offer a promising pathway toward ultrahigh energy density in zinc–iodine (Zn–I2) batteries. However, the conventional ultrahigh-concentration chloride (Cl−) electrolytes suffer from intrinsic sluggish Zn2+ transport, while the reported low Cl− electrolytes have the issues of insufficient I+ stabilization and rampant growth of Zn dendrites, thereby severely hindering the practical deployment of four-electron Zn–I2 batteries. Herein, we explore organic quaternary ammonium chloride salts as low-chloride electrolytes and find that 3-chloro-2-hydroxypropyl trimethylammonium chloride (CHPTAC) containing both –OH and –CH3CH2Cl functional groups not only stabilizes I+ very well under low Cl− concentration, but also facilitates the reversibility of four-electron iodine conversion through the reconstruction of the electrolyte hydrogen-bond network, extending the I+ stabilization mechanism beyond the reported conventional halide coordination. Moreover, CHPTAC cations are demonstrated to enable uniform Zn2+ deposition with a preferred (002) crystal-plane orientation. Accordingly, in this low-chloride CHPTAC electrolyte, the Zn–I2 battery maintains a high specific capacity of over 320 mAh g−1 even after 2100 cycles at 2C, which is superior to the state-of-the-art Zn–I2 batteries. Furthermore, at an ultrahigh areal loading of I2 (10 mg cm−2), the assembled Ah-level pouch cell delivers a stable lifespan over 120 cycles. This work provides an effective electrolyte design strategy for durable high-energy aqueous zinc-ion batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"16 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218229","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}
Carbazole-phosphonic acid-based self-assembled monolayers (SAMs) serves as essential holeselective contacts in perovskite solar cells (PSCs), yet suffer from local aggregation, discontinuous coverage, and poor wettability, resulting in defective buried interfaces and uncontrolled perovskite nucleation. Here, we propose a sequential molecular reconstruction strategy to overcome these limitations. A pre-deposited [4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid (Me-4PACz) host matrix is post-treated with diphenylphosphinic acid (DPPA). Thermodynamically favorable heteromolecular Me-4PACz-DPPA interactions drive local molecular rearrangement, yielding a denser, and smoother SAM with uniform surface potential. The reconstructed interface markedly improves precursor wettability and moderate nucleation kinetics, leading to large-grain perovskite films with improved crystallographic orientation and reduced formation of PbI 2 . The P=O and P-OH functionalities of DPPA coordinatively passivate undercoordinated Pb 2+ defects and stabilize formamidinium cations via hydrogen bonding and electrostatic interactions.Consequently, PSCs utilizing the reconstructed SAM achieve a champion power conversion efficiency (PCE) of 27.43% (certified efficiency of 27.27%) and retain ~90% of their initial PCE after 2000 h of maximum power point tracking under one-sun illumination at 85±5 °C. This work establishes post-deposition small-molecule SAMs that induce dynamic reconstruction of the buried interface, an effective approach for buried-interface engineering in high-performance optoelectronics.
{"title":"Sequential Reconstruction of Self-Assembled Monolayers Enables Efficient Perovskite Photovoltaics","authors":"Shuangwei Lv,Mingyuan Han,Botong Li,Hanqing Yang,Yunxiao Liao,Liwen Zhang,Xiaohan Chen,Zheng Zou,Xuepeng Liu,Zedong Lin,Wenyong Feng,Changqing Lin,Pengfei Wu,Feng Xiaopeng,Zhipeng Shao,Shuzhang Yang,Mohammad Khaja Nazeeruddin,Yong Ding","doi":"10.1039/d6ee05195b","DOIUrl":"https://doi.org/10.1039/d6ee05195b","url":null,"abstract":"Carbazole-phosphonic acid-based self-assembled monolayers (SAMs) serves as essential holeselective contacts in perovskite solar cells (PSCs), yet suffer from local aggregation, discontinuous coverage, and poor wettability, resulting in defective buried interfaces and uncontrolled perovskite nucleation. Here, we propose a sequential molecular reconstruction strategy to overcome these limitations. A pre-deposited [4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid (Me-4PACz) host matrix is post-treated with diphenylphosphinic acid (DPPA). Thermodynamically favorable heteromolecular Me-4PACz-DPPA interactions drive local molecular rearrangement, yielding a denser, and smoother SAM with uniform surface potential. The reconstructed interface markedly improves precursor wettability and moderate nucleation kinetics, leading to large-grain perovskite films with improved crystallographic orientation and reduced formation of PbI 2 . The P=O and P-OH functionalities of DPPA coordinatively passivate undercoordinated Pb 2+ defects and stabilize formamidinium cations via hydrogen bonding and electrostatic interactions.Consequently, PSCs utilizing the reconstructed SAM achieve a champion power conversion efficiency (PCE) of 27.43% (certified efficiency of 27.27%) and retain ~90% of their initial PCE after 2000 h of maximum power point tracking under one-sun illumination at 85±5 °C. This work establishes post-deposition small-molecule SAMs that induce dynamic reconstruction of the buried interface, an effective approach for buried-interface engineering in high-performance optoelectronics.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"188 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173217","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}
Jun Seop Kim,Sangmyeong Lee,Dongho Kim,Sung-Yoon Chung
Correction for ‘Crystal size-mediated solute incorporation and solid-solution stability in RuO2 during acidic oxygen evolution’ by Jun Seop Kim et al., Energy Environ. Sci., 2026, 19, 2585–2596, https://doi.org/10.1039/d5ee03097h.
{"title":"Correction: Crystal size-mediated solute incorporation and solid-solution stability in RuO during acidic oxygen evolution","authors":"Jun Seop Kim,Sangmyeong Lee,Dongho Kim,Sung-Yoon Chung","doi":"10.1039/d6ee90094a","DOIUrl":"https://doi.org/10.1039/d6ee90094a","url":null,"abstract":"Correction for ‘Crystal size-mediated solute incorporation and solid-solution stability in RuO2 during acidic oxygen evolution’ by Jun Seop Kim et al., Energy Environ. Sci., 2026, 19, 2585–2596, https://doi.org/10.1039/d5ee03097h.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"408 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173218","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}
Silicon promises an ideal anode material for all-solid-state lithium-ion battery (ASSLIB) owing to its high capacity, dendrite-free behavior, and low cost. However, the high stack pressures (≥ 50 MPa) typically required to prevent contact deactivation of silicon anode are impractical for large-scale commercialization. Here, we reveal the mechanical design requirements for low-stack-pressure Si-based solid-state anodes and demonstrate low-pressure operation (2 MPa) by introducing mechanically heterogeneous Li1.3Ga, which integrates mixed ionic-electronic conductivity with soft amorphous LixGa for local compliance and rigid crystalline Li1Ga for framework anchoring. This hierarchical soft/hard architecture maintains stable ionic-electronic conducting percolations, suppresses interfacial contact loss and preserves anode integrity. Consequently, the home-made NCM83||Si full cells exhibit a jellyroll specific energy of 337 Wh kg−1 at 2.06 mA cm−2 and sustain stable long-term cycling for over 1200 cycles at 5 MPa, while the pouch cell operates stably at 2 MPa. This work provides a promising pathway toward commercially viable low-stack-pressure silicon anodes for ASSLIBs.
硅承诺一个理想的全固态锂离子电池的阳极材料(ASSLIB)由于其高容量,dendrite-free行为,和低成本。然而，通常防止硅阳极接触失活所需的高堆压（≥50mpa）对于大规模商业化是不切实际的。在这里，我们揭示了低堆叠压力硅基固态阳极的机械设计要求，并通过引入机械非均质Li1.3Ga来演示低压操作（2 MPa）， Li1.3Ga集成了混合离子电子导电性，软非晶LixGa用于局部顺应性，刚性晶体Li1Ga用于框架锚定。这种分层的软/硬结构保持了稳定的离子电子传导渗透，抑制了界面接触损失并保持了阳极的完整性。因此，自制的NCM83||硅电池在2.06 mA cm - 2下具有337 Wh kg - 1的jellyroll比能量，在5 MPa下可以稳定地长期循环超过1200次，而袋状电池在2 MPa下可以稳定地工作。这项工作为asslib的商业上可行的低堆压硅阳极提供了一条有希望的途径。
{"title":"Mechanically heterogeneous alloy enables low-pressure silicon anodes for all-solid-state batteries","authors":"Youlong Sun,Tao Liu,Yuewei Yan,Ziheng Yin,Zhen Ding,Yufan Cui,Lixue Zhou,Xiaowei Wu,Jiahao Xu,Tianpeng Huang,Lang Huang,Yue Zheng,Shanmu Dong,Guanglei Cui","doi":"10.1039/d6ee04829c","DOIUrl":"https://doi.org/10.1039/d6ee04829c","url":null,"abstract":"Silicon promises an ideal anode material for all-solid-state lithium-ion battery (ASSLIB) owing to its high capacity, dendrite-free behavior, and low cost. However, the high stack pressures (≥ 50 MPa) typically required to prevent contact deactivation of silicon anode are impractical for large-scale commercialization. Here, we reveal the mechanical design requirements for low-stack-pressure Si-based solid-state anodes and demonstrate low-pressure operation (2 MPa) by introducing mechanically heterogeneous Li1.3Ga, which integrates mixed ionic-electronic conductivity with soft amorphous LixGa for local compliance and rigid crystalline Li1Ga for framework anchoring. This hierarchical soft/hard architecture maintains stable ionic-electronic conducting percolations, suppresses interfacial contact loss and preserves anode integrity. Consequently, the home-made NCM83||Si full cells exhibit a jellyroll specific energy of 337 Wh kg−1 at 2.06 mA cm−2 and sustain stable long-term cycling for over 1200 cycles at 5 MPa, while the pouch cell operates stably at 2 MPa. This work provides a promising pathway toward commercially viable low-stack-pressure silicon anodes for ASSLIBs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"21 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173134","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}
Jann B. Landgraf,Yashika Gupta,Aleksandra Oranskaia,Oliver Fischer,Edward Butler-Caddle,Sofiia Kosar,Adi Prasetio,Christian Schwarz,Christoph Messmer,Sithisak Chanthalavong,Johanna Modes,Fabian Till Thome,Oussama Er-raji,Stefaan De Wolf,Udo Schwingenschlogl,Rebecca L. Milot,Adam D Wright,Patricia Samia Cerian Schulze,Anna Fischer,Stefan W Glunz,Juliane Borchert
Mitigating non-radiative recombination at the perovskite/C60 interface is critical for achieving high-efficiency perovskite solar cells. A common strategy relies on small organic, mostly amino- or ammonium-functionalized molecules as interfacial layers. Combining these functionalities with carboxylic or phosphonic acids offers a route to target multiple defect types, yet design principles for such bifunctional molecules remain poorly understood. Here, we develop a design framework by systematically varying the functional groups of such molecules. By combining density functional theory, optoelectrical device simulations, and experiment, we link molecular functionality to passivation mechanism, device performance, and stability. While diammonium functionality primarily induces field-effect passivation, phosphonic and carboxylic acids enable chemically selective defect passivation. Furthermore, diammonium-based interlayers deliver strongest recombination suppression, enabling perovskite/silicon tandem solar cells with efficiencies of 30.4%. In contrast, carboxylic acid-based devices show superior stability, revealing a trade-off between passivation strength and operational stability, offering future guidelines for rational design of passivation molecules.
{"title":"Design Rules for Bifunctional Molecules as Perovskite/C Interfacial Passivation: Linking Mechanisms, Efficiency, and Stability","authors":"Jann B. Landgraf,Yashika Gupta,Aleksandra Oranskaia,Oliver Fischer,Edward Butler-Caddle,Sofiia Kosar,Adi Prasetio,Christian Schwarz,Christoph Messmer,Sithisak Chanthalavong,Johanna Modes,Fabian Till Thome,Oussama Er-raji,Stefaan De Wolf,Udo Schwingenschlogl,Rebecca L. Milot,Adam D Wright,Patricia Samia Cerian Schulze,Anna Fischer,Stefan W Glunz,Juliane Borchert","doi":"10.1039/d6ee02985j","DOIUrl":"https://doi.org/10.1039/d6ee02985j","url":null,"abstract":"Mitigating non-radiative recombination at the perovskite/C60 interface is critical for achieving high-efficiency perovskite solar cells. A common strategy relies on small organic, mostly amino- or ammonium-functionalized molecules as interfacial layers. Combining these functionalities with carboxylic or phosphonic acids offers a route to target multiple defect types, yet design principles for such bifunctional molecules remain poorly understood. Here, we develop a design framework by systematically varying the functional groups of such molecules. By combining density functional theory, optoelectrical device simulations, and experiment, we link molecular functionality to passivation mechanism, device performance, and stability. While diammonium functionality primarily induces field-effect passivation, phosphonic and carboxylic acids enable chemically selective defect passivation. Furthermore, diammonium-based interlayers deliver strongest recombination suppression, enabling perovskite/silicon tandem solar cells with efficiencies of 30.4%. In contrast, carboxylic acid-based devices show superior stability, revealing a trade-off between passivation strength and operational stability, offering future guidelines for rational design of passivation molecules.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"167 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172461","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}
Trong Huy Pham,Hung D. T. Lai,Thao-Nguyen Ho,Tai Nguyen,Eduardo Henrique Dias,Viktoria Golovanova,F. Pelayo García de Arquer,Colin P. O'Brien,Christine M. Gabardo,Jackson Crane,David Sinton,Cao-Thang Dinh
Alkaline carbon dioxide (CO2) electrolysis is particularly attractive due to its low cell voltage, high faradaic efficiency (FE), high energy efficiency (EE), and compatibility with non-noble metal catalysts. Practical deployment, however, remains constrained by carbonate chemistry: salt precipitation on cathodic gas diffusion electrodes (GDEs) and carbonate crossover cause performance decay and increase system-level energy costs through CO2 utilization and separation penalties. Here we introduce a dual-function, hydrophilic porous mass-transport control layer that simultaneously suppresses carbonate formation and serves as the wetted separator in a membrane electrode assembly (MEA). Unlike a conventional ion-exchange membrane, the porous layer moderates alkaline electrolyte access to the cathode and reduces homogeneous CO2–OH− reactions, thereby lowering carbonate generation and suppressing carbonate crossover by 60–75% relative to a membrane-free alkaline flow-cell configuration. Using a polyvinylidene fluoride (PVDF) porous film as the dual-function layer, we first observe substantially lower carbonate crossover compared with operation without the layer. We then employ the same PVDF layer as the separator in a MEA, together with a benchmark Cu-sputtered polytetrafluoroethylene (PTFE) cathode and a Ni foam anode and achieve high C2 product selectivity (80–85%) at current densities of 110–147 mA cm−2 with low cell voltages of 2.3–2.6 V. At 110 mA cm−2, the system delivers over 500 h of cumulative operation with an ethylene (C2H4) FE of 65% and a C2 energy efficiency of 40%, corresponding to a total energy cost of 353 GJ t−1 C2H4. These results demonstrate a transport-regulated strategy that breaks the traditional stability-energy efficiency trade-off in alkaline CO2 electrolysis, providing a general design principle for stable and energy-efficient CO2 conversion using low-cost materials.
碱性二氧化碳（CO2）电解因其低电池电压、高法拉第效率（FE）、高能量效率（EE）以及与非贵金属催化剂的相容性而特别具有吸引力。然而，实际应用仍然受到碳酸盐化学的限制：阴极气体扩散电极（GDEs）上的盐沉淀和碳酸盐交叉会导致性能下降，并通过二氧化碳利用和分离带来的损失增加系统级能源成本。在这里，我们介绍了一种双重功能的亲水多孔质输运控制层，它同时抑制碳酸盐的形成，并作为膜电极组件（MEA）中的湿式分离器。与传统的离子交换膜不同，多孔层减缓了碱性电解质进入阴极，减少了均匀的CO2-OH -反应，从而减少了碳酸盐的产生，并抑制了碳酸盐的交叉，相对于无膜的碱性流动电池结构，减少了60-75%。使用聚偏氟乙烯（PVDF）多孔膜作为双功能层，我们首先观察到与不使用该层的操作相比，碳酸盐交叉明显降低。然后，我们在MEA中使用相同的PVDF层作为分离器，再加上基准的cu溅射聚四氟乙烯（PTFE）阴极和Ni泡沫阳极，在电流密度为110-147 mA cm - 2，电池电压为2.3-2.6 V的情况下，实现了高C2产品选择性（80-85%）。在110 mA cm−2的条件下，该系统累计运行超过500小时，乙烯（C2H4） FE为65%，C2能效为40%，相当于总能源成本为353 GJ t−1 C2H4。这些结果证明了一种运输调节策略，打破了碱性CO2电解中传统的稳定性和能效权衡，为使用低成本材料进行稳定和节能的CO2转化提供了一般设计原则。
{"title":"Suppressing carbonate formation in alkaline CO electrolysis","authors":"Trong Huy Pham,Hung D. T. Lai,Thao-Nguyen Ho,Tai Nguyen,Eduardo Henrique Dias,Viktoria Golovanova,F. Pelayo García de Arquer,Colin P. O'Brien,Christine M. Gabardo,Jackson Crane,David Sinton,Cao-Thang Dinh","doi":"10.1039/d6ee02989b","DOIUrl":"https://doi.org/10.1039/d6ee02989b","url":null,"abstract":"Alkaline carbon dioxide (CO2) electrolysis is particularly attractive due to its low cell voltage, high faradaic efficiency (FE), high energy efficiency (EE), and compatibility with non-noble metal catalysts. Practical deployment, however, remains constrained by carbonate chemistry: salt precipitation on cathodic gas diffusion electrodes (GDEs) and carbonate crossover cause performance decay and increase system-level energy costs through CO2 utilization and separation penalties. Here we introduce a dual-function, hydrophilic porous mass-transport control layer that simultaneously suppresses carbonate formation and serves as the wetted separator in a membrane electrode assembly (MEA). Unlike a conventional ion-exchange membrane, the porous layer moderates alkaline electrolyte access to the cathode and reduces homogeneous CO2–OH− reactions, thereby lowering carbonate generation and suppressing carbonate crossover by 60–75% relative to a membrane-free alkaline flow-cell configuration. Using a polyvinylidene fluoride (PVDF) porous film as the dual-function layer, we first observe substantially lower carbonate crossover compared with operation without the layer. We then employ the same PVDF layer as the separator in a MEA, together with a benchmark Cu-sputtered polytetrafluoroethylene (PTFE) cathode and a Ni foam anode and achieve high C2 product selectivity (80–85%) at current densities of 110–147 mA cm−2 with low cell voltages of 2.3–2.6 V. At 110 mA cm−2, the system delivers over 500 h of cumulative operation with an ethylene (C2H4) FE of 65% and a C2 energy efficiency of 40%, corresponding to a total energy cost of 353 GJ t−1 C2H4. These results demonstrate a transport-regulated strategy that breaks the traditional stability-energy efficiency trade-off in alkaline CO2 electrolysis, providing a general design principle for stable and energy-efficient CO2 conversion using low-cost materials.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"9 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172459","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}
Tengfeng Guo,Yiliang He,Xinmin Zhang,Yaping Lu,Shiwu Ma,Quanquan Pang,Yatao Liu
Layered transition metal oxides (LTMOs) are promising cathodes for sodium-ion batteries (SIBs) owing to their high specific capacity and structural tunability, but their practical application is plagued by severe structural degradation, transition metal dissolution, oxygen loss, and unstable cathode–electrolyte interphases (CEIs). Electrolytes play a critical role in mitigating these issues by modulating solvation structures, controlling interfacial chemistry, and stabilizing the LTMO surface. This review systematically analyzes the degradation mechanisms of LTMOs from an electrolyte perspective, including phase transitions, oxygen loss, transition metal dissolution, CEI dynamics, and intrinsic electrolyte properties. We propose design principles for electrolyte engineering, emphasizing the regulation of solvation structures and the construction of robust CEI protecting layers. Furthermore, we summarize recent advances in traditional and emerging electrolyte systems, including high-entropy, weakly solvating, and localized high-concentration electrolytes, along with functional additives. Finally, we propose a forward-looking perspective on the integration of in situ characterization, machine learning, and molecular-level design to accelerate the development of high-performance, stable LTMO-based SIBs.
{"title":"Electrolyte design toward stable layered oxide cathodes of sodium-ion batteries","authors":"Tengfeng Guo,Yiliang He,Xinmin Zhang,Yaping Lu,Shiwu Ma,Quanquan Pang,Yatao Liu","doi":"10.1039/d6ee03563a","DOIUrl":"https://doi.org/10.1039/d6ee03563a","url":null,"abstract":"Layered transition metal oxides (LTMOs) are promising cathodes for sodium-ion batteries (SIBs) owing to their high specific capacity and structural tunability, but their practical application is plagued by severe structural degradation, transition metal dissolution, oxygen loss, and unstable cathode–electrolyte interphases (CEIs). Electrolytes play a critical role in mitigating these issues by modulating solvation structures, controlling interfacial chemistry, and stabilizing the LTMO surface. This review systematically analyzes the degradation mechanisms of LTMOs from an electrolyte perspective, including phase transitions, oxygen loss, transition metal dissolution, CEI dynamics, and intrinsic electrolyte properties. We propose design principles for electrolyte engineering, emphasizing the regulation of solvation structures and the construction of robust CEI protecting layers. Furthermore, we summarize recent advances in traditional and emerging electrolyte systems, including high-entropy, weakly solvating, and localized high-concentration electrolytes, along with functional additives. Finally, we propose a forward-looking perspective on the integration of in situ characterization, machine learning, and molecular-level design to accelerate the development of high-performance, stable LTMO-based SIBs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"90 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149172460","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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