Raising the cut-off voltage to 4.6 V can boost the energy density of lithium metal batteries (LMBs) with LiCoO2 cathode. However, the unfavorable cathode electrolyte interphase (CEI) formed on high-voltage cathode when using Li metal-compatible ether electrolytes leads to short lifespan of batteries. Here we harness the battery intrinsic electric field to manipulate the cathode inner Helmholtz plane (IHP) during the battery’s charge through simply introducing an electric-field-responsive solvent into an ether electrolyte. Specifically, 2,2-difluoroethyl trifluoromethanesulfonate (DTS) as a weak solvated co-solvent preferentially adsorbs on the cathode surface under the electric field activation. Owing to the majority of “high-voltage fragile” 1,2-dimethoxyethane ether molecules squeezed out from the IHP by DTS, a LiF-rich and organics-less stable CEI film is formed, which minimizes cathode cracking and structure degradation under high-voltage. The DTS-containing electrolyte shows superior cycling stability of LMBs under harsh conditions of 4.6 V, 4.2 mAh cm-2 cathode loading and 15 μL lean electrolyte. Furthermore, the feasibility of this concept is validated in practical Ah-level pouch full cells. This work highlights the significance of the IHP modulation and interfacial chemistry, providing an alternative pathway towards ether-based electrolytes engineering for high-voltage LMBs.
{"title":"Regulation of the Cathode Inner Helmholtz Plane in Dilute Ether Electrolytes Using Electric-Field-Responsive Solvent for High-Voltage Lithium Metal Batteries","authors":"Junru Wu, Ziyao Gao, Zhiqiang Fu, Lili Lin, Xianshu Wang, Yun Zhao, Lele Peng, Feiyu Kang, Zhenyu Guo, Maria-Magdalena Titirici, Yunlong Zhao, Xiulin Fan, Baohua Li","doi":"10.1039/d4ee05818f","DOIUrl":"https://doi.org/10.1039/d4ee05818f","url":null,"abstract":"Raising the cut-off voltage to 4.6 V can boost the energy density of lithium metal batteries (LMBs) with LiCoO2 cathode. However, the unfavorable cathode electrolyte interphase (CEI) formed on high-voltage cathode when using Li metal-compatible ether electrolytes leads to short lifespan of batteries. Here we harness the battery intrinsic electric field to manipulate the cathode inner Helmholtz plane (IHP) during the battery’s charge through simply introducing an electric-field-responsive solvent into an ether electrolyte. Specifically, 2,2-difluoroethyl trifluoromethanesulfonate (DTS) as a weak solvated co-solvent preferentially adsorbs on the cathode surface under the electric field activation. Owing to the majority of “high-voltage fragile” 1,2-dimethoxyethane ether molecules squeezed out from the IHP by DTS, a LiF-rich and organics-less stable CEI film is formed, which minimizes cathode cracking and structure degradation under high-voltage. The DTS-containing electrolyte shows superior cycling stability of LMBs under harsh conditions of 4.6 V, 4.2 mAh cm-2 cathode loading and 15 μL lean electrolyte. Furthermore, the feasibility of this concept is validated in practical Ah-level pouch full cells. This work highlights the significance of the IHP modulation and interfacial chemistry, providing an alternative pathway towards ether-based electrolytes engineering for high-voltage LMBs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"33 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640286","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}
Alkaline electrochemical hydrogen evolution reaction (HER) has been a hot topic in energy catalysis and engineering. Theoretically, intensifying OH adsorption on electrocatalyst is vital for promoting water dissociation and thus supplying sufficient proton to expedite alkaline hydrogen evolution. However, overbinding of OH largely impedes the recyclability of active centers and even causes catalyst deactivation. Herein, we report that H2O dissociation and OH desorption presents an undesirable scaling relationship, which poses a major stumbling block to attain maximized alkaline HER performance. While, dispersing highly oxophilic metal centers to single atoms greatly facilitates OH desorption and meanwhile keeps the high oxophilicity-enabled superb water dissociation merit, hence breaking the proportionality limitation. Based on this finding, a remarkable La1-Run catalyst is rationally synthesized, which operates durably at an ampere-level current density of 1000 mA cm-2 for over two months with an ultra-low cell voltage of 1.74 V, showing great promise for practical applications.
{"title":"Breaking the H2O dissociation-OH desorption scaling relationship in alkaline hydrogen evolution by oxophilic single atom M1-Run electrocatalyst","authors":"Xinhu Liang, Zhihao Zhang, Zhe Wang, mingzhen hu, Dan Cheng, Yue Jiang, Hao Ren, Fengyi Shen, Shitu Yang, Xiaoxin Yang, Wenkun Jiang, Xianghui Shi, Zihao Ma, Kebin Zhou","doi":"10.1039/d5ee00152h","DOIUrl":"https://doi.org/10.1039/d5ee00152h","url":null,"abstract":"Alkaline electrochemical hydrogen evolution reaction (HER) has been a hot topic in energy catalysis and engineering. Theoretically, intensifying OH adsorption on electrocatalyst is vital for promoting water dissociation and thus supplying sufficient proton to expedite alkaline hydrogen evolution. However, overbinding of OH largely impedes the recyclability of active centers and even causes catalyst deactivation. Herein, we report that H2O dissociation and OH desorption presents an undesirable scaling relationship, which poses a major stumbling block to attain maximized alkaline HER performance. While, dispersing highly oxophilic metal centers to single atoms greatly facilitates OH desorption and meanwhile keeps the high oxophilicity-enabled superb water dissociation merit, hence breaking the proportionality limitation. Based on this finding, a remarkable La1-Run catalyst is rationally synthesized, which operates durably at an ampere-level current density of 1000 mA cm-2 for over two months with an ultra-low cell voltage of 1.74 V, showing great promise for practical applications.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"16 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640022","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}
Permanent magnets are used in various products and essential for human society. If omnipresent permanent magnets could directly convert heat into electricity, they would lead to innovative energy harvesting and thermal management technologies. However, achieving such “multifunctionality” has been difficult due to poor thermoelectric performance of conventional magnets. In this work, we develop a multifunctional composite magnet (MCM) that enables giant transverse thermoelectric conversion while possessing permanent magnet features. MCM comprising alternately and obliquely stacked SmCo5/Bi0.2Sb1.8Te3 multilayers exhibits an excellent transverse thermoelectric figure of merit zxyT of 0.20 at room temperature owing to the optimized anisotropic structure and extremely low interfacial electrical and thermal resistivities between the SmCo5 and Bi0.2Sb1.8Te3 layers. The MCM-based thermopile module generates a maximum of 204 mW at a temperature difference of 152 K, whose power density normalized by the heat transfer area and temperature gradient is not only record-high among transverse thermoelectric modules but also comparable to those of commercial thermoelectric modules utilizing the Seebeck effect. The multifunctionality of our MCM provides unprecedented opportunities for energy harvesting and thermal management everywhere permanent magnets are currently used.
{"title":"Multifunctional composite magnet realizing record-high transverse thermoelectric generation","authors":"Fuyuki Ando, Takamasa Hirai, Abdulkareem Alasli, Hossein Sepehri-Amin, Yutaka Iwasaki, Hosei Nagano, Ken-ichi Uchida","doi":"10.1039/d4ee04845h","DOIUrl":"https://doi.org/10.1039/d4ee04845h","url":null,"abstract":"Permanent magnets are used in various products and essential for human society. If omnipresent permanent magnets could directly convert heat into electricity, they would lead to innovative energy harvesting and thermal management technologies. However, achieving such “multifunctionality” has been difficult due to poor thermoelectric performance of conventional magnets. In this work, we develop a multifunctional composite magnet (MCM) that enables giant transverse thermoelectric conversion while possessing permanent magnet features. MCM comprising alternately and obliquely stacked SmCo<small><sub>5</sub></small>/Bi<small><sub>0.2</sub></small>Sb<small><sub>1.8</sub></small>Te<small><sub>3</sub></small> multilayers exhibits an excellent transverse thermoelectric figure of merit <em>z</em><small><sub><em>xy</em></sub></small><em>T</em> of 0.20 at room temperature owing to the optimized anisotropic structure and extremely low interfacial electrical and thermal resistivities between the SmCo<small><sub>5</sub></small> and Bi<small><sub>0.2</sub></small>Sb<small><sub>1.8</sub></small>Te<small><sub>3</sub></small> layers. The MCM-based thermopile module generates a maximum of 204 mW at a temperature difference of 152 K, whose power density normalized by the heat transfer area and temperature gradient is not only record-high among transverse thermoelectric modules but also comparable to those of commercial thermoelectric modules utilizing the Seebeck effect. The multifunctionality of our MCM provides unprecedented opportunities for energy harvesting and thermal management everywhere permanent magnets are currently used.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"34 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640281","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}
Yuetao Ma, Likun Chen, Yuhang Li, Boyu Li, Xufei An, Xing Cheng, Hai Su, Ke Yang, Guanyou Xiao, Yang Zhao, Zhuo Han, Shaoke Guo, Jinshuo Mi, Peiran Shi, Ming Liu, Yan-Bing He, Feiyu Kang
Developing solid-state polymer electrolytes with both high voltage and ionic conductivity is essential for practical solid-state batteries. Poly(vinylidene fluoride) (PVDF)-based solid-state electrolytes are attractive for solid-state lithium metal batteries (LMBs). However, their high mesoscale heterogeneity induced by phase separation during electrolyte preparation leads to the formation of large PVDF spherulites. Herein, we demonstrate that the mesoscale heterogeneity causes the accumulation of Li+ on the surfaces of oversized PVDF spherulites. The large spherulites with low interface-bulk ratios greatly impede the efficient long-range Li+ conduction within the electrolyte. We propose an efficient strategy to regulate the geometric structure of PVDF spherulites by introducing the polyvinyl alcohol (PVA) coated dielectric SrTiO3 (PVA@STO) as a nucleating agent in a PVDF-based electrolyte. The excellent interfacial compatibility of the PVA coating layer with PVDF facilitates the uniform dispersion of PVA@STO nano-fillers and regulates the nucleation to form abundant finer PVDF spherulites with more interfaces, thereby providing abundant Li+ transport pathways. Furthermore, the well-dispersed PVA@STO nano-fillers can effectively dissociate lithium salt to generate more mobile Li+ in the PVDF–PVA@STO electrolyte that exhibits a high ionic conductivity of 8.6 × 10−4 S cm−1. The Li|PVDF–PVA@STO|NCM811 batteries demonstrate excellent high rate cycling performance, retaining 80.8% and 70.5% capacity after 2000 cycles at 5C and 10C, respectively. This work clearly demonstrates the significant effect of mesoscale structure regulation on a polymer structure for high-performance fast-charging solid-state lithium metal batteries.
{"title":"Mesoscale polymer regulation for fast-charging solid-state lithium metal batteries","authors":"Yuetao Ma, Likun Chen, Yuhang Li, Boyu Li, Xufei An, Xing Cheng, Hai Su, Ke Yang, Guanyou Xiao, Yang Zhao, Zhuo Han, Shaoke Guo, Jinshuo Mi, Peiran Shi, Ming Liu, Yan-Bing He, Feiyu Kang","doi":"10.1039/d5ee00203f","DOIUrl":"https://doi.org/10.1039/d5ee00203f","url":null,"abstract":"Developing solid-state polymer electrolytes with both high voltage and ionic conductivity is essential for practical solid-state batteries. Poly(vinylidene fluoride) (PVDF)-based solid-state electrolytes are attractive for solid-state lithium metal batteries (LMBs). However, their high mesoscale heterogeneity induced by phase separation during electrolyte preparation leads to the formation of large PVDF spherulites. Herein, we demonstrate that the mesoscale heterogeneity causes the accumulation of Li<small><sup>+</sup></small> on the surfaces of oversized PVDF spherulites. The large spherulites with low interface-bulk ratios greatly impede the efficient long-range Li<small><sup>+</sup></small> conduction within the electrolyte. We propose an efficient strategy to regulate the geometric structure of PVDF spherulites by introducing the polyvinyl alcohol (PVA) coated dielectric SrTiO<small><sub>3</sub></small> (PVA@STO) as a nucleating agent in a PVDF-based electrolyte. The excellent interfacial compatibility of the PVA coating layer with PVDF facilitates the uniform dispersion of PVA@STO nano-fillers and regulates the nucleation to form abundant finer PVDF spherulites with more interfaces, thereby providing abundant Li<small><sup>+</sup></small> transport pathways. Furthermore, the well-dispersed PVA@STO nano-fillers can effectively dissociate lithium salt to generate more mobile Li<small><sup>+</sup></small> in the PVDF–PVA@STO electrolyte that exhibits a high ionic conductivity of 8.6 × 10<small><sup>−4</sup></small> S cm<small><sup>−1</sup></small>. The Li|PVDF–PVA@STO|NCM811 batteries demonstrate excellent high rate cycling performance, retaining 80.8% and 70.5% capacity after 2000 cycles at 5C and 10C, respectively. This work clearly demonstrates the significant effect of mesoscale structure regulation on a polymer structure for high-performance fast-charging solid-state lithium metal batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"54 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640282","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}
Flexible perovskite solar cells (f-PSCs) have garnered increasing research interest owing to their high power-to-weight ratio and ability to integrate into buildings. However, the mismatch of the thermal expansion coefficient between the perovskite film and substrate will result in strain in the perovskite layer, which significantly impairs the photovoltaic and mechanical performance of f-PSCs. Herein, a thermodynamic regulation strategy was proposed to release the stress of perovskite film, realizing highly efficient f-PSCs with excellent flexibility. Camphor exhibits a strong affinity with Pb2+ or FA+ due to the strong electronegativity of the carbonyl functional group. During annealing, the sublimation of camphor exerts a force on the compressed lattice, driving the transformation of the distorted [PbI6]4− into a symmetry arrangement. Furthermore, the camphor-modified perovskite film exhibits lower defect state density, and the obtained f-PSCs achieved a power conversion efficiency of 24.48%, which exhibited outstanding mechanical and operational stability.
{"title":"Stress Release via Thermodynamic Regulation towards Efficient Flexible Perovskite Solar Cells","authors":"Zhiyang Xu, Runnan Yu, Tangyue Xue, Qiang Guo, Qianglong Lv, Chen Zhang, Erjun Zhou, Zhan'ao Tan","doi":"10.1039/d5ee00342c","DOIUrl":"https://doi.org/10.1039/d5ee00342c","url":null,"abstract":"Flexible perovskite solar cells (f-PSCs) have garnered increasing research interest owing to their high power-to-weight ratio and ability to integrate into buildings. However, the mismatch of the thermal expansion coefficient between the perovskite film and substrate will result in strain in the perovskite layer, which significantly impairs the photovoltaic and mechanical performance of f-PSCs. Herein, a thermodynamic regulation strategy was proposed to release the stress of perovskite film, realizing highly efficient f-PSCs with excellent flexibility. Camphor exhibits a strong affinity with Pb2+ or FA+ due to the strong electronegativity of the carbonyl functional group. During annealing, the sublimation of camphor exerts a force on the compressed lattice, driving the transformation of the distorted [PbI6]4− into a symmetry arrangement. Furthermore, the camphor-modified perovskite film exhibits lower defect state density, and the obtained f-PSCs achieved a power conversion efficiency of 24.48%, which exhibited outstanding mechanical and operational stability.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"7 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640284","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}
Xun Jiao, Li Tan, Xiaoxia Tang, Cheng Tong, Tao Wang, Minhua Shao, Bin Liu, Cunpu Li, Zidong Wei
Lithium-sulfur batteries (LSBs) form soluble polysulfides (LiPSs) during discharge, leading to decline of cycling performance, especially the failure of pouch batteries. The failure may be since conventional sulfur hosts can only adsorb LiPSs and cannot rapidly inject and transfer electrons in electrochemical reactions. The sluggish electrochemical interconversion of LiPSs makes the continues loss of the active materials, which is a barrier to long-life commercial LSBs. Herein, an electron-triode-like GeS2-NiS2 heterostructure is successfully designed to serve as a sulfur host. An Ohmic contact rather than a Schottky contact is formed between GeS2 and NiS2, which is proven by the ultraviolet photoelectron spectra and X-ray absorption fine structure spectra. Therefore, the LiPSs can be interconverted with an electron-triode-like model: NiS2 acts as the emitter and injects a bunching of electrons into the LiPSs (the collector) through the GeS2 base electrode, with a maximum reaction current amplification factor (βR) of 105.87. In-situ XRD and ex-situ AFM indicate that the bunching injection of electrons can achieve an advanced deposition of Li2S as early as ~80% SOC. Ultimately, the S@GeS2-NiS2/rGO battery achieves a high specific capacity of 1007.8 mAh g-1 at 0.5 C. The 1.2 Ah pouch battery can achieve a high energy density of 405 Wh kg-1 and work stably for 200 cycles, highlighting its great potential for practical applications.
{"title":"405 Wh kg-1 Ah-level Lithium-Sulfur Pouch Battery Stabilized over 200 Cycles by Electron-Triode-like GeS2-NiS2 Heterostructure","authors":"Xun Jiao, Li Tan, Xiaoxia Tang, Cheng Tong, Tao Wang, Minhua Shao, Bin Liu, Cunpu Li, Zidong Wei","doi":"10.1039/d5ee00615e","DOIUrl":"https://doi.org/10.1039/d5ee00615e","url":null,"abstract":"Lithium-sulfur batteries (LSBs) form soluble polysulfides (LiPSs) during discharge, leading to decline of cycling performance, especially the failure of pouch batteries. The failure may be since conventional sulfur hosts can only adsorb LiPSs and cannot rapidly inject and transfer electrons in electrochemical reactions. The sluggish electrochemical interconversion of LiPSs makes the continues loss of the active materials, which is a barrier to long-life commercial LSBs. Herein, an electron-triode-like GeS2-NiS2 heterostructure is successfully designed to serve as a sulfur host. An Ohmic contact rather than a Schottky contact is formed between GeS<small><sub>2</sub></small> and NiS<small><sub>2</sub></small>, which is proven by the ultraviolet photoelectron spectra and X-ray absorption fine structure spectra. Therefore, the LiPSs can be interconverted with an electron-triode-like model: NiS<small><sub>2</sub></small> acts as the emitter and injects a bunching of electrons into the LiPSs (the collector) through the GeS<small><sub>2</sub></small> base electrode, with a maximum reaction current amplification factor (β<small><sub>R</sub></small>) of 105.87. In-situ XRD and ex-situ AFM indicate that the bunching injection of electrons can achieve an advanced deposition of Li<small><sub>2</sub></small>S as early as ~80% SOC. Ultimately, the S@GeS<small><sub>2</sub></small>-NiS<small><sub>2</sub></small>/rGO battery achieves a high specific capacity of 1007.8 mAh g<small><sup>-1</sup></small> at 0.5 C. The 1.2 Ah pouch battery can achieve a high energy density of 405 Wh kg<small><sup>-1</sup></small> and work stably for 200 cycles, highlighting its great potential for practical applications.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"55 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640283","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}
Dawei Xi, Zheng Yang, Michael S Emanuel, Panlin Zhao, Michael J. Aziz
Carbon dioxide capture and management are critical technologies for achieving carbon neutrality and mitigating the impacts of global warming. One promising approach for decarbonization involves electrochemical generation of concentrated acid and base. This effectively decouples the carbon capture-release process from the electrochemical cell, avoiding the kinetic limitations associated with reactions involving CO2. Designing an electrochemical acid-base generator with high current efficiency and low energy cost is challenging. Following investigations of the crossover rates of protons and hydroxide ions through ion-exchange membranes, we designed a multichambered electrochemical cell for generating weak acid and strong base, which significantly suppressed acid-base crossover. By equipping the center chamber with a serpentine flow field, we achieved acid-base production at high concentrations (> 1 M) and high Coulombic efficiency (> 95%) while maintaining relatively low energy costs. With this device, we demonstrated carbon management examples of simulated flue gas capture, direct air capture, and green production of slaked lime, as one step toward green cement production. The key components of the prototype can be adapted for use in other electrochemical cell designs, ensuring high efficiency in concentrated acid-base generation in other application scenarios.
{"title":"Electrochemical acid-base generators for decoupled carbon management","authors":"Dawei Xi, Zheng Yang, Michael S Emanuel, Panlin Zhao, Michael J. Aziz","doi":"10.1039/d4ee05109b","DOIUrl":"https://doi.org/10.1039/d4ee05109b","url":null,"abstract":"Carbon dioxide capture and management are critical technologies for achieving carbon neutrality and mitigating the impacts of global warming. One promising approach for decarbonization involves electrochemical generation of concentrated acid and base. This effectively decouples the carbon capture-release process from the electrochemical cell, avoiding the kinetic limitations associated with reactions involving CO2. Designing an electrochemical acid-base generator with high current efficiency and low energy cost is challenging. Following investigations of the crossover rates of protons and hydroxide ions through ion-exchange membranes, we designed a multichambered electrochemical cell for generating weak acid and strong base, which significantly suppressed acid-base crossover. By equipping the center chamber with a serpentine flow field, we achieved acid-base production at high concentrations (> 1 M) and high Coulombic efficiency (> 95%) while maintaining relatively low energy costs. With this device, we demonstrated carbon management examples of simulated flue gas capture, direct air capture, and green production of slaked lime, as one step toward green cement production. The key components of the prototype can be adapted for use in other electrochemical cell designs, ensuring high efficiency in concentrated acid-base generation in other application scenarios.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"24 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143635183","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}
Boli Nie, Yanming Meng, Simeng Niu, Longjie Gong, Yufeng Chen, Liujun Guo, Xiang Li, Yan-Chao Wu, Hui-Jing Li, Weiwei Zhang
In contemporary times, the issue of freshwater resource scarcity has become increasingly acute. Interfacial solar evaporation (ISE) technology is highly anticipated to address this conundrum. Nevertheless, in practical applications, the intricate properties of sewage are frequently neglected. At this point, the utilization of Janus films for ISE is undoubtedly a significant breakthrough, which has completely revolutionized the traditional evaporation pattern. Given the immense potential exhibited by Janus films in the domain of ISE, it is of crucial significance to conduct in-depth research and comprehensive analysis thereon. This review commences with a comprehensive examination of the merits possessed by Janus film based ISE. Subsequently, it elaborates in detail from aspects such as structure, manufacturing materials, and practical applications. Meanwhile, vital overall sustainable footprint equations for performance evaluation and practical applications are presented. Additionally, it precisely pinpoints the challenges in light of the current research status. The incorporation of Janus films into the burgeoning ISE technology signifies a revolutionary achievement, presenting extremely prospective solutions within the realms of seawater desalination and wastewater treatment.
{"title":"Janus solar evaporators: a review of innovative technologies and diverse applications","authors":"Boli Nie, Yanming Meng, Simeng Niu, Longjie Gong, Yufeng Chen, Liujun Guo, Xiang Li, Yan-Chao Wu, Hui-Jing Li, Weiwei Zhang","doi":"10.1039/d5ee00159e","DOIUrl":"https://doi.org/10.1039/d5ee00159e","url":null,"abstract":"In contemporary times, the issue of freshwater resource scarcity has become increasingly acute. Interfacial solar evaporation (ISE) technology is highly anticipated to address this conundrum. Nevertheless, in practical applications, the intricate properties of sewage are frequently neglected. At this point, the utilization of Janus films for ISE is undoubtedly a significant breakthrough, which has completely revolutionized the traditional evaporation pattern. Given the immense potential exhibited by Janus films in the domain of ISE, it is of crucial significance to conduct in-depth research and comprehensive analysis thereon. This review commences with a comprehensive examination of the merits possessed by Janus film based ISE. Subsequently, it elaborates in detail from aspects such as structure, manufacturing materials, and practical applications. Meanwhile, vital overall sustainable footprint equations for performance evaluation and practical applications are presented. Additionally, it precisely pinpoints the challenges in light of the current research status. The incorporation of Janus films into the burgeoning ISE technology signifies a revolutionary achievement, presenting extremely prospective solutions within the realms of seawater desalination and wastewater treatment.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"14 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640289","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}
Ziyong Kang, Peng Feng, Kun Wang, Lu Zhang, Rui Meng, Yali Chen, Jiandong Wu, Feng Yang, Xuewen Zhang, Tianxiang Li, Jingzhi Shang, Yu Tong, Hongqiang Wang
Tin perovskite films with two-dimensional/three-dimensional (2D/3D) heterostructures promise high performance lead-free perovskite solar cells (PSCs), while they are challenged by the undesirable carrier transport due to intrinsic multi-quantum wells, and susceptible crystallization kinetics upon the introduced organic spacer cations. We herein propose and validate a strategy that could simultaneously address these challenges based on synchronous dimension-crystallization engineering in 2D/3D tin perovskite films. Different from the conventional dimension engineering that relies on precise n-phase control, the employed 4-guanidinium benzoate hydrochloride (GBAC) in present work has an unforeseen desorption effect between phenylethylamine (PEA) and the perovskite, which leads to a direct transition from the 2D to the 3D phase. It is also found that introducing GBAC results in the formation of elongated organic-inorganic hybrid chains, which improve the crystallization process of the films by accelerating both nucleation and growth rates. By virtue of these merits, the resulted tin PSCs achieve a champion power conversion efficiency of 15.02%, together with an exceptional long-term stability with 87% remaining after 4000 h and 80% after 400 h under working at the maximum power point.
{"title":"Synchronous Dimension-Crystallization Engineering Enables Highly Efficient 2D/3D Tin Perovskite Solar Cells","authors":"Ziyong Kang, Peng Feng, Kun Wang, Lu Zhang, Rui Meng, Yali Chen, Jiandong Wu, Feng Yang, Xuewen Zhang, Tianxiang Li, Jingzhi Shang, Yu Tong, Hongqiang Wang","doi":"10.1039/d4ee06142j","DOIUrl":"https://doi.org/10.1039/d4ee06142j","url":null,"abstract":"Tin perovskite films with two-dimensional/three-dimensional (2D/3D) heterostructures promise high performance lead-free perovskite solar cells (PSCs), while they are challenged by the undesirable carrier transport due to intrinsic multi-quantum wells, and susceptible crystallization kinetics upon the introduced organic spacer cations. We herein propose and validate a strategy that could simultaneously address these challenges based on synchronous dimension-crystallization engineering in 2D/3D tin perovskite films. Different from the conventional dimension engineering that relies on precise n-phase control, the employed 4-guanidinium benzoate hydrochloride (GBAC) in present work has an unforeseen desorption effect between phenylethylamine (PEA) and the perovskite, which leads to a direct transition from the 2D to the 3D phase. It is also found that introducing GBAC results in the formation of elongated organic-inorganic hybrid chains, which improve the crystallization process of the films by accelerating both nucleation and growth rates. By virtue of these merits, the resulted tin PSCs achieve a champion power conversion efficiency of 15.02%, together with an exceptional long-term stability with 87% remaining after 4000 h and 80% after 400 h under working at the maximum power point.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"20 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143627400","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}
Yuxuan Zhang, Minyoung Kim, Dong Hun Lee, Fei Qin, Han Wook Song, Chung Soo Kim, Jeongmin Park, Chohee Kim, Fang Lian, Sunghwan Lee
Although Zn (101) exhibits faster Zn²⁺ plating/stripping kinetics and stronger bonding with Zn2+ compared to Zn (002), the application of Zn (101) in Zn batteries has been limited due to its higher reactivity with water. However, a novel approach utilizing spontaneous self-passivation of plated Zn (101) offers the potential to harness its favorable kinetics and stronger Zn-Zn bonding for battery applications. Here, we present a high-utilization and fast-kinetics Zn anode by promoting selective (101) facet growth and achieving spontaneous passivation of the underlying Zn plating. A non-stoichiometric Sn-O system is selected as the modification material because of its ability of engineering crystal structures (amorphous, rutile, layered) and manipulating electrical polarity (n-type vs p-type). The optimized SnO1.17 saturates dangling bonds of Zn (101), benefiting the preferential growth of well-aligned Zn (101) planes. Besides, the Zn2+ plating location is altered underlying the interphase due to synergetic effects of lower Zn2+ migration barriers of the layered structure and electron-blocking properties of SnO1.17. Consequently, a high Zn utilization ratio of over 91.5% is achieved for 800 hours, with an impressively low overpotential of 43 mV. Furthermore, an anode-free system combining a ZnMn2O4 cathode and a SnO1.17@Cu anode retained 81.6% capacity after 200 cycles.
{"title":"Spontaneous Passivation of Selective Zn (101) Plating via Dangling Bond Saturation and Electrostatic Interaction Regulation for High-Utilization, Fast-Kinetics Zinc Anodes","authors":"Yuxuan Zhang, Minyoung Kim, Dong Hun Lee, Fei Qin, Han Wook Song, Chung Soo Kim, Jeongmin Park, Chohee Kim, Fang Lian, Sunghwan Lee","doi":"10.1039/d4ee05498a","DOIUrl":"https://doi.org/10.1039/d4ee05498a","url":null,"abstract":"Although Zn (101) exhibits faster Zn²⁺ plating/stripping kinetics and stronger bonding with Zn2+ compared to Zn (002), the application of Zn (101) in Zn batteries has been limited due to its higher reactivity with water. However, a novel approach utilizing spontaneous self-passivation of plated Zn (101) offers the potential to harness its favorable kinetics and stronger Zn-Zn bonding for battery applications. Here, we present a high-utilization and fast-kinetics Zn anode by promoting selective (101) facet growth and achieving spontaneous passivation of the underlying Zn plating. A non-stoichiometric Sn-O system is selected as the modification material because of its ability of engineering crystal structures (amorphous, rutile, layered) and manipulating electrical polarity (n-type vs p-type). The optimized SnO1.17 saturates dangling bonds of Zn (101), benefiting the preferential growth of well-aligned Zn (101) planes. Besides, the Zn2+ plating location is altered underlying the interphase due to synergetic effects of lower Zn2+ migration barriers of the layered structure and electron-blocking properties of SnO1.17. Consequently, a high Zn utilization ratio of over 91.5% is achieved for 800 hours, with an impressively low overpotential of 43 mV. Furthermore, an anode-free system combining a ZnMn2O4 cathode and a SnO1.17@Cu anode retained 81.6% capacity after 200 cycles.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"40 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143618815","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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