Halogenated volatile additives play an important role in well regulating blend morphology in polymer solar cells (PSCs). However, the mismatched crystallization rate between the donor and acceptor often leads to the difficulties in realizing desirable morphology, further resulting in non-radiative recombination energy loss (ΔEnon-rad). Herein, a series of halogenated volatile additives of 1-fluoro-3,5-dimethoxybenzene (F-DMB), 1-chloro-3,5-dimethoxybenzene (Cl-DMB), 1-bromo-3,5-dimethoxybenzene (Br-DMB) and 1-iodo-3,5-dimethoxybenzene (I-DMB) have been designed to optimize the interaction with donor and acceptor, thereby regulating the crystallization kinetics, improving morphology quality and reducing ΔEnon-rad. As the weight of halogen atom of additive increased, the promoting effect on PM6 strengthened gradually, thus shortening the crystallization time. However, such promoting effect on L8-BO was weakened, resulting in a longer crystallization time. Therefore, this strategy made the crystallization time ratio approach to unity with a more balanced crystallization behavior. Due to the well-regulated crystallization kinetics and optimized intermolecular aggregation, the optimal morphology with suppressed energy disorder and ΔEnon-rad were realized. The I-DMB-treated PSCs achieved the champion power conversion efficiency (PCE) of 20.40% and minimized ΔEnon-rad of 0.189 eV. This work offers valuable insights into how to utilize volatile additives for regulating crystallization kinetics and optimizing desirable morphology of PSCs for further improving photovoltaic performance.
{"title":"Halogenated Volatile Additive Strategy for Regulating Crystallization Kinetics and Enabling 20.40% Efficiency Polymer Solar Cells with Low Non-Radiative Recombination Energy Loss","authors":"Changjiang Li, Min Deng, Haonan Chen, Yuwei Duan, Chentong Liao, Zeqin Chen, Qiang Peng","doi":"10.1039/d5ee01368b","DOIUrl":"https://doi.org/10.1039/d5ee01368b","url":null,"abstract":"Halogenated volatile additives play an important role in well regulating blend morphology in polymer solar cells (PSCs). However, the mismatched crystallization rate between the donor and acceptor often leads to the difficulties in realizing desirable morphology, further resulting in non-radiative recombination energy loss (ΔEnon-rad). Herein, a series of halogenated volatile additives of 1-fluoro-3,5-dimethoxybenzene (F-DMB), 1-chloro-3,5-dimethoxybenzene (Cl-DMB), 1-bromo-3,5-dimethoxybenzene (Br-DMB) and 1-iodo-3,5-dimethoxybenzene (I-DMB) have been designed to optimize the interaction with donor and acceptor, thereby regulating the crystallization kinetics, improving morphology quality and reducing ΔEnon-rad. As the weight of halogen atom of additive increased, the promoting effect on PM6 strengthened gradually, thus shortening the crystallization time. However, such promoting effect on L8-BO was weakened, resulting in a longer crystallization time. Therefore, this strategy made the crystallization time ratio approach to unity with a more balanced crystallization behavior. Due to the well-regulated crystallization kinetics and optimized intermolecular aggregation, the optimal morphology with suppressed energy disorder and ΔEnon-rad were realized. The I-DMB-treated PSCs achieved the champion power conversion efficiency (PCE) of 20.40% and minimized ΔEnon-rad of 0.189 eV. This work offers valuable insights into how to utilize volatile additives for regulating crystallization kinetics and optimizing desirable morphology of PSCs for further improving photovoltaic performance.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"7 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876348","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}
Substantial VOC loss and halide segregation in wide-bandgap (WBG) perovskite sub-cells pose significant challenges for advancing all-perovskite tandem solar cells (APTSCs). Regarding this, one of the most impactful developments is the application of hole-selective self-assembled monolayers (SAMs), leading to the advancement in APTSC technology. However, SAMs with poor polar-solvent resistance would be inevitably delaminated from substrates during perovskite precursor coating, remaining great challenge in achieving a complete SAMs coverage with derivatization issues, e.g. defective perovskite and considerable interface energy loss. Here, we introduced an in-situ molecular compensation strategy to address the inherent flaw of SAMs within WBG perovskites via incorporating 5-ammonium valeric acid iodide (5-AVAI). The larger-dipole 5-AVAI spontaneously accumulates toward the buried interface to compensate the SAMs-deficient sites when depositing WBG perovskite, effectively minimizing interfacial energy loss. Simultaneously, amphoteric 5-AVAI with amino and carboxyl groups can compensate the defects at grain boundaries for solid passivation. Consequently, a champion efficiency of 20.23% with a record VOC of 1.376 V was realized on WBG devices, enabling an efficiency of 28.9% for the APTSCs. Encouragingly, the tandems showed good operational stability and retained 87.3% of their efficiency after 800 hours of tracking.
{"title":"In-situ molecular compensation in wide-bandgap perovskite for efficient all-perovskite tandem solar cells","authors":"Sheng Fu, Nannan Sun, Shuaifeng Hu, Hao Chen, Xingxing Jiang, Yunfei Li, Xiaotian Zhu, Xuemin Guo, Wenxiao Zhang, Xiaodong Li, Andrey S. Vasenko, Junfeng Fang","doi":"10.1039/d5ee01369k","DOIUrl":"https://doi.org/10.1039/d5ee01369k","url":null,"abstract":"Substantial VOC loss and halide segregation in wide-bandgap (WBG) perovskite sub-cells pose significant challenges for advancing all-perovskite tandem solar cells (APTSCs). Regarding this, one of the most impactful developments is the application of hole-selective self-assembled monolayers (SAMs), leading to the advancement in APTSC technology. However, SAMs with poor polar-solvent resistance would be inevitably delaminated from substrates during perovskite precursor coating, remaining great challenge in achieving a complete SAMs coverage with derivatization issues, e.g. defective perovskite and considerable interface energy loss. Here, we introduced an in-situ molecular compensation strategy to address the inherent flaw of SAMs within WBG perovskites via incorporating 5-ammonium valeric acid iodide (5-AVAI). The larger-dipole 5-AVAI spontaneously accumulates toward the buried interface to compensate the SAMs-deficient sites when depositing WBG perovskite, effectively minimizing interfacial energy loss. Simultaneously, amphoteric 5-AVAI with amino and carboxyl groups can compensate the defects at grain boundaries for solid passivation. Consequently, a champion efficiency of 20.23% with a record VOC of 1.376 V was realized on WBG devices, enabling an efficiency of 28.9% for the APTSCs. Encouragingly, the tandems showed good operational stability and retained 87.3% of their efficiency after 800 hours of tracking.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"42 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876349","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}
Metal/metal oxide composites represent a promising group of catalysts that can substantially reduce the platinum group metal (PGM) loading at the cathode for proton exchange membrane water electrolysis (PEM-WE). However, the complete hydrogen evolution reaction (HER) kinetics at the complex metal/support interface are not fully understood. Here, using Pt nanoparticles on boron-modified oxygen-defective tungsten oxide (Pt/B-WO2.9) as a model system, we establish an overall kinetic framework induced by strong metal-oxide interaction, termed as ordered interfacial domain expansion catalysis (OIDEC), to elucidate the hydrogen behavior through combining in-situ spectroscopic, in-situ electrochemical, and theoretical calculation studies. This mechanism allows favorable proton adsorption on active site (Pt) from ordered interfacial water, sequential hydrogen spillover from active site (Pt) to auxiliary sites (W, O), and direct H-H coupling on auxiliary sites (W, O) for H2 evolution. In a practical PEM-WE device, Pt/B-WO2.9 shows high mass activity (1237 A mgPt-1 at 1.8 V) with a total Pt loading of 8.6×10-4 mg cm−2 and outstanding durability over 850 h multistep operation at industrial current densities from 1 to 2 A cm⁻² and 60°C.
{"title":"Ordered Interfacial Domain Expansion Catalysis Enhances Hydrogen Evolution for Proton Exchange Membrane Electrolysis","authors":"Shu-Hong Yu, Mingrong Qu, Yu-Xiao Cheng, Sihua Feng, Jie Xu, JiaKang Yao, Wensheng Yan, Sheng Zhu, Liang Cao, Rui Wu","doi":"10.1039/d5ee00441a","DOIUrl":"https://doi.org/10.1039/d5ee00441a","url":null,"abstract":"Metal/metal oxide composites represent a promising group of catalysts that can substantially reduce the platinum group metal (PGM) loading at the cathode for proton exchange membrane water electrolysis (PEM-WE). However, the complete hydrogen evolution reaction (HER) kinetics at the complex metal/support interface are not fully understood. Here, using Pt nanoparticles on boron-modified oxygen-defective tungsten oxide (Pt/B-WO2.9) as a model system, we establish an overall kinetic framework induced by strong metal-oxide interaction, termed as ordered interfacial domain expansion catalysis (OIDEC), to elucidate the hydrogen behavior through combining in-situ spectroscopic, in-situ electrochemical, and theoretical calculation studies. This mechanism allows favorable proton adsorption on active site (Pt) from ordered interfacial water, sequential hydrogen spillover from active site (Pt) to auxiliary sites (W, O), and direct H-H coupling on auxiliary sites (W, O) for H2 evolution. In a practical PEM-WE device, Pt/B-WO2.9 shows high mass activity (1237 A mgPt-1 at 1.8 V) with a total Pt loading of 8.6×10-4 mg cm−2 and outstanding durability over 850 h multistep operation at industrial current densities from 1 to 2 A cm⁻² and 60°C.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"14 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872287","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}
Chun Wu, Yunrui Yang, Yifan Li, Xiangxi He, Yinghao Zhang, Wenjie Huang, Qinghang Chen, Xiaohao Liu, Shuangqiang Chen, Qinfen Gu, Lin Li, Sean C. Smith, Xin Tan, Yan Yu, Xingqiao Wu, Shulei Chou
The electrochemical performance of hard carbon anode for sodium-ion batteries is primarily determined by the microstructure of materials, and the challenge lies in establishing structure-performance relationship at molecular level. So far, the understanding of intricate relationship between structure and performance in hard carbon remains piecemeal, with research efforts scattered across various aspects, thereby numerous controversies have arisen in this field. Here, we provide new insights into structure-performance relationship in hard carbon by coupling key structural parameters based on integrating theoretical computations and experimental data. Density functional theory calculations show that interlayer spacing determines diffusion behavior of sodium ions in hard carbon, while appropriate defect and curvature secure high-quality intercalation capacity. Inspired by these theoretical results, we successfully produce high-performance hard carbon with optimal microstructures through in-situ molecular reconfiguration of biomass via thermodynamically-driven approach, which is demonstrated as an effective strategy to rationally regulate the microstructure of hard carbon by comprehensive physical characterizations from macroscopic to atomic level. More importantly, cylindrical batteries (18650 and 33140 types) fabricated from industrial-scale hard carbon exhibit fabulous sodium storage behaviors with excellent wide-range temperature performance (-40-100 oC), demonstrating great potential for achieving practical sodium-ion batteries with high energy density and durability in the future.
{"title":"Unraveling Structure-performance Relationship in Hard Carbon for Sodium-ion Battery by Coupling Key Structural Parameters","authors":"Chun Wu, Yunrui Yang, Yifan Li, Xiangxi He, Yinghao Zhang, Wenjie Huang, Qinghang Chen, Xiaohao Liu, Shuangqiang Chen, Qinfen Gu, Lin Li, Sean C. Smith, Xin Tan, Yan Yu, Xingqiao Wu, Shulei Chou","doi":"10.1039/d5ee00278h","DOIUrl":"https://doi.org/10.1039/d5ee00278h","url":null,"abstract":"The electrochemical performance of hard carbon anode for sodium-ion batteries is primarily determined by the microstructure of materials, and the challenge lies in establishing structure-performance relationship at molecular level. So far, the understanding of intricate relationship between structure and performance in hard carbon remains piecemeal, with research efforts scattered across various aspects, thereby numerous controversies have arisen in this field. Here, we provide new insights into structure-performance relationship in hard carbon by coupling key structural parameters based on integrating theoretical computations and experimental data. Density functional theory calculations show that interlayer spacing determines diffusion behavior of sodium ions in hard carbon, while appropriate defect and curvature secure high-quality intercalation capacity. Inspired by these theoretical results, we successfully produce high-performance hard carbon with optimal microstructures through in-situ molecular reconfiguration of biomass via thermodynamically-driven approach, which is demonstrated as an effective strategy to rationally regulate the microstructure of hard carbon by comprehensive physical characterizations from macroscopic to atomic level. More importantly, cylindrical batteries (18650 and 33140 types) fabricated from industrial-scale hard carbon exhibit fabulous sodium storage behaviors with excellent wide-range temperature performance (-40-100 oC), demonstrating great potential for achieving practical sodium-ion batteries with high energy density and durability in the future.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"33 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872286","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}
Rechargeable aqueous zinc batteries (AZBs) offer a safe and sustainable solution for large-scale energy storage, but the freezing of electrolytes prevents AZBs from working at low temperatures. Recent research shows that the freezing point can be effectively lowered by using either concentrated salt or organic-rich electrolytes. However, these strategies result in either low oxidation stability or sluggish mass transport at low temperatures. Here, we report a multi-tentacle electrolyte (MTE) strategy that enables stable, fast and deep running of AZBs at −40 °C. MTE leverages the abundant hydrogen-bonding sites of multi-tentacle salts and organics. Adding small amounts of multi-tentacle moieties not only effectively confines water molecules’ movement and prevents their icing even at −60 °C, but also maintains low viscosity and high ionic conductivity of the electrolyte at low temperatures. At −40 °C, Zn metal anodes could stably cycle for more than 1100 hours at a high current density of 2 mA cm−2 and a high capacity of 2 mAh cm−2; high-capacity AZBs (3.4 mAh cm−2) sustain 1000 stable cycling with 99.99% retention per cycle in MTE. MTE strategy is also versatile to high-voltage LiMn2O4 cathodes, which further enhances the energy density of AZBs to 154.4 Wh kgLMO−1 at −40 °C.
{"title":"Designing multi-tentacle electrolytes to enable fast and deep cycling of aqueous Zn batteries at low temperatures","authors":"Huimin Wang, Mingzi Sun, Yongqiang Yang, Junhua Zhou, Lingtao Fang, Qiyao Huang, Bolong Huang, Zijian Zheng","doi":"10.1039/d5ee01316j","DOIUrl":"https://doi.org/10.1039/d5ee01316j","url":null,"abstract":"Rechargeable aqueous zinc batteries (AZBs) offer a safe and sustainable solution for large-scale energy storage, but the freezing of electrolytes prevents AZBs from working at low temperatures. Recent research shows that the freezing point can be effectively lowered by using either concentrated salt or organic-rich electrolytes. However, these strategies result in either low oxidation stability or sluggish mass transport at low temperatures. Here, we report a multi-tentacle electrolyte (MTE) strategy that enables stable, fast and deep running of AZBs at −40 °C. MTE leverages the abundant hydrogen-bonding sites of multi-tentacle salts and organics. Adding small amounts of multi-tentacle moieties not only effectively confines water molecules’ movement and prevents their icing even at −60 °C, but also maintains low viscosity and high ionic conductivity of the electrolyte at low temperatures. At −40 °C, Zn metal anodes could stably cycle for more than 1100 hours at a high current density of 2 mA cm−2 and a high capacity of 2 mAh cm−2; high-capacity AZBs (3.4 mAh cm−2) sustain 1000 stable cycling with 99.99% retention per cycle in MTE. MTE strategy is also versatile to high-voltage LiMn2O4 cathodes, which further enhances the energy density of AZBs to 154.4 Wh kgLMO−1 at −40 °C.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"1 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872288","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}
Yi Yuan, Zixuan Li, Rongyu Deng, Shengda D. Pu, Marc Walker, Mingzhi Cai, Feixiang Wu, Peter G. Bruce, Alex Robertson
Zn-ion batteries for practical applications face several challenges, some of which arise from the inevitable degradation of the Zn metal anode. The intrinsic thermodynamic instability of Zn metal anodes in mildly acidic Zn-ion batteries can trigger spontaneous interfacial corrosion, which leads to hydrogen evolution, the formation of byproducts, and the irreversible loss of active species during both storage and operation. Here, we delve into the intricate corrosion processes of the Zn metal anode in mildly acidic electrolytes. With the help of operando electrochemical liquid cell transmission electron microscopy, the self-dissolution of Zn is observed, and the capacity loss due to such corrosion behaviour during the cell rest period is quantified. This dissolution of Zn is found to be closely related to the initial pH value of the electrolyte and can be mitigated by pH adjustment through the slight addition of a pH buffer additive. The self-dissolution of Zn, which causes an increase in the local pH, is a prelude to the formation of corrosion byproducts that continues throughout the entire storage and cycling period. These corrosion issues are exacerbated by the presence of excess Zn metal in the system, suggesting that the feasibility of using excess Zn metal in Zn-ion batteries should be carefully evaluated. These findings further emphasise the importance of considering electrolyte pH in future electrolyte modification research, as well as its potential impacts on the stability of both the anode and cathode, and the shelf life of the entire battery.
{"title":"Identifying the role of Zn self-dissolution in the anode corrosion process in Zn-ion batteries","authors":"Yi Yuan, Zixuan Li, Rongyu Deng, Shengda D. Pu, Marc Walker, Mingzhi Cai, Feixiang Wu, Peter G. Bruce, Alex Robertson","doi":"10.1039/d5ee00485c","DOIUrl":"https://doi.org/10.1039/d5ee00485c","url":null,"abstract":"Zn-ion batteries for practical applications face several challenges, some of which arise from the inevitable degradation of the Zn metal anode. The intrinsic thermodynamic instability of Zn metal anodes in mildly acidic Zn-ion batteries can trigger spontaneous interfacial corrosion, which leads to hydrogen evolution, the formation of byproducts, and the irreversible loss of active species during both storage and operation. Here, we delve into the intricate corrosion processes of the Zn metal anode in mildly acidic electrolytes. With the help of operando electrochemical liquid cell transmission electron microscopy, the self-dissolution of Zn is observed, and the capacity loss due to such corrosion behaviour during the cell rest period is quantified. This dissolution of Zn is found to be closely related to the initial pH value of the electrolyte and can be mitigated by pH adjustment through the slight addition of a pH buffer additive. The self-dissolution of Zn, which causes an increase in the local pH, is a prelude to the formation of corrosion byproducts that continues throughout the entire storage and cycling period. These corrosion issues are exacerbated by the presence of excess Zn metal in the system, suggesting that the feasibility of using excess Zn metal in Zn-ion batteries should be carefully evaluated. These findings further emphasise the importance of considering electrolyte pH in future electrolyte modification research, as well as its potential impacts on the stability of both the anode and cathode, and the shelf life of the entire battery.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"1 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872290","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}
James Han Zhang, Rohith Mittapally, Abimbola Oluwade, Gang Chen
Evaporation fluxes from porous evaporators under sunlight have been reported to exceed the solar-thermal limit, determined by relating the incoming solar energy to the latent and sensible heat of water, for applications in desalination and brine pond drying. Although flat two-dimensional (2D) evaporators exceeding the solar limit implies a non-thermal process, tall three-dimensional (3D) solar evaporators can exceed it by absorbing additional environmental heat into its cold sidewalls. Through modeling, we explain the physics and identify the critical heights in which a fin transitions from 2D to 3D evaporation and exceeds the solar-thermal limit. Our analyses illustrate that environmental heat absorption in 3D evaporators is determined by the ambient relative humidity and the airflow velocity. The model is then coarse-grained into a large-scale fin array device on the meters scale to analyze their scalability. We identify that these devices are unlikely to scale favorably in closed environment settings such as solar stills. Our modeling clearly illustrates the benefits and limitations of 3D evaporating arrays and pinpoints design choices in previous works that hinder the device’s overall performance. This work illustrates the importance in distinguishing 2D from 3D evaporation for mechanisms underlying interfacial evaporation exceeding the solar-thermal limit.
{"title":"Mechanisms and Scale-up Potential of 3D Solar Interfacial-Evaporators","authors":"James Han Zhang, Rohith Mittapally, Abimbola Oluwade, Gang Chen","doi":"10.1039/d5ee01104c","DOIUrl":"https://doi.org/10.1039/d5ee01104c","url":null,"abstract":"Evaporation fluxes from porous evaporators under sunlight have been reported to exceed the solar-thermal limit, determined by relating the incoming solar energy to the latent and sensible heat of water, for applications in desalination and brine pond drying. Although flat two-dimensional (2D) evaporators exceeding the solar limit implies a non-thermal process, tall three-dimensional (3D) solar evaporators can exceed it by absorbing additional environmental heat into its cold sidewalls. Through modeling, we explain the physics and identify the critical heights in which a fin transitions from 2D to 3D evaporation and exceeds the solar-thermal limit. Our analyses illustrate that environmental heat absorption in 3D evaporators is determined by the ambient relative humidity and the airflow velocity. The model is then coarse-grained into a large-scale fin array device on the meters scale to analyze their scalability. We identify that these devices are unlikely to scale favorably in closed environment settings such as solar stills. Our modeling clearly illustrates the benefits and limitations of 3D evaporating arrays and pinpoints design choices in previous works that hinder the device’s overall performance. This work illustrates the importance in distinguishing 2D from 3D evaporation for mechanisms underlying interfacial evaporation exceeding the solar-thermal limit.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"31 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866905","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}
Marc Escribà-Gelonch, Jose Luis Osorio-Tejada, Le Yu, Bart Wanten, Annemie Bogaerts, Volker Hessel
This study combines for the first time techno-economic and life-cycle assessment metrics to evaluate the economic and environmental viability of plasma-assisted dry reforming of methane (DRM) for producing syngas from methane-rich natural gas. The study compares three different processes (plasma-assisted dry reforming (CO<small><sub>2</sub></small>/CH<small><sub>4</sub></small>), oxi-CO<small><sub>2</sub></small> reforming (CO<small><sub>2</sub></small>/CH<small><sub>4</sub></small>/O<small><sub>2</sub></small>) and bi-reforming (CO<small><sub>2</sub></small>/CH<small><sub>4</sub></small>/H<small><sub>2</sub></small>O)), as well as with current state-of-the-art steam reforming technology. Advancements in cost reduction and environmental performance are highlighted. While comparative studies on different plasma processing concepts have been published, their number is not large; meaning this study is bespoke in this aspect. Our study is also bespoken in extensive consideration of industrial gas separation, to provide a holistic view on sustainability with industrial viewpoint. Three different production design scenarios were considered in the analysis: DRM (scenario 1), oxy-CO<small><sub>2</sub></small> reforming of CH<small><sub>4</sub></small> (OCRM) (scenario 2), and bi-reforming of CH<small><sub>4</sub></small> (BRM) (scenario 3). This evaluation was carried out through a techno-economic analysis and a cradle-to-gate life cycle assessment (LCA). Among the scenarios analysed, OCRM demonstrates the most favourable economic performance, leading to a unitary cost of production of 549 $/tonne syngas, followed by DRM and BRM. However, when operating at large scale, the syngas production cost of BRM could compete with the benchmark if 20% reduction in plasma power consumption can be achieved, so in the near future, plasma-based BRM could be competitive against other more mature electric-powered technologies. When assessing environmental performance across 10 environmental categories of LCA metrics, OCRM is again preferred, followed by DRM and BRM. Key impact categories identified include freshwater eutrophication potential and energy consumption, which are significant contributors to environmental impacts. A study on the transition of energy sources indicates a substantial decrease in global environmental impact in the range of 50% when shifting from current electricity generation methods to wind energy sources. Comparative benchmarking reveals that the technologies evaluated in all three plasma scenarios perform better in environmental metrics across 7 over 9 categories assessed, when compared with current state-of-the-art steam reforming technologies. A material circularity indicator around 0.7 is obtained in all scenarios with slight differences, reflecting a medium-high level of circularity. Sectors such as chemicals, and recycling manufacturing could greatly benefit from our findings on plasma-assisted methane reforming. By leveraging these techn
{"title":"Techno-Economic and Life-Cycle Assessment for Syngas Production Using Sustainable Plasma-Assisted Methane Reforming Technologies","authors":"Marc Escribà-Gelonch, Jose Luis Osorio-Tejada, Le Yu, Bart Wanten, Annemie Bogaerts, Volker Hessel","doi":"10.1039/d4ee05129g","DOIUrl":"https://doi.org/10.1039/d4ee05129g","url":null,"abstract":"This study combines for the first time techno-economic and life-cycle assessment metrics to evaluate the economic and environmental viability of plasma-assisted dry reforming of methane (DRM) for producing syngas from methane-rich natural gas. The study compares three different processes (plasma-assisted dry reforming (CO<small><sub>2</sub></small>/CH<small><sub>4</sub></small>), oxi-CO<small><sub>2</sub></small> reforming (CO<small><sub>2</sub></small>/CH<small><sub>4</sub></small>/O<small><sub>2</sub></small>) and bi-reforming (CO<small><sub>2</sub></small>/CH<small><sub>4</sub></small>/H<small><sub>2</sub></small>O)), as well as with current state-of-the-art steam reforming technology. Advancements in cost reduction and environmental performance are highlighted. While comparative studies on different plasma processing concepts have been published, their number is not large; meaning this study is bespoke in this aspect. Our study is also bespoken in extensive consideration of industrial gas separation, to provide a holistic view on sustainability with industrial viewpoint. Three different production design scenarios were considered in the analysis: DRM (scenario 1), oxy-CO<small><sub>2</sub></small> reforming of CH<small><sub>4</sub></small> (OCRM) (scenario 2), and bi-reforming of CH<small><sub>4</sub></small> (BRM) (scenario 3). This evaluation was carried out through a techno-economic analysis and a cradle-to-gate life cycle assessment (LCA). Among the scenarios analysed, OCRM demonstrates the most favourable economic performance, leading to a unitary cost of production of 549 $/tonne syngas, followed by DRM and BRM. However, when operating at large scale, the syngas production cost of BRM could compete with the benchmark if 20% reduction in plasma power consumption can be achieved, so in the near future, plasma-based BRM could be competitive against other more mature electric-powered technologies. When assessing environmental performance across 10 environmental categories of LCA metrics, OCRM is again preferred, followed by DRM and BRM. Key impact categories identified include freshwater eutrophication potential and energy consumption, which are significant contributors to environmental impacts. A study on the transition of energy sources indicates a substantial decrease in global environmental impact in the range of 50% when shifting from current electricity generation methods to wind energy sources. Comparative benchmarking reveals that the technologies evaluated in all three plasma scenarios perform better in environmental metrics across 7 over 9 categories assessed, when compared with current state-of-the-art steam reforming technologies. A material circularity indicator around 0.7 is obtained in all scenarios with slight differences, reflecting a medium-high level of circularity. Sectors such as chemicals, and recycling manufacturing could greatly benefit from our findings on plasma-assisted methane reforming. By leveraging these techn","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"13 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866908","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}
Xinjie Yuan, Pengfei Qiu, Chuanyao Sun, Shiqi Yang, Yi Wu, Yumeng Wang, Ming Gu, Lidong Chen, Xun Shi
Thermoelectric (TE) technology provides a promising self-powered solution to the wearable electronics and Internet of Things (IoT), but the output voltage density and power density of current TE devices are still far below the target values for practical use. In this work, instead of the commonly used TE figure-of-merit (zT = S2σ/κT, where S is the Seebeck coefficient, σ is the electrical conductivity, κ is the thermal conductivity, and T is the absolute temperature), we propose that |S|/κ and S2σ/κ2are more effective indicators to screen the TE materials for the development of powerful TE devices used in the exacting working conditions (e.g. windless indoor environment and extremely limited space) for wearable electronics and IoT. As a case study, both the simulation and experiment well prove that the TE device consisting of n-type Ag1.995Au0.005Te0.7S0.3 and p-type Ag0.9Sb1.1Te2.1 with high |S|/κ and S2σ/κ2 can achieve higher output performance than the Bi2Te3-based TE device. When the Ag1.995Au0.005Te0.7S0.3/Ag0.9Sb1.1Te2.1 TE device is worn on human wrist, record-high voltage density and power density are achieved. This work brings a new insight to the development of advanced TE devices used for the wearable electronics and IoT.
{"title":"Screening thermoelectric materials for high output performance in wearable electronics","authors":"Xinjie Yuan, Pengfei Qiu, Chuanyao Sun, Shiqi Yang, Yi Wu, Yumeng Wang, Ming Gu, Lidong Chen, Xun Shi","doi":"10.1039/d5ee00216h","DOIUrl":"https://doi.org/10.1039/d5ee00216h","url":null,"abstract":"Thermoelectric (TE) technology provides a promising self-powered solution to the wearable electronics and Internet of Things (IoT), but the output voltage density and power density of current TE devices are still far below the target values for practical use. In this work, instead of the commonly used TE figure-of-merit (zT = S2σ/κT, where S is the Seebeck coefficient, σ is the electrical conductivity, κ is the thermal conductivity, and T is the absolute temperature), we propose that |S|/κ and S2σ/κ2are more effective indicators to screen the TE materials for the development of powerful TE devices used in the exacting working conditions (e.g. windless indoor environment and extremely limited space) for wearable electronics and IoT. As a case study, both the simulation and experiment well prove that the TE device consisting of n-type Ag1.995Au0.005Te0.7S0.3 and p-type Ag0.9Sb1.1Te2.1 with high |S|/κ and S2σ/κ2 can achieve higher output performance than the Bi2Te3-based TE device. When the Ag1.995Au0.005Te0.7S0.3/Ag0.9Sb1.1Te2.1 TE device is worn on human wrist, record-high voltage density and power density are achieved. This work brings a new insight to the development of advanced TE devices used for the wearable electronics and IoT.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"18 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862365","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}
Natalie Flores Diaz, Francesca De Rossi, Timo Keller, George Harvey Morritt, Zaida Perez- Bassart, A. Lopez-Rubio, Maria Fabra Rovira, Richard Freitag, Alessio Gagliardi, Francesca Fasulo, Ana Belen Munoz-Garcia, Michele Pavone, Hamed Javanbakht Lomeri, Sandy Sánchez, Michael Grätzel, Francesca Brunetti, Marina Freitag
Driving continuous, low-power artificial intelligence (AI) in the Internet of Things (IoT) requires reliable energy harvesting and storage under indoor or low-light conditions, where batteries face constraints such as finite lifetimes and increased environmental impact. Here, we demonstrate an integrated three-terminal dye-sensitized photocapacitor that unites a dye-sensitized solar cell (DSC) with an asymmetric supercapacitor, leveraging molecularly engi- neered polyviologen electrodes and bioderived chitosan membranes. Under 1000 lux ambient illumination, the photocapacitor delivers photocharging voltages of 920 mV, achieving power conversion efficiencies exceeding 30% and photocharging efficiencies up to 18%. Density Functional Theory calculations reveal low reorganization energies (0.1–0.2 eV) for polyviologen radical cations, promoting efficient charge transfer and stable cycling performance over 3000 charge-discharge cycles. The system reliably powers a multilayer IoT network at 500 lux for 72 hours, surpassing commercial amorphous-silicon modules by a factor of 3.5 in inference throughput. Critically, the photocapacitor driven edge microcontroller achieves 93% accuracy on CIFAR-10 classification with an energy requirement of only 0.81 mJ per inference. By eliminating the need for batteries or grid connection, this work offers a proof of concept for high-efficiency, long-lived indoor power solutions that merge advanced materials chemistry with edge AI, demonstrating a practical route toward self-sustaining, data-driven IoT devices.
{"title":"Unlocking High-Performance Photocapacitors for Edge Computing in Low-Light Environments","authors":"Natalie Flores Diaz, Francesca De Rossi, Timo Keller, George Harvey Morritt, Zaida Perez- Bassart, A. Lopez-Rubio, Maria Fabra Rovira, Richard Freitag, Alessio Gagliardi, Francesca Fasulo, Ana Belen Munoz-Garcia, Michele Pavone, Hamed Javanbakht Lomeri, Sandy Sánchez, Michael Grätzel, Francesca Brunetti, Marina Freitag","doi":"10.1039/d5ee01052g","DOIUrl":"https://doi.org/10.1039/d5ee01052g","url":null,"abstract":"Driving continuous, low-power artificial intelligence (AI) in the Internet of Things (IoT) requires reliable energy harvesting and storage under indoor or low-light conditions, where batteries face constraints such as finite lifetimes and increased environmental impact. Here, we demonstrate an integrated three-terminal dye-sensitized photocapacitor that unites a dye-sensitized solar cell (DSC) with an asymmetric supercapacitor, leveraging molecularly engi- neered polyviologen electrodes and bioderived chitosan membranes. Under 1000 lux ambient illumination, the photocapacitor delivers photocharging voltages of 920 mV, achieving power conversion efficiencies exceeding 30% and photocharging efficiencies up to 18%. Density Functional Theory calculations reveal low reorganization energies (0.1–0.2 eV) for polyviologen radical cations, promoting efficient charge transfer and stable cycling performance over 3000 charge-discharge cycles. The system reliably powers a multilayer IoT network at 500 lux for 72 hours, surpassing commercial amorphous-silicon modules by a factor of 3.5 in inference throughput. Critically, the photocapacitor driven edge microcontroller achieves 93% accuracy on CIFAR-10 classification with an energy requirement of only 0.81 mJ per inference. By eliminating the need for batteries or grid connection, this work offers a proof of concept for high-efficiency, long-lived indoor power solutions that merge advanced materials chemistry with edge AI, demonstrating a practical route toward self-sustaining, data-driven IoT devices.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"24 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862363","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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