Kangwei Mo, Xueliang Zhu, Man Yang, Zexu Xue, Sheng Li, Mubai li, Yujie Yang, Siyang Cheng, Hao Li, Qianqian Lin, Zhiping Wang
Dimethyl sulfoxide (DMSO) is commonly used as a solvent in the fabrication of perovskite solar cells. However, its strong coordination with iodoplumbate makes it difficult to remove during film formation, resulting in defects and voids at the perovskite-substrate interface, which compromise efficiency and long-term stability. Here ethyl acrylate (EA), an unsaturated monomer that aids in the effective removal of DMSO from the perovskite film is introduce. EA forms a complex with DMSO, facilitates DMSO de-intercalation, and enhances the co-evaporation process thanks to its low boiling point. Additionally, by incorporating a small amount of the initiator azobis (isobutyronitrile) (AIBN), EA is successfully polymerized into polyacrylate ethyl ester (poly-EA) during crystallization. The evaporated EA helps remove DMSO, while the poly-EA passivates defects in the perovskite films. This dual-function strategy significantly improves device performance, resulting in efficiencies of 25.4% for small-area devices and 20.3% for 15 cm2 mini-modules. Moreover, poly-EA acts as a protective barrier against moisture and ion migration. Combined with improved DMSO removal, EA-modulated devices demonstrate a T80 lifetime of up to 1800 h under maximum power point tracking at 55–60% relative humidity in ambient air.
{"title":"Minimizing DMSO Residues in Perovskite Films for Efficient and Long-Term Stable Solar Cells","authors":"Kangwei Mo, Xueliang Zhu, Man Yang, Zexu Xue, Sheng Li, Mubai li, Yujie Yang, Siyang Cheng, Hao Li, Qianqian Lin, Zhiping Wang","doi":"10.1002/aenm.202404538","DOIUrl":"https://doi.org/10.1002/aenm.202404538","url":null,"abstract":"Dimethyl sulfoxide (DMSO) is commonly used as a solvent in the fabrication of perovskite solar cells. However, its strong coordination with iodoplumbate makes it difficult to remove during film formation, resulting in defects and voids at the perovskite-substrate interface, which compromise efficiency and long-term stability. Here ethyl acrylate (EA), an unsaturated monomer that aids in the effective removal of DMSO from the perovskite film is introduce. EA forms a complex with DMSO, facilitates DMSO de-intercalation, and enhances the co-evaporation process thanks to its low boiling point. Additionally, by incorporating a small amount of the initiator azobis (isobutyronitrile) (AIBN), EA is successfully polymerized into polyacrylate ethyl ester (poly-EA) during crystallization. The evaporated EA helps remove DMSO, while the poly-EA passivates defects in the perovskite films. This dual-function strategy significantly improves device performance, resulting in efficiencies of 25.4% for small-area devices and 20.3% for 15 cm<sup>2</sup> mini-modules. Moreover, poly-EA acts as a protective barrier against moisture and ion migration. Combined with improved DMSO removal, EA-modulated devices demonstrate a T<sub>80</sub> lifetime of up to 1800 h under maximum power point tracking at 55–60% relative humidity in ambient air.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"22 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142940202","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}
Minmin Gao, Tianxi Zhang, Serene Wen Ling Ng, Wanheng Lu, Guo Tian, Wei Li Ong, Sergey M. Kozlov, Ghim Wei Ho
Conventional suspension photocatalysts face stability and efficiency challenges in harsh, unconditioned environments characterized by high alkalinity, salinity, and organic species in seawater and wastewater. Moreover, suspension-based photothermal-assisted catalysis presents further challenges, particularly concerning formation of heterojunctions between photocatalysts and photothermal materials that disrupt charge-transfer pathways and are exacerbated by photothermal heating-induced carrier recombination. Here, a photocatalytic system is proposed in which three key photoprocesses: photothermal, photogeneration-charge separation, and photoredox are spatially decoupled yet coordinated, aimed at addressing prevalent challenges of photothermal-assisted catalysis and adsorption-mediated catalyst deactivation in harsh environments. Essentially, the proposed polymeric tandem photothermal catalytic (PTPC) film consists of TiO2/Au photocatalytic and CuS photothermal layers, spatially separated and encapsulated by polymeric layers, which serve as spacer inhibitors to conflicting photochemical-photothermal pathways and corrosion-resistant redox medium. The PTPC film exhibits enhanced light absorption, mass transfer, and photothermal effect, surpassing traditional suspension catalysts and enabling interfacial redox reactions on the passive film surface. The PTPC system represents a new paradigm of polymeric film photocatalysis, enabling unimpeded photoredox-photothermal pathways and catalyst stability for application in hostile seawater and plastic waste environments. Such a paradigm can be used to develop localized, onsite solutions for photothermal H2 production that minimize logistical and environmental challenges.
{"title":"Polymeric Layered Films for TiO2-Au/CuS Tandem Photothermal Catalytic H2 Production in Harsh Seawater and Waste Plastic Media","authors":"Minmin Gao, Tianxi Zhang, Serene Wen Ling Ng, Wanheng Lu, Guo Tian, Wei Li Ong, Sergey M. Kozlov, Ghim Wei Ho","doi":"10.1002/aenm.202404198","DOIUrl":"https://doi.org/10.1002/aenm.202404198","url":null,"abstract":"Conventional suspension photocatalysts face stability and efficiency challenges in harsh, unconditioned environments characterized by high alkalinity, salinity, and organic species in seawater and wastewater. Moreover, suspension-based photothermal-assisted catalysis presents further challenges, particularly concerning formation of heterojunctions between photocatalysts and photothermal materials that disrupt charge-transfer pathways and are exacerbated by photothermal heating-induced carrier recombination. Here, a photocatalytic system is proposed in which three key photoprocesses: photothermal, photogeneration-charge separation, and photoredox are spatially decoupled yet coordinated, aimed at addressing prevalent challenges of photothermal-assisted catalysis and adsorption-mediated catalyst deactivation in harsh environments. Essentially, the proposed polymeric tandem photothermal catalytic (PTPC) film consists of TiO<sub>2</sub>/Au photocatalytic and CuS photothermal layers, spatially separated and encapsulated by polymeric layers, which serve as spacer inhibitors to conflicting photochemical-photothermal pathways and corrosion-resistant redox medium. The PTPC film exhibits enhanced light absorption, mass transfer, and photothermal effect, surpassing traditional suspension catalysts and enabling interfacial redox reactions on the passive film surface. The PTPC system represents a new paradigm of polymeric film photocatalysis, enabling unimpeded photoredox-photothermal pathways and catalyst stability for application in hostile seawater and plastic waste environments. Such a paradigm can be used to develop localized, onsite solutions for photothermal H<sub>2</sub> production that minimize logistical and environmental challenges.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"20 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142940281","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}
Adipic acid, an essential building stock for polymers, is conventionally synthesized through thermal oxidation of ketone−alcohol oil. However, this process requires excessive nitric acid as oxidants, causing the emission of ozone−depleting greenhouse gas nitrous oxide. Herein, a photoelectrochemical (PEC) strategy is reported for the efficient synthesize adipic acid by selective oxidation of cyclohexanone (CYC). High adipic acid selectivity (>90%) in a wide potential window (from 0.3 to 1.3 V versus RHE) is achieved under ambient conditions based on TiO2 nanorods array photoanode modified with nickel hydroxide nanosheets (Ni(OH)2/TiO2). Experimental and theoretical data reveal that a new Ni2+δ─OH* reactive center with moderate oxidation capacity is in situ generated on Ni(OH)2/TiO2 photoanode under illumination, which abstracts H atoms from Cα─H bonds in CYC to obtain 2−hydroxycyclohexanone intermediate, and thereby facilitates subsequent C─C cleavage to produce adipic acid. Moreover, the PEC synthesis of adipic acid from industrial raw material of phenol is achieved by coupling cathodic phenol reduction to CYC and photoanodic CYC oxidation to adipic acid, demonstrating a new and sustainable approach for adipic acid synthesis by directly using solar energy.
{"title":"Photoelectrochemical Synthesis of Adipic Acid by Selective Oxidation of Cyclohexanone","authors":"Shanshan Zhang, Lan Luo, Jiangrong Yang, Wangsong Chen, Yucong Miao, Ruikang Zhang, Zhenhua Li, Rengui Li, Mingfei Shao, Xue Duan","doi":"10.1002/aenm.202405052","DOIUrl":"https://doi.org/10.1002/aenm.202405052","url":null,"abstract":"Adipic acid, an essential building stock for polymers, is conventionally synthesized through thermal oxidation of ketone−alcohol oil. However, this process requires excessive nitric acid as oxidants, causing the emission of ozone−depleting greenhouse gas nitrous oxide. Herein, a photoelectrochemical (PEC) strategy is reported for the efficient synthesize adipic acid by selective oxidation of cyclohexanone (CYC). High adipic acid selectivity (>90%) in a wide potential window (from 0.3 to 1.3 V versus RHE) is achieved under ambient conditions based on TiO<sub>2</sub> nanorods array photoanode modified with nickel hydroxide nanosheets (Ni(OH)<sub>2</sub>/TiO<sub>2</sub>). Experimental and theoretical data reveal that a new Ni<sup>2+</sup><i><sup>δ</sup></i>─OH<sup>*</sup> reactive center with moderate oxidation capacity is in situ generated on Ni(OH)<sub>2</sub>/TiO<sub>2</sub> photoanode under illumination, which abstracts H atoms from C<sub>α</sub>─H bonds in CYC to obtain 2−hydroxycyclohexanone intermediate, and thereby facilitates subsequent C─C cleavage to produce adipic acid. Moreover, the PEC synthesis of adipic acid from industrial raw material of phenol is achieved by coupling cathodic phenol reduction to CYC and photoanodic CYC oxidation to adipic acid, demonstrating a new and sustainable approach for adipic acid synthesis by directly using solar energy.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"20 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142940203","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}
Junjun Guo, Martin V. Appleby, Kui Ding, Tong Shan, James Shipp, Igor V. Sazanovich, Dimitri Chekulaev, Zhuoran Qiao, Ricardo J. Fernández-Terán, Rachel Crespo Otero, Nicola Gasparini, Hongliang Zhong, Julia A. Weinstein, Tracey M. Clarke
Non-fullerene acceptors have revolutionised organic photovoltaics. However, greater fundamental understanding is needed of the crucial relationships between molecular structure and photophysical mechanisms. Herein, a combination of spectroscopic, morphology, and device characterization techniques are used to explore these relationships for a high-performing non-fullerene acceptor, anti-PDFC. It focuses on transient absorption spectroscopy across multiple timescales and ultrafast time-resolved vibrational spectroscopy to acquire the “holy grail” of simultaneous structural and dynamic information for anti-PDFC and its blend with the well-known conjugated polymer PM6. Most significantly, it is observed that the singlet exciton of anti-PDFC is localised on the perylene diimide central core of the molecule, but the radical anion is primarily localised on the fluorinated indene malonitrile terminal units (which are common to many state-of-the-art non-fullerene acceptors, including the Y6 family). This electron transfer from the central core to the termini of an adjacent molecule is facilitated by a close interaction between the termini and the central core, as evidenced by single crystal diffraction data and excited state calculations. Finally, the very efficient charge extraction measured for PM6:anti-PDFC photovoltaic devices may be correlated with this anion localization, enabling effective charge transport channels and thus enhancing device performance.
{"title":"Anion Localization on Termini of a Non-Fullerene Acceptor Aids Charge Transport","authors":"Junjun Guo, Martin V. Appleby, Kui Ding, Tong Shan, James Shipp, Igor V. Sazanovich, Dimitri Chekulaev, Zhuoran Qiao, Ricardo J. Fernández-Terán, Rachel Crespo Otero, Nicola Gasparini, Hongliang Zhong, Julia A. Weinstein, Tracey M. Clarke","doi":"10.1002/aenm.202404926","DOIUrl":"https://doi.org/10.1002/aenm.202404926","url":null,"abstract":"Non-fullerene acceptors have revolutionised organic photovoltaics. However, greater fundamental understanding is needed of the crucial relationships between molecular structure and photophysical mechanisms. Herein, a combination of spectroscopic, morphology, and device characterization techniques are used to explore these relationships for a high-performing non-fullerene acceptor, anti-PDFC. It focuses on transient absorption spectroscopy across multiple timescales and ultrafast time-resolved vibrational spectroscopy to acquire the “holy grail” of simultaneous structural and dynamic information for anti-PDFC and its blend with the well-known conjugated polymer PM6. Most significantly, it is observed that the singlet exciton of anti-PDFC is localised on the perylene diimide central core of the molecule, but the radical anion is primarily localised on the fluorinated indene malonitrile terminal units (which are common to many state-of-the-art non-fullerene acceptors, including the Y6 family). This electron transfer from the central core to the termini of an adjacent molecule is facilitated by a close interaction between the termini and the central core, as evidenced by single crystal diffraction data and excited state calculations. Finally, the very efficient charge extraction measured for PM6:anti-PDFC photovoltaic devices may be correlated with this anion localization, enabling effective charge transport channels and thus enhancing device performance.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"45 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142940201","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Aqueous zinc‐ion batteries have garnered significant attention due to their abundant materials, low production costs, and safety. However, these batteries suffer from severe side reactions, which are closely associated with the presence of a substantial amount of solvent at the electrode surfaces. Herein, 1,4,7,10,13,16‐hexaoxacyclooctadecane (18‐crown‐6) is added to the electrolyte to illustrate both theoretically and experimentally its contribution to the rapid desolvation aspect. It is shown that the addition of 18‐crown‐6 to the electrolyte greatly facilitates the desolvation of the solvated structure and prevents the collection of solvent molecules on the surface of zinc anode, thus inhibiting the hydrogen precipitation reaction. It also enhances the transference number of zinc ions, which makes the interfacial electric field on the zinc anode stable and thus promotes the orderly diffusion and uniform nucleation of Zn2+, and inhibits the growth of dendrites. As a result, the electrolyte containing 18‐crown‐6 as additives shows a stable cycle life, Zn||Zn symmetric cell is cycled for nearly 1700 h at 1 mA cm−2, showing a significant improvement in Coulombic efficiency. The assembled Zn||NH4V4O10 cell exhibits excellent electrochemical performance, reaching a capacity of 100.9 mAh g−1 even after 4000 cycles at 10.0 A g−1.
{"title":"Multifunctional Crown Ether Additive Regulates Desolvation Process to Achieve Highly Reversible Zinc‐Metal Batteries","authors":"Aohua Wu, Shaojie Zhang, Qiaohui Li, Wenxian Xue, Chuanyang Li, Baojuan Xi, Wutao Mao, Keyan Bao, Shenglin Xiong","doi":"10.1002/aenm.202404450","DOIUrl":"https://doi.org/10.1002/aenm.202404450","url":null,"abstract":"Aqueous zinc‐ion batteries have garnered significant attention due to their abundant materials, low production costs, and safety. However, these batteries suffer from severe side reactions, which are closely associated with the presence of a substantial amount of solvent at the electrode surfaces. Herein, 1,4,7,10,13,16‐hexaoxacyclooctadecane (18‐crown‐6) is added to the electrolyte to illustrate both theoretically and experimentally its contribution to the rapid desolvation aspect. It is shown that the addition of 18‐crown‐6 to the electrolyte greatly facilitates the desolvation of the solvated structure and prevents the collection of solvent molecules on the surface of zinc anode, thus inhibiting the hydrogen precipitation reaction. It also enhances the transference number of zinc ions, which makes the interfacial electric field on the zinc anode stable and thus promotes the orderly diffusion and uniform nucleation of Zn<jats:sup>2+</jats:sup>, and inhibits the growth of dendrites. As a result, the electrolyte containing 18‐crown‐6 as additives shows a stable cycle life, Zn||Zn symmetric cell is cycled for nearly 1700 h at 1 mA cm<jats:sup>−2</jats:sup>, showing a significant improvement in Coulombic efficiency. The assembled Zn||NH<jats:sub>4</jats:sub>V<jats:sub>4</jats:sub>O<jats:sub>10</jats:sub> cell exhibits excellent electrochemical performance, reaching a capacity of 100.9 mAh g<jats:sup>−1</jats:sup> even after 4000 cycles at 10.0 A g<jats:sup>−1</jats:sup>.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"35 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937213","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The escalating crisis of oceanic plastic pollution demands innovative and effective strategies for resolution. Photocatalysis offers a sustainable, green, and energy‐efficient approach for the upcycling of plastic waste into fuels and value‐added chemicals. In this study, an atomically engineered GeS NS/ZnIn₂S₄ photocatalyst is employed to directly transform raw polyethylene terephthalate (PET), a ubiquitous plastic, into a variety of organic chemicals (13 917 µmol g⁻¹) using Earth's most abundant resources: sunlight, seawater, and air. Advanced ex situ and in situ characterization analyses reveal that sulfur vacancies (Vs) and electrolyte‐assisted polarization effect of seawater play crucial roles in trapping photogenerated electrons and accelerating charge carrier separation, respectively. These effects significantly enhance photocatalytic plastic upcycling efficiency and improve oxidative organic reactions. This research introduces a methodology that accounts for real‐world conditions in photocatalytic plastic upcycling, utilizing abundant natural resources and paving the way for further exploration in this area.
{"title":"Photocatalytic Reforming Raw Plastic in Seawater by Atomically‐Engineered GeS/ZnIn2S4","authors":"Amin Talebian‐Kiakalaieh, Haobo Li, Meijun Guo, Elhussein M. Hashem, Bingquan Xia, Jingrun Ran, Shi‐Zhang Qiao","doi":"10.1002/aenm.202404963","DOIUrl":"https://doi.org/10.1002/aenm.202404963","url":null,"abstract":"The escalating crisis of oceanic plastic pollution demands innovative and effective strategies for resolution. Photocatalysis offers a sustainable, green, and energy‐efficient approach for the upcycling of plastic waste into fuels and value‐added chemicals. In this study, an atomically engineered GeS NS/ZnIn₂S₄ photocatalyst is employed to directly transform raw polyethylene terephthalate (PET), a ubiquitous plastic, into a variety of organic chemicals (13 917 µmol g⁻¹) using Earth's most abundant resources: sunlight, seawater, and air. Advanced ex situ and in situ characterization analyses reveal that sulfur vacancies (Vs) and electrolyte‐assisted polarization effect of seawater play crucial roles in trapping photogenerated electrons and accelerating charge carrier separation, respectively. These effects significantly enhance photocatalytic plastic upcycling efficiency and improve oxidative organic reactions. This research introduces a methodology that accounts for real‐world conditions in photocatalytic plastic upcycling, utilizing abundant natural resources and paving the way for further exploration in this area.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"1 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937215","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}
Jules Bertrandie, Mehmet Alican Noyan, Luis Huerta Hernandez, Anirudh Sharma, Derya Baran
The precise determination of ionization energy (IE) and electron affinity (EA) is crucial for the development and optimization of organic semiconductors (OSCs). These parameters directly impact the performance of organic electronic devices. Experimental techniques to measure IE and EA, such as UV photoelectron spectroscopy (UPS) and low-energy inverse photoelectron spectroscopy (LE-IPES), are accurate but resource-intensive and limited by their availability. Computational approaches, while beneficial, often rely on gas-phase calculations that fail to capture solid-state phenomena, leading to discrepancies in practical applications. In this work, machine learning methods are used to develop a chained model for estimating solid-state IE and EA values. By implementing a transfer learning strategy, the challenge of limited experimental data is effectively addressed, utilizing a large database of intermediate properties to enhance model training. The efficacy of this model is demonstrated through its performance achieving mean absolute errors of 0.13 and 0.14 eV for IE and EA, respectively. The model has also been tested on an external validation dataset comprising newly measured molecules. These findings highlight the potential of machine learning in OSC research, significantly enhancing property accessibility and accelerating molecular design and discovery.
{"title":"From Experimental Values to Predictive Models: Machine Learning-Driven Energy Level Determination in Organic Semiconductors","authors":"Jules Bertrandie, Mehmet Alican Noyan, Luis Huerta Hernandez, Anirudh Sharma, Derya Baran","doi":"10.1002/aenm.202403707","DOIUrl":"https://doi.org/10.1002/aenm.202403707","url":null,"abstract":"The precise determination of ionization energy (IE) and electron affinity (EA) is crucial for the development and optimization of organic semiconductors (OSCs). These parameters directly impact the performance of organic electronic devices. Experimental techniques to measure IE and EA, such as UV photoelectron spectroscopy (UPS) and low-energy inverse photoelectron spectroscopy (LE-IPES), are accurate but resource-intensive and limited by their availability. Computational approaches, while beneficial, often rely on gas-phase calculations that fail to capture solid-state phenomena, leading to discrepancies in practical applications. In this work, machine learning methods are used to develop a chained model for estimating solid-state IE and EA values. By implementing a transfer learning strategy, the challenge of limited experimental data is effectively addressed, utilizing a large database of intermediate properties to enhance model training. The efficacy of this model is demonstrated through its performance achieving mean absolute errors of 0.13 and 0.14 eV for IE and EA, respectively. The model has also been tested on an external validation dataset comprising newly measured molecules. These findings highlight the potential of machine learning in OSC research, significantly enhancing property accessibility and accelerating molecular design and discovery.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"31 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937715","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}
An Duan, Sha Luo, Yuyang Tang, Yu Feng, Ming Li, Bao Zhang, Wei Sun
Electrolyte regulation and electrode/electrolyte interface optimization are recognized as crucial strategies for mitigating parasitic reactions and enhancing zinc plating/stripping in zinc metal batteries. Despite their established importance, the underlying mechanisms of interface behavior and optimization remain elusive, especially in the absence of robust experimental characterization of adsorption-dominated approaches. Herein, in situ monitoring of interfacial adsorption effect is presented, employing a theoretically screened cyclen-based additive. The dynamic adsorption behavior in response to alternating electric fields is identified as pivotal in regulating the metal-electrolyte interfaces, as evidenced by a combination of in situ electrochemical quartz crystal microbalance (eQCM) measurements and constant-potential molecular dynamics simulation. Such dynamic adsorption provides a robust pH buffering effect at the zinc-metal anode interface, facilitating orderly and uniform zinc plating/stripping. Consequently, the electrochemical performance of zinc-based half cells and full cells is markedly enhanced. The findings offer comprehensive insights into the strategic development of functional electrolyte additives for aqueous zinc metal batteries.
{"title":"In Situ Monitoring of Dynamic Adsorption-Induced Interfacial Buffering Toward Highly Stable Zinc Metal Batteries","authors":"An Duan, Sha Luo, Yuyang Tang, Yu Feng, Ming Li, Bao Zhang, Wei Sun","doi":"10.1002/aenm.202404693","DOIUrl":"https://doi.org/10.1002/aenm.202404693","url":null,"abstract":"Electrolyte regulation and electrode/electrolyte interface optimization are recognized as crucial strategies for mitigating parasitic reactions and enhancing zinc plating/stripping in zinc metal batteries. Despite their established importance, the underlying mechanisms of interface behavior and optimization remain elusive, especially in the absence of robust experimental characterization of adsorption-dominated approaches. Herein, in situ monitoring of interfacial adsorption effect is presented, employing a theoretically screened cyclen-based additive. The dynamic adsorption behavior in response to alternating electric fields is identified as pivotal in regulating the metal-electrolyte interfaces, as evidenced by a combination of in situ electrochemical quartz crystal microbalance (eQCM) measurements and constant-potential molecular dynamics simulation. Such dynamic adsorption provides a robust pH buffering effect at the zinc-metal anode interface, facilitating orderly and uniform zinc plating/stripping. Consequently, the electrochemical performance of zinc-based half cells and full cells is markedly enhanced. The findings offer comprehensive insights into the strategic development of functional electrolyte additives for aqueous zinc metal batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"142 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142935660","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}
Gabriel S. Nambafu, Aaron M. Hollas, Peter S. Rice, Jon Mark Weller, Daria Boglaienko, David M. Reed, Vincent L. Sprenkle, Guosheng Li
Redox Flow Batteries
{"title":"Strategically Modified Ligand Incorporating Mixed Phosphonate and Carboxylate Groups to Enhance Performance in All-Iron Redox Flow Batteries (Adv. Energy Mater. 1/2025)","authors":"Gabriel S. Nambafu, Aaron M. Hollas, Peter S. Rice, Jon Mark Weller, Daria Boglaienko, David M. Reed, Vincent L. Sprenkle, Guosheng Li","doi":"10.1002/aenm.202570002","DOIUrl":"https://doi.org/10.1002/aenm.202570002","url":null,"abstract":"<b>Redox Flow Batteries</b>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"30 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142935372","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}
Chunmei Tang, Baoyin Yuan, Xiaohan Zhang, Fangyuan Zheng, Qingwen Su, Ling Meng, Lei Du, Dongxiang Luo, Yoshitaka Aoki, Ning Wang, Siyu Ye
Protonic ceramic cells (PCCs) have gained significant attention as a promising electrochemical device for hydrogen production and power generation at intermediate temperatures. However, the lack of high-performance air electrodes, specifically in terms of proton conduction ability, has severely hindered the improvement of electrochemical performances for PCCs. In this study, a high-efficiency air electrode La0.8Ba0.2CoO3 (LBC) is rationally designed and researched by a machine-learning model and density functional theory (DFT) calculation, which boosts the performances of PCCs. Specifically, an elements-property map for designing high-efficiency oxides is created by predicting and studying the proton uptake ability of La1–xA′xBO3 (A′ = Na, K, Ca, Mg, Ba, Cu, etc.) by an eXtreme Gradient Boosting model. PCC with LBC air electrode yields high current destiny in electrolysis mode (1.72 A cm−2 at 600 °C) and power density in fuel cell mode (1.00 W cm−2 at 600 °C). In addition, an ultra-low air electrode reaction resistance (0.03 Ω cm2 at 600 °C) is achieved, because LBC can significantly facilitate the formation of O2*. This work not only reports an effective air electrode but also presents a new avenue for the rational design of air electrodes for PCCs.
{"title":"Rationally Designed Air Electrode Boosting Electrochemical Performance of Protonic Ceramic Cells","authors":"Chunmei Tang, Baoyin Yuan, Xiaohan Zhang, Fangyuan Zheng, Qingwen Su, Ling Meng, Lei Du, Dongxiang Luo, Yoshitaka Aoki, Ning Wang, Siyu Ye","doi":"10.1002/aenm.202402654","DOIUrl":"https://doi.org/10.1002/aenm.202402654","url":null,"abstract":"Protonic ceramic cells (PCCs) have gained significant attention as a promising electrochemical device for hydrogen production and power generation at intermediate temperatures. However, the lack of high-performance air electrodes, specifically in terms of proton conduction ability, has severely hindered the improvement of electrochemical performances for PCCs. In this study, a high-efficiency air electrode La<sub>0.8</sub>Ba<sub>0.2</sub>CoO<sub>3</sub> (LBC) is rationally designed and researched by a machine-learning model and density functional theory (DFT) calculation, which boosts the performances of PCCs. Specifically, an elements-property map for designing high-efficiency oxides is created by predicting and studying the proton uptake ability of La<sub>1–</sub><i><sub>x</sub></i>A′<i><sub>x</sub></i>BO<sub>3</sub> (A′ = Na, K, Ca, Mg, Ba, Cu, etc.) by an eXtreme Gradient Boosting model. PCC with LBC air electrode yields high current destiny in electrolysis mode (1.72 A cm<sup>−2</sup> at 600 °C) and power density in fuel cell mode (1.00 W cm<sup>−2</sup> at 600 °C). In addition, an ultra-low air electrode reaction resistance (0.03 Ω cm<sup>2</sup> at 600 °C) is achieved, because LBC can significantly facilitate the formation of O<sub>2</sub><sup>*</sup>. This work not only reports an effective air electrode but also presents a new avenue for the rational design of air electrodes for PCCs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"28 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142935371","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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