Xinyue Cui, Yitong Ji, Yuqiang Liu, Xueqing Ma, Hongxiang Li, Pei Cheng, Wenchao Huang, Zhishan Bo
Controlling the packing feature and film morphology of active layers is the precondition for achieving highly efficient organic solar cells (OSCs). The growth transition of donors and acceptors from solution to solid films plays an intrinsic role in shaping these features. In this study, two simple additives, cyanobenzene (CNB) and 1,4-dicyanobenzene (DCNB), are presented to modulate the growth process of active layers to investigate the impact of growth behaviors on molecule packing quality, film morphology, and device performances. Both additives prolong the nucleation and growth period of active layers, resulting in improved molecular packing quality, domain purity, and crystallization. This optimization enhances charge extraction efficiency as well as reduces charge recombination losses. Consequently, devices based on D18:BTP-eC9-4F processed with additives obtain a 19.43% power conversion efficiency (PCE). Furthermore, a PCE of 14.35% is achieved for bladed-coated organic solar modules on 5 cm × 5 cm substrates. These findings underscore the importance of growth processes on film quality and illustrate their fundamental relationship, which promises further advancements in OSC technology.
{"title":"Optimizing Molecular Packing and Film Morphology in Organic Solar Cells via Additive-Modulated Growth Processes","authors":"Xinyue Cui, Yitong Ji, Yuqiang Liu, Xueqing Ma, Hongxiang Li, Pei Cheng, Wenchao Huang, Zhishan Bo","doi":"10.1002/aenm.202403077","DOIUrl":"https://doi.org/10.1002/aenm.202403077","url":null,"abstract":"Controlling the packing feature and film morphology of active layers is the precondition for achieving highly efficient organic solar cells (OSCs). The growth transition of donors and acceptors from solution to solid films plays an intrinsic role in shaping these features. In this study, two simple additives, cyanobenzene (CNB) and 1,4-dicyanobenzene (DCNB), are presented to modulate the growth process of active layers to investigate the impact of growth behaviors on molecule packing quality, film morphology, and device performances. Both additives prolong the nucleation and growth period of active layers, resulting in improved molecular packing quality, domain purity, and crystallization. This optimization enhances charge extraction efficiency as well as reduces charge recombination losses. Consequently, devices based on D18:BTP-eC9-4F processed with additives obtain a 19.43% power conversion efficiency (PCE). Furthermore, a PCE of 14.35% is achieved for bladed-coated organic solar modules on 5 cm × 5 cm substrates. These findings underscore the importance of growth processes on film quality and illustrate their fundamental relationship, which promises further advancements in OSC technology.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142330279","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}
Shuren Zhang, Yitong Han, Rui Zhang, Zhiyuan Zhang, Genban Sun
Modulating the spin states of FeN4 moieties is critical for enhancing the electrocatalytic oxygen reduction reaction (ORR). In this study, Ti4N3Clx and Ti4N3Ox MXenes are synthesized and functionalized with iron phthalocyanine (FePc) to form model catalysts with well-defined FeN4-Cl-Ti and FeN4-O-Ti structures, respectively. The FeN4-Cl-Ti structure, formed within the Ti4N3Clx/FePc composite, enables precise modulation of FeN4 spin states from low to intermediate spin, significantly enhancing ORR performance. In contrast, the FeN4-O-Ti structure in Ti4N3Ox/FePc shows less effective spin state modulation, leading to comparatively lower ORR activity. Compared to FePc and Ti4N3Ox/FePc, Ti4N3Clx/FePc demonstrates superior electrochemical performance, with an ORR half-wave potential of +0.91 V versus RHE and doubled power densities in Zn–air batteries (214.5 mW cm−2). Theoretical studies confirm that the intermediate spin states induced by the weak-field ligand-modified FeN4-Cl-Ti structure in Ti4N3Clx/FePc facilitate electron filling in the antibonding orbital composed of Fe 3dz2 and O2 π* orbitals, greatly enhancing O₂ activation and ORR activity. These findings underscore the superior catalytic properties of FeN4-Cl-Ti compared to FeN4-O-Ti, advancing the understanding of spin state-related catalytic mechanisms and guiding the design of high-performance ORR catalysts.
{"title":"Regulating Fe Intermediate Spin States via FeN4-Cl-Ti Structure for Enhanced Oxygen Reduction","authors":"Shuren Zhang, Yitong Han, Rui Zhang, Zhiyuan Zhang, Genban Sun","doi":"10.1002/aenm.202403899","DOIUrl":"https://doi.org/10.1002/aenm.202403899","url":null,"abstract":"Modulating the spin states of FeN<sub>4</sub> moieties is critical for enhancing the electrocatalytic oxygen reduction reaction (ORR). In this study, Ti<sub>4</sub>N<sub>3</sub>Cl<i><sub>x</sub></i> and Ti<sub>4</sub>N<sub>3</sub>O<i><sub>x</sub></i> MXenes are synthesized and functionalized with iron phthalocyanine (FePc) to form model catalysts with well-defined FeN<sub>4</sub>-Cl-Ti and FeN<sub>4</sub>-O-Ti structures, respectively. The FeN<sub>4</sub>-Cl-Ti structure, formed within the Ti<sub>4</sub>N<sub>3</sub>Cl<i><sub>x</sub></i>/FePc composite, enables precise modulation of FeN<sub>4</sub> spin states from low to intermediate spin, significantly enhancing ORR performance. In contrast, the FeN<sub>4</sub>-O-Ti structure in Ti<sub>4</sub>N<sub>3</sub>O<i><sub>x</sub></i>/FePc shows less effective spin state modulation, leading to comparatively lower ORR activity. Compared to FePc and Ti<sub>4</sub>N<sub>3</sub>O<i><sub>x</sub></i>/FePc, Ti<sub>4</sub>N<sub>3</sub>Cl<i><sub>x</sub></i>/FePc demonstrates superior electrochemical performance, with an ORR half-wave potential of +0.91 V versus RHE and doubled power densities in Zn–air batteries (214.5 mW cm<sup>−2</sup>). Theoretical studies confirm that the intermediate spin states induced by the weak-field ligand-modified FeN<sub>4</sub>-Cl-Ti structure in Ti<sub>4</sub>N<sub>3</sub>Cl<i><sub>x</sub></i>/FePc facilitate electron filling in the antibonding orbital composed of Fe 3dz<sup>2</sup> and O<sub>2</sub> π* orbitals, greatly enhancing O₂ activation and ORR activity. These findings underscore the superior catalytic properties of FeN<sub>4</sub>-Cl-Ti compared to FeN<sub>4</sub>-O-Ti, advancing the understanding of spin state-related catalytic mechanisms and guiding the design of high-performance ORR catalysts.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329846","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}
Fanghua Liu, Kenji Miyatake, Ahmed Mohamed Ahmed Mahmoud, Vikrant Yadav, Fang Xian, Lin Guo, Chun Yik Wong, Toshio Iwataki, Yuto Shirase, Katsuyoshi Kakinuma, Makoto Uchida
Alkaline-stable, highly conductive anion exchange membranes (AEMs) are attentively expected solid polymer electrolytes that contribute to achieving high performance and durability for anion exchange membrane water electrolyzers (AEMWEs). The technical challenges of AEMs mainly stem from the degradation of the polymer backbones, side chains, and anchoring cationic groups. Herein, new and stable AEMs (QTAF) are designed using 3,3′′-dichloro-2′,5′-bis(trifluoromethyl)-1,1′:4′,1′′-terphenyl (TFP) monomers as the hydrophobic component incorporated into the polyphenylene backbone and 3,3′-(2,7-dichloro-9H-fluorene-9,9-diyl)bis(N,N-dimethylpropane-1-amine) (AF) monomers as the hydrophilic component. After tuning the copolymer composition, the highest hydroxide ion conductivity (168.7 mS cm−1 at 80 °C) is achieved with the QTAF-3.0 membrane. The QTAF-3.0 membrane survives in harsh alkaline conditions (8 M KOH solution, 80 °C), with high conductivity (75.8 mS cm−1) after 810 h. A water electrolysis cell with QTAF-3.0 membrane and non-noble Ni0.8Co0.2O anode catalyst operates stably at a constant current density (1.0 A cm−2) for 1000 h with a negligible voltage increase rate of 1.1 µV h−1 after the initial voltage increase. The water electrolysis performance of the post-tested QTAF-3.0 cell is 1.83 V, only a 6.4% increase from the initial performance at 2.0 A cm−2, suggesting the high potential of the QTAF-3.0 membrane for practical AEMWE applications.
碱性稳定的高导电性阴离子交换膜（AEM）是一种备受期待的固态聚合物电解质，有助于实现阴离子交换膜水电解槽（AEMWE）的高性能和耐用性。AEMs 面临的技术挑战主要来自聚合物骨架、侧链和锚定阳离子基团的降解。本文利用 3,3′′-二氯-2′,5′-双（三氟甲基）-1,1′：4′,1′′-三联苯（TFP）单体是聚苯乙烯骨架中的疏水组分，3,3′-(2,7-二氯-9H-芴-9,9-二基)双(N,N-二甲基丙烷-1-胺)（AF）单体是亲水组分。调整共聚物成分后，QTAF-3.0 膜的氢氧根离子导电率最高（80 °C 时为 168.7 mS cm-1）。使用 QTAF-3.0 膜和非贵金属 Ni0.8Co0.2O 阳极催化剂的水电解槽在恒定电流密度（1.0 A cm-2）下可稳定运行 1000 小时，初始电压升高后的电压升高率为 1.1 µV h-1，可忽略不计。经过测试的 QTAF-3.0 电池的电解水性能为 1.83 V，与 2.0 A cm-2 时的初始性能相比仅提高了 6.4%，这表明 QTAF-3.0 膜在实际 AEMWE 应用中具有很大的潜力。
{"title":"Polyphenylene-Based Anion Exchange Membranes with Robust Hydrophobic Components Designed for High-Performance and Durable Anion Exchange Membrane Water Electrolyzers Using Non-PGM Anode Catalysts","authors":"Fanghua Liu, Kenji Miyatake, Ahmed Mohamed Ahmed Mahmoud, Vikrant Yadav, Fang Xian, Lin Guo, Chun Yik Wong, Toshio Iwataki, Yuto Shirase, Katsuyoshi Kakinuma, Makoto Uchida","doi":"10.1002/aenm.202404089","DOIUrl":"https://doi.org/10.1002/aenm.202404089","url":null,"abstract":"Alkaline-stable, highly conductive anion exchange membranes (AEMs) are attentively expected solid polymer electrolytes that contribute to achieving high performance and durability for anion exchange membrane water electrolyzers (AEMWEs). The technical challenges of AEMs mainly stem from the degradation of the polymer backbones, side chains, and anchoring cationic groups. Herein, new and stable AEMs (QTAF) are designed using 3,3′′-dichloro-2′,5′-bis(trifluoromethyl)-1,1′:4′,1′′-terphenyl (TFP) monomers as the hydrophobic component incorporated into the polyphenylene backbone and 3,3′-(2,7-dichloro-9H-fluorene-9,9-diyl)bis(N,N-dimethylpropane-1-amine) (AF) monomers as the hydrophilic component. After tuning the copolymer composition, the highest hydroxide ion conductivity (168.7 mS cm<sup>−1</sup> at 80 °C) is achieved with the QTAF-3.0 membrane. The QTAF-3.0 membrane survives in harsh alkaline conditions (8 M KOH solution, 80 °C), with high conductivity (75.8 mS cm<sup>−1</sup>) after 810 h. A water electrolysis cell with QTAF-3.0 membrane and non-noble Ni<sub>0.8</sub>Co<sub>0.2</sub>O anode catalyst operates stably at a constant current density (1.0 A cm<sup>−2</sup>) for 1000 h with a negligible voltage increase rate of 1.1 µV h<sup>−1</sup> after the initial voltage increase. The water electrolysis performance of the post-tested QTAF-3.0 cell is 1.83 V, only a 6.4% increase from the initial performance at 2.0 A cm<sup>−2</sup>, suggesting the high potential of the QTAF-3.0 membrane for practical AEMWE applications.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329847","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}
Christoph Scherer, Naomi Kinaret, Kun-Han Lin, Muhammad Nawaz Qaisrani, Felix Post, Falk May, Denis Andrienko
Thin films of molecular materials are commonly employed in organic light-emitting diodes, field-effect transistors, and solar cells. The morphology of these organic films is shown to depend heavily on the processing used during manufacturing, such as vapor co-deposition. However, the prediction of processing-dependent morphologies has until now posed a significant challenge, particularly in cases where self-assembly and ordering are involved. In this work, a method is developed based on coarse-graining that is capable of predicting molecular ordering in vapor-deposited films of organic materials. The method is tested on an extensive database of novel and known organic semiconductors. A good agreement between the anisotropy of the refractive indices of the simulated and experimental vapor-deposited films suggests that the method is quantitative and can predict the molecular orientations in organic films at an atomistic resolution. The methodology can be readily utilized for screening materials for organic light-emitting diodes.
{"title":"Predicting Molecular Ordering in Deposited Molecular Films","authors":"Christoph Scherer, Naomi Kinaret, Kun-Han Lin, Muhammad Nawaz Qaisrani, Felix Post, Falk May, Denis Andrienko","doi":"10.1002/aenm.202403124","DOIUrl":"https://doi.org/10.1002/aenm.202403124","url":null,"abstract":"Thin films of molecular materials are commonly employed in organic light-emitting diodes, field-effect transistors, and solar cells. The morphology of these organic films is shown to depend heavily on the processing used during manufacturing, such as vapor co-deposition. However, the prediction of processing-dependent morphologies has until now posed a significant challenge, particularly in cases where self-assembly and ordering are involved. In this work, a method is developed based on coarse-graining that is capable of predicting molecular ordering in vapor-deposited films of organic materials. The method is tested on an extensive database of novel and known organic semiconductors. A good agreement between the anisotropy of the refractive indices of the simulated and experimental vapor-deposited films suggests that the method is quantitative and can predict the molecular orientations in organic films at an atomistic resolution. The methodology can be readily utilized for screening materials for organic light-emitting diodes.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142330283","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}
Gawon Song, Suyeon Lee, Taehun Kim, Min Soo Jung, Kanghyeon Kim, Seung Hyun Choi, Seunghyun Lee, Junsung Park, Minseon Lee, Chanhwi Park, Mi-Sook Kwon, Kyu Tae Lee
Li- and Mn-rich layered oxides (LMROs) are recognized as promising cathode materials for lithium-ion batteries (LIBs) due to their high specific capacity and cost efficiency. However, LMROs encounter challenges such as manganese dissolution in electrolytes and the release of oxygen gas from irreversible oxygen redox reactions, leading to structural degradation and voltage decay that reduce energy density. Consequently, recent research has shifted toward employing LMROs in all-solid-state batteries (ASSBs), where Mn dissolution is negligible. Herein, nanostructured LMROs demonstrate superior electrochemical compatibility with sulfide-based solid electrolytes in ASSBs compared to conventional LIBs. Nanostructured LMRO exhibits outstanding capacity retention (97.1% after 1300 cycles at 30 °C) with significantly suppressed voltage decay. Furthermore, the initial electrochemical activation of Li2MnO3 domains within LMRO is explored in terms of the mechano-electrochemical interactions in the composite cathode. At elevated temperatures, interfacial degradation accelerates due to the chemical oxidation of Li6PS5Cl solid electrolytes, driven by oxygen released from LMRO. To address this, LMRO surfaces are modified with thioglycolic acid through esterification, suppressing interfacial degradation of Li6PS5Cl and ensuring stable capacity retention over 500 cycles at 60 °C. These findings underscore the potential of LMRO materials as promising cathode options for ASSBs, surpassing those used in LIBs.
{"title":"Mechano-Electrochemical Behavior of Nanostructured Li- and Mn-Rich Layered Oxides with Superior Capacity Retention and Voltage Decay for Sulfide-Based All-Solid-State Batteries","authors":"Gawon Song, Suyeon Lee, Taehun Kim, Min Soo Jung, Kanghyeon Kim, Seung Hyun Choi, Seunghyun Lee, Junsung Park, Minseon Lee, Chanhwi Park, Mi-Sook Kwon, Kyu Tae Lee","doi":"10.1002/aenm.202403374","DOIUrl":"https://doi.org/10.1002/aenm.202403374","url":null,"abstract":"Li- and Mn-rich layered oxides (LMROs) are recognized as promising cathode materials for lithium-ion batteries (LIBs) due to their high specific capacity and cost efficiency. However, LMROs encounter challenges such as manganese dissolution in electrolytes and the release of oxygen gas from irreversible oxygen redox reactions, leading to structural degradation and voltage decay that reduce energy density. Consequently, recent research has shifted toward employing LMROs in all-solid-state batteries (ASSBs), where Mn dissolution is negligible. Herein, nanostructured LMROs demonstrate superior electrochemical compatibility with sulfide-based solid electrolytes in ASSBs compared to conventional LIBs. Nanostructured LMRO exhibits outstanding capacity retention (97.1% after 1300 cycles at 30 °C) with significantly suppressed voltage decay. Furthermore, the initial electrochemical activation of Li<sub>2</sub>MnO<sub>3</sub> domains within LMRO is explored in terms of the mechano-electrochemical interactions in the composite cathode. At elevated temperatures, interfacial degradation accelerates due to the chemical oxidation of Li<sub>6</sub>PS<sub>5</sub>Cl solid electrolytes, driven by oxygen released from LMRO. To address this, LMRO surfaces are modified with thioglycolic acid through esterification, suppressing interfacial degradation of Li<sub>6</sub>PS<sub>5</sub>Cl and ensuring stable capacity retention over 500 cycles at 60 °C. These findings underscore the potential of LMRO materials as promising cathode options for ASSBs, surpassing those used in LIBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329845","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}
Yanfang Liu, Hongwei Fu, Caitian Gao, Jie Wen, Ruoya Guo, Wendi Luo, Jiawan Zhou, Bingan Lu
The operation of graphite-based potassium ion batteries (Gr-PIBs) remains challenging at low temperatures, limited by slow dynamic behavior. Herein, the solvation structure dual-regulator strategy of electrolyte is proposed for multidimensional improvement of K+ transfer process including ion transfer at both bulk and interface. The designed electrolyte (an amide solvent, 2,2,2-Trifluoro-N, N-dimethylacetamide) with low freezing point and low viscosity as the primary regulator, and a fluorinated solvent (1,1,2,2-Tetrafluoroethyl-2,2,3,3-tetrafluoropropylether) as the secondary regulator provides a flowing environment and low resistive interface for fast ion transfer. As a result, the regulated electrolyte has a low freezing point of −51.9 °C and exhibits a high ionic conductivity of 3.2 mS cm−1 at −20 °C. Based on the solvation structure dual-regulator, the graphite anode delivered a high capacity of 252 mAh g−1 which is over 85% of room-temperature capacity, and the capacity retention rate of a full cell at −20 °C is over 80%. These results demonstrate that the solvation structure dual-regulator can improve the performances of Gr-PIBs, promoting the development of low-temperature PIBs and beyond.
石墨基钾离子电池（Gr-PIBs）在低温条件下的运行仍然具有挑战性，因为它受到缓慢的动态行为的限制。本文提出了电解质的溶解结构双调节策略，以多维度改善 K+ 的转移过程，包括体外和界面的离子转移。所设计的电解质（酰胺溶剂，2,2,2-三氟-N,N-二甲基乙酰胺）具有低凝固点和低粘度，可作为主要调节剂，而含氟溶剂（1,1,2,2-四氟乙基-2,2,3,3-四氟丙基醚）则可作为辅助调节剂，为快速离子转移提供流动环境和低电阻界面。因此，调节电解质的凝固点低至 -51.9 °C，在 -20 °C时离子电导率高达 3.2 mS cm-1。基于溶解结构双调节器，石墨阳极可提供 252 mAh g-1 的高容量，相当于室温容量的 85% 以上，而全电池在 -20 °C 时的容量保持率超过 80%。这些结果表明，溶解结构双调节剂可以提高 Gr-PIB 的性能，促进低温 PIB 及其他材料的发展。
{"title":"Solvation Structure Dual-Regulator Enabled Multidimensional Improvement for Low-Temperature Potassium Ion Batteries","authors":"Yanfang Liu, Hongwei Fu, Caitian Gao, Jie Wen, Ruoya Guo, Wendi Luo, Jiawan Zhou, Bingan Lu","doi":"10.1002/aenm.202403562","DOIUrl":"https://doi.org/10.1002/aenm.202403562","url":null,"abstract":"The operation of graphite-based potassium ion batteries (Gr-PIBs) remains challenging at low temperatures, limited by slow dynamic behavior. Herein, the solvation structure dual-regulator strategy of electrolyte is proposed for multidimensional improvement of K<sup>+</sup> transfer process including ion transfer at both bulk and interface. The designed electrolyte (an amide solvent, 2,2,2-Trifluoro-N, N-dimethylacetamide) with low freezing point and low viscosity as the primary regulator, and a fluorinated solvent (1,1,2,2-Tetrafluoroethyl-2,2,3,3-tetrafluoropropylether) as the secondary regulator provides a flowing environment and low resistive interface for fast ion transfer. As a result, the regulated electrolyte has a low freezing point of −51.9 °C and exhibits a high ionic conductivity of 3.2 mS cm<sup>−1</sup> at −20 °C. Based on the solvation structure dual-regulator, the graphite anode delivered a high capacity of 252 mAh g<sup>−1</sup> which is over 85% of room-temperature capacity, and the capacity retention rate of a full cell at −20 °C is over 80%. These results demonstrate that the solvation structure dual-regulator can improve the performances of Gr-PIBs, promoting the development of low-temperature PIBs and beyond.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142328884","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 recycling of end-of-life Li-ion batteries (EoL LIBs) is critical for maintaining the sustainable LIB industry. In this study, the compositional restoration method for degraded LiΔNi0.6Co0.2Mn0.2O2 cathode via spontaneous galvanic corrosion, which can be conducted at room temperature, is demonstrated. Achieving the lithiation of spent LiΔNi0.6Co0.2Mn0.2O2 to its pristine state at room temperature requires a strong reducing agent with a redox potential lower than 1.6 V (vs Li/Li+), which is very reactive and expensive. In the designed restoration system, spontaneous restoration can be achieved by using an Aluminum (Al) current collector as a reducing agent which has sufficient reducing power (Al/Al3+, 1.37 V (vs Li/Li+)). Moreover, through a galvanic reaction design that utilizes Li-ion in the electrolyte of spent LIBs, the additional Li source required to replenish the Li-deficient NCM is minimized. The galvanic corrosion-based restoration mechanism is systematically analyzed, and a spent Li0.76Ni0.6Co0.2Mn0.2O2 is successfully restored to its pristine state (Li1.05Ni0.6Co0.2Mn0.2O2). Furthermore, restoration strategies accomplishable in not only the cathode state but also the battery state are presented to ensure applicability in practical recycling processes. The proposed strategy suggests a new insight into the direct cathode recycling technology, possessing economic feasibility, and environmental friendliness.
{"title":"Reviving Spent NCM Cathodes via Spontaneous Galvanic Corrosion in Ambient Atmospheric Condition","authors":"Jinju Song, Hayong Song, Jeonghwan Song, Geumui Noh, Hyungsub Kim, Jiyoung Ma, Jung-Je Woo","doi":"10.1002/aenm.202402106","DOIUrl":"https://doi.org/10.1002/aenm.202402106","url":null,"abstract":"The recycling of end-of-life Li-ion batteries (EoL LIBs) is critical for maintaining the sustainable LIB industry. In this study, the compositional restoration method for degraded Li<sub>Δ</sub>Ni<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub> cathode via spontaneous galvanic corrosion, which can be conducted at room temperature, is demonstrated. Achieving the lithiation of spent Li<sub>Δ</sub>Ni<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub> to its pristine state at room temperature requires a strong reducing agent with a redox potential lower than 1.6 V (vs Li/Li<sup>+</sup>), which is very reactive and expensive. In the designed restoration system, spontaneous restoration can be achieved by using an Aluminum (Al) current collector as a reducing agent which has sufficient reducing power (Al/Al<sup>3+</sup>, 1.37 V (vs Li/Li<sup>+</sup>)). Moreover, through a galvanic reaction design that utilizes Li-ion in the electrolyte of spent LIBs, the additional Li source required to replenish the Li-deficient NCM is minimized. The galvanic corrosion-based restoration mechanism is systematically analyzed, and a spent Li<sub>0.76</sub>Ni<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub> is successfully restored to its pristine state (Li<sub>1.05</sub>Ni<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub>). Furthermore, restoration strategies accomplishable in not only the cathode state but also the battery state are presented to ensure applicability in practical recycling processes. The proposed strategy suggests a new insight into the direct cathode recycling technology, possessing economic feasibility, and environmental friendliness.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325927","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}
Ju Hyun Yang, Gi Beom Sim, So Jeong Park, Choong Kyun Rhee, Chang Woo Myung, Youngku Sohn
Fischer–Tropsch Chemistry
In article number 2402062, Chang Woo Myung, Youngku Sohn, and co-workers demonstrated the production of long-chain hydrocarbon fuels through electrochemistry using gold-loaded SrTiO3 perovskite catalysts under ambient conditions. This innovative conversion process utilizes CO2 and H2O, resembling traditional Fischer–Tropsch chemistry. The underlying mechanism at the interface has been predicted by density functional theory calculations.
费托化学在文章编号 2402062 中，Chang Woo Myung、Youngku Sohn 及其合作者展示了在环境条件下使用金负载 SrTiO3 包晶催化剂通过电化学生产长链碳氢化合物燃料的过程。这一创新的转化过程利用了二氧化碳和水，类似于传统的费托化学。密度泛函理论计算预测了界面的基本机制。
{"title":"Exploring Direct Electrochemical Fischer–Tropsch Chemistry of C1–C7 Hydrocarbons via Perimeter Engineering of Au–SrTiO3 Catalyst (Adv. Energy Mater. 36/2024)","authors":"Ju Hyun Yang, Gi Beom Sim, So Jeong Park, Choong Kyun Rhee, Chang Woo Myung, Youngku Sohn","doi":"10.1002/aenm.202470149","DOIUrl":"https://doi.org/10.1002/aenm.202470149","url":null,"abstract":"<p><b>Fischer–Tropsch Chemistry</b></p><p>In article number 2402062, Chang Woo Myung, Youngku Sohn, and co-workers demonstrated the production of long-chain hydrocarbon fuels through electrochemistry using gold-loaded SrTiO<sub>3</sub> perovskite catalysts under ambient conditions. This innovative conversion process utilizes CO<sub>2</sub> and H<sub>2</sub>O, resembling traditional Fischer–Tropsch chemistry. The underlying mechanism at the interface has been predicted by density functional theory calculations.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":24.4,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/aenm.202470149","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142324735","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Huanhuan Gao, Qian Li, Baobing Fan, Zhaozhao Bi, Wenlin Jiang, Sen Zhang, Qunping Fan, Tianqi Chen, Francis R. Lin, Bin Kan, Dangyuan Lei, Wei Ma, Alex K.-Y. Jen
The structural revolutions of non-fullerene acceptors (NFAs) have driven continuous efficiency breakthroughs in organic solar cells (OSCs). Rational regulation of NFA structures toward efficient exciton dissociation and mitigated non-radiative recombination is pivotal for OSCs. The incorporation of asymmetric side chains on NFAs can often achieve these goals by inducing a desirable aggregate state. However, it lacks the studies to directly correlate the side-chain symmetry of NFAs with the exciton delocalization and triplet dynamics in OSCs. Herein, The influence of structural symmetry on the aggregate properties is systematically investigated and exciton/charge dynamics based on two developed biaxial-conjugated NFAs with varied side-chain symmetry. The symmetric NFA having diverse molecular packing orientations can form multiple charge transfer channels in its blend with polymer donor, which cannot be found in that comprising the asymmetric ones. Moreover, a slower rate and lower ratio of the spin-triplet state are formed in the blend of symmetric NFA, resulting in a much lower non-radiative voltage loss in corresponding OSCs. This study reveals the distinct advantages of symmetric NFAs in both aggregate properties and exciton/charge dynamics over those of asymmetric ones, paving the way for developing high-performance OSCs using easier-to-prepare, low-cost symmetric materials.
{"title":"Regulation of Side-Chain Symmetry for Delaying Triplet Formation and Suppressing Non-Radiative Loss in Organic Solar Cells","authors":"Huanhuan Gao, Qian Li, Baobing Fan, Zhaozhao Bi, Wenlin Jiang, Sen Zhang, Qunping Fan, Tianqi Chen, Francis R. Lin, Bin Kan, Dangyuan Lei, Wei Ma, Alex K.-Y. Jen","doi":"10.1002/aenm.202403121","DOIUrl":"https://doi.org/10.1002/aenm.202403121","url":null,"abstract":"The structural revolutions of non-fullerene acceptors (NFAs) have driven continuous efficiency breakthroughs in organic solar cells (OSCs). Rational regulation of NFA structures toward efficient exciton dissociation and mitigated non-radiative recombination is pivotal for OSCs. The incorporation of asymmetric side chains on NFAs can often achieve these goals by inducing a desirable aggregate state. However, it lacks the studies to directly correlate the side-chain symmetry of NFAs with the exciton delocalization and triplet dynamics in OSCs. Herein, The influence of structural symmetry on the aggregate properties is systematically investigated and exciton/charge dynamics based on two developed biaxial-conjugated NFAs with varied side-chain symmetry. The symmetric NFA having diverse molecular packing orientations can form multiple charge transfer channels in its blend with polymer donor, which cannot be found in that comprising the asymmetric ones. Moreover, a slower rate and lower ratio of the spin-triplet state are formed in the blend of symmetric NFA, resulting in a much lower non-radiative voltage loss in corresponding OSCs. This study reveals the distinct advantages of symmetric NFAs in both aggregate properties and exciton/charge dynamics over those of asymmetric ones, paving the way for developing high-performance OSCs using easier-to-prepare, low-cost symmetric materials.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325928","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}
Zhongrun Xiang, Yu Chen, Zhijiang Xie, Kaiyu Yuan, Yue Shu, Pan Chen, Huiqing Wang, Dongdong Ye
Osmotic Energy Harvesting
In article number 2402304, Huiqing Wang, Dongdong Ye, and co-workers synthesized 2D, hierarchical chitin nanosheets via controlled exfoliation from crab shells, assembling them into all-chitin nanosheet membranes for osmotic energy harvesting. Their reverse electrodialysis system powered a calculator, timer, and LED lights, highlighting the enhanced permeability conversion of biomass materials.
渗透能量收集在文章编号 2402304 中，王慧清、叶冬冬及其合作者通过控制蟹壳剥离合成了二维分层甲壳素纳米片，并将其组装成全甲壳素纳米片膜，用于渗透能量收集。他们的反向电渗析系统为计算器、定时器和 LED 灯提供了动力，凸显了生物质材料增强的渗透转换能力。
{"title":"Sustainable Chitin-Derived 2D Nanosheets with Hierarchical Ion Transport for Osmotic Energy Harvesting (Adv. Energy Mater. 36/2024)","authors":"Zhongrun Xiang, Yu Chen, Zhijiang Xie, Kaiyu Yuan, Yue Shu, Pan Chen, Huiqing Wang, Dongdong Ye","doi":"10.1002/aenm.202470154","DOIUrl":"https://doi.org/10.1002/aenm.202470154","url":null,"abstract":"<p><b>Osmotic Energy Harvesting</b></p><p>In article number 2402304, Huiqing Wang, Dongdong Ye, and co-workers synthesized 2D, hierarchical chitin nanosheets via controlled exfoliation from crab shells, assembling them into all-chitin nanosheet membranes for osmotic energy harvesting. Their reverse electrodialysis system powered a calculator, timer, and LED lights, highlighting the enhanced permeability conversion of biomass materials.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":24.4,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/aenm.202470154","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142324736","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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