ACS Applied Energy Materials最新文献

{"title":"Laser-Assisted Rapid Fabrication of Cobalt Hydroxide@Carbon Fiber Composites for High-Performance, Robust Structural Supercapacitors","authors":"Tae Ho Yun,&nbsp;Taeyong Kim,&nbsp;Yunjae Hwang,&nbsp;Ninad B. Velhal,&nbsp;Hyung Wook Park*,&nbsp;Changyong Yim* and Jisoo Kim*,&nbsp;","doi":"10.1021/acsaem.4c0226110.1021/acsaem.4c02261","DOIUrl":"https://doi.org/10.1021/acsaem.4c02261https://doi.org/10.1021/acsaem.4c02261","url":null,"abstract":"<p >Conventional supercapacitor electrodes often rely on time-consuming hydrothermal methods to create nanostructures. In this study, a laser-assisted process was utilized to fabricate cobalt hydroxide on a carbon fiber (CF) composite, achieving a mechanically stable structural capacitor (SSC) within 50 min. Intensive CO₂ laser irradiation facilitated the rapid deposition and growth of diverse nanoarchitectures on the CF substrate. The outstanding performance of the Co(OH)₂@CF electrode was demonstrated by its rate capability, with a cyclic stability of 96.3% maintained through 15,000 cycles and a Coulombic efficiency of 99.5%. A high specific capacitance of 1448.20 F g^–1 was also observed. The unique morphology of the Co(OH)₂@CF electrode enabled efficient charge storage with a high diffusion contribution, even at 50 mV s^–1. The robust SSC device remained stable under external forces and thus showed promise in addressing the sensitivity issues encountered with current supercapacitor devices.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608500","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Fast Carrier Recombination, Nanoconfinement, and Defects Boost Solar-Driven Hydrogen Evolution Reactions at Z-Scheme Heterojunctions","authors":"Ankita Kumari,&nbsp; and ,&nbsp;Dibyajyoti Ghosh*,&nbsp;","doi":"10.1021/acsaem.4c0210110.1021/acsaem.4c02101","DOIUrl":"https://doi.org/10.1021/acsaem.4c02101https://doi.org/10.1021/acsaem.4c02101","url":null,"abstract":"<p >The vertical heterostructure between phase-different two-dimensional (2D) transition metal dichalcogenides (TMDs) and metal monochalcogenides exhibits a promising photocatalytic performance. We combine several computational methods to explore catalytic processes for solar-driven hydrogen evolution reactions (HERs) on thermodynamically stable Mo<i>X</i>₂/SnS (<i>X</i> = S, Se, and Te). Except for MoTe₂/SnS, these heterostructures have prominent staggered band alignment, significantly reducing the band gap and enhancing optical response to visible light irradiation. The time-domain Kohn–Sham (TD-KS) theory and nonadiabatic molecular dynamics (NAMD) depict fast interlayer electron–hole recombination between band edge states, revealing prominent Z-scheme heterojunction formation. The band-to-band relaxation eventually leads to long carrier lifetimes and high redox potential for photogenerated electrons in the SnS layer, enhancing HER catalytic performance. Moreover, the inner layer of SnS that noncovalently interacts with MoS₂ emerges as a superior photocatalytic surface compared to the traditionally investigated outer one. Nanoconfinement influences the hydrogen bond formation between the reactant H atom and <i>X</i> of Mo<i>X</i>₂ (<i>X</i> = S and Se), boosting the catalytic process at the interlayer space. The defect engineering, especially the facile formation of Sn vacancy sites within the nanoconfined SnS layer emerge as the most thermodynamically favourable sites for enhancing the HER activity in the SnS layer. These vacancies introduce a unique local electronic environment that promotes the adsorption and activation of reaction intermediates. The significant dynamic fluctuations of the transient S–H bond at these sites further depict the optimal binding of the reactant, ensuring the best catalytic activity of Sn vacancies in the inner layer. The <i>in silico</i> study provides a detailed atomistic understanding of the hydrogen evolution process on metal chalcogenide heterostructures, suggesting their strategic design principles to boost photocatalytic activities.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142550138","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Acid Doping of PEDOT:PSS Strengthens Interfacial Compatibility toward Efficient and Stable Perovskite Solar Cells","authors":"Jidong Deng,&nbsp;Yinhu Gao,&nbsp;Yuliang Che,&nbsp;Xubiao Wang,&nbsp;Jingyi Sun,&nbsp;Zhihan Liao,&nbsp;Xiao Wang,&nbsp;Yuanyuan Li,&nbsp;Xiaofeng Li,&nbsp;Jinbao Zhang,&nbsp;Xiaoli Zhang* and Li Yang*,&nbsp;","doi":"10.1021/acsaem.4c0209210.1021/acsaem.4c02092","DOIUrl":"https://doi.org/10.1021/acsaem.4c02092https://doi.org/10.1021/acsaem.4c02092","url":null,"abstract":"<p >Poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate) (PEDOT:PSS) has been widely applied as a hole transport material in s. Although PEDOT:PSS exhibits the advantages of superior conductivity and low material cost, the corresponding devices suffer from low photovoltaic performance due to unsatisfactory interfacial properties. Here, an acid treatment strategy is developed to modify the chemical properties of PEDOT:PSS by different HX (X = Cl, Br, I) acids. We present evidence of an effective ion exchange process between HX and PEDOT:PSS and show that the anion-dependent dedoping of PEDOT:PSS leads to large variation of thin-film conductivity, film hydrophilicity, and interfacial contact between perovskite and PEDOT:PSS. PEDOT:PSS treated by HCl demonstrates optimal interfacial compatibility along with superior charge collection efficiency, which contributes to significantly enhanced device efficiency (17.63%) compared to the control device (14.56%). Moreover, the resulting unencapsulated devices based on HCl show superior long-term stability, maintaining more than 90% of their initial efficiency after 2355 h, whereas the control device only kept about 47% of original PCEs after 1120 h. This work indicates the effectiveness of acid treatment in modulating the doping properties of PEDOT:PSS and provides an efficient way to improve the interfacial performance of perovskite solar cells.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142550340","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Antiflooding Gas Diffusion Electrodes Enabled by Liquid–Solid–Liquid Interfaces for Durable CO2 Electrolysis","authors":"Yue Yang,&nbsp;Nanhui Li,&nbsp;Jianghao Wang,&nbsp;Wei Zhao and Hao Bin Wu*,&nbsp;","doi":"10.1021/acsaem.4c0189610.1021/acsaem.4c01896","DOIUrl":"https://doi.org/10.1021/acsaem.4c01896https://doi.org/10.1021/acsaem.4c01896","url":null,"abstract":"<p >Gas diffusion electrodes (GDEs) show great potential to improve the current densities of the industrial electrochemical carbon dioxide reduction reaction (eCO₂RR). The triple-phase boundary (TPB) in GDEs is the key for promoted reaction kinetics, yet such a reaction interface typically suffers from rapid degradation due to electrolyte flooding and salt precipitation. Herein, we demonstrate that a GDE modified with liquid perfluorocarbon (PFC) would notably prolong the lifespan of the GDE with a Bi catalyst in flow-cell electrolyzers. PFC with superhydrophobicity and high CO₂ solubility would construct a liquid–solid–liquid reaction interface that prevents the intrusion of electrolytes into the microporous layer (MPL) without hampering the mass transport of CO₂. Our work demonstrates an effective strategy to construct a robust and efficient electrochemical reaction interface for the eCO₂RR with improved stability for potential industrial applications.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142550142","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Correction to “Air Stable O3-Type Cathode Material with Nanometer Size for Durable Low-Temperature Sodium-Ion Batteries”","authors":"Yan Jin,&nbsp;Yunbo Li,&nbsp;Jianguo Li,&nbsp;Hongyan Zhou,&nbsp;Xianghong Chen,&nbsp;Pan Jiang,&nbsp;Qinghua Fan,&nbsp;Quan Kuang*,&nbsp;Youzhong Dong and Yanming Zhao*,&nbsp;","doi":"10.1021/acsaem.4c0238410.1021/acsaem.4c02384","DOIUrl":"https://doi.org/10.1021/acsaem.4c02384https://doi.org/10.1021/acsaem.4c02384","url":null,"abstract":"","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142550339","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Decisive Effect of Hydrophobic Rigid-Flexible Coupled Side Chains of Polycarbazoles on the Performance of Anion Exchange Membranes for Fuel Cells","authors":"Ning Xie,&nbsp;Tao Wang,&nbsp;Haowei Kang,&nbsp;Yiting Liu,&nbsp;Xinli Li,&nbsp;Qiang Weng,&nbsp;Xingming Ning,&nbsp;Pei Chen*,&nbsp;Xinbing Chen* and Zhongwei An,&nbsp;","doi":"10.1021/acsaem.4c0218510.1021/acsaem.4c02185","DOIUrl":"https://doi.org/10.1021/acsaem.4c02185https://doi.org/10.1021/acsaem.4c02185","url":null,"abstract":"<p >High-performance anion exchange membranes (AEMs) have garnered increasing attention in recent years. However, commercial progress of the AEM for fuel cells is still hindered by its low ionic conductivity and inadequate alkaline stability. In this study, we propose the incorporation of a hydrophobic rigid-flexible coupled side chain into a polycarbazolyl AEM as an innovative approach to enhance both the conductivity and stability. The results demonstrate that the AEMs with hydrophobic rigid-flexible coupled side chains exhibit superior conductivity and stability compared with those without (PQMC-0). For example, the ion exchange capacity of PQMC-10 is reduced by 11% than PQMC-0, but its conductivity is enhanced by 14%, dimensional change is decreased by almost half, and oxidative stability is increased by more than four times. Improved conductivity of the AEMs can be attributed to the presence of hydrophobic rigid-flexible coupled side chains, making it easier for AEM to construct microphase separation to facilitate ion transport. Furthermore, the introduction of hydrophobic side chains reduces water absorption of the membrane, thereby enhancing its dimensional stability while minimizing the intake of free radicals or hydroxide ions present in water. Consequently, this modification significantly improves the oxidative and alkaline stability as well. Finally, the PQMC-10 shows a maximum power density of 649 mW cm^–2 in a single fuel cell, which is three times bigger than that of PQMC-0, indicating a promising application in the field of fuel cells.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142517081","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Zeolite-Templated Carbons as Supercapacitors: The Fundamental Role of Structural and Textural Properties","authors":"Sirine Zallouz,&nbsp;Thibaud Aumond,&nbsp;Alain Moissette,&nbsp;Alexander Sachse* and Camélia Matei Ghimbeu*,&nbsp;","doi":"10.1021/acsaem.4c0120310.1021/acsaem.4c01203","DOIUrl":"https://doi.org/10.1021/acsaem.4c01203https://doi.org/10.1021/acsaem.4c01203","url":null,"abstract":"<p >Zeolite-templated carbons (ZTCs) with controlled properties (particle size, porous network, and structural organization) were used as model materials to understand their performance in supercapacitors. At low current rates (0.1 A g^–1), the capacitance in 1 M H₂SO₄ electrolyte is governed by the specific surface area and increases with the <i>S</i>_BET up to ∼2300 m² g^–1 and then decreases for higher <i>S</i>_BET. At a high current density (10 A g^–1), the capacitance retention is affected by several ZTC properties. Higher mesoporous volume and lower C/O and C/H ratios (high O-groups and edge defect sites) lead to the capacitance retention enhancement. Among the long-range ordered ZTCs (FAU, EMT, and beta), beta ZTC shows the highest capacitance retention owing to its highest mesopore volume, which favors electrolyte diffusion. Moreover, the structural organization of ZTC proved to play an important role on the capacitance retention as well. Therefore, disordered materials (FAU-ZTC-anthracene) show higher capacitance (∼140 F g^–1 at 0.1 A g^–1), capacitance retention (67% at 10 A g ^–1), and long-term cycling (87% after 10000 cycles) than ordered materials (FAU-ZTC-ethylene). Overall, this work highlights the importance not only of the specific surface area but also of the pore architecture and organization, particle size, and chemical structure.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142551202","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Augmentation of Halide Vacancy Rectification through Copper Ion Polarization in Nonsubstituted Porphyrin for Printable Carbon-Based Perovskite Solar Cells","authors":"Yuting Li,&nbsp;Jingwen He and Wenjun Wu*,&nbsp;","doi":"10.1021/acsaem.4c0091410.1021/acsaem.4c00914","DOIUrl":"https://doi.org/10.1021/acsaem.4c00914https://doi.org/10.1021/acsaem.4c00914","url":null,"abstract":"<p >In the context of porphyrins, enhancing their charge transfer or defect repair function in perovskite solar cells has been a primary focus of the current research, particularly through the introduction of functional groups. This enhancement of the porphyrin framework’s defect repair capability is a crucial strategy for simplifying device assembly processes and reducing costs. In our study, we introduced metal ions into the porphyrin ring via a straightforward one-step reaction, which induced polarization of the large π bond electron cloud within the ring, thereby augmenting its interaction with perovskite defect states. Our research discovered that the introduction of copper ions could significantly increase the dipole moment of the porphyrin ring from 0.0062 to 0.0737D, which is the fundamental reason for ion-induced passivation enhancement. The introduction of copper ions also strengthens the binding ability of the negative electron end with halogen vacancies (uncoordinated Pb²⁺) and inhibits the migration of I^– ions. As a result, the photovoltaic conversion efficiency of fully printable mesoscopic perovskite solar cells (p-MPSCs) increased from 14.15% in the control group to 16.13%. This work has thus opened a new pathway for enhancing the ability to repair perovskite defect states through the electron induction of the porphyrin ring.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142550874","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electron Paramagnetic Resonance Monitoring of Sodium Clustering and Its Effect on the Sodium Storage of Biowaste-Derived Carbons","authors":"Rositsa R. Kukeva,&nbsp;Mariya Kalapsazova*,&nbsp;Sonya Harizanova,&nbsp;Ivan Markov Uzunov,&nbsp;Pavel Markov,&nbsp;Ivanka Spassova and Radostina Stoyanova*,&nbsp;","doi":"10.1021/acsaem.4c0219510.1021/acsaem.4c02195","DOIUrl":"https://doi.org/10.1021/acsaem.4c02195https://doi.org/10.1021/acsaem.4c02195","url":null,"abstract":"<p >Biowaste-derived carbons store large amounts of sodium as many competing reactions of adsorption, intercalation, and pore filling take place. Herein, we report electron paramagnetic resonance (EPR) spectroscopy as a comprehensive method to monitor the interaction of sodium with carbons used as electrodes in sodium-ion cells. It is shown that EPR can distinguish signals due to sodium intercalation and sodium cluster growth. Applying the correlation between the EPR line width and the metallic particle dimension, the sodium clusters are quantified regarding their size. In terms of the EPR, we discuss the sodiation mechanism and sodium storage performance of carbons derived from spent coffee grounds. The smallest sodium clusters (below 2 nm) are formed on closed-pore carbons at a potential of 0.01 V, while the largest clusters (around 200 nm) occur on hydrogen-rich carbons at 0.05 V at the earliest. The small sodium clusters generated at around 0.01 V give extra capacity, while sodium intercalation occurring between 0.5 and 0.1 V ensures good cycle stability.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsaem.4c02195","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142516856","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Non-covalent Immobilization of Metal N-Heterocyclic Carbene Complexes onto Carbon Cloth as Bifunctional Electrodes for Overall Water Splitting in Alkaline Medium","authors":"Zhoveta Yhobu,&nbsp;Mayur Jagdishbhai Patel,&nbsp;Jan Grzegorz Małecki,&nbsp;Doddahalli H. Nagaraju and Srinivasa Budagumpi*,&nbsp;","doi":"10.1021/acsaem.4c0212710.1021/acsaem.4c02127","DOIUrl":"https://doi.org/10.1021/acsaem.4c02127https://doi.org/10.1021/acsaem.4c02127","url":null,"abstract":"<p >The use of molecular complex-modified electrodes presents avenues for their rational and simplistic design to serve as efficient catalysts in emerging electrocatalytic applications. Herein, three molecular electrocatalysts, <b>CoLBr</b>_<b>2</b>, <b>NiLBr</b>₂, and <b>PdLBr2</b>, were synthesized from the pyridine-functionalized N-heterocyclic carbene (NHC) ligand (<b>HLBr</b>) and physisorbed onto CC to obtain complex-modified free-standing electrodes. These complex-modified electrodes were investigated for their hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) activity in 1 M KOH. Among the complex-modified electrodes, the <b>CoLBr</b>_<b>2</b> electrode exhibited the best HER activity with an overpotential of −255 mV vs RHE at 10 mA/cm² and a Tafel slope of 155 mV/dec. For the OER activity, the <b>NiLBr</b>_<b>2</b> electrode exhibited the best performance with an overpotential of 376 mV vs RHE at 10 mA/cm² and a Tafel slope of 86 mV/dec. The bifunctional nature of the complex-modified free-standing CC electrodes enabled the assembly of a symmetric alkaline electrolyzer, i.e., <b>CoLBr</b>_<b>2</b>//<b>CoLBr2</b>, with a cell voltage of 1.81 V at 10 mA/cm². The post-stability analysis of the complex-modified electrodes revealed that the complexes possessed chemical stability despite undergoing long-term stability tests at high overpotentials. These findings authenticate the versatility of metal NHC complexes for fabricating molecularly modified free-standing electrodes for the HER, OER, and overall water splitting, paving the way for the development of sustainable energy conversion technologies.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142550805","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}