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Enhancing the Stability of CaO-Based Looping Materials in Thermochemical Energy Storage by Codoping Y and Mg
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2024-12-10 DOI: 10.1021/acsaem.4c0290510.1021/acsaem.4c02905
Jifu Wang, Wei Xiong, Zhengxin Ding, Pengzhao Wang* and Jinlin Long*, 
{"title":"Enhancing the Stability of CaO-Based Looping Materials in Thermochemical Energy Storage by Codoping Y and Mg","authors":"Jifu Wang,&nbsp;Wei Xiong,&nbsp;Zhengxin Ding,&nbsp;Pengzhao Wang* and Jinlin Long*,&nbsp;","doi":"10.1021/acsaem.4c0290510.1021/acsaem.4c02905","DOIUrl":"https://doi.org/10.1021/acsaem.4c02905https://doi.org/10.1021/acsaem.4c02905","url":null,"abstract":"<p >Aiming to improve the decay in thermochemical energy storage (TCES) performance of CaO-based looping materials with the number of carbonation/calcination cycles, a series of Y/Mg-codoped CaO-based materials were prepared by using the classical sol–gel method and citric acid as a carbon template to enhance the porosity and specific surface area. The structural characterizations showed that Y and Mg were presented in two forms. Part of Y/Mg was presented in the form of Y<sub>2</sub>O<sub>3</sub> and MgO nanoparticles with an average size of 15 and 40 nm, respectively. These Y<sub>2</sub>O<sub>3</sub> and MgO nanoparticles with high Tammann temperature and thermal conductivity were highly dispersed to retard the sintering and growth of CaO grains. The rest of Y and Mg were doped into the framework of the CaO lattice in atomic form by substituting Ca atoms. These Y and Mg created a large amount of the oxygen vacancies surrounding Ca atoms to facilitate the electron transfer from Ca<sup>2+</sup> ions to dopants, which enhanced the CO<sub>2</sub> capture capacity of CaO-based materials by improving the kinetics of the carbonation reaction. As a result, the optimal CaO-based composite denoted as Ca/Y5/Mg10 exhibited a high initial energy storage density of up to &gt;2300 kJ/kg and held an excellent looping reaction stability after 25 carbonation/calcination cycles owing to the cooperation of Y with Mg additives. This work provided effective and economical CaO-based looping materials for application in thermochemical energy storage.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"7 24","pages":"12165–12173 12165–12173"},"PeriodicalIF":5.4,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874983","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}
引用次数: 0
Synergistic Effect of Carbon Encapsulation and Iron Doping Based on Metal–Organic Framework Precursor Enhances NaVPO4F Electrochemical Performance for Sodium-Ion Batteries
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2024-12-10 DOI: 10.1021/acsaem.4c0219910.1021/acsaem.4c02199
Yao Xu, Linwei Yin, Changsheng Yang, Ying Lei, Haiyan Zhang* and Kwunnam Hui, 
{"title":"Synergistic Effect of Carbon Encapsulation and Iron Doping Based on Metal–Organic Framework Precursor Enhances NaVPO4F Electrochemical Performance for Sodium-Ion Batteries","authors":"Yao Xu,&nbsp;Linwei Yin,&nbsp;Changsheng Yang,&nbsp;Ying Lei,&nbsp;Haiyan Zhang* and Kwunnam Hui,&nbsp;","doi":"10.1021/acsaem.4c0219910.1021/acsaem.4c02199","DOIUrl":"https://doi.org/10.1021/acsaem.4c02199https://doi.org/10.1021/acsaem.4c02199","url":null,"abstract":"<p >Sodium fluorovanadium phosphate (NaVPO<sub>4</sub>F) has long been recognized as a promising cathode material for sodium-ion batteries. However, its low conductivity has limited its practical application due to its poor rate performance and long-term stability. The study introduces a method to enhance the electrochemical performance of NaVPO<sub>4</sub>F by using the metal–organic framework (MOF) as a precursor. This method involves the incorporation of Fe-doping and MOF-derived carbon encapsulation. The synthesized NaV<sub>0.94</sub>Fe<sub>0.06</sub>PO<sub>4</sub>F/MC samples (NVPF-Fe/MC) exhibit extraordinary qualities as cathode material for sodium-ion batteries: a high capability (123.1 mAh/g at 1C), outstanding ultralong cyclability (remaining 83.0% of its capacity even after 1000 cycles at a high cycling rate of 5 C), and significantly improved rate performance. The NVPF-Fe/MC||HC full cell also exhibits excellent reversible capacity (retaining 87.7% sodium storage capacity after 100 cycles). The mesoporous carbon nanonetwork shortens the ion-electron diffusion pathway, promoting ionic-electronic conductivity and reaction kinetics. Additionally, Fe<sup>3+</sup> doping increases the cell volume to enlarge the diffusion channel, while activating part of the V<sup>5+</sup>/V<sup>4+</sup> (4.0 V vs Na<sup>+</sup>/Na) due to the induced effect of Fe<sup>3+</sup>, thereby improving the specific capacity and cycling stability.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"7 24","pages":"11890–11899 11890–11899"},"PeriodicalIF":5.4,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142870120","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}
引用次数: 0
Distortion and Destabilization of Mg Hydride Facing High Entropy Alloy Matrix
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2024-12-10 DOI: 10.1021/acsaem.4c0256910.1021/acsaem.4c02569
Kohta Asano*, Lars J. Bannenberg, Herman Schreuders, Hirotada Hashimoto, Shigehito Isobe, Yuki Nakahira, Akihiko Machida, Hyunjeong Kim and Kouji Sakaki, 
{"title":"Distortion and Destabilization of Mg Hydride Facing High Entropy Alloy Matrix","authors":"Kohta Asano*,&nbsp;Lars J. Bannenberg,&nbsp;Herman Schreuders,&nbsp;Hirotada Hashimoto,&nbsp;Shigehito Isobe,&nbsp;Yuki Nakahira,&nbsp;Akihiko Machida,&nbsp;Hyunjeong Kim and Kouji Sakaki,&nbsp;","doi":"10.1021/acsaem.4c0256910.1021/acsaem.4c02569","DOIUrl":"https://doi.org/10.1021/acsaem.4c02569https://doi.org/10.1021/acsaem.4c02569","url":null,"abstract":"<p >The thermal stability of an equilibrium phase may be tuned due to lattice strain and distortion induced by nanosizing. We apply these effects to destabilize magnesium hydride, a promising hydrogen storage material owing to its high gravimetric hydrogen density but with a too high operating temperature/low supply pressure of hydrogen for most practical applications. The destabilization is attempted with MgH<sub>2</sub> in contact with high entropy alloy (HEA), in which multiple metal atoms lead to lattice strain and distortion. Here, two HEAs, CrMnFeCoNi with a face centered cubic (fcc) structure and TiVZrNbHf with a body centered cubic (bcc) structure, were prepared. Subsequently, they were cosputtered with Mg to synthesize Mg–HEA thin films, respectively. Although, in the Mg–CrMnFeCoNi thin films, miscible metals with Mg as Co and Ni may hamper the formation of independent Mg domains, a small proportion of Mg atoms form destabilized MgH<sub>2</sub>. In contrast, Mg and TiVZrNbHf domains are chemically segregated at the nanoscale in the Mg–TiVZrNbHf thin films. The formation of nanometer-sized Mg domains is promoted by atomic rearrangement following the structural change of TiVZrNbHf from a bcc to an fcc structure upon hydrogenation, resulting in distorted and destabilized MgH<sub>2</sub>. Our strategy to use HEAs and the structural change upon hydrogenation for the formation of destabilized MgH<sub>2</sub> is effective and opens up the possibility for the development of advanced and low-cost hydrogen storage and supply systems.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"7 24","pages":"11644–11651 11644–11651"},"PeriodicalIF":5.4,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874980","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}
引用次数: 0
Development of a Robust p-Si/p-Cu2O/PhC2Cu Tandem Photocathode for Photoelectrochemical Water Splitting
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2024-12-09 DOI: 10.1021/acsaem.4c0255110.1021/acsaem.4c02551
Bo Pei, Yinmei Li, Shenhui Ma* and Yuyu Bu*, 
{"title":"Development of a Robust p-Si/p-Cu2O/PhC2Cu Tandem Photocathode for Photoelectrochemical Water Splitting","authors":"Bo Pei,&nbsp;Yinmei Li,&nbsp;Shenhui Ma* and Yuyu Bu*,&nbsp;","doi":"10.1021/acsaem.4c0255110.1021/acsaem.4c02551","DOIUrl":"https://doi.org/10.1021/acsaem.4c02551https://doi.org/10.1021/acsaem.4c02551","url":null,"abstract":"<p >The photoelectrochemical (PEC) water splitting performance of Si-based PEC devices is usually restricted by low stability and weak photogenerated carrier transport ability. Herein, a micropyramid array structure (p-SiMPs)/p-Cu<sub>2</sub>O/PhC<sub>2</sub>Cu/Pt photocathode device with a p-p-n heterojunction structure is developed. In this tandem PEC device, a p-p heterojunction of p-SiMPs/p-Cu<sub>2</sub>O is achieved, endowing a higher interface electric field and stronger energy of photoinduced electrons for PEC water reduction. In addition, a stable n-type PhC<sub>2</sub>Cu protective layer is prepared on the surface of the PEC device by the photoassisted polymerization method, which can improve the stability of PEC water reduction largely. After Pt cocatalytic layer deposition, the p-SiMPs/p-Cu<sub>2</sub>O/PhC<sub>2</sub>Cu/Pt tandem photocathode can achieve a saturation photocurrent density of −30 mA/cm<sup>2</sup> at −0.9 V (vs RHE) and a photocurrent threshold voltage of −0.1 V for water reduction. This work provides a silicon-based p-p-n heterojunction tandem structure for the PEC water splitting; meanwhile, it indicates that PhC<sub>2</sub>Cu is a potential material to improve the stability of silicon-based PEC devices.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"7 24","pages":"12059–12068 12059–12068"},"PeriodicalIF":5.4,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874908","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}
引用次数: 0
Electronic Structure and Photocatalytic Activity of Dual Z-Scheme CdS@Bi2S3–MoS2 Heterostructures with a Full Spectrum
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2024-12-09 DOI: 10.1021/acsaem.4c0217310.1021/acsaem.4c02173
Dan Han, Wei Mo, Ning Yang, Lei Zuo, Qinghua Sun and Xianghua Zeng*, 
{"title":"Electronic Structure and Photocatalytic Activity of Dual Z-Scheme CdS@Bi2S3–MoS2 Heterostructures with a Full Spectrum","authors":"Dan Han,&nbsp;Wei Mo,&nbsp;Ning Yang,&nbsp;Lei Zuo,&nbsp;Qinghua Sun and Xianghua Zeng*,&nbsp;","doi":"10.1021/acsaem.4c0217310.1021/acsaem.4c02173","DOIUrl":"https://doi.org/10.1021/acsaem.4c02173https://doi.org/10.1021/acsaem.4c02173","url":null,"abstract":"<p >Two-dimensional Bi<sub>2</sub>S<sub>3</sub> is considered a better photocatalyst when combined with CdS. To deeply understand electronic structures between CdS and Bi<sub>2</sub>S<sub>3</sub>, CdS@Bi<sub>2</sub>S<sub>3</sub> core–shell nanorods (NRs) were synthesized with a two-step hydrothermal method, and CdS@Bi<sub>2</sub>S<sub>3</sub>–MoS<sub>2</sub> composites were obtained with MoS<sub>2</sub> nanoparticles decorated on the surface of CdS@Bi<sub>2</sub>S<sub>3</sub> NRs. Then, the energy band alignments in CdS@Bi<sub>2</sub>S<sub>3</sub>–MoS<sub>2</sub> were constructed from XPS and UPS measurements, and dual <i>z</i>-scheme CdS@Bi<sub>2</sub>S<sub>3</sub>–MoS<sub>2</sub> heterostructures were confirmed from charge transfer with electron spin resonance (ESR) signals of •O<sub>2</sub><sup>–</sup> and •OH. Finally, the photocatalytic hydrogen activities were carried out with the prepared samples. The results showed that the optimized CdS@Bi<sub>2</sub>S<sub>3</sub> core–shell NRs have a hydrogen production rate of 4.29 mmol·h<sup>–1</sup>·g<sup>–1</sup>, which is 8.4 times higher than that of the pure CdS nanorods, and the optimized CdS@Bi<sub>2</sub>S<sub>3</sub>–MoS<sub>2</sub> heterostructure has a hydrogen production rate of 8.72 mmol·h<sup>–1</sup>·g<sup>–1</sup>, which is 17 times higher than that of the pure CdS NRs. The enhanced photocatalytic activity can be ascribed to the dual <i>z</i>-scheme heterostructure and full-spectrum absorption; the former is favorable for the efficient separation of the photogenerated electron–hole pairs, and the latter is beneficial to the production of more photogenerated carriers. The studies will be helpful to understand the electronic structures of Bi<sub>2</sub>S<sub>3</sub> and the related heterostructures.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"7 24","pages":"11879–11889 11879–11889"},"PeriodicalIF":5.4,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874989","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}
引用次数: 0
Cellulose Nanocrystal-Incorporated MAPbI3 for Inverted Perovskite Solar Cells with Enhanced Efficiency and Stability
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2024-12-09 DOI: 10.1021/acsaem.4c0260210.1021/acsaem.4c02602
Yen-Chung Feng, Cheng-En Cai, Bo-Tau Liu, Hongta Yang and Rong-Ho Lee*, 
{"title":"Cellulose Nanocrystal-Incorporated MAPbI3 for Inverted Perovskite Solar Cells with Enhanced Efficiency and Stability","authors":"Yen-Chung Feng,&nbsp;Cheng-En Cai,&nbsp;Bo-Tau Liu,&nbsp;Hongta Yang and Rong-Ho Lee*,&nbsp;","doi":"10.1021/acsaem.4c0260210.1021/acsaem.4c02602","DOIUrl":"https://doi.org/10.1021/acsaem.4c02602https://doi.org/10.1021/acsaem.4c02602","url":null,"abstract":"<p >Herein, cellulose nanocrystals (CNCs) were added to the MAPbI<sub>3</sub> layer to enhance the photovoltaic properties of MAPbI<sub>3</sub>-based inverted perovskite solar cells (PVSCs). The addition of CNCs to the perovskite active layer helps repair crystal defects, improves crystal quality, and stabilizes the perovskite film structure by forming hydrogen bonds between hydroxyl groups and MAPbI<sub>3</sub>. This defect passivation by CNCs leads to the formation of larger and denser crystal grains along with enhanced light absorption in the CNC-doped perovskite films. Consequently, trap density is reduced and carrier recombination is suppressed, thereby improving the power conversion efficiency (PCE) and stability of the CNC-doped PVSCs. The structure of the CNC-based inverted PVSCs comprises fluorine-doped tin oxide/NiO<sub><i>x</i></sub>/CNC:MAPbI<sub>3</sub>/PC<sub>61</sub>BM/BCP/Ag. The CNC-doped PVSC demonstrated an open-circuit voltage (<i>V</i><sub>OC</sub>) of 1.07 V, a short-circuit current density (<i>J</i><sub>SC</sub>) of 24.43 mA cm<sup>–2</sup>, a fill factor (FF) of 76.1%, and a PCE of 19.90%. Furthermore, the insertion of copolyacrylamide (PMD25) at the interface between the perovskite active layer and the NiO<sub><i>x</i></sub>-based hole-transport layer effectively reduced the number of interfacial crystal defects. The MAPbI<sub>3</sub> layer deposited on PMD25-modified NiO<sub><i>x</i></sub> exhibited denser crystal packing and higher carrier mobility, achieving a <i>V</i><sub>OC</sub> of 1.08 V, a <i>J</i><sub>SC</sub> of 25.03 mA cm<sup>–2</sup>, an FF of 76.7%, and a PCE of 20.72%. Additionally, the CNC-doped PVSC, protected with a hydrophobic electrospun PVDF-HFP film, retained 80% of its initial PCE after storage for 600 h under ambient conditions (30 °C, 50% relative humidity).</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"7 24","pages":"12092–12102 12092–12102"},"PeriodicalIF":5.4,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874904","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}
引用次数: 0
Polyurethane-Encapsulated Mesoporous Carbon-Based Perovskite Solar Cells Resilient to Extreme Humidity and Mitigation of the Related Reversible J–V Bump
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2024-12-09 DOI: 10.1021/acsaem.4c0257210.1021/acsaem.4c02572
Salvatore Valastro, Gaetano Calogero, Emanuele Smecca, Valentina Arena, Giovanni Mannino, Corrado Bongiorno, Ioannis Deretzis, Giuseppe Fisicaro, Antonino La Magna, Simone Galliano*, Gabriele Viada, Matteo Bonomo, Claudia Barolo and Alessandra Alberti*, 
{"title":"Polyurethane-Encapsulated Mesoporous Carbon-Based Perovskite Solar Cells Resilient to Extreme Humidity and Mitigation of the Related Reversible J–V Bump","authors":"Salvatore Valastro,&nbsp;Gaetano Calogero,&nbsp;Emanuele Smecca,&nbsp;Valentina Arena,&nbsp;Giovanni Mannino,&nbsp;Corrado Bongiorno,&nbsp;Ioannis Deretzis,&nbsp;Giuseppe Fisicaro,&nbsp;Antonino La Magna,&nbsp;Simone Galliano*,&nbsp;Gabriele Viada,&nbsp;Matteo Bonomo,&nbsp;Claudia Barolo and Alessandra Alberti*,&nbsp;","doi":"10.1021/acsaem.4c0257210.1021/acsaem.4c02572","DOIUrl":"https://doi.org/10.1021/acsaem.4c02572https://doi.org/10.1021/acsaem.4c02572","url":null,"abstract":"<p >Mesoporous carbon-based (mC) hole-transporting layer-free architectures offer a cost-effective solution for the commercialization of perovskite solar cells (PSCs). Adding 5-aminovaleric acid (AVA) to MAPbI<sub>3</sub> reduces defect concentration and enhances pore filling, while Eu enrichment in CsPbI<sub>3</sub> reduces cation migration and enables device reusability. In this study, AVA-MAPbI<sub>3</sub> mC-PSCs were encapsulated at room temperature (RT) with a solvent- and water-free polyurethane (PU) resin. Under continuous ambient light, RT, and 40% relative humidity (RH), the PU encapsulant acts as a barrier to extend device durability and enable reusability. The formation of a bump in the <i>J</i>–<i>V</i> curve after ∼250 h, already reported at a low scan rate but here observed at 50 mV/s, strongly reduces the photovoltaic performances. We demonstrate that the bump is not linked to the formation of PbI<sub>2</sub> but is explained by a water-vacancy interaction that increases cation mobility and enhances screening effects near the electron-transport layer. The photovoltaic performances are fully restored by drying the devices under N<sub>2</sub> flow for ∼48 h. A further addition of a hydrophobic Kapton tape interlayer between the PU and device mitigates bump formation, boosts <i>t</i><sub>90</sub> to ∼6000 h, and projects <i>t</i><sub>80</sub> to ∼10,800 h. Differently from the Kapton tape used alone, PU provides effective sealing all around the devices, ensuring stability in 100% RH at 90 °C and even underwater. For indoor applications, Eu:CsPbI<sub>3</sub> mC-PSCs typically degrade from the γ- to δ-phase within ∼1 h in air, whereas PU-encapsulated devices achieve <i>t</i><sub>80</sub> ∼250 h, extendable to 1250 h with an additional closure glass slide.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"7 24","pages":"12069–12083 12069–12083"},"PeriodicalIF":5.4,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874972","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}
引用次数: 0
Nonionic Amphiphilic Copolymers of Poly(poly(ethylene Glycol) Methacrylate) Brushes with Methyl Methacrylate Prepared by Atom Transfer Radical Polymerization as Dry Solid Polymer Electrolytes for Next Generation Li-ion Battery Applications
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2024-12-08 DOI: 10.1021/acsaem.4c0251910.1021/acsaem.4c02519
Ákos Szabó, Denis Ershov, Ágnes Ábrahám, Éva Kiss, Györgyi Szarka, Ilona Felhősi, Benjámin Gyarmati, Attila Domján, Béla Iván* and Robert Kun*, 
{"title":"Nonionic Amphiphilic Copolymers of Poly(poly(ethylene Glycol) Methacrylate) Brushes with Methyl Methacrylate Prepared by Atom Transfer Radical Polymerization as Dry Solid Polymer Electrolytes for Next Generation Li-ion Battery Applications","authors":"Ákos Szabó,&nbsp;Denis Ershov,&nbsp;Ágnes Ábrahám,&nbsp;Éva Kiss,&nbsp;Györgyi Szarka,&nbsp;Ilona Felhősi,&nbsp;Benjámin Gyarmati,&nbsp;Attila Domján,&nbsp;Béla Iván* and Robert Kun*,&nbsp;","doi":"10.1021/acsaem.4c0251910.1021/acsaem.4c02519","DOIUrl":"https://doi.org/10.1021/acsaem.4c02519https://doi.org/10.1021/acsaem.4c02519","url":null,"abstract":"<p >Amphiphilic copolymers of comb-like poly(poly(ethylene glycol) methacrylate) (PPEGMA) with methyl methacrylate (MMA) synthesized by one-pot atom transfer radical polymerization were mixed with lithium bis (trifluoromethanesulfonyl) imide salt to formulate dry solid polymer electrolytes (DSPE) for semisolid-state Li-ion battery applications. The PEO-type side chain length (EO monomer’s number) in the PEGMA macromonomer units was varied, and its influence on the mechanical and electrochemical characteristics was investigated. It was found that the copolymers, due to the presence of PMMA segments, possess viscoelastic behavior and less change in mechanical properties than a PEO homopolymer with 100 kDa molecular weight in the investigated temperature range. In contrast to the PEO homopolymer, it was found that no crystallization of the copolymers occurs in the presence of the Li-salt. Solid-state NMR and cross-polarization NMR studies revealed that no crystallization (i.e., ion-pair formation) of the Li-salt occurs in the case of the copolymer samples at ambient temperatures; thereby, no phase separation takes place, in contrast to the reference PEO homopolymer sample, which resulted in fairly good ionic conductivity of the copolymers at lower temperatures. The temperature-dependent Li-ion conductivity analyses showed that the conductivity of the copolymers falls in the 10<sup>–6</sup>–10<sup>–3</sup> S/cm range, which is typical for polyether-type DSPEs, but the much lower mass fraction of EO monomers in the copolymers provides the same ionic conductivity values than that of the PEO homopolymer. From a large-scale practical point of view, this clearly indicates reduced Li-salt usage if such copolymer matrices are used instead of PEO homopolymer. Moreover, linear sweep voltammetry (LSV) polarization measurements showed that the PPEGMA-MMA copolymer electrolytes can exhibit a 200–300 mV broader electrochemical stability window than the PEO homopolymer, which is crucial in designing high energy density semisolid-state Li-ion batteries.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"7 24","pages":"12036–12047 12036–12047"},"PeriodicalIF":5.4,"publicationDate":"2024-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsaem.4c02519","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874962","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}
引用次数: 0
Effects of Different Doping Strategies on Cubic Li7La3Zr2O12 Solid-State Li-Ion Battery Electrolytes
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2024-12-08 DOI: 10.1021/acsaem.4c0270810.1021/acsaem.4c02708
Nikolai Helth Gaukås, Tor Olav Sunde, Bjørnar Arstad, Anita Hamar Reksten, Elena Stefan, Annett Thøgersen, Madeeha Khalid Pedersen, Truls Norby and Yngve Larring*, 
{"title":"Effects of Different Doping Strategies on Cubic Li7La3Zr2O12 Solid-State Li-Ion Battery Electrolytes","authors":"Nikolai Helth Gaukås,&nbsp;Tor Olav Sunde,&nbsp;Bjørnar Arstad,&nbsp;Anita Hamar Reksten,&nbsp;Elena Stefan,&nbsp;Annett Thøgersen,&nbsp;Madeeha Khalid Pedersen,&nbsp;Truls Norby and Yngve Larring*,&nbsp;","doi":"10.1021/acsaem.4c0270810.1021/acsaem.4c02708","DOIUrl":"https://doi.org/10.1021/acsaem.4c02708https://doi.org/10.1021/acsaem.4c02708","url":null,"abstract":"<p >Solid-state Li-ion conductors based on cubic Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO) garnets have received much attention in recent years as potential next-generation battery electrolytes, enabling safer and more energy-dense Li-ion batteries. Aliovalent doping of the LLZO structure is usually necessary to stabilize the cubic garnet phase and increase the ionic conductivity by increasing the concentration of Li vacancies. Here, we report on the synthesis, characterization, and testing of Li<sub>7–3<i>x</i></sub>Al<sub><i>x</i></sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> ceramics with different amounts of Al doping (<i>x</i> = 0.20–0.40). Phase-pure LLZO with a cubic crystal structure was prepared by an aqueous synthesis route, and dense (&gt;93%) ceramic samples were fabricated by conventional sintering at 1200 °C. By analyzing the composition, microstructure, and electrochemical performance, we found that the optimal Al content in LLZO is <i>x</i> = 0.2, the lowest content needed to stabilize the cubic structure in our series. For the composition with <i>x</i> = 0.2, we found a Li-ion conductivity at room temperature of 3.7 × 10<sup>–4</sup> S cm<sup>–1</sup> and an activation energy of <i>E</i><sub>a</sub> = 0.3 eV. At a higher doping concentration, the conductivity decreases, and the activation energy increases; for <i>x</i> ≥ 0.35, secondary Al-rich phases appear. These results indicate an inverse relationship between Li-ion conductivity and Al doping, where the optimal amount of doping is the minimum amount necessary to stabilize the cubic LLZO phase. Additionally, we present an analysis of the available literature on chemical modification of LLZO to compare how different doping strategies affect Li conductivity. Based on our literature review, Ga and Ta doping gives the highest conductivities (≤2 × 10<sup>–3</sup> S cm<sup>–1</sup>). The literature analysis also supports our findings that the primary objective of the dopant is to stabilize the cubic structure rather than create Li vacancies.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"7 24","pages":"12141–12154 12141–12154"},"PeriodicalIF":5.4,"publicationDate":"2024-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsaem.4c02708","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874961","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}
引用次数: 0
Impact of Bromine Complexing Agents and Battery Construction on Hydrogen–Bromine Redox Flow Battery Performance
IF 5.4 3区 材料科学
ACS Applied Energy Materials Pub Date : 2024-12-07 DOI: 10.1021/acsaem.4c0213610.1021/acsaem.4c02136
Jingwen Zhang, Shiming Qiu*, Yinghong Wu*, Yifan Liu, Guangzhi Hu, Qian Liu, Jun Luo and Xijun Liu*, 
{"title":"Impact of Bromine Complexing Agents and Battery Construction on Hydrogen–Bromine Redox Flow Battery Performance","authors":"Jingwen Zhang,&nbsp;Shiming Qiu*,&nbsp;Yinghong Wu*,&nbsp;Yifan Liu,&nbsp;Guangzhi Hu,&nbsp;Qian Liu,&nbsp;Jun Luo and Xijun Liu*,&nbsp;","doi":"10.1021/acsaem.4c0213610.1021/acsaem.4c02136","DOIUrl":"https://doi.org/10.1021/acsaem.4c02136https://doi.org/10.1021/acsaem.4c02136","url":null,"abstract":"<p >Hydrogen–bromine redox flow batteries (HBFBs) offer significant advantages in energy storage, including high energy capacity, efficient round-trip conversion, and low cost, positioning them as optimal solutions for grid applications. However, HBFBs are susceptible to issues such as self-discharge, the bromine shuttle effect, high Br<sub>2</sub> vapor pressure, poisoning, and corrosion. Bromine complexing agents (BCAs) have been employed to mitigate these challenges, albeit with drawbacks such as reduced electrolyte conductivity, catalyst site blockage, and diffusion limitation. This review explores the impact of BCAs on the performance of HBFBs, focusing on cell structures such as electrolytes, membranes, and electrodes. Recent research progress in membrane materials and Pt catalysts is summarized to address these issues, and future prospects and challenges for high-performance HBFBs development are discussed.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"7 24","pages":"11652–11664 11652–11664"},"PeriodicalIF":5.4,"publicationDate":"2024-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142870103","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}
引用次数: 0
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