ACS Materials Letters最新文献_第5页

Role of Anharmonic Effects on the Phase Stability of VNbMoTaW High-Entropy Alloy from Ab Initio Analysis

IF 9.6 1区化学

ACS Materials Letters Pub Date : 2024-10-29 DOI: 10.1021/acsmaterialslett.4c0172510.1021/acsmaterialslett.4c01725

Chao Cheng, and , Xin Zhang*,

引用次数: 0

Trace Rh Activates Surface Ni with Increased Local Charge for Efficient pH-Universal Hydrogen Generation 痕量 Rh 激活表面镍，增加局部电荷，实现高效的 pH 值万能制氢

IF 19.3 1区化学

ACS Materials Letters Pub Date : 2024-10-28 DOI: 10.1021/acsenergylett.4c0265010.1021/acsenergylett.4c02650

Minmin Cai, Qian Zhu, Xiangyan Hou, Lu Yao, Yuan Zhang, Xiaofeng Wu, Xiangdong Yao*, Hao Chen, Yi Jia*, Shouhua Feng and Keke Huang*,

{"title":"Trace Rh Activates Surface Ni with Increased Local Charge for Efficient pH-Universal Hydrogen Generation","authors":"Minmin Cai, Qian Zhu, Xiangyan Hou, Lu Yao, Yuan Zhang, Xiaofeng Wu, Xiangdong Yao*, Hao Chen, Yi Jia*, Shouhua Feng and Keke Huang*, ","doi":"10.1021/acsenergylett.4c0265010.1021/acsenergylett.4c02650","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02650https://doi.org/10.1021/acsenergylett.4c02650","url":null,"abstract":"The unbefitting binding energy for H*/OH* with Ni sites greatly restrains the electrochemical activity of Ni for the hydrogen evolution reaction (HER). Herein, Ni nanograins incorporated with trace Rh (denoted as 3D RhNi) are synthesized through combining a facile ion-absorption and subsequent thermal reduction treatment, in which Rh increases the local charge density of Ni sites, dramatically accelerating the electrochemical kinetics of HER. Experimentally, the Rh–Ni catalyst with only 0.1 at. % Rh element exhibits superior HER activity among the reported Ni-based materials, whose overpotential is only 37 mV and 18 mV at 10 mA/cm2 in 1.0 M KOH and 0.5 M H2SO4, respectively. DFT calculations further identify that the resultant catalyst possesses appropriate intermediate binding energy in both acidic and alkaline conditions toward HER. This study provides a strategy to manipulate the local electronic structure for significantly improving the activity in surface catalysis.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 11","pages":"5587–5595 5587–5595"},"PeriodicalIF":19.3,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608873","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Comparative Analysis of Reactivity of Al and Ga Doped Garnet Solid State Electrolyte at the Interface with Li Metal

IF 9.6 1区化学

ACS Materials Letters Pub Date : 2024-10-28 DOI: 10.1021/acsmaterialslett.4c0123710.1021/acsmaterialslett.4c01237

Matthew Klenk, Neelima Paul, Michael J. Counihan, Zachary D. Hood, Yisi Zhu, Justin G. Connell, Charles Hervoches, Ralph Gilles, Jeff Sakamoto, Sanja Tepavcevic* and Peter Zapol*,

{"title":"Comparative Analysis of Reactivity of Al and Ga Doped Garnet Solid State Electrolyte at the Interface with Li Metal","authors":"Matthew Klenk, Neelima Paul, Michael J. Counihan, Zachary D. Hood, Yisi Zhu, Justin G. Connell, Charles Hervoches, Ralph Gilles, Jeff Sakamoto, Sanja Tepavcevic* and Peter Zapol*, ","doi":"10.1021/acsmaterialslett.4c0123710.1021/acsmaterialslett.4c01237","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01237https://doi.org/10.1021/acsmaterialslett.4c01237","url":null,"abstract":"Lithium garnet (Li7La3Zr2O12, LLZO) based solid electrolytes are leading candidate materials for all-solid-state batteries with lithium metal anodes because of their high ionic conductivity, high mechanical toughness, and superior electrochemical stability. While doping LLZO with Al and Ga increases its ionic conductivity by stabilizing the cubic phase, the impact of dopants on its (electro)chemical stability at the interfaces with Li metal is critical. Our study of differences between Al- and Ga-doped LLZO when interfaced with lithium metal using X-ray photoelectron spectroscopy and density functional theory shows a higher propensity of Ga to move across LLZO interface with Li metal and form Ga–Li alloy. Neutron diffraction reveals loss of cubic phase resulting from the loss of dopant that explains electrochemical behavior differences between Ga- and Al-doped LLZO. Overall, our study reveals the key role of dopant chemistry in enabling stable solid electrolyte materials for all-solid-state batteries.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"6 12","pages":"5216–5221 5216–5221"},"PeriodicalIF":9.6,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142756487","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Asymmetric Bipolar Membrane for High Current Density Electrodialysis Operation with Exceptional Stability 用于高电流密度电渗析操作的非对称双极膜，稳定性极佳

IF 19.3 1区化学

ACS Materials Letters Pub Date : 2024-10-28 DOI: 10.1021/acsenergylett.4c0166210.1021/acsenergylett.4c01662

Éowyn Lucas, Justin C. Bui, Timothy Nathan Stovall, Monica Hwang, Kaiwen Wang, Emily R. Dunn, Ellis Spickermann, Lily Shiau, Ahmet Kusoglu, Adam Z. Weber, Alexis T. Bell, Shane Ardo, Harry A. Atwater* and Chengxiang Xiang*,

{"title":"Asymmetric Bipolar Membrane for High Current Density Electrodialysis Operation with Exceptional Stability","authors":"Éowyn Lucas, Justin C. Bui, Timothy Nathan Stovall, Monica Hwang, Kaiwen Wang, Emily R. Dunn, Ellis Spickermann, Lily Shiau, Ahmet Kusoglu, Adam Z. Weber, Alexis T. Bell, Shane Ardo, Harry A. Atwater* and Chengxiang Xiang*, ","doi":"10.1021/acsenergylett.4c0166210.1021/acsenergylett.4c01662","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01662https://doi.org/10.1021/acsenergylett.4c01662","url":null,"abstract":"Bipolar membranes (BPMs) enable isolated acidic/alkaline regions in electrochemical devices, facilitating optimized environments for electrochemical separations and catalysis. For economic viability, BPMs must attain stable, high current density operation with low overpotentials in a freestanding configuration. We report an asymmetric, graphene oxide (GrOx)-catalyzed BPM capable of freestanding electrodialysis operation at 1 A cm–2 with overpotentials <250 mV. Use of a thin anion-exchange layer improves water transport while maintaining near unity Faradaic efficiency for acid and base generation. Voltage stability exceeding 1100 h with an average drift of 70 μV/h at 80 mA cm–2 and 100 h with an average drift of −300 μV/h at 500 mA cm–2 and implementation in an electrodialysis stack demonstrate real-world applicability. Continuum modeling reveals that water dissociation in GrOx BPMs is both catalyzed and electric-field enhanced, where low pKa moieties on GrOx enhance local electric fields and high pKa moieties serve as active sites for surface-catalyzed water dissociation. These results establish commercially viable BPM electrodialysis and provide fundamental insight to advance design of next-generation devices.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 11","pages":"5596–5605 5596–5605"},"PeriodicalIF":19.3,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608858","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Practical Lithium–Sulfur Batteries: Beyond the Conventional Electrolyte Concentration 实用锂硫电池：超越传统的电解质浓度

IF 19.3 1区化学

ACS Materials Letters Pub Date : 2024-10-26 DOI: 10.1021/acsenergylett.4c0253510.1021/acsenergylett.4c02535

Xiaosheng Song, Xinghui Liang, Hun Kim and Yang-Kook Sun*,

{"title":"Practical Lithium–Sulfur Batteries: Beyond the Conventional Electrolyte Concentration","authors":"Xiaosheng Song, Xinghui Liang, Hun Kim and Yang-Kook Sun*, ","doi":"10.1021/acsenergylett.4c0253510.1021/acsenergylett.4c02535","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02535https://doi.org/10.1021/acsenergylett.4c02535","url":null,"abstract":"Advances in electrolyte chemistry and the development of electrolyte systems have revealed that electrolyte concentration significantly affects battery performance. However, the relationship between electrolyte concentration, polysulfide formation, and lithium–sulfur (Li–S) battery performance remains unclear, which hinders the developmental progress of practical Li–S batteries. In this study, we compared the electrolyte structures and performance of Li–S batteries with various electrolyte concentrations and developed a method that links microscopic interactions, apparent electrolyte parameters, and battery performance. The relationship between polysulfides and the electrolyte system was analyzed at various concentrations, which revealed that systems with a low lithium-salt concentration, especially below 1 M, are better suited to practical Li–S batteries and that polysulfides play crucial roles in ion-transport processes under practical conditions. This study supports the development of electrolytes for practical Li–S batteries and provides guidance for controlling ion-transport processes in liquid electrolytes for other secondary batteries.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 11","pages":"5576–5586 5576–5586"},"PeriodicalIF":19.3,"publicationDate":"2024-10-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608851","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Correction to “Bioorthogonal Nanosystem for Near-Infrared Fluorescence Imaging and Prodrug Activation in Mouse Model”

IF 9.6 1区化学

ACS Materials Letters Pub Date : 2024-10-25 DOI: 10.1021/acsmaterialslett.4c0210210.1021/acsmaterialslett.4c02102

Xin Xie, Bowen Li, Jie Wang, Chenyue Zhan, Yong Huang, Fang Zeng* and Shuizhu Wu*,

引用次数: 0

Solving the Residual Lithium Problem by Substoichiometric Synthesis of Layered Ni-Rich Oxide Cathodes 通过亚计量合成层状富镍氧化物阴极解决残锂问题

IF 19.3 1区化学

ACS Materials Letters Pub Date : 2024-10-25 DOI: 10.1021/acsenergylett.4c0256710.1021/acsenergylett.4c02567

Leonhard Karger, Rui Yao, Karsten Seidel, Barbara Nascimento Nunes, Ananyo Roy, Ruizhuo Zhang, Jürgen Janek, Aleksandr Kondrakov* and Torsten Brezesinski*,

引用次数: 0

Insights from Techno-Economic Analysis Can Guide the Design of Low-Temperature CO2 Electrolyzers toward Industrial Scaleup 技术经济分析的启示可指导低温二氧化碳电解槽的设计实现工业放大

IF 19.3 1区化学

ACS Materials Letters Pub Date : 2024-10-25 DOI: 10.1021/acsenergylett.4c0264710.1021/acsenergylett.4c02647

Shashwati C. da Cunha, and , Joaquin Resasco*,

{"title":"Insights from Techno-Economic Analysis Can Guide the Design of Low-Temperature CO2 Electrolyzers toward Industrial Scaleup","authors":"Shashwati C. da Cunha,  and , Joaquin Resasco*, ","doi":"10.1021/acsenergylett.4c0264710.1021/acsenergylett.4c02647","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02647https://doi.org/10.1021/acsenergylett.4c02647","url":null,"abstract":"The field of CO2 reduction has identified several challenges that must be overcome to realize its immense potential to simultaneously close the carbon cycle, replace fossil-based chemical feedstocks, and store renewable electricity. However, frequently cited research targets were set without quantitatively analyzing their impact on economic viability. Through a physics-informed techno-economic assessment, we offer guidance on top priorities for CO2 reduction. Although separations dominate capital cost, increasing single-pass conversion is unnecessary because it leads to selectivity loss in current membrane electrode assemblies. Decoupling selectivity and single-pass conversion by moving away from a plug flow reactor design would reduce the base case levelized cost from $1.22/kgCO to $0.97/kgCO, as impactful as eliminating CO2R overpotential. Operating at high current densities (>500 mA/cm2) is undesirable unless cell voltages can be lowered. We confirm that levelized product cost is dominated by the cost of electricity to drive electrolysis. Although wholesale wind and solar electricity are cheaper than retail electricity, their capacity factors are too low for economical operation. Adding energy storage to increase the capacity factor of solar electricity triples the capital cost of the process. By updating research priorities based on fundamental electrolyzer behavior, we hope this work accelerates the practical application of CO2 reduction.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 11","pages":"5550–5561 5550–5561"},"PeriodicalIF":19.3,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608671","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Correlation of Dimer-Linker-Induced Conformational Lock with Nonradiative Energy Loss in Organic Solar Cells 有机太阳能电池中二聚体-连接体诱导的构象锁定与非辐射能量损失的相关性

IF 19.3 1区化学

ACS Materials Letters Pub Date : 2024-10-25 DOI: 10.1021/acsenergylett.4c0242910.1021/acsenergylett.4c02429

Huanhuan Gao, Baobing Fan*, Liyang Yu, Yiwen Wang, Ruipeng Li, Wenlin Jiang, Tianqi Chen, Jie Zeng, Francis R. Lin, Bin Kan, Hongxiang Li, Lei Wang and Alex K.-Y. Jen*,

{"title":"Correlation of Dimer-Linker-Induced Conformational Lock with Nonradiative Energy Loss in Organic Solar Cells","authors":"Huanhuan Gao, Baobing Fan*, Liyang Yu, Yiwen Wang, Ruipeng Li, Wenlin Jiang, Tianqi Chen, Jie Zeng, Francis R. Lin, Bin Kan, Hongxiang Li, Lei Wang and Alex K.-Y. Jen*, ","doi":"10.1021/acsenergylett.4c0242910.1021/acsenergylett.4c02429","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02429https://doi.org/10.1021/acsenergylett.4c02429","url":null,"abstract":"The efficiencies of dimer-based devices still lag those of their small molecule-based counterparts. This is primarily due to the considerable dihedrals in the dimer skeleton, which compromises the molecular packing, thus influencing the charge generation and nonradiative voltage loss (ΔVoc,nr). Herein, we developed two dimeric acceptors with varied π-linkers to investigate the influence of linker-induced conformational lock on ΔVoc,nr. We find that the helically lapped O-shaped dimer delivers better intermolecular packing than the planar S-shaped one that incorporates a bulkier π-linker. However, its planar skeleton is instead more favorable for forming a compact and ordered stacking with the host acceptor in ternary blend. This possibly promotes exciton dissociation, thus reducing the nonradiative decay of excited states. Moreover, its longer exciton lifetime could offer additional charge-transfer channels. These contributions effectively minimize ΔVoc,nr to 0.195 eV, while delivering a high efficiency approaching 20% in the derived ternary device.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 11","pages":"5541–5549 5541–5549"},"PeriodicalIF":19.3,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608675","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Impact of Ambient Air Contamination on the Performance of Argyrodite-Based All-Solid-State Lithium–Sulfur Batteries 环境空气污染对基于 Argyrodite 的全固态锂硫电池性能的影响

IF 19.3 1区化学

ACS Materials Letters Pub Date : 2024-10-25 DOI: 10.1021/acsenergylett.4c0188210.1021/acsenergylett.4c01882

Hyunki Sul, and , Arumugam Manthiram*,

{"title":"Impact of Ambient Air Contamination on the Performance of Argyrodite-Based All-Solid-State Lithium–Sulfur Batteries","authors":"Hyunki Sul,  and , Arumugam Manthiram*, ","doi":"10.1021/acsenergylett.4c0188210.1021/acsenergylett.4c01882","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01882https://doi.org/10.1021/acsenergylett.4c01882","url":null,"abstract":"Sulfide-based Li-argyrodites (Li5.5PS4.5Cl1.5) are considered as promising solid-state electrolytes for all-solid-state Li–S batteries (ASSLSBs) due to their high ionic conductivity and suitable mechanical properties. However, their hygroscopic nature and intense decomposition behavior when combined with conductive additives at the sulfur cathode introduce many variables that can affect cell performance. This study demonstrates that an optimized amount of ambient air contamination during cycling can enhance cell performance. Multiple spectroscopic analyses reveal that the hydrolysis of Li5.5PS4.5Cl1.5 can incorporate oxygen into the argyrodite structure, thereby increasing the oxidative stability and generating additional redox active sulfur species. Methods, such as monitoring cell impedance growth, open-circuit voltage changes, and 31P NMR spectroscopic analysis, are proposed to determine the air-tightness of cell configurations. The research findings suggest that verifying the air-tightness of cell configurations is critical for ASSLSBs research to prevent misleading results.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 11","pages":"5562–5572 5562–5572"},"PeriodicalIF":19.3,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608672","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0