Pub Date : 2024-11-13DOI: 10.1016/j.cej.2024.157449
Juan Ramírez, Levi Peene, Maike Baltussen, Kay Buist, Johannes A.M. (Hans) Kuipers
Riser reactors are frequently applied in the process industry for highly important catalytic processes. In this work, a computational fluid dynamics- discrete element method (CFD-DEM) for a riser with liquid injection was developed. This model treats the gas as a continuous phase whereas the liquid droplets and catalyst particles are treated as discrete elements. The presence of droplets causes particles to be wet, which is taken into account via coverage models of the particles. In addition, the liquid on the particles will change the collision behavior, which is included using an energy balance approach. This CFD-DEM study is conducted simulating a lab-scale pseudo-2D riser. Based on the comparison, the assumption of fully covered particles results in a significant increase in the solids holdup and clustering behavior of the riser which, especially at the low liquid flow rate, results in an over-prediction. The partial coverage simulations show that only half of the particles are covered, which has a major effect on the collisions.
{"title":"Three-phase CFD-DEM study on the hydrodynamics of a riser system with liquid injection","authors":"Juan Ramírez, Levi Peene, Maike Baltussen, Kay Buist, Johannes A.M. (Hans) Kuipers","doi":"10.1016/j.cej.2024.157449","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157449","url":null,"abstract":"Riser reactors are frequently applied in the process industry for highly important catalytic processes. In this work, a computational fluid dynamics- discrete element method (CFD-DEM) for a riser with liquid injection was developed. This model treats the gas as a continuous phase whereas the liquid droplets and catalyst particles are treated as discrete elements. The presence of droplets causes particles to be wet, which is taken into account via coverage models of the particles. In addition, the liquid on the particles will change the collision behavior, which is included using an energy balance approach. This CFD-DEM study is conducted simulating a lab-scale pseudo-2D riser. Based on the comparison, the assumption of fully covered particles results in a significant increase in the solids holdup and clustering behavior of the riser which, especially at the low liquid flow rate, results in an over-prediction. The partial coverage simulations show that only half of the particles are covered, which has a major effect on the collisions.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"7 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601625","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mei Cui, Zishuo Jin, Yingzhe Wang, Jiwei Jiang, Sisi Peng, Qiang Wei, Shuting Zhang, Qingzhang Tuo, Junchao Xie, Haixia Leng, Hongxing Wang, Yanxin Zhao, Peng Lei, Jun Xu, Kai Wang, Junjian Zhang, Yanfeng Jiang, Ding Ding, Fang Xie, Jintai Yu, Qiang Dong
Vascular cognitive impairment (VCI) is highly heterogeneous, with unclear pathogenesis. Individuals with vascular risk factors (VRF), cerebral small vessel disease (CSVD), and stroke are all at risk of developing VCI. To address the growing challenges posed by VCI, the “Vascular, Imaging and Cognition Association of China” (VICA) was established.
{"title":"Imaging, biomarkers, and vascular cognitive impairment in China: Rationale and design for the VICA study","authors":"Mei Cui, Zishuo Jin, Yingzhe Wang, Jiwei Jiang, Sisi Peng, Qiang Wei, Shuting Zhang, Qingzhang Tuo, Junchao Xie, Haixia Leng, Hongxing Wang, Yanxin Zhao, Peng Lei, Jun Xu, Kai Wang, Junjian Zhang, Yanfeng Jiang, Ding Ding, Fang Xie, Jintai Yu, Qiang Dong","doi":"10.1002/alz.14352","DOIUrl":"https://doi.org/10.1002/alz.14352","url":null,"abstract":"Vascular cognitive impairment (VCI) is highly heterogeneous, with unclear pathogenesis. Individuals with vascular risk factors (VRF), cerebral small vessel disease (CSVD), and stroke are all at risk of developing VCI. To address the growing challenges posed by VCI, the “Vascular, Imaging and Cognition Association of China” (VICA) was established.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"10 1","pages":""},"PeriodicalIF":14.0,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601248","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Eun Hye Lee, Sung Hoon Kang, Daeun Shin, Young Ju Kim, Henrik Zetterberg, Kaj Blennow, Fernando Gonzalez-Ortiz, Nicholas J. Ashton, Bo Kyoung Cheon, Heejin Yoo, Hongki Ham, Jihwan Yun, Jun Pyo Kim, Hee Jin Kim, Duk L. Na, Hyemin Jang, Sang Won Seo
We aimed to investigate which factors affect plasma biomarker levels via amyloid beta (Aβ)-independent or Aβ-dependent effects and improve the predictive performance of these biomarkers for Aβ positivity on positron emission tomography (PET).
{"title":"Plasma Alzheimer's disease biomarker variability: Amyloid-independent and amyloid-dependent factors","authors":"Eun Hye Lee, Sung Hoon Kang, Daeun Shin, Young Ju Kim, Henrik Zetterberg, Kaj Blennow, Fernando Gonzalez-Ortiz, Nicholas J. Ashton, Bo Kyoung Cheon, Heejin Yoo, Hongki Ham, Jihwan Yun, Jun Pyo Kim, Hee Jin Kim, Duk L. Na, Hyemin Jang, Sang Won Seo","doi":"10.1002/alz.14368","DOIUrl":"https://doi.org/10.1002/alz.14368","url":null,"abstract":"We aimed to investigate which factors affect plasma biomarker levels via amyloid beta (Aβ)-independent or Aβ-dependent effects and improve the predictive performance of these biomarkers for Aβ positivity on positron emission tomography (PET).","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"159 1","pages":""},"PeriodicalIF":14.0,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601249","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
NiCr-LDH and its partial selenization as Ni0.85Se@NiCr-LDH heterostructure is established here as an alkaline water electrolyzer for achieving enhanced overall water splitting efficiency. The hydrothermally synthesized optimized batch of Ni0.85Se@NiCr-LDH is thoroughly characterized to elucidate its structure, morphology, and composition. Compared to pristine NiCr-LDH, the batch of Ni0.85Se@NiCr-LDH exhibits exceptional alkaline OER and HER activity with low overpotentials of 258 and 85 mV at 10 mA cm−2, respectively. Besides, Ni0.85Se@NiCr-LDH also exhibits excellent acidic HER with an overpotential of only 61 mV at 10 mA cm−2, indicating that Ni0.85Se@NiCr-LDH can operate effectively across a wide pH range. The excellent electrochemical stability of Ni0.85Se@NiCr-LDH for 24 h operation is attributed to the formation of a thin layer of SeOx during OER operation. The role of selenization and the effect of Cr in the LDH lattice toward enhanced electrocatalytic water splitting is discussed. The outstanding OER and HER performances of Ni0.85Se@NiCr-LDH are attributed to the higher electrochemical active surface area, favorable conditions for adsorption of HER/OER intermediates, low charge transfer resistance, and improved conductivity. The practical application of Ni0.85Se@NiCr-LDH as a bifunctional electrocatalyst for overall water splitting is reflected from the low cell voltage of 1.548 V at 10 mA cm−2.
本文将镍铬-LDH 及其部分硒化为 Ni0.85Se@NiCr-LDH 异质结构作为碱性水电解槽,以实现更高的整体水分离效率。通过对水热合成的优化批次 Ni0.85Se@NiCr-LDH 进行全面表征,阐明了其结构、形态和组成。与原始 NiCr-LDH 相比,该批 Ni0.85Se@NiCr-LDH 表现出优异的碱性 OER 和 HER 活性,在 10 mA cm-2 条件下,过电位分别为 258 和 85 mV。此外,Ni0.85Se@NiCr-LDH 还表现出优异的酸性 HER 性能,在 10 mA cm-2 时过电位仅为 61 mV,这表明 Ni0.85Se@NiCr-LDH 可以在很宽的 pH 值范围内有效工作。Ni0.85Se@NiCr-LDH 可在 24 小时内保持极佳的电化学稳定性,这归功于在 OER 运行过程中形成了一层薄薄的 SeOx。讨论了硒化的作用和 LDH 晶格中铬对增强电催化水分离的影响。Ni0.85Se@NiCr-LDH 杰出的 OER 和 HER 性能归功于其较高的电化学活性表面积、HER/OER 中间体的有利吸附条件、较低的电荷转移电阻和较高的电导率。Ni0.85Se@NiCr-LDH 作为一种用于整体水分离的双功能电催化剂,在 10 mA cm-2 时的电池电压低至 1.548 V,这反映了它的实际应用价值。
{"title":"Partial Selenization Strategy for Fabrication of Ni0.85Se@NiCr-LDH Heterostructure as an Efficient Bifunctional Electrocatalyst for Overall Water Splitting","authors":"Nitika, R.K. Dutta","doi":"10.1002/smll.202407538","DOIUrl":"https://doi.org/10.1002/smll.202407538","url":null,"abstract":"NiCr-LDH and its partial selenization as Ni<sub>0.85</sub>Se@NiCr-LDH heterostructure is established here as an alkaline water electrolyzer for achieving enhanced overall water splitting efficiency. The hydrothermally synthesized optimized batch of Ni<sub>0.85</sub>Se@NiCr-LDH is thoroughly characterized to elucidate its structure, morphology, and composition. Compared to pristine NiCr-LDH, the batch of Ni<sub>0.85</sub>Se@NiCr-LDH exhibits exceptional alkaline OER and HER activity with low overpotentials of 258 and 85 mV at 10 mA cm<sup>−2</sup>, respectively. Besides, Ni<sub>0.85</sub>Se@NiCr-LDH also exhibits excellent acidic HER with an overpotential of only 61 mV at 10 mA cm<sup>−2</sup>, indicating that Ni<sub>0.85</sub>Se@NiCr-LDH can operate effectively across a wide pH range. The excellent electrochemical stability of Ni<sub>0.85</sub>Se@NiCr-LDH for 24 h operation is attributed to the formation of a thin layer of SeO<sub>x</sub> during OER operation. The role of selenization and the effect of Cr in the LDH lattice toward enhanced electrocatalytic water splitting is discussed. The outstanding OER and HER performances of Ni<sub>0.85</sub>Se@NiCr-LDH are attributed to the higher electrochemical active surface area, favorable conditions for adsorption of HER/OER intermediates, low charge transfer resistance, and improved conductivity. The practical application of Ni<sub>0.85</sub>Se@NiCr-LDH as a bifunctional electrocatalyst for overall water splitting is reflected from the low cell voltage of 1.548 V at 10 mA cm<sup>−2</sup>.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"216 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610450","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-13DOI: 10.1016/j.cej.2024.157657
Haya Khan, V.M. Rajesh, Mahesh K. Ravva, Subhabrata Sen
Herein, we demonstrated the optimization of a blue LED (450 nm) induced C-C bond formation between various aryl and heteroaryl aldehydes with 1,4-quinones at room temperature in ethyl acetate using Design of Experiments (DoE). This reaction was conducted within a flow (micro and milli-fluidic) device using a millifluidic meandering channel reactor (MC2), resulting in a library of diversely substituted diaryl ketones with moderate to good yields. Control experiments and density functional theory (DFT) based computational investigations were performed to elucidate the reaction mechanism.
{"title":"Optimization of blue LED photo-flow synthesis in continuous flow reactors using design of experiments (DoE): Efficient synthesis of diverse diaryl ketones","authors":"Haya Khan, V.M. Rajesh, Mahesh K. Ravva, Subhabrata Sen","doi":"10.1016/j.cej.2024.157657","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157657","url":null,"abstract":"Herein, we demonstrated the optimization of a blue LED (450 nm) induced C-C bond formation between various aryl and heteroaryl aldehydes with 1,4-quinones at room temperature in ethyl acetate using Design of Experiments (DoE). This reaction was conducted within a flow (micro and milli-fluidic) device using a millifluidic meandering channel reactor (MC2), resulting in a library of diversely substituted diaryl ketones with moderate to good yields. Control experiments and density functional theory (DFT) based computational investigations were performed to elucidate the reaction mechanism.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"19 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601408","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jiankang Li, Raju Chetty, Zihang Liu, Weihong Gao, Takao Mori
The n-type Mg3(Sb, Bi)2 compounds show great potential for wasted heat energy harvesting due to their promising thermoelectric properties. This work discovers that doping transition element Ag into the n-type Mg3(Sb, Bi)2 can effectively optimize the power factor and suppress the lattice thermal conductivity simultaneously. Interestingly, the Ag doping has different effects compared to the isoelectronic and same group element Cu addition studied previously. A high power factor of 19.6 µW cm−1 K−2 is obtained at 673 K owing to the increased electrical conductivity. At the same time, the lattice thermal conductivity is reduced to ≈0.5 W m−1 K−1 because of enhanced phonon scattering induced by Ag atoms. These improvements lead to a peak figure of merit (ZT) of 1.64 at 673 K as well as a high average ZT of 1.27 is obtained from 323 K to 673 K. Furthermore, a thermoelectric single leg with a competitive conversion efficiency of ≈11% under a hot-side temperature of 673 K is fabricated successfully. In addition, a 2-pair module composed of n-type Mg3(Sb, Bi)2 alloy and p-type MgAgSb-based compound demonstrates the high conversion efficiency of ≈7.9% at a temperature difference of 277 K, which will significantly upgrade the sustainable energy recycling technology.
n 型 Mg3(Sb,Bi)2 化合物因其良好的热电特性而显示出巨大的废热能量收集潜力。这项研究发现,在 n 型 Mg3(Sb,Bi)2 中掺入过渡元素 Ag 可以有效优化功率因数,同时抑制晶格热导率。有趣的是,与之前研究的等电子和同族元素铜的添加相比,掺杂银具有不同的效果。由于导电率的提高,在 673 K 时获得了 19.6 µW cm-1 K-2 的高功率因数。同时,由于银原子诱导的声子散射增强,晶格热导率降低到≈0.5 W m-1 K-1。这些改进使 673 K 时的峰值功勋值(ZT)达到 1.64,并且在 323 K 至 673 K 期间获得了 1.27 的高平均 ZT。此外,由 n 型 Mg3(Sb,Bi)2 合金和 p 型 MgAgSb 基化合物组成的 2 对模块在 277 K 的温差下实现了≈7.9% 的高转换效率,这将显著提升可持续能源循环利用技术。
{"title":"Enhancing the Thermoelectric Performance of n-Type Mg3Sb2-Based Materials via Ag Doping","authors":"Jiankang Li, Raju Chetty, Zihang Liu, Weihong Gao, Takao Mori","doi":"10.1002/smll.202408059","DOIUrl":"https://doi.org/10.1002/smll.202408059","url":null,"abstract":"The n-type Mg<sub>3</sub>(Sb, Bi)<sub>2</sub> compounds show great potential for wasted heat energy harvesting due to their promising thermoelectric properties. This work discovers that doping transition element Ag into the n-type Mg<sub>3</sub>(Sb, Bi)<sub>2</sub> can effectively optimize the power factor and suppress the lattice thermal conductivity simultaneously. Interestingly, the Ag doping has different effects compared to the isoelectronic and same group element Cu addition studied previously. A high power factor of 19.6 µW cm<sup>−1</sup> K<sup>−2</sup> is obtained at 673 K owing to the increased electrical conductivity. At the same time, the lattice thermal conductivity is reduced to ≈0.5 W m<sup>−1</sup> K<sup>−1</sup> because of enhanced phonon scattering induced by Ag atoms. These improvements lead to a peak figure of merit (<i>ZT</i>) of 1.64 at 673 K as well as a high average <i>ZT</i> of 1.27 is obtained from 323 K to 673 K. Furthermore, a thermoelectric single leg with a competitive conversion efficiency of ≈11% under a hot-side temperature of 673 K is fabricated successfully. In addition, a 2-pair module composed of n-type Mg<sub>3</sub>(Sb, Bi)<sub>2</sub> alloy and p-type MgAgSb-based compound demonstrates the high conversion efficiency of ≈7.9% at a temperature difference of 277 K, which will significantly upgrade the sustainable energy recycling technology.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"20 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601550","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Fatemeh Seifar, Edward J. Fox, Anantharaman Shantaraman, Yue Liu, Eric B. Dammer, Erica Modeste, Duc M. Duong, Luming Yin, Adam N. Trautwig, Qi Guo, Kaiming Xu, Lingyan Ping, Joseph S. Reddy, Mariet Allen, Zachary Quicksall, Laura Heath, Jo Scanlan, Erming Wang, Minghui Wang, Abby Vander Linden, William Poehlman, Xianfeng Chen, Saurabh Baheti, Charlotte Ho, Thuy Nguyen, Geovanna Yepez, Adriana O. Mitchell, Stephanie R. Oatman, Xue Wang, Minerva M. Carrasquillo, Alexi Runnels, Thomas Beach, Geidy E. Serrano, Dennis W. Dickson, Edward B. Lee, Todd E. Golde, Stefan Prokop, Lisa L. Barnes, Bin Zhang, Varham Haroutunian, Marla Gearing, James. J Lah, Philip De Jager, David A Bennett, Anna Greenwood, Nilüfer Ertekin-Taner, Allan I. Levey, Aliza Wingo, Thomas Wingo, Nicholas T. Seyfried
Alzheimer's disease (AD) is the most prevalent neurodegenerative disease, yet our comprehension predominantly relies on studies within non-Hispanic White (NHW) populations. Here we provide an extensive survey of the proteomic landscape of AD across diverse racial/ethnic groups.
{"title":"Large-scale deep proteomic analysis in Alzheimer's disease brain regions across race and ethnicity","authors":"Fatemeh Seifar, Edward J. Fox, Anantharaman Shantaraman, Yue Liu, Eric B. Dammer, Erica Modeste, Duc M. Duong, Luming Yin, Adam N. Trautwig, Qi Guo, Kaiming Xu, Lingyan Ping, Joseph S. Reddy, Mariet Allen, Zachary Quicksall, Laura Heath, Jo Scanlan, Erming Wang, Minghui Wang, Abby Vander Linden, William Poehlman, Xianfeng Chen, Saurabh Baheti, Charlotte Ho, Thuy Nguyen, Geovanna Yepez, Adriana O. Mitchell, Stephanie R. Oatman, Xue Wang, Minerva M. Carrasquillo, Alexi Runnels, Thomas Beach, Geidy E. Serrano, Dennis W. Dickson, Edward B. Lee, Todd E. Golde, Stefan Prokop, Lisa L. Barnes, Bin Zhang, Varham Haroutunian, Marla Gearing, James. J Lah, Philip De Jager, David A Bennett, Anna Greenwood, Nilüfer Ertekin-Taner, Allan I. Levey, Aliza Wingo, Thomas Wingo, Nicholas T. Seyfried","doi":"10.1002/alz.14360","DOIUrl":"https://doi.org/10.1002/alz.14360","url":null,"abstract":"Alzheimer's disease (AD) is the most prevalent neurodegenerative disease, yet our comprehension predominantly relies on studies within non-Hispanic White (NHW) populations. Here we provide an extensive survey of the proteomic landscape of AD across diverse racial/ethnic groups.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"76 1","pages":""},"PeriodicalIF":14.0,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601245","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-13DOI: 10.1016/j.cej.2024.157663
Wenya Lu, He zhao, Razium Ali Soomro, Ning Sun, Bin Xu
Introducing lattice oxygen redox for charge compensation in layered metal oxides is an effective way to develop advanced cathodes for high energy density sodium-ion batteries (SIBs). However, the asymmetry of lattice oxygen oxidation and reduction incurs oxygen release and crystal structure rearrangement, leading to poor reversibility of the charge and discharge process. Herein, a Na2S-assisted sulfuration strategy is firstly proposed to incorporate active sulfur into the crystal lattice of Na0.9Li0.1Zn0.05Ni0.25Mn0.6O2 cathode. The Sulfur anions within the interior lattice participate in the redox process and enhance the integral coordination stability by mitigating undesired excessive oxygen redox, while the exterior sulfur forms a polyanionic layer to protect the particle surface against electrolyte corrosion. The incorporation of an extra redox center efficiently facilitates the increase of the discharge capacity from 159.9 to 179.2 mAh g−1 within the voltage range of 1.5–4.5 V. Moreover, the larger ionic radius of sulfur enlarges the interplanar spacing, thus facilitating Na+ ions transfer, especially at high current density. As a result, the modified cathode exhibits significantly enhanced electrochemical performance, with a capacity retention of 87 % after 100 cycles at 0.2C and an excellent rate capability of 98.0 mAh g−1 at 10 C. Moreover, the assembled Na ion full cell based on a commercial hard carbon anode achieves an impressive capacity of 160.4mAh g−1 at 0.1 C and could cycled steadily for over 100 cycles. The modification of layer oxides via sulfuration strategy provides a promising pathway for the structural design of novel cathodes with superior cycle performance for high-energy-density SIBs applications.
在层状金属氧化物中引入晶格氧氧化还原进行电荷补偿是开发高能量密度钠离子电池(SIB)先进阴极的有效方法。然而,晶格氧氧化和还原的不对称性会造成氧释放和晶体结构重排,导致充放电过程的可逆性差。本文首次提出了一种 Na2S 辅助硫化策略,在 Na0.9Li0.1Zn0.05Ni0.25Mn0.6O2 阴极的晶格中加入活性硫。内部晶格中的硫阴离子参与氧化还原过程,并通过减轻不希望出现的过量氧氧化还原作用来增强整体配位稳定性,而外部硫则形成一个多阴离子层,保护颗粒表面免受电解质腐蚀。额外氧化还原中心的加入有效地促进了放电容量在 1.5-4.5 V 电压范围内从 159.9 mAh g-1 增加到 179.2 mAh g-1。此外,较大的硫离子半径扩大了平面间距,从而促进了 Na+ 离子的转移,尤其是在高电流密度下。因此,改性阴极的电化学性能显著增强,在 0.2 摄氏度条件下循环 100 次后,容量保持率为 87%,在 10 摄氏度条件下,具有 98.0 mAh g-1 的出色速率能力。此外,基于商用硬碳阳极组装的 Na 离子全电池在 0.1 摄氏度时可达到 160.4mAh g-1 的惊人容量,并可稳定循环 100 次以上。通过硫化策略对层氧化物进行改性,为新型阴极的结构设计提供了一条前景广阔的途径,这种阴极具有卓越的循环性能,可用于高能量密度 SIBs 应用。
{"title":"Lattice sulfuration enhanced sodium storage performance of Na0.9Li0.1Zn0.05Ni0.25Mn0.6O2 cathode","authors":"Wenya Lu, He zhao, Razium Ali Soomro, Ning Sun, Bin Xu","doi":"10.1016/j.cej.2024.157663","DOIUrl":"https://doi.org/10.1016/j.cej.2024.157663","url":null,"abstract":"Introducing lattice oxygen redox for charge compensation in layered metal oxides is an effective way to develop advanced cathodes for high energy density sodium-ion batteries (SIBs). However, the asymmetry of lattice oxygen oxidation and reduction incurs oxygen release and crystal structure rearrangement, leading to poor reversibility of the charge and discharge process. Herein, a Na<sub>2</sub>S-assisted sulfuration strategy is firstly proposed to incorporate active sulfur into the crystal lattice of Na<sub>0.9</sub>Li<sub>0.1</sub>Zn<sub>0.05</sub>Ni<sub>0.25</sub>Mn<sub>0.6</sub>O<sub>2</sub> cathode. The Sulfur anions within the interior lattice participate in the redox process and enhance the integral coordination stability by mitigating undesired excessive oxygen redox, while the exterior sulfur forms a polyanionic layer to protect the particle surface against electrolyte corrosion. The incorporation of an extra redox center efficiently facilitates the increase of the discharge capacity from 159.9 to 179.2 mAh g<sup>−1</sup> within the voltage range of 1.5–4.5 V. Moreover, the larger ionic radius of sulfur enlarges the interplanar spacing, thus facilitating Na<sup>+</sup> ions transfer, especially at high current density. As a result, the modified cathode exhibits significantly enhanced electrochemical performance, with a capacity retention of 87 % after 100 cycles at 0.2C and an excellent rate capability of 98.0 mAh g<sup>−1</sup> at 10 C. Moreover, the assembled Na ion full cell based on a commercial hard carbon anode achieves an impressive capacity of 160.4mAh g<sup>−1</sup> at 0.1 C and could cycled steadily for over 100 cycles. The modification of layer oxides via sulfuration strategy provides a promising pathway for the structural design of novel cathodes with superior cycle performance for high-energy-density SIBs applications.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"48 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601620","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Randy Burns, Dylan Chiaro, Harrison Davison, Christopher J. Arendse, Gavin M. King, Suchismita Guha
Halide perovskites are hailed as semiconductors of the 21st century. Chemical vapor deposition (CVD), a solvent-free method, allows versatility in the growth of thin films of 3- and 2D organic–inorganic halide perovskites. Using CVD grown methylammonium lead iodide (MAPbI3) films as a prototype, the impact of electron beam dosage under cryogenic conditions is evaluated. With 5 kV accelerating voltage, the dosage is varied between 50 and 50000 µC cm−2. An optimum dosage of 35 000 µC cm−2 results in a significant blue shift and enhancement of the photoluminescence peak. Concomitantly, a strong increase in the photocurrent is observed. A similar electron beam treatment on chlorine incorporated MAPbI3, where chlorine is known to passivate defects, shows a blue shift in the photoluminescence without improving the photocurrent properties. Low electron beam dosage under cryogenic conditions is found to damage CVD grown 2D phenylethlyammoinum lead iodide films. Monte Carlo simulations reveal differences in electron beam interaction with 3- and 2D halide perovskite films.
{"title":"Stabilizing Metal Halide Perovskite Films via Chemical Vapor Deposition and Cryogenic Electron Beam Patterning","authors":"Randy Burns, Dylan Chiaro, Harrison Davison, Christopher J. Arendse, Gavin M. King, Suchismita Guha","doi":"10.1002/smll.202406815","DOIUrl":"https://doi.org/10.1002/smll.202406815","url":null,"abstract":"Halide perovskites are hailed as semiconductors of the 21<sup>st</sup> century. Chemical vapor deposition (CVD), a solvent-free method, allows versatility in the growth of thin films of 3- and 2D organic–inorganic halide perovskites. Using CVD grown methylammonium lead iodide (MAPbI<sub>3</sub>) films as a prototype, the impact of electron beam dosage under cryogenic conditions is evaluated. With 5 kV accelerating voltage, the dosage is varied between 50 and 50000 µC cm<sup>−2</sup>. An optimum dosage of 35 000 µC cm<sup>−2</sup> results in a significant blue shift and enhancement of the photoluminescence peak. Concomitantly, a strong increase in the photocurrent is observed. A similar electron beam treatment on chlorine incorporated MAPbI<sub>3</sub>, where chlorine is known to passivate defects, shows a blue shift in the photoluminescence without improving the photocurrent properties. Low electron beam dosage under cryogenic conditions is found to damage CVD grown 2D phenylethlyammoinum lead iodide films. Monte Carlo simulations reveal differences in electron beam interaction with 3- and 2D halide perovskite films.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"10 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610447","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Anna H. Boerwinkle, Julie K. Wisch, Benjamin L. Handen, Elizabeth Head, Mark Mapstone, Michael S. Rafii, Sid E. O'Bryant, Sharon J. Krinsky-McHale, Florence Lai, H. Diana Rosas, Shahid Zaman, Ira T. Lott, Dana Tudorascu, Matthew Zammit, Adam M. Brickman, Joseph H. Lee, Beau M. Ances
Development of Alzheimer's disease (AD) pathology in Down's syndrome (DS) occurs within a compressed timeline compared to sporadic or other genetic forms of AD.
{"title":"The mediating role of plasma glial fibrillary acidic protein in amyloid and tau pathology in Down's syndrome","authors":"Anna H. Boerwinkle, Julie K. Wisch, Benjamin L. Handen, Elizabeth Head, Mark Mapstone, Michael S. Rafii, Sid E. O'Bryant, Sharon J. Krinsky-McHale, Florence Lai, H. Diana Rosas, Shahid Zaman, Ira T. Lott, Dana Tudorascu, Matthew Zammit, Adam M. Brickman, Joseph H. Lee, Beau M. Ances","doi":"10.1002/alz.14359","DOIUrl":"https://doi.org/10.1002/alz.14359","url":null,"abstract":"Development of Alzheimer's disease (AD) pathology in Down's syndrome (DS) occurs within a compressed timeline compared to sporadic or other genetic forms of AD.","PeriodicalId":13,"journal":{"name":"ACS Chemical Neuroscience","volume":"95 1","pages":""},"PeriodicalIF":14.0,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601252","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}