HER

家族性巨颌症
  • 文章类型: Journal Article
    创造一种非常稳定和有效的电化学催化剂以实现高效的氢析出是艰巨的,主要是由于Pt的工业利用需要考虑的多种因素。在这项工作中,测试了通过将Pt原位还原到生物多孔二氧化硅(Pt-SiO2)上而形成的杂化物作为制氢的有效催化剂的用途。已经证明了高达200个循环的催化剂具有极高的电催化活性和优异的可重复使用性。具有活性催化位点的低Pt含量为0.48至0.82at%的Pt-SiO2表现出优异的催化活性,Tafel斜率为22mVdec-1,超电势为28mV(与10mAcm-2时的RHE)与Pt线和先前报道的裸Pt-SiO2(Pt的0.65at%和0.48at%)相比,和杂化(Pt/Ag)结构形成在两个不同的生物多孔SiO2基底上。Pt1Ag3团簇的催化机能最好,代表低Pt浓度,已通过密度泛函理论(DFT)计算验证。这里,Pt1Ag3团簇的高产归因于Pt/Ag原子之间的相互协同作用。Pt原子将多余的电荷转移到团簇内最近的Ag邻居,促进氢在活化位点上的扩散。这些重要发现证实了在胺官能化的生物多孔二氧化硅上在降低的Pt浓度下优异的氢气产生。
    The task of creating a remarkably stable and effective electrochemical catalyst for efficient hydrogen evolution is arduous, primarily due to the multitude of factors that need to be taken into account for the industrial utilization of Pt. In this work, hybrid formation through in-situ reduction of Pt onto biogenic porous silica (Pt-SiO2) is tested for its use as an efficient catalyst for hydrogen production. Exceptionally high electrocatalytic activity and excellent reusability of catalysts up to 200 cycles have been demonstrated. Pt-SiO2 with low Pt content of 0.48 to 0.82 at% with active catalytic sites exhibit superior catalytic activity with a Tafel slope of 22 mV dec-1 and an overpotential of 28 mV (vs. RHE at 10 mA cm-2) as compared to the Pt wire and previously reported bare Pt-SiO2 (0.65 at% and 0.48 at% of Pt), and hybrid (Pt/Ag) structures formed onto two different biogenic porous SiO2 substrates. The best catalytic performance of the Pt1Ag3 cluster, representing a low Pt concentration, has been validated by Density Functional Theory (DFT) calculations. Here, the high production from the Pt1Ag3 cluster is assigned to the mutual synergistic effect between Pt/Ag atoms. The Pt atoms transfer the excess charge to the nearest Ag neighbors inside the cluster, facilitating hydrogen diffusion on the activated sites. These important findings authenticate the superior hydrogen production at reduced Pt concentration on amine-functionalized biogenic porous silica.
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  • 文章类型: Journal Article
    背景:先前的研究提供了体内代谢产物与乳腺癌(BC)相关的证据。然而,血液代谢产物与BC之间的因果关系尚不清楚.
    方法:本研究进行了孟德尔双样本综合随机分析,以确定1400个公开的代谢因子遗传数据与人类表皮生长因子受体阳性(HER+)BC或HER-BC之间的因果关系。
    结果:硫酸表雄酮水平(OR=1.07,95%CI=1.02〜1.10,p=0.0013),5α-雄性激素-3β,17β-二醇单硫酸盐(2)水平(OR=1.07,95%CI=1.03~1.12,p=0.0012),糖胆酸水平(OR=0.85,95%CI=0.77〜0.93,p=0.0007)和乙胆醇酮葡糖苷酸水平(OR=1.12,95%CI=1.05〜1.20,p=0.0013)与HERBC有因果关系。5种代谢物与HER-BC有因果关系:香草酸甘氨酸水平(OR=1.14,95%CI=1.06~1.22,p=0.0003),甲状腺素水平(OR=1.26,95%CI=1.11~1.44,p=0.0004),1-棕榈酰-2-亚油酰基-GPI(16:0/18:2)水平(OR=0.86,95%CI=0.79~0.94,p=0.0010),N-乙酰苯丙氨酸水平(OR=1.12,95%CI=1.05~1.19,p=0.0007)和葡萄糖-甘露糖比值(OR=1.15,95%CI=1.06~1.24,p=0.0008)。确定了两种常见的因果关系代谢物:γ-谷氨酰谷氨酸和X-12849水平。
    结论:我们的研究通过遗传手段分别证明了血液代谢产物与HER+或HER-BC之间的联系,从而为治疗目标提供机会。
    BACKGROUND: Previous studies provide evidence that in vivo metabolites are associated with breast cancer (BC). However, the causal relationship between blood metabolites and BC remains unclear.
    METHODS: Comprehensive two-sample Mendelian randomization analysis was conducted to determine the causal association between 1400 publicly available genetic data on metabolic factors and human epidermal growth factor receptor positive (HER+) BC or HER- BC in this study.
    RESULTS: Epiandrosterone sulfate levels (OR = 1.07, 95% CI = 1.02 ~ 1.10, p = 0.0013), 5alpha-androstan-3beta,17beta-diol monosulfate (2) levels (OR = 1.07, 95% CI = 1.03 ~ 1.12, p = 0.0012), glycohyocholate levels (OR = 0.85, 95% CI = 0.77 ~ 0.93, p = 0.0007) and etiocholanolone glucuronide levels (OR = 1.12, 95% CI = 1.05 ~ 1.20, p = 0.0013) were causally correlated with HER+ BC. 5 metabolites were causally correlated with HER- BC: Vanillic acid glycine levels (OR = 1.14, 95% CI = 1.06 ~ 1.22, p = 0.0003), Thyroxine levels (OR = 1.26, 95% CI = 1.11 ~ 1.44, p = 0.0004), 1-palmitoyl-2-linoleoyl-GPI (16:0/18:2) levels (OR = 0.86, 95% CI = 0.79 ~ 0.94, p = 0.0010), N-acetylphenylalanine levels (OR = 1.12, 95% CI = 1.05 ~ 1.19, p = 0.0007) and Glucose-to-mannose ratio (OR = 1.15, 95% CI = 1.06 ~ 1.24, p = 0.0008). Two common causally related metabolites were identified: Gamma-glutamyl glutamate and X-12849 levels.
    CONCLUSIONS: Our study has respectively demonstrated the connection between blood metabolites and HER+ or HER- BC by genetic means, thereby offering opportunities for therapeutic targets.
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  • 文章类型: Journal Article
    在本研究中,通过溶剂热法合成了CdS-rGO-Ag的三元纳米结构,以增强材料的光催化和电催化活性。利用紫外-可见光谱和光致发光(PL)光谱对所制备样品的光学性质进行了表征。观察到CdS-rGO-Ag纳米结构的能隙从2.40±0.08eV(CdS)下降至1.90±0.05,这可能归因于rGO-Ag诱导的在CdS的最高占据分子轨道(HOMO)和最低未占据分子轨道(LUMO)能级之间的陷阱态的产生。观察到的显着PL猝灭也证实了在制备的纳米结构CdS-rGO-Ag中包含陷阱态,表明有效的光活性。CdS-rGO-Ag对亚甲基蓝(MB)染料降解的增强的光催化活性支持了制备的纳米结构的光催化活性。此外,用循环伏安法(CV)研究CdS-rGO-Ag催化剂的光电化学催化活性,线性扫描伏安法(LSV),和电化学阻抗谱(EIS)描绘了改进的电流密度,降低过电位。在光照下电荷转移电阻的减小和光电流密度的增加表明CdS-rGO-Ag具有更好的光电化学性能。
    In the present study, we have synthesized the ternary nanostructure of CdS-rGO-Ag by using the solvothermal method for the enhanced photocatalytic as well as electrocatalytic activity of the material. The optical properties of the prepared samples were characterized by using UV-visible spectroscopy and photoluminescence (PL) spectroscopy. A decline in the energy gap of CdS-rGO-Ag nanostructure to 1.90 ± 0.05 from 2.40 ± 0.08 eV (CdS) is observed and may be attributed due to the rGO-Ag-induced creation of trap states in between the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) levels of CdS. The observed significant PL quenching also confirms the inclusion of trap states in the prepared nanostructure CdS-rGO-Ag, suggesting efficient photoactivity. The enhanced photocatalytic activity of CdS-rGO-Ag for methylene blue (MB) dye degradation supports the photocatalytic activity of prepared nanostructures. Furthermore, the photoelectrochemical catalytic activity of the CdS-rGO-Ag catalyst investigated by using cyclic voltammetry (CV), linear sweep voltammetry (LSV), and electrochemical impedance spectroscopy (EIS) depicts the improved current density, lowering of overpotential. The decrement in charge transfer resistance and enhancement in photocurrent density under light illumination indicates the better photoelectrochemical performance of CdS-rGO-Ag.
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  • 文章类型: Journal Article
    背景:在大流行之前,数字健康只是匈牙利已建立的医疗保健系统的潜在替代方案。该技术是可用的,但没有关于数字健康使用和发展的政府战略。医疗保健数字解决方案的法律框架支离破碎。COVID-19创造了条件,数字解决方案成为最可行的医疗保健提供形式。我们介绍匈牙利政府在大流行期间的立法和决策活动,旨在加强对这些技术的有组织和有系统地使用。
    方法:我们研究中使用的核心方法是使用系统文献综述的原理和方法对立法进行综述。我们搜索了2020年1月31日至2022年6月1日期间数字健康相关立法的国家立法数据库。为分析提供上下文,通过案头研究确定了其他相关文件。
    结果:尽管电子健康记录(EHR)成立于2017年,但仅在大流行爆发后才被广泛使用。匈牙利使用临时紧急状态条例来促进增加远程咨询的次数。我们的搜索确定了7条立法,使医疗保健提供商能够立即使用数字解决方案。他们定义了医疗服务提供者进行远程咨询必须满足的条件,设定可以采取的干预措施,什么可以报销和处理安全问题。2021年7月的国家卫生信息学战略很复杂,但主要涉及技术问题。该战略的三个基本原则是以人为本,数字化转型和综合护理。
    结论:匈牙利数字医疗解决方案和政策在国际比较中表现良好。这是由于大流行期间密集的立法活动。国家健康信息学战略确保在大流行期间实施的数字健康解决方案比COVID-19的寿命更长。
    BACKGROUND: Before the pandemic, digital health was merely a potential alternative to established systems of healthcare provision in Hungary. The technology was available but there was no governmental strategy regarding digital health use and development. The legal framework for digital solutions in healthcare was fragmented. COVID-19 created conditions in which digital solutions became the most feasible form of healthcare provision. We present the legislative and policy-making activities of the Hungarian government during the pandemic aimed at enhancing the organised and systematic use of these technologies.
    METHODS: The core method used in our research is a review of legislation using the principles and methods of a systematic literature review. We searched the National Legislation Database for digital health related legislation for the period January 31, 2020 - June 1, 2022. To provide the context for the analysis, other relevant documents were identified through desk research.
    RESULTS: Although established in 2017, the electronic health records (EHRs) were only widely used after the onset of the pandemic. Hungary used temporary state of emergency regulations to facilitate an increase in the number of teleconsultations. Our search identified 7 pieces of legislation that enabled healthcare providers to put digital solutions to instant use. They defined the conditions healthcare providers must meet for teleconsultations, set what interventions may be done, what can be reimbursed and dealt with security issues. The National Health Informatics Strategy of July 2021 is complex but mainly deals with technical issues. The three basic principles of the strategy are people centeredness, digital transformation and integrated care.
    CONCLUSIONS: Hungarian digital health solutions and policies fare well in international comparison. This is due to the intensive legislative activity of the pandemic period. The National Health Informatics Strategy ensures that the digital health solutions implemented during the pandemic outlive COVID-19.
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  • 文章类型: Journal Article
    高效的发展,稳定,多功能析氢电催化剂具有重要意义,但仍然面临挑战。界面工程和相工程因其独特的物理化学性质在析氢反应(HER)领域得到了广泛的应用。然而,它们通常单独使用,这限制了他们的有效性。在这里,我们提出了一种界面工程的CoMo/CoTe电催化剂,由非晶CoMo(a-CoMo)层封装的晶体CoTe阵列组成,实现催化性能的深刻优化。实验结果和密度泛函理论计算表明,与其晶体-晶体对应物相比,催化剂的d带中心进一步向上移动,优化电子结构和中间吸附,从而降低了HER的动力学障碍。具有超亲水/超氧特性的a-CoMo/CoTe在碱性条件下表现出优异的催化性能,中性,和模拟海水环境。
    The development of efficient, stable, and versatile hydrogen evolution electrocatalysts is of great meaning, but still faces challenging. Interface engineering and phase engineering have been immensely applied in the field of hydrogen evolution reaction (HER) because of their unique physicochemical properties. However, they are typically used separately, which limits their effectiveness. Herein, we propose an interface-engineered CoMo/CoTe electrocatalyst, consisting of an amorphous CoMo (a-CoMo) layer-encapsulated crystalline CoTe array, achieving the profound optimization of catalytic performance. The experimental results and density functional theory calculations show that the d-band center of the catalyst shifts further upward in contrast with its crystalline-crystalline counterpart, optimizing the electronic structure and the intermediate adsorption, thereby reducing the kinetic barrier of HER. The a-CoMo/CoTe with superhydrophilic/superaerophobic features shows excellent catalytic performance in alkaline, neutral, and simulated seawater environments.
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  • 文章类型: Journal Article
    在这里,我们使用溶剂热法制备MoS2和Cu-MoS2催化剂,一种广泛接受的电催化整体水分解应用技术。TEM和SEM图像,材料科学的标准工具,提供了Cu-MoS2形态的清晰视图。HRTEM分析,高分辨率成像技术,确认晶格间距,晶格平面,和Cu-MoS2的晶体结构。HAADF和相应的颜色映射和先进的成像技术揭示了铜掺杂的存在,Mo,Cu-MoS2中的S元素。值得注意的是,与MoS2催化剂相比,Cu在改善Cu-MoS2催化剂的析氢反应(HER)和析氧反应(OER)中起关键作用。此外,Cu-MoS2催化剂显示出显着较低的过电位(167.7mV和290mV)和塔菲尔斜率(121.5mVdec-1和101.5mVdec-1),对于HER和OER,分别为-10mAcm-2和10mAcm-2,分别,与MoS2催化剂相比。此外,使用计时电位法,Cu-MoS2催化剂在-10mAcm-2的HER下显示12h和在10mAcm-2的OER下显示12h的出色稳定性。有趣的是,在整个水分解过程中,与MoS2’MoS2电池1.81V相比,Cu-MoS2’Cu-MoS2电池显示出较低的1.69V的电池电位。此外,当在10mAcm-2下使用计时电位法18小时时,Cu-MoS2'Cu-MoS2电池显示出优异的稳定性。
    Herein, we prepare MoS2 and Cu-MoS2 catalysts using the solvothermal method, a widely accepted technique for electrocatalytic overall water-splitting applications. TEM and SEM images, standard tools in materials science, provide a clear view of the morphology of Cu-MoS2. HRTEM analysis, a high-resolution imaging technique, confirms the lattice spacing, lattice plane, and crystal structure of Cu-MoS2. HAADF and corresponding color mapping and advanced imaging techniques reveal the existence of the Cu-doping, Mo, and S elements in Cu-MoS2. Notably, Cu plays a crucial role in improving the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) of the Cu-MoS2 catalyst as compared with the MoS2 catalyst. In addition, the Cu-MoS2 catalyst demonstrates significantly lower overpotential (167.7 mV and 290 mV) and Tafel slopes (121.5 mV dec-1 and 101.5 mV dec-1), standing at -10 mA cm-2 and 10 mA cm-2 for HER and OER, respectively, compared to the MoS2 catalyst. Additionally, the Cu-MoS2 catalyst displays outstanding stability for 12 h at -10 mA cm-2 of HER and 12 h at 10 mA cm-2 of OER using chronopotentiaometry. Interestingly, the Cu-MoS2‖Cu-MoS2 cell displays a lower cell potential of 1.69 V compared with the MoS2‖MoS2 cell of 1.81 V during overall water splitting. Moreover, the Cu-MoS2‖Cu-MoS2 cell shows excellent stability when using chronopotentiaometry for 18 h at 10 mA cm-2.
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  • 文章类型: Journal Article
    我们提出了一种新颖且稳定的层状结构,以增强用于光电化学(PEC)水分解的硅(Si)光电阴极器件的性能和稳定性。首先,通过金属辅助化学蚀刻,利用Cu纳米颗粒催化剂在n+p黑Si衬底上工作,我们可以实现具有多孔金字塔结构的黑硅。由Cu蚀刻引起的金字塔表面上的低深度孔不仅有助于增强具有相当低的表面反射率(<5%)的光捕获能力,而且有效地保护p-n结免受损坏。为了提高电荷迁移效率,同时减轻助催化剂的寄生光吸收,我们滴下纳米尺寸的量子点(QDs)MoS2作为第一层催化剂。因此,然后,我们可以安全地电沉积助催化剂Co纳米颗粒,以进一步提高界面转移效率。协同作用的助催化剂和优化的光吸收的形态和量子点有助于整体提高PEC的性能,为有效的,低成本,和稳定的(超过100小时)产氢光电阴极。
    We present a novel and stable laminated structure to enhance the performance and stability of silicon (Si) photocathode devices for photoelectrochemical (PEC) water splitting. First, by utilizing Cu nanoparticle catalysts to work on a n+p-black Si substrate via the metal-assisted chemical etching, we can achieve the black silicon with a porous pyramid structure. The low depth holes on the surface of the pyramid caused by Cu etching not only help enhance the light capture capability with quite low surface reflectivity (<5%) but also efficiently protect the p-n junction from damage. To improve the charge migration efficiency and mitigate parasitic light absorption from cocatalysts at the same time, we drop casted quantum dots (QDs) MoS2 with the size of nanometer scale as the first layer of catalyst. Hence, we then can safely electrodeposit cocatalyst Co nanoparticles to further enhance interface transfer efficiency. The synergistic effects of cocatalysts and optimized light absorption from the morphology and QDs contributed to the overall enhancement of PEC performance, offering a promising pathway for an efficient, low cost, and stable (over 100 h) hydrogen production photocathode.
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  • 文章类型: Journal Article
    电催化的进步,特别是在开发用于氢气和氧气析出反应的有效催化剂(HER和OER)方面,对于通过整体水分解等过程的可持续能源生产至关重要。一种著名的双功能电催化剂,CoFe2O4/Co7Fe3被设计为同时促进OER和HER,旨在减少过电位。为了追求进一步提高催化效率,通过在催化剂体系中引入硫源和多壁碳纳米管(MWCNT),产生S-CoFe2O4/Co7Fe3/MWCNTs。这种修饰显著提高了OER和HER的活性。OER的过电位为250mV@10mAcm-2,HER的过电位为270mV@50mAcm-2,表明在相对较低的过电位下具有有效的催化活性。S-CoFe2O4/Co7Fe3/MWCNTs在碱性电解质中具有出色的长期稳定性,OER的最低Tafel斜率为77mV/dec,HER的最低Tafel斜率为70mV/dec,表明在延长的时间内具有持续的催化性能。此外,当在完全水分解的情况下同时用作阴极和阳极时,S-CoFe2O4/Co7Fe3/MWCNT在1MKOH溶液中在10mAcm-2的电流密度下表现出令人印象深刻的1.52V电池电压,展示其实际应用的可行性。鉴于其成本效益和优越的活动,S-CoFe2O4/Co7Fe3/MWCNTs在整体水裂解电催化中具有广泛的应用前景,促进更清洁和可持续的燃料发电技术的发展。
    The advancement in electrocatalysis, particularly in the development of efficient catalysts for hydrogen and oxygen evolution reactions (HER and OER), is crucial for sustainable energy generation through processes like overall water splitting. A notable bifunctional electrocatalyst, CoFe2O4/Co7Fe3, has been engineered to facilitate both OER and HER concurrently, aiming to reduce overpotentials. In the pursuit of further enhancing catalytic efficiency, a morphological transformation has been achieved by introducing a sulphur source and multi-walled carbon nanotubes (MWCNTs) into the catalyst system, resulting in S-CoFe2O4/Co7Fe3/MWCNTs. This modification has significantly improved the activity for both OER and HER. An onset overpotential of 250 mV@10 mAcm-2 for the OER and 270 mV@50 mAcm-2 for the HER, indicating efficient catalytic activity at relatively low overpotentials. S-CoFe2O4/Co7Fe3/MWCNTs display an outstanding long-term stability in alkaline electrolytes, with minimal Tafel slopes of 77 mV/dec for the OER and 70 mV/dec for the HER, suggesting sustained catalytic performance over extended periods. Furthermore, when employed as both the cathode and anode in the context of complete water splitting, S-CoFe2O4/Co7Fe3/MWCNTs demonstrate an impressive cell voltage of 1.52 V at a current density of 10 mA cm-2 in a 1 M KOH solution, showcasing its viability for practical applications. Given its cost-effectiveness and superior activity, S-CoFe2O4/Co7Fe3/MWCNTs hold significant promise for widespread applications in overall water splitting electrocatalysis, contributing to the advancement of cleaner and sustainable fuel generation technologies.
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  • 文章类型: Journal Article
    2D材料的边缘已经成为有前途的电化学催化剂系统,然而,它们的性能仍然落后于贵金属。这里,我们展示了定向电场(OEF)增强2D材料边缘电化学活性的潜力。通过原子设计氟石墨烯/石墨烯/MoS2异质结纳米带的边缘,通过模拟和空间分辨光谱学证实,实现了强大的局部OEF。根据阻抗谱,观察到的边缘OEF导致边缘和电解质之间的异质电荷转移速率提高2个数量级。从头算计算表明,场引起的反应物吸附能降低是这种改善的根源。我们将OEF增强的边缘反应性应用于析氢反应(HER),并观察到显着增强的电化学性能,Tafel斜率降低了30%,周转频率提高了3倍。我们的发现证明了OEF为未来复杂反应定制2D材料边缘的催化性能的潜力。
    The edges of 2D materials have emerged as promising electrochemical catalyst systems, yet their performance still lags behind that of noble metals. Here, we demonstrate the potential of oriented electric fields (OEFs) to enhance the electrochemical activity of 2D materials edges. By atomically engineering the edge of a fluorographene/graphene/MoS2 heterojunction nanoribbon, strong and localized OEFs were realized as confirmed by simulations and spatially resolved spectroscopy. The observed fringing OEF results in an enhancement of the heterogeneous charge transfer rate between the edge and the electrolyte by 2 orders of magnitude according to impedance spectroscopy. Ab initio calculations indicate a field-induced decrease in the reactant adsorption energy as the origin of this improvement. We apply the OEF-enhanced edge reactivity to hydrogen evolution reactions (HER) and observe a significantly enhanced electrochemical performance, as evidenced by a 30% decrease in Tafel slope and a 3-fold enhanced turnover frequency. Our findings demonstrate the potential of OEFs for tailoring the catalytic properties of 2D material edges toward future complex reactions.
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  • 文章类型: Journal Article
    水性Al-空气电池的大规模应用受到Al阳极性能的高度限制。铝阳极在浓碱性电解液中严重的自腐蚀和析氢是主要原因。这里,旨在缓解副反应并提高金属铝的利用率,我们提出了2-巯基苯并噻唑(MBT)和ZnO的混合电解质添加剂,以在阳极/电解质界面形成保护膜并减少析氢活性位点。MBT对金属表面的强吸收能力,随着含锌层的减少,能够在Al表面上形成具有高析氢电位的致密保护膜。有了这个好处,析氢反应(HER)抑制效率高达83.58%,在25mAcm-2的电流密度下,具有能量密度为2376.71WhkgAl-1的优异Al-空气电池。在金属表面构建混合保护膜的概念不仅有利于金属-空气电池的发展,而且有利于金属腐蚀防护。
    The large-scale application of aqueous Al-air batteries is highly restricted by the performance of Al anodes. The severe self-corrosion and hydrogen evolution of the Al anode in a concentrated alkaline electrolyte are the main reason. Here, aimed at relieving side reactions and enhancing the utilization of metal Al, we propose a hybrid electrolyte additive of 2-mercaptobenzothiazole (MBT) and ZnO to form a protective film at the anode/electrolyte interface and to decrease the hydrogen evolution active site. The strong absorption capability of MBT on the metal surface, along with the reduced Zn-containing layer, enables a compact protective film with high hydrogen evolution potential on the Al surface. With this benefit, the hydrogen evolution reaction (HER) inhibition efficiency is up to 83.58%, endowing a superior Al-air battery with an energy density of 2376.71 Wh kgAl-1 under a current density of 25 mA cm-2. The conception of constructing a hybrid protective film on the metal surface not only favors the development of metal-air batteries but also facilitates metal corrosion protection.
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