Hydrogen

氢气
  • 文章类型: Journal Article
    氢化酶和光合反应中心(RC)的融合已被证明是生产可持续生物燃料的有希望的策略。I型(含铁硫)RC,作为光敏剂,能够将电子促进到氧化还原态,氢酶可以利用该氧化还原态将质子还原为二氢(H2)。虽然[FeFe]和[NiFe]氢化酶都已成功使用,由于O2敏感性,它们往往受到限制,结合特异性,或H2生产率。在这项研究中,我们融合了光系统I(PSI)的外围(基质)亚基,PsaE,使用柔性[GGS]4接头基团(CbHydA1-PsaE)从贝氏梭菌中提取耐O2的[FeFe]氢化酶。我们证明了CbHydA1嵌合体可以在体外合成激活以显示双向活性,并且可以定量地与缺乏PsaE亚基的PSI变体结合。当在厌氧环境中照明时,纳米构建体以84.9±3.1µmolH2mgchl-1h-1的速率产生H2。Further,当在O2存在下制备和照射时,纳米结构保留了产生H2的能力,尽管速率降低了2.2±0.5µmolH2mgchl-1h-1。这不仅表明PsaE是基于PSI的纳米构建体的有前途的支架,但是使用耐O2的[FeFe]氢化酶为体内H2产生系统提供了可能性,该系统可以在O2存在下发挥作用。
    The fusion of hydrogenases and photosynthetic reaction centers (RCs) has proven to be a promising strategy for the production of sustainable biofuels. Type I (iron-sulfur-containing) RCs, acting as photosensitizers, are capable of promoting electrons to a redox state that can be exploited by hydrogenases for the reduction of protons to dihydrogen (H2). While both [FeFe] and [NiFe] hydrogenases have been used successfully, they tend to be limited due to either O2 sensitivity, binding specificity, or H2 production rates. In this study, we fuse a peripheral (stromal) subunit of Photosystem I (PS I), PsaE, to an O2-tolerant [FeFe] hydrogenase from Clostridium beijerinckii using a flexible [GGS]4 linker group (CbHydA1-PsaE). We demonstrate that the CbHydA1 chimera can be synthetically activated in vitro to show bidirectional activity and that it can be quantitatively bound to a PS I variant lacking the PsaE subunit. When illuminated in an anaerobic environment, the nanoconstruct generates H2 at a rate of 84.9 ± 3.1 µmol H2 mgchl-1 h-1. Further, when prepared and illuminated in the presence of O2, the nanoconstruct retains the ability to generate H2, though at a diminished rate of 2.2 ± 0.5 µmol H2 mgchl-1 h-1. This demonstrates not only that PsaE is a promising scaffold for PS I-based nanoconstructs, but the use of an O2-tolerant [FeFe] hydrogenase opens the possibility for an in vivo H2 generating system that can function in the presence of O2.
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  • 文章类型: Journal Article
    使用较低成本的原料制造氢气,废弃有机物(WOs),例如,厨房垃圾生物油,是一个双赢的解决方案,因为它既能解决能源问题,又能减少环境污染。超声波在有机分解方面引起了相当大的兴趣;然而,单独应用超声波不是从WOs制氢的好选择,因为能耗和效率。为提高生物油超声空化裂解制氢性能,将光热材料引入制氢系统以形成局部热点。材料炭黑(CB),碳纳米管(CNT),和二氧化硅(SiO2)都对生物油的制氢表现出显着的增强作用,在这些材料中,CB表现出最显著的增强作用。当CB的剂量为5mg时,氢气的产生速率为180.1μmol·h-1,与没有CB的产生速率相比,显着提高了1.7倍。在光和超声波的存在下,与仅存在光而没有超声的情况相比,氢气产生速率可以增加66.7倍。
    The creation of hydrogen using the lower-cost feedstock, waste organics (WOs), e.g. kitchen waste bio-oil, is a win-win solution, because it can both solve energy problems and reduce environmental pollution. Ultrasound has received considerable interest in organic decomposition; however, the application of ultrasound alone is not a good choice for the hydrogen production from WOs, because of the energy consumption and efficiency. To boost the hydrogen production based on ultrasonic cavitation cracking of bio-oil, photothermal materials are introduced into the hydrogen production system to form localized hot spots. Materials carbon black (CB), carbon nanotubes (CNT), and silicon dioxide (SiO2) all exhibit significant enhancing effects on the hydrogen production from bio-oil, and the CB exhibits the most significant strengthening effect among these materials. When the dosage of CB is 5 mg, hydrogen production rate is 180.1 μmol · h-1, representing a notable 1.7-fold increase compared to the production rate without CB. In the presence of light and ultrasound, the hydrogen production rate can be increased by 66.7-fold compared to the situation where only light is present without ultrasound.
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  • 文章类型: Journal Article
    作为化石燃料的替代品,人们对在燃烧系统中使用氨越来越感兴趣,特别是在内燃机中。作为氢的有力竞争者,它有各种优点。然而,为了保持燃烧稳定性,仍然需要添加诸如氢气的点火促进剂。由于使用氨的发动机也遭受高NOx排放,在这项研究中,数值研究了添加不同气体对氨氢双燃料发动机性能和排放的影响。基础发动机是柴油发动机,其参数习惯于以氨-氢作为燃料运行。氢气在进气阶段以180度曲柄角(CAD)通过进气口喷射,并与气缸充气混合。在350-370CAD下将氨直接注入气缸中。不同的气体,包括氩气,氮,二氧化碳,和氧气,之前在不同的曲轴转角注入气缸,during,和氨注入后(330-350CAD,350-370CAD,和370-390CAD)。准备了MATLAB代码来求解控制方程,燃烧机制在Cantera实施。结果表明,在氨喷射定时之前或同时添加CO2对缸内压力峰值以及NO和NO2排放产生不利影响。O2的添加对排放有负面影响。在氨注入(350-370CAD)的同时添加N2和Ar可以减少NO和NO2排放,而不会显著影响缸内压力和温度峰值。
    As an alternative to fossil fuels, there is growing interest in using ammonia in combustion systems, particularly in internal combustion engines. As a competent competitor to hydrogen, it has various advantages. However, adding an ignition promoter such as hydrogen is still necessary to maintain combustion stability. Since the engine using ammonia also suffers from high NOx emissions, in this study, the effects of adding different gases on the performance and emissions of an ammonia-hydrogen dual-fuel engine were numerically investigated. The base engine was a diesel engine whose parameters were accustomed to running with ammonia-hydrogen as fuel. Hydrogen was injected via the port in the intake stage at 180 crank angle degrees (CAD) and mixed with the cylinder charge. Ammonia was directly injected into the cylinder at 350-370 CAD. Different gasses, including argon, nitrogen, carbon dioxide, and oxygen, were injected into the cylinder at various crank angles before, during, and after ammonia injection (330-350 CAD, 350-370 CAD, and 370-390 CAD). A MATLAB code was prepared to solve the governing equations, and the combustion mechanism was implemented in Cantera. The results showed that adding CO2 before or concurrent with the ammonia injection timing had undesirable impacts on the peak in-cylinder pressure and NO and NO2 emissions. The O2 addition had a negative on the emissions. Adding N2 and Ar concurrently with the ammonia injection (350-370 CAD) could diminish NO and NO2 emissions without drastically affecting the peak in-cylinder pressure and temperature.
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  • 文章类型: Journal Article
    二氧化钛是通过使用溶胶-凝胶法水解异丙醇钛(IV)合成的,在中性或基本条件下,并在微波辅助溶剂热反应器和/或高温炉中加热。使用X射线衍射法测定制备的样品的相组成。通过低温氮吸附/解吸研究确定比表面积和孔体积。通过光催化还原二氧化碳测试样品的光活性。使用气相色谱法分析气相的组成,和氢,碳氧化物,甲烷被识别出来了.研究了pH和热处理对二氧化碳光还原过程中二氧化钛基材料物理化学性质的影响。发现在中性环境中制备的光催化剂显示出较高的氢含量,一氧化碳,与在基本条件下获得的光催化剂相比,气相中的甲烷。在使用在微波反应器中加热的光催化剂的过程中检测到最高量的氢气,和双重加热的光催化剂。
    Titanium dioxide was synthesized via hydrolysis of titanium (IV) isopropoxide using a sol-gel method, under neutral or basic conditions, and heated in the microwave-assisted solvothermal reactor and/or high-temperature furnace. The phase composition of the prepared samples was determined using the X-ray diffraction method. The specific surface area and pore volumes were determined through low-temperature nitrogen adsorption/desorption studies. The photoactivity of the samples was tested through photocatalytic reduction of carbon dioxide. The composition of the gas phase was analyzed using gas chromatography, and hydrogen, carbon oxide, and methane were identified. The influence of pH and heat treatment on the physicochemical properties of titania-based materials during photoreduction of carbon dioxide have been studied. It was found that the photocatalysts prepared in neutral environment were shown to result in a higher content of hydrogen, carbon monoxide, and methane in the gas phase compared to photocatalysts obtained under basic conditions. The highest amounts of hydrogen were detected in the processes using photocatalysts heated in the microwave reactor, and double-heated photocatalysts.
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  • 文章类型: Journal Article
    CO的优先氧化(CO-PROX)在净化燃料电池的氢气以避免CO分子引起的催化剂中毒方面具有重大意义。传统的粉末催化剂面临诸多挑战,包括高压降,聚集趋势,热点地层,质量和传热效率差,热稳定性不足。因此,陶瓷整体式催化剂,以其优异的热稳定性而闻名,高表面积,和优越的传质和传热特性,正在获得越来越多的研究关注。这篇综述考察了CO-PROX中陶瓷整体式催化剂的最新研究,强调活性位点的监管(例如,贵金属,如Pt和Au,以及CuO和CeO2等非贵金属),整体结构,和涂层策略。此外,结构-催化性能关系,以及不同陶瓷整体式催化剂在实际应用中的潜力和局限性,正在讨论。最后,重点介绍了整体式催化剂在CO-PROX反应中的挑战和未来的研究前景。
    Preferential oxidation of CO (CO-PROX) has tremendous significance in purifying hydrogen for fuel cells to avoid catalyst poisoning by CO molecules. Traditional powder catalysts face numerous challenges, including high pressure drop, aggregation tendency, hotspot formation, poor mass and heat transfer efficiency, and inadequate thermal stability. Accordingly, ceramic monolithic catalysts, known as their excellent thermal stability, high surface area, and superior mass and heat transfer characteristics, are gaining increasing research attention. This review examines recent studies on ceramic monolithic catalysts in CO-PROX, placing emphasis on the regulation of active sites (e.g., precious metals like Pt and Au, and non-precious metals like CuO and CeO2), monolith structures, and coating strategies. In addition, the structure-catalytic performance relationships, as well as the potential and limitations of different ceramic monolithic catalysts in practical application, are discussed. Finally, the challenges of monolithic catalysts and future research prospects in CO-PROX reactions are highlighted.
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  • 文章类型: Journal Article
    高温超导体(HTS)是飞机推进广泛电气化的推动者。的确,如果用于电机,HTS材料可以大大提高其在功率重量比方面的性能。在超导电机的不同拓扑结构中,基于HTS主体的通量调制机因其紧凑性和重量轻而受到关注。这种机器是在空中客车公司领导的FROST(磁通屏障旋转超导拓扑)项目中提出的,目的是开发新技术,作为国际政策驱动的脱碳目标的一部分。机器的转子将容纳大的环段形HTS主体以增加输出功率。然而,这些散装的性质是鲜为人知的,几乎没有在文献中进行过研究。在这种情况下,目前的工作旨在在FROST的框架内部分填补这种稀缺性。因此,对11种大型REBaCuO散装的性能和均匀性进行了彻底的表征。其中十块将用于机器原型中,最初保留第十一批作为备用。对11个块进行第一组表征。对于这套,估计了被困场映射和临界电流。然后,随后对第十一批进行了一系列深入的表征。它包括临界电流测量,X射线衍射,和扫描电子显微镜在不同位置从散装切出的不同毫米大小的样品。X射线衍射和扫描电子显微镜显示主体内部的弱氧化区域,解释了超导性能的局部下降或损失。目的是确定在所有散装物上测量的被困场中发现的不均匀性的原因,牺牲其中一个,这里是备用的。为了获得更清晰的图像,然后,使用从各种小样本的表征中获得的实验数据,对数值模型进行了阐述,以重现第十一块的现场图。结论是,进一步的表征,包括各种散货的统计数据,仍然需要了解被困场不均匀性的根本原因。尽管如此,所有的散装提出了足够的电流密度,可用于建设拟议的机器。
    High temperature superconductors (HTSs) are enablers of extensive electrification for aircraft propulsion. Indeed, if used in electrical machines, HTS materials can drastically improve their performance in terms of the power-to-weight ratio. Among the different topologies of superconducting electrical machines, a flux modulation machine based on HTS bulks is of interest for its compactness and light weight. Such a machine is proposed in the FROST (Flux-barrier Rotating Superconducting Topology) project led by Airbus to develop new technologies as part of their decarbonization goals driven by international policies. The rotor of the machine will house large ring-segment-shaped HTS bulks in order to increase the output power. However, the properties of those bulks are scarcely known and have barely been investigated in the literature. In this context, the present work aims to fill out partially this scarcity within the framework of FROST. Thus, a thorough characterisation of the performances and homogeneity of 11 large REBaCuO bulks was carried out. Ten of the bulks are to be utilized in the machine prototype, originally keeping the eleventh bulk as a spare. A first set of characterisation was conducted on the eleven bulks. For this set, the trapped field mapping and the critical current were estimated. Then, a series of in-depth characterisations on the eleventh bulk followed. It included critical current measurement, X-ray diffraction, and scanning electron microscopy on different millimetre-size samples cut out from the bulk at various locations. The X-ray diffraction and scanning electron microscopy showed weakly oxygenated regions inside the bulk explaining the local drop or loss in superconducting properties. The objective was to determine the causes of the inhomogeneities found in the trapped field measured on all the bulks, sacrificing one of them, here the spare one. To help obtain a clearer picture, a numerical model was then elaborated to reproduce the field map of the eleventh bulk using the experimental data obtained from the characterisation of its various small samples. It is concluded that further characterisations, including the statistics on various bulks, are still needed to understand the underlying reasons for inhomogeneity in the trapped field. Nonetheless, all the bulks presented enough current density to be usable in the construction of the proposed machine.
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  • 文章类型: Journal Article
    这项研究介绍了一种氢传感器,该传感器由使用称为射频共溅射(RF共溅射)的技术沉积的氧化镁锌(MgZnO)薄膜制成。分别使用氧化镁(MgO)和氧化锌(ZnO)靶来沉积MgZnO薄膜,试验不同的沉积时间和功率水平。当暴露于浓度为百万分之1000(ppm)的氢气时,传感器表现最佳(达到2.46的感测响应)。在300°C的温度下,当MgZnO膜厚度为432纳米(nm)时,出现了该峰值性能。最初,传感器的响应性随着薄膜厚度的增加而增加。这是因为较厚的薄膜倾向于具有更多的氧空位,这些是在传感器功能中起作用的缺陷。然而,膜厚度进一步增加超过最佳点损害性能。这归因于薄膜内晶粒的生长,这阻碍了它的有效性。使用X射线衍射(XRD)和场发射扫描电子显微镜(FE-SEM)对MgZnO薄膜的质量进行了全面表征。这些技术为薄膜的晶体结构和形态提供了有价值的见解,影响其作为氢传感器性能的关键因素。
    This research introduces a hydrogen sensor made from a thin film of magnesium zinc oxide (MgZnO) deposited using a technique called radiofrequency co-sputtering (RF co-sputtering). Separate magnesium oxide (MgO) and zinc oxide (ZnO) targets were used to deposit the MgZnO film, experimenting with different deposition times and power levels. The sensor performed best (reaching a sensing response of 2.46) when exposed to hydrogen at a concentration of 1000 parts per million (ppm). This peak performance occurred with a MgZnO film thickness of 432 nanometers (nm) at a temperature of 300 °C. Initially, the sensor\'s responsiveness increased as the film thickness grew. This is because thicker films tend to have more oxygen vacancies, which are imperfections that play a role in the sensor\'s function. However, further increases in film thickness beyond the optimal point harmed performance. This is attributed to the growth of grains within the film, which hindered its effectiveness. X-ray diffraction (XRD) and field-emission scanning electron microscopy (FE-SEM) were employed to thoroughly characterize the quality of the MgZnO thin film. These techniques provided valuable insights into the film\'s crystal structure and morphology, crucial factors influencing its performance as a hydrogen sensor.
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  • 文章类型: Journal Article
    对用于小分子活化和催化的无过渡金属化合物的兴趣正在增长。我们讨论了合成钠掺杂的非晶硅-氮化硼(Na掺杂的a-SiBN)所带来的机会。Na+阳离子和3-重配位的BIII部分通过聚硅氮烷的化学改性结合到无定形氮化硅网络中,然后在氨中在1000°C下热解。重点放在Na掺杂的a-SiBN结构中氢(H2)活化的机理上。这种材料设计方法允许由SiN4单元包围的Na+和BIII部分的均匀分布,这有助于在遇到H2时将BIII部分转化为4倍配位的几何结构,这可能充当受挫的路易斯酸(FLA)位点。暴露于H2诱导形成受挫的路易斯碱(FLB)N-=具有Na作为电荷补偿阳离子的位点,导致原位形成受挫的刘易斯对(FLP)基序(=BFLA···Hδ-··Hδ···:N-(Na)=)。具有高活化能(124kJmol-1)的可逆H2吸附-解吸行为表明H2在Na掺杂的a-SiBN上的化学吸附。这些发现凸显了我们力所能及的未来前景,我们预计主要基团介导的小分子活化将对更有效的催化过程的设计和新催化转化的发现产生重要影响。
    Interest is growing in transition metal-free compounds for small molecule activation and catalysis. We discuss the opportunities arising from synthesizing sodium-doped amorphous silicon-boron-nitride (Na-doped a-SiBN). Na+ cations and 3-fold coordinated BIII moieties were incorporated into an amorphous silicon nitride network via chemical modification of a polysilazane followed by pyrolysis in ammonia at 1000 °C. Emphasis is placed on the mechanisms of hydrogen (H2) activation within Na-doped a-SiBN structure. This material design approach allows the homogeneous distribution of Na+ and BIII moieties surrounded by SiN4 units contributing to the transformation of the BIII moieties into 4-fold coordinated geometry upon encountering H2, potentially serving as frustrated Lewis acid (FLA) sites. Exposure to H2 induced formation of frustrated Lewis base (FLB) N-= sites with Na+ as a charge-compensating cation, resulting in the in situ formation of a frustrated Lewis pair (FLP) motif (≡BFLA···Hδ-···Hδ+···:N-(Na+)=). Reversible H2 adsorption-desorption behavior with high activation energy for H2 desorption (124 kJ mol-1) suggested the H2 chemisorption on Na-doped a-SiBN. These findings highlight a future landscape full of possibilities within our reach, where we anticipate main-group-mediated small molecule activation will have an important impact on the design of more efficient catalytic processes and the discovery of new catalytic transformations.
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  • 文章类型: Journal Article
    嗜热产乙酸细菌作为生物技术应用如合成气发酵的有希望的候选细菌引起了人们的注意。微生物电合成和甲醇转化。这里,我们旨在从不同的环境中分离和表征新型的嗜热乙酸原。通过基于16SrRNA基因的细菌群落分析监测异养和自养乙酸原的富集。通过基因组和生理分析分离并表征了七个新的Moorella菌株。在自养生长过程中,两种Moorellahumerferrea分离株显示出相当大的差异。将M.humeroperreaLNE分离物(DSM117358)发酵成一氧化碳(CO),而M.humeroperreaOCP分离物(DSM117359)通过水煤气变换反应将CO转化为氢气和二氧化碳(H2CO2)。从活性炭燃烧堆的覆盖土壤中分离出另一种一氧化碳养氢Moorella菌株,并被提议为新型物种Moorellacarbonis的类型菌株(ACPsT)(DSM116161T,CCOS2103T)。其余四个新菌株与Moorellathermocetica相关,并显示,与DSM2955T型应变一起,除乙酸盐外,从H2CO2中生产少量乙醇。对新型Moorella菌株的生理分析揭示了分离株特异性差异,这大大增加了对嗜热乙酸原的知识基础,以供将来应用。
    Thermophilic acetogenic bacteria have attracted attention as promising candidates for biotechnological applications such as syngas fermentation, microbial electrosynthesis, and methanol conversion. Here, we aimed to isolate and characterize novel thermophilic acetogens from diverse environments. Enrichment of heterotrophic and autotrophic acetogens was monitored by 16S rRNA gene-based bacterial community analysis. Seven novel Moorella strains were isolated and characterized by genomic and physiological analyses. Two Moorella humiferrea isolates showed considerable differences during autotrophic growth. The M. humiferrea LNE isolate (DSM 117358) fermented carbon monoxide (CO) to acetate, while the M. humiferrea OCP isolate (DSM 117359) transformed CO to hydrogen and carbon dioxide (H2 + CO2), employing the water-gas shift reaction. Another carboxydotrophic hydrogenogenic Moorella strain was isolated from the covering soil of an active charcoal burning pile and proposed as the type strain (ACPsT) of the novel species Moorella carbonis (DSM 116161T and CCOS 2103T). The remaining four novel strains were affiliated with Moorella thermoacetica and showed, together with the type strain DSM 2955T, the production of small amounts of ethanol from H2 + CO2 in addition to acetate. The physiological analyses of the novel Moorella strains revealed isolate-specific differences that considerably increase the knowledge base on thermophilic acetogens for future applications.
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  • 文章类型: Journal Article
    乳酸已被用作从富含乳酸菌(LAB)的底物生产氢气(H2)的前体,专注于生产和消费用模型底物测试的LAB之间的微生物相互作用。因此,这项研究评估了单个和组合的乳酸菌对发酵食品废物(FW)中乳酸产生的嗜温H2的批量测试的影响。梅加斯皮埃尔斯登尼,贝杰林克氏梭菌,和丁酸梭菌以不同的比例(v/v)接种。此外,将热预处理污泥(TPS)添加到菌株混合物中。最高的产量是用埃尔斯登尼获得的,C.贝耶林基,和丁酸梭菌(17:66:17比例),获得1629.0mL/L反应器。富含TPS的最佳混合物(68:32:0的埃尔斯登氏菌和贝耶林克氏菌)达到1739.3±98.6mLH2/Lreactor,消耗98%的乳酸添加。埃氏M.elsdenii和Clostridium菌株增强了乳酸的H2产生,因为它们持续存在于最初由LAB主导的微生物群落中。
    Lactic acid has been applied as a precursor for hydrogen (H2) production from substrates rich in lactic acid bacteria (LAB), focusing on microbial interactions between producing and consuming LAB tested with model substrates. Therefore, this study evaluated the effect of single and combined lactic acid-consuming bacteria on mesophilic H2 production in batch tests from lactic acid from fermented food waste (FW). Megasphaera elsdenii, Clostridium beijerinckii, and Clostridium butyricum were inoculated at different ratios (v/v). Additionally, thermal pretreated sludge (TPS) was added to the strain mixtures. The highest production was obtained with M. elsdenii, C. beijerinckii, and C. butyricum (17:66:17 ratio), obtaining 1629.0 mL/Lreactor. The optimal mixture (68:32:0 of M. elsdenii and C. beijerinckii) enriched with TPS reached 1739.3 ± 98.6 mL H2/Lreactor, consuming 98 % of lactic acid added. M. elsdenii and Clostridium strains enhance H2 production from lactic acid as they persist in a microbial community initially dominated by LAB.
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