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Amine Synthesis Using the Amine Donor N-Phenyl Putrescine (NPP) and the Johnson Matthey Transaminase Biocatalyst Library 利用胺供体n -苯基腐胺(NPP)和Johnson Matthey转氨酶生物催化剂库合成胺
IF 2.3 4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651323x16843361771150
Kimberley C. Dodds, C. McKenna, B. Domínguez, Andrew L. Lawrence, D. Campopiano
Chiral amines are important building blocks in the pharmaceutical, agrochemical and chemical industries. There is a drive to augment traditional transition metal catalysts with green alternatives such as biocatalysts. Transaminase (TA) biocatalysts can be used in combination with "smart" sacrificial amine donors to synthesise a variety of aliphatic and aromatic amines from the corresponding aldehydes and ketones. Despite their enormous potential, the unfavourable reaction equilibrium often limits the widespread application of TAs for industrial synthesis. Recently we disclosed a new biomimetic amine donor N-phenyl putrescine (NPP), which was inspired by the biosynthesis of the dipyrroloquinoline alkaloids. NPP was demonstrated to have good activity with a library of commercial and wild-type TAs (total 25 TAs). This work focused on exploring the use of NPP with the Johnson Matthey TA kit (17 biocatalysts; 8 S-selective and 9 R-selective) and three different amine acceptors (vanillin, benzaldehyde and acetophenone). NPP worked well with all 17 TAs and gave the corresponding amine products vanillylamine, benzylamine and methylbenzylamine in up to 85% HPLC yield. From the screen, STA-14 was identified as a good biocatalyst for further analysis and used in a comparative screen of NPP versus the commonly used donor iPrNH2. It was found that NPP was the best amine donor and used to prepare S-methylbenzylamine in >99.5% e.e. This work, combined with our previous study, highlights the potential of NPP in the biocatalytic synthesis of amines.
手性胺是制药、农化和化学工业的重要组成部分。有一种动力是用生物催化剂等绿色替代品来增加传统的过渡金属催化剂。转氨酶(TA)生物催化剂可以与“智能”牺牲胺供体结合使用,从相应的醛和酮合成各种脂肪胺和芳香胺。尽管ta具有巨大的潜力,但不利的反应平衡往往限制了ta在工业合成中的广泛应用。最近,我们披露了一种新的仿生胺供体n -苯基腐胺(NPP),它的灵感来自于二吡咯喹啉生物碱的生物合成。NPP对商业和野生型菌株(共25个)具有良好的活性。这项工作的重点是探索NPP与Johnson Matthey TA试剂盒(17种生物催化剂;8个s选择性和9个r选择性)和三种不同的胺受体(香兰素,苯甲醛和苯乙酮)。NPP对所有17种TAs均有良好的反应,并以高达85%的高效液相色谱收率得到相应的香兰胺、苄胺和甲基苄胺。从筛选中,STA-14被确定为一种良好的生物催化剂,可用于进一步分析,并用于NPP与常用供体iPrNH2的比较筛选。结果表明,NPP是最佳的胺供体,并以>99.5%的e - e制备了s -甲基苄胺。本工作结合我们前期的研究,突出了NPP在生物催化合成胺方面的潜力。
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引用次数: 0
Advancements in Green Ammonia Production and Utilisation Technologies 绿色氨生产与利用技术进展
4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651324x16946999404542
John Humphreys, Shanwen Tao
Green ammonia, produced through renewable energy-powered electrochemical and thermal processes, is emerging as a promising candidate to replace fossil fuel-based ammonia in the fertilizer, transportation, and energy sectors. This paper provides an overview of the production methods, utilisation methods, and technological advancements for green ammonia. The electrochemical production and Haber-Bosch with renewable hydrogen and energy, are discussed in detail highlighting recent material advances. Green ammonia utilisation methods are discussed with direct use cases such as ammonia combustion and direct ammonia fuel cells examined. Green ammonia’s potential as a carbon-free hydrogen carrier is also discussed in regards to ammonia cracking for effective hydrogen recovery. This paper concludes that green ammonia has the potential to play a significant role in the transition to a sustainable energy system and offers new opportunities for the fertilizer, transportation, and energy industries.
通过可再生能源驱动的电化学和热过程生产的绿色氨,正在成为化肥、运输和能源领域取代化石燃料氨的有希望的候选产品。综述了绿色氨的生产方法、利用方法及技术进展。详细讨论了可再生氢和能源的电化学生产和Haber-Bosch,重点介绍了材料的最新进展。讨论了氨的绿色利用方法,并考察了氨燃烧和直接氨燃料电池等直接用例。绿色氨作为无碳氢载体的潜力也讨论了关于氨裂解的有效氢回收。本文的结论是,绿色氨有可能在向可持续能源系统的过渡中发挥重要作用,并为肥料、运输和能源行业提供新的机遇。
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引用次数: 0
Inelastic Neutron Scattering Studies of Propene and 1-Octene Oligomerisation in HZSM-5 HZSM-5中丙烯和1-辛烯寡聚的非弹性中子散射研究
4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651324x16964134291592
Alexander P. Hawkins, Andrea Zachariou, Paul Collier, Russell F. Howe, David Lennon, Stewart F. Parker
Neutron scattering methods (quasielastic neutron scattering (QENS) and inelastic neutron scattering (INS)) have been used to study the reactivity of propene and 1-octene over the acid zeolite catalyst H-ZSM 5. The high activity of the catalyst causes the alkenes to form linear oligomers below room temperature. INS has shown that the reaction proceeds through a hydrogen-bonded intermediate. Studies using propane as an inert analogue for propene have found that the adsorbed C3 molecules spend the majority of their time undergoing short jumps within the pore channels of the zeolite. Hydrothermal de-alumination plays an important role in determining the activity of zeolite catalysts. De-alumination was found to delay the onset of catalytic activity for oligomerization to higher temperatures and increase the mobility of hydrocarbons within the zeolite, both due to reduced acid-hydrocarbon interactions.
采用准弹性中子散射(QENS)和非弹性中子散射(INS)方法研究了丙烯和1-辛烯在酸性沸石催化剂h - zsm5上的反应性。催化剂的高活性使烯烃在室温下形成线性低聚物。INS表明反应是通过一个氢键中间产物进行的。使用丙烷作为丙烯的惰性类似物的研究发现,吸附的C3分子大部分时间在沸石的孔隙通道内经历短暂的跳跃。水热脱铝对沸石催化剂的活性有重要影响。研究发现,由于酸-烃相互作用的减少,脱铝可以延缓低聚反应在高温下的催化活性,并增加沸石中碳氢化合物的流动性。
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引用次数: 0
Microbial Production of Hydrogen 微生物产氢
IF 2.3 4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651323x16806845172690
Kathleen L. Dunbar, S. Hingley-Wilson, J. Keddie
Hydrogen offers a source of energy that does not produce any greenhouse gas when combusted. However, some manufacturing methods of hydrogen consume large amounts of energy and produce carbon dioxide as a by-product. The production of hydrogen by bacteria is an attractive alternative, because it is not energy intensive and - under the right conditions - does not release greenhouse gases. In this review, we introduce the five known ways by which bacteria can evolve hydrogen. We then describe methods to encapsulate living bacteria in synthetic layers, called coatings, for applications in bioreactors. We review the few examples in which biocoatings have been used to produce hydrogen via the photo-fermentation method. Although not used in biocoatings so far, the dark fermentation method of hydrogen production avoids the need for illumination while offering a high yield with low oxygen evolution. We identify the potential for using genetically-modified bacteria in future research on biocoatings.
氢提供了一种能源,燃烧时不会产生任何温室气体。然而,一些制造氢气的方法消耗大量的能源,并产生二氧化碳作为副产品。利用细菌生产氢气是一种很有吸引力的替代方法,因为它不需要消耗大量能源,而且在适当的条件下不会释放温室气体。在这篇综述中,我们介绍了五种已知的细菌进化氢的方式。然后,我们描述了将活细菌封装在称为涂层的合成层中的方法,用于生物反应器。本文综述了生物膜利用光发酵法制备氢气的几个实例。虽然到目前为止还没有用于生物涂层,但暗发酵制氢的方法避免了对照明的需求,同时提供了低析氧的高产量。我们确定了在未来生物涂层研究中使用转基因细菌的潜力。
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引用次数: 0
Benchmarking Stability of IrOx in Acidic Media under O2 Evolution Conditions: A Review 酸性介质中氧析出条件下IrOx的基准稳定性研究进展
IF 2.3 4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651323x16848455435118
J. Murawski, S. Scott, Reshma R. Rao, Katie Rigg, C. Zalitis, James Stevens, J. Sharman, G. Hinds, I. Stephens
State-of-the-art proton exchange membrane (PEM) electrolysers employ iridium-based catalysts to facilitate oxygen evolution at the anode. To enable scale-up of the technology to the terawatt level, further improvements in the iridium utilisation are needed, without incurring additional overpotential losses or reducing the device lifetime. The research community has only recently started to attempt systematic benchmarking of catalyst stability. Short term electrochemical methods alone are insufficient to predict catalyst degradation; they can both underestimate and overestimate catalyst durability. Complementary techniques, such as inductively coupled plasma - mass spectrometry, are required to provide more reliable assessment of the amount of catalyst lost through dissolution. Herein, we critically review the state of the art in probing degradation of iridium-based oxide catalysts. We also highlight considerations and best practices for the investigation of activity and stability of oxygen evolution catalysts via short term testing.
最先进的质子交换膜(PEM)电解槽采用铱基催化剂促进阳极的析氧。为了使该技术的规模扩大到太瓦水平,需要进一步提高铱的利用率,而不会产生额外的过电位损失或缩短设备寿命。研究界直到最近才开始尝试对催化剂稳定性进行系统的基准测试。短期电化学方法不足以预测催化剂的降解;他们可能低估或高估催化剂的耐久性。补充技术,如电感耦合等离子体质谱法,需要提供更可靠的评估通过溶解催化剂损失的量。在这里,我们批判性地回顾了目前在探测铱基氧化物催化剂降解方面的研究进展。我们还强调了通过短期测试研究析氧催化剂活性和稳定性的注意事项和最佳实践。
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引用次数: 0
Effect of Ru targets on the growth and electrical properties of sputtering Ru films 钌靶对溅射钌薄膜生长和电性能的影响
IF 2.3 4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651323x16859589078188
Yue Shen, Yanting Xu, Jun Gan, Renyao Zhang, M. Wen
Ruthenium (Ru) targets prepared by vacuum hot pressing of Ru powder with different morphologies. Then Ru films were deposited on SiO2/Si(100) substrate for different times by RF magnetron sputtering. The relationship in terms of the microstructure and electrical properties between Ru targets and resultant films at different conditions were studied by means of FESEM, XRD, AFM, four probe and so on. The results showed that parameters of Ru films, such as the average deposition rate, surface roughness, crystallization properties and the growth rate were directly related to the homogeneity of the microstructure of the Ru targets, but there was no correlation between the crystal orientations of the films and the targets. Moreover, the resistivity of Ru films was positively correlated with that of Ru targets.
采用真空热压法制备不同形貌的钌靶材。然后采用射频磁控溅射法在SiO2/Si(100)衬底上沉积不同时间的Ru薄膜。采用FESEM、XRD、AFM、四探针等手段研究了不同条件下Ru靶材与薄膜的微观结构和电学性能的关系。结果表明,Ru薄膜的平均沉积速率、表面粗糙度、结晶性能和生长速率等参数与Ru靶材微观结构的均匀性有直接关系,而薄膜的晶体取向与靶材没有相关性。钌薄膜的电阻率与钌靶材的电阻率呈正相关。
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引用次数: 0
Influence of Temperature and Orientation on Elastic, Mechanical, Thermophysical and Ultrasonic Properties of Platinum Group Metal Carbides 温度和取向对铂族金属碳化物弹性、力学、热物理和超声性能的影响
IF 2.3 4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651323x16902884637568
Anurag Singh, Devraj Singh
The elastic, mechanical, thermophysical and ultrasonic properties of platinum group metal (PGM) carbides XC (X: Rh, Pd, Ir) have been investigated at room temperature. The Coulomb and Born-Mayer potential model has been used to compute second and third order elastic constants (SOECs and TOECs) at 0K and 300K. The obtained values of SOECs are used to evaluate the mechanical properties such as Young’s modulus, bulk modulus, shear modulus, Pugh’s indicator, Zener anisotropic constant and Poisson’s ratio at room temperature. The materials show the brittle nature as the value of Pugh’s indicator for PGM carbides has been achieved less than or nearly equal to 1.75. Again the values of SOECs are used to compute the ultrasonic velocities along <100>, <110> and <111> directions for the longitudinal and shear modes of wave propagation. Further the values of Debye temperature, thermal conductivity, specific heat per unit volume, energy density, average value of ultrasonic Grüneisen parameter, thermal relaxation time, non-linear parameter have been calculated with the help of SOECs, TOECs, ultrasonic velocities, density and molecular weight. Finally, the ultrasonic attenuation due to phonon-phonon interaction and due to thermoelastic relaxation mechanisms have been calculated with the use of all associated parameters. The calculated values of elastic, mechanical, thermophysical and ultrasonic properties are compared with available literature and discussed.
研究了铂族金属(PGM)碳化物XC (X: Rh, Pd, Ir)在室温下的弹性、力学、热物理和超声性能。库仑和玻恩-梅耶势模型用于计算0K和300K时的二阶和三阶弹性常数(SOECs和TOECs)。利用得到的SOECs的力学性能,如杨氏模量、体积模量、剪切模量、Pugh指标、齐纳各向异性常数和泊松比在室温下进行了评价。PGM碳化物的Pugh指示值小于或接近等于1.75,材料表现出脆性。同样,超声声速的值被用来计算超声波沿波传播的纵向和剪切模式的速度和方向。利用SOECs、TOECs、超声速度、密度和分子量计算了Debye温度、导热系数、单位体积比热、能量密度、超声grisen参数平均值、热松弛时间、非线性参数。最后,利用所有相关参数计算了声子-声子相互作用和热弹性松弛机制引起的超声衰减。将弹性、力学、热物理和超声性能的计算值与现有文献进行了比较和讨论。
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引用次数: 0
“In Silico Dreams: How Artificial Intelligence and Biotechnology will Create the Medicines of the Future” 《硅谷之梦:人工智能和生物技术将如何创造未来的药物》
IF 2.3 4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651323x16904499234318
John G. Hardy
“In Silico Dreams: How Artificial Intelligence and Biotechnology will Create the Medicines of the Future” is authored by Brian Hilbush whose education in biosciences and career in the biotechnology and pharmaceutical sectors (developing and commercialising emerging and next-generation biotechnologies) offers significant insight into the application of bioinformatics (‘gold’ biotechnology) to understand and solve biological issues using computational techniques.
“在硅梦:人工智能和生物技术将如何创造未来的药物”是由Brian Hilbush撰写的,他在生物科学和生物技术和制药领域(开发和商业化新兴和下一代生物技术)的生物科学教育和职业生涯为生物信息学(“黄金”生物技术)的应用提供了重要的见解,以理解和解决使用计算技术的生物问题。
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引用次数: 0
Electrochemical Synthesis of Monodisperse PtCo Nanocrystals 单分散PtCo纳米晶的电化学合成
IF 2.3 4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651323x16799975192215
Daniel J. Rosen, Duncan Zavanelli, Christopher B. Murray
The synthesis of platinum-cobalt Nanocrystals (NCs) using colloidal solvothermal techniques is well understood. However, for monodisperse NCs to form, high temperatures and environmentally detrimental solvents are needed. We report a room temperature, aqueous method of Pt-Co NC synthesis using electrochemical reduction as the driving force for nucleation and growth. It is found that colloidal NCs will form in both the presence and absence of surfactant. Additionally, we report a monodisperse electrochemical deposition of nanocrystals utilizing a transparent conducting oxide electrode. The methods developed here will allow for a synthetic method to produce nanocatalysts with minimal environmental impact and should be readily applicable to other NC systems, including single- and multi-component alloys.
利用胶体溶剂热技术合成铂钴纳米晶体(NCs)已经得到了很好的理解。然而,要形成单分散的nc,需要高温和对环境有害的溶剂。我们报道了一种室温、水相合成Pt-Co NC的方法,利用电化学还原作为成核和生长的驱动力。研究发现,在表面活性剂存在和不存在的情况下,胶体纳米颗粒都会形成。此外,我们报告了利用透明导电氧化物电极的纳米晶体的单分散电化学沉积。这里开发的方法将允许一种合成方法来生产对环境影响最小的纳米催化剂,并且应该很容易适用于其他NC系统,包括单组分和多组分合金。
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引用次数: 0
Fabrication of Two-Dimensional Material Membranes 二维材料膜的制备
4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651324x16981367461019
Haowen Li, Qingqing Pan, Xiao Sui, Yuan Chen
Membrane separation is an energy-efficient separation process. Two-dimensional (2D) materials have shown potential as a new generation of membrane materials due to their unique structures and physio-chemical properties. The separation performance of 2D material membranes crucially depends on how 2D nanosheets are assembled in membranes, such as interlayer spacing between stacked nanosheets, chemical properties of nanosheet surfaces, alignment of nanosheets, and thickness of membranes, which are closely related to their fabrication methods. This short review concisely overviews commonly used membrane fabrication methods for different types of 2D materials, including graphene-based materials, 2D covalent organic frameworks, 2D metal-organic frameworks, MXenes, and other 2D materials. The representative 2D material membranes resulting from their essential fabrication methods are discussed. The advantages and shortcomings of different fabrication methods are compared. The critical challenges to realizing large-scale production of 2D material membranes for practical applications are highlighted.
膜分离是一种高效节能的分离工艺。二维(2D)材料由于其独特的结构和物理化学性质而显示出作为新一代膜材料的潜力。二维材料膜的分离性能在很大程度上取决于二维纳米片在膜中的组装方式,如堆叠纳米片之间的层间距、纳米片表面的化学性质、纳米片的排列以及膜的厚度,这些都与纳米片的制造方法密切相关。本文简要介绍了常用的二维材料的膜制备方法,包括石墨烯基材料、二维共价有机框架、二维金属有机框架、MXenes和其他二维材料。讨论了具有代表性的二维材料膜的基本制备方法。比较了不同制备方法的优缺点。强调了实现大规模生产用于实际应用的二维材料膜的关键挑战。
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引用次数: 0
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Johnson Matthey Technology Review
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