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Impact of Solution Chemistry on the Biotechnological Synthesis and Properties of Palladium Nanoparticles 溶液化学对钯纳米颗粒生物技术合成及性能的影响
IF 2.3 4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651323x16813753335431
Christopher Egan-Morriss, R. Kimber, N. A. Powell, J. Lloyd
The biosynthesis of Pd nanoparticles supported on microbial cells (bio-Pd) has attracted much recent interest, but the effect of solution chemistry on the process remains poorly understood. Biological buffers can be used to maintain physiological pH during the bioreduction of Pd(II) to Pd(0) by microbial cells, however, buffer components have the potential to complex Pd(II), and this may affect the subsequent microbe-metal interaction. In this study, a range of Pd(II) salts and biological buffers were selected to assess the impact of the solution chemistry on the rate of bioreduction of Pd(II) by Geobacter sulfurreducens, and the resulting biogenic Pd nanoparticles. The different buffer and Pd(II) combinations resulted in changes in the dominant Pd(II) species in solution, and this affected the amount of Pd recovered from solution by the microbial cells. The physical properties of the bio-Pd nanoparticles were altered under different solution chemistries; only slight variations were observed in the mean particle size (< 6 nm), but significant variations in particle agglomeration, the extent of Pd(II) bioreduction, and subsequent catalytic activity for the reduction of 4-nitrophenol were observed. The combination of sodium tetrachloropalladate and bicarbonate buffer resulted in bio-Pd with the smallest mean particle size, and the fastest initial rate of reaction for 4-NP reduction (0.33 min-1). Other solution chemistries appeared to damage the cells and result in bio-Pd with relatively poor catalytic performance. This work emphasises that future studies into bio-Pd synthesis should consider the importance of solution chemistry in controlling the speciation of Pd(II) and its impact on both the bioreduction process and the resulting properties of the nanoparticles produced, in order to maximize Pd(II) biorecovery and optimize catalytic properties.
微生物细胞支持的钯纳米颗粒的生物合成引起了人们的广泛关注,但溶液化学对这一过程的影响仍然知之甚少。在微生物细胞将Pd(II)生物还原为Pd(0)的过程中,生物缓冲液可用于维持生理pH值,然而,缓冲液成分有可能使Pd(II)复杂化,这可能会影响随后的微生物-金属相互作用。在这项研究中,选择了一系列Pd(II)盐和生物缓冲液来评估溶液化学对硫还原地球杆菌生物还原Pd(II)速率的影响,以及由此产生的生物源Pd纳米颗粒。不同的缓冲液和Pd(II)组合导致溶液中Pd(II)优势种的变化,从而影响微生物细胞从溶液中回收Pd的量。在不同的溶液化学条件下,生物钯纳米粒子的物理性质发生了变化;平均粒径(< 6 nm)变化不大,但颗粒团聚、Pd(II)生物还原程度以及随后对4-硝基苯酚还原的催化活性变化显著。四氯alladate钠和碳酸氢盐缓冲液的组合使bio-Pd具有最小的平均粒径和最快的4-NP还原初始反应速率(0.33 min-1)。其他溶液化学物质似乎会损害细胞,导致催化性能相对较差的生物钯。这项工作强调,未来的生物Pd合成研究应考虑溶液化学在控制Pd(II)形态及其对生物还原过程和所产生纳米颗粒性能的影响方面的重要性,以最大限度地提高Pd(II)的生物回收率和优化催化性能。
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引用次数: 0
Long-term Evaluation of Culturable Fungi in a Natural Aging Biofilm on Galvanized Steel Surface 镀锌钢表面自然老化生物膜中可培养真菌的长期评价
IF 2.3 4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651323x16748145957998
D. Kadaifçiler, T. Unsal, E. Ilhan‐Sungur
Fungi commonly found in municipal water can participate in the natural biofilm formation on the surfaces of galvanized steel despite the toxic effect of Zn, and also depending on the age of the biofilm, fungal diversity may vary. To examine this hypothesis, natural biofilm formation was allowed on galvanized steel surfaces over 6 months in a model recirculating water system. Fungal colonies with different morphologies were obtained monthly from biofilm and water samples and then identified by both morphological and molecular approaches. In addition, the biofilm layer was examined by electrochemistry impedance spectroscopy (EIS) analyses and scanning electron microscopy. It was determined that the fungi were included in the natural aging biofilm formed on the galvanized steel surfaces over the experiment. The diversity and the number of fungi in the biofilm and water changed over the experiment. All of the fungi isolated from the biofilm and water were found to be members of the Ascomycota phylum. F. oxysporum was the first fungus to be involved in the biofilm formation process and also it is one of the main inhabitants of the biofilm together with Penicillium spp. In addition, EIS data showed that the structure of the biofilm changed as it ages. The results of this study may lead to a better understanding of natural aging biofilms involving fungi in municipal water systems, as well as the development of new strategies for effective disinfection of fungi based on biofilm age.
尽管锌具有毒性作用,但市政用水中常见的真菌可以参与镀锌钢表面天然生物膜的形成,并且根据生物膜的年龄,真菌的多样性可能会有所不同。为了验证这一假设,在模型循环水系统中,允许在镀锌钢表面形成天然生物膜超过6个月。每月从生物膜和水样中获得不同形态的真菌菌落,然后通过形态学和分子方法进行鉴定。此外,采用电化学阻抗谱(EIS)和扫描电镜对生物膜层进行了检测。经实验确定,这些真菌包含在镀锌钢表面形成的自然老化生物膜中。生物膜和水中真菌的多样性和数量在实验过程中发生了变化。所有从生物膜和水中分离的真菌都属于子囊菌门。F. oxysporum是最早参与生物膜形成过程的真菌,与青霉属(Penicillium spp)一起是生物膜的主要居民。此外,EIS数据显示,随着生物膜的老化,生物膜的结构发生了变化。本研究结果可能有助于更好地了解城市供水系统中涉及真菌的自然老化生物膜,以及基于生物膜年龄的真菌有效消毒新策略的开发。
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引用次数: 0
Challenges and Opportunities for Platinum in the Modern Three-Way Catalyst 铂在现代三元催化剂中的挑战与机遇
IF 2.3 4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651323x16759335257118
M. Vlachou, H. R. Marchbank, E. Brooke, A. Kolpin
Gasoline vehicles have generally relied upon a combination of palladium and rhodium for more than 25 years to facilitate the required oxidative and reductive reactions of CO, HCs, and NOx. Recently, steady increases in the price of palladium relative to platinum have fuelled demand to reincorporate platinum into TWCs. However, the fundamental properties of platinum, including susceptibility toward sintering and inhibition under typical gasoline operating conditions, present significant challenges. This article presents an overview of the origins for these challenges, as well as select strategies for maximizing platinum’s contribution to modern-day TWCs. Optimisation of ceria-zirconia supports is one route by which platinum’s performance can be significantly improved through tuning of the ceria:zirconia ratio. Additionally, alloying platinum with a secondary PGM, e.g. rhodium, leverages complimentary properties of both metals, imparting stability and overall activity enhancements. Such routes not only enable PGM flexibility, but also provide opportunities to further improve TWC performance.
汽油车通常依赖钯和铑的组合超过25年,以促进所需的CO, hc和NOx的氧化和还原反应。最近,钯相对于铂金的价格稳步上涨,推动了将铂金重新纳入twc的需求。然而,铂的基本性质,包括在典型汽油操作条件下的烧结敏感性和抑制性,提出了重大挑战。本文概述了这些挑战的起源,以及最大化铂对现代twc的贡献的选择策略。优化二氧化铈支撑是通过调整二氧化铈比来显著改善铂性能的一种途径。此外,将铂与次级PGM(例如铑)合金化,利用两种金属的互补特性,赋予稳定性和整体活性增强。这些路线不仅使PGM具有灵活性,而且为进一步提高TWC性能提供了机会。
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引用次数: 2
Advertisement: Johnson Matthey Virtual Platinum Group Metal Conference 2023 广告:庄信万丰虚拟铂金集团金属会议2023
IF 2.3 4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651323x16869233430585
Emma Schofield
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引用次数: 0
Rhodium and Rhodium-Alloy Films and Nanoparticles 铑和铑合金薄膜和纳米颗粒
IF 2.3 4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651324x16794770872879
Yicheng Zhou, Wangping Wu, Qinqin Wang, Liangbing Wang
Noble metals are key to various research fields and Noble metal nanomaterials are directly relevant to optics, catalysis, medicine, sensing and many other applications. Rhodium-based nanomaterials have been less studied than metals such as gold, silver or platinum. There have been leaps and bounds in characterization tools over the years, and knowledge about rhodium chemistry and nanomaterials are expected to grow. With high expectations driving the use of rhodium nanoparticles as catalysts for automotive exhaust gas, catalysts for hydrogen and oxygen precipitation reactions in electrolytic cells, the established applications of rhodium materials in fields such as electronics and appliances, anti-cancer drugs and aerospace are being revisited. This review covers different strategies for the synthesis of rhodium films and nanoparticles and provides a broad overview of the reported applications.
贵金属是各个研究领域的关键,贵金属纳米材料直接关系到光学、催化、医学、传感等许多应用。与金、银或铂等金属相比,对铑基纳米材料的研究较少。多年来,表征工具的发展突飞猛进,有关铑化学和纳米材料的知识也有望增长。随着人们对铑纳米颗粒作为汽车废气催化剂、电解电池中氢和氧沉淀反应催化剂的期望越来越高,铑材料在电子和电器、抗癌药物和航空航天等领域的既定应用正在重新审视。这篇综述涵盖了铑薄膜和纳米颗粒合成的不同策略,并提供了广泛的应用综述。
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引用次数: 0
Impact of Fermentation Conditions and Purification Strategy on Bacterial Cellulose Properties 发酵条件和纯化策略对细菌纤维素性质的影响
IF 2.3 4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651323x16794186402492
H. Yu, Kacper Bruzda, D. Charalampopoulos, A. Chatzifragkou
Bacterial cellulose (BC) has attracted much research interest, delivering a combination of exclusive properties, such as flexibility, hydrophilicity, crystallinity, and a three-dimensional network. In this study, the effects of carbon source and cultivation conditions on BC production by the bacterium Komagataeibacter xylinus subsp. sucrofermentans DSM 15973 were assessed. Fructose was the most suitable carbon source and high BC concentrations up to 31 g/L were achieved in substrates with 60 g/L fructose, under static culture conditions. Notably, BC production was equally high under the same fermentation conditions in agitated cultures (~30 g/L). Moreover, the effectiveness of NaOH and NaOCl solutions in BC purification, and their potential impact on BC structure and properties were explored. The combination of weak NaOH and sodium hypochlorite (NaOCl) was proved an effective purification method, preserving the fibre structure and crystallinity of BC.
细菌纤维素(BC)由于具有柔韧性、亲水性、结晶性和三维网络等独特特性,引起了广泛的研究兴趣。本研究研究了碳源和培养条件对木质菌Komagataeibacter xylinus subsp生产BC的影响。对sucrofermentans DSM 15973进行评估。果糖是最合适的碳源,在静态培养条件下,在含有60 g/L果糖的培养基中,BC浓度高达31 g/L。值得注意的是,在相同的发酵条件下,在搅拌培养中,BC的产量同样高(~30 g/L)。此外,还探讨了NaOH和NaOCl溶液在BC净化中的效果,以及它们对BC结构和性能的潜在影响。弱氢氧化钠和次氯酸钠(NaOCl)结合是一种有效的净化方法,可以保持BC的纤维结构和结晶度。
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引用次数: 0
Moving from Fuel to Feedstock: Selective Hydrocarbon Activation using Rhodium and Iridium Complexes 从燃料到原料:使用铑和铱配合物的选择性碳氢化合物活化
IF 2.3 4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651323x16765646706676
Paul A. Morton, S. M. Mansell
Carbon-hydrogen bond activations and their subsequent functionalisation have long been an important target in chemistry because C-H bonds are ubiquitous throughout nature, making C-H derivatisation reactions highly desirable. The selective and efficient functionalisation of this bond into many more useful carbon-element bonds (e.g., C-B, C-Si, C-O, and C-S bonds) would have many uses in pharmaceutical and bulk chemical synthesis. Activation of the C-H bond is, however, challenging due to the high strength and low bond-polarity of this bond rendering its cleavage unfavourable. With the correct choice of reagents and systems, especially those utilising directing groups, kinetically and thermodynamically favourable catalytic processes have been developed. However, a key remaining challenge is the development of undirected, intermolecular reactions using catalysts that are both selective and active enough to make useful processes. In this review, the progress towards optimising group 9 C-H activation catalysts is discussed, particularly focusing on undirected reactions that are kinetically more difficult, starting with a brief history of C-H activation, identifying the importance of auxiliary ligands including the nature of anionic ligand (e.g., cyclopentadienyl, indenyl, fluorenyl, trispyrazolylborate) and neutral ligands (e.g., phosphines, carbonyl, alkenes, N-heterocyclic carbenes) that contribute towards the stability and reactivity of these metal complexes. The tethering of the anionic ligand to strong σ-donating ligands is also briefly discussed. The focus of this review is primarily on the group 9 metals rhodium and iridium, however, C-H activation using group 8 and 10 metals are compared where useful. The most recent advances in this field include the development of C-H borylation of many small hydrocarbon substrates such as arenes, heterocycles and n-alkanes as well as the more challenging substrate methane.
碳氢键的活化及其随后的功能化一直是化学领域的重要目标,因为碳氢键在自然界中无处不在,使得碳氢衍生化反应非常理想。该键选择性和高效功能化成许多更有用的碳元素键(例如,C-B, C-Si, C-O和C-S键)将在制药和大宗化学合成中有许多用途。然而,激活碳氢键是具有挑战性的,因为这种键的高强度和低键极性使得它的裂解不利。随着试剂和体系的正确选择,特别是那些利用导向基团的,在动力学和热力学上有利的催化过程已经发展起来。然而,仍然存在的一个关键挑战是开发无方向的分子间反应,使用具有选择性和活性的催化剂来进行有用的过程。在这篇综述中,讨论了优化9族C-H活化催化剂的进展,特别关注那些在动力学上更困难的无向反应,从C-H活化的简史开始,确定辅助配体的重要性,包括阴离子配体的性质(如环戊二烯基、独立基、氟烯基、三吡唑硼酸盐)和中性配体(如膦、羰基、烯烃、n -杂环碳烯)有助于这些金属配合物的稳定性和反应性。本文还简要讨论了阴离子配体与强给σ配体的系结。本综述的重点主要是9族金属铑和铱,然而,在有用的地方比较了8族和10族金属的C-H活化。该领域的最新进展包括许多小碳氢化合物底物如芳烃、杂环和正构烷烃以及更具挑战性的底物甲烷的C-H硼化反应的发展。
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引用次数: 0
Hydrogen Spillover Mechanisms on Cu/ZnO-Based Catalysts for CO2 Hydrogenation to Methanol Cu/ zno基催化剂对CO2加氢制甲醇的氢溢出机理
4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2023-01-01 DOI: 10.1595/205651324x16980703569747
Mustafa Al Salmi
This literature review examines the hydrogen spillover mechanisms on Cu/ZnO-based catalysts for CO2 hydrogenation to methanol. The production of methanol from CO2 is an attractive process for mitigating greenhouse gas emissions and producing a valuable chemical feedstock. Cu/ZnO-based catalysts are known to exhibit high activity and selectivity towards methanol production, and the hydrogen spillover effect is believed to play a crucial role in their performance. The review discusses the current understanding of the hydrogen spillover mechanism, including the nature of the active sites and the factors that affect spillover efficiency. It also summarizes the recent advances in catalyst design, such as the use of promoters and dopants, to enhance the hydrogen spillover effect and improve catalytic performance. This article provides a comprehensive overview of the hydrogen spillover mechanism on Cu/ZnO-based catalysts for CO2 hydrogenation to methanol, highlighting the potential of this technology for sustainable methanol production.
本文综述了Cu/ zno基催化剂对CO2加氢制甲醇的氢溢出机理。从二氧化碳中生产甲醇是减少温室气体排放和生产有价值的化学原料的一个有吸引力的过程。Cu/ zno基催化剂对甲醇生产具有高活性和选择性,氢溢出效应被认为在其性能中起着至关重要的作用。综述了目前对氢溢出机制的认识,包括活性位点的性质和影响溢出效率的因素。总结了近年来在催化剂设计方面的最新进展,如促进剂和掺杂剂的使用,以增强氢溢出效应,提高催化性能。本文全面概述了Cu/ zno基催化剂用于CO2加氢制甲醇的氢溢出机制,强调了该技术在可持续甲醇生产中的潜力。
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引用次数: 0
Emergency Medical Response for Non-Hospitalized Person Events in a Children's Hospital. 儿童医院对非住院病人事件的紧急医疗响应。
IF 8 4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2022-03-15 DOI: 10.1542/hpeds.2021-006268
Olivia L Hoffman, Jane Romano, Monica E Kleinman

Objectives: Hospital-based code blue (CB) teams are designed for hospitalized patients (HP) with unanticipated medical emergencies outside of an ICU. At our freestanding pediatric institution, the same team responds to CB calls involving nonhospitalized persons (NHP) throughout the hospital campus. We hypothesized there are significant differences between the characteristics of NHP and HP requiring emergency medical response, and most responses for NHP do not require advanced critical care.

Methods: We analyzed a retrospective cohort of CB responses at our large, urban, academic children's medical center from January to December 2017. We evaluated the demographic and clinical characteristics of these HP compared with NHP events.

Results: There were 168 CB activations during the study, of which 135 (80.4%) were for NHP. Ninety-one (67.4%) of the NHP responses involved adults (age >18 years) compared with 6 (18.2%) of the HP. Triggers for CB team activation for NHP were most frequently syncope (42.2%), seizure (10.3%), or fall (9.6%) compared with seizure (30.3%), hypoxia (27.3%), or anaphylaxis (12.1%) for HP. Critical interventions such as bag-mask ventilation and cardiopulmonary resuscitation were infrequently performed for either cohort.

Conclusions: CB activations in our pediatric institution more often involve NHP than HP. NHP responses are more likely to involve adults and infrequently require advanced interventions. Use of a pediatric CB team for NHP events may be an unnecessary use of pediatric critical care resources. Future studies are warranted to evaluate the most effective team composition, training, and response system for NHP in a freestanding children's hospital.

目标:以医院为基础的蓝色代码(CB)小组是为在重症监护室以外出现意外医疗紧急情况的住院病人(HP)而设计的。在我们的独立儿科机构中,同一小组负责处理整个医院园区内涉及非住院病人(NHP)的蓝色代码呼叫。我们假设需要紧急医疗响应的 NHP 和 HP 的特征之间存在显著差异,而且大多数 NHP 响应不需要高级重症监护:我们分析了2017年1月至12月在我们的大型城市学术儿童医学中心发生的CB反应的回顾性队列。我们评估了这些 HP 与 NHP 事件相比的人口统计学和临床特征:研究期间共启动了 168 次 CB,其中 135 次(80.4%)是针对 NHP 的。91起(67.4%)国家卫生标准回应涉及成年人(年龄大于 18 岁),而 HP 回应只有 6 起(18.2%)。对 NHP 而言,启动 CB 小组的诱因最常见的是晕厥(42.2%)、癫痫发作(10.3%)或跌倒(9.6%),而对 HP 而言,则是癫痫发作(30.3%)、缺氧(27.3%)或过敏性休克(12.1%)。在这两组人群中,均很少采取关键性干预措施,如面罩通气和心肺复苏:结论:在我们的儿科机构中,CB 激活更多涉及 NHP 而非 HP。结论:在我们的儿科机构中,CB 启动更多涉及 NHP,而非 HP。NHP 响应更多涉及成人,并且很少需要高级干预。在 NHP 事件中使用儿科 CB 小组可能会不必要地使用儿科重症监护资源。未来有必要进行研究,以评估独立儿童医院中最有效的团队组成、培训和 NHP 响应系统。
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引用次数: 0
Using Spraying as an Alternative Method for Transferring Capsules Containing Shea Butter to Denim and Non-Denim Fabrics : Preparation of microcapsules for delivery of active ingredients 使用喷雾作为将含有乳木果油的胶囊转移到牛仔布和非牛仔布织物上的替代方法:制备用于传递活性成分的微胶囊
IF 2.3 4区 化学 Q4 CHEMISTRY, PHYSICAL Pub Date : 2022-01-11 DOI: 10.1595/205651322x16376750190432
İ. İvedi, Bahadır Güneşoğlu, S. Karavana, G. Kartal, G. Erkan, A. M. Sarıışık
The aim of this study was to prepare microcapsules and transfer them to denim and non-denim trousers using different application methods. For this purpose, shea butter as active agent was encapsulated in an ethyl cellulose shell using the spray dryer method, and capsule optimisation was studied. A morphological assessment showed that the capsules had a smooth surface and were spherical in shape. The homogenous size distribution of the capsules was supported by laser diffraction analysis. The capsules showed a narrow size distribution, and the mean particle size of optimum formulations of shea butter was 390 nm. Denim fabrics were treated with shea butter capsules using the methods of exhaustion and spraying in order to compare these application methods. The presence of capsules on the fabrics was tested after five wash cycles. The comparison of application methods found similar preferred characteristics for both the exhaustion and spraying methods. However, the spraying method was found to be more sustainable, because it allows working with low liquor ratios in less water, with lower chemical consumption and less waste than the exhaustion method, which requires working with a high liquor ratio. This study showed that the spraying method can be used as an alternative to other application methods in the market for reducing energy consumption, and shea butter capsules can provide moisturising properties to the fabrics.
本研究的目的是制备微胶囊,并使用不同的应用方法将其转移到牛仔和非牛仔长裤上。为此,使用喷雾干燥器方法将乳木果油作为活性剂封装在乙基纤维素外壳中,并对胶囊优化进行了研究。形态学评估显示,胶囊表面光滑,呈球形。激光衍射分析支持了胶囊的均匀尺寸分布。胶囊显示出窄的尺寸分布,最佳乳木果油配方的平均粒径为390nm。采用乳木果油胶囊对牛仔布进行处理,分别采用脱脂法和喷雾法对两种处理方法进行比较。在五次洗涤循环后测试织物上胶囊的存在。对施用方法的比较发现,耗竭和喷洒方法具有相似的优选特征。然而,发现喷洒方法更具可持续性,因为与需要高液比的耗竭方法相比,它允许在更少的水中以低液比进行工作,具有更低的化学消耗和更少的浪费。这项研究表明,喷洒方法可以作为市场上其他应用方法的替代方法,以降低能耗,乳木果油胶囊可以为织物提供保湿性能。
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引用次数: 1
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Johnson Matthey Technology Review
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