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Catalyzing Transformation: Organo-Inorganic Materials Based Immobilized Lipases in the Ongoing Quest for Sustainable Biodiesel Production 催化转化:基于有机-无机材料的固定化脂肪酶在可持续生物柴油生产中的不断探索
IF 2.8 3区 化学 Q2 CHEMISTRY, APPLIED Pub Date : 2024-02-26 DOI: 10.1007/s11244-024-01915-x
Alvina Khalid, Muhammad Imran, Ayesha Javaid, Shoomaila Latif

The ever-increasing demand for sustainable diesel production, driven by depleting fossil fuel reserves, escalating prices, and environmental concerns has led to an intensive exploration of biodiesel as an alternative. Although chemical catalysis has been a dominant strategy for biodiesel synthesis due to its rapid reaction rates, its limitations in handling low-grade feedstock, susceptibility to product contamination, and high-temperature and pressure demands have prompted a paradigm shift toward lipase catalysis. Lipases, renowned for their ability to function under moderate conditions and prevent product contamination, present an appealing substitute. However, their extensive adoption is hindered by their inherent high cost. To address this challenge, investigators have turned their attention to immobilizing lipases on various support materials, aiming to enhance stability and recyclability and ultimately make lipase-catalyzed biodiesel economically viable on a commercial level. This review provides a comprehensive overview of the raw materials employed, the lipase action mechanism at the interfacial level, and a detailed discussion of the recent works carried out in both traditional and innovative immobilization techniques. The discussion encompasses diverse support materials and factors influencing biodiesel manufacturing, thereby illuminating the dynamic landscape of immobilized lipases in the synthesis of biodiesel. Throughout this paper, our objective is to furnish insights into the current state of the field, pinpoint key challenges, and articulate a roadmap for future research endeavors in the pursuit of sustainable and economically viable biodiesel production.

Graphical Abstract

由于化石燃料储量日益枯竭、价格不断攀升以及对环境的担忧,人们对可持续柴油生产的需求不断增加,这促使人们开始深入探索生物柴油的替代品。虽然化学催化因其反应速度快而一直是生物柴油合成的主要策略,但其在处理低级原料、易受产品污染以及高温高压要求等方面的局限性,促使人们向脂肪酶催化转变。脂肪酶以能够在温和条件下发挥作用和防止产品污染而闻名,是一种极具吸引力的替代品。然而,其固有的高成本阻碍了它们的广泛应用。为了应对这一挑战,研究人员已将注意力转向将脂肪酶固定在各种支持材料上,旨在提高稳定性和可回收性,最终使脂肪酶催化的生物柴油在商业层面上具有经济可行性。本综述全面概述了所采用的原材料、脂肪酶在界面层面的作用机制,并详细讨论了最近在传统和创新固定化技术方面开展的工作。讨论涵盖了各种支持材料和影响生物柴油制造的因素,从而揭示了固定化脂肪酶在生物柴油合成中的动态发展。在本文中,我们将深入探讨该领域的现状,指出主要挑战,并为未来的研究工作绘制路线图,以实现可持续的、经济可行的生物柴油生产。
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引用次数: 0
Detection and Determination of Quercetin in Sour Cherry and Black Tea Samples by Fluorescent Probe Prepared by Green Hydrothermal Method Using Achillea Millefolium Extract 利用绿色水热法制备的荧光探针检测和测定酸樱桃和红茶样品中的槲皮素(Achillea Millefolium Extract
IF 3.6 3区 化学 Q2 CHEMISTRY, APPLIED Pub Date : 2024-02-21 DOI: 10.1007/s11244-024-01914-y
Haniye Iranmanesh, Elham Ashrafzadeh Afshar, Mohammad Ali Taher, Ceren Karaman, Hassan Karimi-Maleh

Quercetin (QCT), as an important flavonoid, has different properties including neuroprotective, anti-hyperlipidemia, decreasing blood pressure and neuroprotective effects. Hence precise determination of quercetin is noteworthy. Herein, a fast, simple, highly sensitive, and new fluorescent sensor was prepared based on Achillea Millefolium extract carbon dots stabilized on sodium alginate structure (CD/Na-Al). For confirm the reliability of synthesized sensor some characterization analysis were performed such as FT-IR and TEM. The CD/Na-Al was applied for the accurate recognition and measurement of QCT molecule. The operation mechanism for the analytical procedure was based on ‘‘turn-off’’ the fluorescence emission signal in 440 nm. The dynamic linear range was obtained in the range of 1–25 and 25–110 µM, with detection of limits equal to 0.32 and 3.9 µM respectively. The observations confirmed that the present method was able to detect trace amounts of quercetin in black tea and sur cherry with satisfy results.

槲皮素(QCT)作为一种重要的类黄酮,具有不同的特性,包括神经保护、抗高脂血症、降低血压和神经保护作用。因此,精确测定槲皮素值得关注。本文基于海藻酸钠结构(CD/Na-Al)上稳定的蓍草提取物碳点,制备了一种快速、简单、高灵敏度的新型荧光传感器。为了证实合成传感器的可靠性,对其进行了一些表征分析,如傅立叶变换红外光谱和 TEM。CD/Na-Al 被用于准确识别和测量 QCT 分子。分析程序的运行机制基于 440 纳米波长的荧光发射信号 "关闭"。该方法的动态线性范围分别为 1-25 µM 和 25-110 µM,检测限分别为 0.32 µM 和 3.9 µM。结果表明,该方法能够检测出红茶和樱桃中的槲皮素,且结果令人满意。
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引用次数: 0
Tuning Catalytic Attributes of Enzymes by Conjugation with Functionalized Carbon Dots 通过与功能化碳点共轭调谐酶的催化属性
IF 2.8 3区 化学 Q2 CHEMISTRY, APPLIED Pub Date : 2024-02-21 DOI: 10.1007/s11244-024-01911-1
Angelica Cruz-Cruz, Andrea Rivas-Sanchez, Reyna Berenice González-González, Roberto Parra-Saldívar

Enzymes are essential biological catalysts that can accelerate multiple reactions. Their outstanding catalytic properties make them highly valuable in different research fields and industries including pharmaceutical, sensing, food, and agriculture. However, the catalytic attributes of free enzymes are limited by their poor stability and resistance to harsh conditions. Recently, the conjugation of different enzymes with carbon dots (CDs) has been explored as a novel strategy for tuning their catalytic properties. CDs possess unique and tunable characteristics such as light stability, electron transfer properties, lower toxicity, cost-efficiency, and outstanding biocompatibility; thus, they represent excellent options for the conjugation of different enzymes to improve their stability, selectivity, and catalytic efficiency. Recently, various CDs-based nano-biocatalysts have been successfully prepared with superior performances compared to their free enzymes. Therefore, this review aims to discuss the most recent reported studies in the synthesis of CDs-based nano-biocatalysts providing an overview of current methodologies and recent research applications. Lastly, we delve into the prospects and the future possibilities of such innovative conjugates that entail an exploration of the faced challenges and their untapped potential for various applications.

Graphical Abstract

摘要 酶是一种重要的生物催化剂,可以加速多种反应。酶的卓越催化特性使其在制药、传感、食品和农业等不同研究领域和行业中具有极高的价值。然而,游离酶的催化特性因其稳定性差和对恶劣条件的耐受性而受到限制。最近,人们探索了将不同的酶与碳点(CD)共轭,作为调整其催化特性的一种新策略。碳点具有独特的可调特性,如光稳定性、电子传递特性、低毒性、成本效益和出色的生物相容性;因此,它们是缀合不同酶以提高其稳定性、选择性和催化效率的绝佳选择。最近,人们成功制备了各种基于 CD 的纳米生物催化剂,其性能优于游离酶。因此,本综述旨在讨论有关合成 CD 基纳米生物催化剂的最新研究报告,概述当前的方法和最新的研究应用。最后,我们将深入探讨此类创新型共轭物的前景和未来可能性,包括所面临的挑战及其在各种应用中尚未开发的潜力。 图表摘要
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引用次数: 0
Hydrogen Generation by Methanolysis of NaBH4 via Efficient CuFe2O4 Nanoparticle Catalyst: A Kinetic Study and DNN Model 通过高效 CuFe2O4 纳米粒子催化剂甲烷分解 NaBH4 产生氢气:动力学研究和 DNN 模型
IF 3.6 3区 化学 Q2 CHEMISTRY, APPLIED Pub Date : 2024-02-20 DOI: 10.1007/s11244-024-01904-0
Muhammad Ali Yousif Al Janabi, Rima Nour El Houda Tiri, Ali Cherif, Elif Esra Altuner, Chul-Jin Lee, Fatih Sen, Elena Niculina Dragoi, Fatemeh Karimi, Shankramma Kalikeri

In this work, CuFe2O4 nanoparticles (NPs) were created using a hydrothermal process. The form and size of the obtained CuFe2O4 NPs were characterized using XRD and TEM techniques. The Scherrer equation and XRD measurements revealed that the crystal size of nanoparticles was 10.79 nm. The TEM study of nanoparticles with an average size of 7.673.75 nm revealed a distinctive core–shell structure. The methanolysis on NaBH4 at various parameters was used to assess the catalytic activity of NPs. The results showed that CuFe2O4 NPs are an effective catalyst for the methanolysis of NaBH4 in alkaline solutions, as demonstrated by the activation energy of 33.31 kJ/mol and turnover frequency (TOF), which was estimated as 2774.61 min−1 under ambient circumstances. These obtained NPs also showed an excellent (92%) reusability. A deep neural network architecture was determined using a neuro-evolutive approach based on a genetic algorithm to model the process and predict the catalyst performance in changing operating conditions. The determined models had a correlation > 0.9 and a mean squared error in the testing phase < 7.5%, indicating their capacity to capture the process dynamic effectively.

本研究采用水热法制备了 CuFe2O4 纳米粒子(NPs)。利用 XRD 和 TEM 技术对获得的 CuFe2O4 NPs 的形态和尺寸进行了表征。舍勒方程和 XRD 测量显示,纳米粒子的晶体尺寸为 10.79 nm。对平均尺寸为 7.673.75 nm 的纳米颗粒进行的 TEM 研究表明,它们具有独特的核壳结构。在不同参数下对 NaBH4 进行甲醇分解,以评估纳米粒子的催化活性。结果表明,CuFe2O4 NPs 是碱性溶液中 NaBH4 甲醇分解的有效催化剂,其活化能为 33.31 kJ/mol,周转频率(TOF)为 2774.61 min-1。这些获得的 NPs 还显示出极佳的重复利用率(92%)。利用基于遗传算法的神经进化方法确定了深度神经网络架构,以建立工艺模型并预测催化剂在不断变化的操作条件下的性能。确定的模型在测试阶段的相关性为 0.9,平均平方误差为 7.5%,这表明它们能够有效捕捉工艺动态。
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引用次数: 0
Prospecting Carbon-Based Nanomaterials for Harnessing Multienzyme-Like Activities 探索利用类多酶活性的碳基纳米材料
IF 2.8 3区 化学 Q2 CHEMISTRY, APPLIED Pub Date : 2024-02-20 DOI: 10.1007/s11244-024-01910-2
Iqra Batool, Ayesha Anwar, Muhammad Imran, Zara Idress Alvi
<div><p>Nanozymes (NZs), or nanostructures exhibiting enzyme mimicking exertion, have drawn a lot of attention recently owing to their ability to substitute enzymes that are naturally occurring in an array of bio-medical applications, notably biological detection, therapeutics, pharmaceutical administration, as well as biological imaging. In comparison to single enzymatic NZs, multi-enzymatic NZs have additional benefits, especially improved selectivity, a more favorable ecological impact, and synergistic effects. In contrast, the catalytic mechanism and rational design of multi-enzymatic NZs are more complex than those of single enzymatic NZs, which have simple catalytic mechanisms. NZs that can regulate cellular redox equilibrium by emulating the antioxidant enzymes in cells are particularly crucial towards alleviating ailments induced on by cellular oxidative stress. Carbonaceous materials i.e. graphene, fullerenes, quantum dots, carbon nano-sheets, nano-rods, MOFs etc. demonstrated peroxidase (POD), oxidase (OXD), superoxide dismutase (SOD), and catalase (CAT)-like functioning in a range of domains on the basis of oxidation mitigation mechanisms employing electron transport channels. Furthermore, integrating a couple of hetero-atoms to carbon-based materials enhanced their efficacy in various industries. NZs derived from bioactive materials demonstrate catalytic properties similar to those of enzymes. Bioactive material-based NZs are essential because of their unique catalytic properties, which surpass the efficiency, selectivity, and flexibility of traditional catalysts moreover, offering a cost-effective and environmentally friendly alternative to conventional precursors in catalysis. Their surfaces can be precisely modified, opening up new possibilities for selective and green synthetic techniques. Bioactive materials-based NZs have exceptional biological activity and compatibility in the field of medicine, thus rendering them useful instruments for both diagnosis and therapy. Due to their innate capacity to imitate the catalytic functions of natural enzymes, they can be utilized to develop intricate bio-sensors, precise drug delivery systems, and extremely sensitive diagnostic platforms. Moreover, low cytotoxicity of these materials facilitates the easier integration of chemicals into biological systems. This review provided an overview of the multi-enzymatic activities of rationally designed carbon-based NMs, both the internal and external variables that regulate the multi-enzymatic enzymes endeavours, and current advancements in application areas which benefit from multi-enzymatic distinctive characteristics. Prospective uses and development of multi-enzymatic carbon-based NZs might confront multiple challenges. This review aims to stimulate and improve our understanding of multi-enzymatic carbon-based processes to a greater extent.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></di
纳米酶(NZs),即具有酶模仿能力的纳米结构,由于其能够在一系列生物医学应用中替代天然存在的酶,特别是在生物检测、治疗、药物管理以及生物成像方面,近来引起了广泛关注。与单酶 NZs 相比,多酶 NZs 具有更多优点,尤其是选择性更强、对生态环境的影响更有利以及具有协同效应。相比之下,多酶 NZs 的催化机理和合理设计要比催化机理简单的单酶 NZs 复杂得多。通过模拟细胞中的抗氧化酶来调节细胞氧化还原平衡的 NZs 对于缓解细胞氧化应激引起的疾病尤为重要。碳质材料,如石墨烯、富勒烯、量子点、碳纳米片、纳米棒、MOFs 等,在利用电子传输通道的氧化缓解机制的基础上,在一系列领域展示了类似过氧化物酶 (POD)、氧化酶 (OXD)、超氧化物歧化酶 (SOD) 和过氧化氢酶 (CAT) 的功能。此外,在碳基材料中加入几个杂原子也提高了它们在各行各业中的功效。从生物活性材料中提取的 NZ 具有与酶类似的催化特性。基于生物活性材料的 NZs 具有独特的催化特性,其催化效率、选择性和灵活性都超过了传统催化剂,是催化领域中传统前体的一种具有成本效益且环保的替代品,因此非常重要。它们的表面可以精确修饰,为选择性和绿色合成技术开辟了新的可能性。基于生物活性材料的 NZs 在医学领域具有卓越的生物活性和兼容性,因此成为诊断和治疗的有用工具。由于它们天生具有模仿天然酶催化功能的能力,因此可用于开发复杂的生物传感器、精确的给药系统和极其灵敏的诊断平台。此外,这些材料的细胞毒性低,使化学物质更容易融入生物系统。本综述概述了合理设计的碳基 NMs 的多酶活性、调节多酶工作的内部和外部变量,以及受益于多酶独特特性的应用领域的当前进展。多酶碳基 NZ 的未来用途和发展可能面临多重挑战。本综述旨在促进和提高我们对多酶碳基工艺的理解。
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引用次数: 0
Enhanced Activity and Water Resistance on CuO/SiO2-TiO2 Catalyst for CO Oxidation and NO Reduction by CO: The Promotion Effect of SiO2 增强 CuO/SiO2-TiO2 催化剂的活性和耐水性,促进 CO 氧化和 CO 还原 NO:SiO2 的促进作用
IF 3.6 3区 化学 Q2 CHEMISTRY, APPLIED Pub Date : 2024-02-19 DOI: 10.1007/s11244-024-01917-9

Abstract

Non-precious metal catalysts with enhanced low-temperature activity and improved water resistance are highly demanded for emission control. CuO-based catalysts are promising alternatives to precious metal catalysts due to their acceptable activity and cost-effectiveness. However, there is an urgent need to further enhance their low-temperature activity and water resistance for industrial applications. Herein, CuO catalysts supported by various SiO2-TiO2 supports were prepared and evaluated for CO oxidation and NO reduction by CO reactions under the testing conditions with and without water. Among the studied catalysts with different SiO2 contents, CuO/5SiO2-TiO2, in which CuO was supported by SiO2-TiO2 with 5 wt.% SiO2, exhibited the best performance for CO oxidation. Compared with CuO/TiO2 and CuO/SiO2 reference catalysts, the CuO/5SiO2-TiO2 catalyst showed enhanced catalytic activity in both CO oxidation and NO reduction by CO under dry and wet conditions. Comprehensive characterizations revealed that the presence of SiO2 in TiO2 support facilitated the CuO/5SiO2-TiO2 catalyst with a high dispersion and reduced oxidation states of CuOx species. This not only improved the low-temperature reducibility but also enhanced the adsorption of reactive CO species. As a result, the CuO/5SiO2-TiO2 catalyst demonstrated superior catalytic activity. Furthermore, the inclusion of SiO2 in the catalyst inhibited H2O adsorption, contributing to the enhanced water resistance on CuO/5SiO2-TiO2 catalyst. These advantages in catalytic activity and water resistance make CuO/5SiO2-TiO2 a promising candidate for applications in emission control.

摘要 排放控制领域对低温活性更强、耐水性更好的非贵金属催化剂的需求量很大。氧化铜基催化剂具有可接受的活性和成本效益,是贵金属催化剂的有前途的替代品。然而,工业应用迫切需要进一步提高其低温活性和耐水性。本文制备了由不同二氧化硅-二氧化钛(SiO2-TiO2)载体支撑的氧化铜催化剂,并对其在有水和无水试验条件下通过 CO 反应氧化 CO 和还原 NO 的性能进行了评估。在所研究的不同 SiO2 含量的催化剂中,CuO 被含 5 wt.% SiO2 的 SiO2-TiO2 支持的 CuO/5SiO2-TiO2 的 CO 氧化性能最好。与 CuO/TiO2 和 CuO/SiO2 参考催化剂相比,CuO/5SiO2-TiO2 催化剂在干法和湿法条件下 CO 氧化和 CO 还原 NO 的催化活性都有所提高。综合表征结果表明,TiO2 载体中 SiO2 的存在促进了 CuO/5SiO2-TiO2 催化剂的高度分散,并降低了 CuOx 物种的氧化态。这不仅提高了低温还原性,还增强了对活性 CO 物种的吸附。因此,CuO/5SiO2-TiO2 催化剂表现出更高的催化活性。此外,催化剂中 SiO2 的加入抑制了 H2O 的吸附,从而增强了 CuO/5SiO2-TiO2 催化剂的耐水性。CuO/5SiO2-TiO2 催化剂在催化活性和耐水性方面的这些优势使其在排放控制领域的应用前景广阔。
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引用次数: 0
Environmental Energy Production and Wastewater Treatment Using Synthesized Pd Nanoparticles with Biological and Photocatalytic Activity 利用具有生物和光催化活性的合成钯纳米粒子进行环境能源生产和废水处理
IF 3.6 3区 化学 Q2 CHEMISTRY, APPLIED Pub Date : 2024-02-18 DOI: 10.1007/s11244-024-01912-0

Abstract

Metallic nanoparticles have attracted great attention in catalytic, medical diagnosis, and treatment research in recent years. The formation of palladium nanoparticles using rosemary (Rosmarinus officinalis L.) extract was carried out using the green synthesis method. The plant was extracted using 70% ethanol by microwave techniques. The novelty of this study is the investigation of the biological activities of green synthesis of Pd nanoparticles, such as DNA cleavage activity, antimicrobial activity, DPPH scavenging activity, and its electro-catalytic performance in alcohol oxidation. Additionally, photocatalytic activities were also evaluated. The characterization of synthesized palladium nanoparticles (Pd NPs) was performed by UV-spectrometry, XRD, FTIR, and TEM. According to TEM results, Pd nanoparticles were observed to have a spherical shape and an average particle size of 4.91 nm. The Pd NPs showed the photodegradation of MB solution by up to 79.9% at 120 min. The newly synthesized plant-mediated green synthesized Pd NPs showed the max and the min antimicrobial activity at 16 µg/mL and 256 µg/mL against L. pneumophila and C. albicans, respectively. The current density ratio of 48.22 mA/cm2 obtained in the study indicates that the obtained materials may be of interest in different applications. According to the results obtained, a direct relationship of extract use is observed in the synthesis of Pd nanoparticles and is a good way to reduce and stabilize metal salts. It has been determined that green Pd NPs have potential for use in energy production from alcohol oxidation and in medical applications.

摘要 近年来,金属纳米粒子在催化、医疗诊断和治疗研究中备受关注。本研究采用绿色合成法,利用迷迭香(Rosmarinus officinalis L.)提取物制备了钯纳米粒子。采用微波技术用 70% 的乙醇提取迷迭香。本研究的新颖之处在于研究了绿色合成钯纳米粒子的生物活性,如 DNA 裂解活性、抗菌活性、DPPH 清除活性及其在酒精氧化中的电催化性能。此外,还对光催化活性进行了评估。合成的钯纳米粒子(Pd NPs)通过紫外光谱、XRD、傅里叶变换红外光谱和 TEM 进行了表征。根据 TEM 结果,钯纳米粒子呈球形,平均粒径为 4.91 nm。Pd NPs 在 120 分钟内对甲基溴溶液的光降解率高达 79.9%。新合成的植物介导绿色合成 Pd NPs 对嗜肺菌和白僵菌的最大和最小抗菌活性分别为 16 µg/mL 和 256 µg/mL。研究中获得的电流密度比为 48.22 mA/cm2,这表明所获得的材料在不同的应用中可能会产生兴趣。根据所得结果,萃取物的使用与钯纳米粒子的合成有直接关系,是减少和稳定金属盐的好方法。经确定,绿色钯纳米粒子在利用酒精氧化生产能源和医疗应用方面具有潜力。
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引用次数: 0
Graph Theory in Chemical Kinetics Practice Problems 化学动力学中的图形理论练习题
IF 3.6 3区 化学 Q2 CHEMISTRY, APPLIED Pub Date : 2024-02-15 DOI: 10.1007/s11244-024-01918-8
Mirosław K. Szukiewicz, Elżbieta Chmiel-Szukiewicz, Adrian Szałek

In this work, a novel idea for obtaining in processes performed in real-world processes (here, the illustrative example is the gas phase hydrogenation of propene) a precise kinetic equation that corresponds to the experimental results was examined. The considerations are based on quasi-steady-state hypothesis and using elements of graph theory. The mathematical basis of the method used was developed by Lazman and Yablonsky [1], further considerations are presented in Yablonski et al. [2], Marin et al. [3]. The exemplary derivations of kinetic equations without simplifications are presented in the aforementioned works. The lack of assumptions allows consideration of all possible interactions between the reagents and the surface species, which is a pro of the method. However, the equation obtained usually has a complex form. Some of the parameters that result from theoretical considerations are simply insignificant for the real-world process. To eliminate this problem, the original procedure, based on statistical and process analysis, was employed. The previously determined kinetic equation, which does not have additional assumptions, was simplified. Statistical analysis helps to find and justify possible simplifications of the kinetic equation by eliminating insignificant parameters present in the kinetic equation and provides strong evidence for the correctness of the approach. The resulting kinetic equation indicates that the new proposed mechanism for the propene hydrogenation process that accepts reactions between adsorbed propene and gaseous hydrogen corresponds to the experiment. The residual sum of squares is significantly lower than those for the equations presented in the literature. The statistical test (the Akaike criterion) also indicates that the new model is better than the others. The results obtained indicate that the commonly applied approach based on the rate-determining step concept has become obsolete, apart from obvious cases. The application of the more advanced mathematical approach gives better results, as was presented.

在这项工作中,研究了一种新的想法,即在实际过程中(此处以丙烯的气相氢化为例)获得与实验结果相对应的精确动力学方程。这些考虑基于准稳态假设,并使用了图论元素。所使用方法的数学基础由 Lazman 和 Yablonsky [1] 提出,Yablonski 等人[2]和 Marin 等人[3]提出了进一步的考虑。上述著作介绍了不加简化的动力学方程的示例推导。由于没有假设,因此可以考虑试剂和表面物种之间所有可能的相互作用,这是该方法的优点。然而,得到的方程通常形式复杂。一些从理论上得出的参数对于实际过程来说根本不重要。为了解决这个问题,我们采用了基于统计和过程分析的原始程序。之前确定的动力学方程没有额外的假设,因此进行了简化。通过消除动力学方程中不重要的参数,统计分析有助于找到动力学方程可能的简化并证明其合理性,同时也为该方法的正确性提供了有力的证据。由此得出的动力学方程表明,新提出的丙烯加氢过程机制接受了吸附的丙烯和气态氢之间的反应,与实验相符。残差平方和明显低于文献中的方程。统计检验(Akaike 准则)也表明,新模型优于其他模型。所得结果表明,除了明显的情况外,基于速率决定步骤概念的常用方法已经过时。应用更先进的数学方法可以得到更好的结果,正如上文所述。
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引用次数: 0
Additive-Free Oxidative Cleavage of a Simple Lignin Model Compound in Air using Vanadium Complexes 利用钒络合物在空气中无添加地氧化裂解简单木质素模型化合物
IF 3.6 3区 化学 Q2 CHEMISTRY, APPLIED Pub Date : 2024-02-06 DOI: 10.1007/s11244-023-01902-8
Paul W. Musharbash, Jerome B. Torres, Tristhan Trieu-Tran, Peng Sun, S. Chantal E. Stieber, Alex John

Three vanadium complexes supported by salophan and salan ligands featuring differences in steric, electronic, and oxidation state (IV vs V) of the metal center have been evaluated for their potential in catalyzing the oxidative cleavage of a simple lignin model compound. All complexes were found to be effective, and under optimized conditions (145 °C, 48 h, in air) produced the cleavage products, phenol and benzoic acid, in good yields (62–69%) and selectivity (69–77%); significant differences in reactivity were not observed except at a lower temperature (125 °C). Complex 3c featuring sterically bulky tert butyl groups at ortho/para positions of the phenol arms, a cyclohexyl backbone and a V(V) center resulted in the highest yields and selectivity at 135 °C over 72 h (69–78% yield; 78–89% selectivity). Longer reaction times as well as reaction temperatures were found to compromise yield and selectivity for both cleavage products. An oxidizing atmosphere was found to be crucial for the observed reactivity as reactions attempted under an inert atmosphere did not result in significant conversion. Preliminary mechanistic investigations suggest that the lignin model compound is oxidized prior to undergoing cleavage, and the vanadium(V) complex is more effective at cleaving the oxidized product in comparison to the vanadium(IV) counterparts. Quite significantly, the oxidative cleavage was achieved in the absence of any basic or acidic additives.

Graphical Abstract

我们评估了由柳烷配体和柳烷配体支持的三种钒配合物,它们在催化一种简单木质素模型化合物的氧化裂解方面具有不同的立体、电子和氧化态(IV 与 V)。结果发现,所有络合物都是有效的,并且在优化条件下(145 °C、48 小时、空气中)都能以良好的产率(62-69%)和选择性(69-77%)生成裂解产物苯酚和苯甲酸;除了在较低温度(125 °C)下,反应活性没有明显差异。络合物 3c 在苯酚臂的正/副位置上具有立体笨重的叔丁基、环己基骨架和 V(V) 中心,在 135 °C 温度下反应 72 小时,产率和选择性最高(产率 69-78%;选择性 78-89%)。较长的反应时间和反应温度会影响两种裂解产物的产率和选择性。由于在惰性气氛下进行的反应不能产生显著的转化率,因此氧化气氛对观察到的反应活性至关重要。初步的机理研究表明,木质素模型化合物在发生裂解之前已被氧化,与钒(IV)复合物相比,钒(V)复合物能更有效地裂解氧化产物。值得注意的是,这种氧化裂解是在没有任何碱性或酸性添加剂的情况下实现的。
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引用次数: 0
Development of Electrochemical Immunosensors for Early Diagnosis of Polycystic Ovary Syndrome (PCOS), and Their Potential Mobile Phone Application 开发用于多囊卵巢综合征 (PCOS) 早期诊断的电化学免疫传感器及其潜在的手机应用
IF 3.6 3区 化学 Q2 CHEMISTRY, APPLIED Pub Date : 2024-02-03 DOI: 10.1007/s11244-023-01899-0
Muhammad Ali Yousif Al-Janabi, Ramazan Bayat, Muhammed Bekmezci, Tiri Rima Nour Elhouda, Fatih Sen, Afsaneh Kaffash, Mehdi Baghayeri, Hassan Rokni, Fatemeh Karimi

An effective way of monitoring the biomarker is with electrochemical sensor studies. In this work, it was formed using electrochemical deposition of high conductivity gold nanoparticles (AuNPs) and an amine-functional reduced graphene oxide (NH2-RGO) nanocomposite. This technique not only reduced HAuCl4 and graphene oxide in situ but also improved the electrocatalytic performance. XRD, SEM, and FTIR analytical methods confirmed the size and structure of the AuNPs/NH2-RGO nanoparticle. As a result of XRD analysis, AuNPs/NH2-RGO crystal structure was formed. In addition, antibodies (Ab) were immobilized on the modified electrode surface using a self-assembled monolayer. Cyclic voltammetry (CV) and differential pulse voltammetry (DPV) methods were used to evaluate the interaction of Ab with antigen. SHBG detection had a dynamic linear range of 0.6–12 nmol/L and a limit of detection (LOD) of 0.0043 µM in enhanced sensor applications. The AuNPs/NH2-RGO based sensor has the potential to be a valuable tool in clinical diagnostic applications in the future.

电化学传感器研究是监测生物标志物的有效方法。在这项工作中,利用电化学沉积高电导率金纳米粒子(AuNPs)和胺功能还原氧化石墨烯(NH2-RGO)纳米复合材料形成了这种传感器。这种技术不仅能原位还原 HAuCl4 和氧化石墨烯,还能提高电催化性能。XRD、SEM 和 FTIR 分析方法证实了 AuNPs/NH2-RGO 纳米粒子的尺寸和结构。XRD 分析结果表明,AuNPs/NH2-RGO 形成了晶体结构。此外,还利用自组装单层法将抗体(Ab)固定在改性电极表面。采用循环伏安法(CV)和差分脉冲伏安法(DPV)评估抗体与抗原的相互作用。在增强型传感器应用中,SHBG 检测的动态线性范围为 0.6-12 nmol/L,检测限 (LOD) 为 0.0043 µM。基于 AuNPs/NH2-RGO 的传感器有望成为未来临床诊断应用的重要工具。
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引用次数: 0
期刊
Topics in Catalysis
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